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Sample records for ultrafast solvation dynamics

  1. Achieving atomistic understanding of solvation dynamics from...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Mechanics and Quantum Mechanical Molecular Mechanics calculations, we have been ... Achieving atomistic understanding of solvation dynamics from X-ray free-electron laser ...

  2. Ionic Liquids: Radiation Chemistry, Solvation Dynamics and Reactivity Patterns

    SciTech Connect (OSTI)

    Wishart, J.F.

    2011-06-12

    , which need to be quantified for the successful use under radiolytic conditions. Electron solvation dynamics in ILs are measured directly when possible and estimated using proxies (e.g. coumarin-153 dynamic emission Stokes shifts or benzophenone anion solvation) in other cases. Electron reactivity is measured using ultrafast kinetics techniques for comparison with the solvation process.

  3. Solvation!

    SciTech Connect (OSTI)

    Ivana Adamovic

    2004-12-19

    This dissertation consists of two closely related parts: theory development and coding of correlation effects in a model potential for solvation, and study of solvent effects on chemical reactions and processes. The effective fragment potential (EFP) method has been re-parameterized, using density functional theory (DFT), more specifically, the B3LYP functional. The DFT based EFP method includes short-range correlation effects; hence it is a first step in incorporating the treatment of correlation in the EFP solvation model. In addition, the gradient of the charge penetration term in the EFP model was derived and coded. The new method has been implemented in the electronic structure code GAMESS and is in use. Formulas for the dynamic dipole polarizability, C{sub 6} dispersion coefficient and dispersion energy were derived and coded as a part of a treatment of the dispersion interactions in the general solvation model, EFP2. Preliminary results are in good agreement with experimental and other theoretical data. The DFT based EFP (EFP1/DFT) method was used in the study of microsolvation effects on the S{sub N}2 substitution reaction, between chloride and methyl bromide. Changes in the central barrier, for several lowest lying isomers of the systems with one, two, three and four waters, were studied using second order perturbation theory (MP2), DFT and mixed quantum mechanics (QM)/(EFP1/DFT) methods. EFP1/DFT is found to reproduce QM results with high accuracy, at just a fraction of the cost. Molecular structures and potential energy surfaces for IHI{sup -} {center_dot} Ar{sub n} (n=1-7) were studied using the MP2 method. Experimentally observed trends in the structural arrangement of the Ar atoms were explained through the analysis of the geometrical parameters and three-dimensional MP2 molecular electrostatic potentials.

  4. Ultrafast studies of solution dynamics

    SciTech Connect (OSTI)

    Woodruff, W.H.; Dyer, R.B.; Callender, R.H.

    1997-10-01

    This is the final report of a one-year, Laboratory Directed Research and Development (LDRD) project at Los Alamos National Laboratory (LANL). Fast chemical dynamics generally must be initiated photochemically. This limits the applicability of modern laser methods for following the structural changes that occur during chemical and biological reactions to those systems that have an electronic chromophore that has a significant yield of photoproduct when excited. This project has developed a new and entirely general approach to ultrafast initiation of reactions in solution: laser-induced temperature jump (T-jump). The results open entire new fields of study of ultrafast molecular dynamics in solution. The authors have demonstrated the T-jump technique on time scales of 50 ps and longer, and have applied it to study of the fast events in protein folding. They find that a general lifetime of alpha-helix formation is ca 100 ns, and that tertiary folds (in apomyoglobin) form in ca 100 {mu}s.

  5. Interfacial effects revealed by ultrafast relaxation dynamics...

    Office of Scientific and Technical Information (OSTI)

    Title: Interfacial effects revealed by ultrafast relaxation dynamics in BiFeO 3 YBa 2 Cu 3 O 7 bilayers Authors: Springer, D. ; Nair, Saritha K. ; He, Mi ; Lu, C. L. ; Cheong, S. ...

  6. Ionic Liquids: Radiation Chemistry, Solvation Dynamics and Reactivity Patterns

    SciTech Connect (OSTI)

    Wishart,J.F.

    2008-09-29

    Ionic liquids (ILs) are a rapidly expanding family of condensed-phase media with important applications in energy production, nuclear fuel and waste processing, improving the efficiency and safety of industrial chemical processes, and pollution prevention. ILs are generally nonvolatile, noncombustible, highly conductive, recyclable and capable of dissolving a wide variety of materials. They are finding new uses in chemical synthesis, catalysis, separations chemistry, electrochemistry and other areas. Ionic liquids have dramatically different properties compared to conventional molecular solvents, and they provide a new and unusual environment to test our theoretical understanding of charge transfer and other reactions. We are interested in how IL properties influence physical and dynamical processes that determine the stability and lifetimes of reactive intermediates and thereby affect the courses of chemical reactions and product distributions. Successful use of ionic liquids in radiation-filled environments, where their safety advantages could be significant, requires an understanding of ionic liquid radiation chemistry. For example, characterizing the primary steps of IL radiolysis will reveal radiolytic degradation pathways and suggest ways to prevent them or mitigate their effects on the properties of the material. An understanding of ionic liquid radiation chemistry will also facilitate pulse radiolysis studies of general chemical reactivity in ILs, which will aid in the development of applications listed above. Very early in our radiolysis studies it became evident that slow solvation dynamics of the excess electron in ILs (which vary over a wide viscosity range) increases the importance of pre-solvated electron reactivity and consequently alters product distributions. Parallel studies of IL solvation phenomena using coumarin-153 dynamic Stokes shifts and polarization anisotropy decay rates are done to compare with electron solvation studies and to evaluate

  7. IONIC LIQUIDS: RADIATION CHEMISTRY, SOLVATION DYNAMICS AND REACTIVITY PATTERNS.

    SciTech Connect (OSTI)

    WISHART,J.F.

    2007-10-01

    energy production, nuclear fuel and waste processing, improving the efficiency and safety of industrial chemical processes, and pollution prevention. ILs are generally nonvolatile, noncombustible, highly conductive, recyclable and capable of dissolving a wide variety of materials. They are finding new uses in chemical synthesis, catalysis, separations chemistry, electrochemistry and other areas. Ionic liquids have dramatically different properties compared to conventional molecular solvents, and they provide a new and unusual environment to test our theoretical understanding of charge transfer and other reactions. We are interested in how IL properties influence physical and dynamical processes that determine the stability and lifetimes of reactive intermediates and thereby affect the courses of chemical reactions and product distributions. Successful use of ionic liquids in radiation-filled environments, where their safety advantages could be significant, requires an understanding of ionic liquid radiation chemistry. For example, characterizing the primary steps of IL radiolysis will reveal radiolytic degradation pathways and suggest ways to prevent them or mitigate their effects on the properties of the material. An understanding of ionic liquid radiation chemistry will also facilitate pulse radiolysis studies of general chemical reactivity in ILs, which will aid in the development of applications listed above. Very early in our radiolysis studies it became evident that slow solvation dynamics of the excess electron in ILs (which vary over a wide viscosity range) increases the importance of pre-solvated electron reactivity and consequently alters product distributions. Parallel studies of IL solvation phenomena using coumarin-153 dynamic Stokes shifts and polarization anisotropy decay rates are done to compare with electron solvation studies and to evaluate the influence of ILs on charge transport processes. Methods. Picosecond pulse radiolysis studies at BNL

  8. Ultrafast optical control of magnetization dynamics in polycrystalline...

    Office of Scientific and Technical Information (OSTI)

    bismuth doped iron garnet thin films Citation Details In-Document Search Title: Ultrafast optical control of magnetization dynamics in polycrystalline bismuth doped iron ...

  9. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    isotope substitution experiments and molecular dynamics simulations, researchers from Sweden, Germany, and the U.S. have shown that the ultrafast (0- to 10-fs) dissociation...

  10. Ultrafast Charge Dynamics Initiated by High-Intensity, Ultrashort...

    Office of Scientific and Technical Information (OSTI)

    Journal Article: Ultrafast Charge Dynamics Initiated by High-Intensity, Ultrashort Laser-Matter Interaction Citation ... We report results of recent experiment in which such charge ...

  11. Ultrafast carriers dynamics in filled-skutterudites

    SciTech Connect (OSTI)

    Guo, Liang; Xu, Xianfan; Salvador, James R.

    2015-06-08

    Carrier dynamics of filled-skutterudites, an important class of thermoelectric materials, is investigated using ultrafast optical spectroscopy. By tuning the wavelength of the probe laser, charge transfers at different electronic energy levels are interrogated. Analysis based on the Kramers-Kronig relation explains the complex spectroscopy data, which is mainly due to band filling caused by photo-excited carriers and free carrier absorption. The relaxation time of hot carriers is found to be about 0.4–0.6 ps, depending on the electronic energy level, and the characteristic time for carrier-phonon equilibrium is about 0.95 ps. These studies of carrier dynamics, which fundamentally determines the transport properties of thermoelectric material, can provide guidance for the design of materials.

  12. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Core-Hole Induced Dynamics in Water Ultrafast Core-Hole Induced Dynamics in Water Print Wednesday, 22 February 2006 00:00 A thorough understanding of the chemical processes that are initiated when radiation interacts with aqueous systems is essential for many diverse fields, from condensed matter physics to medicine to environmental science. An incoming photon with enough energy to produce a core hole in a water molecule sets off motions that can affect bonding configurations, which in

  13. Ultrafast Dynamic Response of Single Crystal PETN and Beta-HMX...

    Office of Scientific and Technical Information (OSTI)

    Conference: Ultrafast Dynamic Response of Single Crystal PETN and Beta-HMX Citation Details In-Document Search Title: Ultrafast Dynamic Response of Single Crystal PETN and Beta-HMX...

  14. Ultrafast resonant soft x-ray diffraction dynamics of the charge...

    Office of Scientific and Technical Information (OSTI)

    Ultrafast resonant soft x-ray diffraction dynamics of the charge density wave in TbTe 3 ... Title: Ultrafast resonant soft x-ray diffraction dynamics of the charge density wave in ...

  15. Ultrafast Magnetism Dynamics Measure Using Tabletop Ultrafast EUV Sources

    SciTech Connect (OSTI)

    Silva, Thomas J.; Murnane, Margaret

    2013-08-21

    In our work to date, we made two significant advances. First we demonstrated element-selective demagnetization dynamics for the first time, with a record time resolution for x-ray probing of 55 fs. Second, in new work, we were able to probe the timescale of the exchange interaction in magnetic materials, also for the first time. Our measurements were made using the transverse magneto-optic Kerr effect (T-MOKE) geometry, since the reflectivity of a magnetic material changes with the direction of the magnetization vector of a surface. In our experiment, we periodically reversed the magnetization direction of a grating structure made of Permalloy (Ni80Fe20) using an external magnetic field. To achieve maximum contrast, we used HHG light spanning the M-shell (3p) absorption edges of Fe and Ni. Our characterization of the static magnetization of a Permalloy sample shows high magnetic asymmetry at photon energies just above and below the absorption edges at 55 eV and 65 eV, respectively. This result is in excellent agreement with measurements done on the same using a synchrotron source.

  16. First Principals and Classical Molecular Dynamics Simulations of Solvated Benzene

    SciTech Connect (OSTI)

    Allesch, M; Lightstone, F; Schwegler, E; Galli, G

    2007-09-11

    We have performed extensive ab initio and classical MD simulations of benzene in water in order to examine the unique solvation structures that are formed. Qualitative differences between classical and ab initio MD simulations are found and the importance of various technical simulation parameters is examined. Our comparison indicates that non-polarizable classical models are not capable of describing the solute-water interface correctly if local interactions become energetically comparable to water hydrogen bonds. In addition, a comparison is made between a rigid water model and fully flexible water within ab initio MD simulations which shows that both models agree qualitatively for this challenging system.

  17. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Core-Hole Induced Dynamics in Water Print A thorough understanding of the chemical processes that are initiated when radiation interacts with aqueous systems is essential for many diverse fields, from condensed matter physics to medicine to environmental science. An incoming photon with enough energy to produce a core hole in a water molecule sets off motions that can affect bonding configurations, which in turn affect subsequent chemical-reaction pathways. However, it is a fundamental

  18. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Core-Hole Induced Dynamics in Water Print A thorough understanding of the chemical processes that are initiated when radiation interacts with aqueous systems is essential for many diverse fields, from condensed matter physics to medicine to environmental science. An incoming photon with enough energy to produce a core hole in a water molecule sets off motions that can affect bonding configurations, which in turn affect subsequent chemical-reaction pathways. However, it is a fundamental

  19. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Core-Hole Induced Dynamics in Water Print A thorough understanding of the chemical processes that are initiated when radiation interacts with aqueous systems is essential for many diverse fields, from condensed matter physics to medicine to environmental science. An incoming photon with enough energy to produce a core hole in a water molecule sets off motions that can affect bonding configurations, which in turn affect subsequent chemical-reaction pathways. However, it is a fundamental

  20. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Core-Hole Induced Dynamics in Water Print A thorough understanding of the chemical processes that are initiated when radiation interacts with aqueous systems is essential for many diverse fields, from condensed matter physics to medicine to environmental science. An incoming photon with enough energy to produce a core hole in a water molecule sets off motions that can affect bonding configurations, which in turn affect subsequent chemical-reaction pathways. However, it is a fundamental

  1. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Core-Hole Induced Dynamics in Water Print A thorough understanding of the chemical processes that are initiated when radiation interacts with aqueous systems is essential for many diverse fields, from condensed matter physics to medicine to environmental science. An incoming photon with enough energy to produce a core hole in a water molecule sets off motions that can affect bonding configurations, which in turn affect subsequent chemical-reaction pathways. However, it is a fundamental

  2. Ultrafast image-based dynamic light scattering for nanoparticle...

    Office of Scientific and Technical Information (OSTI)

    An ultrafast sizing method for nanoparticles is proposed, called as UIDLS (Ultrafast ... This method makes use of the intensity fluctuation of scattered light from nanoparticles ...

  3. Ultrafast dynamic ellipsometry and spectroscopy of laser shocked materials

    SciTech Connect (OSTI)

    Mcgrane, Shawn David [Los Alamos National Laboratory; Bolme, Cindy B [Los Alamos National Laboratory; Whitley, Von H [Los Alamos National Laboratory; Moore, David S [Los Alamos National Laboratory

    2010-01-01

    Shock waves create extreme states of matter with very high pressures, temperatures, and volumetric compressions, at an exceedingly rapid rate of change. We review how to use a beamsplitter and a note card to turn a typical chirp pulse amplified femtosecond laser system into an ultrafast shock dynamics machine. Open scientific questions that can be addressed with such an apparatus are described. We report on the development of several single shot time resolved diagnostics needed to answer these questions. These single shot diagnostics are expected to be broadly applicable to other types of laser ablation experiments. Experimental results measured from shocked material dynamics of several systems are detailed. Finally, we report on progress towards using transient absorption as a measure of electronic excitation and coherent Raman as a picosecond probe of temperature in shock compressed condensed matter.

  4. Ultrafast myoglobin structural dynamics observed with an X-ray...

    Office of Scientific and Technical Information (OSTI)

    An ultrafast increase of myoglobin radius of gyration occurs within 1 picosecond and is followed by a delayed protein expansion. As the system approaches equilibrium it undergoes ...

  5. Ultrafast Structural Dynamics in Combustion Relevant Model Systems

    SciTech Connect (OSTI)

    Weber, Peter M.

    2014-03-31

    The research project explored the time resolved structural dynamics of important model reaction system using an array of novel methods that were developed specifically for this purpose. They include time resolved electron diffraction, time resolved relativistic electron diffraction, and time resolved Rydberg fingerprint spectroscopy. Toward the end of the funding period, we also developed time-resolved x-ray diffraction, which uses ultrafast x-ray pulses at LCLS. Those experiments are just now blossoming, as the funding period expired. In the following, the time resolved Rydberg Fingerprint Spectroscopy is discussed in some detail, as it has been a very productive method. The binding energy of an electron in a Rydberg state, that is, the energy difference between the Rydberg level and the ground state of the molecular ion, has been found to be a uniquely powerful tool to characterize the molecular structure. To rationalize the structure sensitivity we invoke a picture from electron diffraction: when it passes the molecular ion core, the Rydberg electron experiences a phase shift compared to an electron in a hydrogen atom. This phase shift requires an adjustment of the binding energy of the electron, which is measurable. As in electron diffraction, the phase shift depends on the molecular, geometrical structure, so that a measurement of the electron binding energy can be interpreted as a measurement of the molecules structure. Building on this insight, we have developed a structurally sensitive spectroscopy: the molecule is first elevated to the Rydberg state, and the binding energy is then measured using photoelectron spectroscopy. The molecules structure is read out as the binding energy spectrum. Since the photoionization can be done with ultrafast laser pulses, the technique is inherently capable of a time resolution in the femtosecond regime. For the purpose of identifying the structures of molecules during chemical reactions, and for the analysis of

  6. Dynamics of electron solvation in methanol: Excited state relaxation and generation by charge-transfer-to-solvent

    SciTech Connect (OSTI)

    Elkins, Madeline H.; Williams, Holly L.; Neumark, Daniel M.

    2015-06-21

    The charge-transfer-to-solvent dynamics (CTTS) and excited state relaxation mechanism of the solvated electron in methanol are studied by time-resolved photoelectron spectroscopy on a liquid methanol microjet by means of two-pulse and three-pulse experiments. In the two-pulse experiment, CTTS excitation is followed by a probe photoejection pulse. The resulting time-evolving photoelectron spectrum reveals multiple time scales characteristic of relaxation and geminate recombination of the initially generated electron which are consistent with prior results from transient absorption. In the three-pulse experiment, the relaxation dynamics of the solvated electron following electronic excitation are measured. The internal conversion lifetime of the excited electron is found to be 130 40 fs, in agreement with extrapolated results from clusters and the non-adiabatic relaxation mechanism.

  7. Structural aspects of the solvation shell of lysine and acetylated lysine: A Car-Parrinello and classical molecular dynamics investigation

    SciTech Connect (OSTI)

    Carnevale, V.; Raugei, S.

    2009-12-14

    Lysine acetylation is a post-translational modification, which modulates the affinity of protein-protein and/or protein-DNA complexes. Its crucial role as a switch in signaling pathways highlights the relevance of charged chemical groups in determining the interactions between water and biomolecules. A great effort has been recently devoted to assess the reliability of classical molecular dynamics simulations in describing the solvation properties of charged moieties. In the spirit of these investigations, we performed classical and Car-Parrinello molecular dynamics simulations on lysine and acetylated-lysine in aqueous solution. A comparative analysis between the two computational schemes is presented with a focus on the first solvation shell of the charged groups. An accurate structural analysis unveils subtle, yet statistically significant, differences which are discussed in connection to the significant electronic density charge transfer occurring between the solute and the surrounding water molecules.

  8. Electron Solvation Dynamics and Reactivity in Ionic Liquids Observed by Picosecond RadiolysisTechniques

    SciTech Connect (OSTI)

    Wishart J. F.; Funston, A.M.; Szreder, T.; Cook, A.R.; Gohdo, M.

    2012-01-01

    On time scales of a nanosecond or less, radiolytically-generated excess electrons in ionic liquids undergo solvation processes and reactions that determine all subsequent chemistry and the accumulation of radiolytic damage. Using picosecond pulse radiolysis detection methods, we observed and quantified the solvation response of the electron in 1-methyl-1-butyl-pyrrolidinium bis(trifluoromethylsulfonyl)amide and used it to understand electron scavenging by a typical solute, duroquinone.

  9. Simultaneous investigation of ultrafast structural dynamics and transient electric field by sub-picosecond electron pulses

    SciTech Connect (OSTI)

    Li, Run-Ze; Zhu, Pengfei; Chen, Long; Chen, Jie E-mail: jzhang1@sjtu.edu.cn; Sheng, Zheng-Ming; Zhang, Jie E-mail: jzhang1@sjtu.edu.cn; Cao, Jianming

    2014-05-14

    The ultrafast structure dynamics and surface transient electric field, which are concurrently induced by laser excited electrons of an aluminum nanofilm, have been investigated simultaneously by the same transmission electron diffraction patterns. These two processes are found to be significantly different and distinguishable by tracing the time dependent changes of electron diffraction and deflection angles, respectively. This study also provides a practical means to evaluate simultaneously the effect of transient electric field during the study of structural dynamics under low pump fluence by transmission ultrafast electron diffraction.

  10. Lattice and Carrier Dynamics in Quantum-Confined Materials on Ultrafast

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Timescales | MIT-Harvard Center for Excitonics Lattice and Carrier Dynamics in Quantum-Confined Materials on Ultrafast Timescales April 3, 2014 at 3pm/36-428 Richard Schaller Department of Chemistry, Northwestern University, Argonne National Laboratory richard-schaller_000 Abstract: Excess carrier energy, which many aim to utilize for advanced energy conversion technologies, rapidly dissipates from electrons and holes in both bulk and quantum confined semiconductors despite expectation of

  11. Ultrafast Dynamic Response of Single Crystal PETN and Beta-HMX (Conference)

    Office of Scientific and Technical Information (OSTI)

    | SciTech Connect Dynamic Response of Single Crystal PETN and Beta-HMX Citation Details In-Document Search Title: Ultrafast Dynamic Response of Single Crystal PETN and Beta-HMX Authors: Zaug, J M ; Armstrong, M R ; Crowhurst, J C ; Feranti, L ; Swan, R ; Gross, R ; Teshlich, N E ; Wall, M ; Austin, R A ; Fried, L E Publication Date: 2014-06-30 OSTI Identifier: 1149550 Report Number(s): LLNL-CONF-656341 DOE Contract Number: DE-AC52-07NA27344 Resource Type: Conference Resource Relation:

  12. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    with pump-probe measurements. Using a combination of isotope substitution experiments and molecular dynamics simulations, researchers from Sweden, Germany, and the U.S. have shown...

  13. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Waters If you look deeply enough at even the stillest of waters, as deep as the molecular level, you will find a surprisingly turbulent, dynamic universe. The water...

  14. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    radiation therapy. The detailed study of substances in the condensed and dynamic liquid state poses unique challenges that aren't an issue with isolated gas molecules or solids...

  15. Ultrafast dynamics of type-II GaSb/GaAs quantum dots

    SciTech Connect (OSTI)

    Komolibus, K.; Piwonski, T.; Gradkowski, K.; Reyner, C. J.; Liang, B.; Huffaker, D. L.; Huyet, G.; Houlihan, J.

    2015-01-19

    In this paper, room temperature two-colour pump-probe spectroscopy is employed to study ultrafast carrier dynamics in type-II GaSb/GaAs quantum dots. Our results demonstrate a strong dependency of carrier capture/escape processes on applied reverse bias voltage, probing wavelength and number of injected carriers. The extracted timescales as a function of both forward and reverse bias may provide important information for the design of efficient solar cells and quantum dot memories based on this material. The first few picoseconds of the dynamics reveal a complex behaviour with an interesting feature, which does not appear in devices based on type-I materials, and hence is linked to the unique carrier capture/escape processes possible in type-II structures.

  16. Spatially resolved ultrafast magnetic dynamics initiated at a complex oxide heterointerface

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Forst, M.; Wilkins, S. B.; Caviglia, A. D.; Scherwitz, R.; Mankowsky, R.; Zubko, P.; Khanna, V.; Bromberger, H.; Chuang, Y. -D.; Lee, W. S.; et al

    2015-07-06

    Static strain in complex oxide heterostructures1,2 has been extensively used to engineer electronic and magnetic properties at equilibrium3. In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across heterointerfaces dynamically4. Here, by exciting large-amplitude infrared-active vibrations in a LaAlO3 substrate we induce magnetic order melting in a NdNiO3 film across a heterointerface. Femtosecond resonant soft X-ray diffraction is used to determine the spatiotemporal evolution of the magnetic disordering. We observe a magnetic melt front that propagates from the substrate interface into the film, at a speed that suggests electronically driven motion.more » Lastly, light control and ultrafast phase front propagation at heterointerfaces may lead to new opportunities in optomagnetism, for example by driving domain wall motion to transport information across suitably designed devices.« less

  17. Spatially resolved ultrafast magnetic dynamics initiated at a complex oxide heterointerface

    SciTech Connect (OSTI)

    Forst, M.; Wilkins, S. B.; Caviglia, A. D.; Scherwitz, R.; Mankowsky, R.; Zubko, P.; Khanna, V.; Bromberger, H.; Chuang, Y. -D.; Lee, W. S.; Schlotter, W. F.; Turner, J. J.; Dakovski, G. L.; Minitti, M. P.; Robinson, J.; Clark, S. R.; Jaksch, D.; Triscone, J. -M.; Hill, J. P.; Dhesi, S. S.; Cavalleri, A.

    2015-07-06

    Static strain in complex oxide heterostructures1,2 has been extensively used to engineer electronic and magnetic properties at equilibrium3. In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across heterointerfaces dynamically4. Here, by exciting large-amplitude infrared-active vibrations in a LaAlO3 substrate we induce magnetic order melting in a NdNiO3 film across a heterointerface. Femtosecond resonant soft X-ray diffraction is used to determine the spatiotemporal evolution of the magnetic disordering. We observe a magnetic melt front that propagates from the substrate interface into the film, at a speed that suggests electronically driven motion. Lastly, light control and ultrafast phase front propagation at heterointerfaces may lead to new opportunities in optomagnetism, for example by driving domain wall motion to transport information across suitably designed devices.

  18. Ultrafast carrier dynamics in the large-magnetoresistance material WTe2

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Dai, Y. M.; Bowlan, J.; Li, H.; Miao, H.; Wu, S. F.; Kong, W. D.; Shi, Y. G.; Trugman, S. A.; Zhu, J. -X.; Ding, H.; et al

    2015-10-07

    In this study, ultrafast optical pump-probe spectroscopy is used to track carrier dynamics in the large-magnetoresistance material WTe2. Our experiments reveal a fast relaxation process occurring on a subpicosecond time scale that is caused by electron-phonon thermalization, allowing us to extract the electron-phonon coupling constant. An additional slower relaxation process, occurring on a time scale of ~5–15 ps, is attributed to phonon-assisted electron-hole recombination. As the temperature decreases from 300 K, the time scale governing this process increases due to the reduction of the phonon population. However, below ~50 K, an unusual decrease of the recombination time sets in, mostmore » likely due to a change in the electronic structure that has been linked to the large magnetoresistance observed in this material.« less

  19. Lithium Ion Solvation and Diffusion in Bulk Organic Electrolytes...

    Office of Scientific and Technical Information (OSTI)

    Title: Lithium Ion Solvation and Diffusion in Bulk Organic Electrolytes from First Principles and Classical Reactive Molecular Dynamics Authors: Ong, M T ; Verners, O ; Draeger, E ...

  20. Lithium Ion Solvation and Diffusion in Bulk Organic Electrolytes...

    Office of Scientific and Technical Information (OSTI)

    in Bulk Organic Electrolytes from First Principles Molecular Dynamics Citation Details In-Document Search Title: Lithium Ion Solvation and Diffusion in Bulk Organic ...

  1. Ultrafast dynamics of liquid water: Frequency fluctuations of the OH stretch and the HOH bend

    SciTech Connect (OSTI)

    Imoto, Sho; Xantheas, Sotiris S.; Saito, Shinji

    2013-07-28

    Frequency fluctuations of the OH stretch and the HOH bend in liquid water are reported from the third-order response function evaluated using the TTM3-F potential for water. The simulated two-dimensional infrared (IR) spectra of the OH stretch are similar to previously reported theoretical results. The present study suggests that the frequency fluctuation of the HOH bend is faster than that of the OH stretch. The ultrafast loss of the frequency correlation of the HOH bend is due to the strong couplings with the OH stretch as well as the intermolecular hydrogen bond bend.

  2. Dynamic Processes in Biology, Chemistry, and Materials Science: Opportunities for UltraFast Transmission Electron Microscopy - Workshop Summary Report

    SciTech Connect (OSTI)

    Kabius, Bernd C.; Browning, Nigel D.; Thevuthasan, Suntharampillai; Diehl, Barbara L.; Stach, Eric A.

    2012-07-25

    This report summarizes a 2011 workshop that addressed the potential role of rapid, time-resolved electron microscopy measurements in accelerating the solution of important scientific and technical problems. A series of U.S. Department of Energy (DOE) and National Academy of Science workshops have highlighted the critical role advanced research tools play in addressing scientific challenges relevant to biology, sustainable energy, and technologies that will fuel economic development without degrading our environment. Among the specific capability needs for advancing science and technology are tools that extract more detailed information in realistic environments (in situ or operando) at extreme conditions (pressure and temperature) and as a function of time (dynamic and time-dependent). One of the DOE workshops, Future Science Needs and Opportunities for Electron Scattering: Next Generation Instrumentation and Beyond, specifically addressed the importance of electron-based characterization methods for a wide range of energy-relevant Grand Scientific Challenges. Boosted by the electron optical advancement in the last decade, a diversity of in situ capabilities already is available in many laboratories. The obvious remaining major capability gap in electron microscopy is in the ability to make these direct in situ observations over a broad spectrum of fast (µs) to ultrafast (picosecond [ps] and faster) temporal regimes. In an effort to address current capability gaps, EMSL, the Environmental Molecular Sciences Laboratory, organized an Ultrafast Electron Microscopy Workshop, held June 14-15, 2011, with the primary goal to identify the scientific needs that could be met by creating a facility capable of a strongly improved time resolution with integrated in situ capabilities. The workshop brought together more than 40 leading scientists involved in applying and/or advancing electron microscopy to address important scientific problems of relevance to DOE’s research

  3. Ultrafast myoglobin structural dynamics observed with an X-ray free-electron laser

    SciTech Connect (OSTI)

    Levantino, Matteo; Schirò, Giorgio; Lemke, Henrik Till; Cottone, Grazia; Glownia, James Michael; Zhu, Diling; Chollet, Mathieu; Ihee, Hyotcherl; KAIST, Daejeon; Cupane, Antonio; Cammarata, Marco

    2015-04-02

    Light absorption can trigger biologically relevant protein conformational changes. The light induced structural rearrangement at the level of a photoexcited chromophore is known to occur in the femtosecond timescale and is expected to propagate through the protein as a quake-like intramolecular motion. Here we report direct experimental evidence of such ‘proteinquake’ observed in myoglobin through femtosecond X-ray solution scattering measurements performed at the Linac Coherent Light Source X-ray free-electron laser. An ultrafast increase of myoglobin radius of gyration occurs within 1 picosecond and is followed by a delayed protein expansion. As the system approaches equilibrium it undergoes damped oscillations with a ~3.6-picosecond time period. Our results unambiguously show how initially localized chemical changes can propagate at the level of the global protein conformation in the picosecond timescale.

  4. Ultrafast myoglobin structural dynamics observed with an X-ray free-electron laser

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Levantino, Matteo; Schirò, Giorgio; Lemke, Henrik Till; Cottone, Grazia; Glownia, James Michael; Zhu, Diling; Chollet, Mathieu; Ihee, Hyotcherl; KAIST, Daejeon; Cupane, Antonio; et al

    2015-04-02

    Light absorption can trigger biologically relevant protein conformational changes. The light induced structural rearrangement at the level of a photoexcited chromophore is known to occur in the femtosecond timescale and is expected to propagate through the protein as a quake-like intramolecular motion. Here we report direct experimental evidence of such ‘proteinquake’ observed in myoglobin through femtosecond X-ray solution scattering measurements performed at the Linac Coherent Light Source X-ray free-electron laser. An ultrafast increase of myoglobin radius of gyration occurs within 1 picosecond and is followed by a delayed protein expansion. As the system approaches equilibrium it undergoes damped oscillations withmore » a ~3.6-picosecond time period. Our results unambiguously show how initially localized chemical changes can propagate at the level of the global protein conformation in the picosecond timescale.« less

  5. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Transformations in Superionic Nanocrystals Ultrafast Transformations in Superionic Nanocrystals Print Wednesday, 29 January 2014 00:00 A superionic material is a multi-component solid with simultaneous characteristics of both a solid and a liquid. Above a critical temperature associated with a structural phase transition, one of the atomic species in the material will exhibit liquid-like ionic conductivity and dynamic disorder within the rigid crystalline structure of the other.

  6. Ultrafast dynamics of liquid water: Energy relaxation and transfer processes of the OH stretch and the HOH bend

    SciTech Connect (OSTI)

    Imoto, Sho; Xantheas, Sotiris S.; Saito, Shinji

    2015-08-27

    The vibrational energy relaxation and transfer processes of the OH stretching and the HOH bending vibrations in liquid water are investigated via the theoretical calculation of the pump-probe spectra obtained from non-equilibrium molecular dynamics simulations with the TTM3-F interaction potential. The excitation of the OH stretch induces an instantaneous response of the high frequency librational motions in the 600-1000 cm-1 range. In addition, the excess energy of the OH stretch of a water molecule quickly transfers to the OH stretches of molecules in its first hydration shell with a time constant of ~50 fs, followed by relaxation to the HOH bends of the surrounding molecules with a time constant of 230 fs. The excitation of the HOH bend also results in the ultrafast excitation of the high frequency librational motions. The energy of the excited HOH bend of a water molecule decays, with a time constant of 200 fs, mainly to the relaxation of the HOH bends of its surrounding molecules. The energies of the HOH bends were found to transfer quickly to the intermolecular motions via the coupling with the high frequency librational motions. The excess energy of the OH stretch or the HOH bend relaxes to the high frequency intermolecular librational motions and eventually to the hot ground state with a time scale of ~1 ps via the coupling with the librational and translational motions. The energy relaxation and transfer processes were found to depend on the local hydrogen bonding network; the relaxations of the excess energy of the OH stretch and the HOH bend of four- and five-coordinated molecules are faster than those of a three-coordinated molecule due to the delocalization of the vibrational motions of the former (four- and five-coordinated molecules) compared to those of the later (three-coordinated molecules). The present results highlight the importance of the high frequency intermolecular librational modes in facilitating the ultrafast energy relaxation process in

  7. Ultrafast laser spectroscopy in complex solid state materials

    SciTech Connect (OSTI)

    Li, Tianqi

    2014-12-01

    This thesis summarizes my work on applying the ultrafast laser spectroscopy to the complex solid state materials. It shows that the ultrafast laser pulse can coherently control the material properties in the femtosecond time scale. And the ultrafast laser spectroscopy can be employed as a dynamical method for revealing the fundamental physical problems in the complex material systems.

  8. Structural Interactions within Lithium Salt Solvates: Acyclic...

    Office of Scientific and Technical Information (OSTI)

    Structural Interactions within Lithium Salt Solvates: Acyclic Carbonates and Esters Citation Details In-Document Search Title: Structural Interactions within Lithium Salt Solvates: ...

  9. Ultrafast harmonic rf kicker design and beam dynamics analysis for an energy recovery linac based electron circulator cooler ring

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Huang, Yulu; Wang, Haipeng; Rimmer, Robert A.; Wang, Shaoheng; Guo, Jiquan

    2016-08-01

    An ultrafast kicker system is being developed for the energy recovery linac (ERL) based electron circulator cooler ring (CCR) in the proposed Jefferson Lab Electron Ion Collider (JLEIC, previously named MEIC). In the CCR, the injected electron bunches can be recirculated while performing ion cooling for 10–30 turns before the extraction, thus reducing the recirculation beam current in the ERL to 1/10–1/30 (150mA–50 mA) of the cooling beam current (up to 1.5 A). Assuming a bunch repetition rate of 476.3 MHz and a recirculating factor of 10 in the CCR, the kicker is required to operate at a pulse repetitionmore » rate of 47.63 MHz with pulse width of around 2 ns, so that only every 10th bunch in the CCR will experience a transverse kick while the rest of the bunches will not be disturbed. Such a kicker pulse can be synthesized by ten harmonic modes of the 47.63 MHz kicker pulse repetition frequency, using up to four quarter wavelength resonator (QWR) based deflecting cavities. In this paper, several methods to synthesize such a kicker waveform will be discussed and a comparison of their beam dynamics performance is made using ELEGANT. Four QWR cavities are envisaged with high transverse shunt impedance requiring less than 100 W of total rf power for a Flat-Top kick pulse. Multipole fields due to the asymmetry of this type of cavity are analyzed. The transverse emittance growth due to the sextupole component is simulated in ELEGANT. In conclusion, off-axis injection and extraction issues and beam optics using a multicavity kick-drift scheme will also be discussed.« less

  10. Single shot ultrafast dynamic ellipsometry (UDE) of laser-driven shocks in single crystal explosives

    SciTech Connect (OSTI)

    Whitley, Von H; Mcgrane, Shawn D; Moore, David S; Eakins, Dan E; Bolme, Cindy A

    2009-01-01

    We report on the first experiments to measure states in shocked energetic single crystals with dynamic ellipsometry. We demonstrate that these ellipsometric techniques can produce reasonable Hugoniot values using small amounts of crystalline RDX and PETN. Pressures, particle velocities and shock velocities obtained using shocked ellipsometry are comparable to those found using gas-gun flyer plates and molecular dynamics calculations. The adaptation of the technique from uniform thin films of polymers to thick non-perfect crystalline materials was a significant achievement. Correct sample preparation proved to be a crucial component. Through trial and error, we were able to resolve polishing issues, sample quality problems, birefringence effects and mounting difficulties that were not encountered using thin polymer films.

  11. Low-power, ultrafast, and dynamic all-optical tunable plasmonic analog to electromagnetically induced transparency in two resonators side-coupled with a waveguide system

    SciTech Connect (OSTI)

    Wang, Boyun; Wang, Tao Li, Xiaoming; Han, Xu; Zhu, Youjiang

    2015-06-07

    We theoretically and numerically investigate a low-power, ultrafast, and dynamic all-optical tunable plasmonic analog to electromagnetically induced transparency (EIT) in two nanodisk resonators side-coupled to a metal-insulator-metal plasmonic waveguide system. The optical Kerr effect is enhanced by the slow light effect of the plasmonic EIT-like effect and the plasmonic waveguide based on graphene-Ag composite material structures with giant effective Kerr nonlinear coefficient. The optical Kerr effect modulation method is applied to improve tuning rate with response time of subpicoseconds or even femtoseconds. With dynamically tuning the propagation phase of the plasmonic waveguide, π-phase shift of the transmission spectrum in the plasmonic EIT-like system is achieved under excitation of a pump light with an intensity as low as 5.85 MW/cm{sup 2}. The group delay is controlled between 0.09 and 0.4 ps. All observed schemes are analyzed rigorously through finite-difference time-domain simulations and coupled-mode formalism. Results show a new direction toward the low power consumption and ultrafast responses of integration plasmonic photonic devices and all-optical dynamical storage of light devices in optical communication and quantum information processing.

  12. Tracing ultrafast dynamics of strong fields at plasma-vacuum interfaces with longitudinal proton probing

    SciTech Connect (OSTI)

    Abicht, F.; Braenzel, J.; Koschitzki, Ch.; Schnürer, M.; Priebe, G.; Andreev, A. A.; Nickles, P. V.; Sandner, W.

    2014-07-21

    If regions of localized strong fields at plasma-vacuum interfaces are probed longitudinally with laser accelerated proton beams their velocity distribution changes sensitively and very fast. Its measured variations provide indirectly a higher temporal resolution as deduced from deflection geometries which rely on the explicit temporal resolution of the proton beam at the position of the object to probe. With help of reasonable models and comparative measurements changes of proton velocity can trace the field dynamics even at femtosecond time scale. In longitudinal probing, the very low longitudinal emittance together with a broad band kinetic energy distribution of laser accelerated protons is the essential prerequisite of the method. With a combination of energy and one-dimensional spatial resolution, we resolve fast field changes down to 100 fs. The used pump probe setup extends previous schemes and allows discriminating simultaneously between electric and magnetic fields in their temporal evolution.

  13. MAUI: Modeling, Analysis, and Ultrafast Imaging | Argonne National...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    interfaces. Our goal is to integrate ultrafast time-resolved imaging with large-scale molecular dynamics modeling and in situ data analysis and visualization. This will allow...

  14. Ultrafast charge localization in a stripe-phase nickelate (Journal...

    Office of Scientific and Technical Information (OSTI)

    Ultrafast excitation triggers a sub-picosecond dynamics exposing the synchronous ... Publisher: Nature Publishing Group Research Org: Ernest Orlando Lawrence Berkeley National ...

  15. Anion Solvation in Carbonate Electrolytes

    SciTech Connect (OSTI)

    Zhang, Zhengcheng

    2015-11-16

    With the correlation between Li+ solvation and interphasial chemistry on anodes firmly established in Li-ion batteries, the effect of cation–solvent interaction has gone beyond bulk thermodynamic and transport properties and become an essential element that determines the reversibility of electrochemistry and kinetics of Li-ion intercalation chemistries. As of now, most studies are dedicated to the solvation of Li+, and the solvation of anions in carbonate-based electrolytes and its possible effect on the electrochemical stability of such electrolytes remains little understood. As a mirror effort to prior Li+ solvation studies, this work focuses on the interactions between carbonate-based solvents and two anions (hexafluorophosphate, PF6–, and tetrafluoroborate, BF4–) that are most frequently used in Li-ion batteries. The possible correlation between such interaction and the interphasial chemistry on cathode surface is also explored.

  16. Ultrafast Laser Facility | Photosynthetic Antenna Research Center

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Laser Facility Ultrafast Laser Facility Click for an Overview of the Ultrafast Laser Facility The PARC Ultrafast Laser Facility, under the direction of Associate Director ...

  17. Ultrafast carrier dynamics in the large-magnetoresistance material WTe2

    SciTech Connect (OSTI)

    Dai, Y. M.; Bowlan, J.; Li, H.; Miao, H.; Wu, S. F.; Kong, W. D.; Shi, Y. G.; Trugman, S. A.; Zhu, J. -X.; Ding, H.; Taylor, A. J.; Yarotski, D. A.; Prasankumar, R. P.

    2015-10-07

    In this study, ultrafast optical pump-probe spectroscopy is used to track carrier dynamics in the large-magnetoresistance material WTe2. Our experiments reveal a fast relaxation process occurring on a subpicosecond time scale that is caused by electron-phonon thermalization, allowing us to extract the electron-phonon coupling constant. An additional slower relaxation process, occurring on a time scale of ~5–15 ps, is attributed to phonon-assisted electron-hole recombination. As the temperature decreases from 300 K, the time scale governing this process increases due to the reduction of the phonon population. However, below ~50 K, an unusual decrease of the recombination time sets in, most likely due to a change in the electronic structure that has been linked to the large magnetoresistance observed in this material.

  18. Effect of carrier recombination on ultrafast carrier dynamics in thin films of the topological insulator Bi{sub 2}Se{sub 3}

    SciTech Connect (OSTI)

    Glinka, Yuri D.; Babakiray, Sercan; Johnson, Trent A.; Holcomb, Mikel B.; Lederman, David

    2014-10-27

    Transient reflectivity (TR) from thin films (6–40 nm thick) of the topological insulator Bi{sub 2}Se{sub 3} revealed ultrafast carrier dynamics, which suggest the existence of both radiative and non-radiative recombination between electrons residing in the upper cone of initially unoccupied high energy Dirac surface states (SS) and holes residing in the lower cone of occupied low energy Dirac SS. The modeling of measured TR traces allowed us to conclude that recombination is induced by the depletion of bulk electrons in films below ∼20 nm thick due to the charge captured on the surface defects. We predict that such recombination processes can be observed using time-resolved photoluminescence techniques.

  19. 2D heterodyne-detected sum frequency generation study on the ultrafast vibrational dynamics of H{sub 2}O and HOD water at charged interfaces

    SciTech Connect (OSTI)

    Inoue, Ken-ichi; Singh, Prashant C.; Nihonyanagi, Satoshi; Tahara, Tahei; Yamaguchi, Shoichi

    2015-06-07

    Two-dimensional heterodyne-detected vibrational sum-frequency generation (2D HD-VSFG) spectroscopy is applied to study the ultrafast vibrational dynamics of water at positively charged aqueous interfaces, and 2D HD-VSFG spectra of cetyltrimethylammonium bromide (CTAB)/water interfaces in the whole hydrogen-bonded OH stretch region (3000 cm{sup ?1} ? ?{sub pump} ? 3600 cm{sup ?1}) are measured. 2D HD-VSFG spectrum of the CTAB/isotopically diluted water (HOD-D{sub 2}O) interface exhibits a diagonally elongated bleaching lobe immediately after excitation, which becomes round with a time constant of ?0.3 ps due to spectral diffusion. In contrast, 2D HD-VSFG spectrum of the CTAB/H{sub 2}O interface at 0.0 ps clearly shows two diagonal peaks and their cross peaks in the bleaching region, corresponding to the double peaks observed at 3230 cm{sup ?1} and 3420 cm{sup ?1} in the steady-state HD-VSFG spectrum. Horizontal slices of the 2D spectrum show that the relative intensity of the two peaks of the bleaching at the CTAB/H{sub 2}O interface gradually change with the change of the pump frequency. We simulate the pump-frequency dependence of the bleaching feature using a model that takes account of the Fermi resonance and inhomogeneity of the OH stretch vibration, and the simulated spectra reproduce the essential features of the 2D HD-VSFG spectra of the CTAB/H{sub 2}O interface. The present study demonstrates that heterodyne detection of the time-resolved VSFG is critically important for studying the ultrafast dynamics of water interfaces and for unveiling the underlying mechanism.

  20. Preparation of cerium halide solvate complexes

    DOE Patents [OSTI]

    Vasudevan, Kalyan V; Smith, Nickolaus A; Gordon, John C; McKigney, Edward A; Muenchaussen, Ross E

    2013-08-06

    Crystals of a solvated cerium(III) halide solvate complex resulted from a process of forming a paste of a cerium(III) halide in an ionic liquid, adding a solvent to the paste, removing any undissolved solid, and then cooling the liquid phase. Diffusing a solvent vapor into the liquid phase also resulted in crystals of a solvated cerium(III) halide complex.

  1. Structure, solvation, and dynamics of Mg{sup 2+}, Ca{sup 2+}, Sr{sup 2+}, and Ba{sup 2+} complexes with 3-hydroxyflavone and perchlorate anion in acetonitrile medium: A molecular dynamics simulation study

    SciTech Connect (OSTI)

    Agieienko, Vira N.; Kolesnik, Yaroslav V.; Kalugin, Oleg N.

    2014-05-21

    Molecular dynamics simulations of complexes of Mg{sup 2+}, Ca{sup 2+}, Sr{sup 2+}, and Ba{sup 2+} with 3-hydroxyflavone (flavonol, 3HF) and ClO {sub 4}{sup ?} in acetonitrile were performed. The united atoms force field model was proposed for the 3HF molecule using the results of DFT quantum chemical calculations. 3HF was interpreted as a rigid molecule with two internal degrees of freedom, i.e., rotation of the phenyl ring and of the OH group with respect to the chromone moiety. The interatomic radial distribution functions showed that interaction of the cations with flavonol occurs via the carbonyl group of 3HF and it is accompanied with substitution of one of the acetonitrile molecules in the cations first solvation shells. Formation of the cation3HF complexes does not have significant impact on the rotation of the phenyl ring with respect to the chromone moiety. However, the orientation of the flavonol's OH-group is more sensitive to the interaction with doubly charged cations. When complex with Mg{sup 2+} is formed, the OH-group turns out of the plane of the chromone moiety that leads to rupture of intramolecular H-bond in the ligand molecule. Complexation of Ca{sup 2+}, Sr{sup 2+}, and BaClO {sub 4}{sup +} with 3HF produces two structures with different OH-positions, as in the free flavonol with the intramolecular H-bond and as in the complex with Mg{sup 2+} with disrupted H-bonding. It was shown that additional stabilization of the [MgClO{sub 4}(3HF)]{sup +} and [BaClO{sub 4}(3HF)]{sup +} complexes is determined by strong affinity of perchlorate anion to interact with flavonol via intracomplex hydrogen bond between an oxygen atom of the anion and the hydrogen atom of the 3-hydroxyl group. Noticeable difference in the values of the self-diffusion coefficients for Kt{sup 2+} from one side and ClO {sub 4}{sup ?}, 3HF, and AN in the cations coordination shell from another side implies quite weak interaction between cation, anion, and ligands in the

  2. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Transformations in Superionic Nanocrystals Print A superionic material is a multi-component solid with simultaneous characteristics of both a solid and a liquid. Above a critical temperature associated with a structural phase transition, one of the atomic species in the material will exhibit liquid-like ionic conductivity and dynamic disorder within the rigid crystalline structure of the other. Discovered by Michael Faraday almost 200 years ago, superionic materials today hold promise

  3. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Transformations in Superionic Nanocrystals Print A superionic material is a multi-component solid with simultaneous characteristics of both a solid and a liquid. Above a critical temperature associated with a structural phase transition, one of the atomic species in the material will exhibit liquid-like ionic conductivity and dynamic disorder within the rigid crystalline structure of the other. Discovered by Michael Faraday almost 200 years ago, superionic materials today hold promise

  4. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Transformations in Superionic Nanocrystals Print A superionic material is a multi-component solid with simultaneous characteristics of both a solid and a liquid. Above a critical temperature associated with a structural phase transition, one of the atomic species in the material will exhibit liquid-like ionic conductivity and dynamic disorder within the rigid crystalline structure of the other. Discovered by Michael Faraday almost 200 years ago, superionic materials today hold promise

  5. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Transformations in Superionic Nanocrystals Print A superionic material is a multi-component solid with simultaneous characteristics of both a solid and a liquid. Above a critical temperature associated with a structural phase transition, one of the atomic species in the material will exhibit liquid-like ionic conductivity and dynamic disorder within the rigid crystalline structure of the other. Discovered by Michael Faraday almost 200 years ago, superionic materials today hold promise

  6. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Transformations in Superionic Nanocrystals Print A superionic material is a multi-component solid with simultaneous characteristics of both a solid and a liquid. Above a critical temperature associated with a structural phase transition, one of the atomic species in the material will exhibit liquid-like ionic conductivity and dynamic disorder within the rigid crystalline structure of the other. Discovered by Michael Faraday almost 200 years ago, superionic materials today hold promise

  7. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Transformations in Superionic Nanocrystals Print A superionic material is a multi-component solid with simultaneous characteristics of both a solid and a liquid. Above a critical temperature associated with a structural phase transition, one of the atomic species in the material will exhibit liquid-like ionic conductivity and dynamic disorder within the rigid crystalline structure of the other. Discovered by Michael Faraday almost 200 years ago, superionic materials today hold promise

  8. Indirect excitation of ultrafast demagnetization

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Vodungbo, Boris; Tudu, Bahrati; Perron, Jonathan; Delaunay, Renaud; Müller, Leonard; Berntsen, Magnus H.; Grübel, Gerhard; Malinowski, Grégory; Weier, Christian; Gautier, Julien; et al

    2016-01-06

    Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset andmore » at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. As a result, our data thus confirm recent theoretical predictions.« less

  9. Excited state carrier dynamics in CdS{sub x}Se{sub 1-x} semisconductor alloys as studied by ultrafast fluorescence spectroscopy

    SciTech Connect (OSTI)

    Gadd, S.E.

    1995-08-01

    This dissertation discusses studies of the electron-hole pair dynamics of CdS{sub x}Se{sub 1-x} semiconductor alloys for the entire compositional range from x = 1 to x = 0 as examined by the ultrafast fluorescence techniques of time correlated single photon counting and fluorescence upconversion. Specifically, samples with x = 1, .75, .5, .25, and 0 were studied each at a spread of wavelengths about its respective emission maximum which varies according to {lambda} = 718nm - 210x nm. The decays of these samples were found to obey a Kohlrausch distribution, exp [(t/{tau}){sup {beta}}], with the exponent 3 in the range .5-.7 for the alloys. These results are in agreement with those expected for localization due to local potential variations resulting from the random distribution of sulfur and selenium atoms on the element VI A sub-lattice. This localization can be understood in terms of Anderson localization of the holes in states whose energy distribution tails into the forbidden energy band-gap. Because these states have energy dependent lifetimes, the carriers can decay via many parallel channels. This distribution of channels is the ultimate source of the Kohlrausch form of the fluorescence decays.

  10. Ultrafast dynamics of strong-field dissociative ionization ofCH2Br2 probed by femtosecond soft x-ray transient absorptionspectroscopy

    SciTech Connect (OSTI)

    Loh, Zhi-Heng; Leone, Stephen R.

    2008-01-15

    Femtosecond time-resolved soft x-ray transient absorption spectroscopy based on a high-order harmonic generation source is used to investigate the dissociative ionization of CH{sub 2}Br{sub 2} induced by 800 nm strong-field irradiation. At moderate peak intensities (2.0 x 10{sup 14} W/cm{sup 2}), strong-field ionization is accompanied by ultrafast C-Br bond dissociation, producing both neutral Br ({sup 2}P{sub 3/2}) and Br* ({sup 2}P{sub 1/2}) atoms together with the CH{sub 2}Br{sup +} fragment ion. The measured rise times for Br and Br* are 130 {+-} 22 fs and 74 {+-} 10 fs, respectively. The atomic bromine quantum state distribution shows that the Br/Br* population ratio is 8.1 {+-} 3.8 and that the Br {sup 2}P{sub 3/2} state is not aligned. The observed product distribution and the timescales of the photofragment appearances suggest that multiple field-dressed potential energy surfaces are involved in the dissociative ionization process. In addition, the transient absorption spectrum of CH{sub 2}Br{sub 2}{sup +} suggests that the alignment of the molecule relative to the polarization axis of the strong-field ionizing pulse determines the electronic symmetry of the resulting ion; alignment of the Br-Br, H-H, and C{sub 2} axis of the molecule along the polarization axis results in the production of the ion {tilde X}({sup 2}B{sub 2}), {tilde B}({sup 2}B{sub 1}) and {tilde C}({sup 2}A{sub 1}) states, respectively. At higher peak intensities (6.2 x 10{sup 14} W/cm{sup 2}), CH{sub 2}Br{sub 2}{sup +} undergoes sequential ionization to form the metastable CH{sub 2}Br{sub 2}{sup 2+} dication. These results demonstrate the potential of core-level probing with high-order harmonic transient absorption spectroscopy for studying ultrafast molecular dynamics.

  11. Solvation Structure and Transport Properties of Alkali Cations in Dimethyl

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Sulfoxide Under Exogenous Static Electric Fields - Joint Center for Energy Storage Research June 14, 2015, Research Highlights Solvation Structure and Transport Properties of Alkali Cations in Dimethyl Sulfoxide Under Exogenous Static Electric Fields Top: Snapshots of molecular dynamics simulations of alkali ions in DMSO at 298 K and zero-applied electric field: (left) Li+ and (right) Cs+. Sulfur atoms are shown in yellow, oxygen atoms in red, and methyl groups in gray. Graph: Average

  12. Ultrafast Laser Facility - Virtual Tour | Photosynthetic Antenna...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Laser Facility - Virtual Tour December 10, 2015 Ultrafast Laser Facility - Virtual Tour A look at the technology and science in the Ultrafast lab PARC Research Scientist ...

  13. Dynamics-based selective 2D {sup 1}H/{sup 1}H chemical shift correlation spectroscopy under ultrafast MAS conditions

    SciTech Connect (OSTI)

    Zhang, Rongchun; Ramamoorthy, Ayyalusamy

    2015-05-28

    Dynamics plays important roles in determining the physical, chemical, and functional properties of a variety of chemical and biological materials. However, a material (such as a polymer) generally has mobile and rigid regions in order to have high strength and toughness at the same time. Therefore, it is difficult to measure the role of mobile phase without being affected by the rigid components. Herein, we propose a highly sensitive solid-state NMR approach that utilizes a dipolar-coupling based filter (composed of 12 equally spaced 90° RF pulses) to selectively measure the correlation of {sup 1}H chemical shifts from the mobile regions of a material. It is interesting to find that the rotor-synchronized dipolar filter strength decreases with increasing inter-pulse delay between the 90° pulses, whereas the dipolar filter strength increases with increasing inter-pulse delay under static conditions. In this study, we also demonstrate the unique advantages of proton-detection under ultrafast magic-angle-spinning conditions to enhance the spectral resolution and sensitivity for studies on small molecules as well as multi-phase polymers. Our results further demonstrate the use of finite-pulse radio-frequency driven recoupling pulse sequence to efficiently recouple weak proton-proton dipolar couplings in the dynamic regions of a molecule and to facilitate the fast acquisition of {sup 1}H/{sup 1}H correlation spectrum compared to the traditional 2D NOESY (Nuclear Overhauser effect spectroscopy) experiment. We believe that the proposed approach is beneficial to study mobile components in multi-phase systems, such as block copolymers, polymer blends, nanocomposites, heterogeneous amyloid mixture of oligomers and fibers, and other materials.

  14. Final Progress Report for Linking Ion Solvation and Lithium Battery

    Office of Scientific and Technical Information (OSTI)

    for Linking Ion Solvation and Lithium Battery Electrolyte Properties Henderson, Wesley 25 ENERGY STORAGE battery, electrolyte, solvation, ionic association battery, electrolyte,...

  15. New Polymer Architectures for Imidazole Solvating groups, Anion...

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Polymer Architectures for Imidazole Solvating groups, Anion Mobility and Flexibility New Polymer Architectures for Imidazole Solvating groups, Anion Mobility and Flexibility ...

  16. Ultrafast Photovoltaic Response in Ferroelectric Nanolayers ...

    Office of Scientific and Technical Information (OSTI)

    Ultrafast Photovoltaic Response in Ferroelectric Nanolayers Citation Details In-Document Search Title: Ultrafast Photovoltaic Response in Ferroelectric Nanolayers Authors:...

  17. Imaging the ultrafast Kerr effect, free carrier generation, relaxation and ablation dynamics of Lithium Niobate irradiated with femtosecond laser pulses

    SciTech Connect (OSTI)

    Garcia-Lechuga, Mario, E-mail: mario@io.cfmac.csic.es; Siegel, Jan, E-mail: j.siegel@io.cfmac.csic.es; Hernandez-Rueda, Javier; Solis, Javier [Laser Processing Group, Instituto de Optica, CSIC, Serrano 121, 28006 Madrid (Spain)

    2014-09-21

    The interaction of high-power single 130 femtosecond (fs) laser pulses with the surface of Lithium Niobate is experimentally investigated in this work. The use of fs-resolution time-resolved microscopy allows us to separately observe the instantaneous optical Kerr effect induced by the pulse and the generation of a free electron plasma. The maximum electron density is reached 550 fs after the peak of the Kerr effect, confirming the presence of a delayed carrier generation mechanism. We have also observed the appearance of transient Newton rings during the ablation process, related to optical interference of the probe beam reflected at the front and back surface of the ablating layer. Finally, we have analyzed the dynamics of the photorefractive effect on a much longer time scale by measuring the evolution of the transmittance of the irradiated area for different fluences below the ablation threshold.

  18. Solvate Structures and Computational/Spectroscopic Characterization...

    Office of Scientific and Technical Information (OSTI)

    The present study characterizes the PF6- anion P-F Raman symmetric stretching vibrational band for evaluating the PF6-...Li+ cation interactions within LiPF6 crystalline solvates ...

  19. Electronic Coupling Dependence of Ultrafast Interfacial Electron Transfer

    Office of Scientific and Technical Information (OSTI)

    on Nanocrystalline Thin Films and Single Crystal (Technical Report) | SciTech Connect Electronic Coupling Dependence of Ultrafast Interfacial Electron Transfer on Nanocrystalline Thin Films and Single Crystal Citation Details In-Document Search Title: Electronic Coupling Dependence of Ultrafast Interfacial Electron Transfer on Nanocrystalline Thin Films and Single Crystal The long-term goal of the proposed research is to understand electron transfer dynamics in nanoparticle/liquid interface.

  20. Solvation structure and transport properties of alkali cations in dimethyl sulfoxide under exogenous static electric fields

    SciTech Connect (OSTI)

    Kerisit, Sebastien; Vijayakumar, M. E-mail: karl.mueller@pnnl.gov; Han, Kee Sung; Mueller, Karl T. E-mail: karl.mueller@pnnl.gov

    2015-06-14

    A combination of molecular dynamics simulations and pulsed field gradient nuclear magnetic resonance spectroscopy is used to investigate the role of exogenous electric fields on the solvation structure and dynamics of alkali ions in dimethyl sulfoxide (DMSO) and as a function of temperature. Good agreement was obtained, for select alkali ions in the absence of an electric field, between calculated and experimentally determined diffusion coefficients normalized to that of pure DMSO. Our results indicate that temperatures of up to 400 K and external electric fields of up to 1 V nm{sup −1} have minimal effects on the solvation structure of the smaller alkali cations (Li{sup +} and Na{sup +}) due to their relatively strong ion-solvent interactions, whereas the solvation structures of the larger alkali cations (K{sup +}, Rb{sup +}, and Cs{sup +}) are significantly affected. In addition, although the DMSO exchange dynamics in the first solvation shell differ markedly for the two groups, the drift velocities and mobilities are not significantly affected by the nature of the alkali ion. Overall, although exogenous electric fields induce a drift displacement, their presence does not significantly affect the random diffusive displacement of the alkali ions in DMSO. System temperature is found to have generally a stronger influence on dynamical properties, such as the DMSO exchange dynamics and the ion mobilities, than the presence of electric fields.

  1. Reactions of Solvated Ions Final Report

    DOE R&D Accomplishments [OSTI]

    Taube, H.

    1962-09-24

    Brief summaries are presented on isotopic dilution studies on salts dissolved in CH{sub 3}OH, studies on metal and metal salts in solvents of the amine type, and studies on phosphato complexes of the pentammine Co(III) series. A list of papers published on reactions of solvated ions is included. (N.W.R.)

  2. Solvation and Reaction in Ionic Liquids

    SciTech Connect (OSTI)

    Maroncelli, Mark

    2015-01-15

    The long-range goal of our DOE-sponsored research is to obtain a fundamental understanding of solvation effects on photo-induced charge transfer and related processes. Much of the focus during the past funding period has been on studies of ionic liquids and on characterizing various reactions with which to probe the nature of this interesting new solvent medium.

  3. The Solvation Structure of Mg Ions in Dichloro Complex Solutions from

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    First-Principles Molecular Dynamics and Simulated X-ray Absorption Spectra - Joint Center for Energy Storage Research September 22, 2014, Research Highlights The Solvation Structure of Mg Ions in Dichloro Complex Solutions from First-Principles Molecular Dynamics and Simulated X-ray Absorption Spectra The coordination of a Mg-ion dimer complex extracted from solution phase simulations at room temperature indicating 4- and 5-fold coordination of Mg ions (orange) by Cl counterions (green) and

  4. Navigating Space-Time with Ultrafast Exciton Photolithography or

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Scintillating Near-fields to Follow Dynamic Processes in Molecular Materials | MIT-Harvard Center for Excitonics Navigating Space-Time with Ultrafast Exciton Photolithography or Scintillating Near-fields to Follow Dynamic Processes in Molecular Materials May 5, 2015 at 4:30pm/ rm: 4-370 Naomi Ginsberg University of California/Department of Chemistry and Physics nsginsberg abstract: A cross-cutting theme in my research group is to examine dynamic processes in spatially-heterogeneous condensed

  5. Quasiparticle dynamics across the full Brillouin zone of Bi2Sr2CaCu2O8+δ traced with ultrafast time and angle-resolved photoemission spectroscopy

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Dakovski, Georgi L.; Durakiewicz, Tomasz; Zhu, Jian-Xin; Riseborough, Peter S.; Gu, Genda; Gilbertson, Steve M.; Taylor, Antoinette; Rodriguez, George

    2015-10-12

    A hallmark in the cuprate family of high-temperature superconductors is the nodal-antinodal dichotomy. In this regard, angle-resolved photoemission spectroscopy (ARPES) has proven especially powerful, providing band structure information directly in energy-momentum space. Time-resolved ARPES (trARPES) holds great promise of adding ultrafast temporal information, in an attempt to identify different interaction channels in the time domain. Previous studies of the cuprates using trARPES were handicapped by the low probing energy which significantly limits the accessible momentum space. Using 20.15eV, 12 fs pulses we show for the first time the evolution of quasiparticles in the antinodal region of Bi2Sr2CaCu2O8+δ and demonstrate thatmore » nonmonotonic relaxation dynamics dominates above a certain fluence threshold. The dynamics is heavily influenced by transient modification of the electron-phonon interaction and phase space restrictions, in severe contrast to the monotonic relaxation in the nodal and off-nodal regions.« less

  6. Quasiparticle dynamics across the full Brillouin zone of Bi2Sr2CaCu2O8+δ traced with ultrafast time and angle-resolved photoemission spectroscopy

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Dakovski, Georgi L.; Durakiewicz, Tomasz; Zhu, Jian-Xin; Riseborough, Peter S.; Gu, Genda; Gilbertson, Steve M.; Taylor, Antoinette; Rodriguez, George

    2015-10-12

    A hallmark in the cuprate family of high-temperature superconductors is the nodal-antinodal dichotomy. In this regard, angle-resolved photoemission spectroscopy (ARPES) has proven especially powerful, providing band structure information directly in energy-momentum space. Time-resolved ARPES (trARPES) holds great promise of adding ultrafast temporal information, in an attempt to identify different interaction channels in the time domain. Previous studies of the cuprates using trARPES were handicapped by the low probing energy which significantly limits the accessible momentum space. Using 20.15eV, 12 fs pulses we show for the first time the evolution of quasiparticles in the antinodal region of Bi2Sr2CaCu2O8+δ and demonstrate thatmore »nonmonotonic relaxation dynamics dominates above a certain fluence threshold. The dynamics is heavily influenced by transient modification of the electron-phonon interaction and phase space restrictions, in severe contrast to the monotonic relaxation in the nodal and off-nodal regions.« less

  7. Sparingly Solvating Electrolytes for High Energy Density Lithium-Sulfur

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Batteries - Joint Center for Energy Storage Research July 11, 2016, Research Highlights Sparingly Solvating Electrolytes for High Energy Density Lithium-Sulfur Batteries Precipitation-dissolution Li-S chemistry achieved by sparingly solvating electrolyte and various electrolyte design concepts Scientific Achievement This work presents the promising new concepts of using sparingly solvating electrolyte to enable Li-S battery operation at lean electrolyte condition, as well as the design rules

  8. Final Progress Report for Linking Ion Solvation and Lithium Battery

    Office of Scientific and Technical Information (OSTI)

    Electrolyte Properties (Technical Report) | SciTech Connect Progress Report for Linking Ion Solvation and Lithium Battery Electrolyte Properties Citation Details In-Document Search Title: Final Progress Report for Linking Ion Solvation and Lithium Battery Electrolyte Properties The research objective of this proposal was to provide a detailed analysis of how solvent and anion structure govern the solvation state of Li+ cations in solvent-LiX mixtures and how this, in turn, dictates the

  9. Femtosecond laser studies of ultrafast intramolecular processes

    SciTech Connect (OSTI)

    Hayden, C.

    1993-12-01

    The goal of this research is to better understand the detailed mechanisms of chemical reactions by observing, directly in time, the dynamics of fundamental chemical processes. In this work femtosecond laser pulses are used to initiate chemical processes and follow the progress of these processes in time. The authors are currently studying ultrafast internal conversion and subsequent intramolecular relaxation in unsaturated hydrocarbons. In addition, the authors are developing nonlinear optical techniques to prepare and monitor the time evolution of specific vibrational motions in ground electronic state molecules.

  10. Lithium Ion Solvation and Intercalation at Anode-Electrolyte...

    Office of Scientific and Technical Information (OSTI)

    Interface from First Principles Citation Details In-Document Search Title: Lithium Ion Solvation and Intercalation at Anode-Electrolyte Interface from First ...

  11. Lithium Ion Solvation and Intercalation at Anode-Electrolyte...

    Office of Scientific and Technical Information (OSTI)

    Title: Lithium Ion Solvation and Intercalation at Anode-Electrolyte Interface from First Principles Authors: Ong, M T ; Lordi, V ; Draeger, E W ; Pask, J E Publication Date: ...

  12. Ultrafast Probes for Dirac Materials Yarotski, Dmitry Anatolievitch...

    Office of Scientific and Technical Information (OSTI)

    Science(36) Material Science; topological insulators, ultrafast spectroscopy, graphene Material Science; topological insulators, ultrafast spectroscopy, graphene Abstract...

  13. Competitive lithium solvation of linear and cyclic carbonates from quantum chemistry

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Kent, Paul R. C.; Ganesh, Panchapakesan; Borodin, Oleg; Olguin, Marco; Allen, Joshua L.; Henderson, Wesley A.

    2015-11-17

    The composition of the lithium cation (Li+) solvation shell in mixed linear and cyclic carbonate-based electrolytes has been re-examined using Born–Oppenheimer molecular dynamics (BOMD) as a function of salt concentration and cluster calculations with ethylene carbonate:dimethyl carbonate (EC:DMC)–LiPF6 as a model system. A coordination preference for EC over DMC to a Li+ was found at low salt concentrations, while a slightly higher preference for DMC over EC was found at high salt concentrations. Analysis of the relative binding energies of the (EC)n(DMC)m–Li+ and (EC)n(DMC)m–LiPF6 solvates in the gas-phase and for an implicit solvent (as a function of the solvent dielectricmore » constant) indicated that the DMC-containing Li+ solvates were stabilized relative to (EC4)–Li+ and (EC)3–LiPF6 by immersing them in the implicit solvent. Such stabilization was more pronounced in the implicit solvents with a high dielectric constant. Results from previous Raman and IR experiments were reanalyzed and reconciled by correcting them for changes of the Raman activities, IR intensities and band shifts for the solvents which occur upon Li+ coordination. After these correction factors were applied to the results of BOMD simulations, the composition of the Li+ solvation shell from the BOMD simulations was found to agree well with the solvation numbers extracted from Raman experiments. Finally, the mechanism of the Li+ diffusion in the dilute (EC:DMC)LiPF6 mixed solvent electrolyte was studied using the BOMD simulations.« less

  14. Competitive lithium solvation of linear and cyclic carbonates from quantum chemistry

    SciTech Connect (OSTI)

    Kent, Paul R. C.; Ganesh, Panchapakesan; Borodin, Oleg; Olguin, Marco; Allen, Joshua L.; Henderson, Wesley A.

    2015-11-17

    The composition of the lithium cation (Li+) solvation shell in mixed linear and cyclic carbonate-based electrolytes has been re-examined using Born–Oppenheimer molecular dynamics (BOMD) as a function of salt concentration and cluster calculations with ethylene carbonate:dimethyl carbonate (EC:DMC)–LiPF6 as a model system. A coordination preference for EC over DMC to a Li+ was found at low salt concentrations, while a slightly higher preference for DMC over EC was found at high salt concentrations. Analysis of the relative binding energies of the (EC)n(DMC)m–Li+ and (EC)n(DMC)m–LiPF6 solvates in the gas-phase and for an implicit solvent (as a function of the solvent dielectric constant) indicated that the DMC-containing Li+ solvates were stabilized relative to (EC4)–Li+ and (EC)3–LiPF6 by immersing them in the implicit solvent. Such stabilization was more pronounced in the implicit solvents with a high dielectric constant. Results from previous Raman and IR experiments were reanalyzed and reconciled by correcting them for changes of the Raman activities, IR intensities and band shifts for the solvents which occur upon Li+ coordination. After these correction factors were applied to the results of BOMD simulations, the composition of the Li+ solvation shell from the BOMD simulations was found to agree well with the solvation numbers extracted from Raman experiments. Finally, the mechanism of the Li+ diffusion in the dilute (EC:DMC)LiPF6 mixed solvent electrolyte was studied using the BOMD simulations.

  15. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Researchers have recently carried out a range of ultrafast x-ray spectroscopy and scattering experiments at three x-ray light sources, including the ALS, to obtain an atomic-level, ...

  16. Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory

    SciTech Connect (OSTI)

    Weathersby, S. P.; Brown, G.; Centurion, M.; Chase, T. F.; Coffee, R.; Corbett, J.; Eichner, J. P.; Frisch, J. C.; Fry, A. R.; Gühr, M.; Hartmann, N.; Hast, C.; Hettel, R.; Jobe, R. K.; Jongewaard, E. N.; Lewandowski, J. R.; Li, R. K.; Lindenberg, A. M.; Makasyuk, I.; May, J. E.; McCormick, D.; Nguyen, M. N.; Reid, A. H.; Shen, X.; Sokolowski-Tinten, K.; Vecchione, T.; Vetter, S. L.; Wu, J.; Yang, J.; Dürr, H. A.; Wang, X. J.

    2015-07-01

    Ultrafast electron probes are powerful tools, complementary to x-ray free-electron lasers, used to study structural dynamics in material, chemical, and biological sciences. High brightness, relativistic electron beams with femtosecond pulse duration can resolve details of the dynamic processes on atomic time and length scales. SLAC National Accelerator Laboratory recently launched the Ultrafast Electron Diffraction (UED) and microscopy Initiative aiming at developing the next generation ultrafast electron scattering instruments. As the first stage of the Initiative, a mega-electron-volt (MeV) UED system has been constructed and commissioned to serve ultrafast science experiments and instrumentation development. The system operates at 120-Hz repetition rate with outstanding performance. In this paper, we report on the SLAC MeV UED system and its performance, including the reciprocal space resolution, temporal resolution, and machine stability.

  17. Electrolyte Solvation and Ionic Association. VI. Acetonitrile-Lithium Salt Mixtures. Highly Associated Salts Revisited

    SciTech Connect (OSTI)

    Borodin, Oleg; Han, Sang D.; Daubert, James S.; Seo, D. M.; Yun, Sung-Hyun; Henderson, Wesley A.

    2015-01-14

    Molecular dynamics (MD) simulations of acetonitrile (AN) mixtures with LiBF4, LiCF3SO3 and LiCF3CO2 provide extensive details about the molecular- and mesoscale-level solution interactions and thus explanations as to why these electrolytes have very different thermal phase behavior and electrochemical/physicochemical properties. The simulation results are in full accord with a previous experimental study of these (AN)n-LiX electrolytes. This computational study reveals how the structure of the anions strongly influences the ionic association tendency of the ions, the manner in which the aggregate solvates assemble in solution and the length of time in which the anions remain coordinated to the Li+ cations in the solvates which result in dramatic variations in the transport properties of the electrolytes.

  18. Ultrafast Spectroscopy of Midinfrared Internal Exciton Transitions...

    Office of Scientific and Technical Information (OSTI)

    Journal Article: Ultrafast Spectroscopy of Midinfrared ... Carbon Nanotubes Citation Details In-Document ... Carbon Nanotubes We report a femtosecond midinfrared ...

  19. Ultrafast scanning probe microscopy

    DOE Patents [OSTI]

    Weiss, S.; Chemla, D.S.; Ogletree, D.F.; Botkin, D.

    1995-05-16

    An ultrafast scanning probe microscopy method is described for achieving subpicosecond-temporal resolution and submicron-spatial resolution of an observation sample. In one embodiment of the present claimed invention, a single short optical pulse is generated and is split into first and second pulses. One of the pulses is delayed using variable time delay means. The first pulse is then directed at an observation sample located proximate to the probe of a scanning probe microscope. The scanning probe microscope produces probe-sample signals indicative of the response of the probe to characteristics of the sample. The second pulse is used to modulate the probe of the scanning probe microscope. The time delay between the first and second pulses is then varied. The probe-sample response signal is recorded at each of the various time delays created between the first and second pulses. The probe-sample response signal is then plotted as a function of time delay to produce a cross-correlation of the probe sample response. In so doing, the present invention provides simultaneous subpicosecond-temporal resolution and submicron-spatial resolution of the sample. 6 Figs.

  20. Ultrafast scanning probe microscopy

    DOE Patents [OSTI]

    Weiss, Shimon; Chemla, Daniel S.; Ogletree, D. Frank; Botkin, David

    1995-01-01

    An ultrafast scanning probe microscopy method for achieving subpicosecond-temporal resolution and submicron-spatial resolution of an observation sample. In one embodiment of the present claimed invention, a single short optical pulse is generated and is split into first and second pulses. One of the pulses is delayed using variable time delay means. The first pulse is then directed at an observation sample located proximate to the probe of a scanning probe microscope. The scanning probe microscope produces probe-sample signals indicative of the response of the probe to characteristics of the sample. The second pulse is used to modulate the probe of the scanning probe microscope. The time delay between the first and second pulses is then varied. The probe-sample response signal is recorded at each of the various time delays created between the first and second pulses. The probe-sample response signal is then plotted as a function of time delay to produce a cross-correlation of the probe sample response. In so doing, the present invention provides simultaneous subpicosecond-temporal resolution and submicron-spatial resolution of the sample.

  1. Ultrafast X-Ray Coherent Control

    SciTech Connect (OSTI)

    Reis, David

    2009-05-01

    This main purpose of this grant was to develop the nascent #12;eld of ultrafast x-ray science using accelerator-based sources, and originally developed from an idea that a laser could modulate the di#11;racting properties of a x-ray di#11;racting crystal on a fast enough time scale to switch out in time a shorter slice from the already short x-ray pulses from a synchrotron. The research was carried out primarily at the Advanced Photon Source (APS) sector 7 at Argonne National Laboratory and the Sub-Picosecond Pulse Source (SPPS) at SLAC; in anticipation of the Linac Coherent Light Source (LCLS) x-ray free electron laser that became operational in 2009 at SLAC (all National User Facilities operated by BES). The research centered on the generation, control and measurement of atomic-scale dynamics in atomic, molecular optical and condensed matter systems with temporal and spatial resolution . It helped develop the ultrafast physics, techniques and scienti#12;c case for using the unprecedented characteristics of the LCLS. The project has been very successful with results have been disseminated widely and in top journals, have been well cited in the #12;eld, and have laid the foundation for many experiments being performed on the LCLS, the world's #12;rst hard x-ray free electron laser.

  2. Ultrafast free-carrier dynamics in Cu{sub 2}ZnSnS{sub 4} single crystals studied using femtosecond time-resolved optical spectroscopy

    SciTech Connect (OSTI)

    Phuong, L. Q.; Kanemitsu, Y.; Okano, M.; Yamada, Y.; Yamashita, G.; Morimoto, T.; Nagai, M.; Ashida, M.; Nagaoka, A.; Yoshino, K.

    2014-12-08

    We studied the dynamics of photogenerated carriers in Cu{sub 2}ZnSnS{sub 4} (CZTS) single crystals using femtosecond transient reflectivity (TR) and optical pump-THz probe transient absorption (THz-TA) spectroscopy. The TR and THz-TA decay dynamics consistently showed that free carriers have long lifetimes of up to a few nanoseconds. The excitation-photon-energy-dependent TR measurements revealed a slow picosecond energy relaxation of free carriers to the band edge in CZTS. The relaxation and recombination dynamics of free carriers were affected by nonradiative recombinations at the surface. Our results revealed a global feature of energy relaxation and recombination processes of free carriers in CZTS single crystals.

  3. A spectroelectrochemical cell for ultrafast two-dimensional infrared spectroscopy

    SciTech Connect (OSTI)

    El Khoury, Youssef; Van Wilderen, Luuk J. G. W.; Vogt, Tim; Winter, Ernst; Bredenbeck, Jens E-mail: bredenbeck@biophysik.uni-frankfurt.de

    2015-08-15

    A spectroelectrochemical cell has been designed to combine electrochemistry and ultrafast two-dimensional infrared (2D-IR) spectroscopy, which is a powerful tool to extract structure and dynamics information on the femtosecond to picosecond time scale. Our design is based on a gold mirror with the dual role of performing electrochemistry and reflecting IR light. To provide the high optical surface quality required for laser spectroscopy, the gold surface is made by electron beam evaporation on a glass substrate. Electrochemical cycling facilitates in situ collection of ultrafast dynamics of redox-active molecules by means of 2D-IR. The IR beams are operated in reflection mode so that they travel twice through the sample, i.e., the signal size is doubled. This methodology is optimal for small sample volumes and successfully tested with the ferricyanide/ferrocyanide redox system of which the corresponding electrochemically induced 2D-IR difference spectrum is reported.

  4. Structural Interactions within Lithium Salt Solvates: Acyclic Carbonates and Esters

    SciTech Connect (OSTI)

    Afroz, Taliman; Seo, D. M.; Han, Sang D.; Boyle, Paul D.; Henderson, Wesley A.

    2015-03-06

    Solvate crystal structures serve as useful models for the molecular-level interactions within the diverse solvates present in liquid electrolytes. Although acyclic carbonate solvents are widely used for Li-ion battery electrolytes, only three solvate crystal structures with lithium salts are known for these and related solvents. The present work, therefore, reports six lithium salt solvate structures with dimethyl and diethyl carbonate: (DMC)2:LiPF6, (DMC)1:LiCF3SO3, (DMC)1/4:LiBF4, (DEC)2:LiClO4, (DEC)1:LiClO4 and (DEC)1:LiCF3SO3 and four with the structurally related methyl and ethyl acetate: (MA)2:LiClO4, (MA)1:LiBF4, (EA)1:LiClO4 and (EA)1:LiBF4.

  5. Ionic strength independence of charge distributions in solvation of biomolecules

    SciTech Connect (OSTI)

    Virtanen, J. J.; Sosnick, T. R.; Freed, K. F.

    2014-12-14

    Electrostatic forces enormously impact the structure, interactions, and function of biomolecules. We perform all-atom molecular dynamics simulations for 5 proteins and 5 RNAs to determine the dependence on ionic strength of the ion and water charge distributions surrounding the biomolecules, as well as the contributions of ions to the electrostatic free energy of interaction between the biomolecule and the surrounding salt solution (for a total of 40 different biomolecule/solvent combinations). Although water provides the dominant contribution to the charge density distribution and to the electrostatic potential even in 1M NaCl solutions, the contributions of water molecules and of ions to the total electrostatic interaction free energy with the solvated biomolecule are comparable. The electrostatic biomolecule/solvent interaction energies and the total charge distribution exhibit a remarkable insensitivity to salt concentrations over a huge range of salt concentrations (20 mM to 1M NaCl). The electrostatic potentials near the biomolecule's surface obtained from the MD simulations differ markedly, as expected, from the potentials predicted by continuum dielectric models, even though the total electrostatic interaction free energies are within 11% of each other.

  6. Solvation Properties of Microhydrated Sulfate Anion Clusters: Insights from

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    abInitio Calculations | Argonne Leadership Computing Facility Solvation Properties of Microhydrated Sulfate Anion Clusters: Insights from abInitio Calculations Authors: Wan, Q., Spanu, L., Galli, G. Sulfate-water clusters play an important role in environmental and industrial processes, yet open questions remain on their physical and chemical properties. We investigated the smallest hydrated sulfate anion clusters believed to have a full solvation shell, with 12 or 13 water molecules. We

  7. Water-enhanced solvation of organics

    SciTech Connect (OSTI)

    Lee, J.H.

    1993-07-01

    Water-enhanced solvation (WES) was explored for Lewis acid solutes in Lewis base organic solvents, to develop cheap extract regeneration processes. WES for solid solutes was determined from ratios of solubilities of solutes in water-sat. and low-water solvent; both were determined from solid-liquid equilibrium. Vapor-headspace analysis was used to determine solute activity coefficients as function of organic phase water concentration. WES magnitudes of volatile solutes were normalized, set equal to slope of log {gamma}{sub s} vs x{sub w}/x{sub s} curve. From graph shape {Delta}(log {gamma}{sub s}) represents relative change in solute activity coefficient. Solutes investigated by vapor-headspace analysis were acetic acid, propionic acid, ethanol, 1,2-propylene glycol, 2,3-butylene glycol. Monocarboxylic acids had largest decrease in activity coefficient with water addition followed by glycols and alcohols. Propionic acid in cyclohexanone showed greatest water-enhancement {Delta} (log {gamma}{sub acid})/{Delta}(x{sub w}/x{sub acid}) = {minus}0.25. In methylcyclohexanone, the decrease of the activity coefficient of propionic acid was {minus}0.19. Activity coefficient of propionic acid in methylcyclohexanone stopped decreasing once the water reached a 2:1 water to acid mole ratio, implying a stoichiometric relation between water, ketone, and acid. Except for 2,3-butanediol, activity coefficients of the solutes studied decreased monotonically with water content. Activity coefficient curves of ethanol, 1,2-propanediol and 2,3-butanediol did not level off at large water/solute mole ratio. Solutes investigated by solid-liquid equilibrium were citric acid, gallic acid, phenol, xylenols, 2-naphthol. Saturation concentration of citric acid in anhydrous butyl acetate increased from 0.0009 to 0.087 mol/L after 1.3 % (g/g) water co-dissolved into organic phase. Effect of water-enhanced solvation for citric acid is very large but very small for phenol and its derivatives.

  8. Ultrafast chirped optical waveform recorder using a time microscope...

    Office of Scientific and Technical Information (OSTI)

    DOepatents Search Results Ultrafast chirped optical waveform recorder using a time microscope Title: Ultrafast chirped optical waveform recorder using a time microscope A new ...

  9. Ultrafast chirped optical waveform recorder using a time microscope...

    Office of Scientific and Technical Information (OSTI)

    Data Explorer Search Results Ultrafast chirped optical waveform recorder using a time microscope Title: Ultrafast chirped optical waveform recorder using a time microscope A new ...

  10. Plasmas, Dielectrics and the Ultrafast: First Science and Operational...

    Office of Scientific and Technical Information (OSTI)

    Ultrafast: First Science and Operational Experience at FACET Citation Details In-Document Search Title: Plasmas, Dielectrics and the Ultrafast: First Science and Operational ...

  11. Ultrafast Laser Fabrication: a Rapid Prototyping Capability for...

    Office of Scientific and Technical Information (OSTI)

    Technical Report: Ultrafast Laser Fabrication: a Rapid Prototyping Capability for CINT Citation Details In-Document Search Title: Ultrafast Laser Fabrication: a Rapid Prototyping...

  12. Ultrafast laser diagnostics for studies of shock initiation in...

    Office of Scientific and Technical Information (OSTI)

    Ultrafast laser diagnostics for studies of shock initiation in energetic materials. Citation Details In-Document Search Title: Ultrafast laser diagnostics for studies of shock ...

  13. Surface modified CFx cathode material for ultrafast discharge...

    Office of Scientific and Technical Information (OSTI)

    Surface modified CFx cathode material for ultrafast discharge and high energy density Prev Next Title: Surface modified CFx cathode material for ultrafast discharge and high...

  14. Ultrafast Probes for Dirac Materials (Technical Report) | SciTech...

    Office of Scientific and Technical Information (OSTI)

    SciTech Connect Search Results Technical Report: Ultrafast Probes for Dirac Materials Citation Details In-Document Search Title: Ultrafast Probes for Dirac Materials Authors: ...

  15. Ultrafast all-optical manipulation of interfacial magnetoelectric...

    Office of Scientific and Technical Information (OSTI)

    Technical Report: Ultrafast all-optical manipulation of interfacial magnetoelectric coupling Citation Details In-Document Search Title: Ultrafast all-optical manipulation of ...

  16. Ultrafast Laser Fabrication: a Rapid Prototyping Capability for...

    Office of Scientific and Technical Information (OSTI)

    Technical Report: Ultrafast Laser Fabrication: a Rapid Prototyping Capability for CINT Citation Details In-Document Search Title: Ultrafast Laser Fabrication: a Rapid Prototyping ...

  17. Cavity-Enhanced Transient Absorption Spectroscopy: Ultrafast...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Cavity-Enhanced Transient Absorption Spectroscopy: Ultrafast Spectroscopy goes Ultra-Sensitive Wednesday, November 11, 2015 - 3:00pm SLAC, Redtail Hawk Conference Room 108A...

  18. Electronic Coupling Dependence of Ultrafast Interfacial Electron...

    Office of Scientific and Technical Information (OSTI)

    Electronic Coupling Dependence of Ultrafast Interfacial Electron Transfer on Nanocrystalline Thin Films and Single Crystal Citation Details In-Document Search Title: Electronic ...

  19. Order and correlation contributions to the entropy of hydrophobic solvation

    SciTech Connect (OSTI)

    Liu, Maoyuan; Besford, Quinn Alexander; Mulvaney, Thomas; Gray-Weale, Angus

    2015-03-21

    The entropy of hydrophobic solvation has been explained as the result of ordered solvation structures, of hydrogen bonds, of the small size of the water molecule, of dispersion forces, and of solvent density fluctuations. We report a new approach to the calculation of the entropy of hydrophobic solvation, along with tests of and comparisons to several other methods. The methods are assessed in the light of the available thermodynamic and spectroscopic information on the effects of temperature on hydrophobic solvation. Five model hydrophobes in SPC/E water give benchmark solvation entropies via Widom’s test-particle insertion method, and other methods and models are tested against these particle-insertion results. Entropies associated with distributions of tetrahedral order, of electric field, and of solvent dipole orientations are examined. We find these contributions are small compared to the benchmark particle-insertion entropy. Competitive with or better than other theories in accuracy, but with no free parameters, is the new estimate of the entropy contributed by correlations between dipole moments. Dipole correlations account for most of the hydrophobic solvation entropy for all models studied and capture the distinctive temperature dependence seen in thermodynamic and spectroscopic experiments. Entropies based on pair and many-body correlations in number density approach the correct magnitudes but fail to describe temperature and size dependences, respectively. Hydrogen-bond definitions and free energies that best reproduce entropies from simulations are reported, but it is difficult to choose one hydrogen bond model that fits a variety of experiments. The use of information theory, scaled-particle theory, and related methods is discussed briefly. Our results provide a test of the Frank-Evans hypothesis that the negative solvation entropy is due to structured water near the solute, complement the spectroscopic detection of that solvation structure by

  20. Ultrafast Optical Microscopy of Single Monolayer Molybdenum Disulfide Flakes

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Seo, Minah; Yamaguchi, Hisato; Mohite, Aditya D.; Boubanga-Tombet, Stephane; Blancon, Jean-Christophe; Najmaei, Sina; Ajayan, Pulickel M.; Lou, Jun; Taylor, Antoinette J.; Prasankumar, Rohit P.

    2016-02-15

    We performed ultrafast optical microscopy on single flakes of atomically thin CVD-grown molybdenum disulfide, using non-degenerate femtosecond pump-probe spectroscopy to excite and probe carriers above and below the indirect and direct band gaps. These measurements reveal the influence of layer thickness on carrier dynamics when probing near the band gap. Furthermore, fluence-dependent measurements indicate that carrier relaxation is primarily influenced by surface-related defect and trap states after above-bandgap photoexcitation. Furthermore, the ability to probe femtosecond carrier dynamics in individual flakes can thus give much insight into light-matter interactions in these two-dimensional nanosystems.

  1. Preferential solvation of lithium cations and impacts on oxygen reduction in lithium–air batteries

    SciTech Connect (OSTI)

    Zheng, Dong; Qu, Deyu; Yang, Xiao -Qing; Lee, Hung -Sui; Qu, Deyang

    2015-09-16

    The solvation of Li⁺ with eleven non-aqueous solvents commonly used as the electrolytes for Li batteries were studied. The solvation preferences of different solvents were compared by means of electrospray mass spectrometry and collision-induced dissociation. The relative strength of the solvent for the solvation of Li⁺ was determined. The Lewis acidity of the solvated Li⁺ cations was determined by the preferential solvation of the solvent in the solvation shell. The kinetics of the catalytic disproportionation of the O₂⁻ depends on the relative Lewis acidity of the solvated Li⁺ ion. The impact of the solvated Li⁺ cation on the O₂ redox reaction was also investigated.

  2. Preferential solvation of lithium cations and impacts on oxygen reduction in lithium–air batteries

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Zheng, Dong; Qu, Deyu; Yang, Xiao -Qing; Lee, Hung -Sui; Qu, Deyang

    2015-09-16

    The solvation of Li⁺ with eleven non-aqueous solvents commonly used as the electrolytes for Li batteries were studied. The solvation preferences of different solvents were compared by means of electrospray mass spectrometry and collision-induced dissociation. The relative strength of the solvent for the solvation of Li⁺ was determined. The Lewis acidity of the solvated Li⁺ cations was determined by the preferential solvation of the solvent in the solvation shell. The kinetics of the catalytic disproportionation of the O₂⁻ depends on the relative Lewis acidity of the solvated Li⁺ ion. The impact of the solvated Li⁺ cation on the O₂ redoxmore » reaction was also investigated.« less

  3. SISGR: Linking Ion Solvation and Lithium Battery Electrolyte Properties

    SciTech Connect (OSTI)

    Trulove, Paul C; Foley, Matthew P

    2013-03-14

    The solvation and phase behavior of the model battery electrolyte salt lithium trifluoromethanesulfonate (LiCF3SO3) in commonly used organic solvents; ethylene carbonate (EC), gamma-butyrolactone (GBL), and propylene carbonate (PC) was explored. Data from differential scanning calorimetry (DSC), Raman spectroscopy, and X-ray diffraction were correlated to provide insight into the solvation states present within a sample mixture. Data from DSC analyses allowed the construction of phase diagrams for each solvent system. Raman spectroscopy enabled the determination of specific solvation states present within a solvent-????salt mixture, and X-ray diffraction data provided exact information concerning the structure of a solvates that could be isolated Thermal analysis of the various solvent-salt mixtures revealed the phase behavior of the model electrolytes was strongly dependent on solvent symmetry. The point groups of the solvents were (in order from high to low symmetry): C2V for EC, CS for GBL, and C1 for PC(R). The low symmetry solvents exhibited a crystallinity gap that increased as solvent symmetry decreased; no gap was observed for EC-LiTf, while a crystallinity gap was observed spanning 0.15 to 0.3 mole fraction for GBL-LiTf, and 0.1 to 0.33 mole fraction for PC(R)-LiTf mixtures. Raman analysis demonstrated the dominance of aggregated species in almost all solvent compositions. The AGG and CIP solvates represent the majority of the species in solutions for the more concentrated mixtures, and only in very dilute compositions does the SSIP solvate exist in significant amounts. Thus, the poor charge transport characteristics of CIP and AGG account for the low conductivity and transport properties of LiTf and explain why is a poor choice as a source of Li+ ions in a Li-ion battery.

  4. Unusual dynamic properties of water near the ice-binding plane of hyperactive antifreeze protein

    SciTech Connect (OSTI)

    Kuffel, Anna; Czapiewski, Dariusz; Zielkiewicz, Jan

    2015-10-07

    The dynamical properties of solvation water of hyperactive antifreeze protein from Choristoneura fumiferana (CfAFP) are analyzed and discussed in context of its antifreeze activity. The protein comprises of three well-defined planes and one of them binds to the surface of ice. The dynamical properties of solvation water around each of these planes were analyzed separately; the results are compared with the dynamical properties of solvation water of ice around its two crystallographic planes: basal and prism. Three main conclusions are inferred from our investigations. The first one is that the solvation shell of CfAFP does not seem to be particularly far-ranged, at least not beyond what is usually observed for proteins that do not interact with ice. Therefore, it does not appear to us that the antifreeze activity is enhanced by a long-ranged retardation of water mobility. Also the correlation between the collective mobility of water and the collective mobility of protein atoms highly resembles the one measured for the protein that does not interact with ice. Our second conclusion is that the dynamical properties of solvation water of CfAFP are non-uniform. The dynamics of solvation water of ice-binding plane is, in some respects, different from the dynamics of solvation water of the two remaining planes. The feature that distinguishes the dynamics of solvation water of the three planes is the activation energy of diffusion process. The third conclusion is that—from the three analyzed solvation shells of CfAFP—the dynamical properties of solvation water of the ice-binding plane resemble the most the properties of solvation water of ice; note, however, that these properties still clearly differ from the dynamic properties of solvation water of ice.

  5. Impact system for ultrafast synchrotron experiments

    SciTech Connect (OSTI)

    Jensen, B. J.; Owens, C. T.; Ramos, K. J.; Yeager, J. D.; Saavedra, R. A.; Luo, S. N.; Hooks, D. E.; Iverson, A. J.; Fezzaa, K.

    2013-01-15

    The impact system for ultrafast synchrotron experiments, or IMPULSE, is a 12.6-mm bore light-gas gun (<1 km/s projectile velocity) designed specifically for performing dynamic compression experiments using the advanced imaging and X-ray diffraction methods available at synchrotron sources. The gun system, capable of reaching projectile velocities up to 1 km/s, was designed to be portable for quick insertion/removal in the experimental hutch at Sector 32 ID-B of the Advanced Photon Source (Argonne, IL) while allowing the target chamber to rotate for sample alignment with the beam. A key challenge in using the gun system to acquire dynamic data on the nanosecond time scale was synchronization (or bracketing) of the impact event with the incident X-ray pulses (80 ps width). A description of the basic gun system used in previous work is provided along with details of an improved launch initiation system designed to significantly reduce the total system time from launch initiation to impact. Experiments were performed to directly measure the gun system time and to determine the gun performance curve for projectile velocities ranging from 0.3 to 0.9 km/s. All results show an average system time of 21.6 {+-} 4.5 ms, making it possible to better synchronize the gun system and detectors to the X-ray beam.

  6. Pure Optical Dephasing Dynamics in Semiconducting Single-Walled...

    Office of Scientific and Technical Information (OSTI)

    Journal Article: Pure Optical Dephasing Dynamics in Semiconducting Single-Walled Carbon Nanotubes Citation ... We report a detailed study of ultrafast exciton dephasing ...

  7. Ultrafast carrier capture in InGaAs quantum posts

    SciTech Connect (OSTI)

    Talbayev, Diyar; Taylor, Antoinette J; Stehr, D; Morris, C M; Wagner, M; Kim, H C; Schneider, H; Petroff, P M; Sherwin, M S

    2009-01-01

    To explore the capture dynamics of photoexcited carriers in semiconductor quantum posts, optical pump - THz probe and time-resolved photoluminescence spectroscopy were performed. The results of the THz experiment show that after ultrafast excitation, electrons relax within a few picoseconds into the quantum posts, which are acting as efficient traps. The saturation of the quantum post states, probed by photoluminescence, was reached approximately at ten times the quantum post density in the samples. The results imply that quantum posts are posts highly attractive nanostructures for future device applications.

  8. Computational observation of enhanced solvation of the hydroxyl radical with increased NaCl concentration

    SciTech Connect (OSTI)

    Wick, Collin D.; Dang, Liem X.

    2006-05-11

    Classical molecular dynamics simulations with many-body potentials were carried out to quantitatively determine the effect of NaCl salt concentration on the aqueous solvation and surface concentration of hydroxyl radicals. The potential of mean force technique was used to track the incremental free energy of the hydroxyl radical from the vapor, crossing the air-water interface into the aqueous bulk. Results showed increased NaCl salt concentration significantly enhanced hydroxyl radical solvation, which should significantly increase its accommodation on water droplets. This has been experimentally observed for ozone aqueous accommodation with increased NaI concentration, but to our knowledge, no experimental study has probed this for hydroxyl radicals. The origin for this effect was found to be very favorable hydroxyl radical-chloride ion interactions, being stronger than for water-chloride. This work was performed at Pacific Northwest National Laboratory (PNNL) under the auspices of the Division of Chemical Sciences, Office of Basic Energy Sciences, U.S. Department of Energy. Battelle operates PNNL for the Department of Energy.

  9. Dissecting ion-specific dielectric spectra of sodium-halide solutions into solvation water and ionic contributions

    SciTech Connect (OSTI)

    Rinne, Klaus F.; Netz, Roland R.; Gekle, Stephan

    2014-12-07

    Using extensive equilibrium molecular dynamics simulations we determine the dielectric spectra of aqueous solutions of NaF, NaCl, NaBr, and NaI. The ion-specific and concentration-dependent shifts of the static dielectric constants and the dielectric relaxation times match experimental results very well, which serves as a validation of the classical and non-polarizable ionic force fields used. The purely ionic contribution to the dielectric response is negligible, but determines the conductivity of the salt solutions. The ion-water cross correlation contribution is negative and reduces the total dielectric response by about 5%-10% for 1?M solutions. The dominating water dielectric response is decomposed into different water solvation shells and ion-pair configurations, by this the spectral blue shift and the dielectric decrement of salt solutions with increasing salt concentration is demonstrated to be primarily caused by first-solvation shell water. With rising salt concentration the simulated spectra show more pronounced deviations from a single-Debye form and can be well described by a Cole-Cole fit, in quantitative agreement with experiments. Our spectral decomposition into ionic and different water solvation shell contributions does not render the individual contributions more Debye-like, this suggests the non-Debye-like character of the dielectric spectra of salt solutions not to be due to the superposition of different elementary relaxation processes with different relaxation times. Rather, the non-Debye-like character is likely to be an inherent spectral signature of solvation water around ions.

  10. Strong influence of coadsorbate interaction on CO desorption dynamics on

    Office of Scientific and Technical Information (OSTI)

    Ru(0001) probed by ultrafast x-ray spectroscopy and ab initio simulations (Journal Article) | SciTech Connect Journal Article: Strong influence of coadsorbate interaction on CO desorption dynamics on Ru(0001) probed by ultrafast x-ray spectroscopy and ab initio simulations Citation Details In-Document Search Title: Strong influence of coadsorbate interaction on CO desorption dynamics on Ru(0001) probed by ultrafast x-ray spectroscopy and ab initio simulations We show that coadsorbed oxygen

  11. Ultrafast infrared studies of complex ligand rearrangements in solution

    SciTech Connect (OSTI)

    Payne, Christine K.

    2003-05-31

    , this research demonstrates the importance of examining reaction dynamics on the ultrafast timescale. In the case of both ring slip and alkyne polymerization, early time dynamics have been invaluable in understanding the exact reaction mechanisms which show important differences from previously accepted models.

  12. Ultrafast Spectroscopy of Warm Dense Matter

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Spectroscopy of Warm Dense Matter Ultrafast Spectroscopy of Warm Dense Matter Print Wednesday, 25 April 2012 00:00 Being neither solid, liquid, gas, nor plasma, warm dense matter (WDM) occupies a no man's land in the map of material phases. Its temperature can range between that of planetary cores (tens of thousands K) to that of stellar cores (hundreds of thousands K). Not only is it prevalent throughout the universe, it is relevant to inertial confinement fusion (ICF) and material

  13. An ultrafast carbon nanotube terahertz polarisation modulator

    SciTech Connect (OSTI)

    Docherty, Callum J.; Stranks, Samuel D.; Habisreutinger, Severin N.; Joyce, Hannah J.; Herz, Laura M.; Nicholas, Robin J.; Johnston, Michael B.

    2014-05-28

    We demonstrate ultrafast modulation of terahertz radiation by unaligned optically pumped single-walled carbon nanotubes. Photoexcitation by an ultrafast optical pump pulse induces transient terahertz absorption in nanowires aligned parallel to the optical pump. By controlling the polarisation of the optical pump, we show that terahertz polarisation and modulation can be tuned, allowing sub-picosecond modulation of terahertz radiation. Such speeds suggest potential for semiconductor nanowire devices in terahertz communication technologies.

  14. Structural Interactions within Lithium Salt Solvates: Cyclic Carbonates and Esters

    SciTech Connect (OSTI)

    Seo, D. M.; Afroz, Taliman; Allen, Joshua L.; Boyle, Paul D.; Trulove, Paul C.; De Long, Hugh C.; Henderson, Wesley A.

    2014-11-13

    Only limited information is available regarding the manner in which cyclic carbonate and ester solvents coordinate Li+ cations in electrolyte solutions for lithium batteries. One approach to gleaning significant insight into these interactions is to examine crystalline solvate structures. To this end, eight new solvate structures are reported with ethylene carbonate, ?-butyrolactone and ?-valerolactone: (EC)3:LiClO4, (EC)2:LiClO4, (EC)2:LiBF4, (GBL)4:LiPF6, (GBL)1:LiClO4, (GVL)1:LiClO4, (GBL)1:LiBF4 and (GBL)1:LiCF3SO3. The crystal structure of (EC)1:LiCF3SO3 is also re-reported for comparison. These structures enable the factors which govern the manner in which the ions are coordinated and the ion/solvent packingin the solid-stateto be scrutinized in detail.

  15. Sparingly Solvating Electrolytes for High Energy Density Lithium-Sulfur

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Batteries - Joint Center for Energy Storage Research August 24, 2016, Videos Sparingly Solvating Electrolytes for High Energy Density Lithium-Sulfur Batteries As JCESR scientists work to develop lighter and less expensive chemistries than those used in current lithium-ion batteries, lithium-sulfur shows tremendous promise. However, current lithium-sulfur batteries require an excessive amount of electrolyte to achieve moderate cycle life. This perspective presents an alternate approach of

  16. Understanding the Role of Solvation Forces on the Preferential Attachment of Nanoparticles in Liquid

    SciTech Connect (OSTI)

    Welch, David A.; Woehl, Taylor J.; Park, Chiwoo; Faller, Roland; Evans, James E.; Browning, Nigel D.

    2015-11-20

    We discuss optimization of colloidal nanoparticle synthesis techniques, which requires an understanding of underlying particle growth mechanisms. Nonclassical growth mechanisms are particularly important as they affect nanoparticle size and shape distributions, which in turn influence functional properties. For example, preferential attachment of nanoparticles is known to lead to the formation of mesocrystals, although the formation mechanism is currently not well-understood. Here we employ in situ liquid cell scanning transmission electron microscopy and steered molecular dynamics (SMD) simulations to demonstrate that the experimentally observed preference for end-to-end attachment of silver nanorods is a result of weaker solvation forces occurring at rod ends. In conclusion, SMD reveals that when the side of a nanorod approaches another rod, perturbation in the surface-bound water at the nanorod surface creates significant energy barriers to attachment. Additionally, rod morphology (i.e., facet shape) effects can explain the majority of the side attachment effects that are observed experimentally.

  17. Ultrafast terahertz gating of the polarization and giant nonlinear...

    Office of Scientific and Technical Information (OSTI)

    Journal Article: Ultrafast terahertz gating of the polarization and giant nonlinear optical response in BiFeO3 thin films Citation Details In-Document Search Title: Ultrafast ...

  18. Electronic/photonic interfaces for ultrafast data processing...

    Office of Scientific and Technical Information (OSTI)

    and hybrid integration processes, two key elements of an ultrafast data processor. ... TRANSMISSION; TECHNOLOGY ASSESSMENT Numerical analysis-Data processing.; ...

  19. Electrolyte Solvation and Ionic Association. V. Acetonitrile-Lithium Bis(fluorosulfonyl)imide (LiFSI) Mixtures

    SciTech Connect (OSTI)

    Han, Sang D.; Borodin, Oleg; Seo, D. M.; Zhou, Zhi B.; Henderson, Wesley A.

    2014-09-30

    Electrolytes with the salt lithium bis(fluorosulfonyl)imide (LiFSI) have been evaluated relative to comparable electrolytes with other lithium salts. Acetonitrile (AN) has been used as a model electrolyte solvent. The information obtained from the thermal phase behavior, solvation/ionic association interactions, quantum chemical (QC) calculations and molecular dynamics (MD) simulations (with an APPLE&P many-body polarizable force field for the LiFSI salt) of the (AN)n-LiFSI mixtures provides detailed insight into the coordination interactions of the FSI- anions and the wide variability noted in the electrolyte transport property (i.e., viscosity and ionic conductivity).

  20. A self-consistent phase-field approach to implicit solvation...

    Office of Scientific and Technical Information (OSTI)

    Publisher's Accepted Manuscript: A self-consistent phase-field approach to implicit solvation of charged molecules with Poisson-Boltzmann electrostatics This content will become...

  1. Quasiparticle dynamics across the full Brillouin zone of Bi2Sr2CaCu2O8+δ traced with ultrafast time and angle-resolved photoemission spectroscopy

    SciTech Connect (OSTI)

    Dakovski, Georgi L.; Durakiewicz, Tomasz; Zhu, Jian-Xin; Riseborough, Peter S.; Gu, Genda; Gilbertson, Steve M.; Taylor, Antoinette; Rodriguez, George

    2015-10-12

    A hallmark in the cuprate family of high-temperature superconductors is the nodal-antinodal dichotomy. In this regard, angle-resolved photoemission spectroscopy (ARPES) has proven especially powerful, providing band structure information directly in energy-momentum space. Time-resolved ARPES (trARPES) holds great promise of adding ultrafast temporal information, in an attempt to identify different interaction channels in the time domain. Previous studies of the cuprates using trARPES were handicapped by the low probing energy which significantly limits the accessible momentum space. Using 20.15eV, 12 fs pulses we show for the first time the evolution of quasiparticles in the antinodal region of Bi2Sr2CaCu2O8+δ and demonstrate that nonmonotonic relaxation dynamics dominates above a certain fluence threshold. The dynamics is heavily influenced by transient modification of the electron-phonon interaction and phase space restrictions, in severe contrast to the monotonic relaxation in the nodal and off-nodal regions.

  2. Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Ma, X.; Fang, F.; Li, Q.; Zhu, J.; Yang, Y.; Wu, Y. Z.; Zhao, H. B.; Lüpke, G.

    2015-10-28

    In this study, optical control of spin is of central importance in the research of ultrafast spintronic devices utilizing spin dynamics at short time scales. Recently developed optical approaches such as ultrafast demagnetization, spin-transfer and spin-orbit torques open new pathways to manipulate spin through its interaction with photon, orbit, charge or phonon. However, these processes are limited by either the long thermal recovery time or the low-temperature requirement. Here we experimentally demonstrate ultrafast coherent spin precession via optical charge-transfer processes in the exchange-coupled Fe/CoO system at room temperature. The efficiency of spin precession excitation is significantly higher and the recoverymore » time of the exchange-coupling torque is much shorter than for the demagnetization procedure, which is desirable for fast switching. The exchange coupling is a key issue in spin valves and tunnelling junctions, and hence our findings will help promote the development of exchange-coupled device concepts for ultrafast coherent spin manipulation.« less

  3. Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes

    SciTech Connect (OSTI)

    Ma, X.; Fang, F.; Li, Q.; Zhu, J.; Yang, Y.; Wu, Y. Z.; Zhao, H. B.; Lüpke, G.

    2015-10-28

    In this study, optical control of spin is of central importance in the research of ultrafast spintronic devices utilizing spin dynamics at short time scales. Recently developed optical approaches such as ultrafast demagnetization, spin-transfer and spin-orbit torques open new pathways to manipulate spin through its interaction with photon, orbit, charge or phonon. However, these processes are limited by either the long thermal recovery time or the low-temperature requirement. Here we experimentally demonstrate ultrafast coherent spin precession via optical charge-transfer processes in the exchange-coupled Fe/CoO system at room temperature. The efficiency of spin precession excitation is significantly higher and the recovery time of the exchange-coupling torque is much shorter than for the demagnetization procedure, which is desirable for fast switching. The exchange coupling is a key issue in spin valves and tunnelling junctions, and hence our findings will help promote the development of exchange-coupled device concepts for ultrafast coherent spin manipulation.

  4. Multibody correlations in the hydrophobic solvation of glycine peptides

    SciTech Connect (OSTI)

    Harris, Robert C.; Drake, Justin A.; Pettitt, B. Montgomery

    2014-12-14

    Protein collapse during folding is often assumed to be driven by a hydrophobic solvation energy (ΔG{sub vdw}) that scales linearly with solvent-accessible surface area (A). In a previous study, we argued that ΔG{sub vdw}, as well as its attractive (ΔG{sub att}) and repulsive (ΔG{sub rep}) components, was not simply a linear function of A. We found that the surface tensions, γ{sub rep}, γ{sub att}, and γ{sub vdw}, gotten from ΔG{sub rep}, ΔG{sub att}, and ΔG{sub vdw} against A for four configurations of deca-alanine differed from those obtained for a set of alkanes. In the present study, we extend our analysis to fifty decaglycine structures and atomic decompositions. We find that different configurations of decaglycine generate different estimates of γ{sub rep}. Additionally, we considered the reconstruction of the solvation free energy from scaling the free energy of solvation of each atom type, free in solution. The free energy of the isolated atoms, scaled by the inverse surface area the atom would expose in the molecule does not reproduce the γ{sub rep} for the intact decaglycines. Finally, γ{sub att} for the decaglycine conformations is much larger in magnitude than those for deca-alanine or the alkanes, leading to large negative values of γ{sub vdw} (−74 and −56 cal/mol/Å{sup 2} for CHARMM27 and AMBER ff12sb force fields, respectively). These findings imply that ΔG{sub vdw} favors extended rather than compact structures for decaglycine. We find that ΔG{sub rep} and ΔG{sub vdw} have complicated dependencies on multibody correlations between solute atoms, on the geometry of the molecular surface, and on the chemical identities of the atoms.

  5. Bond-valence methods for pKa prediction. II. Bond-valence, electrostatic, molecular geometry, and solvation effects

    SciTech Connect (OSTI)

    Bickmore, Barry R.; Rosso, Kevin M.; Tadanier, Christopher J.; Bylaska, Eric J.; Doud, Darrin

    2006-08-15

    In a previous contribution, we outlined a method for predicting (hydr)oxy-acid and oxide surface acidity constants based on three main factors: bond valence, Me?O bond ionicity, and molecular shape. Here electrostatics calculations and ab initio molecular dynamics simulations are used to qualitatively show that Me?O bond ionicity controls the extent to which the electrostatic work of proton removal departs from ideality, bond valence controls the extent of solvation of individual functional groups, and bond valence and molecular shape controls local dielectric response. These results are consistent with our model of acidity, but completely at odds with other methods of predicting acidity constants for use in multisite complexation models. In particular, our ab initio molecular dynamics simulations of solvated monomers clearly indicate that hydrogen bonding between (hydr)oxo-groups and water molecules adjusts to obey the valence sum rule, rather than maintaining a fixed valence based on the coordination of the oxygen atom as predicted by the standard MUSIC model.

  6. Ultrafast photodetectors allow direct observation of multiple electrons

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    generated by a single photon Ultrafast photodetectors Ultrafast photodetectors allow direct observation of multiple electrons generated by a single photon The new technique involves monitoring photocurrent transients in specially engineered photodetectors that provide very high temporal resolution of only 50 picoseconds. September 11, 2015 Andrew Fidler of Los Alamos National Laboratory examines an ultrafast photodetector used to measure quantum dot carrier multiplication in real time.

  7. Solvation Free Energies of Alanine Peptides: The Effect of Flexibility

    SciTech Connect (OSTI)

    Kokubo, Hironori; Harris, Robert C.; Asthagiri, Dilip; Pettitt, Bernard M.

    2013-12-03

    The electrostatic (?Gel), cavity-formation (?Gvdw), and total (?G) solvation free energies for 10 alanine peptides ranging in length (n) from 1 to 10 monomers were calculated. The free energies were computed both with xed, extended conformations of the peptides and again for some of the peptides without constraints. The solvation free energies, ?Gel, ?Gvdw, and ?G, were found to be linear in n, with the slopes of the best-fit lines being gamma_el, gamma_vdw, and gamma, respectively. Both gamma_el and gamma were negative for fixed and flexible peptides, and gamma_vdw was negative for fixed peptides. That gamma_vdw was negative was surprising, as experimental data on alkanes, theoretical models, and MD computations on small molecules and model systems generally suggest that gamma_vdw should be positive. A negative gamma_vdw seemingly contradicts the notion that ?Gvdw drives the initial collapse of the protein when it folds by favoring conformations with small surface areas, but when we computed ?Gvdw for the flexible peptides, thereby allowing the peptides to assume natural ensembles of more compact conformations, gamma-vdw was positive. Because most proteins do not assume extended conformations, a ?Gvdw that increases with increasing surface area may be typical for globular proteins. An alternative hypothesis is that the collapse is driven by intramolecular interactions. We show that the intramolecular van der Waal's interaction energy is more favorable for the flexible than for the extended peptides, seemingly favoring this hypothesis, but the large fluctuations in this energy may make attributing the collapse of the peptide to this intramolecular energy difficult.

  8. Morphological changes in ultrafast laser ablation plumes with varying spot size

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Harilal, S. S.; Diwakar, P. K.; Polek, M. P.; Phillips, M. C.

    2015-06-04

    We investigated the role of spot size on plume morphology during ultrafast laser ablation of metal targets. Our results show that the spatial features of fs LA plumes are strongly dependent on the focal spot size. Two-dimensional self-emission images showed that the shape of the ultrafast laser ablation plumes changes from spherical to cylindrical with an increasing spot size from 100 to 600 ?m. The changes in plume morphology and internal structures are related to ion emission dynamics from the plasma, where broader angular ion distribution and faster ions are noticed for the smallest spot size used. The present resultsmoreclearly show that the morphological changes in the plume with spot size are independent of laser pulse width.less

  9. Ultrafast Probes for Dirac Materials (Technical Report) | SciTech...

    Office of Scientific and Technical Information (OSTI)

    Subject: Materials Science(36) Material Science; topological insulators, ultrafast spectroscopy, graphene Word Cloud More Like This Full Text File size NAView Full Text View Full ...

  10. Prospects for Electron Imaging with Ultrafast Time Resolution...

    Office of Scientific and Technical Information (OSTI)

    Service, Springfield, VA at www.ntis.gov. Many pivotal aspects of material science, biomechanics, and chemistry would benefit from nanometer imaging with ultrafast time resolution....

  11. Ultrafast Structural Rearrangements in the MLCT Excited State...

    Office of Scientific and Technical Information (OSTI)

    Ultrafast Structural Rearrangements in the MLCT Excited State for Copper(I) ... previous laser-initiated time-resolved x-ray absorption spectroscopy (LITR-XAS) results. ...

  12. Ultrafast Laser Diagnostics for Energetic-Material Ignition Mechanisms...

    Office of Scientific and Technical Information (OSTI)

    for Physics-Based Model Development. Citation Details In-Document Search Title: Ultrafast Laser Diagnostics for Energetic-Material Ignition Mechanisms: Tools for Physics-Based ...

  13. Ultrafast kinetics subsequent to shock compression in an oxygen...

    Office of Scientific and Technical Information (OSTI)

    to shock compression in an oxygen-balanced mixture of nitromethane and hydrogen peroxide Citation Details In-Document Search Title: Ultrafast kinetics subsequent to shock ...

  14. Ultrafast Laser Diagnostics for Studies of Shock Initiation in...

    Office of Scientific and Technical Information (OSTI)

    Studies of Shock Initiation in Energetic Materials. Citation Details In-Document Search Title: Ultrafast Laser Diagnostics for Studies of Shock Initiation in Energetic Materials. ...

  15. Ultrafast kinetics subsequent to shock in an unreacted, oxygen...

    Office of Scientific and Technical Information (OSTI)

    shock in an unreacted, oxygen balanced mixture of nitromethane and hydrogen peroxide Citation Details In-Document Search Title: Ultrafast kinetics subsequent to shock in an ...

  16. Ultrafast Shock Initiation of Exothermic Chemistry in Hydrogen...

    Office of Scientific and Technical Information (OSTI)

    Shock Initiation of Exothermic Chemistry in Hydrogen Peroxide Citation Details In-Document Search Title: Ultrafast Shock Initiation of Exothermic Chemistry in Hydrogen Peroxide ...

  17. New Algorithm Enables Faster Simulations of Ultrafast Processes

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Algorithm Enables Faster Simulations of Ultrafast Processes New Algorithm Enables Faster ... Academy of Sciences, have developed a new real-time time-dependent density function ...

  18. Ultrafast Structural Rearrangements in the MLCT Excited State...

    Office of Scientific and Technical Information (OSTI)

    Copper(I) bis-Phenanthrolines in Solution Ultrafast excited state structural ... Resource Type: Journal Article Resource Relation: Journal Name: Journal of the American Chemical ...

  19. Ultra-fast framing camera tube

    DOE Patents [OSTI]

    Kalibjian, Ralph

    1981-01-01

    An electronic framing camera tube features focal plane image dissection and synchronized restoration of the dissected electron line images to form two-dimensional framed images. Ultra-fast framing is performed by first streaking a two-dimensional electron image across a narrow slit, thereby dissecting the two-dimensional electron image into sequential electron line images. The dissected electron line images are then restored into a framed image by a restorer deflector operated synchronously with the dissector deflector. The number of framed images on the tube's viewing screen is equal to the number of dissecting slits in the tube. The distinguishing features of this ultra-fast framing camera tube are the focal plane dissecting slits, and the synchronously-operated restorer deflector which restores the dissected electron line images into a two-dimensional framed image. The framing camera tube can produce image frames having high spatial resolution of optical events in the sub-100 picosecond range.

  20. Quantum Transport Effects and Coherent Ultrafast Multidimensional

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Spectroscopy of Light Harvesting Photosynthetic Complexes | MIT-Harvard Center for Excitonics Transport Effects and Coherent Ultrafast Multidimensional Spectroscopy of Light Harvesting Photosynthetic Complexes March 16, 2010 at 3pm/36-428 Shaul Mukamel Department of Chemistry, University of California, Irvine shaul_001 abstract: The harvesting of solar energy and its conversion to chemical energy is essential for all forms of life. Whether quantum effects persist in the energy transport is

  1. Ultrafast Spectroscopy of Warm Dense Matter

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Spectroscopy of Warm Dense Matter Print Being neither solid, liquid, gas, nor plasma, warm dense matter (WDM) occupies a no man's land in the map of material phases. Its temperature can range between that of planetary cores (tens of thousands K) to that of stellar cores (hundreds of thousands K). Not only is it prevalent throughout the universe, it is relevant to inertial confinement fusion (ICF) and material performance under extreme conditions. However, because of its extreme

  2. Ultrafast Spectroscopy of Warm Dense Matter

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultrafast Spectroscopy of Warm Dense Matter Print Being neither solid, liquid, gas, nor plasma, warm dense matter (WDM) occupies a no man's land in the map of material phases. Its temperature can range between that of planetary cores (tens of thousands K) to that of stellar cores (hundreds of thousands K). Not only is it prevalent throughout the universe, it is relevant to inertial confinement fusion (ICF) and material performance under extreme conditions. However, because of its extreme

  3. Structural and thermodynamic properties of the CmIII ion solvated by water and methanol

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Kelley, Morgan P.; Yang, Ping; Clark, Sue B.; Clark, Aurora E.

    2016-04-27

    The geometric and electronic structures of the 9-coordinate Cm3+ ion solvated with both water and methanol are systematically investigated in the gas phase at each possible solvent-shell composition and configuration using density functional theory and second-order Møller–Plesset perturbation theory. Ab initio molecular dynamics simulations are employed to assess the effects of second and third solvent shells on the gas-phase structure. The ion–solvent dissociation energy for methanol is greater than that of water, potentially because of increased charge donation to the ion made possible by the electron-rich methyl group. Further, the ion–solvent dissociation energy and the ion–solvent distance are shown tomore » be dependent on the solvent-shell composition. Furthermore, this has implications for solvent exchange, which is generally the rate-limiting step in complexation reactions utilized in the separation of curium from complex metal mixtures that derive from the advanced nuclear fuel cycle.« less

  4. Understanding the Role of Solvation Forces on the Preferential Attachment of Nanoparticles in Liquid

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Welch, David A.; Woehl, Taylor J.; Park, Chiwoo; Faller, Roland; Evans, James E.; Browning, Nigel D.

    2015-11-20

    We discuss optimization of colloidal nanoparticle synthesis techniques, which requires an understanding of underlying particle growth mechanisms. Nonclassical growth mechanisms are particularly important as they affect nanoparticle size and shape distributions, which in turn influence functional properties. For example, preferential attachment of nanoparticles is known to lead to the formation of mesocrystals, although the formation mechanism is currently not well-understood. Here we employ in situ liquid cell scanning transmission electron microscopy and steered molecular dynamics (SMD) simulations to demonstrate that the experimentally observed preference for end-to-end attachment of silver nanorods is a result of weaker solvation forces occurring at rodmore » ends. In conclusion, SMD reveals that when the side of a nanorod approaches another rod, perturbation in the surface-bound water at the nanorod surface creates significant energy barriers to attachment. Additionally, rod morphology (i.e., facet shape) effects can explain the majority of the side attachment effects that are observed experimentally.« less

  5. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Transformations in Superionic Nanocrystals Print A superionic material is a multi-component solid with simultaneous characteristics of both a solid and a liquid. Above a critical temperature associated with a structural phase transition, one of the atomic species in the material will exhibit liquid-like ionic conductivity and dynamic disorder within the rigid crystalline structure of the other. Discovered by Michael Faraday almost 200 years ago, superionic materials today hold promise for use in

  6. Solvation thermodynamics of amino acid side chains on a short peptide backbone

    SciTech Connect (OSTI)

    Hajari, Timir; Vegt, Nico F. A. van der

    2015-04-14

    The hydration process of side chain analogue molecules differs from that of the actual amino acid side chains in peptides and proteins owing to the effects of the peptide backbone on the aqueous solvent environment. A recent molecular simulation study has provided evidence that all nonpolar side chains, attached to a short peptide backbone, are considerably less hydrophobic than the free side chain analogue molecules. In contrast to this, the hydrophilicity of the polar side chains is hardly affected by the backbone. To analyze the origin of these observations, we here present a molecular simulation study on temperature dependent solvation free energies of nonpolar and polar side chains attached to a short peptide backbone. The estimated solvation entropies and enthalpies of the various amino acid side chains are compared with existing side chain analogue data. The solvation entropies and enthalpies of the polar side chains are negative, but in absolute magnitude smaller compared with the corresponding analogue data. The observed differences are large; however, owing to a nearly perfect enthalpy-entropy compensation, the solvation free energies of polar side chains remain largely unaffected by the peptide backbone. We find that a similar compensation does not apply to the nonpolar side chains; while the backbone greatly reduces the unfavorable solvation entropies, the solvation enthalpies are either more favorable or only marginally affected. This results in a very small unfavorable free energy cost, or even free energy gain, of solvating the nonpolar side chains in strong contrast to solvation of small hydrophobic or nonpolar molecules in bulk water. The solvation free energies of nonpolar side chains have been furthermore decomposed into a repulsive cavity formation contribution and an attractive dispersion free energy contribution. We find that cavity formation next to the peptide backbone is entropically favored over formation of similar sized nonpolar side

  7. Ultrafast band engineering and transient spin currents in antiferromagnetic oxides

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Gu, Mingqiang; Rondinelli, James M.

    2016-04-29

    Here, we report a dynamic structure and band engineering strategy with experimental protocols to induce indirect-to-direct band gap transitions and coherently oscillating pure spin-currents in three-dimensional antiferromagnets (AFM) using selective phononic excitations. In the Mott insulator LaTiO3, we show that a photo-induced nonequilibrium phonon mode amplitude destroys the spin and orbitally degenerate ground state, reduces the band gap by 160 meV and renormalizes the carrier masses. The time scale of this process is a few hundreds of femtoseconds. Then in the hole-doped correlated metallic titanate, we show how pure spin-currents can be achieved to yield spin-polarizations exceeding those observed inmore » classic semiconductors. Last, we demonstrate the generality of the approach by applying it to the non-orbitally degenerate AFM CaMnO3. These results advance our understanding of electron-lattice interactions in structures out-of-equilibrium and establish a rational framework for designing dynamic phases that may be exploited in ultrafast optoelectronic and optospintronic devices.« less

  8. Calculation of the Gibbs Free Energy of Solvation and Dissociation of HCl in Water via Monte Carlo Simulations and Continuum Solvation Models

    SciTech Connect (OSTI)

    McGrath, Matthew; Kuo, I-F W.; Ngouana, Brice F.; Ghogomu, Julius N.; Mundy, Christopher J.; Marenich, Aleksandr; Cramer, Christopher J.; Truhlar, Donald G.; Siepmann, Joern I.

    2013-08-28

    The free energy of solvation and dissociation of hydrogen chloride in water is calculated through a combined molecular simulation quantum chemical approach at four temperatures between T = 300 and 450 K. The free energy is first decomposed into the sum of two components: the Gibbs free energy of transfer of molecular HCl from the vapor to the aqueous liquid phase and the standard-state free energy of acid dissociation of HCl in aqueous solution. The former quantity is calculated using Gibbs ensemble Monte Carlo simulations using either Kohn-Sham density functional theory or a molecular mechanics force field to determine the system’s potential energy. The latter free energy contribution is computed using a continuum solvation model utilizing either experimental reference data or micro-solvated clusters. The predicted combined solvation and dissociation free energies agree very well with available experimental data. CJM was supported by the US Department of Energy,Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. Pacific Northwest National Laboratory is operated by Battelle for the US Department of Energy.

  9. Anion Coordination Interactions in Solvates with the Lithium Salts LiDCTA and LiTDI

    SciTech Connect (OSTI)

    McOwen, Dennis W.; Delp, Samuel A.; Paillard, Elie; Herriot, Cristelle; Han, Sang D.; Boyle, Paul D.; Sommer, Roger D.; Henderson, Wesley A.

    2014-04-17

    Lithium 4,5-dicyano-1,2,3-triazolate (LiDCTA) and lithium 2-trifluoromethyl-4,5-dicyanoimidazole (LiTDI) are two salts proposed for lithium battery electrolyte applications, but little is known about the manner in which the DCTA- and TDI- anions coordinate Li+ cations. To explore this in-depth, crystal structures are reported here for two solvates with LiDCTA: (G2)1:LiDCTA and (G1)1:LiDCTA with diglyme and monoglyme, respectively, and seven solvates with LiTDI: (G1)2:LiTDI, (G2)2:LiTDI, (G3)1:LiTDI, (THF)1:LiTDI, (EC)1:LiTDI, (PC)1:LiTDI and (DMC)1/2:LiTDI with monoglyme, diglyme, triglyme, tetrahydrofuran, ethylene carbonate, propylene carbonate and dimethyl carbonate, respectively. These latter solvate structures are compared with the previously reported acetonitrile (AN)2:LiTDI structure. The solvates indicate that the LiTDI salt is much less associated than the LiDCTA salt and that the ions in LiTDI, when aggregated in solvates, have a very similar TDI-...Li+ cation mode of coordination through both the anion ring and cyano nitrogen atoms. Such coordination facilitates the formation of polymeric ion aggregates, instead of dimers. Insight into such ion speciation is instrumental for understanding the electrolyte properties of aprotic solvent mixtures with these salts.

  10. Differential ultrafast all-optical switching of the resonances of a micropillar cavity

    SciTech Connect (OSTI)

    Thyrrestrup, Henri Yce, Emre; Ctistis, Georgios; Vos, Willem L.; Claudon, Julien; Grard, Jean-Michel

    2014-09-15

    We perform frequency- and time-resolved all-optical switching of a GaAs-AlAs micropillar cavity using an ultrafast pump-probe setup. The switching is achieved by two-photon excitation of free carriers. We track the cavity resonances in time with a high frequency resolution. The pillar modes exhibit simultaneous frequency shifts, albeit with markedly different maximum switching amplitudes and relaxation dynamics. These differences stem from the non-uniformity of the free carrier density in the micropillar, and are well understood by taking into account the spatial distribution of injected free carriers, their spatial diffusion and surface recombination at micropillar sidewalls.

  11. Ultrafast magneto-photocurrents in GaAs: Separation of surface and bulk contributions

    SciTech Connect (OSTI)

    Schmidt, Christian B. Priyadarshi, Shekhar; Bieler, Mark; Tarasenko, Sergey A.

    2015-04-06

    We induce ultrafast magneto-photocurrents in a GaAs crystal employing interband excitation with femtosecond laser pulses at room temperature and non-invasively separate surface and bulk contributions to the overall current response. The separation between the different symmetry contributions is achieved by measuring the simultaneously emitted terahertz radiation for different sample orientations. Excitation intensity and photon energy dependences of the magneto-photocurrents for linearly and circularly polarized excitations reveal an involvement of different microscopic origins, one of which is the inverse spin Hall effect. Our experiments are important for a better understanding of the complex momentum-space carrier dynamics in magnetic fields.

  12. Ultrafast transient reflectance of epitaxial semiconducting perovskite thin films

    SciTech Connect (OSTI)

    Smolin, S. Y.; Guglietta, G. W.; Baxter, J. B. E-mail: smay@coe.drexel.edu; Scafetta, M. D.; May, S. J. E-mail: smay@coe.drexel.edu

    2014-07-14

    Ultrafast pump-probe transient reflectance (TR) spectroscopy was used to study carrier dynamics in an epitaxial perovskite oxide thin film of LaFeO{sub 3} (LFO) with a thickness of 40 unit cells (16?nm) grown by molecular beam epitaxy on (LaAlO{sub 3}){sub 0.3}(Sr{sub 2}AlTaO{sub 6}){sub 0.7} (LSAT). TR spectroscopy shows two negative transients in reflectance with local maxima at ?2.5?eV and ?3.5?eV which correspond to two optical transitions in LFO as determined by ellipsometry. The kinetics at these transients were best fit with an exponential decay model with fast (540 ps), medium (?200 ps), and slow (??3?ns) components that we attribute mainly to recombination of photoexcited carriers. Moreover, these reflectance transients did not completely decay within the observable time window, indicating that ?10% of photoexcited carriers exist for at least 3?ns. This work illustrates that TR spectroscopy can be performed on thin (<20?nm) epitaxial oxide films to provide a quantitative understanding of recombination lifetimes, which are important parameters for the potential utilization of perovskite films in photovoltaic and photocatalytic applications.

  13. Solvation of molecules in superfluid helium enhances the interaction induced localization effect

    SciTech Connect (OSTI)

    Walewski, ?ukasz Forbert, Harald; Marx, Dominik

    2014-04-14

    Atomic nuclei become delocalized at low temperatures as a result of quantum effects, whereas they are point-like in the high temperature (classical) limit. For non-interacting nuclei, the delocalization upon lowering the temperature is quantitatively described in terms of the thermal de Broglie wavelength of free particles. Clearly, light non-interacting nuclei the proton being a prominent one are much more delocalized at low temperatures compared to heavy nuclei, such as non-interacting oxygen having water in mind. However, strong interactions due to chemical bonding in conjunction with ultra-low temperatures characteristic to superfluid helium nanodroplets change this common picture substantially for nuclei in molecules or clusters. It turns out that protons shared in hydrogen bonds undergo an extreme interaction induced localization at temperatures on the order of 1 K, which compresses the protonic spatial distributions to the size of the much heavier donor or acceptor atoms, such as O or Cl nuclei, corresponding to about 0.1% of the volume occupied by a non-interacting proton at the same temperature. Moreover, applying our recently developed hybrid ab initio path integral molecular dynamics/bosonic path integral Monte Carlo quantum simulation technique to a HCl/water cluster, HCl(H{sub 2}O){sub 4}, we find that helium solvation has a significant additional localizing effect of up to about 30% in volume. In particular, the solvent-induced excess localization is the stronger the lesser the given nucleus is already localized in the gas phase reference situation.

  14. Apparatus and method for characterizing ultrafast polarization varying optical pulses

    DOE Patents [OSTI]

    Smirl, Arthur; Trebino, Rick P.

    1999-08-10

    Practical techniques are described for characterizing ultrafast potentially ultraweak, ultrashort optical pulses. The techniques are particularly suited to the measurement of signals from nonlinear optical materials characterization experiments, whose signals are generally too weak for full characterization using conventional techniques.

  15. Ultra-Fast Quantum Efficiency Solar Cell Test - Energy Innovation...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ultra-Fast Quantum Efficiency Solar Cell Test National Renewable Energy Laboratory Contact NREL About This Technology Real-Time QE quickly measures how each solar cell responds to ...

  16. Pulse radiolysis studies of solvated electrons in supercritical ethane with methanol as cosolvent.

    SciTech Connect (OSTI)

    Dimitrijevic, N. M.; Takahashi, K.; Bartels, D. M.; Jonah, C. D.; Chemistry

    2001-08-02

    Pulse radiolysis has been used to study the solvated electron in supercritical ethane with methanol as a cosolvent. These measurements give information about the liquid structure of the cosolvent in these systems. The results show that at temperatures below 110 {sup o}C, there are high local concentrations of alcohol molecules (clusters), which are capable of solvating an electron. The agglomeration number of methanol clusters depends on mole fraction of alcohol at a fixed temperature. Addition of salts increases the size of methanol clusters.

  17. New Algorithm Enables Faster Simulations of Ultrafast Processes

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Algorithm Enables Faster Simulations of Ultrafast Processes New Algorithm Enables Faster Simulations of Ultrafast Processes Opens the Door for Real-Time Simulations in Atomic-Level Materials Research February 20, 2015 Contact: Rachel Berkowitz, 510-486-7254, rberkowitz@lbl.gov femtosecondalgorithm copy Model of ion (Cl) collision with atomically thin semiconductor (MoSe2). Collision region is shown in blue and zoomed in; red points show initial positions of Cl. The simulation calculates the

  18. Ultrafast all-optical manipulation of interfacial magnetoelectric coupling

    Office of Scientific and Technical Information (OSTI)

    (Technical Report) | SciTech Connect Ultrafast all-optical manipulation of interfacial magnetoelectric coupling Citation Details In-Document Search Title: Ultrafast all-optical manipulation of interfacial magnetoelectric coupling Authors: Sheu, Yu-Miin [1] + Show Author Affiliations Los Alamos National Laboratory Publication Date: 2014-04-24 OSTI Identifier: 1129830 Report Number(s): LA-UR-14-22829 DOE Contract Number: AC52-06NA25396 Resource Type: Technical Report Research Org: Los Alamos

  19. Plasmas, Dielectrics and the Ultrafast: First Science and Operational

    Office of Scientific and Technical Information (OSTI)

    Experience at FACET (Conference) | SciTech Connect Conference: Plasmas, Dielectrics and the Ultrafast: First Science and Operational Experience at FACET Citation Details In-Document Search Title: Plasmas, Dielectrics and the Ultrafast: First Science and Operational Experience at FACET FACET (Facility for Advanced Accelerator and Experimental Tests) is an accelerator R&D test facility that has been recently constructed at SLAC National Accelerator Laboratory. The facility provides 20 GeV,

  20. An ultrafast silicon nanoplasmonic ballistic triode

    SciTech Connect (OSTI)

    Greig, S. R. Elezzabi, A. Y.

    2014-12-15

    A nanoscale three terminal silicon based nanoplasmonic triode is proposed as a nanometer transistor. The device is suitable for monolithic integration with complementary-metal-oxide-semiconductor technology. Due to the highly spatially inhomogeneous, highly confined nanoplasmonic mode, electrons generated through two-photon absorption in the silicon are ponderomotively accelerated towards the copper anode producing an output current. Application of a negative grid voltage allows for control of the output current. The nanoplasmonic triode is able to achieve output current as high as 628?mA/?m on an ultrafast timescale of 150 fs in a compact footprint of 0.07??m{sup 2}. Reduction of the plasmonic field strength allows for a CMOS compatible current of 11.7?mA/?m. The results demonstrate the potential for the compact optical control of current useful for applications in high-speed, high current switching, and amplification.

  1. Solvation Phenomena in Dilute Solutions: Formal, Experimental Evidence, and Modeling Implications

    SciTech Connect (OSTI)

    Chialvo, Ariel A

    2013-01-01

    We review the fundamentals underlying a general molecular-based formalism for the microscopic interpretation of the solvation phenomena involving sparingly soluble solutes in compressible media, an approach that hinges around the unambiguous splitting of the species correlation function integrals into short-(finite) and long-ranged (diverging) contributions at infinite dilution, where this condition is taken as the reference system for the derivation of composition expansions. Then, we invoke the formalism (a) to illustrate the well-behaved nature of the solvation contributions to the mechanical partial molecular properties of solutes at infinite dilution, (b) to guide the development of, and provide molecular-based support to, the macroscopic modeling of high-temperature dilute aqueous-electrolyte solutions, (c) to study solvation effects on the kinetic rate constants of reactions in near-critical solvents in an attempt to understand from a microscopic perspective the macroscopic evidence regarding the thermodynamic pressure effects, and (d) to interpret the microscopic mechanism behind synergistic solvation effects involving either co-solutes or co-solvents, and provide a molecular argument on the unsuitability of the van der Waals one-fluid (vdW-1f) mixing rules for the 2 description of weakly attractive solutes in compressible solvents. Finally, we develop thermodynamically consistent perturbation expansions, around the infinite dilution reference, for the species residual properties in binary and ternary mixtures, and discuss the theoretical and modeling implications behind ad hoc first-order truncated expansions.

  2. Solvation and Acid Strength Effects on Catalysis by Faujasite Zeolites

    SciTech Connect (OSTI)

    Gounder, Rajamani P.; Jones, Andrew J.; Carr, Robert T.; Iglesia, Enrique

    2012-02-01

    Kinetic, spectroscopic, and chemical titration data indicate that differences in monomolecular isobutane cracking and dehydrogenation and methanol dehydration turnover rates (per H+) among FAU zeolites treated thermally with steam (H-USY) and then chemically with ammonium hexafluorosilicate (CDHUSY) predominantly reflect differences in the size and solvating properties of their supercage voids rather than differences in acid strength. The number of protons on a given sample was measured consistently by titrations with Na+, with CH3 groups via reactions of dimethyl ether, and with 2,6-di-tert-butylpyridine during methanol dehydration catalysis; these titration values were also supported by commensurate changes in acidic OH infrared band areas upon exposure to titrant molecules. The number of protons, taken as the average of the three titration methods, was significantly smaller than the number of framework Al atoms (Alf) obtained from X-ray diffraction and 27Al magic angle spinning nuclear magnetic resonance spectroscopy on H-USY (0.35 H+/Alf) and CD-HUSY (0.69 H+/Alf). These data demonstrate that the ubiquitous use of Alf sites as structural proxies for active H+ sites in zeolites can be imprecise, apparently because distorted Al structures that are not associated with acidic protons are sometimes detected as Alf sites. Monomolecular isobutane cracking and dehydrogenation rate constants, normalized non-rigorously by the number of Alf species, decreased with increasing Na+ content on both H-USY and CD-HUSY samples and became undetectable at sub-stoichiometric exchange levels (0.32 and 0.72 Na+/Alf ratios, respectively), an unexpected finding attributed incorrectly in previous studies to the presence of minority ‘‘super-acidic’’ sites. These rate constants, when normalized rigorously by the number of residual H+ sites were independent of Na+ content on both H-USY and CD-HUSY samples, reflecting the stoichiometric replacement of protons that are uniform in

  3. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    aqueous systems is essential for many diverse fields, from condensed matter physics to medicine to environmental science. An incoming photon with enough energy to produce a core...

  4. Ultrafast laser-driven proton sources and dynamic proton imaging...

    Office of Scientific and Technical Information (OSTI)

    Language: English Subject: 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 43 PARTICLE ACCELERATORS; ACCELERATION; ELECTRIC FIELDS; ELECTRONS; EVOLUTION; EXPANSION; FOILS; ION ...

  5. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Design » Design for Efficiency » Ultra-Efficient Home Design Ultra-Efficient Home Design All Kaupuni Village homes in Oahu, Hawaii, incorporate energy efficiency and renewable energy technologies to produce as much energy as they consume. Credit: Kenneth Kelly, NREL. All Kaupuni Village homes in Oahu, Hawaii, incorporate energy efficiency and renewable energy technologies to produce as much energy as they consume. Credit: Kenneth Kelly, NREL. Ultra-efficient home design combines

  6. Ultrafast myoglobin structural dynamics observed with an X-ray...

    Office of Scientific and Technical Information (OSTI)

    Univ. of Palermo (Italy). Dept. of Physics. Univ. of Grenoble Alpes and Institute of Structural Biology (France) SLAC National Accelerator Laboratory, Menlo Park, CA (Untied ...

  7. Ultrafast Core-Hole Induced Dynamics in Water

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Swedish Research Council, Swedish National Supercomputer Center, Center for Parallel Computers (Sweden), German Federal Ministry of Education and Research. Operation of the...

  8. In the OSTI Collections: Ultrafast Processes | OSTI, US Dept of Energy

    Office of Scientific and Technical Information (OSTI)

    Office of Scientific and Technical Information Ultrafast Processes Article Acknowledgement: Dr. William N. Watson, Physicist DOE Office of Scientific and Technical Information Examples of ultrafast chemical and electronic processes Further examples of electronic processes Chemical reactions from shock waves Ultrafast instruments References Research Organizations Reports available through OSTI's SciTech Connect Patent available through OSTI's DOepatents Additional References Because the atoms

  9. The role of collective motion in the ultrafast charge transfer in van der Waals heterostructures

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Wang, Han; Bang, Junhyeok; Sun, Yiyang; West, Damien; Meunier, Vincent; Zhang, Shengbai; Liang, Linagbo

    2016-05-10

    Here, the success of van der Waals (vdW) heterostructures, made of graphene, metal dichalcogenides, and other layered materials, hinges on the understanding of charge transfer across the interface as the foundation for new device concepts and applications. In contrast to conventional heterostructures, where a strong interfacial coupling is essential to charge transfer, recent experimental findings indicate that vdW heterostructues can exhibit ultra-fast charge transfer despite the weak binding of the heterostructure. Using time-dependent density functional theory molecular dynamics, we identify a strong dynamic coupling between the vdW layers associated with charge transfer. This dynamic coupling results in rapid nonlinear coherentmore » charge oscillations which constitute a purely electronic phenomenon and are shown to be a general feature of vdW heterostructures provided they have a critical minimum dipole coupling. Application to MoS2/WS2 heterostructure yields good agreement with experiment, indicating near complete charge transfer within a timescale of 100 fs.The success of van der Waals heterostructures made of graphene, metal dichalcogenides and other layered materials, hinges on the understanding of charge transfer across the interface as the foundation for new device concepts and applications. In contrast to conventional heterostructures, where a strong interfacial coupling is essential to charge transfer, recent experimental findings indicate that van der Waals heterostructues can exhibit ultrafast charge transfer despite the weak binding of these heterostructures. Here we find, using time-dependent density functional theory molecular dynamics, that the collective motion of excitons at the interface leads to plasma oscillations associated with optical excitation. By constructing a simple model of the van der Waals heterostructure, we show that there exists an unexpected criticality of the oscillations, yielding rapid charge transfer across the

  10. CITIUS: An infrared-extreme ultraviolet light source for fundamental and applied ultrafast science

    SciTech Connect (OSTI)

    Grazioli, C.; Gauthier, D.; Ivanov, R.; De Ninno, G.; Elettra Sincrotrone Trieste, Trieste ; Callegari, C.; Spezzani, C.; Ciavardini, A.; Coreno, M.; Institute of Inorganic Methodologies and Plasmas , Montelibretti, Roma ; Frassetto, F.; Miotti, P.; Poletto, L.; Golob, D.; Kivimäki, A.; Mahieu, B.; Service des Photons Atomes et Molécules, Commissariat à l'Energie Atomique, Centre d'Etudes de Saclay, Bâtiment 522, 91191 Gif-sur-Yvette ; Bučar, B.; Merhar, M.; Polo, E.; Ressel, B.

    2014-02-15

    We present the main features of CITIUS, a new light source for ultrafast science, generating tunable, intense, femtosecond pulses in the spectral range from infrared to extreme ultraviolet (XUV). The XUV pulses (about 10{sup 5}-10{sup 8} photons/pulse in the range 14-80 eV) are produced by laser-induced high-order harmonic generation in gas. This radiation is monochromatized by a time-preserving monochromator, also allowing one to work with high-resolution bandwidth selection. The tunable IR-UV pulses (10{sup 12}-10{sup 15} photons/pulse in the range 0.4-5.6 eV) are generated by an optical parametric amplifier, which is driven by a fraction of the same laser pulse that generates high order harmonics. The IR-UV and XUV pulses follow different optical paths and are eventually recombined on the sample for pump-probe experiments. We also present the results of two pump-probe experiments: with the first one, we fully characterized the temporal duration of harmonic pulses in the time-preserving configuration; with the second one, we demonstrated the possibility of using CITIUS for selective investigation of the ultra-fast dynamics of different elements in a magnetic compound.

  11. Dynamic

    Office of Legacy Management (LM)

    Dynamic , and Static , Res.ponse of the Government Oil Shale Mine at ' , . , Rifle, ... AND STATIC RESPONSE 'OF THE GOVERNMENT OIL SHALE MINE A T RIFLE, COLORADO, T O THE, ...

  12. Apparatus and method for characterizing ultrafast polarization varying optical pulses

    DOE Patents [OSTI]

    Smirl, A.; Trebino, R.P.

    1999-08-10

    Practical techniques are described for characterizing ultrafast potentially ultraweak, ultrashort optical pulses. The techniques are particularly suited to the measurement of signals from nonlinear optical materials characterization experiments, whose signals are generally too weak for full characterization using conventional techniques. 2 figs.

  13. Ultrafast spin tunneling and injection in coupled nanostructures of InGaAs quantum dots and quantum well

    SciTech Connect (OSTI)

    Yang, Xiao-Jie Kiba, Takayuki; Yamamura, Takafumi; Takayama, Junichi; Subagyo, Agus; Sueoka, Kazuhisa; Murayama, Akihiro

    2014-01-06

    We investigate the electron-spin injection dynamics via tunneling from an In{sub 0.1}Ga{sub 0.9}As quantum well (QW) to In{sub 0.5}Ga{sub 0.5}As quantum dots (QDs) in coupled QW-QDs nanostructures. These coupled nanostructures demonstrate ultrafast (5 to 20 ps) spin injection into the QDs. The degree of spin polarization up to 45% is obtained in the QDs after the injection, essentially depending on the injection time. The spin injection and conservation are enhanced with thinner barriers due to the stronger electronic coupling between the QW and QDs.

  14. Ultrafast Control of Magnetism in Ferromagnetic Semiconductors via Photoexcited Transient Carriers

    SciTech Connect (OSTI)

    Cotoros, Ingrid A.

    2008-12-12

    The field of spintronics offers perspectives for seamless integration of coupled and inter-tunable electrical and magnetic properties in a single device. For integration of the spin degree of freedom with current electronic technology, new semiconductors are needed that show electrically-tunable magnetic properties at room temperature and above. Dilute magnetic semiconductors derived from III-V compounds, like GaMnAs and InMnAs, show coupled and tunable magnetic, transport, and optical properties, due to the fact that their ferromagnetism is hole-mediated. These unconventional materials are ideal systems for manipulating the magnetic order by changing the carrier polarization, population density, and energy band distribution of the complementary subsystem of holes. This is the main theme we cover in this thesis. In particular, we develop a unique setup by use of ultraviolet pump, near-infrared probe femtosecond laser pulses, that allows for magneto-optical Kerr effect (MOKE) spectroscopy experiments. We photo-excite transient carriers in our samples, and measure the induced transient magnetization dynamics. One set of experiments performed allowed us to observe for the first time enhancement of the ferromagnetic order in GaMnAs, on an ultrafast time scale of hundreds of picoseconds. The corresponding transient increase of Curie temperature (Tc, the temperature above which a ferromagnetic material loses its permanent magnetism) of about 1 K for our experimental conditions is a very promising result for potential spintronics applications, especially since it is seconded by observation of an ultrafast ferromagnetic to paramagnetic phase transition above Tc. In a different set of experiments, we"write" the magnetization in a particular orientation in the sample plane. Using an ultrafast scheme, we alter the distribution of holes in the system and detect signatures of the particular memory state in the subsequent magnetization dynamics, with unprecedented hundreds of

  15. Calculating time-resolved differential absorbance spectra for ultrafast pump-probe experiments with surface hopping trajectories

    SciTech Connect (OSTI)

    Petit, Andrew S.; Subotnik, Joseph E.

    2014-10-21

    We report a surface hopping approach for modeling the full time- and frequency-resolved differential absorbance spectra (beyond the inhomogenous limit) obtained in ultrafast pump-probe experiments. In our approach, we combine dynamical information obtained from ensembles of classical trajectories propagated on the ground and on the excited potential energy surfaces to directly calculate optical response functions and hence spectral lineshapes. We demonstrate that our method is exact for the model problem of two shifted harmonic potentials with identical harmonic frequencies in the absence of electronic relaxation. We then consider a model three state system with electronic relaxation and show that our method is able to capture the effects of nonadiabatic excited state dynamics on the time-dependent differential absorbance spectra. Furthermore, by comparing our spectra against those spectra calculated with either an (1) inhomogenous expression, (2) ground-state Kubo theory, or (3) excited-state Kubo theory, we show that including dynamical information from both the ground and excited potential energy surfaces significantly improves the reliability of the semiclassical approximations. As such, our surface hopping method should find immediate use in modeling the time-dependent differential abosrbance spectra of ultrafast pump-probe experiments.

  16. Combined Quantum Chemical/Raman Spectroscopic Analyses of Li+ Cation Solvation: Cyclic Carbonate Solvents - Ethylene Carbonate and Propylene Earbonate

    SciTech Connect (OSTI)

    Allen, Joshua L.; Borodin, Oleg; Seo, D. M.; Henderson, Wesley A.

    2014-12-01

    Combined computational/Raman spectroscopic analyses of ethylene carbonate (EC) and propylene carbonate (PC) solvation interactions with lithium salts are reported. It is proposed that previously reported Raman analyses of (EC)n-LiX mixtures have utilized faulty assumptions. In the present studies, density functional theory (DFT) calculations have provided corrections in terms of both the scaling factors for the solvent's Raman band intensity variations and information about band overlap. By accounting for these factors, the solvation numbers obtained from two different EC solvent bands are in excellent agreement with one another. The same analysis for PC, however, was found to be quite challenging. Commercially available PC is a racemic mixture of (S)- and (R)-PC isomers. Based upon the quantum chemistry calculations, each of these solvent isomers may exist as multiple conformers due to a low energy barrier for ring inversion, making deconvolution of the Raman bands daunting and inherently prone to significant error. Thus, Raman spectroscopy is able to accurately determine the extent of the EC...Li+ cation solvation interactions using the provided methodology, but a similar analysis of PC...Li+ cation solvation results in a significant underestimation of the actual solvation numbers.

  17. The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Focus The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into Focus Print Studying the world of the ultrasmall and the ultrafast is at the frontier of scientific research. Two x-ray approaches can be used for ultrafast examinations. The first entails developing sources that have short x-ray pulses such as free-electron lasers and slicing sources, which will provide the ultrafast temporal information. The other approach is to develop a detector that is fast enough to resolve

  18. The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Focus The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into Focus Print Studying the world of the ultrasmall and the ultrafast is at the frontier of scientific research. Two x-ray approaches can be used for ultrafast examinations. The first entails developing sources that have short x-ray pulses such as free-electron lasers and slicing sources, which will provide the ultrafast temporal information. The other approach is to develop a detector that is fast enough to resolve

  19. The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Focus The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into Focus Print Studying the world of the ultrasmall and the ultrafast is at the frontier of scientific research. Two x-ray approaches can be used for ultrafast examinations. The first entails developing sources that have short x-ray pulses such as free-electron lasers and slicing sources, which will provide the ultrafast temporal information. The other approach is to develop a detector that is fast enough to resolve

  20. The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Focus The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into Focus The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into Focus Print Wednesday, 26 March 2008 00:00 Studying the world of the ultrasmall and the ultrafast is at the frontier of scientific research. Two x-ray approaches can be used for ultrafast examinations. The first entails developing sources that have short x-ray pulses such as free-electron lasers and slicing sources, which will provide the

  1. Ultrafast X-ray Phase-Enhanced Microimaging for Visualizing Fuel...

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Fuel Injection Process and Diesel Sprays Ultrafast X-ray Phase-Enhanced Microimaging for Visualizing Fuel Injection Process and Diesel Sprays 2005 Diesel Engine Emissions ...

  2. The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Focus The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into Focus Print Studying the world of the ultrasmall and the ultrafast is at the frontier of scientific research. Two x-ray approaches can be used for ultrafast examinations. The first entails developing sources that have short x-ray pulses such as free-electron lasers and slicing sources, which will provide the ultrafast temporal information. The other approach is to develop a detector that is fast enough to resolve

  3. The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Focus The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into Focus Print Studying the world of the ultrasmall and the ultrafast is at the frontier of scientific research. Two x-ray approaches can be used for ultrafast examinations. The first entails developing sources that have short x-ray pulses such as free-electron lasers and slicing sources, which will provide the ultrafast temporal information. The other approach is to develop a detector that is fast enough to resolve

  4. Surface Protonation at the Rutile (110) Interface: Explicit Incorporation of Solvation Structure within the Refined MUSIC Model Framework

    SciTech Connect (OSTI)

    Machesky, Michael L.; Predota, M.; Wesolowski, David J

    2008-11-01

    The detailed solvation structure at the (110) surface of rutile ({alpha}-TiO{sub 2}) in contact with bulk liquid water has been obtained primarily from experimentally verified classical molecular dynamics (CMD) simulations of the ab initio-optimized surface in contact with SPC/E water. The results are used to explicitly quantify H-bonding interactions, which are then used within the refined MUSIC model framework to predict surface oxygen protonation constants. Quantum mechanical molecular dynamics (QMD) simulations in the presence of freely dissociable water molecules produced H-bond distributions around deprotonated surface oxygens very similar to those obtained by CMD with nondissociable SPC/E water, thereby confirming that the less computationally intensive CMD simulations provide accurate H-bond information. Utilizing this H-bond information within the refined MUSIC model, along with manually adjusted Ti-O surface bond lengths that are nonetheless within 0.05 {angstrom} of those obtained from static density functional theory (DFT) calculations and measured in X-ray reflectivity experiments (as well as bulk crystal values), give surface protonation constants that result in a calculated zero net proton charge pH value (pHznpc) at 25 C that agrees quantitatively with the experimentally determined value (5.4 {+-} 0.2) for a specific rutile powder dominated by the (110) crystal face. Moreover, the predicted pH{sub znpc} values agree to within 0.1 pH unit with those measured at all temperatures between 10 and 250 C. A slightly smaller manual adjustment of the DFT-derived Ti-O surface bond lengths was sufficient to bring the predicted pH{sub znpc} value of the rutile (110) surface at 25 C into quantitative agreement with the experimental value (4.8 {+-} 0.3) obtained from a polished and annealed rutile (110) single crystal surface in contact with dilute sodium nitrate solutions using second harmonic generation (SHG) intensity measurements as a function of ionic

  5. Development and application of QM/MM methods to study the solvation effects and surfaces

    SciTech Connect (OSTI)

    Dibya, Pooja Arora

    2010-05-16

    Quantum mechanical (QM) calculations have the advantage of attaining high-level accuracy, however QM calculations become computationally inefficient as the size of the system grows. Solving complex molecular problems on large systems and ensembles by using quantum mechanics still poses a challenge in terms of the computational cost. Methods that are based on classical mechanics are an inexpensive alternative, but they lack accuracy. A good trade off between accuracy and efficiency is achieved by combining QM methods with molecular mechanics (MM) methods to use the robustness of the QM methods in terms of accuracy and the MM methods to minimize the computational cost. Two types of QM combined with MM (QM/MM) methods are the main focus of the present dissertation: the application and development of QM/MM methods for solvation studies and reactions on the Si(100) surface. The solvation studies were performed using a discreet solvation model that is largely based on first principles called the effective fragment potential method (EFP). The main idea of combining the EFP method with quantum mechanics is to accurately treat the solute-solvent and solvent-solvent interactions, such as electrostatic, polarization, dispersion and charge transfer, that are important in correctly calculating solvent effects on systems of interest. A second QM/MM method called SIMOMM (surface integrated molecular orbital molecular mechanics) is a hybrid QM/MM embedded cluster model that mimics the real surface.3 This method was employed to calculate the potential energy surfaces for reactions of atomic O on the Si(100) surface. The hybrid QM/MM method is a computationally inexpensive approach for studying reactions on larger surfaces in a reasonably accurate and efficient manner. This thesis is comprised of four chapters: Chapter 1 describes the general overview and motivation of the dissertation and gives a broad background of the computational methods that have been employed in this work

  6. Ultrafast electron transport across nano gaps in nanowire circuits

    SciTech Connect (OSTI)

    Potma, Eric O.

    2015-07-31

    In this Program we aim for a closer look at electron transfer through single molecules. To achieve this, we use ultrafast laser pulses to time stamp an electron tunneling event in a molecule that is connected between two metallic electrodes, while reading out the electron current. A key aspect of this project is the use of metallic substrates with plasmonic activity to efficiently manipulate the tunneling probability. The first Phase of this program is concerned with developing highly sensitive tools for the ultrafast optical manipulation of tethered molecules through the evanescent surface field of plasmonic substrates. The second Phase of the program aims to use these tools for exercising control over the electron tunneling probability.

  7. Ultrafast Nanoplasmonics: Toward Coherently Controlled Chemistry at the

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Time-space Limit | MIT-Harvard Center for Excitonics Ultrafast Nanoplasmonics: Toward Coherently Controlled Chemistry at the Time-space Limit November 3, 2015 at 4:30 PM/ RLE Allen 36-462* Tamar Seideman Department of Chemistry, Northwestern University, Illinois seideman Electronics has long reached the molecular scale; not only do single-molecule junctions exhibit interesting conduction behaviors that have no analog in macroscopic electronics, they can also be tailored to induce a variety

  8. New 'Molecular Movie' Reveals Ultrafast Chemistry in Motion

    SciTech Connect (OSTI)

    Minitti, Michael

    2015-06-22

    Scientists for the first time tracked ultrafast structural changes, captured in quadrillionths-of-a-second steps, as ring-shaped gas molecules burst open and unraveled. Ring-shaped molecules are abundant in biochemistry and also form the basis for many drug compounds. The study points the way to a wide range of real-time X-ray studies of gas-based chemical reactions that are vital to biological processes.

  9. Ultrafast Time-Resolved Electron Diffraction with Megavolt Electron Beams

    SciTech Connect (OSTI)

    Hastings, J.B.; Rudakov, F.M.; Dowell, D.H.; Schmerge, J.F.; Cardoza, J.D.; Castro, J.M.; Gierman, S.M.; Loos, H.; Weber, P.M.; /Brown U.

    2006-10-24

    An rf photocathode electron gun is used as an electron source for ultrafast time-resolved pump-probe electron diffraction. We observed single-shot diffraction patterns from a 160 nm Al foil using the 5.4 MeV electron beam from the Gun Test Facility at the Stanford Linear Accelerator. Excellent agreement with simulations suggests that single-shot diffraction experiments with a time resolution approaching 100 fs are possible.

  10. Ultrafast kinetics subsequent to shock in an unreacted, oxygen balanced

    Office of Scientific and Technical Information (OSTI)

    mixture of nitromethane and hydrogen peroxide (Conference) | SciTech Connect kinetics subsequent to shock in an unreacted, oxygen balanced mixture of nitromethane and hydrogen peroxide Citation Details In-Document Search Title: Ultrafast kinetics subsequent to shock in an unreacted, oxygen balanced mixture of nitromethane and hydrogen peroxide Authors: Armstrong, M R ; Zaug, J M ; Grant, C D ; Crowhurst, J C ; Bastea, S Publication Date: 2014-06-24 OSTI Identifier: 1149544 Report Number(s):

  11. Advanced Instrumentation for Ultrafast Science at the LCLS

    SciTech Connect (OSTI)

    Berrah, Nora

    2015-10-13

    This grant supported a Single Investigator and Small Group Research (SISGR) application to enable multi-user research in Ultrafast Science using the Linac Coherent Light Source (LCLS), the world’s first hard x-ray free electron laser (FEL) which lased for the first time at 1.5 Å on April 20, 2009. The goal of our proposal was to enable a New Era of Science by requesting funds to purchase and build Advanced Instrumentation for Ultrafast Science (AIUS), to utilize the intense, short x-ray pulses produced by the LCLS. The proposed instrumentation will allow peer review selected users to probe the ultrasmall and capture the ultrafast. These tools will expand on the investment already made in the construction of the light source and its instrumentation in both the LCLS and LUSI projects. The AIUS will provide researchers in the AMO, Chemical, Biological and Condensed Matter communities with greater flexibility in defining their scientific agenda at the LCLS. The proposed instrumentation will complement and significantly augment the present AMO instrument (funded through the LCLS project) through detectors and capabilities not included in the initial suite of instrumentation at the facility. We have built all of the instrumentations and they have been utilized by scientists. Please see report attached.

  12. Final Progress Report for Linking Ion Solvation and Lithium Battery Electrolyte Properties

    SciTech Connect (OSTI)

    Henderson, Wesley

    2014-08-29

    The research objective of this proposal was to provide a detailed analysis of how solvent and anion structure govern the solvation state of Li+ cations in solvent-LiX mixtures and how this, in turn, dictates the electrolyte physicochemical and electrochemical properties which govern (in part) battery performance. Lithium battery electrolytes remain a poorly understood and hardly studied topic relative to the research devoted to battery electrodes. This is due to the fact that it is the electrodes which determine the energy (capacity) of the battery. The electrolyte, however, plays a crucial role in the practical energy density, power, low and/or high temperature performance, lifetime, safety, etc. which is achievable. The development within this project of a "looking glass" into the molecular interactions (i.e., solution structure) in bulk electrolytes through a synergistic experimental approach involving three research thrusts complements work by other researchers to optimize multi-solvent electrolytes and efforts to understand/control the electrode-electrolyte interfaces, thereby enabling the rational design of electrolytes for a wide variety of battery chemistries and applications (electrolytes-on-demand). The three research thrusts pursued include: (1) conduction of an in-depth analysis of the thermal phase behavior of diverse solvent-LiX mixtures, (2) exploration of the ionic association/solvate formation behavior of select LiX salts with a wide variety of solvents, and (3) linking structure to properties-determination of electrolyte physicochemical and electrochemical properties for comparison with the ionic association and phase behavior.

  13. Ultrafast Chemistry under Nonequilibrium Conditions and the Shock to Deflagration Transition at the Nanoscale

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Wood, Mitchell A.; Cherukara, Mathew J.; Kober, Edward M.; Strachan, Alejandro

    2015-06-13

    We use molecular dynamics simulations to describe the chemical reactions following shock-induced collapse of cylindrical pores in the high-energy density material RDX. For shocks with particle velocities of 2 km/s we find that the collapse of a 40 nm diameter pore leads to a deflagration wave. Molecular collisions during the collapse lead to ultrafast, multistep chemical reactions that occur under nonequilibrium conditions. WE found that exothermic products formed during these first few picoseconds prevent the nanoscale hotspot from quenching. Within 30 ps, a local deflagration wave develops. It propagates at 0.25 km/s and consists of an ultrathin reaction zone ofmore » only ~5 nm, thus involving large temperature and composition gradients. Contrary to the assumptions in current models, a static thermal hotspot matching the dynamical one in size and thermodynamic conditions fails to produce a deflagration wave indicating the importance of nonequilibrium loading in the criticality of nanoscale hot spots. These results provide insight into the initiation of reactive decomposition.« less

  14. Ultrafast Chemistry under Nonequilibrium Conditions and the Shock to Deflagration Transition at the Nanoscale

    SciTech Connect (OSTI)

    Wood, Mitchell A.; Cherukara, Mathew J.; Kober, Edward M.; Strachan, Alejandro

    2015-06-13

    We use molecular dynamics simulations to describe the chemical reactions following shock-induced collapse of cylindrical pores in the high-energy density material RDX. For shocks with particle velocities of 2 km/s we find that the collapse of a 40 nm diameter pore leads to a deflagration wave. Molecular collisions during the collapse lead to ultrafast, multistep chemical reactions that occur under nonequilibrium conditions. WE found that exothermic products formed during these first few picoseconds prevent the nanoscale hotspot from quenching. Within 30 ps, a local deflagration wave develops. It propagates at 0.25 km/s and consists of an ultrathin reaction zone of only ~5 nm, thus involving large temperature and composition gradients. Contrary to the assumptions in current models, a static thermal hotspot matching the dynamical one in size and thermodynamic conditions fails to produce a deflagration wave indicating the importance of nonequilibrium loading in the criticality of nanoscale hot spots. These results provide insight into the initiation of reactive decomposition.

  15. Ultrafast recovery time and broadband saturable absorption properties of black phosphorus suspension

    SciTech Connect (OSTI)

    Wang, Yingwei; Huang, Guanghui; Chen, Jiazhang; Xiao, Si He, Jun; Mu, Haoran; Bao, Qiaoliang; Lin, Shenghuang

    2015-08-31

    As a new type of two-dimensional crystal material, black phosphorus (BP) exhibits excellent electronics and optical performance. Herein, we focus on carrier relaxation dynamics and nonlinear optical properties of BP suspension. Atomic force microscopy, transmission electron microscopy, and optical transmission spectrum are employed to characterize the structure and linear optical properties of the BP. Additionally, pump-probe experiments at wavelength of 1550 nm were carried out to study the carrier dynamics in BP suspension, and ultrafast recovery time was observed (τ{sub s} = 24 ± 2 fs). Furthermore, we demonstrate the saturable absorption signals by open aperture Z-scan experiments at wavelengths of 1550 nm, 532 nm, and 680 nm. The results indicate that BP has broadband saturable absorption properties and the nonlinear absorption coefficients were determined to be β{sub 2} = −0.20 ± 0.08 × 10{sup −3 }cm/GW (532 nm), β{sub 2} = −0.12 ± 0.05 × 10{sup −3 }cm/GW (680 nm), and β{sub 2} = −0.15 ± 0.09 × 10{sup −3 }cm/GW (1550 nm)

  16. Quantum chemical approach for condensed-phase thermochemistry: Proposal of a harmonic solvation model

    SciTech Connect (OSTI)

    Nakai, Hiromi; Ishikawa, Atsushi

    2014-11-07

    We propose a novel quantum chemical method, called the harmonic solvation model (HSM), for calculating thermochemical parameters in the condensed phase, particularly in the liquid phase. The HSM represents translational and rotational motions of a solute as vibrations interacting with a cavity wall of solvent molecules. As examples, the HSM and the ideal-gas model (IGM) were used for the standard formation reaction of liquid water, combustion reactions of liquid formic acid, methanol, and ethanol, vapor–liquid equilibration of water and ethanol, and dissolution of gaseous CO{sub 2} in water. The numerical results confirmed the reliability and applicability of the HSM. In particular, the temperature dependence of the Gibbs energy of liquid molecules was accurately reproduced by the HSM; for example, the boiling point of water was reasonably determined using the HSM, whereas the conventional IGM treatment failed to obtain a crossing of the two Gibbs energy curves for gaseous and liquid water.

  17. Rise time measurement for ultrafast X-ray pulses

    DOE Patents [OSTI]

    Celliers, Peter M.; Weber, Franz A.; Moon, Stephen J.

    2005-04-05

    A pump-probe scheme measures the rise time of ultrafast x-ray pulses. Conventional high speed x-ray diagnostics (x-ray streak cameras, PIN diodes, diamond PCD devices) do not provide sufficient time resolution to resolve rise times of x-ray pulses on the order of 50 fs or less as they are being produced by modern fast x-ray sources. Here, we are describing a pump-probe technique that can be employed to measure events where detector resolution is insufficient to resolve the event. The scheme utilizes a diamond plate as an x-ray transducer and a p-polarized probe beam.

  18. Rise Time Measurement for Ultrafast X-Ray Pulses

    DOE Patents [OSTI]

    Celliers, Peter M.; Weber, Franz A.; Moon, Stephen J.

    2005-04-05

    A pump-probe scheme measures the rise time of ultrafast x-ray pulses. Conventional high speed x-ray diagnostics (x-ray streak cameras, PIN diodes, diamond PCD devices) do not provide sufficient time resolution to resolve rise times of x-ray pulses on the order of 50 fs or less as they are being produced by modern fast x-ray sources. Here, we are describing a pump-probe technique that can be employed to measure events where detector resolution is insufficient to resolve the event. The scheme utilizes a diamond plate as an x-ray transducer and a p-polarized probe beam.

  19. Ultrafast pulsed laser utilizing broad bandwidth laser glass

    DOE Patents [OSTI]

    Payne, S.A.; Hayden, J.S.

    1997-09-02

    An ultrafast laser uses a Nd-doped phosphate laser glass characterized by a particularly broad emission bandwidth to generate the shortest possible output pulses. The laser glass is composed primarily of P{sub 2}O{sub 5}, Al{sub 2}O{sub 3} and MgO, and possesses physical and thermal properties that are compatible with standard melting and manufacturing methods. The broad bandwidth laser glass can be used in modelocked oscillators as well as in amplifier modules. 7 figs.

  20. Ultrafast pulsed laser utilizing broad bandwidth laser glass

    DOE Patents [OSTI]

    Payne, Stephen A.; Hayden, Joseph S.

    1997-01-01

    An ultrafast laser uses a Nd-doped phosphate laser glass characterized by a particularly broad emission bandwidth to generate the shortest possible output pulses. The laser glass is composed primarily of P.sub.2 O.sub.5, Al.sub.2 O.sub.3 and MgO, and possesses physical and thermal properties that are compatible with standard melting and manufacturing methods. The broad bandwidth laser glass can be used in modelocked oscillators as well as in amplifier modules.

  1. Driving magnetic order in a manganite by ultrafast lattice excitation.

    SciTech Connect (OSTI)

    Forst, M.; Tobey, R. I.; Wall, S.; Bromberger, H.; Khanna, V.; Cavalieri, A. L.; Chuang, Y.-D.; Lee, W. S.; Moore, R.; Schlotter, W. F.; Turner, J. J.; Krupin, O.; Trigo, M.; Zheng, H.; Mitchell, J. F.; Dhesi, S. S.; Hill, J. P.; Cavalleri, A.

    2011-01-01

    Femtosecond midinfrared pulses are used to directly excite the lattice of the single-layer manganite La{sub 0.5}Sr{sub 1.5}MnO{sub 4}. Magnetic and orbital orders, as measured by femtosecond resonant soft x-ray diffraction with an x-ray free-electron laser, are reduced within a few picoseconds. This effect is interpreted as a displacive exchange quench, a prompt shift in the equilibrium value of the magnetic- and orbital-order parameters after the lattice has been distorted. Control of magnetism through ultrafast lattice excitation may be of use for high-speed optomagnetism.

  2. Ultrafast laser control of backward superfluorescence towards standoff sensing

    SciTech Connect (OSTI)

    Ariunbold, Gombojav O.; Sautenkov, Vladimir A.; Rostovtsev, Yuri V.; Scully, Marlan O.

    2014-01-13

    We study infrared backward cooperative emission in a rubidium vapor induced by ultrafast two-photon optical excitations. The laser coherent control of the backward emission is demonstrated by using a pair of 100 fs pulses with a variable time delay. The temporal variation (quantum beat) of the backward beam intensity due to interference of atomic transitions in the rubidium atomic level system 5S-5P-5D is produced and controlled. Based on the obtained experimental results, we discuss possible applications of the developed approach for creation of an effective “guide star” in the sodium atomic layer in the upper atmosphere (mesosphere)

  3. Ultrafast terahertz Faraday rotation in graphene

    SciTech Connect (OSTI)

    Heyman, J. N.; Foo Kune, R. F.; Alebachew, B. A.; Nguyen, M. D.; Robinson, J. T.

    2014-12-07

    Terahertz (THz) Faraday rotation measurements were performed to investigate carrier dynamics in p-type Chemical vapor deposition (CVD) graphene. We used static and time-resolved polarization-sensitive THz transmission measurements in a magnetic field to probe free carriers in GaAs, InP, and Graphene. Static measurements probe the equilibrium carrier density and momentum scattering rate. Time-resolved (optical pump/THz probe) measurements probe the change in these quantities following photoexcitation. In a typical CVD graphene sample, we found that 0.5 ps following photoexcitation with 1 × 10{sup 13} photons/cm{sup 2} pulses at 800 nm the effective hole scattering time decreased from 37 fs to 34.5 fs, while the carrier concentration increased from 2.0 × 10{sup 12} cm{sup −2} to 2.04 × 10{sup 12} cm{sup −2}, leading to a transient decrease in the conductivity of the film.

  4. Ultrafast pulse radiolysis using a terawatt laser wakefield accelerator

    SciTech Connect (OSTI)

    Oulianov, Dmitri A.; Crowell, Robert A.; Gosztola, David J.; Shkrob, Ilya A.; Korovyanko, Oleg J.; Rey-de-Castro, Roberto C.

    2007-03-01

    We report ultrafast pulse radiolysis transient absorption (TA) spectroscopy measurements from the Terawatt Ultrafast High Field Facility (TUHFF) at Argonne National Laboratory. TUHFF houses a 20 TW Ti:sapphire laser system that generates 2.5 nC subpicosecond pulses of multi-mega-electron-volt electrons at 10 Hz using laser wakefield acceleration. The system has been specifically optimized for kinetic TA measurements in a pump-probe fashion. This requires averaging over many shots which necessitates stable, reliable generation of electron pulses. The latter were used to generate excess electrons in pulse radiolysis of liquid water and concentrated solutions of perchloric acid. The hydronium ions in the acidic solutions react with the hydrated electrons resulting in the rapid decay of the transient absorbance at 800 nm on the picosecond time scale. Normalization of the TA signal leads to an improvement in the signal to noise ratio by a factor of 5 to 6. Due the pointing instability of the laser this improvement was limited to a 5 to 10 min acquisition period, requiring periodic recalibration and realignment. Time resolution, defined by the rise time of TA signal from hydrated electron in pulse radiolysis of liquid water, of a few picoseconds, has been demonstrated. The current time resolution is determined primarily by the physical dimensions of the sample and the detection sensitivity. Subpicosecond time resolution can be achieved by using thinner samples, more sensitive detection techniques, and improved electron beam quality.

  5. Quantum Hooke's Law to classify pulse laser induced ultrafast melting

    SciTech Connect (OSTI)

    Hu, Hao; Ding, Hepeng; Liu, Feng

    2015-02-03

    Ultrafast crystal-to-liquid phase transition induced by femtosecond pulse laser excitation is an interesting material's behavior manifesting the complexity of light-matter interaction. There exist two types of such phase transitions: one occurs at a time scale shorter than a picosecond via a nonthermal process mediated by electron-hole plasma formation; the other at a longer time scale via a thermal melting process mediated by electron-phonon interaction. However, it remains unclear what material would undergo which process and why? Here, by exploiting the property of quantum electronic stress (QES) governed by quantum Hooke's law, we classify the transitions by two distinct classes of materials: the faster nonthermal process can only occur in materials like ice having an anomalous phase diagram characterized with dTm/dP < 0, where Tm is the melting temperature and P is pressure, above a high threshold laser fluence; while the slower thermal process may occur in all materials. Especially, the nonthermal transition is shown to be induced by the QES, acting like a negative internal pressure, which drives the crystal into a super pressing state to spontaneously transform into a higher-density liquid phase. Our findings significantly advance fundamental understanding of ultrafast crystal-to-liquid phase transitions, enabling quantitative a priori predictions.

  6. Quantum Hooke's Law to classify pulse laser induced ultrafast melting

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Hu, Hao; Ding, Hepeng; Liu, Feng

    2015-02-03

    Ultrafast crystal-to-liquid phase transition induced by femtosecond pulse laser excitation is an interesting material's behavior manifesting the complexity of light-matter interaction. There exist two types of such phase transitions: one occurs at a time scale shorter than a picosecond via a nonthermal process mediated by electron-hole plasma formation; the other at a longer time scale via a thermal melting process mediated by electron-phonon interaction. However, it remains unclear what material would undergo which process and why? Here, by exploiting the property of quantum electronic stress (QES) governed by quantum Hooke's law, we classify the transitions by two distinct classes ofmore » materials: the faster nonthermal process can only occur in materials like ice having an anomalous phase diagram characterized with dTm/dP < 0, where Tm is the melting temperature and P is pressure, above a high threshold laser fluence; while the slower thermal process may occur in all materials. Especially, the nonthermal transition is shown to be induced by the QES, acting like a negative internal pressure, which drives the crystal into a “super pressing” state to spontaneously transform into a higher-density liquid phase. Our findings significantly advance fundamental understanding of ultrafast crystal-to-liquid phase transitions, enabling quantitative a priori predictions.« less

  7. UPGRADING METHANE USING ULTRA-FAST THERMAL SWING ADSORPTION

    SciTech Connect (OSTI)

    Anna Lee Tonkovich

    2004-01-01

    The purpose of this project is to design and demonstrate an approach to upgrade low-BTU methane streams from coal mines to pipeline-quality natural gas. The objective of Phase I of the project was to assess the feasibility of upgrading low-Btu methane streams using ultra-fast thermal swing adsorption (TSA) using Velocys' modular microchannel process technology. The project is on schedule and under budget. For Task 1.1, the open literature, patent information, and vendor contacts were surveyed to identify adsorbent candidates for experimental validation and subsequent demonstration in an MPT-based ultra-fast TSA separation for methane upgrading. The leading candidates for preferential adsorption of methane over nitrogen are highly microporous carbons. A Molecular Gate{trademark} zeolite from Engelhard Corporation has emerged as a candidate. For Task 1.2, experimental evaluation of adsorbents was initiated, and data were collected on carbon (MGN-101) from PICA, Inc. This carbon demonstrated a preferential capacity for methane over nitrogen, as well as a reasonable thermal swing differential capacity for a 90% methane and 10% nitrogen mixture. A similar methane swing capacity at 2 psig was measured. The mixture composition is relevant because gob gas contains nearly 85% methane and must be purified to 97% methane for pipeline quality.

  8. High-Energy and Ultrafast X-Ray Imaging Technologies and Applications

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    MaRIE High-energy and Ultrafast X-Ray Imaging Technologies and Applications Date : August 2-3, 2016 Hotel venue: Hilton Santa Fe at Buffalo Thunder The goal of this workshop is to gather leading experts in the fields related to ultrafast high-energy photon imaging and prioritize the path forward for ultrafast hard x-ray imaging technology development, identify important applications in the next 5-10 years, and establish foundations for near-term R&D collaboration. This workshop is one in a

  9. High-energy and Ultrafast X-Ray Imaging Technologies and Applications

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    August » High-energy and Ultrafast X-Ray Imaging Technologies and Applications High-energy and Ultrafast X-Ray Imaging Technologies and Applications WHEN: Aug 02, 2016 8:00 AM - Aug 03, 2016 5:00 PM WHERE: Hilton Santa Fe at Buffalo Thunder CONTACT: Zhehui (Jeff) Wang (505) 665-5353 CATEGORY: Community Science TYPE: Conference INTERNAL: Calendar Login Event Description The goal of this workshop is to gather leading experts in the fields related to ultrafast high-energy photon imaging and

  10. Dynamic Transmission Electron Microscopy

    SciTech Connect (OSTI)

    Evans, James E.; Jungjohann, K. L.; Browning, Nigel D.

    2012-10-12

    Dynamic transmission electron microscopy (DTEM) combines the benefits of high spatial resolution electron microscopy with the high temporal resolution of ultrafast lasers. The incorporation of these two components into a single instrument provides a perfect platform for in situ observations of material processes. However, previous DTEM applications have focused on observing structural changes occurring in samples exposed to high vacuum. Therefore, in order to expand the pump-probe experimental regime to more natural environmental conditions, in situ gas and liquid chambers must be coupled with Dynamic TEM. This chapter describes the current and future applications of in situ liquid DTEM to permit time-resolved atomic scale observations in an aqueous environment, Although this chapter focuses mostly on in situ liquid imaging, the same research potential exists for in situ gas experiments and the successful integration of these techniques promises new insights for understanding nanoparticle, catalyst and biological protein dynamics with unprecedented spatiotemporal resolution.

  11. The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    The first entails developing sources that have short x-ray pulses such as free-electron lasers and slicing sources, which will provide the ultrafast temporal information. The other ...

  12. Ultrafast spin exchange-coupling torque via photo-excited charge...

    Office of Scientific and Technical Information (OSTI)

    Title: Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes In this study, optical control of spin is of central importance in the research of ...

  13. Ultrafast Terahertz-Induced Response of GeSbTe Phase-Change Materials...

    Office of Scientific and Technical Information (OSTI)

    Title: Ultrafast Terahertz-Induced Response of GeSbTe Phase-Change Materials ... Resource Relation: Journal Name: Appl. Phys. Lett.; Journal Volume: 104; Journal Issue: 25 Research ...

  14. Ultrafast Probes for Dirac Materials (Technical Report) | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    Technical Report: Ultrafast Probes for Dirac Materials Citation Details In-Document Search Title: Ultrafast Probes for Dirac Materials Authors: Yarotski, Dmitry Anatolievitch [1] + Show Author Affiliations Los Alamos National Laboratory Publication Date: 2015-03-12 OSTI Identifier: 1172825 Report Number(s): LA-UR-15-21802 DOE Contract Number: AC52-06NA25396 Resource Type: Technical Report Research Org: Los Alamos National Laboratory (LANL) Sponsoring Org: UCRP Country of Publication: United

  15. Ultrafast Terahertz-Induced Response of GeSbTe Phase-Change Materials

    Office of Scientific and Technical Information (OSTI)

    (Journal Article) | SciTech Connect Journal Article: Ultrafast Terahertz-Induced Response of GeSbTe Phase-Change Materials Citation Details In-Document Search Title: Ultrafast Terahertz-Induced Response of GeSbTe Phase-Change Materials Authors: Shu, Michael J. ; Zalden, Peter ; Chen, Frank ; Weems, Ben ; Chatzakis, Ioannis ; Xiong, Feng ; Jeyasingh, Rakesh ; Hoffmann, Matthias C. ; Pop, Eric ; Wong, H.-S.Philip ; Wuttig, Matthias ; Lindenberg, Aaron M. Publication Date: 2014-07-08 OSTI

  16. Ultrafast X-ray Phase-Enhanced Microimaging for Visualizing Fuel Injection

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Process and Diesel Sprays | Department of Energy Ultrafast X-ray Phase-Enhanced Microimaging for Visualizing Fuel Injection Process and Diesel Sprays Ultrafast X-ray Phase-Enhanced Microimaging for Visualizing Fuel Injection Process and Diesel Sprays 2005 Diesel Engine Emissions Reduction (DEER) Conference Presentations and Posters 2005_deer_wang.pdf (980 KB) More Documents & Publications Fuel Injection and Spray Research Using X-Ray Diagnostics Fuel Injection and Spray Research Using

  17. Ultrafast transient grating radiation to optical image converter

    DOE Patents [OSTI]

    Stewart, Richard E; Vernon, Stephen P; Steel, Paul T; Lowry, Mark E

    2014-11-04

    A high sensitivity transient grating ultrafast radiation to optical image converter is based on a fixed transmission grating adjacent to a semiconductor substrate. X-rays or optical radiation passing through the fixed transmission grating is thereby modulated and produces a small periodic variation of refractive index or transient grating in the semiconductor through carrier induced refractive index shifts. An optical or infrared probe beam tuned just below the semiconductor band gap is reflected off a high reflectivity mirror on the semiconductor so that it double passes therethrough and interacts with the radiation induced phase grating therein. A small portion of the optical beam is diffracted out of the probe beam by the radiation induced transient grating to become the converted signal that is imaged onto a detector.

  18. Ultrafast laser diagnostics to investigate initiation fundamentals in energetic materials.

    SciTech Connect (OSTI)

    Farrow, Darcie; Jilek, Brook Anton; Kohl, Ian Thomas; Kearney, Sean Patrick

    2013-08-01

    We present the results of a two year early career LDRD project, which has focused on the development of ultrafast diagnostics to measure temperature, pressure and chemical change during the shock initiation of energetic materials. We compare two single-shot versions of femtosecond rotational CARS to measure nitrogen temperature: chirped-probe-pulse and ps/fs hybrid CARS thermometry. The applicability of measurements to the combustion of energetic materials will be discussed. We have also demonstrated laser shock and particle velocity measurements in thin film explosives using stretched femtosecond laser pulses. We will discuss preliminary results from Al and PETN thin films. Agreement between our results and previous work will be discussed.

  19. Ultrafast stimulated Raman parallel adiabatic passage by shaped pulses

    SciTech Connect (OSTI)

    Dridi, G.; Guerin, S.; Hakobyan, V.; Jauslin, H. R.; Eleuch, H.

    2009-10-15

    We present a general and versatile technique of population transfer based on parallel adiabatic passage by femtosecond shaped pulses. Their amplitude and phase are specifically designed to optimize the adiabatic passage corresponding to parallel eigenvalues at all times. We show that this technique allows the robust adiabatic population transfer in a Raman system with the total pulse area as low as 3{pi}, corresponding to a fluence of one order of magnitude below the conventional stimulated Raman adiabatic passage process. This process of short duration, typically picosecond and subpicosecond, is easily implementable with the modern pulse shaper technology and opens the possibility of ultrafast robust population transfer with interesting applications in quantum information processing.

  20. Ultrafast electron diffraction with megahertz MeV electron pulses from a superconducting radio-frequency photoinjector

    SciTech Connect (OSTI)

    Feng, L. W.; Lin, L.; Huang, S. L.; Quan, S. W.; Hao, J. K.; Zhu, F.; Wang, F.; Liu, K. X.; Jiang, T.; Zhu, P. F.; Fu, F.; Wang, R.; Zhao, L.; Xiang, D.

    2015-11-30

    We report ultrafast relativistic electron diffraction operating at the megahertz repetition rate where the electron beam is produced in a superconducting radio-frequency (rf) photoinjector. We show that the beam quality is sufficiently high to provide clear diffraction patterns from gold and aluminium samples. With the number of electrons, several orders of magnitude higher than that from a normal conducting photocathode rf gun, such high repetition rate ultrafast MeV electron diffraction may open up many new opportunities in ultrafast science.

  1. Mixed direct-iterative methods for boundary integral formulations of continuum dielectric solvation models

    SciTech Connect (OSTI)

    Corcelli, S.A.; Kress, J.D.; Pratt, L.R.

    1995-08-07

    This paper develops and characterizes mixed direct-iterative methods for boundary integral formulations of continuum dielectric solvation models. We give an example, the Ca{sup ++}{hor_ellipsis}Cl{sup {minus}} pair potential of mean force in aqueous solution, for which a direct solution at thermal accuracy is difficult and, thus for which mixed direct-iterative methods seem necessary to obtain the required high resolution. For the simplest such formulations, Gauss-Seidel iteration diverges in rare cases. This difficulty is analyzed by obtaining the eigenvalues and the spectral radius of the non-symmetric iteration matrix. This establishes that those divergences are due to inaccuracies of the asymptotic approximations used in evaluation of the matrix elements corresponding to accidental close encounters of boundary elements on different atomic spheres. The spectral radii are then greater than one for those diverging cases. This problem is cured by checking for boundary element pairs closer than the typical spatial extent of the boundary elements and for those cases performing an ``in-line`` Monte Carlo integration to evaluate the required matrix elements. These difficulties are not expected and have not been observed for the thoroughly coarsened equations obtained when only a direct solution is sought. Finally, we give an example application of hybrid quantum-classical methods to deprotonation of orthosilicic acid in water.

  2. Solvate Structures and Computational/Spectroscopic Characterization of LiBF4 Electrolytes

    SciTech Connect (OSTI)

    Seo, D. M.; Boyle, Paul D.; Allen, Joshua L.; Han, Sang D.; Jonsson, Erlendur; Johansson, Patrik; Henderson, Wesley A.

    2014-07-21

    Crystal structures have been determined for both LiBF4 and HBF4 solvates—(acetonitrile)2:LiBF4, (ethylene glycol diethyl ether)1:LiBF4, (diethylene glycol diethyl ether)1:LiBF4, (tetrahydrofuran)1:LiBF4, (methyl methoxyacetate)1:LiBF4, (suc-cinonitrile)1:LiBF4, (N,N,N',N",N"-pentamethyldiethylenetriamine)1:HBF4, (N,N,N',N'-tetramethylethylenediamine)3/2:HBF4 and (phenanthroline)2:HBF4. These, as well as other known LiBF4 solvate structures, have been characterized by Raman vibrational spectroscopy to unambiguously assign the anion Raman band positions to specific forms of BF4-...Li+ cation coordination. In addition, complementary DFT calculations of BF4-...Li+ cation complexes have provided additional insight into the challenges associated with accurately interpreting the anion interactions from experimental Raman spectra. This information provides a crucial tool for the characterization of the ionic association interactions within electrolytes.

  3. The cavity electromagnetic field within the polarizable continuum model of solvation

    SciTech Connect (OSTI)

    Pipolo, Silvio; Department of Physics, University of Modena and Reggio Emilia, Modena ; Corni, Stefano; Cammi, Roberto

    2014-04-28

    Cavity field effects can be defined as the consequences of the solvent polarization induced by the probing electromagnetic field upon spectroscopies of molecules in solution, and enter in the definitions of solute response properties. The polarizable continuum model of solvation (PCM) has been extended in the past years to address the cavity-field issue through the definition of an effective dipole moment that couples to the external electromagnetic field. We present here a rigorous derivation of such cavity-field treatment within the PCM starting from the general radiation-matter Hamiltonian within inhomogeneous dielectrics and recasting the interaction term to a dipolar form within the long wavelength approximation. To this aim we generalize the Göppert-Mayer and Power-Zienau-Woolley gauge transformations, usually applied in vacuo, to the case of a cavity vector potential. Our derivation also allows extending the cavity-field correction in the long-wavelength limit to the velocity gauge through the definition of an effective linear momentum operator. Furthermore, this work sets the basis for the general PCM treatment of the electromagnetic cavity field, capable to describe the radiation-matter interaction in dielectric media beyond the long-wavelength limit, providing also a tool to investigate spectroscopic properties of more complex systems such as molecules close to large nanoparticles.

  4. Ultrafast Multiphoton Pump-probe Photoemission Excitation Pathways in Rutile TiO2(110)

    SciTech Connect (OSTI)

    Argondizzo, Adam; Cui, Xuefeng; Wang, Cong; Sun, Huijuan; Shang, Honghui; Zhao, Jin; Petek, Hrvoje

    2015-04-27

    We investigate the spectroscopy and photoinduced electron dynamics within the conduction band of reduced rutile TiO2(110) surface by multiphoton photoemission (mPP) spectroscopy with wavelength tunable ultrafast (!20 fs) laser pulse excitation. Tuning the mPP photon excitation energy between 2.9 and 4.6 eV reveals a nearly degenerate pair of new unoccupied states located at 2.73 ± 0.05 and 2.85 ± 0.05 eV above the Fermi level, which can be analyzed through the polarization and sample azimuthal orientation dependence of the mPP spectra. Based on the calculated electronic structure and optical transition moments, as well as related spectroscopic evidence, we assign these resonances to transitions between Ti 3d bands of nominally t2g and eg symmetry, which are split by crystal field. The initial states for the optical transition are the reduced Ti3+ states of t2g symmetry populated by formation oxygen vacancy defects, which exist within the band gap of TiO2. Furthermore,we studied the electron dynamics within the conduction band of TiO2 by three-dimensional time-resolved pump-probe interferometric mPP measurements. The spectroscopic and time-resolved studies reveal competition between 2PP and 3PP processes where the t2g-eg transitions in the 2PP process saturate, and are overtaken by the 3PP process initiated by the band-gap excitation from the valence band of TiO2.

  5. Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO)5 to Fe(CO)4EtOH

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Kunnus, K.; Josefsson, I.; Rajkovic, I.; Schreck, S.; Quevedo, W.; Beye, M.; Weniger, C.; Grübel, S.; Scholz, M.; Nordlund, D.; et al

    2016-02-09

    We utilized femtosecond time-resolved resonant inelastic X-ray scattering and ab initio theory to study the transient electronic structure and the photoinduced molecular dynamics of a model metal carbonyl photocatalyst Fe(CO)5 in ethanol solution. We propose mechanistic explanation for the parallel ultrafast intra-molecular spin crossover and ligation of the Fe(CO)4 which are observed following a charge transfer photoexcitation of Fe(CO)5 as reported in our previous study [Wernet et al., Nature 520, 78 (2015)]. We find that branching of the reaction pathway likely happens in the 1A1 state of Fe(CO)4. A sub-picosecond time constant of the spin crossover from 1B2 tomore » 3B2 is rationalized by the proposed 1B2 → 1A1 → 3B2 mechanism. Ultrafast ligation of the 1B2 Fe(CO)4 state is significantly faster than the spin-forbidden and diffusion limited ligation process occurring from the 3B2 Fe(CO)4 ground state that has been observed in the previous studies. We propose that the ultrafast ligation occurs via 1B2 → 1A1 → 1A' Fe(CO)4EtOH pathway and the time scale of the 1A1 Fe(CO)4 state ligation is governed by the solute-solvent collision frequency. In conclusion, our study emphasizes the importance of understanding the interaction of molecular excited states with the surrounding environment to explain the relaxation pathways of photoexcited metal carbonyls in solution.« less

  6. Ultrafast photo-induced nuclear relaxation of a conformationally disordered conjugated polymer probed with transient absorption and femtosecond stimulated Raman spectroscopies

    SciTech Connect (OSTI)

    Yu, Wenjian; Donohoo-Vallett, Paul J.; Zhou, Jiawang; Bragg, Arthur E.

    2014-07-28

    A combination of transient absorption (TAS) and femtosecond stimulated Raman (FSRS) spectroscopies were used to interrogate the photo-induced nuclear relaxation dynamics of poly(3-cyclohexyl,4-methylthiophene) (PCMT). The large difference in inter-ring dihedral angles of ground and excited-state PCMT make it an ideal candidate for studying large-amplitude vibrational relaxation associated with exciton trapping. Spectral shifting in the S{sub 1} TA spectra on sub-ps timescales (110 ± 20 and 800 ± 100 fs) is similar to spectroscopic signatures of excited-state relaxation observed with related photoexcited conjugated polymers and which have been attributed to exciton localization and a combination of resonant energy transfer and torsional relaxation, respectively. Measurements made with both techniques reveal fast PCMT S{sub 1} decay and triplet formation (τ{sub S1} = 25–32 ps), which is similar to the excited-state dynamics of short oligothiophenes and highly twisted polyconjugated molecules. On ultrafast timescales FSRS of S{sub 1} PCMT offers a new perspective on the nuclear dynamics that underlie localization of excitons in photoexcited conjugated polymers: Spectral dynamics in the C=C stretching region (1400–1600 cm{sup −1}) include a red-shift of the in-phase C=C stretching frequency, as well as a change in the relative intensity of in-phase and out-of-phase stretch intensities on a timescale of ∼100 fs. Both changes indicate an ultrafast vibrational distortion that increases the conjugation length in the region of the localized excitation and are consistent with exciton self-localization or trapping. Wavelength-dependent excited-state FSRS measurements further demonstrate that the C=C stretching frequency provides a useful spectroscopic handle for interrogating the degree of delocalization in excited conjugated polymers given the selectivity achieved via resonance enhancement.

  7. Isotopically Enriched Films and Nanostructures by Ultrafast Pulsed Laser Deposition

    SciTech Connect (OSTI)

    Peter Pronko

    2004-12-13

    This project involved a systematic study to apply newly discovered isotopic enrichment effects in laser ablation plumes to the fabrication of isotopically engineered thin films, superlattices, and nanostructures. The approach to this program involved using ultrafast lasers as a method for generating ablated plasmas that have preferentially structured isotopic content in the body of the ablation plasma plumes. In examining these results we have attempted to interpret the observations in terms of a plasma centrifuge process that is driven by the internal electro-magnetic fields of the plasma itself. The research plan involved studying the following phenomena in regard to the ablation plume and the isotopic mass distribution within it: (1) Test basic equations of steady state centrifugal motion in the ablation plasma. (2) Investigate angular distribution of ions in the ablation plasmas. (3) Examine interactions of plasma ions with self-generated magnetic fields. (3) Investigate ion to neutral ratios in the ablation plasmas. (5) Test concepts of plasma pumping. (6) Fabricate isotopically enriched nanostructures.

  8. ULTRAFAST OUTFLOWS: GALAXY-SCALE ACTIVE GALACTIC NUCLEUS FEEDBACK

    SciTech Connect (OSTI)

    Wagner, A. Y.; Umemura, M.; Bicknell, G. V.

    2013-01-20

    We show, using global three-dimensional grid-based hydrodynamical simulations, that ultrafast outflows (UFOs) from active galactic nuclei (AGNs) result in considerable feedback of energy and momentum into the interstellar medium (ISM) of the host galaxy. The AGN wind interacts strongly with the inhomogeneous, two-phase ISM consisting of dense clouds embedded in a tenuous, hot, hydrostatic medium. The outflow floods through the intercloud channels, sweeps up the hot ISM, and ablates and disperses the dense clouds. The momentum of the UFO is primarily transferred to the dense clouds via the ram pressure in the channel flow, and the wind-blown bubble evolves in the energy-driven regime. Any dependence on UFO opening angle disappears after the first interaction with obstructing clouds. On kpc scales, therefore, feedback by UFOs operates similarly to feedback by relativistic AGN jets. Negative feedback is significantly stronger if clouds are distributed spherically rather than in a disk. In the latter case, the turbulent backflow of the wind drives mass inflow toward the central black hole. Considering the common occurrence of UFOs in AGNs, they are likely to be important in the cosmological feedback cycles of galaxy formation.

  9. Extension - Upgrading Methane Using Ultra-Fast Thermal Swing Adsorption

    SciTech Connect (OSTI)

    Anna Lee Tonkovich

    2008-08-11

    The need for cost effective technologies for upgrading coal mine methane to pipeline quality natural gas is becoming ever greater. The current work presents and investigates a new approach to reduce the impact of the most costly step in the conventional technology, nitrogen rejection. The proposed approach is based on the Velocys microchannel platform, which is being developed to commercialize compact and cost efficient chemical processing technology. For this separation, ultra fast thermal swing sorption is enabled by the very high rates of heat and mass transfer inherent in microchannel processing. In a first phase of the project solid adsorbents were explored. Feasibility of ultrafast thermal swing was demonstrated but the available adsorbents had insufficient differential methane capacity to achieve the required commercial economics. In a second phase, ionic liquids were adopted as absorbents of choice, and experimental work and economic analyses, performed to gauge their potential, showed promise for this novel alternative. Final conclusions suggest that a combination of a required cost target for ionic liquids or a methane capacity increase or a combination of both is required for commercialization.

  10. Coherent orbital waves during an Ultrafast Photo-induced Isulator-metal Transition in a magnetoresistive manganite

    SciTech Connect (OSTI)

    ULTRAS-INFM-CNR Dipartimento di Fisica, Politecnico di Milano, Italy; Department of Physics - Cavalleri Group, Clarendon Laboratory, University of Oxford, U.K.; Correlated Electron Research Center, Tsukuba, Japan; Schoenlein, Robert William; Polli, D.; Rini, M.; Wall, S.; Schoenlein, R.W.; Tomioka, Y.; Tokura, Y.; Cerullo, G.; Cavalleri, A.

    2007-06-01

    Photo-excitation can drive strongly correlated electron insulators into competing conducting phases1,2, resulting in giant and ultrafast changes of their electronic and magnetic properties. The underlying non-equilibrium dynamics involve many degrees of freedom at once, whereby sufficiently short optical pulses can trigger the corresponding collective modes of the solid along temporally coherent pathways. The characteristic frequencies of these modes range between the few GHz of acoustic vibrations3 to the tens or even hundreds of THz for purely electronic excitations. Virtually all experiments so far have used 100 fs or longer pulses, detecting only comparatively slow lattice dynamics4,5. Here, we use sub-10-fs optical pulses to study the photo-induced insulator-metal transition in the magneto-resistive manganite Pr0.7Ca0.3MnO3. At room temperature, we find that the time-dependent pathway towards the metallic phase is accompanied by coherent 31 THz oscillations of the optical reflectivity, significantly faster than all lattice vibrations. These high-frequency oscillations are suggestive of coherent orbital waves6,7, crystal-field excitations triggered here by impulsive stimulated Raman scattering. Orbital waves are likely to be initially localized to the small polarons of this room-temperature manganite, coupling to other degrees of freedom at longer times, as photo-domains coalesce into a metallic phase.

  11. Laser-induced short-range disorder in aluminum revealed by ultrafast electron diffuse scattering

    SciTech Connect (OSTI)

    Zhu, Pengfei; Chen, Jie; Li, Runze; Chen, Long; Cao, Jianming; Sheng, Zhengming; Zhang, Jie; Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190

    2013-12-02

    We report ultrafast electron diffuse scattering intensity (DSI) measurement in order to study the structural response of aluminum to femtosecond laser excitation. In this measurement, the evolutions of DSI and Bragg peak intensities after the laser excitation are measured and compared in the time domain. Their differences suggest that two kinds of lattice disorder, short-range and long-range, are triggered simultaneously. The former, induced by electron excitation, arises and decays with a faster rate than the latter which is subject to lattice heating. The results presented show that the time-resolved DSI measurements provide complementary insights to the ultrafast diffraction measurements.

  12. Ultrafast thermionic emission from metal irradiated using a femtosecond laser and an electric field in combination

    SciTech Connect (OSTI)

    Wang, Tingfeng; Guo, Jin; Shao, Junfeng; Wang, Dinan; Chen, Anmin E-mail: mxjin@jlu.edu.cn; Jin, Mingxing E-mail: mxjin@jlu.edu.cn

    2015-03-15

    Ultrafast thermionic emission from gold film irradiated with a femtosecond laser pulse in the presence of an additional electric field is analyzed using a two-temperature equation combined with a modified Richardson equation. The calculated results show that the duration of the emission is below 1 ps. Supplying an additional electric field is found to change the emission from the metal surface. Given the same laser fluence, this additional field reduces the work function of the metal, and thus improves the efficiency of thermionic emission. These results help to understand the mechanism and suggest ways to improve emissions in the context of ultrafast thermalized electron systems.

  13. An ultrafast electron microscope gun driven by two-photon photoemission from a nanotip cathode

    SciTech Connect (OSTI)

    Bormann, Reiner; Strauch, Stefanie; Schäfer, Sascha Ropers, Claus

    2015-11-07

    We experimentally and numerically investigate the performance of an advanced ultrafast electron source, based on two-photon photoemission from a tungsten needle cathode incorporated in an electron microscope gun geometry. Emission properties are characterized as a function of the electrostatic gun settings, and operating conditions leading to laser-triggered electron beams of very low emittance (below 20 nm mrad) are identified. The results highlight the excellent suitability of optically driven nano-cathodes for the further development of ultrafast transmission electron microscopy.

  14. The H2O2+OH ? HO2+H2O reaction in aqueous solution from a charge-dependent continuum model of solvation

    SciTech Connect (OSTI)

    Ginovska, Bojana; Camaioni, Donald M.; Dupuis, Michel

    2008-07-07

    We applied our recently developed protocol of the conductor-like continuum model of solvation to describe the title reaction in aqueous solution. The model has the unique feature of the molecular cavity being dependent on the atomic charges in the solute, and can be extended naturally to transition states and reaction pathways. It was used to calculate the reaction energetics and reaction rate in solution for the title reaction. The rate of reaction calculated using canonical variational transition state theory CVT in the context of the equilibrium solvation path (ESP) approximation, and including correction for tunneling through the small curvature approximation (SCT) was found to be 3.6 106 M-1 s-1, in very good agreement with experiment, These results suggest that the present protocol of the conductor-like continuum model of solvation with the charge-dependent cavity definition captures accurately the solvation effects at transition states and allows for quantitative estimates of reaction rates in solutions. This work was supported by the U.S. Department of Energy's (DOE) Office of Basic Energy Sciences, Chemical Sciences program. The Pacific Northwest National Laboratory is operated by Battelle for DOE.

  15. Decoupling Bulk and Surface Contributions in Water- Splitting Photocatalysts by In Situ Ultrafast Spectroscopy

    SciTech Connect (OSTI)

    Appavoo, Kannatassen; Mingzhao, Liu; Black, Charles T.; Sfeir, Matthew Y.

    2015-05-10

    By performing ultrafast emission spectroscopy in an operating, bias-controlled photoelectrochemical cell, we distinguish between bulk (charge transport) and surface (chemical reaction) recombination processes in a nanostructured photocatalyst and correlate its electronic properties directly with its incident-photon-to-current efficiency.

  16. DEVELOPMENT OF NEW MID-INFRARED ULTRAFAST LASER SOURCES FOR COMPACT COHERENT X-RAY SOURCES

    SciTech Connect (OSTI)

    Sterling Backus

    2012-05-14

    In this project, we proposed to develop laser based mid-infrared lasers as a potentially robust and reliable source of ultrafast pulses in the mid-infrared region of the spectrum, and to apply this light source to generating bright, coherent, femtosecond-to-attosecond x-ray beams.

  17. Ultrafast Laser Diagnostics for Energetic-Material Ignition Mechanisms...

    Office of Scientific and Technical Information (OSTI)

    presented here. SRS a nd transient absorption diagnostics are demonstrated on static thin - film samples, and paths forward to dynamic experiments are presented. Sandia...

  18. LCLS Ultrafast Science Instruments:Conceptual Design Report

    SciTech Connect (OSTI)

    Arthur, J.; Boutet, S.; Castagna, J-C.; Chapman, H.; Feng, Y.; Foyt, W.; Fritz, D.M.; Gaffney, K.J.; Gr|bel, G.; Hajdu, J.; Hastings, J.B.; Kurita, N.; Larsson, J.; Ludwig, K.; Messerschmidt, M.; Miao, J.; Reis, D.A.; Robert, A.; Stephenson, G.B.; Tschentscher, Th.; van Bakel, N.; /SLAC /LLNL, Livermore /DESY /Lund Inst. Tech. /Boston U. /UCLA /Michigan U. /Argonne

    2007-10-16

    The Stanford Linear Accelerator Center (SLAC), along with Argonne National Laboratory (ANL), Lawrence Livermore National Laboratory (LLNL), and the University of California at Los Angeles (UCLA), is constructing a Free-Electron Laser (FEL) facility, which will operate in the wavelength range 1.5 nm - 0.15 nm. This FEL, the Linac Coherent Light Source (LCLS), utilizes the SLAC linac and will produce sub-picosecond pulses of short wavelength X-rays with very high peak brightness and almost complete transverse coherence. The final one-third of the SLAC linac will be used as the source of electrons for the LCLS. The high energy electrons will be transported across the SLAC Research Yard, into a tunnel which will house a long undulator. In passing through the undulator, the electrons will be bunched by the force of their own synchrotron radiation and produce an intense, monochromatic, spatially coherent beam of X-rays. By varying the electron energy, the FEL X-ray wavelength will be tunable from 1.5 nm to 0.15 nm. The LCLS will include two experimental halls as well as X-ray optics and infrastructure necessary to create a facility that can be developed for research in a variety of disciplines such as atomic physics, materials science, plasma physics and biosciences. This Conceptual Design Report, the authors believe, confirms the feasibility of designing and constructing three X-ray instruments in order to exploit the unique scientific capability of this new LCLS facility. The technical objective of the LCLS Ultrafast Science Instruments (LUSI) project is to design, build, and install at the LCLS three hard X-ray instruments that will complement the initial instrument included in the LCLS construction. As the science programs advance and new technological challenges appear, instrumentation needs to be developed and ready to conquer these new opportunities. The LCLS instrument concepts have been developed in close consultation with the scientific community through a

  19. Proton chemical shift tensors determined by 3D ultrafast MAS double-quantum NMR spectroscopy

    SciTech Connect (OSTI)

    Zhang, Rongchun; Mroue, Kamal H.; Ramamoorthy, Ayyalusamy

    2015-10-14

    Proton NMR spectroscopy in the solid state has recently attracted much attention owing to the significant enhancement in spectral resolution afforded by the remarkable advances in ultrafast magic angle spinning (MAS) capabilities. In particular, proton chemical shift anisotropy (CSA) has become an important tool for obtaining specific insights into inter/intra-molecular hydrogen bonding. However, even at the highest currently feasible spinning frequencies (110–120 kHz), {sup 1}H MAS NMR spectra of rigid solids still suffer from poor resolution and severe peak overlap caused by the strong {sup 1}H–{sup 1}H homonuclear dipolar couplings and narrow {sup 1}H chemical shift (CS) ranges, which render it difficult to determine the CSA of specific proton sites in the standard CSA/single-quantum (SQ) chemical shift correlation experiment. Herein, we propose a three-dimensional (3D) {sup 1}H double-quantum (DQ) chemical shift/CSA/SQ chemical shift correlation experiment to extract the CS tensors of proton sites whose signals are not well resolved along the single-quantum chemical shift dimension. As extracted from the 3D spectrum, the F1/F3 (DQ/SQ) projection provides valuable information about {sup 1}H–{sup 1}H proximities, which might also reveal the hydrogen-bonding connectivities. In addition, the F2/F3 (CSA/SQ) correlation spectrum, which is similar to the regular 2D CSA/SQ correlation experiment, yields chemical shift anisotropic line shapes at different isotropic chemical shifts. More importantly, since the F2/F1 (CSA/DQ) spectrum correlates the CSA with the DQ signal induced by two neighboring proton sites, the CSA spectrum sliced at a specific DQ chemical shift position contains the CSA information of two neighboring spins indicated by the DQ chemical shift. If these two spins have different CS tensors, both tensors can be extracted by numerical fitting. We believe that this robust and elegant single-channel proton-based 3D experiment provides useful atomistic

  20. Ultrafast Dynamic Response of Single Crystal PETN and Beta-HMX...

    Office of Scientific and Technical Information (OSTI)

    Report Number(s): LLNL-CONF-656341 DOE Contract Number: DE-AC52-07NA27344 Resource Type: Conference Resource Relation: Conference: Presented at: International Detonation Symposium ...

  1. Ultrafast dynamics of a near-solid-density layer in an intense...

    Office of Scientific and Technical Information (OSTI)

    nm) femtosecond laser using time-resolved pump-probe Doppler spectrometry. An initial red-shift is observed in the reflected third harmonic ( 266 nm) probe pulse, which gets...

  2. Ultrafast Dynamic Response of Single Crystal PETN and Beta-HMX...

    Office of Scientific and Technical Information (OSTI)

    Close Cite: Bibtex Format Close 0 pages in this document matching the terms "" Search For Terms: Enter terms in the toolbar above to search the full text of this document for ...

  3. Ultrafast Power Processor for Smart Grid Power Module Development

    SciTech Connect (OSTI)

    MAITRA, ARINDAM; LITWIN, RAY; lai, Jason; Syracuse, David

    2012-12-30

    This project’s goal was to increase the switching speed and decrease the losses of the power semiconductor devices and power switch modules necessary to enable Smart Grid energy flow and control equipment such as the Ultra-Fast Power Processor. The primary focus of this project involves exploiting the new silicon-based Super-GTO (SGTO) technology and build on prototype modules already being developed. The prototype super gate-turn-off thyristor (SGTO) has been tested fully under continuously conducting and double-pulse hard-switching conditions for conduction and switching characteristics evaluation. The conduction voltage drop measurement results indicate that SGTO has excellent conduction characteristics despite inconsistency among some prototype devices. Tests were conducted with two conditions: (1) fixed gate voltage and varying anode current condition, and (2) fixed anode current and varying gate voltage condition. The conduction voltage drop is relatively a constant under different gate voltage condition. In terms of voltage drop as a function of the load current, there is a fixed voltage drop about 0.5V under zero current condition, and then the voltage drop is linearly increased with the current. For a 5-kV voltage blocking device that may operate under 2.5-kV condition, the projected voltage drop is less than 2.5 V under 50-A condition, or 0.1%. If the device is adopted in a converter operating under soft-switching condition, then the converter can achieve an ultrahigh efficiency, typically above 99%. The two-pulse switching test results indicate that SGTO switching speed is very fast. The switching loss is relatively low as compared to that of the insulated-gate-bipolar-transistors (IGBTs). A special phenomenon needs to be noted is such a fast switching speed for the high-voltage switching tends to create an unexpected Cdv/dt current, which reduces the turn-on loss because the dv/dt is negative and increases the turn-off loss because the dv/dt is

  4. Effect of bound state of water on hydronium ion mobility in hydrated Nafion using molecular dynamics simulations

    SciTech Connect (OSTI)

    Mabuchi, Takuya; Tokumasu, Takashi

    2014-09-14

    We have performed a detailed analysis of the structural properties of the sulfonate groups in terms of isolated and overlapped solvation shells in the nanostructure of hydrated Nafion membrane using classical molecular dynamics simulations. Our simulations have demonstrated the correlation between the two different areas in bound water region, i.e., the first solvation shell, and the vehicular transport of hydronium ions at different water contents. We have employed a model of the Nafion membrane using the improved force field, which is newly modified and validated by comparing the density and water diffusivity with those obtained experimentally. The first solvation shells were classified into the two types, the isolated area and the overlapped area. The mean residence times of solvent molecules explicitly showed the different behaviors in each of those areas in terms of the vehicular transport of protons: the diffusivity of classical hydronium ions in the overlapped area dominates their total diffusion at lower water contents while that in the isolated area dominates for their diffusion at higher water contents. The results provided insights into the importance role of those areas in the solvation shells for the diffusivity of vehicular transport of hydronium ions in hydrated Nafion membrane.

  5. Modeling of coherent ultrafast magneto-optical experiments: Light-induced molecular mean-field model

    SciTech Connect (OSTI)

    Hinschberger, Y.; Hervieux, P.-A.

    2015-12-28

    We present calculations which aim to describe coherent ultrafast magneto-optical effects observed in time-resolved pump-probe experiments. Our approach is based on a nonlinear semi-classical Drude-Voigt model and is used to interpret experiments performed on nickel ferromagnetic thin film. Within this framework, a phenomenological light-induced coherent molecular mean-field depending on the polarizations of the pump and probe pulses is proposed whose microscopic origin is related to a spin-orbit coupling involving the electron spins of the material sample and the electric field of the laser pulses. Theoretical predictions are compared to available experimental data. The model successfully reproduces the observed experimental trends and gives meaningful insight into the understanding of magneto-optical rotation behavior in the ultrafast regime. Theoretical predictions for further experimental studies are also proposed.

  6. Time-domain sampling of x-ray pulses using an ultrafast sample response

    SciTech Connect (OSTI)

    Gaal, P.; Shayduk, R.; Schick, D.; Herzog, M.; Bojahr, A.; Goldshteyn, J.; Navirian, H. A.; Leitenberger, W.; Vrejoiu, I.; Khakhulin, D.; Wulff, M.; Bargheer, M.

    2012-12-10

    We employ the ultrafast response of a 15.4 nm thin SrRuO{sub 3} layer grown epitaxially on a SrTiO{sub 3} substrate to perform time-domain sampling of an x-ray pulse emitted from a synchrotron storage ring. Excitation of the sample with an ultrashort laser pulse triggers coherent expansion and compression waves in the thin layer, which turn the diffraction efficiency on and off at a fixed Bragg angle during 5 ps. This is significantly shorter than the duration of the synchrotron x-ray pulse of 100 ps. Cross-correlation measurements of the ultrafast sample response and the synchrotron x-ray pulse allow to reconstruct the x-ray pulse shape.

  7. Ablation experiment and threshold calculation of titanium alloy irradiated by ultra-fast pulse laser

    SciTech Connect (OSTI)

    Zheng, Buxiang; Jiang, Gedong; Wang, Wenjun Wang, Kedian; Mei, Xuesong; State Key Laboratory for Manufacturing Systems Engineering, Xi'an Jiaotong University, Xi'an 710054

    2014-03-15

    The interaction between an ultra-fast pulse laser and a material's surface has become a research hotspot in recent years. Micromachining of titanium alloy with an ultra-fast pulse laser is a very important research direction, and it has very important theoretical significance and application value in investigating the ablation threshold of titanium alloy irradiated by ultra-fast pulse lasers. Irradiated by a picosecond pulse laser with wavelengths of 1064 nm and 532 nm, the surface morphology and feature sizes, including ablation crater width (i.e. diameter), ablation depth, ablation area, ablation volume, single pulse ablation rate, and so forth, of the titanium alloy were studied, and their ablation distributions were obtained. The experimental results show that titanium alloy irradiated by a picosecond pulse infrared laser with a 1064 nm wavelength has better ablation morphology than that of the green picosecond pulse laser with a 532 nm wavelength. The feature sizes are approximately linearly dependent on the laser pulse energy density at low energy density and the monotonic increase in laser pulse energy density. With the increase in energy density, the ablation feature sizes are increased. The rate of increase in the feature sizes slows down gradually once the energy density reaches a certain value, and gradually saturated trends occur at a relatively high energy density. Based on the linear relation between the laser pulse energy density and the crater area of the titanium alloy surface, and the Gaussian distribution of the laser intensity on the cross section, the ablation threshold of titanium alloy irradiated by an ultra-fast pulse laser was calculated to be about 0.109 J/cm{sup 2}.

  8. An ultrafast nanotip electron gun triggered by grating-coupled surface plasmons

    SciTech Connect (OSTI)

    Schröder, Benjamin; Sivis, Murat; Bormann, Reiner; Schäfer, Sascha; Ropers, Claus

    2015-12-07

    We demonstrate multiphoton photoelectron emission from gold nanotips induced by nanofocusing surface plasmons, resonantly excited on the tip shaft by a grating coupler. The tip is integrated into an electron gun assembly, which facilitates control over the spatial emission sites and allows us to disentangle direct grating emission from plasmon-triggered apex emission. The nanoscale source size of this electron gun concept enables highly coherent electron pulses with applications in ultrafast electron imaging and diffraction.

  9. Extracting the diffusion tensor from molecular dynamics simulation with Milestoning

    SciTech Connect (OSTI)

    Mugnai, Mauro L.; Elber, Ron

    2015-01-07

    We propose an algorithm to extract the diffusion tensor from Molecular Dynamics simulations with Milestoning. A Kramers-Moyal expansion of a discrete master equation, which is the Markovian limit of the Milestoning theory, determines the diffusion tensor. To test the algorithm, we analyze overdamped Langevin trajectories and recover a multidimensional Fokker-Planck equation. The recovery process determines the flux through a mesh and estimates local kinetic parameters. Rate coefficients are converted to the derivatives of the potential of mean force and to coordinate dependent diffusion tensor. We illustrate the computation on simple models and on an atomically detailed system—the diffusion along the backbone torsions of a solvated alanine dipeptide.

  10. The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales (A "Life at the Frontiers of Energy Research" contest entry from the 2011 Energy Frontier Research Centers (EFRCs) Summit and Forum)

    ScienceCinema (OSTI)

    Mao, Ho-kwang (Director, Center for Energy Frontier Research in Extreme Environments); EFree Staff

    2011-11-02

    'The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales ' was submitted by the Center for Energy Frontier Research in Extreme Environments (EFree) to the 'Life at the Frontiers of Energy Research' video contest at the 2011 Science for Our Nation's Energy Future: Energy Frontier Research Centers (EFRCs) Summit and Forum. Twenty-six EFRCs created short videos to highlight their mission and their work. EFree is directed by Ho-kwang Mao at the Carnegie Institute of Washington and is a partnership of scientists from thirteen institutions.The Office of Basic Energy Sciences in the U.S. Department of Energy's Office of Science established the 46 Energy Frontier Research Centers (EFRCs) in 2009. These collaboratively-organized centers conduct fundamental research focused on 'grand challenges' and use-inspired 'basic research needs' recently identified in major strategic planning efforts by the scientific community. The overall purpose is to accelerate scientific progress toward meeting the nation's critical energy challenges. The mission of Energy Frontier Research in Extreme Environments is 'to accelerate the discovery and creation of energy-relevant materials using extreme pressures and temperatures.' Research topics are: catalysis (CO{sub 2}, water), photocatalysis, solid state lighting, optics, thermelectric, phonons, thermal conductivity, solar electrodes, fuel cells, superconductivity, extreme environment, radiation effects, defects, spin dynamics, CO{sub 2} (capture, convert, store), greenhouse gas, hydrogen (fuel, storage), ultrafast physics, novel materials synthesis, and defect tolerant materials.

  11. The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales (A "Life at the Frontiers of Energy Research" contest entry from the 2011 Energy Frontier Research Centers (EFRCs) Summit and Forum)

    SciTech Connect (OSTI)

    Mao, Ho-kwang; EFree Staff

    2011-05-01

    'The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales ' was submitted by the Center for Energy Frontier Research in Extreme Environments (EFree) to the 'Life at the Frontiers of Energy Research' video contest at the 2011 Science for Our Nation's Energy Future: Energy Frontier Research Centers (EFRCs) Summit and Forum. Twenty-six EFRCs created short videos to highlight their mission and their work. EFree is directed by Ho-kwang Mao at the Carnegie Institute of Washington and is a partnership of scientists from thirteen institutions.The Office of Basic Energy Sciences in the U.S. Department of Energy's Office of Science established the 46 Energy Frontier Research Centers (EFRCs) in 2009. These collaboratively-organized centers conduct fundamental research focused on 'grand challenges' and use-inspired 'basic research needs' recently identified in major strategic planning efforts by the scientific community. The overall purpose is to accelerate scientific progress toward meeting the nation's critical energy challenges. The mission of Energy Frontier Research in Extreme Environments is 'to accelerate the discovery and creation of energy-relevant materials using extreme pressures and temperatures.' Research topics are: catalysis (CO{sub 2}, water), photocatalysis, solid state lighting, optics, thermelectric, phonons, thermal conductivity, solar electrodes, fuel cells, superconductivity, extreme environment, radiation effects, defects, spin dynamics, CO{sub 2} (capture, convert, store), greenhouse gas, hydrogen (fuel, storage), ultrafast physics, novel materials synthesis, and defect tolerant materials.

  12. Following the dynamics of matter with femtosecond precision using the X-ray streaking method

    SciTech Connect (OSTI)

    David, C.; Karvinen, P.; Sikorski, M.; Song, S.; Vartiainen, I.; Milne, C. J.; Mozzanica, A.; Kayser, Y.; Diaz, A.; Mohacsi, I.; Carini, G. A.; Herrmann, S.; Färm, E.; Ritala, M.; Fritz, D. M.; Robert, A.

    2015-01-06

    X-ray Free Electron Lasers (FELs) can produce extremely intense and very short pulses, down to below 10 femtoseconds (fs). Among the key applications are ultrafast time-resolved studies of dynamics of matter by observing responses to fast excitation pulses in a pump-probe manner. Detectors with sufficient time resolution for observing these processes are not available. Therefore, such experiments typically measure a sample's full dynamics by repeating multiple pump-probe cycles at different delay times. This conventional method assumes that the sample returns to an identical or very similar state after each cycle. Here we describe a novel approach that can provide a time trace of responses following a single excitation pulse, jitter-free, with fs timing precision. We demonstrate, in an X-ray diffraction experiment, how it can be applied to the investigation of ultrafast irreversible processes.

  13. Following the dynamics of matter with femtosecond precision using the X-ray streaking method

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    David, C.; Karvinen, P.; Sikorski, M.; Song, S.; Vartiainen, I.; Milne, C. J.; Mozzanica, A.; Kayser, Y.; Diaz, A.; Mohacsi, I.; et al

    2015-01-06

    X-ray Free Electron Lasers (FELs) can produce extremely intense and very short pulses, down to below 10 femtoseconds (fs). Among the key applications are ultrafast time-resolved studies of dynamics of matter by observing responses to fast excitation pulses in a pump-probe manner. Detectors with sufficient time resolution for observing these processes are not available. Therefore, such experiments typically measure a sample's full dynamics by repeating multiple pump-probe cycles at different delay times. This conventional method assumes that the sample returns to an identical or very similar state after each cycle. Here we describe a novel approach that can provide amore » time trace of responses following a single excitation pulse, jitter-free, with fs timing precision. We demonstrate, in an X-ray diffraction experiment, how it can be applied to the investigation of ultrafast irreversible processes.« less

  14. Ultrafast laser based coherent control methods for explosives detection

    SciTech Connect (OSTI)

    Moore, David Steven

    2010-12-06

    The detection of explosives is a notoriously difficult problem, especially at stand-off, due to their (generally) low vapor pressure, environmental and matrix interferences, and packaging. We are exploring Optimal Dynamic Detection of Explosives (ODD-Ex), which exploits the best capabilities of recent advances in laser technology and recent discoveries in optimal shaping of laser pulses for control of molecular processes to significantly enhance the standoff detection of explosives. The core of the ODD-Ex technique is the introduction of optimally shaped laser pulses to simultaneously enhance sensitivity to explosives signatures while dramatically improving specificity, particularly against matrix materials and background interferences. These goals are being addressed by operating in an optimal non-linear fashion, typically with a single shaped laser pulse inherently containing within it coherently locked control and probe subpulses. Recent results will be presented.

  15. Ultrafast spectroscopy of super high frequency mechanical modes of doubly clamped beams

    SciTech Connect (OSTI)

    Ristow, Oliver; Merklein, Moritz; Grossmann, Martin; Hettich, Mike; Schubert, Martin; Bruchhausen, Axel; Scheer, Elke; Dekorsy, Thomas; Barretto, Elaine C. S.; Grebing, Jochen; Erbe, Artur; Mounier, Denis; Gusev, Vitalyi

    2013-12-02

    We use ultrafast pump-probe spectroscopy to study the mechanical vibrations in the time domain of doubly clamped silicon nitride beams. Beams with two different clamping conditions are investigated. Finite element method calculations are performed to analyse the mode spectra of both structures. By calculating the strain integral on the surface of the resonators, we are able to reproduce the effect of the detection mechanism and identify all the measured modes. We show that our spectroscopy technique combined with our modelling tools allow the investigation of several different modes in the super high frequency range (3-30?GHz) and above, bringing more information about the vibration modes of nanomechanical resonators.

  16. Intracavity terahertz generation inside a high-energy ultrafast soliton fiber laser

    SciTech Connect (OSTI)

    Matthaeus, Gabor; Ortac, Buelend; Limpert, Jens; Nolte, Stefan; Hohmuth, Rico; Voitsch, Martin; Richter, Wolfgang; Pradarutti, Boris; Tuennermann, Andreas

    2008-12-29

    Intracavity terahertz emission inside a high-energy ultrafast Yb-doped fiber laser is presented. The terahertz radiation is generated by a transient photocurrent induced at the surface of a saturable InGaAs multiquantum well grown by molecular beam epitaxy on top of a semiconductor Bragg reflector. This device simultaneously works as the saturable absorber mirror for initiating and managing the passive mode locking required for the ultrashort pulse operation of the laser system. The maximum terahertz average power achieved is 4.2 {mu}W, which reveals a net conversion efficiency of 3.1x10{sup -5}.

  17. High Brightness, Laser-Driven X-ray Source for Nanoscale Metrology and Femtosecond Dynamics

    SciTech Connect (OSTI)

    Siders, C W; Crane, J K; Semenov, V; Betts, S; Kozioziemski, B; Wharton, K; Wilks, S; Barbee, T; Stuart, B; Kim, D E; An, J; Barty, C

    2007-02-26

    This project developed and demonstrated a new, bright, ultrafast x-ray source based upon laser-driven K-alpha generation, which can produce an x-ray flux 10 to 100 times greater than current microfocus x-ray tubes. The short-pulse (sub-picosecond) duration of this x-ray source also makes it ideal for observing time-resolved dynamics of atomic motion in solids and thin films.

  18. Probing the Early Stages of Solvation of cis-Pinate Dianions by Water, Acetonitrile, and Methanol: A Photoelectron Spectroscopy and Theoretical Study

    SciTech Connect (OSTI)

    Hou, Gao-Lei; Kong, Xiang-Tao; Valiev, Marat; Jiang, Ling; Wang, Xue B.

    2016-01-01

    Cis-pinic acid is one of the most important oxidation products of α-pinene – a key monoterpene compound in biogenic emission processes affecting the atmosphere. Molecular level understanding of interactions involved in the cluster formations around cis-pinic acid is an important and necessary prerequisite toward ascertaining its role in the aerosol formation processes. In this work, we studied the structures and energetics of the solvated clusters of cis-pinate (cis-PA²⁻), the doubly deprotonated dicarboxylate of cis-pinic acid, with H₂O, CH₃OH, and CH₃CN by negative ion photoelectron spectroscopy and ab initio theoretical calculations. We found that cis-PA²⁻ prefers being solvated alternately on the two -CO₂⁻ groups with increase of solvent coverage, a well-known solvation pattern that has been observed in microhydrated linear dicarboxylate dianion (DCn²⁻) clusters. Experiments and calculations further reveal an intriguing feature for the existence of the asymmetric type isomers for cis-PA2–(H2O)2 and cis-PA²⁻(CH₃OH)₂, in which both solvent molecules interact with only one of the -CO²⁻ groups – a phenomena that has not been observed in DCn²⁻ water clusters and exhibits the subtle effect of the rigid four-membered carbon ring brought in on the cis-PA²⁻ solvation. The dominant interactions between cis-PA²⁻ and solvent molecules are forming bidentate O–···H–O H-bonds for H₂O, O–···H–O and O–···H–C H-bonds for CH₃OH, and tridentate O–···H–C H-bonds for CH₃CN. The formation of inter-solvent H-bonds between H₂O and CH₃CN is found to be favorable in mixed solvent clusters, distinctly different from that between H₂O and CH₃OH. These findings have important implications for understanding the mechanism of cluster growth and nucleation of atmospheric organic aerosols and the nature of structure-function relationship of proteins containing carboxylate groups under various solvent

  19. Capturing ultrafast photoinduced local structural distortions of BiFeO3

    SciTech Connect (OSTI)

    Wen, Haidan; Sassi, Michel JPC; Luo, Zhenlin; Adamo, Carolina; Schlom, Darrell; Rosso, Kevin M.; Zhang, Xiaoyi

    2015-10-14

    The interaction of light with materials is an intensively studied research forefront, in which the coupling of radiation energy to selective degrees of freedom offers contact-free tuning of functionalities on ultrafast time scales. Capturing the fundamental processes and understanding the mechanism of photoinduced structural rearrangement are essential to applications such as photo-active actuators and efficient photovoltaic devices. Using ultrafast x-ray absorption spectroscopy aided by density functional theory calculations, we reveal the local structural arrangement around the transition metal atom in a unit cell of the photoferroelectric archetype BiFeO3 film. The out-of-plane elongation of the unit cell is accompanied by the in-plane shrinkage with minimal change of interaxial lattice angles upon photoexcitation. This uniaxial elastic deformation of the unit cell is driven by localized electric field as a result of photoinduced charge separation, in contrast to a global lattice constant increase and lattice angle variations as a result of heating. The finding of a photoinduced elastic unit cell deformation elucidates a microscopic picture of photocarrier-mediated nonequilibrium processes in polar materials.

  20. Capturing ultrafast photoinduced local structural distortions of BiFeO3

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Wen, Haidan; Sassi, Michel JPC; Luo, Zhenlin; Adamo, Carolina; Schlom, Darrell; Rosso, Kevin M.; Zhang, Xiaoyi

    2015-10-14

    The interaction of light with materials is an intensively studied research forefront, in which the coupling of radiation energy to selective degrees of freedom offers contact-free tuning of functionalities on ultrafast time scales. Capturing the fundamental processes and understanding the mechanism of photoinduced structural rearrangement are essential to applications such as photo-active actuators and efficient photovoltaic devices. Using ultrafast x-ray absorption spectroscopy aided by density functional theory calculations, we reveal the local structural arrangement around the transition metal atom in a unit cell of the photoferroelectric archetype BiFeO3 film. The out-of-plane elongation of the unit cell is accompanied by themore » in-plane shrinkage with minimal change of interaxial lattice angles upon photoexcitation. This uniaxial elastic deformation of the unit cell is driven by localized electric field as a result of photoinduced charge separation, in contrast to a global lattice constant increase and lattice angle variations as a result of heating. The finding of a photoinduced elastic unit cell deformation elucidates a microscopic picture of photocarrier-mediated nonequilibrium processes in polar materials.« less

  1. Direct observation of a photoinduced Wolff rearrangement in PMMA using ultrafast infrared spectroscopy

    SciTech Connect (OSTI)

    Lippert, T.; Koskelo, A.; Stoutland, P.O.

    1996-02-14

    As part of a program to develop diagnostics for laser-driven reaction in polymer matrices, we have investigated the photoinduced decomposition of 5-diazo-2,2-dimethyl-1,3-dioxane-4,6-dione (5-diazo Meldrum`s acid, DM) in a PMMA matrix. This particular diazoketone is sensitive to deep UV (200-260nm), making it suitable for high-resolution lithographic applications. It has historically been difficult to study the chemistry of such resists as many of the intermediates are short-lived and absorb only in the UV. Recent advances in ultrafast infrared spectroscopy, however, now allow us to directly examine the initial steps occurring in UV photoresists with infrared spectroscopy. Herein, we describe the first room temperature observation of intermediates in the photochemistry of DM with utlrafast infrared spectroscopy. In summary, these experiments have provided the first example of how ultrafast infrared spectroscopy may be used to examine laser-driven reactions in polymeric matrices. We have determined that the photoinduced Wolff rearrangement of DM in a PMMA matrix is complete within 20 ps. The IR band assignable to the ketene is centered at 2161 cm{sup -1} and has a width of 29 cm{sup -1}. The rapid formation of the ketene is a key element of the high quantum yield of carboxylic acid formation and a key element as well for the use of DM as an ablation sensitizer. 22 refs., 3 figs.

  2. H.sub.2O doped WO.sub.3, ultra-fast, high-sensitivity hydrogen sensors

    DOE Patents [OSTI]

    Liu, Ping; Tracy, C. Edwin; Pitts, J. Roland; Lee, Se-Hee

    2011-03-22

    An ultra-fast response, high sensitivity structure for optical detection of low concentrations of hydrogen gas, comprising: a substrate; a water-doped WO.sub.3 layer coated on the substrate; and a palladium layer coated on the water-doped WO.sub.3 layer.

  3. Accurate static and dynamic properties of liquid-electrolytes for Li-ion batteries from ab initio molecular dynamics

    SciTech Connect (OSTI)

    Ganesh, Panchapakesan; Jiang, Deen; Kent, Paul R

    2011-01-01

    Lithium-ion batteries have the potential to revolutionize the transportation industry, as they did for wireless communication. A judicious choice of the liquid electrolytes used in these systems is required to achieve a good balance among high-energy storage, long cycle life and stability, and fast charging. Ethylene-carbonate (EC) and propylene-carbonate (PC) are popular electrolytes. However, to date, almost all molecular-dynamics simulations of these fluids rely on classical force fields, while a complete description of the functionality of Li-ion batteries will eventually require quantum mechanics. We perform accurate ab initio molecular-dynamics simulations of ethylene- and propylene-carbonate with LiPF6 at experimental concentrations to build solvation models which explain available neutron scattering and nuclear magnetic resonance (NMR) results and to compute Li-ion solvation energies and diffusion constants. Our results suggest some similarities between the two liquids as well as some important differences. Simulations also provide useful insights into formation of solid-electrolyte interphases in the presence of electrodes in conventional Li-ion batteries.

  4. Accurate static and dynamic properties of liquid electrolytes for Li-ion batteries from ab initio molecular dynamics

    SciTech Connect (OSTI)

    Ganesh, P.; Jiang, D.; Kent, P.R.C.

    2011-03-31

    Lithium-ion batteries have the potential to revolutionize the transportation industry, as they did for wireless communication. A judicious choice of the liquid electrolytes used in these systems is required to achieve a good balance among high-energy storage, long cycle life and stability, and fast charging. Ethylene-carbonate (EC) and propylene-carbonate (PC) are popular electrolytes. However, to date, almost all molecular-dynamics simulations of these fluids rely on classical force fields, while a complete description of the functionality of Li-ion batteries will eventually require quantum mechanics. We perform accurate ab initio molecular-dynamics simulations of ethylene- and propylene-carbonate with LiPF6 at experimental concentrations to build solvation models which explain available neutron scattering and nuclear magnetic resonance (NMR) results and to compute Li-ion solvation energies and diffusion constants. Our results suggest some similarities between the two liquids as well as some important differences. Simulations also provide useful insights into formation of solid-electrolyte interphases in the presence of electrodes in conventional Li-ion batteries.

  5. Possible Demonstration of a Polaronic Bose-Einstein(-Mott) Condensate in UO2(+x) by Ultrafast THz Spectroscopy and Microwave Dissipation

    SciTech Connect (OSTI)

    Conradson, Steven D.; Gilbertson, Steven M.; Daifuku, Stephanie L.; Kehl, Jeffrey A.; Durakiewicz, Tomasz; Andersson, David A.; Bishop, Alan R.; Byler, Darrin D.; Maldonado, Pablo; Oppeneer, Peter M.; Valdez, James A.; Neidig, Michael L.; Rodriguez, George

    2015-10-16

    Bose-Einstein condensates (BECs) composed of polarons would be an advance because they would combine coherently charge, spin, and a crystal lattice. Following our earlier report of unique structural and spectroscopic properties, we now identify potentially definitive evidence for polaronic BECs in photo- and chemically doped UO2(+x) on the basis of exceptional coherence in the ultrafast time dependent terahertz absorption and microwave spectroscopy results that show collective behavior including dissipation patterns whose precedents are condensate vortex and defect disorder and condensate excitations. Furthermore, that some of these signatures of coherence in an atom-based system extend to ambient temperature suggests a novel mechanism that could be a synchronized, dynamical, disproportionation excitation, possibly via the solid state analog of a Feshbach resonance that promotes the coherence. Such a mechanism would demonstrate that the use of ultra-low temperatures to establish the BEC energy distribution is a convenience rather than a necessity, with the actual requirement for the particles being in the same state that is not necessarily the ground state attainable by other means. Interestingly, a macroscopic quantum object created by chemical doping that can persist to ambient temperature and resides in a bulk solid would be revolutionary in a number of scientific and technological fields.

  6. Possible Demonstration of a Polaronic Bose-Einstein(-Mott) Condensate in UO2(+x) by Ultrafast THz Spectroscopy and Microwave Dissipation

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Conradson, Steven D.; Gilbertson, Steven M.; Daifuku, Stephanie L.; Kehl, Jeffrey A.; Durakiewicz, Tomasz; Andersson, David A.; Bishop, Alan R.; Byler, Darrin D.; Maldonado, Pablo; Oppeneer, Peter M.; et al

    2015-10-16

    Bose-Einstein condensates (BECs) composed of polarons would be an advance because they would combine coherently charge, spin, and a crystal lattice. Following our earlier report of unique structural and spectroscopic properties, we now identify potentially definitive evidence for polaronic BECs in photo- and chemically doped UO2(+x) on the basis of exceptional coherence in the ultrafast time dependent terahertz absorption and microwave spectroscopy results that show collective behavior including dissipation patterns whose precedents are condensate vortex and defect disorder and condensate excitations. Furthermore, that some of these signatures of coherence in an atom-based system extend to ambient temperature suggests a novelmore » mechanism that could be a synchronized, dynamical, disproportionation excitation, possibly via the solid state analog of a Feshbach resonance that promotes the coherence. Such a mechanism would demonstrate that the use of ultra-low temperatures to establish the BEC energy distribution is a convenience rather than a necessity, with the actual requirement for the particles being in the same state that is not necessarily the ground state attainable by other means. Interestingly, a macroscopic quantum object created by chemical doping that can persist to ambient temperature and resides in a bulk solid would be revolutionary in a number of scientific and technological fields.« less

  7. Possible Demonstration of a Polaronic Bose-Einstein(-Mott) Condensate in UO2(+x) by Ultrafast THz Spectroscopy and Microwave Dissipation

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Conradson, Steven D.; Gilbertson, Steven M.; Daifuku, Stephanie L.; Kehl, Jeffrey A.; Durakiewicz, Tomasz; Andersson, David A.; Bishop, Alan R.; Byler, Darrin D.; Maldonado, Pablo; Oppeneer, Peter M.; et al

    2015-10-16

    Bose-Einstein condensates (BECs) composed of polarons would be an advance because they would combine coherently charge, spin, and a crystal lattice. Following our earlier report of unique structural and spectroscopic properties, we now identify potentially definitive evidence for polaronic BECs in photo- and chemically doped UO2(+x) on the basis of exceptional coherence in the ultrafast time dependent terahertz absorption and microwave spectroscopy results that show collective behavior including dissipation patterns whose precedents are condensate vortex and defect disorder and condensate excitations. Furthermore, that some of these signatures of coherence in an atom-based system extend to ambient temperature suggests a novelmore »mechanism that could be a synchronized, dynamical, disproportionation excitation, possibly via the solid state analog of a Feshbach resonance that promotes the coherence. Such a mechanism would demonstrate that the use of ultra-low temperatures to establish the BEC energy distribution is a convenience rather than a necessity, with the actual requirement for the particles being in the same state that is not necessarily the ground state attainable by other means. Interestingly, a macroscopic quantum object created by chemical doping that can persist to ambient temperature and resides in a bulk solid would be revolutionary in a number of scientific and technological fields.« less

  8. Effective Analysis of NGS Metagenomic Data with Ultra-Fast Clustering Algorithms (MICW - Metagenomics Informatics Challenges Workshop: 10K Genomes at a Time)

    ScienceCinema (OSTI)

    Li, Weizhong [San Diego Supercomputer Center

    2013-01-22

    San Diego Supercomputer Center's Weizhong Li on "Effective Analysis of NGS Metagenomic Data with Ultra-fast Clustering Algorithms" at the Metagenomics Informatics Challenges Workshop held at the DOE JGI on October 12-13, 2011.

  9. Water around fullerene shape amphiphiles: A molecular dynamics simulation study of hydrophobic hydration

    SciTech Connect (OSTI)

    Varanasi, S. R. E-mail: guskova@ipfdd.de; John, A.; Guskova, O. A. E-mail: guskova@ipfdd.de; Sommer, J.-U.

    2015-06-14

    Fullerene C{sub 60} sub-colloidal particle with diameter ?1 nm represents a boundary case between small and large hydrophobic solutes on the length scale of hydrophobic hydration. In the present paper, a molecular dynamics simulation is performed to investigate this complex phenomenon for bare C{sub 60} fullerene and its amphiphilic/charged derivatives, so called shape amphiphiles. Since most of the unique properties of water originate from the pattern of hydrogen bond network and its dynamics, spatial, and orientational aspects of water in solvation shells around the solute surface having hydrophilic and hydrophobic regions are analyzed. Dynamical properties such as translational-rotational mobility, reorientational correlation and occupation time correlation functions of water molecules, and diffusion coefficients are also calculated. Slower dynamics of solvent moleculeswater retardationin the vicinity of the solutes is observed. Both the topological properties of hydrogen bond pattern and the dangling OH groups that represent surface defects in water network are monitored. The fraction of such defect structures is increased near the hydrophobic cap of fullerenes. Some dry regions of C{sub 60} are observed which can be considered as signatures of surface dewetting. In an effort to provide molecular level insight into the thermodynamics of hydration, the free energy of solvation is determined for a family of fullerene particles using thermodynamic integration technique.

  10. Terahertz Spectroscopy of Low-Dimensional Nanomaterials: Nonlinear Emission and Ultrafast Electrodynamics

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Luo, Liang; Wang, Jigang

    2016-01-01

    Nonlinear and non-equilibrium properties of low-dimensional quantum materials are fundamental in nanoscale science yet transformative in nonlinear imaging/photonic technology today. These have been poorly addressed in many nano-materials despite of their well-established equilibrium optical and transport properties. The development of ultrafast terahertz (THz) sources and nonlinear spectroscopy tools facilitates understanding these issues and reveals a wide range of novel nonlinear and quantum phenomena that are not expected in bulk solids or atoms. In this paper, we discuss our recent discoveries in two model photonic and electronic nanostructures to solve two outstanding questions: (1) how to create nonlinear broadband terahertz emittersmore » using deeply subwavelength nanoscale meta-atom resonators? (2) How to access one-dimensional (1D) dark excitons and their non-equilibrium correlated states in single-walled carbon nanotubes (SWMTs)?« less

  11. Terahertz Spectroscopy of Low-Dimensional Nanomaterials: Nonlinear Emission and Ultrafast Electrodynamics

    SciTech Connect (OSTI)

    Luo, Liang; Wang, Jigang

    2016-01-01

    Nonlinear and non-equilibrium properties of low-dimensional quantum materials are fundamental in nanoscale science yet transformative in nonlinear imaging/photonic technology today. These have been poorly addressed in many nano-materials despite of their well-established equilibrium optical and transport properties. The development of ultrafast terahertz (THz) sources and nonlinear spectroscopy tools facilitates understanding these issues and reveals a wide range of novel nonlinear and quantum phenomena that are not expected in bulk solids or atoms. In this paper, we discuss our recent discoveries in two model photonic and electronic nanostructures to solve two outstanding questions: (1) how to create nonlinear broadband terahertz emitters using deeply subwavelength nanoscale meta-atom resonators? (2) How to access one-dimensional (1D) dark excitons and their non-equilibrium correlated states in single-walled carbon nanotubes (SWMTs)?

  12. Ultrafast terahertz-induced response of GeSbTe phase-change materials

    SciTech Connect (OSTI)

    Shu, Michael J.; Zalden, Peter; Chen, Frank; Weems, Ben; Chatzakis, Ioannis; Xiong, Feng; Jeyasingh, Rakesh; Pop, Eric; Philip Wong, H.-S.; Hoffmann, Matthias C.; Wuttig, Matthias; Lindenberg, Aaron M.

    2014-06-23

    The time-resolved ultrafast electric field-driven response of crystalline and amorphous GeSbTe films has been measured all-optically, pumping with single-cycle terahertz pulses as a means of biasing phase-change materials on a sub-picosecond time-scale. Utilizing the near-band-gap transmission as a probe of the electronic and structural response below the switching threshold, we observe a field-induced heating of the carrier system and resolve the picosecond-time-scale energy relaxation processes and their dependence on the sample annealing condition in the crystalline phase. In the amorphous phase, an instantaneous electroabsorption response is observed, quadratic in the terahertz field, followed by field-driven lattice heating, with Ohmic behavior up to 200 kV/cm.

  13. Ultrafast proton radiography of the magnetic fields generated by a laser-driven coil current

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Gao, Lan; Ji, Hantao; Fiksel, Gennady; Fox, William; Evans, Michelle; Alfonso, Noel

    2016-04-15

    Magnetic fields generated by a current flowing through a U-shaped coil connecting two copper foils were measured using ultrafast proton radiography. Two ~ 1.25 kJ, 1-ns laser pulses propagated through laser entrance holes in the front foil and were focused to the back foil with an intensity of ~ 3 x 1016 W/cm2. The intense laser-solid interaction induced a high voltage between the copper foils and generated a large current in the connecting coil. The proton data show ~ 40-50 T magnetic fields at the center of the coil ~ 3-4 ns after laser irradiation. In conclusion, the experiments providemore » significant insight for future target designs that aim to develop a powerful source of external magnetic fields for various applications in high-energy-density science.« less

  14. Observing Structure and Motion in Molecules with Ultrafast Strong Field and Short Wavelength Laser Radiation

    SciTech Connect (OSTI)

    Bucksbaum, Philip H

    2011-04-13

    The term "molecular movie" has come to describe efforts to track and record Angstrom-scale coherent atomic and electronic motion in a molecule. The relevant time scales for this range cover several orders of magnitude, from sub-femtosecond motion associated with electron-electron correlations, to 100-fs internal vibrations, to multi-picosecond motion associated with the dispersion and quantum revivals of molecular reorientation. Conventional methods of cinematography do not work well in this ultrafast and ultrasmall regime, but stroboscopic "pump and probe" techniques can reveal this motion with high fidelity. This talk will describe some of the methods and recent progress in exciting and controlling this motion, using both laboratory lasers and the SLAC Linac Coherent Light Source x-ray free electron laser, and will further try to relate the date to the goal of molecular movies.

  15. Efficient terahertz-wave generation and its ultrafast optical modulation in charge ordered organic ferroelectrics

    SciTech Connect (OSTI)

    Itoh, Hirotake Iwai, Shinichiro; Itoh, Keisuke; Goto, Kazuki; Yamamoto, Kaoru; Yakushi, Kyuya

    2014-04-28

    Efficient terahertz (THz) wave generation in strongly correlated organic compounds ?-(ET){sub 2}I{sub 3} and ??-(ET){sub 2}IBr{sub 2} (ET:bis(ethylenedithio)-tetrathiafulvalene) was demonstrated. The spontaneous polarization induced by charge ordering or electronic ferroelectricity was revealed to trigger the THz-wave generation via optical rectification; the estimated 2nd-order nonlinear optical susceptibility for ?-(ET){sub 2}I{sub 3} is over 70 times larger than that for prototypical THz-source ZnTe. Ultrafast (<1 ps) and sensitive (?40%) photoresponse of the THz wave was observed for ?-(ET){sub 2}I{sub 3}, which is attributable to photoinduced quenching of the polarization accompanied by insulator(ferroelectric)-to-metal transition. Modulation of the THz wave was observed for ??-(ET){sub 2}IBr{sub 2} upon the poling procedure, indicating the alignment of polar domains.

  16. Chirped-pulse manipulated carrier dynamics in low-temperature molecular-beam-epitaxy grown GaAs

    SciTech Connect (OSTI)

    Lee, Chao-Kuei; Lin, Yuan-Yao; Lin, Sung-Hui; Lin, Gong-Ru; Pan, Ci-Ling

    2014-04-28

    Chirped pulse controlled carrier dynamics in low-temperature molecular-beam-epitaxy grown GaAs are investigated by degenerate pump-probe technique. Varying the chirped condition of excited pulse from negative to positive increases the carrier relaxation time so as to modify the dispersion and reshape current pulse in time domain. The spectral dependence of carrier dynamics is analytically derived and explained by Shockley-Read Hall model. This observation enables the new feasibility of controlling carrier dynamics in ultrafast optical devices via the chirped pulse excitations.

  17. Photodissociation dynamics of hydroxybenzoic acids

    SciTech Connect (OSTI)

    Yang Yilin; Dyakov, Yuri; Lee, Y. T.; Ni, Chi-Kung; Sun Yilun; Hu Weiping

    2011-01-21

    Aromatic amino acids have large UV absorption cross-sections and low fluorescence quantum yields. Ultrafast internal conversion, which transforms electronic excitation energy to vibrational energy, was assumed to account for the photostability of amino acids. Recent theoretical and experimental investigations suggested that low fluorescence quantum yields of phenol (chromophore of tyrosine) are due to the dissociation from a repulsive excited state. Radicals generated from dissociation may undergo undesired reactions. It contradicts the observed photostability of amino acids. In this work, we explored the photodissociation dynamics of the tyrosine chromophores, 2-, 3- and 4-hydroxybenzoic acid in a molecular beam at 193 nm using multimass ion imaging techniques. We demonstrated that dissociation from the excited state is effectively quenched for the conformers of hydroxybenzoic acids with intramolecular hydrogen bonding. Ab initio calculations show that the excited state and the ground state potential energy surfaces change significantly for the conformers with intramolecular hydrogen bonding. It shows the importance of intramolecular hydrogen bond in the excited state dynamics and provides an alternative molecular mechanism for the photostability of aromatic amino acids upon irradiation of ultraviolet photons.

  18. Heterogeneous nucleation and growth dynamics in the light-induced phase transition in vanadium dioxide

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Brady, Nathaniel F.; Appavoo, Kannatassen; Seo, Minah; Nag, Joyeeta; Prasankumar, Rohit P.; Haglund, Richard F.; Hilton, David J.

    2016-03-02

    Here we report on ultrafast optical investigations of the light-induced insulator-to-metal phase transition in vanadium dioxide with controlled disorder generated by substrate mismatch. These results reveal common dynamics of this optically-induced phase transition that are independent of this disorder. Lastly, above the fluence threshold for completing the transition to the rutile crystalline phase, we find a common time scale, independent of sample morphology, of 40.5 ± 2 ps that is consistent with nucleation and growth dynamics of the R phase from the parent M1 ground state.

  19. Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Vortices Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic Vortices Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic Vortices Print Wednesday, 27 August 2008 00:00 Soft magnetic, micron-sized thin-film structures with magnetic vortices are intriguing systems that may one day be used in ultrafast computer memories. In such systems, the otherwise in-plane magnetization turns perpendicular to the plane at the center of the vortex, forming the vortex core.

  20. Atomistic Simulation of Nafion Membrane: 2. Dynamics of Water Molecules and Hydronium Ions

    SciTech Connect (OSTI)

    Devanathan, Ram; Venkatnathan, Arun; Dupuis, Michel

    2007-10-20

    We have performed a detailed and comprehensive analysis of the dynamics of water molecules and hydronium ions in hydrated Nafion using classical molecular dynamics simulations with the DREIDING force field. In addition to calculating diffusion coefficients as a function of hydration level, we have also determined mean residence time of H2O molecules and H3O+ ions in the first solvation shell of SO3- groups. The diffusion coefficient of H2O molecules increases with increasing hydration level and is in good agreement with experiment. The mean residence time of H2O molecules decreases with increasing membrane hydration from 1 ns at a low hydration level to 75 ps at the highest hydration level studied. These dynamical changes are related to the changes in membrane nanostructure reported in the first part of this work. Our results provide insights into slow proton dynamics observed in neutron scattering experiments and are consistent with the Gebel model of Nafion structure.

  1. Drama in Dynamics: Boom, Splash, and Speed

    SciTech Connect (OSTI)

    Heather Marie Netzloff

    2004-12-19

    The full nature of chemistry and physics cannot be captured by static calculations alone. Dynamics calculations allow the simulation of time-dependent phenomena. This facilitates both comparisons with experimental data and the prediction and interpretation of details not easily obtainable from experiments. Simulations thus provide a direct link between theory and experiment, between microscopic details of a system and macroscopic observed properties. Many types of dynamics calculations exist. The most important distinction between the methods and the decision of which method to use can be described in terms of the size and type of molecule/reaction under consideration and the type and level of accuracy required in the final properties of interest. These considerations must be balanced with available computational codes and resources as simulations to mimic ''real-life'' may require many time steps. As indicated in the title, the theme of this thesis is dynamics. The goal is to utilize the best type of dynamics for the system under study while trying to perform dynamics in the most accurate way possible. As a quantum chemist, this involves some level of first principles calculations by default. Very accurate calculations of small molecules and molecular systems are now possible with relatively high-level ab initio quantum chemistry. For example, a quantum chemical potential energy surface (PES) can be developed ''on-the-fly'' with dynamic reaction path (DRP) methods. In this way a classical trajectory is developed without prior knowledge of the PES. In order to treat solvation processes and the condensed phase, large numbers of molecules are required, especially in predicting bulk behavior. The Effective Fragment Potential (EFP) method for solvation decreases the cost of a fully quantum mechanical calculation by dividing a chemical system into an ab initio region that contains the solute and an ''effective fragment'' region that contains the remaining solvent

  2. Solvation of fluoro-acetonitrile in water by 2D-IR spectroscopy: A combined experimental-computational study

    SciTech Connect (OSTI)

    Cazade, Pierre-André; Das, Akshaya K.; Tran, Halina; Kläsi, Felix; Hamm, Peter; Bereau, Tristan; Meuwly, Markus

    2015-06-07

    The solvent dynamics around fluorinated acetonitrile is characterized by 2-dimensional infrared spectroscopy and atomistic simulations. The lineshape of the linear infrared spectrum is better captured by semiempirical (density functional tight binding) mixed quantum mechanical/molecular mechanics simulations, whereas force field simulations with multipolar interactions yield lineshapes that are significantly too narrow. For the solvent dynamics, a relatively slow time scale of 2 ps is found from the experiments and supported by the mixed quantum mechanical/molecular mechanics simulations. With multipolar force fields fitted to the available thermodynamical data, the time scale is considerably faster—on the 0.5 ps time scale. The simulations provide evidence for a well established CF–HOH hydrogen bond (population of 25%) which is found from the radial distribution function g(r) from both, force field and quantum mechanics/molecular mechanics simulations.

  3. Surface modified CFx cathode material for ultrafast discharge and high energy density

    SciTech Connect (OSTI)

    Dai, Yang; Zhu, Yimei; Cai, Sendan; Wu, Lijun; Yang, Weijing; Xie, Jingying; Wen, Wen; Zheng, Jin-Cheng; Zheng, Yi

    2014-11-10

    Li/CFx primary possesses the highest energy density of 2180 W h kg⁻¹ among all primary lithium batteries. However, a key limitation for the utility of this type of battery is in its poor rate capability because the cathode material, CFx, is an intrinsically poor electronic conductor. Here, we report on our development of a controlled process of surface de-fluorination under mild hydrothermal conditions to modify the highly fluorinated CFx. The modified CFx, consisting of an in situ generated shell component of F-graphene layers, possesses good electronic conductivity and removes the transporting barrier for lithium ions, yielding a high-capacity performance and an excellent rate-capability. Indeed, a capacity of 500 mA h g⁻¹ and a maximum power density of 44 800 W kg⁻¹ can be realized at the ultrafast rate of 30 C (24 A g⁻¹), which is over one order of magnitude higher than that of the state-of-the-art primary lithium-ion batteries.

  4. Surface modified CFx cathode material for ultrafast discharge and high energy density

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Dai, Yang; Zhu, Yimei; Cai, Sendan; Wu, Lijun; Yang, Weijing; Xie, Jingying; Wen, Wen; Zheng, Jin-Cheng; Zheng, Yi

    2014-11-10

    Li/CFx primary possesses the highest energy density of 2180 W h kg⁻¹ among all primary lithium batteries. However, a key limitation for the utility of this type of battery is in its poor rate capability because the cathode material, CFx, is an intrinsically poor electronic conductor. Here, we report on our development of a controlled process of surface de-fluorination under mild hydrothermal conditions to modify the highly fluorinated CFx. The modified CFx, consisting of an in situ generated shell component of F-graphene layers, possesses good electronic conductivity and removes the transporting barrier for lithium ions, yielding a high-capacity performance andmore » an excellent rate-capability. Indeed, a capacity of 500 mA h g⁻¹ and a maximum power density of 44 800 W kg⁻¹ can be realized at the ultrafast rate of 30 C (24 A g⁻¹), which is over one order of magnitude higher than that of the state-of-the-art primary lithium-ion batteries.« less

  5. Phase-contrast imaging using ultrafast x-rays in laser-shocked materials

    SciTech Connect (OSTI)

    Workman, Jonathan B; Cobble, James A; Flippo, Kirk; Gautier, Donald C; Montgomery, David S; Offermann, Dustin T

    2010-01-01

    High-energy x-rays, > 10-keV, can be efficiently produced from ultrafast laser target interactions with many applications to dense target materials in Inertial Confinement Fusion (ICF) and High-Energy Density Physics (HEDP). These same x-rays can also be applied to measurements of low-density materials inside high-density hohlraum environments. In the experiments presented, high-energy x-ray images of laser-shocked polystyrene are produced through phase contrast imaging. The plastic targets are nominally transparent to traditional x-ray absorption but show detailed features in regions of high density gradients due to refractive effects often called phase contrast imaging. The 200-TW Trident laser is used both to produce the x-ray source and to shock the polystyrene target. X-rays at 17-keV produced from 2-ps, 100-J laser interactions with a 12-micron molybdenum wire are used to produce a small source size, required for optimizing refractive effects. Shocks are driven in the 1-mm thick polystyrene target using 2-ns, 250-J, 532-nm laser drive with phase plates. X-ray images of shocks compare well to 1-D hydro calculations, HELIOS-CR.

  6. Ultrafast and Highly Reversible Sodium Storage in Zinc-Antimony Intermetallic Nanomaterials

    SciTech Connect (OSTI)

    Nie, Anmin; Gan, Li-yong; Cheng, Yingchun; Tao, Xinyong; Yuan, Yifei; Sharifi-Asl, Soroosh; He, Kun; Asayesh-Ardakani, Hasti; Vasiraju, Venkata; Lu, Jun; Mashayek, Farzad; Klie, Robert; Vaddiraju, Sreeram; Schwingenschlögl, Udo; Shahbazian-Yassar, Reza

    2015-12-17

    The progress on sodium-ion battery technology faces many grand challenges, one of which is the considerably lower rate of sodium insertion/deinsertion in electrode materials due to the larger size of sodium (Na) ions and complicated redox reactions compared to the lithium-ion systems. Here, it is demonstrated that sodium ions can be reversibly stored in Zn-Sb intermetallic nanowires at speeds that can exceed 295 nm s-1. Remarkably, these values are one to three orders of magnitude higher than the sodiation rate of other nanowires electrochemically tested with in situ transmission electron micro­scopy. It is found that the nanowires display about 161% volume expansion after the first sodiation and then cycle with an 83% reversible volume expansion. Despite their massive expansion, the nanowires can be cycled without any cracking or facture during the ultrafast sodiation/desodiation process. Additionally, most of the phases involved in the sodiation/desodiation process possess high electrical conductivity. More specifically, the NaZnSb exhibits a layered structure, which provides channels for fast Na+ diffusion. This observation indicates that Zn-Sb intermetallic nanomaterials offer great promise as high rate and good cycling stability anodic materials for the next generation of sodium-ion batteries.

  7. Ultrafast nanolaser device for detecting cancer in a single live cell.

    SciTech Connect (OSTI)

    Gourley, Paul Lee; McDonald, Anthony Eugene

    2007-11-01

    Emerging BioMicroNanotechnologies have the potential to provide accurate, realtime, high throughput screening of live tumor cells without invasive chemical reagents when coupled with ultrafast laser methods. These optically based methods are critical to advancing early detection, diagnosis, and treatment of disease. The first year goals of this project are to develop a laser-based imaging system integrated with an in- vitro, live-cell, micro-culture to study mammalian cells under controlled conditions. In the second year, the system will be used to elucidate the morphology and distribution of mitochondria in the normal cell respiration state and in the disease state for normal and disease states of the cell. In this work we designed and built an in-vitro, live-cell culture microsystem to study mammalian cells under controlled conditions of pH, temp, CO2, Ox, humidity, on engineered material surfaces. We demonstrated viability of cell culture in the microsystem by showing that cells retain healthy growth rates, exhibit normal morphology, and grow to confluence without blebbing or other adverse influences of the material surfaces. We also demonstrated the feasibility of integrating the culture microsystem with laser-imaging and performed nanolaser flow spectrocytometry to carry out analysis of the cells isolated mitochondria.

  8. The Influence of Chain Dynamics on the Far Infrared Spectrum of Liquid Methanol-Water Mixtures

    SciTech Connect (OSTI)

    Woods, K.N.; Wiedemann, H.; /SLAC, SSRL

    2005-07-12

    Far-infrared absorption spectroscopy has been used to study the low frequency ({center_dot} 100 cm{sup -1}) intermolecular modes of methanol in mixtures with water. With the aid of a first principles molecular dynamics simulation on an equivalent system, a detailed understanding about the origin of the low frequency IR modes has been established. The total dipole spectrum from the simulation suggests that the bands appearing in the experimental spectra at approximately 55 cm{sup -1} and 70 cm{sup -1} in methanol and methanol-rich mixtures arise from both fluctuations and torsional motions occurring within the methanol hydrogen-bonded chains. The influence of these modes on both the solvation dynamics and the relaxation mechanisms in the liquid are discussed within the context of recent experimental and theoretical results that have emerged from studies focusing on the short time dynamics in the methanol hydrogen bond network.

  9. Synthesis and Structural Features of [4,4'-Diisopropoxyester-2,2'-bipyridine], [Dichloro(4,4'-diisopropoxyester-2,2'-bi-pyridine)-platinum(ii)] and Its Dichloromethane Solvated Pseudo-Polymorph: Versatile Supramolecular Interactions

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Browning, Charles; Nesterov, Vladimir N.; Wang, Xiaoping; Omary, Mohammad A.

    2015-06-03

    We report that the organic ligand 4,4'-diisopropoxyester-2,2'-bipyridine, C18H20N2O4 (1), crystallizes in the triclinic crystal system P-1 and the molecule occupies a special position in the unit cell. In the crystal, molecules form stacks with partial overlapping of the pyridine rings. The Pt(II) dichloro complex of 1 crystallizes from a mixture of ethanol/hexane and from dichloromethane to form orange and yellow crystals, respectively. The orange non-solvated crystals of the (bipyridine)(dichloro)platinum(II) complex C18H20N2O4PtCl2 (2) crystallize in the triclinic crystal system P-1 as well with two independent molecules in the unit cell. In the crystal packing, molecules form two types of dimers withmore » Pt1 ··· Pt1A and Pt2···Pt2A distances of 3.478 and 5.186 angstrom respectively. The yellow crystals, as a solvated pseudo-polymorph C18H20N2O4PtCl2·1.5 CH2Cl2 (3) also crystallize in the triclinic crystal system P-1 with two independent molecules in the unit cell. In the crystal packing, molecules form Pt2 ···Pt1 ···Pt1A ···Pt2A intermolecular contacts with alternating distances 3.501 and 3.431 angstrom, respectively, forming infinite chains. Graphical Abstract The dichloro(bipyridine)platinum complex, dichloro(4,4'-diisopropoxyester-2,2'-bipyridine)platinum(II), forms single crystals as a stable non-solvated form and a solvated polymorph with dramatically different supramolecular structure and short contacts.« less

  10. Modeling nanoscale hydrodynamics by smoothed dissipative particle dynamics

    SciTech Connect (OSTI)

    Lei, Huan; Mundy, Christopher J.; Schenter, Gregory K.; Voulgarakis, Nikolaos

    2015-05-21

    Thermal fluctuation and hydrophobicity are two hallmarks of fluid hydrodynamics on the nano-scale. It is a challenge to consistently couple the small length and time scale phenomena associated with molecular interaction with larger scale phenomena. The development of this consistency is the essence of mesoscale science. In this study, we develop a nanoscale fluid model based on smoothed dissipative particle dynamics that accounts for the phenomena of associated with density fluctuations and hydrophobicity. We show consistency in the fluctuation spectrum across scales. In doing so, it is necessary to account for finite fluid particle size. Furthermore, we demonstrate that the present model can capture of the void probability and solvation free energy of apolar particles of different sizes. The present fluid model is well suited for a understanding emergent phenomena in nano-scale fluid systems.

  11. Quantum dynamics of solid Ne upon photo-excitation of a NO impurity: A Gaussian wave packet approach

    SciTech Connect (OSTI)

    Unn-Toc, W.; Meier, C.; Halberstadt, N.; Uranga-Pina, Ll.; Rubayo-Soneira, J.

    2012-08-07

    A high-dimensional quantum wave packet approach based on Gaussian wave packets in Cartesian coordinates is presented. In this method, the high-dimensional wave packet is expressed as a product of time-dependent complex Gaussian functions, which describe the motion of individual atoms. It is applied to the ultrafast geometrical rearrangement dynamics of NO doped cryogenic Ne matrices after femtosecond laser pulse excitation. The static deformation of the solid due to the impurity as well as the dynamical response after femtosecond excitation are analyzed and compared to reduced dimensionality studies. The advantages and limitations of this method are analyzed in the perspective of future applications to other quantum solids.

  12. Structure and dynamics of aqueous solution of uranyl ions

    SciTech Connect (OSTI)

    Chopra, Manish; Choudhury, Niharendu

    2014-04-24

    The present work describes a molecular dynamics simulation study of structure and dynamics of aqueous solution of uranyl ions in water. Structural properties of the system in terms of radial distribution functions and dynamical characteristics as obtained through velocity autocorrelation function and mean square displacements have been analyzed. The results for radial distribution functions show the oxygen of water to form the first solvation shell at 2.4 around the uranium atom, whereas the hydrogen atoms of water are distributed around the uranium atom with the major peak at around 3.0 . Analyses of transport behaviors of ions and water through MSD indicates that the diffusion of the uranyl ion is much less as compared to that of the water molecules. It is also observed that the dynamical behavior of water molecules gets modified due to the presence of uranyl ion. The effect of increase in concentration of uranyl ions on the structure and dynamics of water molecules is also studied.

  13. Water adsorption, solvation and deliquescence of alkali halide thin films on SiO2 studied by ambient pressure X-ray photoelectron spectroscopy

    SciTech Connect (OSTI)

    Arima, Kenta; Jiang, Peng; Deng, Xingyi; Bluhm, Henrik; Salmeron, Miquel

    2010-03-31

    The adsorption of water on KBr thin films evaporated onto SiO2 was investigated as a function of relative humidity (RH) by ambient pressure X-ray photoelectron spectroscopy. At 30percent RH adsorbed water reaches a coverage of approximately one monolayer. As the humidity continues to increase, the coverage of water remains constant or increases very slowly until 60percent RH, followed by a rapid increase up to 100percent RH. At low RH a significant number of the Br atoms are lost due to irradiation damage. With increasing humidity solvation increases ion mobility and gives rise to a partial recovery of the Br/K ratio. Above 60percent RH the increase of the Br/K ratio accelerates. Above the deliquescence point (85percent RH), the thickness of the water layer continues to increase and reaches more than three layers near saturation. The enhancement of the Br/K ratio at this stage is roughly a factor 2.3 on a 0.5 nm KBr film, indicating a strong preferential segregation of Br ions to the surface of the thin saline solution on SiO2.

  14. Ultrafast dark-field surface inspection with hybrid-dispersion laser scanning

    SciTech Connect (OSTI)

    Yazaki, Akio; Kim, Chanju; Chan, Jacky; Mahjoubfar, Ata; Goda, Keisuke; Watanabe, Masahiro; Jalali, Bahram

    2014-06-23

    High-speed surface inspection plays an important role in industrial manufacturing, safety monitoring, and quality control. It is desirable to go beyond the speed limitation of current technologies for reducing manufacturing costs and opening a new window onto a class of applications that require high-throughput sensing. Here, we report a high-speed dark-field surface inspector for detection of micrometer-sized surface defects that can travel at a record high speed as high as a few kilometers per second. This method is based on a modified time-stretch microscope that illuminates temporally and spatially dispersed laser pulses on the surface of a fast-moving object and detects scattered light from defects on the surface with a sensitive photodetector in a dark-field configuration. The inspector's ability to perform ultrafast dark-field surface inspection enables real-time identification of difficult-to-detect features on weakly reflecting surfaces and hence renders the method much more practical than in the previously demonstrated bright-field configuration. Consequently, our inspector provides nearly 1000 times higher scanning speed than conventional inspectors. To show our method's broad utility, we demonstrate real-time inspection of the surface of various objects (a non-reflective black film, transparent flexible film, and reflective hard disk) for detection of 10??m or smaller defects on a moving target at 20?m/s within a scan width of 25?mm at a scan rate of 90.9?MHz. Our method holds promise for improving the cost and performance of organic light-emitting diode displays for next-generation smart phones, lithium-ion batteries for green electronics, and high-efficiency solar cells.

  15. Laser plasma x-ray source for ultrafast time-resolved x-ray absorption spectroscopy

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Miaja-Avila, L.; O'Neil, G. C.; Uhlig, J.; Cromer, C. L.; Dowell, M. L.; Jimenez, R.; Hoover, A. S.; Silverman, K. L.; Ullom, J. N.

    2015-03-02

    We describe a laser-driven x-ray plasma source designed for ultrafast x-ray absorption spectroscopy. The source is comprised of a 1 kHz, 20 W, femtosecond pulsed infrared laser and a water target. We present the x-ray spectra as a function of laser energy and pulse duration. Additionally, we investigate the plasma temperature and photon flux as we vary the laser energy. We obtain a 75 μm FWHM x-ray spot size, containing ~106 photons/s, by focusing the produced x-rays with a polycapillary optic. Since the acquisition of x-ray absorption spectra requires the averaging of measurements from >107 laser pulses, we also presentmore » data on the source stability, including single pulse measurements of the x-ray yield and the x-ray spectral shape. In single pulse measurements, the x-ray flux has a measured standard deviation of 8%, where the laser pointing is the main cause of variability. Further, we show that the variability in x-ray spectral shape from single pulses is low, thus justifying the combining of x-rays obtained from different laser pulses into a single spectrum. Finally, we show a static x-ray absorption spectrum of a ferrioxalate solution as detected by a microcalorimeter array. Altogether, our results demonstrate that this water-jet based plasma source is a suitable candidate for laboratory-based time-resolved x-ray absorption spectroscopy experiments.« less

  16. Laser plasma x-ray source for ultrafast time-resolved x-ray absorption spectroscopy

    SciTech Connect (OSTI)

    Miaja-Avila, L.; O'Neil, G. C.; Uhlig, J.; Cromer, C. L.; Dowell, M. L.; Jimenez, R.; Hoover, A. S.; Silverman, K. L.; Ullom, J. N.

    2015-03-02

    We describe a laser-driven x-ray plasma source designed for ultrafast x-ray absorption spectroscopy. The source is comprised of a 1 kHz, 20 W, femtosecond pulsed infrared laser and a water target. We present the x-ray spectra as a function of laser energy and pulse duration. Additionally, we investigate the plasma temperature and photon flux as we vary the laser energy. We obtain a 75 μm FWHM x-ray spot size, containing ~106 photons/s, by focusing the produced x-rays with a polycapillary optic. Since the acquisition of x-ray absorption spectra requires the averaging of measurements from >107 laser pulses, we also present data on the source stability, including single pulse measurements of the x-ray yield and the x-ray spectral shape. In single pulse measurements, the x-ray flux has a measured standard deviation of 8%, where the laser pointing is the main cause of variability. Further, we show that the variability in x-ray spectral shape from single pulses is low, thus justifying the combining of x-rays obtained from different laser pulses into a single spectrum. Finally, we show a static x-ray absorption spectrum of a ferrioxalate solution as detected by a microcalorimeter array. Altogether, our results demonstrate that this water-jet based plasma source is a suitable candidate for laboratory-based time-resolved x-ray absorption spectroscopy experiments.

  17. Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Vortices Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic Vortices Print Soft magnetic, micron-sized thin-film structures with magnetic vortices are intriguing systems that may one day be used in ultrafast computer memories. In such systems, the otherwise in-plane magnetization turns perpendicular to the plane at the center of the vortex, forming the vortex core. Because such a core has two possible polarizations (up or down) and can be switched between these two states

  18. Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Vortices Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic Vortices Print Soft magnetic, micron-sized thin-film structures with magnetic vortices are intriguing systems that may one day be used in ultrafast computer memories. In such systems, the otherwise in-plane magnetization turns perpendicular to the plane at the center of the vortex, forming the vortex core. Because such a core has two possible polarizations (up or down) and can be switched between these two states

  19. Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Vortices Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic Vortices Print Soft magnetic, micron-sized thin-film structures with magnetic vortices are intriguing systems that may one day be used in ultrafast computer memories. In such systems, the otherwise in-plane magnetization turns perpendicular to the plane at the center of the vortex, forming the vortex core. Because such a core has two possible polarizations (up or down) and can be switched between these two states

  20. Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Vortices Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic Vortices Print Soft magnetic, micron-sized thin-film structures with magnetic vortices are intriguing systems that may one day be used in ultrafast computer memories. In such systems, the otherwise in-plane magnetization turns perpendicular to the plane at the center of the vortex, forming the vortex core. Because such a core has two possible polarizations (up or down) and can be switched between these two states

  1. Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Vortices Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic Vortices Print Soft magnetic, micron-sized thin-film structures with magnetic vortices are intriguing systems that may one day be used in ultrafast computer memories. In such systems, the otherwise in-plane magnetization turns perpendicular to the plane at the center of the vortex, forming the vortex core. Because such a core has two possible polarizations (up or down) and can be switched between these two states

  2. Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Vortices Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic Vortices Print Soft magnetic, micron-sized thin-film structures with magnetic vortices are intriguing systems that may one day be used in ultrafast computer memories. In such systems, the otherwise in-plane magnetization turns perpendicular to the plane at the center of the vortex, forming the vortex core. Because such a core has two possible polarizations (up or down) and can be switched between these two states

  3. Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Vortices Influence of Domain Wall Pinning on the Dynamic Behavior of Magnetic Vortices Print Soft magnetic, micron-sized thin-film structures with magnetic vortices are intriguing systems that may one day be used in ultrafast computer memories. In such systems, the otherwise in-plane magnetization turns perpendicular to the plane at the center of the vortex, forming the vortex core. Because such a core has two possible polarizations (up or down) and can be switched between these two states

  4. Constructing Surrogate Models of Complex Systems with Enhanced Sparsity: Quantifying the Influence of Conformational Uncertainty in Biomolecular Solvation

    SciTech Connect (OSTI)

    Lei, Huan; Yang, Xiu; Zheng, Bin; Lin, Guang; Baker, Nathan A.

    2015-12-31

    Biomolecules exhibit conformational fluctuations near equilibrium states, inducing uncertainty in various biological properties in a dynamic way. We have developed a general method to quantify the uncertainty of target properties induced by conformational fluctuations. Using a generalized polynomial chaos (gPC) expansion, we construct a surrogate model of the target property with respect to varying conformational states. We also propose a method to increase the sparsity of the gPC expansion by defining a set of conformational “active space” random variables. With the increased sparsity, we employ the compressive sensing method to accurately construct the surrogate model. We demonstrate the performance of the surrogate model by evaluating fluctuation-induced uncertainty in solvent-accessible surface area for the bovine trypsin inhibitor protein system and show that the new approach offers more accurate statistical information than standard Monte Carlo approaches. Further more, the constructed surrogate model also enables us to directly evaluate the target property under various conformational states, yielding a more accurate response surface than standard sparse grid collocation methods. In particular, the new method provides higher accuracy in high-dimensional systems, such as biomolecules, where sparse grid performance is limited by the accuracy of the computed quantity of interest. Our new framework is generalizable and can be used to investigate the uncertainty of a wide variety of target properties in biomolecular systems.

  5. Ultra-fast Laser Synthesis of Nanopore Arrays in Silicon for Bio-molecule Separation and Detection

    SciTech Connect (OSTI)

    Tringe, J W; Ileri, N; Letant, S E; Stroeve, P; Shirk, M; Zaidi, S; Balhorn, R L; Siders, C W

    2008-02-07

    We demonstrate that interference of ultra-fast pulses of laser light can create regular patterns in thin silicon membranes that are compatible with the formation of a uniform array of nanopores. The spacing and size of these pores can be tuned by changing the laser energy, wavelength and number of ultra-short pulses. Short pulses and wavelengths ({approx}550 nm and smaller) are needed to define controllable nanoscale features in silicon. Energy must be localized in time and space to produce the etching, ablation or amorphization effects over the {approx}100 nm length scales appropriate for definition of single pores. Although in this brief study pattern uniformity was limited by laser beam quality, a complementary demonstration reported here used continuous-wave interferometric laser exposure of photoresist to show the promise of the ultra-fast approach for producing uniform pore arrays. The diameters of these interferometrically-defined features are significantly more uniform than the diameters of pores in state-of-the-art polycarbonate track etch membranes widely used for molecular separations.

  6. Polarizability effects on the structure and dynamics of ionic liquids

    SciTech Connect (OSTI)

    Cavalcante, Ary de Oliveira; Ribeiro, Mauro C. C.; Skaf, Munir S.

    2014-04-14

    Polarization effects on the structure and dynamics of ionic liquids are investigated using molecular dynamics simulations. Four different ionic liquids were simulated, formed by the anions Cl{sup ?} and PF{sub 6}{sup ?}, treated as single fixed charge sites, and the 1-n-alkyl-3-methylimidazolium cations (1-ethyl and 1-butyl-), which are polarizable. The partial charge fluctuation of the cations is provided by the electronegativity equalization model (EEM) and a complete parameter set for the cations electronegativity (?) and hardness (J) is presented. Results obtained from a non-polarizable model for the cations are also reported for comparison. Relative to the fixed charged model, the equilibrium structure of the first solvation shell around the imidazolium cations shows that inclusion of EEM polarization forces brings cations closer to each other and that anions are preferentially distributed above and below the plane of the imidazolium ring. The polarizable model yields faster translational and reorientational dynamics than the fixed charges model in the rotational-diffusion regime. In this sense, the polarizable model dynamics is in better agreement with the experimental data.

  7. Luminescence dynamics of bound exciton of hydrogen doped ZnO nanowires

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Yoo, Jinkyoung; Yi, Gyu -Chul; Chon, Bonghwan; Joo, Taiha; Wang, Zhehui

    2016-04-11

    In this study, all-optical camera, converting X-rays into visible photons, is a promising strategy for high-performance X-ray imaging detector requiring high detection efficiency and ultrafast detector response time. Zinc oxide is a suitable material for all-optical camera due to its fast radiative recombination lifetime in sub-nanosecond regime and its radiation hardness. ZnO nanostructures have been considered as proper building blocks for ultrafast detectors with spatial resolution in sub-micrometer scale. To achieve remarkable enhancement of luminescence efficiency n-type doping in ZnO has been employed. However, luminescence dynamics of doped ZnO nanostructures have not been thoroughly investigated whereas undoped ZnO nanostructures havemore » been employed to study their luminescence dynamics. Here we report a study of luminescence dynamics of hydrogen doped ZnO nanowires obtained by hydrogen plasma treatment. Hydrogen doping in ZnO nanowires gives rise to significant increase in the near-band-edge emission of ZnO and decrease in averaged photoluminescence lifetime from 300 to 140 ps at 10 K. The effects of hydrogen doping on the luminescent characteristics of ZnO nanowires were changed by hydrogen doping process variables.« less

  8. Large-Scale First-Principles Molecular Dynamics Simulations with Electrostatic Embedding: Application to Acetylcholinesterase Catalysis

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Fattebert, Jean-Luc; Lau, Edmond Y.; Bennion, Brian J.; Huang, Patrick; Lightstone, Felice C.

    2015-10-22

    Enzymes are complicated solvated systems that typically require many atoms to simulate their function with any degree of accuracy. We have recently developed numerical techniques for large scale First-Principles molecular dynamics simulations and applied them to study the enzymatic reaction catalyzed by acetylcholinesterase. We carried out Density functional theory calculations for a quantum mechanical (QM) sub- system consisting of 612 atoms with an O(N) complexity finite-difference approach. The QM sub-system is embedded inside an external potential field representing the electrostatic effect due to the environment. We obtained finite temperature sampling by First-Principles molecular dynamics for the acylation reaction of acetylcholinemore » catalyzed by acetylcholinesterase. Our calculations shows two energies barriers along the reaction coordinate for the enzyme catalyzed acylation of acetylcholine. In conclusion, the second barrier (8.5 kcal/mole) is rate-limiting for the acylation reaction and in good agreement with experiment.« less

  9. Large-Scale First-Principles Molecular Dynamics Simulations with Electrostatic Embedding: Application to Acetylcholinesterase Catalysis

    SciTech Connect (OSTI)

    Fattebert, Jean-Luc; Lau, Edmond Y.; Bennion, Brian J.; Huang, Patrick; Lightstone, Felice C.

    2015-10-22

    Enzymes are complicated solvated systems that typically require many atoms to simulate their function with any degree of accuracy. We have recently developed numerical techniques for large scale First-Principles molecular dynamics simulations and applied them to study the enzymatic reaction catalyzed by acetylcholinesterase. We carried out Density functional theory calculations for a quantum mechanical (QM) sub- system consisting of 612 atoms with an O(N) complexity finite-difference approach. The QM sub-system is embedded inside an external potential field representing the electrostatic effect due to the environment. We obtained finite temperature sampling by First-Principles molecular dynamics for the acylation reaction of acetylcholine catalyzed by acetylcholinesterase. Our calculations shows two energies barriers along the reaction coordinate for the enzyme catalyzed acylation of acetylcholine. In conclusion, the second barrier (8.5 kcal/mole) is rate-limiting for the acylation reaction and in good agreement with experiment.

  10. Structural dynamics in complex liquids studied with multidimensional vibrational spectroscopy

    SciTech Connect (OSTI)

    Tokmakoff, Andrei

    2013-08-31

    The development of new sustainable energy sources is linked to our understanding of the molecular properties of water and aqueous solutions. Energy conversion, storage, and transduction processes, particularly those that occur in biology, fuel cells, and batteries, make use of water for the purpose of moving energy in the form of charges and mediating the redox chemistry that allows this energy to be stored as and released from chemical bonds. To build our fundamental knowledge in this area, this project supports work in the Tokmakoff group to investigate the molecular dynamics of water’s hydrogen bond network, and how these dynamics influence its solutes and the mechanism of proton transport in water. To reach the goals of this grant, we developed experiments to observe molecular dynamics in water as directly as possible, using ultrafast multidimensional vibrational spectroscopy. We excite and probe broad vibrational resonances of water, molecular solutes, and protons in water. By correlating how molecules evolve from an initial excitation frequency to a final frequency, we can describe the underlying molecular dynamics. Theoretical modeling of the data with the help of computational spectroscopy coupled with molecular dynamics simulations provided the atomistic insight in these studies.

  11. Origin and dynamics of vortex rings in drop splashing

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Lee, Ji San; Park, Su Ji; Lee, Jun Ho; Weon, Byung Mook; Fezzaa, Kamel; Je, Jung Ho

    2015-09-04

    A vortex is a flow phenomenon that is very commonly observed in nature. More than a century, a vortex ring that forms during drop splashing has caught the attention of many scientists due to its importance in understanding fluid mixing and mass transport processes. However, the origin of the vortices and their dynamics remain unclear, mostly due to the lack of appropriate visualization methods. Here, with ultrafast X-ray phase-contrast imaging, we show that the formation of vortex rings originates from the energy transfer by capillary waves generated at the moment of the drop impact. Interestingly, we find a row ofmore » vortex rings along the drop wall, as demonstrated by a phase diagram established here, with different power-law dependencies of the angular velocities on the Reynolds number. These results provide important insight that allows understanding and modelling any type of vortex rings in nature, beyond just vortex rings during drop splashing.« less

  12. Origin and dynamics of vortex rings in drop splashing

    SciTech Connect (OSTI)

    Lee, Ji San; Park, Su Ji; Lee, Jun Ho; Weon, Byung Mook; Fezzaa, Kamel; Je, Jung Ho

    2015-09-04

    A vortex is a flow phenomenon that is very commonly observed in nature. More than a century, a vortex ring that forms during drop splashing has caught the attention of many scientists due to its importance in understanding fluid mixing and mass transport processes. However, the origin of the vortices and their dynamics remain unclear, mostly due to the lack of appropriate visualization methods. Here, with ultrafast X-ray phase-contrast imaging, we show that the formation of vortex rings originates from the energy transfer by capillary waves generated at the moment of the drop impact. Interestingly, we find a row of vortex rings along the drop wall, as demonstrated by a phase diagram established here, with different power-law dependencies of the angular velocities on the Reynolds number. These results provide important insight that allows understanding and modelling any type of vortex rings in nature, beyond just vortex rings during drop splashing.

  13. Water exchange dynamics around H?O? and OH? ions

    SciTech Connect (OSTI)

    Roy, Santanu; Dang, Liem X.

    2015-05-01

    Proton transfer in water and other solvents is a complicated process and an active research area. Conformational changes of water hydrating a proton can have a significant influence on proton dynamics. A hydrated proton leads to H?O? that forms three hydrogen bonds with neighboring water molecules. In this letter, we report the first computer simulation of the dynamics of water exchanging between the first and second solvation shells of H?O?. Employing different rate theories for chemical reactions such as the transition state theory, the Grote-Hynes theory, the reactive flux method, and the Impey-Madden-McDonald method, we calculate the solvent exchange rates from molecular dynamics simulations that account for explicit polarization effects. In addition, we also study water exchanges around OH? and find that the corresponding time scale (~50 picoseconds [ps]) is much smaller than that for H?O? (~100 ps). Results from all the rate theories are computed and compared. This work was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. The calculations were carried out using computer resources provided by the Office of Basic Energy Sciences.

  14. Ultrafast time-resolved spectroscopy of the light-harvesting complex 2 (LH2) from the photosynthetic bacterium Thermochromatium tepidum

    SciTech Connect (OSTI)

    Niedzwiedzki, Dariusz M.; Fuciman, Marcel; Kobayashi, Masayuki; Frank, Harry A.; Blankenship, Robert E.

    2011-10-08

    The light-harvesting complex 2 from the thermophilic purple bacterium Thermochromatium tepidum was purified and studied by steady-state absorption and fluorescence, sub-nanosecond-time-resolved fluorescence and femtosecond time-resolved transient absorption spectroscopy. The measurements were performed at room temperature and at 10 K. The combination of both ultrafast and steady-state optical spectroscopy methods at ambient and cryogenic temperatures allowed the detailed study of carotenoid (Car)-to-bacteriochlorophyll (BChl) as well BChl-to-BChl excitation energy transfer in the complex. The studies show that the dominant Cars rhodopin (N = 11) and spirilloxanthin (N = 13) do not play a significant role as supportive energy donors for BChl a. This is related with their photophysical properties regulated by long ?-electron conjugation. On the other hand, such properties favor some of the Cars, particularly spirilloxanthin (N = 13) to play the role of the direct quencher of the excited singlet state of BChl.

  15. High quality single shot ultrafast MeV electron diffraction from a photocathode radio-frequency gun

    SciTech Connect (OSTI)

    Fu, Feichao; Liu, Shengguang; Zhu, Pengfei; Xiang, Dao Zhang, Jie; Cao, Jianming

    2014-08-15

    A compact ultrafast electron diffractometer, consisting of an s-band 1.6 cell photocathode radio-frequency gun, a multi-function changeable sample chamber, and a sensitive relativistic electron detector, was built at Shanghai Jiao Tong University. High-quality single-shot transmission electron diffraction patterns have been recorded by scattering 2.5 MeV electrons off single crystalline gold and polycrystalline aluminum samples. The high quality diffraction pattern indicates an excellent spatial resolution, with the ratio of the diffraction ring radius over the ring rms width beyond 10. The electron pulse width is estimated to be about 300 fs. The high temporal and spatial resolution may open new opportunities in various areas of sciences.

  16. Cost effective nanostructured copper substrates prepared with ultrafast laser pulses for explosives detection using surface enhanced Raman scattering

    SciTech Connect (OSTI)

    Hamad, Syed; Podagatlapalli, G. Krishna; Soma, Venugopal Rao E-mail: soma-venu@yahoo.com; Mohiddon, Md. Ahamad

    2014-06-30

    Ultrafast laser pulses induced surface nanostructures were fabricated on a copper (Cu) target through ablation in acetone, dichloromethane, acetonitrile, and chloroform. Surface morphological information accomplished from the field emission scanning electron microscopic data demonstrated the diversities of ablation mechanism in each case. Fabricated Cu substrates were utilized exultantly to investigate the surface plasmon (localized and propagating) mediated enhancements of different analytes using surface enhance Raman scattering (SERS) studies. Multiple utility of these substrates were efficiently demonstrated by collecting the SERS data of Rhodamine 6G molecule and two different secondary explosive molecules such as 5-amino-3-nitro-l,2,4-triazole and trinitrotoluene on different days which were weeks apart. We achieved significant enhancement factors of >10{sup 5} through an easily adoptable cleaning procedure.

  17. System and method for ultrafast optical signal detecting via a synchronously coupled anamorphic light pulse encoded laterally

    DOE Patents [OSTI]

    Heebner, John E.

    2010-08-03

    In one general embodiment, a method for ultrafast optical signal detecting is provided. In operation, a first optical input signal is propagated through a first wave guiding layer of a waveguide. Additionally, a second optical input signal is propagated through a second wave guiding layer of the waveguide. Furthermore, an optical control signal is applied to a top of the waveguide, the optical control signal being oriented diagonally relative to the top of the waveguide such that the application is used to influence at least a portion of the first optical input signal propagating through the first wave guiding layer of the waveguide. In addition, the first and the second optical input signals output from the waveguide are combined. Further, the combined optical signals output from the waveguide are detected. In another general embodiment, a system for ultrafast optical signal recording is provided comprising a waveguide including a plurality of wave guiding layers, an optical control source positioned to propagate an optical control signal towards the waveguide in a diagonal orientation relative to a top of the waveguide, at least one optical input source positioned to input an optical input signal into at least a first and a second wave guiding layer of the waveguide, and a detector for detecting at least one interference pattern output from the waveguide, where at least one of the interference patterns results from a combination of the optical input signals input into the first and the second wave guiding layer. Furthermore, propagation of the optical control signal is used to influence at least a portion of the optical input signal propagating through the first wave guiding layer of the waveguide.

  18. Physical mechanisms of SiN{sub x} layer structuring with ultrafast lasers by direct and confined laser ablation

    SciTech Connect (OSTI)

    Rapp, S.; Heinrich, G.; Wollgarten, M.; Huber, H. P.; Schmidt, M.

    2015-03-14

    In the production process of silicon microelectronic devices and high efficiency silicon solar cells, local contact openings in thin dielectric layers are required. Instead of photolithography, these openings can be selectively structured with ultra-short laser pulses by confined laser ablation in a fast and efficient lift off production step. Thereby, the ultrafast laser pulse is transmitted by the dielectric layer and absorbed at the substrate surface leading to a selective layer removal in the nanosecond time domain. Thermal damage in the substrate due to absorption is an unwanted side effect. The aim of this work is to obtain a deeper understanding of the physical laser-material interaction with the goal of finding a damage-free ablation mechanism. For this, thin silicon nitride (SiN{sub x}) layers on planar silicon (Si) wafers are processed with infrared fs-laser pulses. Two ablation types can be distinguished: The known confined ablation at fluences below 300 mJ/cm{sup 2} and a combined partial confined and partial direct ablation at higher fluences. The partial direct ablation process is caused by nonlinear absorption in the SiN{sub x} layer in the center of the applied Gaussian shaped laser pulses. Pump-probe investigations of the central area show ultra-fast reflectivity changes typical for direct laser ablation. Transmission electron microscopy results demonstrate that the Si surface under the remaining SiN{sub x} island is not damaged by the laser ablation process. At optimized process parameters, the method of direct laser ablation could be a good candidate for damage-free selective structuring of dielectric layers on absorbing substrates.

  19. Towards simultaneous measurements of electronic and structural properties in ultra-fast x-ray free electron laser absorption spectroscopy experiments

    SciTech Connect (OSTI)

    Gaudin, J.; Fourment, C.; Cho, B. I.; Engelhorn, K.; Galtier, E.; Harmand, M.; Leguay, P. M.; Lee, H. J.; Nagler, B.; Nakatsutsumi, M.; Ozkan, C.; Strmer, M.; Toleikis, S.; Tschentscher, Th.; Heimann, P. A.; Dorchies, F.

    2014-04-17

    The rapidly growing ultrafast science with X-ray lasers unveils atomic scale processes with unprecedented time resolution bringing the so called molecular movie within reach. X-ray absorption spectroscopy is one of the most powerful x-ray techniques providing both local atomic order and electronic structure when coupled with ad-hoc theory. Collecting absorption spectra within few x-ray pulses is possible only in a dispersive setup. We demonstrate ultrafast time-resolved measurements of the LIII-edge x-ray absorption near-edge spectra of irreversibly laser excited Molybdenum using an average of only few x-ray pulses with a signal to noise ratio limited only by the saturation level of the detector. The simplicity of the experimental set-up makes this technique versatile and applicable for a wide range of pump-probe experiments, particularly in the case of non-reversible processes.

  20. Towards simultaneous measurements of electronic and structural properties in ultra-fast x-ray free electron laser absorption spectroscopy experiments

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Gaudin, J.; Fourment, C.; Cho, B. I.; Engelhorn, K.; Galtier, E.; Harmand, M.; Leguay, P. M.; Lee, H. J.; Nagler, B.; Nakatsutsumi, M.; et al

    2014-04-17

    The rapidly growing ultrafast science with X-ray lasers unveils atomic scale processes with unprecedented time resolution bringing the so called “molecular movie” within reach. X-ray absorption spectroscopy is one of the most powerful x-ray techniques providing both local atomic order and electronic structure when coupled with ad-hoc theory. Collecting absorption spectra within few x-ray pulses is possible only in a dispersive setup. We demonstrate ultrafast time-resolved measurements of the LIII-edge x-ray absorption near-edge spectra of irreversibly laser excited Molybdenum using an average of only few x-ray pulses with a signal to noise ratio limited only by the saturation level ofmore » the detector. The simplicity of the experimental set-up makes this technique versatile and applicable for a wide range of pump-probe experiments, particularly in the case of non-reversible processes.« less

  1. Ultrafast laser and swift heavy ion irradiation: Response of Gd{sub 2}O{sub 3} and ZrO{sub 2} to intense electronic excitation

    SciTech Connect (OSTI)

    Rittman, Dylan R.; Tracy, Cameron L.; Cusick, Alex B.; Abere, Michael J.; Yalisove, Steven M.; Torralva, Ben; Ewing, Rodney C.

    2015-04-27

    In order to investigate the response of materials to extreme conditions, there are several approaches to depositing extremely high concentrations of energy into very small volumes of material, including ultrafast laser and swift heavy ion (SHI) irradiation. In this study, crystalline-to-crystalline phase transformations in cubic Gd{sub 2}O{sub 3} and monoclinic ZrO{sub 2} have been investigated using ultrafast laser irradiation. The phases produced by the extreme conditions of irradiation were characterized by grazing incidence x-ray diffraction (GIXRD) and Raman spectroscopy. Gd{sub 2}O{sub 3} exhibited a cubic-to-monoclinic phase transformation, as evidenced by the appearance of the monoclinic (402{sup ¯}), (003), (310), and (112{sup ¯}) peaks in the GIXRD pattern and of four A{sub g} and three B{sub g} Raman modes. ZrO{sub 2} underwent a monoclinic-to-tetragonal phase transformation, as evidenced by the emergence of the tetragonal (101) peak in the GIXRD pattern and of E{sub g} and A{sub 1g} Raman modes. The new phases formed by ultrafast laser irradiation are high temperature polymorphs of the two materials. No evidence of amorphization was seen in the GIXRD data, though Raman spectroscopy indicated point defect accumulation. These results are identical to those produced by irradiation with SHIs, which also deposit energy in materials primarily through electronic excitation. The similarity in damage process and material response between ultrafast laser and SHI irradiation suggests a fundamental relationship between these two techniques.

  2. Dynamics of soft Nanomaterials captured by transmission electron microscopy in liquid water

    SciTech Connect (OSTI)

    Proetto, Maria T.; Rush, Anthony M.; Chien, Miao-Ping; Abellan Baeza, Patricia; Patterson, Joseph P.; Thompson, Matthew P.; Olson, Norman H.; Moore, Curtis E.; Rheingold, Arnold L.; Andolina, Christopher; Millstone, Jill; Howell, Stephen B.; Browning, Nigel D.; Evans, James E.; Gianneschi, Nathan C.

    2014-01-14

    In this paper we present in situ transmission electron microscopy (TEM) of soft, synthetic nanoparticles with a comparative analysis using conventional TEM methods. This comparison is made with the simple aim of describing what is an unprecedented example of in situ imaging by TEM. However, we contend the technique will quickly become essential in the characterization of analogous systems, especially where dynamics are of interest in the solvated state. In this case, particles were studied which were obtained from the direct polymerization of an oxaliplatin analog, designed for an ongoing program in novel chemotherapeutic delivery systems. The resulting nanoparticles provided sufficient contrast for facile imaging in situ, and point toward key design parameters that enable this new characterization approach for organic nanomaterials. We describe the preparation of the synthetic micellar nanoparticles to- gether with their characterization in liquid water.

  3. Fano resonance control in a photonic crystal structure and its application to ultrafast switching

    SciTech Connect (OSTI)

    Yu, Yi Heuck, Mikkel; Hu, Hao; Xue, Weiqi; Peucheret, Christophe; Chen, Yaohui; Oxenløwe, Leif Katsuo; Yvind, Kresten; Mørk, Jesper

    2014-08-11

    We experimentally demonstrate a photonic crystal structure that allows easy and robust control of the Fano spectrum. Its operation relies on controlling the amplitude of light propagating along one of the light paths in the structure from which the Fano resonance is obtained. Short-pulse dynamic measurements show that besides drastically increasing the switching contrast, the transmission dynamics itself is strongly affected by the nature of the resonance. The influence of slow-recovery tails implied by a long carrier lifetime can thus be reduced using a Fano resonance due to a hitherto unrecognized reshaping effect of the nonlinear Fano transfer function. As an example, we present a system application of a Fano structure, demonstrating its advantages by the experimental realization of 10 Gbit/s all-optical modulation with optical control power less than 1 mW.

  4. TH-A-18C-04: Ultrafast Cone-Beam CT Scatter Correction with GPU-Based Monte Carlo Simulation

    SciTech Connect (OSTI)

    Xu, Y; Bai, T; Yan, H; Ouyang, L; Wang, J; Pompos, A; Jiang, S; Jia, X; Zhou, L

    2014-06-15

    Purpose: Scatter artifacts severely degrade image quality of cone-beam CT (CBCT). We present an ultrafast scatter correction framework by using GPU-based Monte Carlo (MC) simulation and prior patient CT image, aiming at automatically finish the whole process including both scatter correction and reconstructions within 30 seconds. Methods: The method consists of six steps: 1) FDK reconstruction using raw projection data; 2) Rigid Registration of planning CT to the FDK results; 3) MC scatter calculation at sparse view angles using the planning CT; 4) Interpolation of the calculated scatter signals to other angles; 5) Removal of scatter from the raw projections; 6) FDK reconstruction using the scatter-corrected projections. In addition to using GPU to accelerate MC photon simulations, we also use a small number of photons and a down-sampled CT image in simulation to further reduce computation time. A novel denoising algorithm is used to eliminate MC scatter noise caused by low photon numbers. The method is validated on head-and-neck cases with simulated and clinical data. Results: We have studied impacts of photo histories, volume down sampling factors on the accuracy of scatter estimation. The Fourier analysis was conducted to show that scatter images calculated at 31 angles are sufficient to restore those at all angles with <0.1% error. For the simulated case with a resolution of 512×512×100, we simulated 10M photons per angle. The total computation time is 23.77 seconds on a Nvidia GTX Titan GPU. The scatter-induced shading/cupping artifacts are substantially reduced, and the average HU error of a region-of-interest is reduced from 75.9 to 19.0 HU. Similar results were found for a real patient case. Conclusion: A practical ultrafast MC-based CBCT scatter correction scheme is developed. The whole process of scatter correction and reconstruction is accomplished within 30 seconds. This study is supported in part by NIH (1R01CA154747-01), The Core Technology Research

  5. Ultrafast pulse amplification in mode-locked vertical external-cavity surface-emitting lasers

    SciTech Connect (OSTI)

    Böttge, C. N. Hader, J.; Kilen, I.; Moloney, J. V.; Koch, S. W.

    2014-12-29

    A fully microscopic many-body Maxwell–semiconductor Bloch model is used to investigate the influence of the non-equilibrium carrier dynamics on the short-pulse amplification in mode-locked semiconductor microlaser systems. The numerical solution of the coupled equations allows for a self-consistent investigation of the light–matter coupling dynamics, the carrier kinetics in the saturable absorber and the multiple-quantum-well gain medium, as well as the modification of the light field through the pulse-induced optical polarization. The influence of the pulse-induced non-equilibrium modifications of the carrier distributions in the gain medium and the saturable absorber on the single-pulse amplification in the laser cavity is identified. It is shown that for the same structure, quantum wells, and gain bandwidth the non-equilibrium carrier dynamics lead to two preferred operation regimes: one with pulses in the (sub-)100 fs-regime and one with multi-picosecond pulses. The recovery time of the saturable absorber determines in which regime the device operates.

  6. Ultrafast electrochemical preparation of graphene/CoS nanosheet counter electrodes for efficient dye-sensitized solar cells

    SciTech Connect (OSTI)

    Zhu, Chongyang; Zhu, Yimei; Min, Huihua; Xu, Feng; Chen, Jing; Dong, Hui; Tong, Ling; Sun, Litao

    2015-10-05

    Utilizing inexpensive, high-efficiency counter electrodes (CEs) to replace the traditional platinum counterparts in dye-sensitized solar cells (DSSCs) is worthwhile. In this paper, we detail how we synchronously prepared composite CEs of CoS nanosheet arrays and reduced graphene oxide (rGO) layers for the first time via a low temperature, ultrafast one-step electrochemical strategy. With this approach, the whole fabrication process of the composite CEs was only a small percentage of the average time (~15 hours) using other methods. The DSSC assembled with the rGO–CoS composite CE achieved an enhanced power conversion efficiency (PCE) of 8.34%, which is dramatically higher than 6.27% of pure CoS CE-based DSSC and even exceeds 7.50% of Pt CE-based DSSC. The outstanding PCE breakthrough is undoubtedly attributed to the enhancement in electrocatalytic ability of the rGO–CoS composite CE due to the incorporation of highly conducting rGO layers and the GO layers-induced growth of CoS nanosheet arrays with higher density and larger surface area. Therefore, lower charge-transfer resistance and higher exchange current density can be achieved as corroborated by the electrochemical impedance spectra (EIS) and Tafel polarization curves (TPCs). As a result, further experiments also proved that the electrochemical strategy exhibited its universality of fabricating other graphene-enhanced chalcogenide functional composite films.

  7. NuSTAR REVEALS RELATIVISTIC REFLECTION BUT NO ULTRA-FAST OUTFLOW IN THE QUASAR PG 1211+143

    SciTech Connect (OSTI)

    Zoghbi, A.; Miller, J. M.; Walton, D. J.; Stern, D.; Harrison, F. A.; Fabian, A. C.; Reynolds, C. S.; Boggs, S. E.; Craig, W.; Christensen, F. E.; Hailey, C. J.; Zhang, W. W.

    2015-02-01

    We report on four epochs of observations of the quasar PG 1211+143 using NuSTAR. The net exposure time is 300 ks. Prior work on this source found suggestive evidence of an ultra-fast outflow (UFO) in the Fe K band with a velocity of approximately 0.1c. The putative flow would carry away a high-mass flux and kinetic power, with broad implications for feedback and black hole--galaxy co-evolution. NuSTAR detects PG 1211+143 out to 30 keV, meaning that the continuum is well-defined both through and above the Fe K band. A characteristic relativistic disk reflection spectrum is clearly revealed via a broad Fe K emission line and Compton back-scattering curvature. The data offer only weak constraints on the spin of the black hole. A careful search for UFOs shows no significant absorption feature above 90% confidence. The limits are particularly tight when relativistic reflection is included. We discuss the statistics and the implications of these results in terms of connections between accretion onto quasars, Seyferts, and stellar-mass black holes, and feedback into their host environments.

  8. Optimization of chemical compositions in low-carbon Al-killed enamel steel produced by ultra-fast continuous annealing

    SciTech Connect (OSTI)

    Dong, Futao; Du, Linxiu; Liu, Xianghua; Xue, Fei

    2013-10-15

    The influence of Mn,S and B contents on microstructural characteristics, mechanical properties and hydrogen trapping ability of low-carbon Al-killed enamel steel was investigated. The materials were produced and processed in a laboratory and the ultra-fast continuous annealing processing was performed using a continuous annealing simulator. It was found that increasing Mn,S contents in steel can improve its hydrogen trapping ability which is attributed by refined ferrite grains, more dispersed cementite and added MnS inclusions. Nevertheless, it deteriorates mechanical properties of steel sheet. Addition of trace boron results in both good mechanical properties and significantly improved hydrogen trapping ability. The boron combined with nitrogen segregating at grain boundaries, cementite and MnS inclusions, provides higher amount of attractive hydrogen trapping sites and raises the activation energy for hydrogen desorption from them. - Highlights: We study microstructures and properties in low-carbon Al-killed enamel steel. Hydrogen diffusion coefficients are measured to reflect fish-scale resistance. Manganese improves hydrogen trapping ability but decrease deep-drawing ability. Boron improves both hydrogen trapping ability and deep-drawing ability. Both excellent mechanical properties and fish-scale resistance can be matched.

  9. Ultrafast electrochemical preparation of graphene/CoS nanosheet counter electrodes for efficient dye-sensitized solar cells

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Zhu, Chongyang; Zhu, Yimei; Min, Huihua; Xu, Feng; Chen, Jing; Dong, Hui; Tong, Ling; Sun, Litao

    2015-10-05

    Utilizing inexpensive, high-efficiency counter electrodes (CEs) to replace the traditional platinum counterparts in dye-sensitized solar cells (DSSCs) is worthwhile. In this paper, we detail how we synchronously prepared composite CEs of CoS nanosheet arrays and reduced graphene oxide (rGO) layers for the first time via a low temperature, ultrafast one-step electrochemical strategy. With this approach, the whole fabrication process of the composite CEs was only a small percentage of the average time (~15 hours) using other methods. The DSSC assembled with the rGO–CoS composite CE achieved an enhanced power conversion efficiency (PCE) of 8.34%, which is dramatically higher than 6.27%more » of pure CoS CE-based DSSC and even exceeds 7.50% of Pt CE-based DSSC. The outstanding PCE breakthrough is undoubtedly attributed to the enhancement in electrocatalytic ability of the rGO–CoS composite CE due to the incorporation of highly conducting rGO layers and the GO layers-induced growth of CoS nanosheet arrays with higher density and larger surface area. Therefore, lower charge-transfer resistance and higher exchange current density can be achieved as corroborated by the electrochemical impedance spectra (EIS) and Tafel polarization curves (TPCs). As a result, further experiments also proved that the electrochemical strategy exhibited its universality of fabricating other graphene-enhanced chalcogenide functional composite films.« less

  10. Study of beam loading and its compensation in the Compact Ultrafast Terahertz Free-Electron Laser injector linac

    SciTech Connect (OSTI)

    Lal, Shankar Pant, K. K.

    2014-12-15

    The RF properties of an accelerating structure, and the pulse structure and charge per bunch in the electron beam propagating through it are important parameters that determine the impact of beam loading in the structure. The injector linac of the Compact Ultrafast Terahertz Free-Electron Laser (CUTE-FEL) has been operated with two different pulse structures during initial commissioning experiments and the effect of beam loading on the accelerated electron beam parameters has been studied analytically for these two pulse structures. This paper discusses the analytical study of beam loading in a Standing Wave, Plane Wave Transformer linac employed in the CUTE-FEL setup, and a possible technique for its compensation for the electron beam parameters of the CUTE-FEL. A parametric study has been performed to study beam loading for different beam currents and to optimize injection time of the electron beam to compensate beam loading. Results from the parametric study have also been used to explain previously observed results from acceleration experiments in the CUTE-FEL setup.

  11. Photodissociation Dynamics

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Photodissociation Dynamics - Sandia Energy Energy Search Icon Sandia Home Locations Contact Us Employee Locator Energy & Climate Secure & Sustainable Energy Future Stationary Power Energy Conversion Efficiency Solar Energy Wind Energy Water Power Supercritical CO2 Geothermal Natural Gas Safety, Security & Resilience of the Energy Infrastructure Energy Storage Nuclear Power & Engineering Grid Modernization Battery Testing Nuclear Energy Defense Waste Management Programs Advanced

  12. Scattering Dynamics

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Scattering Dynamics - Sandia Energy Energy Search Icon Sandia Home Locations Contact Us Employee Locator Energy & Climate Secure & Sustainable Energy Future Stationary Power Energy Conversion Efficiency Solar Energy Wind Energy Water Power Supercritical CO2 Geothermal Natural Gas Safety, Security & Resilience of the Energy Infrastructure Energy Storage Nuclear Power & Engineering Grid Modernization Battery Testing Nuclear Energy Defense Waste Management Programs Advanced Nuclear

  13. Itinerant and localized magnetization dynamics in antiferromagnetic Ho

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Rettig, L.; Dornes, C.; Thielemann-Kuhn, N.; Pontius, N.; Zabel, H.; Schlagel, D. L.; Lograsso, T. A.; Chollet, M.; Robert, A.; Sikorski, M.; et al

    2016-06-21

    Using femtosecond time-resolved resonant magnetic x-ray diffraction at the Ho L3 absorption edge, we investigate the demagnetization dynamics in antiferromagnetically ordered metallic Ho after femtosecond optical excitation. Here, tuning the x-ray energy to the electric dipole (E1, 2p → 5d) or quadrupole (E2, 2p → 4f) transition allows us to selectively and independently study the spin dynamics of the itinerant 5d and localized 4f electronic subsystems via the suppression of the magnetic (2 1 3–τ) satellite peak. We find demagnetization time scales very similar to ferromagnetic 4f systems, suggesting that the loss of magnetic order occurs via a similar spin-flipmore » process in both cases. The simultaneous demagnetization of both subsystems demonstrates strong intra-atomic 4f–5d exchange coupling. In addition, an ultrafast lattice contraction due to the release of magneto-striction leads to a transient shift of the magnetic satellite peak.« less

  14. DISCOVERY OF ULTRA-FAST OUTFLOWS IN A SAMPLE OF BROAD-LINE RADIO GALAXIES OBSERVED WITH SUZAKU

    SciTech Connect (OSTI)

    Tombesi, F.; Sambruna, R. M.; Mushotzky, R. F.; Braito, V.; Ballo, L.; Cappi, M.

    2010-08-10

    We present the results of a uniform and systematic search for blueshifted Fe K absorption lines in the X-ray spectra of five bright broad-line radio galaxies observed with Suzaku. We detect, for the first time in radio-loud active galactic nuclei (AGNs) at X-rays, several absorption lines at energies greater than 7 keV in three out of five sources, namely, 3C 111, 3C 120, and 3C 390.3. The lines are detected with high significance according to both the F-test and extensive Monte Carlo simulations. Their likely interpretation as blueshifted Fe XXV and Fe XXVI K-shell resonance lines implies an origin from highly ionized gas outflowing with mildly relativistic velocities, in the range v {approx_equal} 0.04-0.15c. A fit with specific photoionization models gives ionization parameters in the range log {xi} {approx_equal} 4-5.6 erg s{sup -1} cm and column densities of N {sub H} {approx_equal} 10{sup 22}-10{sup 23} cm{sup -2}. These characteristics are very similar to those of the ultra-fast outflows (UFOs) previously observed in radio-quiet AGNs. Their estimated location within {approx}0.01-0.3 pc of the central super-massive black hole suggests a likely origin related with accretion disk winds/outflows. Depending on the absorber covering fraction, the mass outflow rate of these UFOs can be comparable to the accretion rate and their kinetic power can correspond to a significant fraction of the bolometric luminosity and is comparable to their typical jet power. Therefore, these UFOs can play a significant role in the expected feedback from the AGN to the surrounding environment and can give us further clues on the relation between the accretion disk and the formation of winds/jets in both radio-quiet and radio-loud AGNs.

  15. Effect of focal geometry on radiation from atomic ionization in an ultrastrong and ultrafast laser field

    SciTech Connect (OSTI)

    Ghebregziabher, Isaac; Walker, Barry C.

    2007-08-15

    We use a tunneling-Monte Carlo model to calculate the dynamics and emitted Larmor radiation from electrons ionized in an ultrashort and ultrastrong pulsed laser focus over the intensity range from 10{sup 17} to 10{sup 20} W/cm{sup 2}. We find the spatial variation of a laser field affects the radiation and can no longer be neglected at laser intensities leading to relativistic effects. We identify three regimes for the interaction as a function of the ratio of the single cycle quiver amplitude of the photoelectron to the laser focus waist. Adopting a one-dimensional or plane wave approximation when the laser driven excursion of the photoelectron exceeds the focus waist overestimates the total radiated energy by as much as an order of magnitude. Despite this, the spectral amplitude of the highest-energy photons from ionization in a laser focus is comparable to the plane wave case for excursions up to the beam waist since the laser focus imparts an extra boost of speed for electrons exiting the focus. Full spatial and temporal integration that includes the ionization of charge states before the peak of the pulse do not differ significantly from results that include only the radiation from ionization of the charge state at the peak of the laser field.

  16. Theory of ultrafast photoinduced electron transfer from a bulk semiconductor to a quantum dot

    SciTech Connect (OSTI)

    Rasmussen, Andrew M. Ramakrishna, S.; Weiss, Emily A.; Seideman, Tamar

    2014-04-14

    This paper describes analytical and numerical results from a model Hamiltonian method applied to electron transfer (ET) from a quasicontinuum (QC) of states to a set of discrete states, with and without a mediating bridge. Analysis of the factors that determine ET dynamics yields guidelines for achieving high-yield electron transfer in these systems, desired for instance for applications in heterogeneous catalysis. These include the choice of parameters of the laser pulse that excites the initial state into a continuum electronic wavepacket and the design of the coupling between the bridge molecule and the donor and acceptor. The vibrational mode on a bridging molecule between donor and acceptor has an influence on the yield of electron transfer via Franck-Condon factors, even in cases where excited vibrational states are only transiently populated. Laser-induced coherence of the initial state as well as energetic overlap is crucial in determining the ET yield from a QC to a discrete state, whereas the ET time is influenced by competing factors from the coupling strength and the coherence properties of the electronic wavepacket.

  17. Research | Argonne National Laboratory

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    and Ultrafast Imaging Integrating ultrafast time-resolved imaging with large-scale molecular dynamics modeling and in situ data analysis and visualization in order to...

  18. Stochastic formation of magnetic vortex structures in asymmetric disks triggered by chaotic dynamics

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Im, Mi-Young; Lee, Ki-Suk; Vogel, Andreas; Hong, Jung-Il; Meier, Guido; Fischer, Peter

    2014-12-17

    The non-trivial spin configuration in a magnetic vortex is a prototype for fundamental studies of nanoscale spin behaviour with potential applications in magnetic information technologies. Arrays of magnetic vortices interfacing with perpendicular thin films have recently been proposed as enabler for skyrmionic structures at room temperature, which has opened exciting perspectives on practical applications of skyrmions. An important milestone for achieving not only such skyrmion materials but also general applications of magnetic vortices is a reliable control of vortex structures. However, controlling magnetic processes is hampered by stochastic behaviour, which is associated with thermal fluctuations in general. Here we showmore » that the dynamics in the initial stages of vortex formation on an ultrafast timescale plays a dominating role for the stochastic behaviour observed at steady state. Our results show that the intrinsic stochastic nature of vortex creation can be controlled by adjusting the interdisk distance in asymmetric disk arrays.« less

  19. Correlated proton-electron hole dynamics in protonated water clusters upon extreme ultraviolet photoionization

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Li, Zheng; Vendrell, Oriol

    2016-01-13

    The ultrafast nuclear and electronic dynamics of protonated water clusters H+(H2O)n after extreme ultraviolet photoionization is investigated. In particular, we focus on cluster cations with n = 3, 6, and 21. Upon ionization, two positive charges are present in the cluster related to the excess proton and the missing electron, respectively. A correlation is found between the cluster's geometrical conformation and initial electronic energy with the size of the final fragments produced. As a result, for situations in which the electron hole and proton are initially spatially close, the two entities become correlated and separate in a time-scale of 20more » to 40 fs driven by strong non-adiabatic effects.« less

  20. Linewidth of the harmonics in a microwave frequency comb generated by focusing a mode-locked ultrafast laser on a tunneling junction

    SciTech Connect (OSTI)

    Hagmann, Mark J.; Stenger, Frank S.; Yarotski, Dmitry A.

    2013-12-14

    Previous analyses suggest that microwave frequency combs (MFCs) with harmonics having extremely narrow linewidths could be produced by photodetection with a mode-locked ultrafast laser. In the MFC generated by focusing a passively mode-locked ultrafast laser on a tunneling junction, 200 harmonics from 74.254 MHz to 14.85 GHz have reproducible measured linewidths approximating the 1 Hz resolution bandwidth (RBW) of the spectrum analyzer. However, in new measurements at a RBW of 0.1 Hz, the linewidths are distributed from 0.12 to 1.17 Hz. Measurements and analysis suggest that, because the laser is not stabilized, the stochastic drift in the pulse repetition rate is the cause for the distribution in measured linewidths. It appears that there are three cases in which the RBW is (1) greater than, (2) less than, or (3) comparable with the intrinsic linewidth. The measured spectra in the third class are stochastic and may show two or more peaks at a single harmonic.

  1. Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses

    SciTech Connect (OSTI)

    Canton, Sophie E.; Kjr, Kasper S.; Vank, Gyrgy; van Driel, Tim B.; Adachi, Shin -ichi; Bordage, Amlie; Bressler, Christian; Chabera, Pavel; Christensen, Morten; Dohn, Asmus O.; Galler, Andreas; Gawelda, Wojciech; Gosztola, David; Haldrup, Kristoffer; Harlang, Tobias; Liu, Yizhu; Mller, Klaus B.; Nmeth, Zoltn; Nozawa, Shunsuke; Ppai, Mtys; Sato, Tokushi; Sato, Takahiro; Suarez-Alcantara, Karina; Togashi, Tadashi; Tono, Kensuke; Uhlig, Jens; Vithanage, Dimali A.; Wrnmark, Kenneth; Yabashi, Makina; Zhang, Jianxin; Sundstrm, Villy; Nielsen, Martin M.

    2015-03-02

    Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donoracceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances. Thus experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined.

  2. Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Canton, Sophie E.; Kjær, Kasper S.; Vankó, György; van Driel, Tim B.; Adachi, Shin -ichi; Bordage, Amélie; Bressler, Christian; Chabera, Pavel; Christensen, Morten; Dohn, Asmus O.; et al

    2015-03-02

    Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor–acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances.more » Thus experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined.« less

  3. Nanoparticle generation and transport resulting from femtosecond laser ablation of ultrathin metal films: Time-resolved measurements and molecular dynamics simulations

    SciTech Connect (OSTI)

    Rouleau, C. M. Puretzky, A. A.; Geohegan, D. B.; Shih, C.-Y.; Wu, C.; Zhigilei, L. V.

    2014-05-12

    The synthesis of metal nanoparticles by ultrafast laser ablation of nanometers-thick metal films has been studied experimentally and computationally. Near-threshold backside laser ablation of 2–20 nm-thick Pt films deposited on fused silica substrates was found to produce nanoparticles with size distributions that were bimodal for the thicker films, but collapsed into a single mode distribution for the thinnest film. Time-resolved imaging of blackbody emission from the Pt nanoparticles was used to reveal the nanoparticle propagation dynamics and estimate their temperatures. The observed nanoparticle plume was compact and highly forward-directed with a well-defined collective velocity that permitted multiple rebounds with substrates to be revealed. Large-scale molecular dynamics simulations were used to understand the evolution of compressive and tensile stresses in the thicker melted liquid films that lead to their breakup and ejection of two groups of nanoparticles with different velocity and size distributions. Ultrafast laser irradiation of ultrathin (few nm) metal films avoids the splitting of the film and appears to be a method well-suited to cleanly synthesize and deposit nanoparticles from semitransparent thin film targets in highly directed beams.

  4. Ultrafast optical pump-probe spectroscopy is used to reveal the coexistence of coupled antiferromagnetic (AFM)/ferroelectric (FE) and ferromagnetic (FM) orders in multiferroic TbMnO3 films, which can guide researchers in creating new kinds of multiferroic materials.

    SciTech Connect (OSTI)

    Qi, Jingbo; Zhu, Jianxin; Trugman, Stuart A.; Taylor, Antoinette; Jia, Quanxi; Prasankumar, Rohit

    2012-07-06

    , experimental techniques capable of dynamically unraveling the interplay between these degrees of freedom on an ultrafast timescale are needed. Here, we use ultrafast optical pump-probe spectroscopy to reveal coexisting coupled magnetic orders in epitaxial TMO thin films grown on (001)-STO, which were not observed in previous work. Our temperature (T)-dependent transient differential reflectivity ({Delta}R/R) measurements show clear signatures of sinusoidal AFM, spiral AFM (FE) and FM phases developing as the film thickness changes. We carry out first-principle density functional theory (DFT) calculations to explain the coupling between AFM/FE and FM orders. These results reveal that the coupling between different magnetic orders observed in our multiferroic TMO thin films may offer greater control of functionality as compared to bulk single crystal multiferroics.

  5. Nonadiabatic ab initio molecular dynamics of photoisomerization in bridged azobenzene

    SciTech Connect (OSTI)

    Gao Aihua; Li Bin; Zhang Peiyu; Han Keli

    2012-11-28

    The photoisomerization mechanisms of bridged azobenzene are investigated by means of surface hopping dynamics simulations based on the Zhu-Nakamura theory. In the geometry optimizations and potential energy surface calculations, four minimum-energy conical intersections between the ground state and the lowest excited state are found to play important roles in the trans-cis and cis-trans isomerization processes. The trans-cis photoisomerization proceeds through two minimum-energy conical intersections. Ultrafast pedal motion of the N atoms and twisting of phenyl rings around their N-C bonds allows the molecule to move to a minimum-energy conical intersection, after which surface hopping from S{sub 1} to S{sub 0} occurs. In the S{sub 0} state, further rotation occurs around the N=N bond and two N-C bonds until the azo moiety and phenyl rings complete their isomerization. Finally, the cis form is achieved by subsequent adjustment of the ethylene bridge. In the cis-trans photodynamics, there is one rotational pathway, in the middle of which two CIs are responsible for the surface hopping to the S{sub 0} state. After the nonadiabatic transition, the molecule reaches the trans form through a barrierless pathway and the two phenyl rings and the additional bridge complete their reorientation almost at the same time.

  6. High efficiency, high quality x-ray optic based on ellipsoidally bent highly oriented pyrolytic graphite crystal for ultrafast x-ray diffraction experiments

    SciTech Connect (OSTI)

    Uschmann, I.; Nothelle, U.; Foerster, E.; Arkadiev, V.; Langhoff, N.; Antonov, A.; Grigorieva, I.; Steinkopf, R.; Gebhardt, A

    2005-08-20

    By the use of a thin highly oriented pyrolytic graphite crystal (HOPG) bent to a high-performance ellipsoidal shape it was possible to focus monochromatic x-rays of 4.5 keV photon energy with an efficiency of 0.0033, which is 30 times larger than for previously used bent crystals. Isotropic TiK{sub a}lpha radiation of a 150 {mu}m source was focused onto a 450 {mu}m spot. The size of the focal spot can be explained by broadening due to the mosaic crystal rocking curve. The rocking curve width (FWHM) of the thin graphite foil was determined to 0.11 deg. . The estimated temporal broadening of an ultrashort Kalpha pulse by the crystal is not larger than 300 fs. These properties make the x-ray optic very attractive for ultrafast time-resolved x-ray measurements.

  7. Adaptive resolution simulation of a biomolecule and its hydration shell: Structural and dynamical properties

    SciTech Connect (OSTI)

    Fogarty, Aoife C. Potestio, Raffaello Kremer, Kurt

    2015-05-21

    A fully atomistic modelling of many biophysical and biochemical processes at biologically relevant length- and time scales is beyond our reach with current computational resources, and one approach to overcome this difficulty is the use of multiscale simulation techniques. In such simulations, when system properties necessitate a boundary between resolutions that falls within the solvent region, one can use an approach such as the Adaptive Resolution Scheme (AdResS), in which solvent particles change their resolution on the fly during the simulation. Here, we apply the existing AdResS methodology to biomolecular systems, simulating a fully atomistic protein with an atomistic hydration shell, solvated in a coarse-grained particle reservoir and heat bath. Using as a test case an aqueous solution of the regulatory protein ubiquitin, we first confirm the validity of the AdResS approach for such systems, via an examination of protein and solvent structural and dynamical properties. We then demonstrate how, in addition to providing a computational speedup, such a multiscale AdResS approach can yield otherwise inaccessible physical insights into biomolecular function. We use our methodology to show that protein structure and dynamics can still be correctly modelled using only a few shells of atomistic water molecules. We also discuss aspects of the AdResS methodology peculiar to biomolecular simulations.

  8. Energetics and dynamics of solvent reorganization in charge-transfer excited states

    SciTech Connect (OSTI)

    Kozik, M.; Sutin, N.; Winkler, J.R.

    1989-01-01

    The dynamics of solvation of the Ru(bpy){sub 2}(CN){sub 2} metal-to-ligand charge-transfer excited state have been examined in a series of aliphatic alcohols. Steady-state emission spectra recorded at low temperature ({approx} 10 K) and at room temperature were used to resolve internal-mode and solvent contributions to the emission bandshape. Time-resolved emission spectra were fit to a model that takes into account internal-mode distortions as well as time-dependent broadening and shifts in emission maxima. A single- exponential solvent relaxation function does not adequately describe the temporal development of the emission profile of Ru(bpy){sub 2}(CN){sub 2} in alcohols. The evolution of the emission spectrum is clearly biphasic, and can be reasonably fit with a biexponential function. The slower of the two relaxation times is comparable to the longest longitudinal relaxation time reported for the bulk solvent. These slower components, however, represent less than half of the overall approach to equilibrium. Local heating due to above-threshold excitation, and local solvent relaxation are two likely sources of the faster dynamics. 25 refs., 3 figs., 2 tabs.

  9. Role of nuclear dynamics in the Asymmetric molecular-frame photoelectron angular distributions for C 1s photoejection from CO{sub 2}

    SciTech Connect (OSTI)

    Miyabe, Shungo; Haxton, Dan; Rescigno, Tom; McCurdy, Bill

    2010-11-30

    We report the results of semiclassical calculations of the asymmetric molecular-frame photoelectron angular distributions for C 1s ionization of CO{sub 2} measured with respect to the CO{sup +} and O{sup +} ions produced by subsequent Auger decay, and show how the decay event can be used to probe ultrafast molecular dynamics of the transient cation. The fixed-nuclei photoionization amplitudes were constructed using variationally obtained electron-molecular ion scattering wave functions. The amplitudes are then used in a semiclassical manner to investigate their dependence on the nuclear dynamics of the cation. The method introduced here can be used to study other core-level ionization events.

  10. Ultrafast neutron detector

    DOE Patents [OSTI]

    Wang, C.L.

    1985-06-19

    A neutron detector of very high temporal resolution is described. It may be used to measure distributions of neutrons produced by fusion reactions that persist for times as short as about 50 picoseconds.

  11. Ultrafast neutron detector

    DOE Patents [OSTI]

    Wang, Ching L.

    1987-01-01

    The invention comprises a neutron detector (50) of very high temporal resolution that is particularly well suited for measuring the fusion reaction neutrons produced by laser-driven inertial confinement fusion targets. The detector comprises a biased two-conductor traveling-wave transmission line (54, 56, 58, 68) having a uranium cathode (60) and a phosphor anode (62) as respective parts of the two conductors. A charge line and Auston switch assembly (70, 72, 74) launch an electric field pulse along the transmission line. Neutrons striking the uranium cathode at a location where the field pulse is passing, are enabled to strike the phosphor anode and produce light that is recorded on photographic film (64). The transmission line may be variously configured to achieve specific experimental goals.

  12. Non-linear optical studies of adsorbates: Spectroscopy and dynamics

    SciTech Connect (OSTI)

    Zhu, Xiangdong.

    1989-08-01

    In the first part of this thesis, we have established a systematic procedure to apply the surface optical second-harmonic generation (SHG) technique to study surface dynamics of adsorbates. In particular, we have developed a novel technique for studies of molecular surface diffusions. In this technique, the laser-induced desorption with two interfering laser beams is used to produce a monolayer grating of adsorbates. The monolayer grating is detected with diffractions of optical SHG. By monitoring the first-order second-harmonic diffraction, we can follow the time evolution of the grating modulation from which we are able to deduce the diffusion constant of the adsorbates on the surface. We have successfully applied this technique to investigate the surface diffusion of CO on Ni(111). The unique advantages of this novel technique will enable us to readily study anisotropy of a surface diffusion with variable grating orientation, and to investigate diffusion processes of a large dynamic range with variable grating spacings. In the second part of this work, we demonstrate that optical infrared-visible sum-frequency generation (SFG) from surfaces can be used as a viable surface vibrational spectroscopic technique. We have successfully recorded the first vibrational spectrum of a monolayer of adsorbates using optical infrared-visible SFG. The qualitative and quantitative correlation of optical SFG with infrared absorption and Raman scattering spectroscopies are examined and experimentally demonstrated. We have further investigated the possibility to use transient infrared-visible SFG to probe vibrational transients and ultrafast relaxations on surfaces. 146 refs.

  13. 2012 ATOMIC AND MOLECULAR INTERACTIONS GORDON RESEARCH CONFERENCE AND GORDON RESEARCH SEMINAR, JULY 15-20, 2012

    SciTech Connect (OSTI)

    Zwier, Timothy

    2012-07-20

    At the 2012 Atomic and Molecular Interactions Gordon Conference, there will be talks in several broadly defined and partially overlapping areas: ? Intramolecular and single-collision reaction dynamics; ? Photophysics and photochemistry of excited states; ? Clusters, aerosols and solvation; ? Interactions at interfaces; ? Conformations and folding of large molecules; ? Interactions under extreme conditions of temperature and pressure. The theme of the Gordon Research Seminar on Atomic & Molecular Interactions, in keeping with the tradition of the Atomic and Molecular Interactions Gordon Research Conference, is far-reaching and involves fundamental research in the gas and condensed phases along with application of these ideas to practical chemical fields. The oral presentations, which will contain a combination of both experiment and theory, will focus on four broad categories: ? Ultrafast Phenomena; ? Excited States, Photoelectrons, and Photoions; ? Chemical Reaction Dynamics; ? Biomolecules and Clusters.

  14. Structure, dynamics and stability of water/scCO2/mineral interfaces from ab initio molecular dynamics simulations

    SciTech Connect (OSTI)

    Lee, Mal Soon; McGrail, B. Peter; Rousseau, Roger J.; Glezakou, Vassiliki Alexandra

    2015-10-12

    The interface between a solid and a complex multi-component liquid forms a unique reaction environment whose structure and composition can significantly deviate from either bulk or liquid phase and is poorly understood due the innate difficulty to obtain molecular level information. Feldspar minerals, as typified by the Ca-end member Anorthite, serve as prototypical model systems to assess the reactivity and ion mobility at solid/water-bearing supercritical fluid (WBSF) interfaces due to recent X-ray based measurements that provide information on water-film formation, and cation vacancies at these surfaces. Using density functional theory based molecular dynamics, which allows the evaluation of reactivity and condensed phase dynamics on equal footing, we report on the structure and dynamics of water nucleation and surface aggregation, carbonation and Ca mobilization under geologic carbon sequestration scenarios (T=323 K and P=90 bar). We find that water has a strong enthalpic preference for aggregation on a Ca-rich, O-terminated anorthite (001) surface, but entropy strongly hinders the film formation at very low water concentrations. Carbonation reactions readily occur at electron-rich terminal Oxygen sites adjacent to cation vacancies, when in contact with supercritical CO2. Cation vacancies of this type can form readily in the presence of a water layer that allows for facile and enthalpicly favorable Ca2+ extraction and solvation. Apart from providing unprecedented molecular level detail of a complex three component (mineral, water and scCO2) system), this work highlights the ability of modern capabilities of AIMD methods to begin to qualitatively and quantitatively address structure and reactivity at solid-liquid interfaces of high chemical complexity. This work was supported by the US Department of Energy, Office of Fossil Energy (M.-S. L., B. P. M. and V.-A. G.) and the Office of Basic Energy Science, Division of Chemical Sciences, Geosciences and Biosciences

  15. Shared and Dynamic Libraries

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Shared and Dynamic Libraries Shared and Dynamic Libraries The Edison system can support applications that use dynamic shared libraries (DSL) on the compute nodes. Some "out-of-the-box" applications require DSLs and some popular applications like Python use DSLs as well. Using System Shared and Dynamic Libraries "System" DSLs include those that support software packages found in "typical" Linux distributions, e.g. Python and Perl. To build an application that will

  16. Shared and Dynamic Libraries

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Shared and Dynamic Libraries Shared and Dynamic Libraries The Hopper system can support applications that use dynamic shared libraries (DSL) on the compute nodes. Some "out-of-the-box" applications require DSLs and some popular applications like Python use DSLs as well. Using System Shared and Dynamic Libraries "System" DSLs include those that support software packages found in "typical" Linux distributions, e.g. Python and Perl. To build an application that will

  17. Intramolecular and nonlinear dynamics

    SciTech Connect (OSTI)

    Davis, M.J.

    1993-12-01

    Research in this program focuses on three interconnected areas. The first involves the study of intramolecular dynamics, particularly of highly excited systems. The second area involves the use of nonlinear dynamics as a tool for the study of molecular dynamics and complex kinetics. The third area is the study of the classical/quantum correspondence for highly excited systems, particularly systems exhibiting classical chaos.

  18. Theoretical and experimental study of dynamics of photoexcited carriers in GaN

    SciTech Connect (OSTI)

    Shishehchi, Sara; Bellotti, Enrico; Rudin, Sergey; Garrett, Gregory A.; Wraback, Michael

    2013-12-21

    We present a theoretical and experimental study of the sub-picosecond dynamics of photo-excited carriers in GaN. In the theoretical model, interaction with an external ultrafast laser pulse is treated coherently and to account for the scattering mechanisms and dephasing processes, a generalized Monte-Carlo simulation is used. The scattering mechanisms included are carrier interactions with polar optical phonons and acoustic phonons, and carrier-carrier Coulomb interactions. We study the effect of different scattering mechanisms on the carrier densities. In the case that the excitation energy satisfies the threshold for polar optical scattering, phonon contribution is the dominant process in relaxing the system, otherwise, carrier-carrier mechanism is dominant. Furthermore, we present the temperature and pulse power dependent normalized luminescence intensity. The results are presented over a range of temperatures, electric field, and excitation energy of the laser pulse. For comparison, we also report the experimental time-resolved photoluminescence studies on GaN samples. There is a good agreement between the simulation and experiment in normalized luminescence intensity results. Therefore, we show that we can explain the dynamics of the photo-excited carriers in GaN by including only carrier-carrier and carrier-phonon interactions and a relatively simple two-band electronic structure model.

  19. Hybrid DFT Functional-Based Static and Molecular Dynamics Studies of Excess Electron in Liquid Ethylene Carbonate

    SciTech Connect (OSTI)

    Yu, J. M.; Balbuena, P. B.; Budzien, J. L.; Leung, Kevin

    2011-02-22

    We applied static and dynamic hybrid functional density functional theory (DFT) calculations to study the interactions of one and two excess electrons with ethylene carbonate (EC) liquid and clusters. Optimal structures of (EC)n and (EC)n- clusters devoid of Li+ ions, n = 16, were obtained. The excess electron was found to be localized on a single EC in all cases, and the EC dimeric radical anion exhibits a reduced barrier associated with the breaking of the ethylene carbonoxygen covalent bond compared to EC-. In ab initio molecular dynamics (AIMD) simulations of EC- solvated in liquid EC, large fluctuations in the carbonyl carbonoxygen bond lengths were observed. AIMD simulations of a two-electron attack on EC in EC liquid and on Li metal surfaces yielded products similar to those predicted using nonhybrid DFT functionals, except that CO release did not occur for all attempted initial configurations in the liquid state.

  20. Bright, Coherent, Ultrafast Soft X-Ray Harmonics Spanning the Water Window from a Tabletop Light Source

    SciTech Connect (OSTI)

    Chen, M.-C.; Arpin, P.; Popmintchev, T.; Gerrity, M.; Zhang, B.; Seaberg, M.; Popmintchev, D.; Murnane, M. M.; Kapteyn, H. C.

    2010-10-22

    We demonstrate fully phase-matched high harmonic emission spanning the water window spectral region important for nano- and bioimaging and a breadth of materials and molecular dynamics studies. We also generate the broadest bright coherent bandwidth ({approx_equal}300 eV) to date from any light source, small or large, that is consistent with a single subfemtosecond burst. The harmonic photon flux at 0.5 keV is 10{sup 3} higher than demonstrated previously. This work extends bright, spatially coherent, attosecond pulses into the soft x-ray region for the first time.

  1. Electrolyte Solvation and Ionic Association. VI. Acetonitrile...

    Office of Scientific and Technical Information (OSTI)

    different thermal phase behavior and electrochemicalphysicochemical properties. The simulation results are in full accord with a previous experimental study of these (AN)n-LiX ...

  2. Electrolyte Solvation and Ionic Association. V. Acetonitrile...

    Office of Scientific and Technical Information (OSTI)

    mixtures provides detailed insight into the coordination interactions of the FSI- anions and the wide variability noted in the electrolyte transport property (i.e., viscosity ...

  3. The solvated electron in supercritical water

    SciTech Connect (OSTI)

    Bartels, D. M.; Takahashi, K.; Cline, J.; Jonah, C. D.

    2000-03-09

    In order to investigate the feasibility for high-efficiency supercritical-water-cooled nuclear reactors, a study of radiation chemistry in supercritical water has been undertaken. Preliminary results in measurement of the optical absorption of the hydrated electron are reported, and compared with recent anion cluster data.

  4. Solvate Structures and Computational/Spectroscopic Characterization...

    Office of Scientific and Technical Information (OSTI)

    Sponsoring Org: USDOE Country of Publication: United States Language: English Subject: coordination; crystal structure; ionic association; lithium; Raman Word Cloud More Like This ...

  5. Structural Interactions within Lithium Salt Solvates: Cyclic...

    Office of Scientific and Technical Information (OSTI)

    and ester solvents coordinate Li+ cations in electrolyte solutions for lithium batteries. One approach to gleaning significant insight into these interactions is to examine...

  6. Dynamical principles in neuroscience

    SciTech Connect (OSTI)

    Rabinovich, Mikhail I.; Varona, Pablo; Selverston, Allen I.; Abarbanel, Henry D. I.

    2006-10-15

    Dynamical modeling of neural systems and brain functions has a history of success over the last half century. This includes, for example, the explanation and prediction of some features of neural rhythmic behaviors. Many interesting dynamical models of learning and memory based on physiological experiments have been suggested over the last two decades. Dynamical models even of consciousness now exist. Usually these models and results are based on traditional approaches and paradigms of nonlinear dynamics including dynamical chaos. Neural systems are, however, an unusual subject for nonlinear dynamics for several reasons: (i) Even the simplest neural network, with only a few neurons and synaptic connections, has an enormous number of variables and control parameters. These make neural systems adaptive and flexible, and are critical to their biological function. (ii) In contrast to traditional physical systems described by well-known basic principles, first principles governing the dynamics of neural systems are unknown. (iii) Many different neural systems exhibit similar dynamics despite having different architectures and different levels of complexity. (iv) The network architecture and connection strengths are usually not known in detail and therefore the dynamical analysis must, in some sense, be probabilistic. (v) Since nervous systems are able to organize behavior based on sensory inputs, the dynamical modeling of these systems has to explain the transformation of temporal information into combinatorial or combinatorial-temporal codes, and vice versa, for memory and recognition. In this review these problems are discussed in the context of addressing the stimulating questions: What can neuroscience learn from nonlinear dynamics, and what can nonlinear dynamics learn from neuroscience?.

  7. Computational Fluid Dynamics

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    scour-tracc-cfd TRACC RESEARCH Computational Fluid Dynamics Computational Structural Mechanics Transportation Systems Modeling Computational Fluid Dynamics Overview of CFD: Video Clip with Audio Computational fluid dynamics (CFD) research uses mathematical and computational models of flowing fluids to describe and predict fluid response in problems of interest, such as the flow of air around a moving vehicle or the flow of water and sediment in a river. Coupled with appropriate and prototypical

  8. Protein Dynamics and Biocatalysis

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Protein Dynamics and Biocatalysis Protein Dynamics and Biocatalysis 1998 Annual Report Grand Challenge Projects biocatalysis.gif A model of the Michaelis complex for the TEM-1/penicillin system from molecular dynamics simulations. Investigators: P. A. Bash, Northwestern University Medical School and M. Karplus, Harvard University Research Objectives A guiding principle of molecular biology is that the structure of a biomolecule defines its function. This principle is especially true in the case

  9. Shared and Dynamic Libraries

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Some "out-of-the-box" applications require DSLs and some popular applications like Python use DSLs as well. Using System Shared and Dynamic Libraries "System" DSLs include...

  10. Accelerated Molecular Dynamics Methods

    Broader source: Energy.gov [DOE]

    This presentation on Accelerated Molecular Dynamics Methods was given at the DOE Theory Focus Session on Hydrogen Storage Materials on May 18, 2006.

  11. Solar Dynamics | Open Energy Information

    Open Energy Info (EERE)

    Dynamics Jump to: navigation, search Name: Solar Dynamics Place: Ottumwa, Iowa Zip: IA 52501 Sector: Solar Product: Solar Dynamics is a US-based solar powered attic roof vents...

  12. Batch crystallization of rhodopsin for structural dynamics using an X-ray free-electron laser

    SciTech Connect (OSTI)

    Wu, Wenting; Nogly, Przemyslaw; Rheinberger, Jan; Kick, Leonhard M.; Gati, Cornelius; Nelson, Garrett; Deupi, Xavier; Standfuss, Jrg; Schertler, Gebhard; Panneels, Valrie

    2015-06-27

    A new batch preparation method is presented for high-density micrometre-sized crystals of the G protein-coupled receptor rhodopsin for use in time-resolved serial femtosecond crystallography at an X-ray free-electron laser using a liquid jet. Rhodopsin is a membrane protein from the G protein-coupled receptor family. Together with its ligand retinal, it forms the visual pigment responsible for night vision. In order to perform ultrafast dynamics studies, a time-resolved serial femtosecond crystallography method is required owing to the nonreversible activation of rhodopsin. In such an approach, microcrystals in suspension are delivered into the X-ray pulses of an X-ray free-electron laser (XFEL) after a precise photoactivation delay. Here, a millilitre batch production of high-density microcrystals was developed by four methodical conversion steps starting from known vapour-diffusion crystallization protocols: (i) screening the low-salt crystallization conditions preferred for serial crystallography by vapour diffusion, (ii) optimization of batch crystallization, (iii) testing the crystal size and quality using second-harmonic generation (SHG) imaging and X-ray powder diffraction and (iv) production of millilitres of rhodopsin crystal suspension in batches for serial crystallography tests; these crystals diffracted at an XFEL at the Linac Coherent Light Source using a liquid-jet setup.

  13. Final Technical Report Structural Dynamics in Complex Liquids Studied with Multidimensional Vibrational Spectroscopy

    SciTech Connect (OSTI)

    Tokmakoff, Andrei; Fiechtner, Gregory J.

    2015-12-10

    This grant supported work in the Tokmakoff lab at the University of Chicago aimed at understanding the fundamental properties of water at a molecular level, and how water participates in proton transport in aqueous media. The physical properties of water and aqueous solutions are inextricably linked with efforts to develop new sustainable energy sources. Energy conversion, storage, and transduction processes, particularly those that occur in biology and soft matter, make use of water for the purpose of storing and moving charge. Water’s unique physical and chemical properties depend on the ability of water molecules to participate in up to four hydrogen bonds, and the rapid fluctuations and ultrafast energy dissipation of its hydrogenbonded networks. Our work during the grant period led to advances in four areas: (1) the generation of short pulses of broadband infrared light (BBIR) for use in time-resolved twodimensional spectroscopy (2D IR), (2) the investigation of the spectroscopy and transport of excess protons in water, (3) the study of aqueous hydroxide to describe the interaction of the ion and water and the dynamics of proton transfer, and (4) the coupled motion of water and its hydrogen-bonding solutes.

  14. Dynamics of femtosecond laser absorption of fused silica in the ablation regime

    SciTech Connect (OSTI)

    Lebugle, M. Sanner, N.; Varkentina, N.; Sentis, M.; Utéza, O.

    2014-08-14

    We investigate the ultrafast absorption dynamics of fused silica irradiated by a single 500 fs laser pulse in the context of micromachining applications. A 60-fs-resolution pump-probe experiment that measures the reflectivity and transmissivity of the target under excitation is developed to reveal the evolution of plasma absorption. Above the ablation threshold, an overcritical plasma with highly non-equilibrium conditions is evidenced in a thin layer at the surface. The maximum electron density is reached at a delay of 0.5 ps after the peak of the pump pulse, which is a strong indication of the occurrence of electronic avalanche. The results are further analyzed to determine the actual feedback of the evolution of the optical properties of the material on the pump pulse. We introduce an important new quantity, namely, the duration of absorption of the laser by the created plasma, corresponding to the actual timespan of laser absorption by inverse Bremsstrahlung. Our results indicate an increasing contribution of plasma absorption to the total material absorption upon raising the excitation fluence above the ablation threshold. The role of transient optical properties during the energy deposition stage is characterized and our results emphasize the necessity to take it into account for better understanding and control of femtosecond laser-dielectrics interaction.

  15. Predicting solute partitioning in lipid bilayers: Free energies and partition coefficients from molecular dynamics simulations and COSMOmic

    SciTech Connect (OSTI)

    Jakobtorweihen, S. Ingram, T.; Gerlach, T.; Smirnova, I.; Zuniga, A. Chaides; Keil, F. J.

    2014-07-28

    Quantitative predictions of biomembrane/water partition coefficients are important, as they are a key property in pharmaceutical applications and toxicological studies. Molecular dynamics (MD) simulations are used to calculate free energy profiles for different solutes in lipid bilayers. How to calculate partition coefficients from these profiles is discussed in detail and different definitions of partition coefficients are compared. Importantly, it is shown that the calculated coefficients are in quantitative agreement with experimental results. Furthermore, we compare free energy profiles from MD simulations to profiles obtained by the recent method COSMOmic, which is an extension of the conductor-like screening model for realistic solvation to micelles and biomembranes. The free energy profiles from these molecular methods are in good agreement. Additionally, solute orientations calculated with MD and COSMOmic are compared and again a good agreement is found. Four different solutes are investigated in detail: 4-ethylphenol, propanol, 5-phenylvaleric acid, and dibenz[a,h]anthracene, whereby the latter belongs to the class of polycyclic aromatic hydrocarbons. The convergence of the free energy profiles from biased MD simulations is discussed and the results are shown to be comparable to equilibrium MD simulations. For 5-phenylvaleric acid the influence of the carboxyl group dihedral angle on free energy profiles is analyzed with MD simulations.

  16. Solution-state structure and affinities of cyclodextrin: Fentanyl complexes by nuclear magnetic resonance spectroscopy and molecular dynamics simulation

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Mayer, Brian P.; Kennedy, Daniel J.; Lau, Edmond Y.; Valdez, Carlos A.

    2016-02-04

    Cyclodextrins (CDs) are investigated for their ability to form inclusion complexes with the analgesic fentanyl and three similar molecules: acetylfentanyl, thiofentanyl, and acetylthiofentanyl. Stoichiometry, binding strength, and complex structure are revealed through nuclear magnetic resonance (NMR) techniques and discussed in terms of molecular dynamics (MD) simulations. It was found that β-cyclodextrin is generally capable of forming the strongest complexes with the fentanyl panel. Two-dimensional NMR data and computational chemical calculations are used to derive solution-state structures of the complexes. Binding of the fentanyls to the CDs occurs at the amide phenyl ring, leaving the majority of the molecule solvated bymore » water, an observation common to all four fentanyls. This finding suggests a universal binding behavior, as the vast majority of previously synthesized fentanyl analogues contain this structural moiety. Furthermore, this baseline study serves as the most complete work on CD:fentanyl complexes to date and provides the insights into strategies for producing future generations of designer cyclodextrins capable of stronger and more selective complexation of fentanyl and its analogues.« less

  17. Role of direct electron-phonon coupling across metal-semiconductor interfaces in thermal transport via molecular dynamics

    SciTech Connect (OSTI)

    Lin, Keng-Hua; Strachan, Alejandro

    2015-07-21

    Motivated by significant interest in metal-semiconductor and metal-insulator interfaces and superlattices for energy conversion applications, we developed a molecular dynamics-based model that captures the thermal transport role of conduction electrons in metals and heat transport across these types of interface. Key features of our model, denoted eleDID (electronic version of dynamics with implicit degrees of freedom), are the natural description of interfaces and free surfaces and the ability to control the spatial extent of electron-phonon (e-ph) coupling. Non-local e-ph coupling enables the energy of conduction electrons to be transferred directly to the semiconductor/insulator phonons (as opposed to having to first couple to the phonons in the metal). We characterize the effect of the spatial e-ph coupling range on interface resistance by simulating heat transport through a metal-semiconductor interface to mimic the conditions of ultrafast laser heating experiments. Direct energy transfer from the conduction electrons to the semiconductor phonons not only decreases interfacial resistance but also increases the ballistic transport behavior in the semiconductor layer. These results provide new insight for experiments designed to characterize e-ph coupling and thermal transport at the metal-semiconductor/insulator interfaces.

  18. System Dynamics Model | NISAC

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Dynamics Model content top Chemical Supply Chain Analysis Posted by Admin on Mar 1, 2012 in | Comments 0 comments Chemical Supply Chain Analysis NISAC has developed a range of...

  19. Accelerated Molecular Dynamics Methods

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    ... Los Alamos Parallel Replica Dynamics Procedure Start clock and run thermostatted MD on ... Sum the trajectory times over all M processors. Advance simulation clock by this t sum Los ...

  20. Multipulsed dynamic moire interferometer

    DOE Patents [OSTI]

    Deason, Vance A.

    1991-01-01

    An improved dynamic moire interferometer comprised of a lasing medium providing a plurality of beams of coherent light, a multiple q-switch producing multiple trains of 100,000 or more pulses per second, a combining means collimating multiple trains of pulses into substantially a single train and directing beams to specimen gratings affixed to a test material, and a controller, triggering and sequencing the emission of the pulses with the occurrence and recording of a dynamic loading event.

  1. Photochemical reaction dynamics

    SciTech Connect (OSTI)

    Moore, B.C.

    1993-12-01

    The purpose of the program is to develop a fundamental understanding of unimolecular and bimolecular reaction dynamics with application in combustion and energy systems. The energy dependence in ketene isomerization, ketene dissociation dynamics, and carbonyl substitution on organometallic rhodium complexes in liquid xenon have been studied. Future studies concerning unimolecular processes in ketene as well as energy transfer and kinetic studies of methylene radicals are discussed.

  2. EVIDENCE FOR ULTRA-FAST OUTFLOWS IN RADIO-QUIET ACTIVE GALACTIC NUCLEI. II. DETAILED PHOTOIONIZATION MODELING OF Fe K-SHELL ABSORPTION LINES

    SciTech Connect (OSTI)

    Tombesi, F.; Reeves, J. N.; Palumbo, G. G. C.; Braito, V.

    2011-11-20

    X-ray absorption line spectroscopy has recently shown evidence for previously unknown Ultra-fast Outflows (UFOs) in radio-quiet active galactic nuclei (AGNs). These have been detected essentially through blueshifted Fe XXV/XXVI K-shell transitions. In the previous paper of this series we defined UFOs as those highly ionized absorbers with an outflow velocity higher than 10,000 km s{sup -1} and assessed the statistical significance of the associated blueshifted absorption lines in a large sample of 42 local radio-quiet AGNs observed with XMM-Newton. The present paper is an extension of that work. First, we report a detailed curve of growth analysis of the main Fe XXV/XXVI transitions in photoionized plasmas. Then, we estimate an average spectral energy distribution for the sample sources and directly model the Fe K absorbers in the XMM-Newton spectra with the detailed Xstar photoionization code. We confirm that the frequency of sources in the radio-quiet sample showing UFOs is >35% and that the majority of the Fe K absorbers are indeed associated with UFOs. The outflow velocity distribution spans from {approx}10,000 km s{sup -1} ({approx}0.03c) up to {approx}100,000 km s{sup -1} ({approx}0.3c), with a peak and mean value of {approx}42,000 km s{sup -1} ({approx}0.14c). The ionization parameter is very high and in the range log {xi} {approx} 3-6 erg s{sup -1} cm, with a mean value of log {xi} {approx} 4.2 erg s{sup -1} cm. The associated column densities are also large, in the range N{sub H} {approx} 10{sup 22}-10{sup 24} cm{sup -2}, with a mean value of N{sub H} {approx} 10{sup 23} cm{sup -2}. We discuss and estimate how selection effects, such as those related to the limited instrumental sensitivity at energies above 7 keV, may hamper the detection of even higher velocities and higher ionization absorbers. We argue that, overall, these results point to the presence of extremely ionized and possibly almost Compton-thick outflowing material in the innermost regions of

  3. Ab initio implementation of quantum trajectory mean-field approach and dynamical simulation of the N{sub 2}CO photodissociation

    SciTech Connect (OSTI)

    Xie, Binbin; Liu, Lihong; Cui, Ganglong; Fang, Wei-Hai; Cao, Jun; Feng, Wei; Li, Xin-qi

    2015-11-21

    In this work, the recently introduced quantum trajectory mean-field (QTMF) approach is implemented and employed to explore photodissociation dynamics of diazirinone (N{sub 2}CO), which are based on the high-level ab initio calculation. For comparison, the photodissociation process has been simulated as well with the fewest-switches surface hopping (FSSH) and the ab initio multiple spawning (AIMS) methods. Overall, the dynamical behavior predicted by the three methods is consistent. The N{sub 2}CO photodissociation at λ > 335 nm is an ultrafast process and the two C—N bonds are broken in a stepwise way, giving birth to CO and N{sub 2} as the final products in the ground state. Meanwhile, some noticeable differences were found in the QTMF, FSSH, and AIMS simulated time constants for fission of the C—N bonds, excited-state lifetime, and nonadiabatic transition ratios in different intersection regions. These have been discussed in detail. The present study provides a clear evidence that direct ab initio QTMF approach is one of the reliable tools for simulating nonadiabatic dynamics processes.

  4. Dynamic cable analysis models

    SciTech Connect (OSTI)

    Palo, P.A.; Meggitt, D.J.; Nordell, W.J.

    1983-05-01

    This paper presents a summary of the development and validation of undersea cable dynamics computer models by the Naval Civil Engineering Laboratory (NCEL) under the sponsorship of the Naval Facilities Engineering Command. These models allow for the analysis of both small displacement (strumming) and large displacement (static and dynamic) deformations of arbitrarily configured cable structures. All of the large displacement models described in this paper are available to the public. This paper does not emphasize the theoretical development of the models (this information is available in other references) but emphasizes the various features of the models, the comparisons between model output and experimental data, and applications for which the models have been used.

  5. Substructured multibody molecular dynamics.

    SciTech Connect (OSTI)

    Grest, Gary Stephen; Stevens, Mark Jackson; Plimpton, Steven James; Woolf, Thomas B. (Johns Hopkins University, Baltimore, MD); Lehoucq, Richard B.; Crozier, Paul Stewart; Ismail, Ahmed E.; Mukherjee, Rudranarayan M. (Rensselaer Polytechnic Institute, Troy, NY); Draganescu, Andrei I.

    2006-11-01

    We have enhanced our parallel molecular dynamics (MD) simulation software LAMMPS (Large-scale Atomic/Molecular Massively Parallel Simulator, lammps.sandia.gov) to include many new features for accelerated simulation including articulated rigid body dynamics via coupling to the Rensselaer Polytechnic Institute code POEMS (Parallelizable Open-source Efficient Multibody Software). We use new features of the LAMMPS software package to investigate rhodopsin photoisomerization, and water model surface tension and capillary waves at the vapor-liquid interface. Finally, we motivate the recipes of MD for practitioners and researchers in numerical analysis and computational mechanics.

  6. Dynamics of helium films

    SciTech Connect (OSTI)

    Clements, B.E.; Epstein, J.L.; Krotscheck, E.; Tymczak, C.J.; Saarela, M.

    1992-11-01

    The authors present quantitative calculations for the static structure and the dynamics of quantum liquid films on a translationally invariant substrate. The excitation spectrum is calculated by solving the equations of motion for time-dependent one- and two-body densities. They find significant corrections to the Feynman spectrum for the phonon-like collective excitations. 8 refs., 2 figs.

  7. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    By subtracting the laser-off spectrum from the laser-on spectrum (at a probe delay time of 400 ps), the team obtained a differential spectrum with features corresonding to a...

  8. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    ... soft x-ray pulses generated at ALS Beamline 6.0.2 ... The resulting near-edge x-ray absorption fine-structure ... state in which diffusional motion of the ions leads to the ...

  9. LUSI :: LCLS Ultrafast Science Instruments

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    search Go Home Project Pages LUSI Instruments Uniqueness of FEL X-rays X-ray FEL Science About LCLS Science with LCLS Calendar & Meetings Contact Us Office of Science/U.S. DOE Current News: Job Openings Oct. 3, 3:00 PM- SPPS: A window to the world of LCLS Science Meetings: LCLS SAC Meeting October 19-20, 2006 LUSI Lehman Review January 23-24, 2007 LUSI Bi-weekly Team Leader meeting June 23, 2006 LUSI Science Group Leaders Meeting October 18-19 SSRL User Meeting - Soft X-ray Workshop Oct

  10. Ultra-fast laser system

    DOE Patents [OSTI]

    Dantus, Marcos; Lozovoy, Vadim V

    2014-01-21

    A laser system is provided which selectively excites Raman active vibrations in molecules. In another aspect of the present invention, the system includes a laser, pulse shaper and detection device. A further aspect of the present invention employs a femtosecond laser and binary pulse shaping (BPS). Still another aspect of the present invention uses a laser beam pulse, a pulse shaper and remote sensing.

  11. Indirect excitation of ultrafast demagnetization

    Office of Scientific and Technical Information (OSTI)

    ... our observations are in qualitative agreement with the model ... L. et al. e Soft X-ray Research instrument at the Linac ... optical cross-correlation method for improved experimental ...

  12. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    real-time view of the transition state in superionic copper sulfide (Cu2S) nanocrystals. ... Depiction of the copper sulfide superionic state with copper in blue and sulfur in yellow. ...

  13. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    is a key step in moving charges between electrodes when recharging a lithium-ion battery. ... The samples were photoexcited with 400-nm laser pulses then probed using synchronized ...

  14. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    ALS, to obtain an atomic-level, real-time view of the transition state in superionic copper sulfide (Cu2S) nanocrystals. Solid-State Ionics At the dawn of the Information Age,...

  15. Ultrafast Transformations in Superionic Nanocrystals

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    ... Upon heating to 103 C (217.4 F), the sulfur cage expands into a largely vacant hexagonal structure, permitting the copper ions to hop from one local sweet spot to another ...

  16. Impacts of side chain and excess energy on the charge photogeneration dynamics of low-bandgap copolymer-fullerene blends

    SciTech Connect (OSTI)

    Huo, Ming-Ming Zhang, Jian-Ping E-mail: hjhzlz@iccas.ac.cn; Department of Chemistry, Renmin University of China, Beijing 100872 ; Hu, Rong Xing, Ya-Dong Liu, Yu-Chen Ai, Xi-Cheng; Hou, Jian-Hui E-mail: hjhzlz@iccas.ac.cn

    2014-02-28

    Primary charge photogeneration dynamics in neat and fullerene-blended films of a pair of alternating benzo[1,2-b:4,5-b{sup ?}]dithiophene (BDT) and thieno[3,4-b]thiophene (TT) copolymers are comparatively studied by using near-infrared, time-resolved absorption (TA) spectroscopy under low excitation photon fluence. PBDTTT-E and PBDTTT-C, differed merely in the respective TT-substituents of ester (-E) and carbonyl (-C), show distinctly different charge photogeneration dynamics. The pair of neat PBDTTT films show exciton lifetimes of ?0.1 ns and fluorescence quantum yields below 0.2%, as well as prominent excess-energy enhanced exciton dissociation. In addition, PBDTTT-C gives rise to >50% higher P{sup +} yield than PBDTTT-E does irrespective to the excitation photon energy. Both PBDTTT-E:PC{sub 61}BM and PBDTTT-C:PC{sub 61}BM blends show subpicosecond exciton lifetimes and nearly unitary fluorescence quenching efficiency and, with respect to the former blend, the latter one shows substantially higher branching ratio of charge separated (CS) state over interfacial charge transfer (ICT) state, and hence more efficient exciton-to-CS conversion. For PBDTTT-C:PC{sub 61}BM, the ultrafast charge dynamics clearly show the processes of ICT-CS interconversion and P{sup +} migration, which are possibly influenced by the ICT excess energy. However, such processes are relatively indistinctive in the case of PBDTTT-E:PC{sub 61}BM. The results strongly prove the importance of ICT dissociation in yielding free charges, and are discussed in terms of the film morphology and the precursory solution-phase macromolecular conformation.

  17. Fluid Dynamics and Solid Mechanics

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    and Solid Mechanics Basic and applied research in theoretical continuum dynamics, modern hydrodynamic theory, materials modeling, global climate modeling, numerical...

  18. Entanglement dynamics in chaotic systems

    SciTech Connect (OSTI)

    Ghose, Shohini [Institute for Quantum Information Science, University of Calgary, Alberta, T2N 1N4 (Canada); Department of Physics and Astronomy, University of New Mexico, Albuquerque, New Mexico 87131 (United States); Sanders, Barry C. [Institute for Quantum Information Science, University of Calgary, Alberta, T2N 1N4 (Canada); Centre for Quantum Computer Technology, Macquarie University, Sydney, New South Wales (Australia)

    2004-12-01

    We study quantum chaos for systems with more than one degree of freedom, for which we present an analysis of the dynamics of entanglement. Our analysis explains the main features of entanglement dynamics and identifies entanglement-based signatures of quantum chaos. We discuss entanglement dynamics for a feasible experiment involving an atom in a magneto-optical trap and compare the results with entanglement dynamics for the well-studied quantum kicked top.

  19. Roaming Molecule Dynamics

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Roaming Molecule Dynamics - Sandia Energy Energy Search Icon Sandia Home Locations Contact Us Employee Locator Energy & Climate Secure & Sustainable Energy Future Stationary Power Energy Conversion Efficiency Solar Energy Wind Energy Water Power Supercritical CO2 Geothermal Natural Gas Safety, Security & Resilience of the Energy Infrastructure Energy Storage Nuclear Power & Engineering Grid Modernization Battery Testing Nuclear Energy Defense Waste Management Programs Advanced

  20. Beam Dynamics for ARIA

    SciTech Connect (OSTI)

    Ekdahl, Carl August Jr.

    2014-10-14

    Beam dynamics issues are assessed for a new linear induction electron accelerator being designed for flash radiography of large explosively driven hydrodynamic experiments. Special attention is paid to equilibrium beam transport, possible emittance growth, and beam stability. It is concluded that a radiographic quality beam will be produced possible if engineering standards and construction details are equivalent to those on the present radiography accelerators at Los Alamos.

  1. Dynamic radioactive particle source

    DOE Patents [OSTI]

    Moore, Murray E.; Gauss, Adam Benjamin; Justus, Alan Lawrence

    2012-06-26

    A method and apparatus for providing a timed, synchronized dynamic alpha or beta particle source for testing the response of continuous air monitors (CAMs) for airborne alpha or beta emitters is provided. The method includes providing a radioactive source; placing the radioactive source inside the detection volume of a CAM; and introducing an alpha or beta-emitting isotope while the CAM is in a normal functioning mode.

  2. Dynamical impurity problems

    SciTech Connect (OSTI)

    Emery, V.J.; Kivelson, S.A.

    1993-12-31

    In the past few years there has been a resurgence of interest in dynamical impurity problems, as a result of developments in the theory of correlated electron systems. The general dynamical impurity problem is a set of conduction electrons interacting with an impurity which has internal degrees of freedom. The simplest and earliest example, the Kondo problem, has attracted interest since the mid-sixties not only because of its physical importance but also as an example of a model displaying logarithmic divergences order by order in perturbation theory. It provided one of the earliest applications of the renormalization group method, which is designed to deal with just such a situation. As we shall see, the antiferromagnetic Kondo model is controlled by a strong-coupling fixed point, and the essence of the renormalization group solution is to carry out the global renormalization numerically starting from the original (weak-coupling) Hamiltonian. In these lectures, we shall describe an alternative route in which we identify an exactly solvable model which renormalizes to the same fixed point as the original dynamical impurity problem. This approach is akin to determining the critical behavior at a second order phase transition point by solving any model in a given universality class.

  3. Effect of Fe-doping on nonlinear optical responses and carrier trapping dynamics in GaN single crystals

    SciTech Connect (OSTI)

    Fang, Yu; Yang, Junyi; Yang, Yong; Zhou, Feng; Wu, Xingzhi; Xiao, Zhengguo; Song, Yinglin

    2015-08-03

    We presented a quantitative study on the Fe-doping concentration dependence of optical nonlinearities and ultrafast carrier dynamics in Fe-doped GaN (GaN:Fe) single crystals using picosecond Z-scan and femtosecond pump-probe with phase object techniques under two-photon excitation. In contrast to the two-photon absorption that was found to be independent on the Fe-doping, the nonlinear refraction decreased with the Fe concentration due to the fast carrier trapping effect of Fe{sup 3+}/Fe{sup 2+} deep acceptors, which simultaneously acted as an efficient non-radiative recombination channels for excess carriers. Remarkably, compared to that of Si-doped GaN bulk crystal, the free-carrier refraction effect in GaN:Fe crystals was found to be enhanced considerably since Fe-doping and the effective carrier lifetime (∼10 ps) could be tuned over three orders of magnitude at high Fe-doping level of 1 × 10{sup 19 }cm{sup −3}.

  4. Photo-modulated thin film transistor based on dynamic charge transfer within quantum-dots-InGaZnO interface

    SciTech Connect (OSTI)

    Liu, Xiang; Yang, Xiaoxia; Liu, Mingju; Tao, Zhi; Wei, Lei Li, Chi Zhang, Xiaobing; Wang, Baoping; Dai, Qing; Nathan, Arokia

    2014-03-17

    The temporal development of next-generation photo-induced transistor across semiconductor quantum dots and Zn-related oxide thin film is reported in this paper. Through the dynamic charge transfer in the interface between these two key components, the responsibility of photocurrent can be amplified for scales of times (?10{sup 4}?A/W 450?nm) by the electron injection from excited quantum dots to InGaZnO thin film. And this photo-transistor has a broader waveband (from ultraviolet to visible light) optical sensitivity compared with other Zn-related oxide photoelectric device. Moreover, persistent photoconductivity effect can be diminished in visible waveband which lead to a significant improvement in the device's relaxation time from visible illuminated to dark state due to the ultrafast quenching of quantum dots. With other inherent properties such as integrated circuit compatible, low off-state current and high external quantum efficiency resolution, it has a great potential in the photoelectric device application, such as photodetector, phototransistor, and sensor array.

  5. Effect of deuterium substitution for hydrogen in surface functionalisation of hydrophilic nanosilicon particles on their spectral and dynamic properties

    SciTech Connect (OSTI)

    Kompanets, V O; Chekalin, S V; Dorofeev, S G; Kononov, N N; Barzilovich, P Yu; Ishchenko, A A

    2014-06-30

    Broadband femtosecond spectroscopy has been used to study two types of hydrophilic silicon nanoparticles: (1) photoluminescent, passivated with deuterium and oxidised in fully deuterated dimethyl sulphoxide, and (2) nonluminescent (control samples having a similar crystalline core), passivated with hydrogen and oxidised in dimethyl sulphoxide. We have found significant differences in ultrafast spectral temporal induced absorption dynamics between the two types of nanoparticles in the energy range corresponding to their calculated band gap. The observed distinction is due to the considerably higher oxidation rate of silicon on the surface of the deuterated samples in comparison with the undeuterated ones and with the associated increase in the number of photoluminescence centres on the surface of the nanoparticles. In the samples containing self-trapped exciton (STE) energy states responsible for the photoluminescence in the red spectral region, carrier capture at these levels and carrier relaxation to the ground state have characteristic times in the femtosecond range. In the samples free of STE states, excited carriers relax to the conduction band bottom in a characteristic time of several picoseconds. (extreme light fields and their applications)

  6. Static and dynamic optical properties of La1-xSrxFeO3-δ: The effects of A-site and oxygen stoichiometry

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Sergey Y. Smolin; Sfeir, Matthew Y.; Scafetta, Mark D.; Choquette, Amber K.; Baxter, Jason B.; May, Steven J.

    2015-12-09

    Perovskite oxides are a promising material class for photovoltaic and photocatalytic applications due to their visible band gaps, nanosecond recombination lifetimes, and great chemical diversity. However, there is limited understanding of the link between composition and static and dynamic optical properties, despite the critical role these properties play in the design of light-harvesting devices. To clarify these relationships, we systemically studied the optoelectronic properties in La1-xSrxFeO3-δ epitaxial films, uncovering the effects of A-site cation substitution and oxygen stoichiometry. Variable-angle spectroscopic ellipsometry was used to measure static optical properties, revealing a linear increase in absorption coefficient at 1.25 eV and amore » red-shifting of the optical absorption edge with increasing Sr fraction. The absorption spectra can be similarly tuned through the introduction of oxygen vacancies, indicating the critical role that nominal Fe valence plays in optical absorption. Dynamic optoelectronic properties were studied with ultrafast transient reflectance spectroscopy, revealing similar nanosecond photoexcited carrier lifetimes for oxygen deficient and stoichiometric films with the same nominal Fe valence. Furthermore, these results demonstrate that while the static optical absorption is strongly dependent on nominal Fe valence tuned through cation or anion stoichiometry, oxygen vacancies do not appear to play a significantly detrimental role in the recombination kinetics.« less

  7. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    ... energy (4) water (4) adsorption (3) inorganic, organic, physical and analytical chemistry (3) molecular dynamics method (3) nitrates (3) solvation (3) air-water interactions ...

  8. Time-resolved THz studies of carrier dynamics in semiconductors, superconductors, and strongly-correlated electron materials

    SciTech Connect (OSTI)

    Kaindl, Robert A.; Averitt, Richard D.

    2006-11-14

    materials occur at lower energies. The terahertz (THz) regime is particularly rich in such fundamental resonances. This includes ubiquitous lattice vibrations and low-energy collective oscillations of conduction charges. In nanoscale materials, band structure quantization also yields novel infrared and THz transitions, including intersubband absorption in quantum wells. The formation of excitons in turn leads to low-energy excitations analogous to inter-level transitions in atoms. In transition-metal oxides, fundamental excitation gaps arise from charge pairing into superconducting condensates and other correlated states. This motivates the use of ultrafast THz spectroscopy as a powerful tool to study light-matter interactions and microscopic processes in nanoscale and correlated-electron materials.A distinct advantage of coherent THz pulses is that the amplitude and phase of the electric field can be measured directly, as the THz fields are coherent with the fs pulses from which they are generated. Using THz time-domain spectroscopy (THz-TDS), both the real and imaginary parts of the response functions (such as the dielectric function) are obtained directly without the need for Kramers?Kronig transforms. The THz response can also be expressed in terms of absorption and refractive index, or as the optical conductivity. The optical conductivity describes the current response of a many-body system to an electric field, an ideal tool to study conducting systems. A second important advantage is the ultrafast time resolution that results from the short temporal duration of the THz time-domain sources. In particular, optical-pump THz-probe spectroscopy enables a delicate probe of the transient THz conductivity after optical photoexcitation. These experiments can provide insight into quasiparticle interactions, phase transitions, or nonequilibrium dynamics. In this chapter we will provide many such examples. Since THz spectroscopy of solids is a quickly expanding field

  9. Dynamic Underground Stripping Project

    SciTech Connect (OSTI)

    Aines, R.; Newmark, R.; McConachie, W.; Udell, K.; Rice, D.; Ramirez, A.; Siegel, W.; Buettner, M.; Daily, W.; Krauter, P.; Folsom, E.; Boegel, A.J.; Bishop, D.; Udell, K.

    1992-01-01

    LLNL is collaborating with the UC Berkeley College of Engineering to develop and demonstrate a system of thermal remediation and underground imaging techniques for use in rapid cleanup of localized underground spills. Called ``Dynamic Stripping`` to reflect the rapid and controllable nature of the process, it will combine steam injection, direct electrical heating, and tomographic geophysical imaging in a cleanup of the LLNL gasoline spill. In the first 8 months of the project, a Clean Site engineering test was conducted to prove the field application of the techniques before moving the contaminated site in FY 92.

  10. Effect of the spin-twist structure on the spin-wave dynamics in Fe{sub 55}Pt{sub 45}/Ni{sub 80}Fe{sub 20} exchange coupled bi-layers with varying Ni{sub 80}Fe{sub 20} thickness

    SciTech Connect (OSTI)

    Pal, Semanti; Barman, Saswati Barman, Anjan; Hellwig, Olav

    2014-05-07

    We have investigated optically induced ultrafast magnetization dynamics of a series of Fe{sub 55}Pt{sub 45}/Ni{sub 80}Fe{sub 20} exchange spring bi-layers with varying Ni{sub 80}Fe{sub 20} thickness. Rich spin-wave spectra are observed; whose frequency shows a strong dependence on the Ni{sub 80}Fe{sub 20} layer thickness. Micromagnetic simulations based on a simplified magnetic microstructure were able to reproduce the experimental data qualitatively. The spin twist structure introduced in the Ni{sub 80}Fe{sub 20} layer gives rise to new modes in the composite system as opposed to the bare Ni{sub 80}Fe{sub 20} films.

  11. Atomic-scale dynamics of a model glass-forming metallic liquid: Dynamical crossover, dynamical decoupling, and dynamical clustering

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Jaiswal, Abhishek; Egami, Takeshi; Zhang, Yang

    2015-04-01

    The phase behavior of multi-component metallic liquids is exceedingly complex because of the convoluted many-body and many-elemental interactions. Herein, we present systematic studies of the dynamic aspects of such a model ternary metallic liquid Cu40Zr51Al9 using molecular dynamics simulation with embedded atom method. We observed a dynamical crossover from Arrhenius to super-Arrhenius behavior in the transport properties (diffusion coefficient, relaxation times, and shear viscosity) bordered at Tx ~1300K. Unlike in many molecular and macromolecular liquids, this crossover phenomenon occurs in the equilibrium liquid state well above the melting temperature of the system (Tm ~ 900K), and the crossover temperature ismore » roughly twice of the glass-transition temperature (Tg). Below Tx, we found the elemental dynamics decoupled and the Stokes-Einstein relation broke down, indicating the onset of heterogeneous spatially correlated dynamics in the system mediated by dynamic communications among local configurational excitations. To directly characterize and visualize the correlated dynamics, we employed a non-parametric, unsupervised machine learning technique and identified dynamical clusters of atoms with similar atomic mobility. The revealed average dynamical cluster size shows an accelerated increase below Tx and mimics the trend observed in other ensemble averaged quantities that are commonly used to quantify the spatially heterogeneous dynamics such as the non-Gaussian parameter and the four-point correlation function.« less

  12. Cantera Aerosol Dynamics Simulator

    Energy Science and Technology Software Center (OSTI)

    2004-09-01

    The Cantera Aerosol Dynamics Simulator (CADS) package is a general library for aerosol modeling to address aerosol general dynamics, including formation from gas phase reactions, surface chemistry (growth and oxidation), bulk particle chemistry, transport by Brownian diffusion, thermophoresis, and diffusiophoresis with linkage to DSMC studies, and thermal radiative transport. The library is based upon Cantera, a C++ Cal Tech code that handles gas phase species transport, reaction, and thermodynamics. The method uses a discontinuous galerkinmore » formulation for the condensation and coagulation operator that conserves particles, elements, and enthalpy up to round-off error. Both O-D and 1-D time dependent applications have been developed with the library. Multiple species in the solid phase are handled as well. The O-D application, called Tdcads (Time Dependent CADS) is distributed with the library. Tdcads can address both constant volume and constant pressure adiabatic homogeneous problems. An extensive set of sample problems for Tdcads is also provided.« less

  13. Los Alamos Dynamics Summer School

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Los Alamos Dynamics Summer School » Los Alamos Dynamics Summer School The Seventeenth Los Alamos Dynamics Summer School Program Information and Application Process Contact Institute Director Charles Farrar (505) 665-0860 Email Executive Administrator Ellie Vigil (505) 667-2718 Email Administrative Assistant Rebecca Duran (505) 665-8899 Email How to Apply Students should email the following documents to LADSSApply@lanl.gov Application Form (pdf) A one-page cover letter describing your interest

  14. Los Alamos Dynamics Summer School

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Los Alamos Dynamics Summer School The Seventeenth Los Alamos Dynamics Summer School School overview and focus. Contact Institute Director Charles Farrar (505) 665-0860 Email Executive Administrator Ellie Vigil (505) 667-2818 Email Administrative Assistant Rebecca Duran (505) 665-8899 Email The Los Alamos Dynamics Summer School is a very selective summer school in which top upper-level US-citizen undergraduate students from universities around the nation attend lectures and work in teams of three

  15. Dynamics, Spectral Geometry and Topology

    SciTech Connect (OSTI)

    Burghelea, Dan

    2011-02-10

    The paper is an informal report on joint work with Stefan Haller on Dynamics in relation with Topology and Spectral Geometry. By dynamics one means a smooth vector field on a closed smooth manifold; the elements of dynamics of concern are the rest points, instantons and closed trajectories. One discusses their counting in the case of a generic vector field which has some additional properties satisfied by a still very large class of vector fields.

  16. Look-ahead Dynamic Simulation

    Energy Science and Technology Software Center (OSTI)

    2015-10-20

    Look-ahead dynamic simulation software system incorporates the high performance parallel computing technologies, significantly reduces the solution time for each transient simulation case, and brings the dynamic simulation analysis into on-line applications to enable more transparency for better reliability and asset utilization. It takes the snapshot of the current power grid status, functions in parallel computing the system dynamic simulation, and outputs the transient response of the power system in real time.

  17. The solvent dependent shift of the amide I band of a fully solvated peptide in methanol/water mixtures as a local probe for the solvent composition in the peptide/solvent interface

    SciTech Connect (OSTI)

    Gnanakaran, S

    2008-01-01

    We determine the shift and line-shape of the amide I band of a model AK-peptide from molecular dynamics (MD) simulations of the peptide dissolved in methanol/water mixtures with varying composition. The IR-spectra are determined from a transition dipole coupling exciton model. A simplified empirical model Hamiltonian is employed, taking both the effect of hydrogen bonding, as well as intramolecular vibrational coupling into account. We consider a single isolated AK-peptide in a mostly helical conformation, while the solvent is represented by 2600 methanol or water molecules, simulated for a pressure of 1 bar and a temperature of 300 K. Over the course of the simulations minor reversible conformational changes at the termini are observed, which are found to only slightly affect the calculated spectral properties. Over the entire composition range, varying from pure water to the pure methanol solvent, a monotonous blue-shift of the IR amide I band of about 8 wavenumbers is observed. The shift is found to be caused by two counter-compensating effects: An intramolecular red-shift of about 1.2 wavenumbers, due to stronger intramolecular hydrogen-bonding in a methanol-rich environment. Dominating, however, is the intermolecular solvent-dependent blue-shift of about 10 wavenumbers, being attributed to the less effective hydrogen bond donor capabilities of methanol compared to water. The importance of solvent-contribution to the IR-shift, as well as the significantly different hydrogen formation capabilities of water and methanol make the amide I band sensitive to composition changes in the local environment close the peptide/solvent interface. This allows, in principle, an experimental determination of the composition of the solvent in close proximity to the peptide surface. For the AK-peptide case they observe at low methanol concentrations a significantly enhanced methanol concentration at the peptide/solvent-interface, supposedly promoted by the partially hydrophobic

  18. Los Alamos Dynamics Summer School

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    The Seventeenth Los Alamos Dynamics Summer School Program Information and Application Process Contact Institute Director Charles Farrar (505) 663-5330 Email Executive...

  19. Dynamic bed reactor

    DOE Patents [OSTI]

    Stormo, Keith E. (Moscow, ID)

    1996-07-02

    A dynamic bed reactor is disclosed in which a compressible open cell foam matrix is periodically compressed and expanded to move a liquid or fluid through the matrix. In preferred embodiments, the matrix contains an active material such as an enzyme, biological cell, chelating agent, oligonucleotide, adsorbent or other material that acts upon the liquid or fluid passing through the matrix. The active material may be physically immobilized in the matrix, or attached by covalent or ionic bonds. Microbeads, substantially all of which have diameters less than 50 microns, can be used to immobilize the active material in the matrix and further improve reactor efficiency. A particularly preferred matrix is made of open cell polyurethane foam, which adsorbs pollutants such as polychlorophenol or o-nitrophenol. The reactors of the present invention allow unidirectional non-laminar flow through the matrix, and promote intimate exposure of liquid reactants to active agents such as microorganisms immobilized in the matrix.

  20. Dynamic Information Architecture System

    Energy Science and Technology Software Center (OSTI)

    1997-02-12

    The Dynamic Information System (DIAS) is a flexible object-based software framework for concurrent, multidiscplinary modeling of arbitrary (but related) processes. These processes are modeled as interrelated actions caused by and affecting the collection of diverse real-world objects represented in a simulation. The DIAS architecture allows independent process models to work together harmoniously in the same frame of reference and provides a wide range of data ingestion and output capabilities, including Geographic Information System (GIS) typemore » map-based displays and photorealistic visualization of simulations in progress. In the DIAS implementation of the object-based approach, software objects carry within them not only the data which describe their static characteristics, but also the methods, or functions, which describe their dynamic behaviors. There are two categories of objects: (1) Entity objects which have real-world counterparts and are the actors in a simulation, and (2) Software infrastructure objects which make it possible to carry out the simulations. The Entity objects contain lists of Aspect objects, each of which addresses a single aspect of the Entity''s behavior. For example, a DIAS Stream Entity representing a section of a river can have many aspects correspondimg to its behavior in terms of hydrology (as a drainage system component), navigation (as a link in a waterborne transportation system), meteorology (in terms of moisture, heat, and momentum exchange with the atmospheric boundary layer), and visualization (for photorealistic visualization or map type displays), etc. This makes it possible for each real-world object to exhibit any or all of its unique behaviors within the context of a single simulation.« less

  1. Molecular dynamics simulation of diffusion coefficients and structural properties of some alkylbenzenes in supercritical carbon dioxide at infinite dilution

    SciTech Connect (OSTI)

    Wang, Jinyang; Zhong, Haimin; Qiu, Wenda; Chen, Liuping; Feng, Huajie

    2014-03-14

    The binary infinite dilute diffusion coefficients, D{sub 12}{sup ?}, of some alkylbenzenes (Ph-C{sub n}, from Ph-H to Ph-C{sub 12}) from 313 K to 333 K at 15 MPa in supercritical carbon dioxide (scCO{sub 2}) have been studied by molecular dynamics (MD) simulation. The MD values agree well with the experimental ones, which indicate MD simulation technique is a powerful way to predict and obtain diffusion coefficients of solutes in supercritical fluids. Besides, the local structures of Ph-C{sub n}/CO{sub 2} fluids are further investigated by calculating radial distribution functions and coordination numbers. It qualitatively convinces that the first solvation shell of Ph-C{sub n} in scCO{sub 2} is significantly influenced by the structure of Ph-C{sub n} solute. Meanwhile, the mean end-to-end distance, the mean radius of gyration and dihedral angle distribution are calculated to gain an insight into the structural properties of Ph-C{sub n} in scCO{sub 2}. The abnormal trends of radial distribution functions and coordination numbers can be reasonably explained in term of molecular flexibility. Moreover, the computed results of dihedral angle clarify that flexibility of long-chain Ph-C{sub n} is the result of internal rotation of C-C single bond (?{sub c-c}) in alkyl chain. It is interesting that compared with n-alkane, because of the existence of benzene ring, the flexibility of alkyl chain in Ph-C{sub n} with same carbon atom number is significantly reduced, as a result, the carbon chain dependence of diffusion behaviors for long-chain n-alkane (n ? 5) and long-chain Ph-C{sub n} (n ? 4) in scCO{sub 2} are different.

  2. Dynamic granularity of imaging systems

    SciTech Connect (OSTI)

    Geissel, Matthias; Smith, Ian C.; Shores, Jonathon E.; Porter, John L.

    2015-11-04

    Imaging systems that include a specific source, imaging concept, geometry, and detector have unique properties such as signal-to-noise ratio, dynamic range, spatial resolution, distortions, and contrast. Some of these properties are inherently connected, particularly dynamic range and spatial resolution. It must be emphasized that spatial resolution is not a single number but must be seen in the context of dynamic range and consequently is better described by a function or distribution. We introduce the “dynamic granularity” Gdyn as a standardized, objective relation between a detector’s spatial resolution (granularity) and dynamic range for complex imaging systems in a given environment rather than the widely found characterization of detectors such as cameras or films by themselves. We found that this relation can partly be explained through consideration of the signal’s photon statistics, background noise, and detector sensitivity, but a comprehensive description including some unpredictable data such as dust, damages, or an unknown spectral distribution will ultimately have to be based on measurements. Measured dynamic granularities can be objectively used to assess the limits of an imaging system’s performance including all contributing noise sources and to qualify the influence of alternative components within an imaging system. Our article explains the construction criteria to formulate a dynamic granularity and compares measured dynamic granularities for different detectors used in the X-ray backlighting scheme employed at Sandia’s Z-Backlighter facility.

  3. Dynamic granularity of imaging systems

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Geissel, Matthias; Smith, Ian C.; Shores, Jonathon E.; Porter, John L.

    2015-11-04

    Imaging systems that include a specific source, imaging concept, geometry, and detector have unique properties such as signal-to-noise ratio, dynamic range, spatial resolution, distortions, and contrast. Some of these properties are inherently connected, particularly dynamic range and spatial resolution. It must be emphasized that spatial resolution is not a single number but must be seen in the context of dynamic range and consequently is better described by a function or distribution. We introduce the “dynamic granularity” Gdyn as a standardized, objective relation between a detector’s spatial resolution (granularity) and dynamic range for complex imaging systems in a given environment rathermore » than the widely found characterization of detectors such as cameras or films by themselves. We found that this relation can partly be explained through consideration of the signal’s photon statistics, background noise, and detector sensitivity, but a comprehensive description including some unpredictable data such as dust, damages, or an unknown spectral distribution will ultimately have to be based on measurements. Measured dynamic granularities can be objectively used to assess the limits of an imaging system’s performance including all contributing noise sources and to qualify the influence of alternative components within an imaging system. Our article explains the construction criteria to formulate a dynamic granularity and compares measured dynamic granularities for different detectors used in the X-ray backlighting scheme employed at Sandia’s Z-Backlighter facility.« less

  4. Atomic-scale dynamics of a model glass-forming metallic liquid: Dynamical crossover, dynamical decoupling, and dynamical clustering

    SciTech Connect (OSTI)

    Jaiswal, Abhishek; Egami, Takeshi; Zhang, Yang

    2015-04-01

    The phase behavior of multi-component metallic liquids is exceedingly complex because of the convoluted many-body and many-elemental interactions. Herein, we present systematic studies of the dynamic aspects of such a model ternary metallic liquid Cu40Zr51Al9 using molecular dynamics simulation with embedded atom method. We observed a dynamical crossover from Arrhenius to super-Arrhenius behavior in the transport properties (diffusion coefficient, relaxation times, and shear viscosity) bordered at Tx ~1300K. Unlike in many molecular and macromolecular liquids, this crossover phenomenon occurs in the equilibrium liquid state well above the melting temperature of the system (Tm ~ 900K), and the crossover temperature is roughly twice of the glass-transition temperature (Tg). Below Tx, we found the elemental dynamics decoupled and the Stokes-Einstein relation broke down, indicating the onset of heterogeneous spatially correlated dynamics in the system mediated by dynamic communications among local configurational excitations. To directly characterize and visualize the correlated dynamics, we employed a non-parametric, unsupervised machine learning technique and identified dynamical clusters of atoms with similar atomic mobility. The revealed average dynamical cluster size shows an accelerated increase below Tx and mimics the trend observed in other ensemble averaged quantities that are commonly used to quantify the spatially heterogeneous dynamics such as the non-Gaussian parameter and the four-point correlation function.

  5. Dynamic Fault Detection Chassis

    SciTech Connect (OSTI)

    Mize, Jeffery J

    2007-01-01

    Abstract The high frequency switching megawatt-class High Voltage Converter Modulator (HVCM) developed by Los Alamos National Laboratory for the Oak Ridge National Laboratory's Spallation Neutron Source (SNS) is now in operation. One of the major problems with the modulator systems is shoot-thru conditions that can occur in a IGBTs H-bridge topology resulting in large fault currents and device failure in a few microseconds. The Dynamic Fault Detection Chassis (DFDC) is a fault monitoring system; it monitors transformer flux saturation using a window comparator and dV/dt events on the cathode voltage caused by any abnormality such as capacitor breakdown, transformer primary turns shorts, or dielectric breakdown between the transformer primary and secondary. If faults are detected, the DFDC will inhibit the IGBT gate drives and shut the system down, significantly reducing the possibility of a shoot-thru condition or other equipment damaging events. In this paper, we will present system integration considerations, performance characteristics of the DFDC, and discuss its ability to significantly reduce costly down time for the entire facility.

  6. ICFA Beam Dynamics Newsletter

    SciTech Connect (OSTI)

    Ben-Zvi I.; Kuczewski A.; Altinbas, Z.; Beavis, D.; Belomestnykh,; Dai, J. et al

    2012-07-01

    The Collider-Accelerator Department at Brookhaven National Laboratory is building a high-brightness 500 mA capable Energy Recovery Linac (ERL) as one of its main R&D thrusts towards eRHIC, the polarized electron - hadron collider as an upgrade of the operating RHIC facility. The ERL is in final assembly stages, with injection commisioning starting in October 2012. The objective of this ERL is to serve as a platform for R&D into high current ERL, in particular issues of halo generation and control, Higher-Order Mode (HOM) issues, coherent emissions for the beam and high-brightness, high-power beam generation and preservation. The R&D ERL features a superconducting laser-photocathode RF gun with a high quantum efficiency photoccathode served with a load-lock cathode delivery system, a highly damped 5-cell accelerating cavity, a highly flexible single-pass loop and a comprehensive system of beam instrumentation. In this ICFA Beam Dynamics Newsletter article we will describe the ERL in a degree of detail that is not usually found in regular publications. We will discuss the various systems of the ERL, following the electrons from the photocathode to the beam dump, cover the control system, machine protection etc and summarize with the status of the ERL systems.

  7. Computational Fluid Dynamics Library

    Energy Science and Technology Software Center (OSTI)

    2005-03-04

    CFDLib05 is the Los Alamos Computational Fluid Dynamics LIBrary. This is a collection of hydrocodes using a common data structure and a common numerical method, for problems ranging from single-field, incompressible flow, to multi-species, multi-field, compressible flow. The data structure is multi-block, with a so-called structured grid in each block. The numerical method is a Finite-Volume scheme employing a state vector that is fully cell-centered. This means that the integral form of the conservation lawsmore » is solved on the physical domain that is represented by a mesh of control volumes. The typical control volume is an arbitrary quadrilateral in 2D and an arbitrary hexahedron in 3D. The Finite-Volume scheme is for time-unsteady flow and remains well coupled by means of time and space centered fluxes; if a steady state solution is required, the problem is integrated forward in time until the user is satisfied that the state is stationary.« less

  8. Atomistic Time-Domain Simulations of Light-Harvesting and Charge-Transfer Dynamics in Novel Nanoscale Materials for Solar Hydrogen Production.

    SciTech Connect (OSTI)

    Prezhdo, Oleg V.

    2012-03-22

    provided a unified atomistic picture of the nature and dynamics of photoexcited states in semiconductor QDs. We also summarized our recent findings about the photoinduced electron dynamics at the chromophore-semiconductor interfaces from a time-domain ab initio perspective. The interface provides the foundation for a new, promising type of solar cell and presents a fundamentally important case study for several fields, including photo-, electro- and analytical chemistries, molecular electronics, and photography. Further, the interface offers a classic example of an interaction between an organic molecular species and an inorganic bulk material. Scientists employ different concepts and terminologies to describe molecular and solid states of matter, and these differences make it difficult to describe the interface with a single model. At the basic atomistic level of description, however, this challenge can be largely overcome. Recent advances in non-adiabatic molecular dynamics and time-domain density functional theory have created a unique opportunity for simulating the ultrafast, photoinduced processes on a computer very similar to the way that they occur in nature. These state-of-the-art theoretical tools offered a comprehensive picture of a variety of electron transfer processes that occur at the interface, including electron injection from the chromophore to the semiconductor, electron relaxation and delocalization inside the semiconductor, back-transfer of the electron to the chromophore and to the electrolyte, and regeneration of the neutral chromophore by the electrolyte. The ab initio time-domain modeling is particularly valuable for understanding these dynamic features of the ultrafast electron transfer processes, which cannot be represented by a simple rate description. We demonstrated using symmetry adapted cluster theory with configuration interaction (SAC-CI) that charging of small PbSe nanocrystals (NCs) greatly modifies their electronic states and optical

  9. Wed Thu Fri Sat Sun

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    NdNiO3 interface: charge-order dynamics LF16 XPP GAFFNEY, KELLY Observing ligand torsion dynamics in a solvated Cu(I)(diimine)2+ compound to understand excited-state dynamics...

  10. Femtosecond photoelectron spectroscopy: a new tool for the study of anion dynamics

    SciTech Connect (OSTI)

    Greenblatt, B.J.

    1999-02-01

    A new experimental technique for the time-resolved study of anion reactions is presented. Using femtosecond laser pulses, which provide extremely fast ({approx} 100 fs) time resolution, in conjunction with photoelectron spectroscopy, which reveals differences between anion and neutral potential energy surfaces, a complex anion reaction can be followed from its inception through the formation of asymptotic products. Experimental data can be modeled quantitatively using established theoretical approaches, allowing for the refinement of potential energy surfaces as well as dynamical models. After a brief overview, a detailed account of the construction of the experimental apparatus is presented. Documentation of the data acquisition program is contained in the Appendix. The first experimental demonstration of the technique is then presented for I{sub 2}{sup -} photodissociation, modeled using a simulation program which is also detailed in the Appendix. The investigation of I{sub 2}{sup -} photodissociation in several size-selected I{sub 2}{sup -}(Ar){sub n} (n = 6-20) and I{sub 2}{sup -}(CO{sub 2}){sub n} (n = 4-16) clusters forms the heart of the dissertation. In a series of chapters, the numerous effects of solvation on this fundamental bond-breaking reaction are explored, the most notable of which is the recombination of I{sub 2}{sup -} on the ground {tilde X}({sup 2}{Sigma}{sub u}{sup +}) state in sufficiently large clusters. Recombination and trapping of I{sub 2}{sup -} on the excited {tilde A}({sup 2}{Pi}{sub 3/2,g}) state is also observed in both types of clusters. The studies have revealed electronic state transitions, the first step in recombination, on a {approx}500 fs to {approx}10 ps timescale. Accompanying the changes in electronic state is solvent reorganization, which occurs on a similar timescale. Over longer periods ({approx}1 ps to >200 ps), energy is transferred from vibrationally excite d I{sub 2}{sup -} to modes of the solvent, which in turn leads

  11. Static and dynamic optical properties of La1-xSrxFeO3-δ: The effects of A-site and oxygen stoichiometry

    SciTech Connect (OSTI)

    Sergey Y. Smolin; Sfeir, Matthew Y.; Scafetta, Mark D.; Choquette, Amber K.; Baxter, Jason B.; May, Steven J.

    2015-12-09

    Perovskite oxides are a promising material class for photovoltaic and photocatalytic applications due to their visible band gaps, nanosecond recombination lifetimes, and great chemical diversity. However, there is limited understanding of the link between composition and static and dynamic optical properties, despite the critical role these properties play in the design of light-harvesting devices. To clarify these relationships, we systemically studied the optoelectronic properties in La1-xSrxFeO3-δ epitaxial films, uncovering the effects of A-site cation substitution and oxygen stoichiometry. Variable-angle spectroscopic ellipsometry was used to measure static optical properties, revealing a linear increase in absorption coefficient at 1.25 eV and a red-shifting of the optical absorption edge with increasing Sr fraction. The absorption spectra can be similarly tuned through the introduction of oxygen vacancies, indicating the critical role that nominal Fe valence plays in optical absorption. Dynamic optoelectronic properties were studied with ultrafast transient reflectance spectroscopy, revealing similar nanosecond photoexcited carrier lifetimes for oxygen deficient and stoichiometric films with the same nominal Fe valence. Furthermore, these results demonstrate that while the static optical absorption is strongly dependent on nominal Fe valence tuned through cation or anion stoichiometry, oxygen vacancies do not appear to play a significantly detrimental role in the recombination kinetics.

  12. Global/Local Dynamic Models

    SciTech Connect (OSTI)

    Pfeffer, A; Das, S; Lawless, D; Ng, B

    2006-10-10

    Many dynamic systems involve a number of entities that are largely independent of each other but interact with each other via a subset of state variables. We present global/local dynamic models (GLDMs) to capture these kinds of systems. In a GLDM, the state of an entity is decomposed into a globally influenced state that depends on other entities, and a locally influenced state that depends only on the entity itself. We present an inference algorithm for GLDMs called global/local particle filtering, that introduces the principle of reasoning globally about global dynamics and locally about local dynamics. We have applied GLDMs to an asymmetric urban warfare environment, in which enemy units form teams to attack important targets, and the task is to detect such teams as they form. Experimental results for this application show that global/local particle filtering outperforms ordinary particle filtering and factored particle filtering.

  13. Gas-phase chemical dynamics

    SciTech Connect (OSTI)

    Weston, R.E. Jr.; Sears, T.J.; Preses, J.M.

    1993-12-01

    Research in this program is directed towards the spectroscopy of small free radicals and reactive molecules and the state-to-state dynamics of gas phase collision, energy transfer, and photodissociation phenomena. Work on several systems is summarized here.

  14. Fluid Dynamics with Free Surfaces

    Energy Science and Technology Software Center (OSTI)

    1992-02-01

    RIPPLE is a two-dimensional, transient, free surface incompressible fluid dynamics program. It allows multiple free surfaces with surface tension and wall adhesion forces and has a partial cell treatment which allows curved boundaries and interior obstacles.

  15. Dynamic Worldwide Solar Energy | Open Energy Information

    Open Energy Info (EERE)

    Worldwide Solar Energy Jump to: navigation, search Name: Dynamic Worldwide Solar Energy Sector: Solar Product: US-based solar developer and financer. References: Dynamic Worldwide...

  16. Soil Machine Dynamics Ltd | Open Energy Information

    Open Energy Info (EERE)

    Machine Dynamics Ltd Jump to: navigation, search Name: Soil Machine Dynamics Ltd Region: United Kingdom Sector: Marine and Hydrokinetic Website: http: This company is listed in the...

  17. Dynamic stall on wind turbine blades

    SciTech Connect (OSTI)

    Butterfield, C.P.; Simms, D.; Scott, G. ); Hansen, A.C. )

    1991-12-01

    Dynamic loads must be predicted accurately in order to estimate the fatigue life of wind turbines operating in turbulent environments. Dynamic stall contributes to increased dynamic loads during normal operation of all types of horizontal-axis wind turbine (HAWTs). This report illustrates how dynamic stall varies throughout the blade span of a 10 m HAWT during yawed and unyawed operating conditions. Lift, drag, and pitching moment coefficients during dynamics stall are discussed. Resulting dynamic loads are presented, and the effects of dynamic stall on yaw loads are demonstrated using a yaw loads dynamic analysis (YAWDYN). 12 refs., 22 figs., 1 tab.

  18. Magnetofluid dynamics in curved spacetime (Journal Article) ...

    Office of Scientific and Technical Information (OSTI)

    Magnetofluid dynamics in curved spacetime Citation Details In-Document Search Title: Magnetofluid dynamics in curved spacetime Authors: Bhattacharjee, Chinmoy ; Das, Rupam ; ...

  19. Dynamical symmetries in nuclear structure

    SciTech Connect (OSTI)

    Casten, R.F.

    1986-01-01

    In recent years the concept of dynamical symmetries in nuclei has witnessed a renaissance of interest and activity. Much of this work has been developed in the context of the Interacting Boson Approximation (or IBA) model. The appearance and properties of dynamical symmetries in nuclei will be reviewed, with emphasis on their characteristic signatures and on the role of the proton-neutron interaction in their formation, systematics and evolution. 36 refs., 20 figs.

  20. HAWT performance with dynamic stall

    SciTech Connect (OSTI)

    Hibbs, B.D.

    1986-02-01

    In this report we calculated the effects of flow nonuniformities (wing shear, tower wake, yaw, and large-scale turbulence) on the performance of a horizontal axis wind turbine, accounting for dynamic stall. We modified the PROP program to incorporate and compare these effects with the uniform flow case. The MIT model, which predicts dynamic lift coefficients substantially higher than the static maximum values and includes a crude model of the vortex roll-off phenomenon, represented dynamic stall. As associated model for drag was also used. The dynamic stall model was tested against experimental data for three typical reduced frequencies. Good instantaneous correlation was obtained. The effects of nonuniformities with and without the dynamic stall were calculated using the Westinghouse Mod O and Enertech 44/25 turbines. Modeling the dynamic stall has little effect on performance. Furthermore, the performance with nonuniform flow differed only slightly from the uniform flow case. Thus the now PROP model provides a powerful general capability to handle nonuniform flows.

  1. Dynamics near QCD critical point by dynamic renormalization group

    SciTech Connect (OSTI)

    Minami, Yuki

    2011-05-01

    We work out the basic analysis on dynamics near the QCD critical point (CP) by the dynamic renormalization group (RG). In addition to the RG analysis by coarse-graining, we construct the nonlinear Langevin equation as a basic equation for the critical dynamics. Our construction is based on the generalized Langevin theory and the relativistic hydrodynamics. Applying the dynamic RG to the constructed equation, we derive the RG equation for the transport coefficients and analyze their critical behaviors. We find that the resulting RG equation turns out to be the same as that for the liquid-gas CP except for an insignificant constant. Therefore, the bulk viscosity and the thermal conductivity strongly diverge at the QCD CP. We also show that the thermal and viscous diffusion modes exhibit critical slowing down with the dynamic critical exponents z{sub thermal}{approx}3 and z{sub viscous}{approx}2, respectively. In contrast, the sound propagating mode shows critical speeding up with the negative exponent z{sub sound}{approx}-0.8.

  2. Simple Dynamic Gasifier Model That Runs in Aspen Dynamics

    SciTech Connect (OSTI)

    Robinson, P.J.; Luyben, W.L.

    2008-10-15

    Gasification (or partial oxidation) is a vital component of 'clean coal' technology. Sulfur and nitrogen emissions can be reduced, overall energy efficiency is increased, and carbon dioxide recovery and sequestration are facilitated. Gasification units in an electric power generation plant produce a fuel for driving combustion turbines. Gasification units in a chemical plant generate gas, which can be used to produce a wide spectrum of chemical products. Future plants are predicted to be hybrid power/chemical plants with gasification as the key unit operation. The widely used process simulator Aspen Plus provides a library of models that can be used to develop an overall gasifier model that handles solids. So steady-state design and optimization studies of processes with gasifiers can be undertaken. This paper presents a simple approximate method for achieving the objective of having a gasifier model that can be exported into Aspen Dynamics. The basic idea is to use a high molecular weight hydrocarbon that is present in the Aspen library as a pseudofuel. This component should have the same 1:1 hydrogen-to-carbon ratio that is found in coal and biomass. For many plantwide dynamic studies, a rigorous high-fidelity dynamic model of the gasifier is not needed because its dynamics are very fast and the gasifier gas volume is a relatively small fraction of the total volume of the entire plant. The proposed approximate model captures the essential macroscale thermal, flow, composition, and pressure dynamics. This paper does not attempt to optimize the design or control of gasifiers but merely presents an idea of how to dynamically simulate coal gasification in an approximate way.

  3. Excitons, biexcitons, and higher-order correlations: Direct observations of

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    ultrafast many-body dynamics | MIT-Harvard Center for Excitonics Excitons, biexcitons, and higher-order correlations: Direct observations of ultrafast many-body dynamics April 15, 2009 at 3pm/36-428 Keith A. Nelson Department of Chemistry Massachusetts Institute of Technology nelson abstract: Much is known about the ultrafast dynamics of excitons in semiconductors and organic molecular systems. Far less is understood about higher-order correlations that may lead to bound multi-exciton

  4. The handbook of fluid dynamics

    SciTech Connect (OSTI)

    Johnson, R.W.

    1998-07-01

    This book provides professionals in the field of fluid dynamics with a comprehensive guide and resource. The book balances three traditional areas of fluid mechanics--theoretical, computational, and experimental--and expounds on basic science and engineering techniques. Each chapter introduces a topic, discusses the primary issues related to this subject, outlines approaches taken by experts, and supplies references for further information. Topics discussed include: (1) basic engineering fluid dynamics; (2) classical fluid dynamics; (3) turbulence modeling; (4) reacting flows; (5) multiphase flows; (6) flow and porous media; (7) high Reynolds number asymptotic theories; (8) finite difference method; (9) finite volume method; (10) finite element methods; (11) spectral element methods for incompressible flows; (12) experimental methods, such as hot-wire anemometry, laser-Doppler velocimetry, and flow visualization; and (13) applications, such as axial-flow compressor and fan aerodynamics, turbomachinery, airfoils and wings, atmospheric flows, and mesoscale oceanic flows.

  5. Fissile solution dynamics: Student research

    SciTech Connect (OSTI)

    Hetrick, D.L.

    1994-09-01

    There are two research projects in criticality safety at the University of Arizona: one in dynamic simulation of hypothetical criticality accidents in fissile solutions, and one in criticality benchmarks using transport theory. We have used the data from nuclear excursions in KEWB, CRAC, and SILENE to help in building models for solution excursions. An equation of state for liquids containing gas bubbles has been developed and coupled to point-reactor dynamics in an attempt to predict fission rate, yield, pressure, and kinetic energy. It appears that radiolytic gas is unimportant until after the first peak, but that it does strongly affect the shape of the subsequent power decrease and also the dynamic pressure.

  6. Dynamics of femtosecond laser produced tungsten nanoparticle plumes

    SciTech Connect (OSTI)

    Harilal, S. S.; Hassanein, A.; Farid, N.; School of Physics and Optical Engineering, Dalian University of Technology, Dalian 116024 ; Kozhevin, V. M.

    2013-11-28

    We investigated the expansion features of femtosecond laser generated tungsten nanoparticle plumes in vacuum. Fast gated images showed distinct two components expansion features, viz., plasma and nanoparticle plumes, separated by time of appearance. The persistence of plasma and nanoparticle plumes are ?500 ns and ?100 ?s, respectively, and propagating with velocities differed by 25 times. The estimated temperature of the nanoparticles showed a decreasing trend with increasing time and space. Compared to low-Z materials (e.g., Si), ultrafast laser ablation of high-Z materials like W provides significantly higher nanoparticle yield. A comparison between the nanoparticle plumes generated by W and Si is also discussed along with other metals.

  7. reactive ion solvation and solid-liquid interfacial reactions...

    Office of Scientific and Technical Information (OSTI)

    Biology: Theory, simulation, modelling held July 9-12, 2012 in Telluride, CO.; Related Information: Proposed for presentation at the Ions in Aqueous Solutions and Molecular Biology...

  8. Lithium Ion Solvation and Diffusion in Bulk Organic Electrolytes...

    Office of Scientific and Technical Information (OSTI)

    DOE Contract Number: DE-AC52-07NA27344 Resource Type: Conference Resource Relation: Conference: Presented at: ACS Spring Meeting 2015, Denver, CO, United States, Mar 22 - Mar 26, ...

  9. Anomalous Density Properties and Ion Solvation in Liquid Water...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    to a number of fields, ranging from biologybiochemistry to energy storage and electrochemistry. Several key properties of water, are crucial for understanding and predicting...

  10. Linking Ion Solvation and Lithium Battery Electrolyte Properties

    Broader source: Energy.gov [DOE]

    2010 DOE Vehicle Technologies and Hydrogen Programs Annual Merit Review and Peer Evaluation Meeting, June 7-11, 2010 -- Washington D.C.

  11. Influence of Molecular Solvation on the Conformation of Star...

    Office of Scientific and Technical Information (OSTI)

    Authors: Li, Xin 1 ; Porcar, L. 2 ; Sanchez-Diaz, Luis E 1 ; Do, Changwoo 1 ; Liu, Yun 2 ; Smith, Gregory Scott 1 ; Hong, Kunlun 1 ; Chen, Wei-Ren 1 + Show Author ...

  12. Lithium Ion Solvation and Diffusion in Bulk Organic Electrolytes...

    Office of Scientific and Technical Information (OSTI)

    DOE Contract Number: DE-AC52-07NA27344 Resource Type: Journal Article Resource Relation: Journal Name: Journal of Physical Chemistry B, vol. 119, no. 14, December 19, 2014, pp. ...

  13. Linking Ion Solvation and Lithium Battery Electrolyte Properties...

    Broader source: Energy.gov (indexed) [DOE]

    Liquids for Lithium Battery Electrolytes Inexpensive, Nonfluorinated (or Partially Fluorinated) Anions for Lithium Salts and Ionic Liquids for Lithium Battery Electrolytes ...

  14. Final Progress Report for Linking Ion Solvation and Lithium Battery...

    Office of Scientific and Technical Information (OSTI)

    of an in-depth analysis of the thermal phase behavior of diverse solvent-LiX ... Country of Publication: United States Language: English Subject: 25 ENERGY STORAGE ...

  15. Ionic strength independence of charge distributions in solvation...

    Office of Scientific and Technical Information (OSTI)

    surrounding the biomolecules, as well as the contributions of ions to the electrostatic free energy of interaction between the biomolecule and the surrounding salt solution (for...

  16. Tuned range separated hybrid functionals for solvated low bandgap...

    Office of Scientific and Technical Information (OSTI)

    and the ambiguities of straightforward parameter tuning in solution are elucidated. ... Resource Type: Journal Article Resource Relation: Journal Name: Journal of Chemical Physics; ...

  17. Final Progress Report for Linking Ion Solvation and Lithium Battery...

    Office of Scientific and Technical Information (OSTI)

    ... Close Cite: Bibtex Format Close 0 pages in this document matching the terms "" Search For Terms: Enter terms in the toolbar above to search the full text of this document for ...

  18. Dynamics of Block Copolymer Nanocomposites

    SciTech Connect (OSTI)

    Mochrie, Simon G. J.

    2014-09-09

    A detailed study of the dynamics of cadmium sulfide nanoparticles suspended in polystyrene homopolymer matrices was carried out using X-ray photon correlation spectroscopy for temperatures between 120 and 180 C. For low molecular weight polystyrene homopolymers, the observed dynamics show a crossover from diffusive to hyper-diffusive behavior with decreasing temperatures. For higher molecular weight polystyrene, the nanoparticle dynamics appear hyper-diffusive at all temperatures studied. The relaxation time and characteristic velocity determined from the measured hyper-diffusive dynamics reveal that the activation energy and underlying forces determined are on the order of 2.14 10?19 J and 87 pN, respectively. We also carried out a detailed X-ray scattering study of the static and dynamic behavior of a styrene isoprene diblock copolymer melt with a styrene volume fraction of 0.3468. At 115 and 120 C, we observe splitting of the principal Bragg peak, which we attribute to phase coexistence of hexagonal cylindrical and cubic double- gyroid structure. In the disordered phase, above 130 C, we have characterized the dynamics of composition fluctuations via X-ray photon correlation spectroscopy. Near the peak of the static structure factor, these fluctuations show stretched-exponential relaxations, characterized by a stretching exponent of about 0.36 for a range of temperatures immediately above the MST. The corresponding characteristic relaxation times vary exponentially with temperature, changing by a factor of 2 for each 2 C change in temperature. At low wavevectors, the measured relaxations are diffusive with relaxation times that change by a factor of 2 for each 8 C change in temperature.

  19. Fairness and dynamic pricing: comments

    SciTech Connect (OSTI)

    Hogan, William W.

    2010-07-15

    In ''The Ethics of Dynamic Pricing,'' Ahmad Faruqui lays out a case for improved efficiency in using dynamic prices for retail electricity tariffs and addresses various issues about the distributional effects of alternative pricing mechanisms. The principal contrast is between flat or nearly constant energy prices and time-varying prices that reflect more closely the marginal costs of energy and capacity. The related issues of fairness criteria, contracts, risk allocation, cost allocation, means testing, real-time pricing, and ethical policies of electricity market design also must be considered. (author)

  20. Theoretical studies of combustion dynamics

    SciTech Connect (OSTI)

    Bowman, J.M.

    1993-12-01

    The basic objectives of this research program are to develop and apply theoretical techniques to fundamental dynamical processes of importance in gas-phase combustion. There are two major areas currently supported by this grant. One is reactive scattering of diatom-diatom systems, and the other is the dynamics of complex formation and decay based on L{sup 2} methods. In all of these studies, the authors focus on systems that are of interest experimentally, and for which potential energy surfaces based, at least in part, on ab initio calculations are available.

  1. Austenite stabilization and high strength-elongation product of a low silicon aluminum-free hot-rolled directly quenched and dynamically partitioned steel

    SciTech Connect (OSTI)

    Tan, Xiao-Dong; Xu, Yun-Bo; Yang, Xiao-Long; Hu, Zhi-Ping; Peng, Fei; Ju, Xiao-Wei; Wu, Di

    2015-06-15

    Microstructures composed of lath martensite and retained austenite with volume fraction between 8.0 vol.% and 12.0 vol.% were obtained in a low-C low-Si Al-free steel through hot-rolling direct quenching and dynamical partitioning (HDQ&DP) processes. The austenite stabilization mechanism in the low-C low-Si Al-free steel under the special dynamical partitioning processes is investigated by analyzing the carbon partition behavior from martensite to austenite and the carbide precipitation-coarsening behavior in martensite laths combining with the possible hot rolling deformation inheritance. Results show that the satisfying retained austenite amount in currently studied low-Si Al-free HDQ&DP steel is caused by the high-efficiency carbon enrichment in the 30–80 nm thick regions of austenite near the interfaces in the hot-rolled ultra-fast cooled structure and the avoidance of serious carbides coarsening during the continuous cooling procedures. The excellent strength-elongation product reaching up to 26,000 MPa% shows that the involved HDQ&DP process is a promising method to develop a new generation of advanced high strength steel. - Highlights: • HDQ&DP processes were applied to a low-C low-Si Al-free steel. • Effective partitioning time during the continuous cooling processes is 1–220 s. • Retained austenite with volume fraction between 8.0 vol. % and 12.0 vol. % has been obtained. • The special austenite stabilization mechanism has been expounded.

  2. Haidan Wen | Argonne National Laboratory

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    and Technology of China in 2001. Dr. Wen's research is focused on investigating ultrafast dynamics of multiple degrees of freedom such as lattice, charge, spin and magnetic orders...

  3. 2D heterodyne-detected sum frequency generation study on the...

    Office of Scientific and Technical Information (OSTI)

    sum frequency generation study on the ultrafast vibrational dynamics of Hsub 2O and HOD water at charged interfaces Citation Details In-Document Search Title:...

  4. Dr. Naomi Ginsberg | Photosynthetic Antenna Research Center

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Naomi Ginsberg October 17, 2013 Dr. Naomi Ginsberg Imaging heterogeneous ultrafast exciton dynamics in organic semiconducting thin films Published: October 17, 2013

  5. Uncovering the Operating Principles of Photoelectrodes

    SciTech Connect (OSTI)

    2015-12-01

    NREL Highlights Fact Sheet: NREL scientists developed an ultrafast spectroscopic probe that is specifically sensitive to the carrier dynamics at critically important interfaces.

  6. Applied Science/Techniques

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    New Spectroscopic Technique Reveals the Dynamics of Operating Battery Electrodes ... The ALS X-Ray Streak Camera: Bringing the Ultrafast and Ultrasmall into Focus Laser ...

  7. Beamline 6.0.1

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    1 Print Ultrafast Femtosecond Dynamics Hard X Ray GENERAL BEAMLINE INFORMATION Operational Yes, but not open to General Users Source characteristics 3-cm period undulator (U3)...

  8. Frederic Laquai Seminar: Photocurrent Generation in Low-Bandgap...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    ... In: G. Gurzadyan, G. Lanzani, C. Soci, T.C. Sum (Ed.): Ultrafast Dynamics in Molecules, Nanostructures and Interfaces, World Scientific - Series in Optics and Photonics - Vol. 8 ...

  9. Center for Advanced Solar Photophysics | Members

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    of ultrafast charge-carrier dynamics in nanomaterials of interest for use in third-generation photovoltaics. An introduction to well-established femtosecond spectroscopy...

  10. Shock compression of precompressed deuterium (Conference) | SciTech...

    Office of Scientific and Technical Information (OSTI)

    VA at www.ntis.gov. Here we report quasi-isentropic dynamic compression and thermodynamic characterization of solid, precompressed deuterium over an ultrafast time scale (< 100 ps)...

  11. Dynamical systems probabilistic risk assessment.

    SciTech Connect (OSTI)

    Denman, Matthew R.; Ames, Arlo Leroy

    2014-03-01

    Probabilistic Risk Assessment (PRA) is the primary tool used to risk-inform nuclear power regulatory and licensing activities. Risk-informed regulations are intended to reduce inherent conservatism in regulatory metrics (e.g., allowable operating conditions and technical specifications) which are built into the regulatory framework by quantifying both the total risk profile as well as the change in the risk profile caused by an event or action (e.g., in-service inspection procedures or power uprates). Dynamical Systems (DS) analysis has been used to understand unintended time-dependent feedbacks in both industrial and organizational settings. In dynamical systems analysis, feedback loops can be characterized and studied as a function of time to describe the changes to the reliability of plant Structures, Systems and Components (SSCs). While DS has been used in many subject areas, some even within the PRA community, it has not been applied toward creating long-time horizon, dynamic PRAs (with time scales ranging between days and decades depending upon the analysis). Understanding slowly developing dynamic effects, such as wear-out, on SSC reliabilities may be instrumental in ensuring a safely and reliably operating nuclear fleet. Improving the estimation of a plant's continuously changing risk profile will allow for more meaningful risk insights, greater stakeholder confidence in risk insights, and increased operational flexibility.

  12. HelioDynamics Ltd | Open Energy Information

    Open Energy Info (EERE)

    HelioDynamics Ltd Jump to: navigation, search Name: HelioDynamics Ltd Place: Cambridge, United Kingdom Zip: CB23 2SH Sector: Solar Product: Manufactures the HD211 product - a solar...

  13. Dynamic imaging with electron microscopy

    ScienceCinema (OSTI)

    Campbell, Geoffrey; McKeown, Joe; Santala, Melissa

    2014-05-30

    Livermore researchers have perfected an electron microscope to study fast-evolving material processes and chemical reactions. By applying engineering, microscopy, and laser expertise to the decades-old technology of electron microscopy, the dynamic transmission electron microscope (DTEM) team has developed a technique that can capture images of phenomena that are both very small and very fast. DTEM uses a precisely timed laser pulse to achieve a short but intense electron beam for imaging. When synchronized with a dynamic event in the microscope's field of view, DTEM allows scientists to record and measure material changes in action. A new movie-mode capability, which earned a 2013 R&D 100 Award from R&D Magazine, uses up to nine laser pulses to sequentially capture fast, irreversible, even one-of-a-kind material changes at the nanometer scale. DTEM projects are advancing basic and applied materials research, including such areas as nanostructure growth, phase transformations, and chemical reactions.

  14. Predissociation dynamics of lithium iodide

    SciTech Connect (OSTI)

    Schmidt, H.; Vangerow, J. von; Stienkemeier, F.; Mudrich, M.; Bogomolov, A. S.; Baklanov, A. V.; Reich, D. M.; Skomorowski, W.; Koch, C. P.

    2015-01-28

    The predissociation dynamics of lithium iodide (LiI) in the first excited A-state is investigated for molecules in the gas phase and embedded in helium nanodroplets, using femtosecond pump-probe photoionization spectroscopy. In the gas phase, the transient Li{sup +} and LiI{sup +} ion signals feature damped oscillations due to the excitation and decay of a vibrational wave packet. Based on high-level ab initio calculations of the electronic structure of LiI and simulations of the wave packet dynamics, the exponential signal decay is found to result from predissociation predominantly at the lowest avoided X-A potential curve crossing, for which we infer a coupling constant V{sub XA} = 650(20) cm{sup −1}. The lack of a pump-probe delay dependence for the case of LiI embedded in helium nanodroplets indicates fast droplet-induced relaxation of the vibrational excitation.

  15. Los Alamos Dynamics Summer School Projects

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Los Alamos Dynamics Summer School » Los Alamos Dynamics Summer School-Overview Los Alamos Dynamics Summer School Projects Los Alamos Dynamics Summer School Projects and Resources Contact Institute Director Charles Farrar (505) 665-0860 Email Executive Administrator Ellie Vigil (505) 667-2818 Email Administrative Assistant Rebecca Duran (505) 665-8899 Email Past Programs and Resources 2015 2014 STUDENT RESOURCES Precollege Undergrads Graduates Postdocs Housing Los Alamos National Laboratory Logo

  16. Development of a Dynamic DOE Calibration Model

    Broader source: Energy.gov [DOE]

    A dynamic heavy duty diesel engine model was developed. The model can be applied for calibration and control system optimization.

  17. Insight Gained from Simplified Dynamic Analysis

    Broader source: Energy.gov [DOE]

    Insight Gained from Simplified Dynamic Analysis ... or Everything Old is New Again October 21, 2014 Greg Mertz Consultant

  18. Dynamical coupled-channel analysis at EBAC

    SciTech Connect (OSTI)

    T.-S. H. Lee

    2007-08-01

    The status and progress of the dynamical coupled-channel analysis at the Excited Baryon Analysis Center (EBAC) is reported.

  19. Sandia National Laboratories: Dynamic Materials

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Dynamic Materials Compressing materials under extreme conditions Pushing forward the frontiers of high-energy-density science Sandia Physicist, Marcus Knudson Sandia scientists are investigating the behavior of a wide-range of materials under the extreme conditions of very high pressures and densities. They seek the answers to such questions as: When do insulators become a metal? How strong do materials become when they are compressed? How and when do materials change their phase at very high

  20. Sierra Structural Dynamics User's Notes

    SciTech Connect (OSTI)

    Reese, Garth M.

    2015-10-19

    Sierra/SD provides a massively parallel implementation of structural dynamics finite element analysis, required for high fidelity, validated models used in modal, vibration, static and shock analysis of weapons systems. This document provides a users guide to the input for Sierra/SD. Details of input specifications for the different solution types, output options, element types and parameters are included. The appendices contain detailed examples, and instructions for running the software on parallel platforms.