National Library of Energy BETA

Sample records for ultrafast solvation dynamics

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

    SciTech Connect (OSTI)

    Wishart, J.F.

    2011-06-12

    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 generally have low volatilities and are combustion-resistant, 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 primary radiation chemistry, 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 reactions and product distributions. We study these issues by characterization of primary radiolysis products and measurements of their yields and reactivity, quantification of electron solvation dynamics and scavenging of electrons in different states of solvation. From this knowledge we wish to learn how to predict radiolytic mechanisms and control them or mitigate their effects on the properties of materials used in nuclear fuel processing, for example, and to apply IL radiation chemistry to answer questions about general chemical reactivity in ionic liquids that will aid in the development of applications listed above. Very early in our radiolysis studies it became evident that the slow solvation dynamics of the excess electron in ILs (which vary over a wide viscosity range) increase the importance of pre-solvated electron reactivity and consequently alter product distributions and subsequent chemistry. This difference from conventional solvents has profound effects on predicting and controlling radiolytic yields, 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.

  2. 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.

  3. 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.

  4. Ultrafast dynamic ellipsometry of laser driven shock waves

    E-Print Network [OSTI]

    Bolme, Cynthia Anne

    2008-01-01

    The experimental measurement technique of ultrafast dynamic ellipsometry (UDE) was developed for measuring material motion and changes in optical properties of samples under laser driven shock loading. Ultrafast dynamic ...

  5. Mode coupling theory of electrolyte dynamics: Time dependent diffusion, dynamic structure factor and solvation dynamics

    E-Print Network [OSTI]

    Susmita Roy; Subramanian Yashonath; Biman Bagchi

    2015-01-08

    A self-consistent mode coupling theory (MCT) with microscopic inputs of equilibrium pair correlation functions is developed to analyze electrolyte dynamics. We apply the theory to calculate concentration dependence of (i) time dependent ion diffusion, (ii) dynamic structure factor of the constituent ions, and (iii) ion solvation dynamics in electrolyte solution. Brownian dynamics (BD) with implicit water molecules and molecular dynamics (MD) method with explicit water are used to check the theoretical predictions. The time dependence of ionic self-diffusion coefficient and the corresponding dynamic structure factor evaluated from our MCT approach show quantitative agreement with early experimental and present Brownian dynamic simulation results. With increasing concentration, the dispersion of electrolyte friction is found to occur at increasingly higher frequency, due to the faster relaxation of the ion atmosphere. The wave number dependence of total dynamic structure factor F(k,t), exhibits markedly different relaxation dynamics at different length scales. At small wave numbers, we find the emergence of a step-like relaxation, indicating the presence of both fast and slow time scales in the system. Such behaviour allows an intriguing analogy with temperature dependent relaxation dynamics of supercooled liquids. We find that solvation dynamics of a tagged ion exhibits a power law decay at long times- the decay can also be fitted to a stretched exponential form. The emergence of the power law in solvation dynamics has been tested by carrying out long Brownian dynamics simulations with varying ionic concentrations. This solvation time correlation and ion-ion dynamic structure factor indeed exhibits highly interesting, non-trivial dynamical behaviour at intermediate to longer times that require further experimental and theoretical studies.

  6. Probing Ultrafast Solvation Dynamics with High Repetition-Rate...

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

    systems. Thanks to implementation of a high-repetition-rate (54 kHz-6.5 MHz), high-power (>10 W) laser system at the X-ray Science Division 7-ID-D beamline at the Advanced...

  7. Ultrafast Core-Hole Induced Dynamics in Water

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

    the fluorescence from an electron reoccupying the oxygen 1s core level is measured. For hydrogen-bonded systems such as liquid water, ultrafast dynamics that occur during the...

  8. Multiple time step molecular dynamics in the optimized isokinetic ensemble steered with the molecular theory of solvation: Accelerating with advanced extrapolation of effective solvation forces

    SciTech Connect (OSTI)

    Omelyan, Igor, E-mail: omelyan@ualberta.ca, E-mail: omelyan@icmp.lviv.ua [National Institute for Nanotechnology, 11421 Saskatchewan Drive, Edmonton, Alberta T6G 2M9 (Canada) [National Institute for Nanotechnology, 11421 Saskatchewan Drive, Edmonton, Alberta T6G 2M9 (Canada); Department of Mechanical Engineering, University of Alberta, Edmonton, Alberta T6G 2G8 (Canada); Institute for Condensed Matter Physics, National Academy of Sciences of Ukraine, 1 Svientsitskii Street, Lviv 79011 (Ukraine); Kovalenko, Andriy, E-mail: andriy.kovalenko@nrc-cnrc.gc.ca [National Institute for Nanotechnology, 11421 Saskatchewan Drive, Edmonton, Alberta T6G 2M9 (Canada) [National Institute for Nanotechnology, 11421 Saskatchewan Drive, Edmonton, Alberta T6G 2M9 (Canada); Department of Mechanical Engineering, University of Alberta, Edmonton, Alberta T6G 2G8 (Canada)

    2013-12-28

    We develop efficient handling of solvation forces in the multiscale method of multiple time step molecular dynamics (MTS-MD) of a biomolecule steered by the solvation free energy (effective solvation forces) obtained from the 3D-RISM-KH molecular theory of solvation (three-dimensional reference interaction site model complemented with the Kovalenko-Hirata closure approximation). To reduce the computational expenses, we calculate the effective solvation forces acting on the biomolecule by using advanced solvation force extrapolation (ASFE) at inner time steps while converging the 3D-RISM-KH integral equations only at large outer time steps. The idea of ASFE consists in developing a discrete non-Eckart rotational transformation of atomic coordinates that minimizes the distances between the atomic positions of the biomolecule at different time moments. The effective solvation forces for the biomolecule in a current conformation at an inner time step are then extrapolated in the transformed subspace of those at outer time steps by using a modified least square fit approach applied to a relatively small number of the best force-coordinate pairs. The latter are selected from an extended set collecting the effective solvation forces obtained from 3D-RISM-KH at outer time steps over a broad time interval. The MTS-MD integration with effective solvation forces obtained by converging 3D-RISM-KH at outer time steps and applying ASFE at inner time steps is stabilized by employing the optimized isokinetic Nosé-Hoover chain (OIN) ensemble. Compared to the previous extrapolation schemes used in combination with the Langevin thermostat, the ASFE approach substantially improves the accuracy of evaluation of effective solvation forces and in combination with the OIN thermostat enables a dramatic increase of outer time steps. We demonstrate on a fully flexible model of alanine dipeptide in aqueous solution that the MTS-MD/OIN/ASFE/3D-RISM-KH multiscale method of molecular dynamics steered by effective solvation forces allows huge outer time steps up to tens of picoseconds without affecting the equilibrium and conformational properties, and thus provides a 100- to 500-fold effective speedup in comparison to conventional MD with explicit solvent. With the statistical-mechanical 3D-RISM-KH account for effective solvation forces, the method provides efficient sampling of biomolecular processes with slow and/or rare solvation events such as conformational transitions of hydrated alanine dipeptide with the mean life times ranging from 30 ps up to 10 ns for “flip-flop” conformations, and is particularly beneficial for biomolecular systems with exchange and localization of solvent and ions, ligand binding, and molecular recognition.

  9. Ultrafast Core-Hole Induced Dynamics in Water

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

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  10. Hydrogen Bond Dynamics Probed with Ultrafast Infrared Heterodyne-Detected Multidimensional Vibrational Stimulated Echoes

    E-Print Network [OSTI]

    Fayer, Michael D.

    Hydrogen Bond Dynamics Probed with Ultrafast Infrared Heterodyne-Detected Multidimensional, USA (Received 24 February 2003; published 3 December 2003) Hydrogen bond dynamics are explicated hydrogen bonded network are measured with ultrashort (

  11. Dynamics of Solvated Electrons in Clusters Ryan M. Young,

    E-Print Network [OSTI]

    Neumark, Daniel M.

    in Water-Based Cluster Anions 5561 3.3. Dynamics in Halide-Water Clusters 5563 4. Methanol 5564 5. Ammonia 5567 6. Acetonitrile and Primary Amides 5568 7. Benzene, Toluene, and Other Aromatic Solvents 5571 8

  12. 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.

  13. Ultrafast Dynamics of 1,3-Cyclohexadiene in Highly Excited States

    E-Print Network [OSTI]

    Minitti, Michael P.

    2011-01-01

    The ultrafast dynamics of 1,3-cyclohexadiene has been investigated via structurally sensitive Rydberg electron binding energies and shown to differ upon excitation to the 1B state and the 3p Rydberg state. Excitation of ...

  14. 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 molecule’s 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 molecule’s 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 molecular species in the hot environments of combustion processes, there are several features that make the Rydberg ionization spectroscopy uniquely useful. First, the Rydberg electron’s orbit is quite large and covers the entire molecule for most molecular structures of combustion interest. Secondly, the ionization does not change vibrational quantum numbers, so that even complicated and large molecules can be observed with fairly well resolved spectra. In fact, the spectroscopy is blind to vibrational excitation of the molecule. This has the interesting consequence for the study of chemical dynamics, where the molecules are invariably very energetic, that the molecular structures are observed unobstructed by the vibrational congestion that dominates other spectroscopies. This implies also that, as a tool to probe the time-dependent structural dynamics of chemically interesting molecules, Rydberg spectroscopy may well be better suited than electron or x-ray diffraction. With recent progress in calculating Rydberg binding energy spectra, we are approaching the point where the method can be evolved into a structure determination method. To implement the Rydberg ionization spectroscopy we use a molecular beam based, time-resolved pump-probe multi-photon ionization/photoelectron scheme in which a first laser pulse excites the molecule to a Rydberg state, and a probe pulse ionizes the molecule. A time-of-flight detector measures the kinetic energy spectrum of the photoelectrons. The photoelectron spectrum directly provides the binding energy of the electron, and thereby reveals the molecule’s time-dependent structural fingerprint. Only the duration of the laser pulses limits the time resolution. With a new laser system, we have now reached time resolutions better than 100 fs, although very deep UV wavelengths (down to 190 nm) have slightly longer instrument functions. The structural dynamics of molecules in Rydberg-excited states is obtained by delaying the probe ionization photon from the pump photon; the structural dynamics of molecules in their ground state or e

  15. Neuroglobin dynamics observed with ultrafast 2D-IR vibrational echo spectroscopy

    E-Print Network [OSTI]

    Fayer, Michael D.

    Neuroglobin dynamics observed with ultrafast 2D-IR vibrational echo spectroscopy Haruto Ishikawa Contributed by Michael D. Fayer, August 15, 2007 (sent for review July 25, 2007) Neuroglobin (Ngb), a protein energy minimum. myoglobin mutants protein dynamics energy landscape Neuroglobin (Ngb) is a recently

  16. Ultrafast Electron Dynamics at Alkali/Ice Structures

    E-Print Network [OSTI]

    Wolf, Martin

    trapping sites, i.e. at local potential minima, are formed. Photoinjection of excess electrons into these alkali-ion covered amorphous ice layers, results in the trapping of a solvated electron at an alkali, i.e. pump-probe time delay, the electron transfer is mediated by tunneling through a potential

  17. Ultrafast Core-Hole Induced Dynamics in Water

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

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  18. Ultrafast dynamics of nonequilibrium electrons in metals under femtosecond laser irradiation B. Rethfeld*

    E-Print Network [OSTI]

    von der Linde, D.

    Ultrafast dynamics of nonequilibrium electrons in metals under femtosecond laser irradiation B with an ultrashort laser pulse leads to a disturbance of the free-electron gas out of thermal equilibrium. We investigate theoretically the transient evolution of the distribution function of the electron gas in a metal

  19. Control of ultrafast electron dynamics with shaped femtosecond laser pulses: from atoms to solids

    E-Print Network [OSTI]

    Peinke, Joachim

    focus on advanced control of ultrafast electron dynamics with shaped femtosecond laser pulses of a femtosecond laser pulse, in addition to its temporal envelope and phase. Before we present some recent the photoionization of potassium atoms with a phase-coherent double pulse sequence. Building on this simple example we

  20. Dynamics of Hemoglobin in Human Erythrocytes and in Solution: Influence of Viscosity Studied by Ultrafast

    E-Print Network [OSTI]

    Fayer, Michael D.

    Dynamics of Hemoglobin in Human Erythrocytes and in Solution: Influence of Viscosity Studied by Ultrafast Vibrational Echo Experiments Brian L. McClain, Ilya J. Finkelstein, and M. D. Fayer* Contribution experiments are used to measure the vibrational dephasing of the CO stretching mode of hemoglobin-CO (Hb

  1. Water Dynamics in Salt Solutions Studied with Ultrafast Two-Dimensional Infrared (2D IR)

    E-Print Network [OSTI]

    Fayer, Michael D.

    Water Dynamics in Salt Solutions Studied with Ultrafast Two-Dimensional Infrared (2D IR. Many of these species are charged. In the ocean, water interacts with dissolved salts. In biological systems, water interacts with dissolved salts as well as charged amino acids, the zwitterionic head groups

  2. Probing Ultrafast Dynamics with Time-resolved Multi-dimensional Coincidence Imaging: Butadiene

    E-Print Network [OSTI]

    Hockett, Paul; Rytwinski, Andrew; Stolow, Albert

    2013-01-01

    Time-resolved coincidence imaging of photoelectrons and photoions represents the most complete experimental measurement of ultrafast excited state dynamics, a multi-dimensional measurement for a multi-dimensional problem. Here we present the experimental data from recent coincidence imaging experiments, undertaken with the aim of gaining insight into the complex ultrafast excited-state dynamics of 1,3-butadiene initiated by absorption of 200 nm light. We discuss photoion and photoelectron mappings of increasing dimensionality, and focus particularly on the time-resolved photoelectron angular distributions (TRPADs), expected to be a sensitive probe of the electronic evolution of the excited state and to provide significant information beyond the time-resolved photoelectron spectrum (TRPES). Complex temporal behaviour is observed in the TRPADs, revealing their sensitivity to the dynamics while also emphasising the difficulty of interpretation of these complex observables. From the experimental data some details...

  3. Ultrafast Core-Hole Induced Dynamics in Water

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  4. Ultrafast Core-Hole Induced Dynamics in Water

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

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  5. Analysis of the Ultra-fast Switching Dynamics in a Hybrid MOSFET/Driver

    SciTech Connect (OSTI)

    Tang, T.; Burkhart, C.; /SLAC

    2011-08-17

    The turn-on dynamics of a power MOSFET during ultra-fast, {approx} ns, switching are discussed in this paper. The testing was performed using a custom hybrid MOSFET/Driver module, which was fabricated by directly assembling die-form components, power MOSFET and drivers, on a printed circuit board. By using die-form components, the hybrid approach substantially reduces parasitic inductance, which facilitates ultra-fast switching. The measured turn on time of the hybrid module with a resistive load is 1.2 ns with an applied voltage of 1000 V and drain current of 33 A. Detailed analysis of the switching waveforms reveals that switching behavior must be interpreted differently in the ultra-fast regime. For example, the gate threshold voltage to turn on the device is observed to increase as the switching time decreases. Further analysis and simulation of MOSFET switching behavior shows that the minimum turn on time scales with the product of the drain-source on resistance and drain-source capacitance, R{sub DS(on)}C{sub OSS}. This information will be useful in power MOSFET selection and gate driver design for ultra-fast switching applications.

  6. Semiclassical molecular dynamics simulations of ultrafast photodissociation dynamics associated with the Chappuis band of ozone

    SciTech Connect (OSTI)

    Batista, V.S.; Miller, W.H. [Department of Chemistry, University of California, and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)] [Department of Chemistry, University of California, and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)

    1998-01-01

    In this paper we investigate the nonadiabatic ultrafast dynamics of interconversion between the two lower lying excited states of {sup 1}A{sup {double_prime}} symmetry (1 {sup 1}A{sup {double_prime}} and 2 {sup 1}A{sup {double_prime}}) of ozone following photoexcitation of the molecule in the gas phase with visible light. Our algorithm involves a semiclassical initial value representation method which is able to describe electronically nonadiabatic processes within the time dependent picture through the quantization of the classical electron{endash}nuclear model Hamiltonian of Meyer and Miller [J. Chem. Phys. {bold 70}, 7 (1979)]. We explore the capabilities of these techniques as applied to studying the dynamics of a realistic reaction of photodissociation on full {ital ab initio} electronic potential energy surfaces. Our semiclassical results provide an intuitive understanding of the most fundamental dynamical features involved in the process of predissociation, such as decay and recurrence events, as well as an interpretation of experimental studies of the Chappuis band of ozone in the frequency domain. {copyright} {ital 1998 American Institute of Physics.}

  7. Structure and energetics of solvated ferrous and ferric ions: Car-Parrinello molecular dynamics in the DFT+U formalism

    E-Print Network [OSTI]

    P. H. -L. Sit; Matteo Cococcioni; Nicola Marzari

    2007-01-12

    We implemented a rotationally-invariant Hubbard U extension to density-functional theory in the Car-Parrinello molecular dynamics framework, with the goal of bringing the accuracy of the DFT+U approach to finite-temperature simulations, especially for liquids or solids containing transition-metal ions. First, we studied the effects on the Hubbard U on the static equilibrium structure of the hexa-aqua ferrous and ferric ions, and the inner-sphere reorganization energy for the electron-transfer reaction between aqueous ferrous and ferric ions. It is found that the reorganization energy is increased, mostly as a result of the Fe-O distance elongation in the hexa-aqua ferrous ion. Second, we performed a first-principles molecular dynamics study of the solvation structure of the two aqueous ferrous and ferric ions. The Hubbard term is found to change the Fe-O radial distribution function for the ferrous ion, while having a negligible effect on the aqueous ferric ion. Moreover, the frequencies of vibrations between Fe and oxygen atoms in the first-solvation shell are shown to be unaffected by the Hubbard corrections for both ferrous and ferric ions.

  8. Ultrafast Core-Hole Induced Dynamics in Water

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

    probed. In addition, by performing the same measurements using molecules of different nuclear masses, any differences in the dynamics will become apparent, and an observed isotope...

  9. Ultrafast reaction dynamics in cluster ions: Simulation of the transient photoelectron spectrum of I2 Arn photodissociation

    E-Print Network [OSTI]

    Faeder, Jim

    Hamiltonian model of electronic structure with nonadiabatic molecular dynamics simulations, we calculate of the electronic structure of a manifold of states strongly coupled to the many solvent degrees of freedomUltrafast reaction dynamics in cluster ions: Simulation of the transient photoelectron spectrum

  10. Ultrafast optical studies of electronic dynamics in semiconductors

    E-Print Network [OSTI]

    Ruzicka, Brian Andrew

    2012-05-31

    The dynamics of charge carriers in semiconductors are of fundamental importance for semiconductor applications. This includes studies of energy relaxation, carrier recombination, and carrier transport (both diffusive and ballistic). Due...

  11. Evidence for Conical Intersection Dynamics Mediating Ultrafast Singlet Exciton Fission

    E-Print Network [OSTI]

    Musser, Andrew J.; Liebel, Matz; Schnedermann, Christoph; Wende, Torsten; Kehoe, Tom B.; Rao, Akshay; Kukura, Philipp

    2015-03-16

    films of pentacene and TIPS-pentacene exhibit triplet formation with a time constant of 80 fs and yields of 200%2,3. Current interest in this phenomenon is driven by its potential to circumvent the Shockley-Queisser limit for single-junction solar... of the coupling between states. More sophisticated spectroscopic approaches are therefore required to build a clear picture of such underlying dynamics. At the same time, there is a growing awareness of the central role of vibronic coupling in a range...

  12. Ultrafast Laser Pulse Control of Exciton Dynamics: A Computational Study on the FMO Ben Bru1ggemann and Volkhard May*

    E-Print Network [OSTI]

    Röder, Beate

    Ultrafast Laser Pulse Control of Exciton Dynamics: A Computational Study on the FMO Complex Ben Bru, D-12489 Berlin, Germany ReceiVed: February 4, 2004; In Final Form: May 23, 2004 Femtosecond laser-pulse on the Frenkel exciton model for the bacteriochlorophyll (BChl) Qy-excitations, the laser- pulse-driven exciton

  13. New Algorithm Enables Fast Simulations of Ultrafast Processes

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

    real-time simulations of ultrafast processes and electron dynamics, such as excitation in photovoltaic materials and ultrafast demagnetization following an optical excitation. "We...

  14. 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

  15. Ultrafast infrared studies of chemical reaction dynamics in room-temperature liquids

    E-Print Network [OSTI]

    Yang, H.

    2011-01-01

    B, 1981, B37, 1052. b For the ethane dicarbonyl complexes inFigure 5.9, the ethane molecule interacts with the metalof the parent molecules, the ethane-solvate, and the final

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

    Office of Scientific and Technical Information (OSTI)

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

  17. Contribution of Fluorophore Dynamics and Solvation to Resonant Energy Transfer in Protein-DNA Complexes: A Molecular-Dynamics Study

    E-Print Network [OSTI]

    Nielsen, Steven O.

    at Dallas, Richardson, Texas; and 5 Department of Physics and Astronomy, University of Leeds, Leeds, UK- phore dynamics for an ATTO donor/acceptor dye pair and specifically consider as case studies dye-labeled

  18. Direct observation of ultrafast many-body electron dynamics in a strongly-correlated ultracold Rydberg gas

    E-Print Network [OSTI]

    Nobuyuki Takei; Christian Sommer; Claudiu Genes; Guido Pupillo; Haruka Goto; Kuniaki Koyasu; Hisashi Chiba; Matthias Weidemüller; Kenji Ohmori

    2015-04-14

    Many-body interactions govern a variety of important quantum phenomena ranging from superconductivity and magnetism in condensed matter to solvent effects in chemistry. Understanding those interactions beyond mean field is a holy grail of modern sciences. AMO physics with advanced laser technologies has recently emerged as a new platform to study quantum many-body systems. One of its latest developments is the study of long-range interactions among ultracold particles to reveal the effects of many-body correlations. Rydberg atoms distinguish themselves by their large dipole moments and tunability of dipolar interactions. Most of ultracold Rydberg experiments have been performed with narrow-band lasers in the Rydberg blockade regime. Here we demonstrate an ultracold Rydberg gas in a complementary regime, where electronic coherence is created using a broadband picosecond laser pulse, thus circumventing the Rydberg blockade to induce strong many-body correlations. The effects of long-range Rydberg interactions have been investigated by time-domain Ramsey interferometry with attosecond precision. This approach allows for the real-time observation of coherent and ultrafast many-body dynamics in which the electronic coherence is modulated by the interaction-induced correlations. The modulation evolves more rapidly than expected for two-body correlations by several orders of magnitude. We have actively controlled such ultrafast many-body dynamics by tuning the principal quantum number and the population of the Rydberg state. The observed Ramsey interferograms are well reproduced by a theoretical model beyond mean-field approximation, which can be relevant to other similar many-body phenomena in condensed matter physics and chemistry. Our new approach opens a new avenue to observe and manipulate nonequilibrium dynamics of strongly-correlated quantum many-body systems on the ultrafast timescale.

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

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design andBiofuelsUltrafast Core-Hole InducedUltrafast|

  20. Use of Ultrafast Dispersed Pump-Dump-Probe and Pump-Repump-Probe Spectroscopies to Explore the Light-Induced Dynamics of Peridinin in Solution

    E-Print Network [OSTI]

    van Stokkum, Ivo

    Use of Ultrafast Dispersed Pump-Dump-Probe and Pump-Repump-Probe Spectroscopies to Explore Form: NoVember 14, 2005 Optical pump-induced dynamics of the highly asymmetric carotenoid peridinin in methanol was studied by dispersed pump-probe, pump-dump-probe, and pump-repump-probe transient absorption

  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. A dynamic and ultrafast group delay tuning mechanism in two microcavities side-coupled with a waveguide system

    SciTech Connect (OSTI)

    Wang, Boyun; Wang, Tao, E-mail: wangtao@hust.edu.cn; Tang, Jian; Li, Xiaoming; Zhu, Youjiang [Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074 (China)

    2014-10-07

    We theoretically propose a dynamic and ultrafast group delay tuning mechanism in two microcavities side-coupled to a waveguide system through external optical pump beams. The optical Kerr effect modulation method is applied to improve tuning rate with response time of subpicoseconds or even femtoseconds. The group delay of an all-optical analog to electromagnetically induced transparency effect can be controlled by tuning either the frequency of photonic crystal microcavities or the propagation phase of line waveguide. Group delay is controlled between 5.88 and 70.98 ps by dynamically tuning resonant frequencies of the microcavities. Alternatively, the group delay is controlled between 1.86 and 12.08 ps by dynamically tuning the propagation phase of line waveguide. All observed schemes are analyzed rigorously through finite-difference time-domain simulations and coupled-mode formalism. Results show a new direction toward microstructure integration optical pulse trapping and all-optical dynamical storage of light devices in optical communication and quantum information processing.

  3. 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 mission. This workshop built on previous workshops and included three breakout sessions identifying scientific challenges in biology, biogeochemistry, catalysis, and materials science frontier areas of fundamental science that underpin energy and environmental science that would significantly benefit from ultrafast transmission electron microscopy (UTEM). In addition, the current status of time-resolved electron microscopy was examined, and the technologies that will enable future advances in spatio-temporal resolution were identified in a fourth breakout session.

  4. Hydrogen bonding and solvation dynamics of n-methylacetamide in denatured water (D?O) or denatured chloroform (CDCl?) from nonlinear spectroscopy

    E-Print Network [OSTI]

    McCracken, Justine M. (Justine Meghan), 1979-

    2004-01-01

    Hydrogen bonding between N-methylacetamide (NMA) and different solvents (D?O or CDCl?) was studied by using two-dimensional infrared spectroscopy to probe the frequency fluctuations of the amide I mode of the solvated NMA. ...

  5. 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

  6. Ultrafast Strong-Field Vibrational Dynamics Studied by Femtosecond Extreme-Ultraviolet Transient Absorption Spectroscopy

    E-Print Network [OSTI]

    Hosler, Erik Robert

    2013-01-01

    dynamics. Tunnel ionization rate determinations are employed to model the pump, while electronic structure calculations

  7. Current Theoretical Challenges in Proton-Coupled Electron Transfer: Electron Proton Nonadiabaticity, Proton Relays, and Ultrafast Dynamics

    SciTech Connect (OSTI)

    Hammes-Schiffer, Sharon

    2011-06-16

    Proton-coupled electron transfer (PCET) reactions play an important role in a wide range of biological and chemical processes. The motions of the electrons, transferring protons, solute nuclei, and solvent nuclei occur on a wide range of time scales and are often strongly coupled. As a result, the theoretical description of these processes requires a combination of quantum and classical methods. This Perspective discusses three of the current theoretical challenges in the field of PCET. The first challenge is the calculation of electron proton nonadiabatic effects, which are significant for these reactions because the hydrogen tunneling is often faster than the electronic transition. The second challenge is the modeling of electron transfer coupled to proton transport along hydrogen-bonded networks. The third challenge is the simulation of the ultrafast dynamics of nonequilibrium photoinduced PCET reactions in solution. Insights provided by theoretical studies may assist in the design of more effective catalysts for energy conversion processes. The proton relay portion of this review is based upon work supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences.

  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. Spatiotemporal dynamics of photoexcited quasiparticles in two-dimensional crystals studied by ultrafast laser techniques

    E-Print Network [OSTI]

    Kumar, Nardeep

    2014-12-31

    dynamics. First, a second harmonic generation technique that can be used to find the crystalline orientation, thickness uniformity, layer stacking, and single-crystal domain size is discussed, with results presented on exfoliated and chemical vapor...

  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. Water-like solvation thermodynamics in a spherically symmetric solvent model

    E-Print Network [OSTI]

    Buldyrev, Sergey

    Water-like solvation thermodynamics in a spherically symmetric solvent model with two. The Jagla fluid has been recently shown to possess water-like structural, dynamic, and thermodynamic and thereby show that the Jagla fluid also displays water-like solvation thermodynamics. We further find low

  12. 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.

  13. Ultrafast scanning tunneling microscopy

    SciTech Connect (OSTI)

    Botkin, D.A. [California Univ., Berkeley, CA (United States). Dept. of Physics]|[Lawrence Berkeley Lab., CA (United States)

    1995-09-01

    I have developed an ultrafast scanning tunneling microscope (USTM) based on uniting stroboscopic methods of ultrafast optics and scanned probe microscopy to obtain nanometer spatial resolution and sub-picosecond temporal resolution. USTM increases the achievable time resolution of a STM by more than 6 orders of magnitude; this should enable exploration of mesoscopic and nanometer size systems on time scales corresponding to the period or decay of fundamental excitations. USTM consists of a photoconductive switch with subpicosecond response time in series with the tip of a STM. An optical pulse from a modelocked laser activates the switch to create a gate for the tunneling current, while a second laser pulse on the sample initiates a dynamic process which affects the tunneling current. By sending a large sequence of identical pulse pairs and measuring the average tunnel current as a function of the relative time delay between the pulses in each pair, one can map the time evolution of the surface process. USTM was used to measure the broadband response of the STM`s atomic size tunnel barrier in frequencies from tens to hundreds of GHz. The USTM signal amplitude decays linearly with the tunnel junction conductance, so the spatial resolution of the time-resolved signal is comparable to that of a conventional STM. Geometrical capacitance of the junction does not appear to play an important role in the measurement, but a capacitive effect intimately related to tunneling contributes to the measured signals and may limit the ultimate resolution of the USTM.

  14. 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.

  15. 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 cation–3HF 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 investigated complexes.

  16. Ultrafast dynamics of interfacial electric fields in semiconductor heterostructures monitored by pump-probe second-harmonic generation

    E-Print Network [OSTI]

    Tolk, Norman H.

    an eletric-field-induced SHG signal. We distinguish between several stages of dynamics originating from

  17. Non-Fourier heat transport in metal-dielectric core-shell nanoparticles under ultrafast laser pulse excitation

    E-Print Network [OSTI]

    Paris-Sud XI, Université de

    1 Non-Fourier heat transport in metal-dielectric core-shell nanoparticles under ultrafast laser and Baluchistan, Zahedan, Iran 10 PACS : Keywords : ballistic heat transfer, core-shell, nanoparticle, ultrafast laser Abstract15 Relaxation dynamics of embedded metal nanoparticles after ultrafast laser pulse

  18. 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.

  19. 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.

  20. Electrolyte Solvation and Ionic Association. VI. Acetonitrile...

    Office of Scientific and Technical Information (OSTI)

    Electrolyte Solvation and Ionic Association. VI. Acetonitrile-Lithium Salt Mixtures: Highly Associated Salts Revisited Citation Details In-Document Search Title: Electrolyte...

  1. 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,...

  2. A Systematic Study of Chloride Ion Solvation in Water using van der Waals Inclusive Hybrid Density Functional Theory

    E-Print Network [OSTI]

    Bankura, Arindam; DiStasio, Robert A; Swartz, Charles W; Klein, Michael L; Wu, Xifan

    2015-01-01

    In this work, the solvation and electronic structure of the aqueous chloride ion solution was investigated using Density Functional Theory (DFT) based \\textit{ab initio} molecular dynamics (AIMD). From an analysis of radial distribution functions, coordination numbers, and solvation structures, we found that exact exchange ($E_{\\rm xx}$) and non-local van der Waals (vdW) interactions effectively \\textit{weaken} the interactions between the Cl$^-$ ion and the first solvation shell. With a Cl-O coordination number in excellent agreement with experiment, we found that most configurations generated with vdW-inclusive hybrid DFT exhibit 6-fold coordinated distorted trigonal prism structures, which is indicative of a significantly disordered first solvation shell. By performing a series of band structure calculations on configurations generated from AIMD simulations with varying DFT potentials, we found that the solvated ion orbital energy levels (unlike the band structure of liquid water) strongly depend on the un...

  3. Exciton Dynamics in CdS-Ag2S Nanorods with Tunable Composition Probed by Ultrafast Transient Absorption Spectroscopy

    E-Print Network [OSTI]

    Cohen, Ronald C.

    electron microscopy (TEM) and X-ray diffraction (XRD) show that the crystals retain their size and shape, 2010 Electron relaxation dynamics in CdS-Ag2S nanorods have been measured as a function of the relative corresponding to fast relaxation of the excited electrons into trap states. This signal completely disappears

  4. Supporting Information for: Single-Ion Solvation Free Energies and the

    E-Print Network [OSTI]

    Truhlar, Donald G

    1 Supporting Information for: Single-Ion Solvation Free Energies and the Normal Hydrogen Electrode Absolute Solvation Free Energies......................................................... 3 Conventional Solvation Free Energies....................................................4 Standard Reduction Potentials

  5. 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.

  6. Lithium Ion Solvation: Amine and Unsaturated Hydrocarbon Solvates of Lithium Hexamethyldisilazide (LiHMDS)

    E-Print Network [OSTI]

    Collum, David B.

    Lithium Ion Solvation: Amine and Unsaturated Hydrocarbon Solvates of Lithium Hexamethyldisilazide, and 13C NMR spectroscopic studies of 6Li-15N labeled lithium hexamethyldisilazide ([6Li,15N]- Li ligand structure and lithium amide aggregation state is a complex and sensitive function of amine alkyl

  7. Influence of solvation on the structural and capacitive properties of electrical double layer capacitors

    E-Print Network [OSTI]

    Paris-Sud XI, Université de

    . The electrolytes, represented by coarse-grained models, are enclosed between graphite electrodes. We employ capacitance, solvation, molecular dynamics simulations, interfacial structure, graphite 2 hal-00853396,version batteries. They can be used as high-power generators and can undergo one million charge/discharge cycles

  8. Quantum Chemistry for Solvated Molecules on Graphical Processing Units (GPUs)using Polarizable Continuum Models

    E-Print Network [OSTI]

    Liu, Fang; Kulik, Heather J; Martínez, Todd J

    2015-01-01

    The conductor-like polarization model (C-PCM) with switching/Gaussian smooth discretization is a widely used implicit solvation model in chemical simulations. However, its application in quantum mechanical calculations of large-scale biomolecular systems can be limited by computational expense of both the gas phase electronic structure and the solvation interaction. We have previously used graphical processing units (GPUs) to accelerate the first of these steps. Here, we extend the use of GPUs to accelerate electronic structure calculations including C-PCM solvation. Implementation on the GPU leads to significant acceleration of the generation of the required integrals for C-PCM. We further propose two strategies to improve the solution of the required linear equations: a dynamic convergence threshold and a randomized block-Jacobi preconditioner. These strategies are not specific to GPUs and are expected to be beneficial for both CPU and GPU implementations. We benchmark the performance of the new implementat...

  9. Photo-Induced Spin-State Conversion in Solvated Transition Metal Complexes Probed via Time-Resolved Soft X-ray Spectroscopy

    E-Print Network [OSTI]

    Huse, Nils

    2010-01-01

    Photo-Induced Spin-State Conversion in Solvated TransitionAbstract: Solution-phase photo-induced low-spin to high-spinquestions concerning photo-induced dynamics difficult to

  10. Ultrafast Transformations in Superionic Nanocrystals

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design andBiofuelsUltrafastUltrafastUltrafastUltrafast

  11. Ultrafast supercontinuum fiber-laser based pump-probe scanning magneto-optical Kerr effect microscope for the investigation of electron spin dynamics in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution

    SciTech Connect (OSTI)

    Henn, T.; Kiessling, T., E-mail: tobias.kiessling@physik.uni-wuerzburg.de; Ossau, W.; Molenkamp, L. W. [Physikalisches Institut (EP3), Universität Würzburg, 97074 Würzburg (Germany)] [Physikalisches Institut (EP3), Universität Würzburg, 97074 Würzburg (Germany); Biermann, K.; Santos, P. V. [Paul-Drude-Institut für Festkörperelektronik, 10117 Berlin (Germany)] [Paul-Drude-Institut für Festkörperelektronik, 10117 Berlin (Germany)

    2013-12-15

    We describe a two-color pump-probe scanning magneto-optical Kerr effect microscope which we have developed to investigate electron spin phenomena in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution. The key innovation of our microscope is the usage of an ultrafast “white light” supercontinuum fiber-laser source which provides access to the whole visible and near-infrared spectral range. Our Kerr microscope allows for the independent selection of the excitation and detection energy while avoiding the necessity to synchronize the pulse trains of two separate picosecond laser systems. The ability to independently tune the pump and probe wavelength enables the investigation of the influence of excitation energy on the optically induced electron spin dynamics in semiconductors. We demonstrate picosecond real-space imaging of the diffusive expansion of optically excited electron spin packets in a (110) GaAs quantum well sample to illustrate the capabilities of the instrument.

  12. Solvated electron lithium electrode for high energy density battery

    SciTech Connect (OSTI)

    Sammels, A.F.

    1987-08-04

    A solvated electron lithium negative electrode is described containing: containment means holding a solution of lithium dissolved in liquid ammonia to form a solvated electron solution, the solvated electron solution contacting a lithium intercalating membrane and providing lithium to the intercalating membrane during discharge and accepting it from the intercalating membrane during charge.

  13. Direct Observation of Optically Induced Transient Structures in Graphite Using Ultrafast Electron Crystallography

    E-Print Network [OSTI]

    initio density functional calculations, we trace the governing mechanism back to electronic structure changes in the electronic properties, direct de- termination of lattice structural dynamics from opticalDirect Observation of Optically Induced Transient Structures in Graphite Using Ultrafast Electron

  14. Development of ultrafast computed tomography of highly transient fuel sprays

    E-Print Network [OSTI]

    Gruner, Sol M.

    Development of ultrafast computed tomography of highly transient fuel sprays Xin Liu, Jinyuan Liu University, Ithaca, NY, USA 14853 ABSTRACT The detailed analysis of the fuel sprays has been well recognized emissions. However, the structure and dynamics of highly transient fuel sprays have never been visualized

  15. 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...

  16. Femtosecond laser studies of ultrafast intramolecular processes

    SciTech Connect (OSTI)

    Hayden, C. [Sandia National Laboratories, Livermore, CA (United States)

    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.

  17. Ultrafast Transformations in Superionic Nanocrystals

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design andBiofuelsUltrafastUltrafastUltrafast

  18. Ultrafast laser-induced changes in optical properties of semiconductors

    SciTech Connect (OSTI)

    Chirila, C. C.; Lim, Freda C. H.; Gavaza, M. G. [Institute of High Performance Computing, 1 Fusionopolis Way, 16-16 Connexis, 138632 (Singapore)

    2012-04-01

    We study the effect of laser radiation on optical properties of semiconductors of industrial interest. The material is pumped with a laser of chosen central frequency, for which the absorption is maximal, thus inducing electron dynamics, which modifies the optical properties. By using an improved theoretical model, we study ultrafast dynamic changes in the refraction index and reflectivity corresponding to a wide frequency-interval of probing radiation and identify that interval where these optical changes are most significant.

  19. Solvation and Ionic Transport in Polymer Electrolyte Membranes

    SciTech Connect (OSTI)

    Zawodzinski, T.A., Jr.; Paddison, S.J.; Reagor, D.; Pratt, L.R.

    1999-06-03

    We developed a general theoretical framework to study the problem of proton solvation and transport in Nafion{reg_sign} and related materials.

  20. A Systematic Study of Chloride Ion Solvation in Water using van der Waals Inclusive Hybrid Density Functional Theory

    E-Print Network [OSTI]

    Arindam Bankura; Biswajit Santra; Robert A. DiStasio Jr.; Charles W. Swartz; Michael L. Klein; Xifan Wu

    2015-03-25

    In this work, the solvation and electronic structure of the aqueous chloride ion solution was investigated using Density Functional Theory (DFT) based \\textit{ab initio} molecular dynamics (AIMD). From an analysis of radial distribution functions, coordination numbers, and solvation structures, we found that exact exchange ($E_{\\rm xx}$) and non-local van der Waals (vdW) interactions effectively \\textit{weaken} the interactions between the Cl$^-$ ion and the first solvation shell. With a Cl-O coordination number in excellent agreement with experiment, we found that most configurations generated with vdW-inclusive hybrid DFT exhibit 6-fold coordinated distorted trigonal prism structures, which is indicative of a significantly disordered first solvation shell. By performing a series of band structure calculations on configurations generated from AIMD simulations with varying DFT potentials, we found that the solvated ion orbital energy levels (unlike the band structure of liquid water) strongly depend on the underlying molecular structures. In addition, these orbital energy levels were also significantly affected by the DFT functional employed for the electronic structure; as the fraction of $E_{\\rm xx}$ was increased, the gap between the highest occupied molecular orbital of Cl$^-$ and the valence band maximum of liquid water steadily increased towards the experimental value.

  1. 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 O?? depends on the relative Lewis acidity of the solvated Li? ion. The impact of the solvated Li? cation on the O? redoxmore »reaction was also investigated.« less

  2. Lithium Hexamethyldisilazide: A View of Lithium Ion Solvation

    E-Print Network [OSTI]

    Collum, David B.

    Lithium Hexamethyldisilazide: A View of Lithium Ion Solvation through a Glass-Bottom Boat BRETT L and reactivities, we were drawn to lithium hexamethyldisilazide (LiHMDS; (Me3Si)2NLi) by its promi- nence principles of lithium ion coordination chemistry.2 Understanding how solvation influences organolithium

  3. 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.

  4. Ultrafast Transformations in Superionic Nanocrystals

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

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  5. Cells containing solvated electron lithium negative electrodes

    SciTech Connect (OSTI)

    Uribe, F.A.; Semkow, K.W.; Sammells, A.F. (Eltron Research, Incorporated, Aurora, IL (US))

    1989-12-01

    Preliminary work performed on a novel solvated electron lithium negative electrode which may have application in either high energy density secondary or reserve battery systems is discussed. The lithium electrode investigated consisted of lithium initially dissolved in liquid ammonia to give a solvated electron solution. Containment of this liquid negative active material from direct contact with a liquid nonaqueous electrolyte present in the cell positive electrode compartment was addressed via the use of a lithium intercalated electronically conducting ceramic membrane of the general composition Li{sub x}WO{sub 2}(0.1{lt}x{lt} 1.0). Secondary electrochemical cells having the general configuration Li,NH{sub 3}/Li{sub x}WO{sub 2}NAE/TiS{sub 2} using nonaqueous electrolytes (NAE) based upon both propylene carbonate and 2Me-THF. Depending upon initial lithium activity in the negative electrode compartments the cell possessed an initial open-circuit potential (OCP 3.44V). Both cells, which were operated at ambient pressure (low temperature) and ambient temperature (high pressure) showed evidence for electrochemical reversibility.

  6. A coupled RISM/MD or MC simulation methodology for solvation free energies

    E-Print Network [OSTI]

    Truong, Thanh N.

    A coupled RISM/MD or MC simulation methodology for solvation free energies Holly Freedman, Thanh N methods for determination of solvation free energies. We employ the RISM formulation of solvation free-netted chain equations. We apply this approach to determining free energies of solvation for several small

  7. Ultrafast Laser Spectroscopyof Chemical Reactions

    E-Print Network [OSTI]

    Zewail, Ahmed

    Ultrafast Laser Spectroscopyof Chemical Reactions - Joseph L. Kneeand AhmedH. Zewail California of chemical physics is to understand how chemi- cal reactions complete their journey from reactants to prod at the molecular level. The making of new bonds (and the breaking of old ones) in elementary chemical reactions

  8. Ultrafast Laser Diagnostics to Investigate Initiation in Energetic...

    Office of Scientific and Technical Information (OSTI)

    Ultrafast Laser Diagnostics to Investigate Initiation in Energetic Materials. Citation Details In-Document Search Title: Ultrafast Laser Diagnostics to Investigate Initiation in...

  9. 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 Citation Details In-Document Search Title: Surface modified CFx cathode material for ultrafast...

  10. 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...

  11. Ultrafast Surface Plasmonic Switch in Non-Plasmonic Metals

    E-Print Network [OSTI]

    Bévillon, E; Recoules, V; Zhang, H; Li, C; Stoian, R

    2015-01-01

    We demonstrate that ultrafast carrier excitation can drastically affect electronic structures and induce brief surface plasmonic response in non-plasmonic metals, potentially creating a plasmonic switch. Using first-principles molecular dynamics and Kubo-Greenwood formalism for laser-excited tungsten we show that carrier heating mobilizes d electrons into collective inter and intraband transitions leading to a sign flip in the imaginary optical conductivity, activating plasmonic properties for the initial non-plasmonic phase. The drive for the optical evolution can be visualized as an increasingly damped quasi-resonance at visible frequencies for pumping carriers across a chemical potential located in a d-band pseudo-gap with energy-dependent degree of occupation. The subsequent evolution of optical indices for the excited material is confirmed by time-resolved ultrafast ellipsometry. The large optical tunability extends the existence spectral domain of surface plasmons in ranges typically claimed in laser se...

  12. 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.

  13. Problem of Polar Solvation (Born vs Onsager Picture)

    E-Print Network [OSTI]

    Matyushov, Dmitry

    Problem of Polar Solvation (Born vs Onsager Picture) Telluride, July 19, 2004 #12;Born Model (1920 (numerical) Born picture is a part of Onsager (Poisson equation) picture #12;Experiment hst=-solvsolv el hst

  14. 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.

  15. Ultrafast Diagnostics for Electron Beams from Laser Plasma Accelerators

    E-Print Network [OSTI]

    Matlis, N. H.

    2011-01-01

    Ultrafast Diagnostics for Electron Beams from Laser Plasmadiagnostic techniques [2]. While the field of electron beam

  16. 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.

  17. Water at the Surfaces of Aligned Phospholipid Multibilayer Model Membranes Probed with Ultrafast Vibrational

    E-Print Network [OSTI]

    Fayer, Michael D.

    Water at the Surfaces of Aligned Phospholipid Multibilayer Model Membranes Probed with Ultrafast@stanford.edu Abstract: The dynamics of water at the surface of artificial membranes composed of aligned multibilayers pump-probe spectroscopy. The experiments are performed at various hydration levels, x ) 2 - 16 water

  18. Ultrafast Transformations in Superionic Nanocrystals

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

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  19. Ultrafast Transformations in Superionic Nanocrystals

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal designUltrafast Transformations in Superionic

  20. Proton Solvation and Proton Mobility Department of Physical Chemistry and the Fritz Haber Research Center,

    E-Print Network [OSTI]

    Agmon, Noam

    Proton Solvation and Proton Mobility NOAM AGMON Department of Physical Chemistry and the Fritz for proton solvation and proton mobility is analyzed and the results are compared with recent simulations. Three factors con­ tribute to differences in proton solvation energies: hydrogen­bond cleavage, changes

  1. On the validity of dielectric continuum models in application to solvation in molecular solvents

    E-Print Network [OSTI]

    Matyushov, Dmitry

    On the validity of dielectric continuum models in application to solvation in molecular solvents simulations of solvation of a point dipole in dipolar­quadrupolar solvents of varying dipole moment and axial of a monotonic increase of the absolute value of the solvation chemical potential p with the solvent dielectric

  2. Studies on free energy calculations. II. A theoretical approach to molecular solvation

    E-Print Network [OSTI]

    Mezei, Mihaly

    Studies on free energy calculations. II. A theoretical approach to molecular solvation Haluk Resat methods of performing the thermodynamic integration in solvation free energy calculations are also at the particle creation limit in obtaining quantitatively reliable results for the solvation free energies. I

  3. Estimating ProteinLigand Binding Free Energy: Atomic Solvation Parameters for Partition Coefficient and

    E-Print Network [OSTI]

    Luhua, Lai

    Estimating Protein­Ligand Binding Free Energy: Atomic Solvation Parameters for Partition Coefficient and Solvation Free Energy Calculation Jianfeng Pei,1,2 Qi Wang,1,2 Jiaju Zhou,3 and Luhua Lai1 free energy and the correct scoring in docking studies. We have developed a new solvation energy

  4. 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-Ã?Â?Ã?Â?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.

  5. 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.

  6. Ultrafast Spectroscopy of Warm Dense Matter

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

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  7. 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., E-mail: m.johnston@physics.ox.ac.uk [Department of Physics, University of Oxford, Clarendon Laboratory, Parks Road, Oxford OX1 3PU (United Kingdom)

    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.

  8. Ultrafast Optimal Sideband Cooling under Non-Markovian Evolution

    E-Print Network [OSTI]

    Johan F. Triana; Andrés F. Estrada; Leonardo A. Pachon

    2015-08-20

    A sideband cooling strategy that incorporates (i) the dynamics induced by structured (non-Markovian) environments in the target and auxiliary systems and (ii) the optimally-time-modulated interaction between them is developed. For the context of cavity optomechanics, when non-Markovian dynamics are considered in the target system, ground state cooling is reached at much faster rates and at much lower phonon occupation number than previously reported. In constrast to similar current strategies, ground state cooling is reached here for coupling-strength rates that are experimentally accesible for the state-of-the-art implementations. After the ultrafast optimal-ground-state-cooling protocol is accomplished, an additional optimal control strategy is considered to maintain the phonon number as closer as possible to the one obtained in the cooling procedure. Contrary to the conventional expectation, when non-Markovian dynamics are considered in the auxiliary system, the efficiency of the cooling protocol is undermined.

  9. Temperature-dependent solvation modulates the dimensions of disordered proteins

    E-Print Network [OSTI]

    Schuler, Ben

    ­solvent interactions, the collapse allows us to probe the physical interactions governing the dimensions of disorderedTemperature-dependent solvation modulates the dimensions of disordered proteins René Wuttkea, 2014 (received for review July 10, 2013) For disordered proteins, the dimensions of the chain are an im

  10. 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.

  11. 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.

  12. Reorientation and Solvation Dynamics of Bulk and Confined Alcohols

    E-Print Network [OSTI]

    Vartia, Anthony Andrew

    2012-12-31

    of the additional timescales, appear in free energy profiles for reorientation, solvent viscosity must also be considered. Ethanol and a Stockmayer model solute were confined within a roughly cylindrical silica pore to investigate the effect of confinement...

  13. Multibounce light transport analysis using ultrafast imaging for material acquisition

    E-Print Network [OSTI]

    Naik, Nikhil, S.M. Massachusetts Institute of Technology

    2012-01-01

    This thesis introduces a novel framework for analysis of multibounce light transport using time-of-flight imaging for the applications of ultrafast reflectance acquisition and imaging through scattering media. Using ultrafast ...

  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 packing—in the solid-state—to be scrutinized in detail.

  15. 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).

  16. Solvated electron lithium electrode for high energy density battery

    SciTech Connect (OSTI)

    Sammells, A.F.

    1987-05-26

    A rechargeable high energy density lithium-based cell is described comprising: a solvated electron lithium negative electrode comprising a solution of lithium dissolved in liquid ammonia; a lithium ion conducting solid electrolyte contacting the negative electrode; a liquid non-aqueous lithium ion conducting electrolyte comprising a lithium ion conducting supporting electrolyte dissolved in a non-aqueous solvent. The liquid electrolyte contacting the lithium ion conducting solid electrolyte; and a solid lithium intercalation positive electrode contacting the liquid electrolyte.

  17. Atomic Resolution Coherent Diffractive Imaging and Ultrafast Science

    SciTech Connect (OSTI)

    Zuo, Jian-min (University of Illinois) [University of Illinois

    2011-01-12

    A major scientific challenge is determining the 3-D atomic structure of small nanostructures, including single molecules. Coherent diffractive imaging (CDI) is a promising approach. Recent progress has demonstrated coherent diffraction patterns can be recorded from individual nanostructures and phased to reconstruct their structure. However, overcoming the dose limit imposed by radiation damage is a major obstacle toward the full potential of CDI. One approach is to use ultrafast x-ray or electron pulses. In electron diffraction, amplitudes recorded in a diffraction pattern are unperturbed by lens aberrations, defocus, and other microscope resolution-limiting factors. Sub-A signals are available beyond the information limit of direct imaging. Significant contrast improvement is obtained compared to high-resolution electron micrographs. progress has also been made in developing time-resolved electron diffraction and imaging for the study of ultrafast dynamic processes in materials. This talk will cover these crosscutting issues and the convergence of electron and x-ray diffraction techniques toward structure determination of single molecules.

  18. 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...

  19. Ultrafast Laser Facility | Photosynthetic Antenna Research Center

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design andBiofuelsUltrafast Core-HoleUltrafast Laser

  20. Ultrafast Spectroscopy of Warm Dense Matter

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design andBiofuelsUltrafastUltrafast Spectroscopy of

  1. Ultrafast Spectroscopy of Warm Dense Matter

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design andBiofuelsUltrafastUltrafast Spectroscopy

  2. PURDUE UNIVERSITY ULTRAFAST OPTICS & OPTICAL FIBER COMMUNICATIONS LABORATORY Photonic RF Waveform Synthesis,

    E-Print Network [OSTI]

    Purdue University

    PURDUE UNIVERSITY ULTRAFAST OPTICS & OPTICAL FIBER COMMUNICATIONS LABORATORY Photonic RF Waveform, Shijun Xiao Funding from ARO, DARPA, and NSF #12;PURDUE UNIVERSITY ULTRAFAST OPTICS & OPTICAL FIBER performance (spectral engineering, dispersion compensation) #12;PURDUE UNIVERSITY ULTRAFAST OPTICS & OPTICAL

  3. PURDUE UNIVERSITY ULTRAFAST OPTICS & OPTICAL FIBER COMMUNICATIONS LABORATORY Andrew M. Weiner and Ehsan Hamidi

    E-Print Network [OSTI]

    Purdue University

    PURDUE UNIVERSITY ULTRAFAST OPTICS & OPTICAL FIBER COMMUNICATIONS LABORATORY Andrew M. Weiner ULTRAFAST OPTICS & OPTICAL FIBER COMMUNICATIONS LABORATORY Ultrawideband (UWB) Radio-frequency Photonics UWB;PURDUE UNIVERSITY ULTRAFAST OPTICS & OPTICAL FIBER COMMUNICATIONS LABORATORY Femtosecond Pulse Shaping A

  4. 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.

  5. Dispersion Stabilization of Solvated Electrons and Dipole-Bound Anions Maciej Gutowski*,, and Piotr Skurski,|

    E-Print Network [OSTI]

    Simons, Jack

    Dispersion Stabilization of Solvated Electrons and Dipole-Bound Anions Maciej Gutowski*,, and Piotr, 1997; In Final Form: September 9, 1997X It has long been assumed that stability of "solvated electrons" and dipole-bound anions results primarily from the static Coulomb interaction of an excess electron

  6. Electron solvation in methane and ethane Zhihua Liu and Bruce J. Berne

    E-Print Network [OSTI]

    Berne, Bruce J.

    Electron solvation in methane and ethane Zhihua Liu and Bruce J. Berne Department of Chemistry; accepted 27 August 1993) The solvation of excess electrons in fluid methane and ethane is studied by path that the electron is in an extended state throughout the whole fluid density range studied. In ethane, it is found

  7. Dielectric Boundary Force in Molecular Solvation with the PoissonBoltzmann Free Energy: A Shape

    E-Print Network [OSTI]

    Li, Bo

    Dielectric Boundary Force in Molecular Solvation with the Poisson­Boltzmann Free Energy: A Shape boundary force acting on such a boundary is the negative first variation of the elec- trostatic free energy [17,18,35,43,44]. Such a predefined interface is used to compute the solvation free energy as the sum

  8. Computing Relative Free Energies of Solvation Using Single Reference Thermodynamic Integration Augmented

    E-Print Network [OSTI]

    Computing Relative Free Energies of Solvation Using Single Reference Thermodynamic Integration relative transformation free energies in a series of molecules with respect to a single reference state of the SR-TI variant is demonstrated in calculations of relative solvation free energies for a series

  9. Ultrafast Transformations in Superionic Nanocrystals

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

    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,...

  10. 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 resultsmore »clearly show that the morphological changes in the plume with spot size are independent of laser pulse width.« less

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

    Office of Scientific and Technical Information (OSTI)

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

  12. Membrane formation by preferential solvation of ions in mixture of water, 3-methylpyridine, and sodium tetraphenylborate

    SciTech Connect (OSTI)

    Sadakane, Koichiro, E-mail: sadakane@fc.ritsumei.ac.jp [Department of Physics, Ritsumeikan University, Noji-Higashi 1-1-1, Kusatsu 525-8577 (Japan)] [Department of Physics, Ritsumeikan University, Noji-Higashi 1-1-1, Kusatsu 525-8577 (Japan); Nagao, Michihiro [NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899-6102 (United States) [NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899-6102 (United States); Center for Exploration of Energy and Matter, Indiana University, Bloomington, Indiana 47408-1398 (United States); Endo, Hitoshi; Seto, Hideki [KENS and CMRC, Institute of Materials Structure Science, High Energy Accelerator Research Organization, Tsukuba 305-0801 (Japan)] [KENS and CMRC, Institute of Materials Structure Science, High Energy Accelerator Research Organization, Tsukuba 305-0801 (Japan)

    2013-12-21

    The structure and dynamics of a ternary system composed of deuterium oxide (D{sub 2}O), 3-methylpyridine (3MP), and sodium tetraphenylborate (NaBPh{sub 4}) are investigated by means of small-angle neutron scattering (SANS) and neutron spin echo (NSE) techniques. In the SANS experiments, a structural phase transition is confirmed between a disordered-phase and an ordered-lamellar-phase upon variation of the composition and/or temperature of the mixture. The characteristic lengths of the structures is on the sub-micrometer scale. A dispersion relation of the structure is measured through NSE experiments, which shows that the relaxation rate follows a cubic relation with momentum transfer. This implies that the dynamics of the system are determined predominantly by membrane fluctuations. The present results indicate that 3MP-rich domains are microscopically separated from bulk water in the presence of NaBPh{sub 4}, and that the layers behave as membranes. These results are interpreted that preferential solvation of salt in each solvent induces a microphase separation between the solvents, and the periodic structure of 3MP-rich domains is stabilized by the long-range electrostatic interaction arising from Na{sup +} ions in D{sub 2}O-rich domains.

  13. Ultrafast Spectroscopy of Warm Dense Matter

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design andBiofuelsUltrafast

  14. Communication Interlaced Fourier transformation of ultrafast 2D NMR data

    E-Print Network [OSTI]

    Frydman, Lucio

    Communication Interlaced Fourier transformation of ultrafast 2D NMR data Mor Mishkovsky, Lucio in ultrafast 2D NMR is discussed and exemplified, based on the interlaced Fourier transformation. This approach in the achievable digital resolution. These expectations were tested by carrying out a series of homo

  15. 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.

  16. Layering Transitions and Solvation Forces in an Asymmetrically Confined Fluid

    E-Print Network [OSTI]

    Maria C. Stewart; Robert Evans

    2014-08-29

    We consider a simple fluid confined between two parallel walls (substrates), separated by a distance L. The walls exert competing surface fields so that one wall is attractive and may be completely wet by liquid (it is solvophilic) while the other is solvophobic. Such asymmetric confinement is sometimes termed a `Janus Interface'. The second wall is: (i) purely repulsive and therefore completely dry (contact angle 180 degrees) or (ii) weakly attractive and partially dry (the contact angle is typically in the range 160-170 degrees). At low temperatures, but above the bulk triple point, we find using classical density functional theory (DFT) that the fluid is highly structured in the liquid part of the density profile. In case (i) a sequence of layering transitions occurs: as L is increased at fixed chemical potential (mu) close to bulk gas--liquid coexistence, new layers of liquid-like density develop discontinuously. In contrast to confinement between identical walls, the solvation force is repulsive for all wall separations and jumps discontinuously at each layering transition and the excess grand potential exhibits many metastable minima as a function of the adsorption. For a fixed temperature T=0.56Tc, where Tc is the bulk critical temperature, we determine the transition lines in the L, mu plane. In case (ii) we do not find layering transitions and the solvation force oscillates about zero. We discuss how our mean-field DFT results might be altered by including effects of fluctuations and comment on how the phenomenology we have revealed might be relevant for experimental and simulation studies of water confined between hydrophilic and hydrophobic substrates, emphasizing it is important to distinguish between cases (i) and (ii).

  17. Single-shot spectroscopy of solid-state photoinduced dynamics far from equilibrium

    E-Print Network [OSTI]

    Wolfson, Johanna Wendlandt

    2013-01-01

    Ultrafast single-shot spectroscopy was developed and improved as a method to observe photoinduced dynamics far from equilibrium. The method was then employed to illuminate material dynamics in platinum-halide quasi-one-dimensional ...

  18. How trehalose protects DNA in the dry state: a molecular dynamics simulation 

    E-Print Network [OSTI]

    Fu, Xuebing

    2008-10-10

    Molecular dynamics simulations were conducted on a system consisting of a decamer DNA solvated by trehalose and water (molecular ratio= 1:2), to mimic a relatively dry state for the DNA molecule. Simulations were performed ...

  19. Biological Water Dynamics and Entropy: A Biophysical Origin of Cancer and Other Diseases

    E-Print Network [OSTI]

    Davidson, Robert M.

    This paper postulates that water structure is altered by biomolecules as well as by disease-enabling entities such as certain solvated ions, and in turn water dynamics and structure affect the function of biomolecular ...

  20. The SM8 Universal Solvation Model Christopher J. Cramer and Donald G. Truhlar, University of Minnesota

    E-Print Network [OSTI]

    Truhlar, Donald G

    constants, redox potentials, solubilities, temperature-dependent absolute free energies of solvation pollutants, and the thermodynamics of processes taking place in electrochemical fuel cells. q1 q2 q3 q2 q1 q

  1. Solvation of positive ions in water: The dominant role of water-water interaction

    E-Print Network [OSTI]

    Christian Krekeler; Luigi Delle Site

    2007-02-09

    Local polarization effects, induced by mono and divalent positive ions in water, influence (and in turn are influenced by) the large scale structural properties of the solvent. Experiments can only distinguish this process of interplay in a generic qualitative way. Instead, first principles quantum calculations can address the question at both electronic and atomistic scale, accounting for electronic polarization as well as geometrical conformations. For this reason we study the extension of the scales' interconnection by means of first principle Car-Parrinello molecular dynamics applied to systems of different size. In this way we identify the general aspects dominating the physics of the first solvation shell and their connection to the effects related to the formation of the outer shells and eventually the bulk. We show that while the influence of the ions is extended to the first shell only, the water-water interaction is instead playing a dominant role even within the first shell independently from the size or the charge of the ion.

  2. Fast Computation of Solvation Free Energies with Molecular Density Functional Theory: Thermodynamic-Ensemble Partial Molar Volume Corrections

    E-Print Network [OSTI]

    Volodymyr P. Sergiievskyi; Guillaume Jeanmairet; Maximilien Levesque; Daniel Borgis

    2014-06-11

    Molecular Density Functional Theory (MDFT) offers an efficient implicit- solvent method to estimate molecule solvation free-energies whereas conserving a fully molecular representation of the solvent. Even within a second order ap- proximation for the free-energy functional, the so-called homogeneous reference uid approximation, we show that the hydration free-energies computed for a dataset of 500 organic compounds are of similar quality as those obtained from molecular dynamics free-energy perturbation simulations, with a computer cost reduced by two to three orders of magnitude. This requires to introduce the proper partial volume correction to transform the results from the grand canoni- cal to the isobaric-isotherm ensemble that is pertinent to experiments. We show that this correction can be extended to 3D-RISM calculations, giving a sound theoretical justifcation to empirical partial molar volume corrections that have been proposed recently.

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

    SciTech Connect (OSTI)

    Thyrrestrup, Henri Yüce, Emre; Ctistis, Georgios; Vos, Willem L.; Claudon, Julien; Gérard, 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.

  4. 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.

  5. 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 (5–40 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.

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

    DOE Patents [OSTI]

    Smirl, Arthur (1020 Cherry La. Northwest, Iowa City, IA 52240); Trebino, Rick P. (425 Mulqueeny St., Livermore, CA 94550)

    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.

  7. Ultrafast pump-probe force microscopy with nanoscale resolution

    E-Print Network [OSTI]

    2015-01-01

    Cerullo, “Confocal ultrafast pump-probe spectroscopy: A newand H. J. Maris, “Time-resolved pump-probe experiments withand U. Keller, “Femtosecond pump-porbe near-field optical

  8. A Source for Ultrafast Continuum Infrared and Terahertz Radiation

    E-Print Network [OSTI]

    Petersen, Poul B.

    A compact and stable method for generating high-intensity linearly polarized continuum mid-IR and terahertz light using ultrafast femtosecond (fs) laser pulses is demonstrated. Continuous light generation from <400cm?1 ...

  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. Ion distribution around a charged rod in one and two component solvents: Preferential solvation and first order ionization phase transition

    E-Print Network [OSTI]

    Ion distribution around a charged rod in one and two component solvents: Preferential solvation 2009; publisher error corrected 8 September 2009 In one and two component polar solvents, we calculate solvation of the charged particles and the short-range interaction between the rod and the solvent

  11. Solvation Free Energy of Biomacromolecules: Parameters for a Modified Generalized Born Model Consistent with the AMBER Force Field

    E-Print Network [OSTI]

    Jayaram, Bhyravabotla

    Solvation Free Energy of Biomacromolecules: Parameters for a Modified Generalized Born Model provides rapid estimates of the electrostatic free energies of solvation for diverse molecules of parameters compatible with the AMBER force field is described. The method is used to estimate free energies

  12. Ultrafast Optics and Optical Fiber Communications Laboratory http://purcell.ecn.purdue.edu/~fsoptics/

    E-Print Network [OSTI]

    Purdue University

    Ultrafast Optics and Optical Fiber Communications Laboratory http, A. M. Weiner Purdue University C. Lin Avanex Corporation Conference on Lasers and Electro Optics;Ultrafast Optics and Optical Fiber Communications Laboratory http://purcell.ecn.purdue.edu/~fsoptics/ 2

  13. Ultrafast optical pulse manipulation in three dimensional-resolved microscope imaging and microfabrication

    E-Print Network [OSTI]

    Kim, Daekeun, Ph. D. Massachusetts Institute of Technology

    2009-01-01

    The availability of lasers with femtosecond, ultrafast light pulses provides new opportunities and challenges in instrument design. This thesis addresses three aspects of utilizing ultrafast light pulses in two-photon ...

  14. Solvation of the Fluorine Containing Anions and Their Lithium Salts in Propylene Carbonate and Dimethoxyethane

    E-Print Network [OSTI]

    Chaban, Vitaly

    2015-01-01

    Electrolyte solutions based on the propylene carbonate (PC)-dimethoxyethane (DME) mixtures are of significant importance and urgency due to emergence of lithium-ion batteries. Solvation and coordination of the lithium cation in these systems have been recently attended in detail. However, analogous information concerning anions (tetrafluoroborate, hexafluorophosphate) is still missed. This work reports PM7-MD simulations (electronic-structure level of description) to include finite-temperature effects on the anion solvation regularities in the PC-DME mixture. The reported result evidences that the anions appear weakly solvated. This observation is linked to the absence of suitable coordination sites in the solvent molecules. In the concentrated electrolyte solutions, both BF4 and PF6 prefer to exist as neutral ion pairs (LiBF4, LiPF6).

  15. 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.

  16. Fourier information optics for the ultrafast time domain Andrew M. Weiner

    E-Print Network [OSTI]

    Purdue University

    Fourier information optics for the ultrafast time domain Andrew M. Weiner School of Electrical); published 26 November 2007 Ultrafast photonic signal processing based on Fourier optics principles offers of ultrafast optical signals via conversion between time, space, and optical frequency (Fourier) domains

  17. Ultrafast energy transfer from rigid, branched side-chains into a conjugated, alternating copolymer

    SciTech Connect (OSTI)

    Griffin, Graham B.; Rolczynski, Brian S.; Linkin, Alexander; McGillicuddy, Ryan D.; Engel, Gregory S., E-mail: gsengel@uchicago.edu [Department of Chemistry, The James Franck Institute, Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637 (United States); Lundin, Pamela M. [Department of Chemical Engineering, Stanford University, Stauffer III, 381 North-South Mall, Stanford, California 94305 (United States) [Department of Chemical Engineering, Stanford University, Stauffer III, 381 North-South Mall, Stanford, California 94305 (United States); A. R. Smith Department of Chemistry, Appalachian State University, 417 CAP Building, 525 Rivers Street, Boone, North Carolina 28608 (United States); Bao, Zhenan [Department of Chemical Engineering, Stanford University, Stauffer III, 381 North-South Mall, Stanford, California 94305 (United States)] [Department of Chemical Engineering, Stanford University, Stauffer III, 381 North-South Mall, Stanford, California 94305 (United States)

    2014-01-21

    We present the synthesis and characterization of a benzodithiophene/thiophene alternating copolymer decorated with rigid, singly branched pendant side chains. We characterize exciton migration and recombination dynamics in these molecules in tetrahydrofuran solution, using a combination of static and time-resolved spectroscopies. As control experiments, we also measure electronic relaxation dynamics in isolated molecular analogues of both the side chain and polymer moieties. We employ semi-empirical and time-dependent density functional theory calculations to show that photoexcitation of the decorated copolymer using 395 nm laser pulses results in excited states primarily localized on the pendant side chains. We use ultrafast transient absorption spectroscopy to show that excitations are transferred to the polymer backbone faster than the instrumental response function, ?250 fs.

  18. Water in the Half Shell: Structure of Water, Focusing on Angular Structure and Solvation

    E-Print Network [OSTI]

    Sharp, Kim

    Water in the Half Shell: Structure of Water, Focusing on Angular Structure and Solvation KIM A 14, 2009 C O N S P E C T U S Water is a highly polar molecule, consisting of a very electronegative. These features give water remarkable physical prop- erties, some of which are anomalous, such as its lower

  19. Lithium Phenolates Solvated by Tetrahydrofuran and 1,2-Dimethoxyethane: Structure Determination Using the

    E-Print Network [OSTI]

    Collum, David B.

    Lithium Phenolates Solvated by Tetrahydrofuran and 1,2-Dimethoxyethane: Structure Determination: The method of continuous variation in conjunction with 6 Li NMR spectroscopy was used to characterize lithium substrate- and solvent-dependent combinations of lithium phenolate monomers, dimers, trimers, tetramers

  20. Lithium Diisopropylamide Solvated by Monodentate and Bidentate Ligands: Solution Structures and Ligand Binding

    E-Print Network [OSTI]

    Collum, David B.

    Lithium Diisopropylamide Solvated by Monodentate and Bidentate Ligands: Solution Structures, 1997X Abstract: 6Li and 15N NMR spectroscopic studies of lithium diisopropylamide ([6Li]LDA and [6Li,15 are correlated with those obtained previously for lithium hexamethyldisilazide. Introduction Despite

  1. Fast Analytical Continuum Treatments of Solvation Franois Marchand and Amedeo Caflisch

    E-Print Network [OSTI]

    Caflisch, Amedeo

    in the simulation system, at the price of high computational cost. In fact, the solvent molecules greatly increase]. Furthermore, such a model directly yields the so-called effective energy, which is the sum of the solute potential energy in vacuo and the solvation free energy. In contrast, explicit water simulations have

  2. Ultrafast Core-Hole Induced Dynamics in Water

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

    The situation gets further complicated when you add ionizing x-ray radiation to the mix: the energy from the radiation is enough to eject an electron from the core of the...

  3. Ultrafast Core-Hole Induced Dynamics in Water

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

    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...

  4. Ultrafast Core-Hole Induced Dynamics in Water

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity ofkandz-cm11 Outreach Home RoomPreservationBio-Inspired SolarAbout /Two0 - 19 Publications 1.Design » Design for Efficiency

  5. Ultrafast Core-Hole Induced Dynamics in Water

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity ofkandz-cm11 Outreach Home RoomPreservationBio-Inspired SolarAbout /Two0 - 19 Publications 1.Design » Design for

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

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfateSciTechtail.Theory of rare Kaon and(Conference) |Article) |Fe(phen)

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

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfateSciTechtail.Theory of rare Kaon and(Conference) |Article) |Fe(phen)free-electron laser (Journal

  8. Ultrafast Core-Hole Induced Dynamics in Water

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design andBiofuels

  9. 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 reactivity by Na+ cations. Monomolecular isobutane cracking and dehydrogenation rate constants (per H+; 763 K), however, were higher on H-USY than CD-HUSY (by a factor of 1.4). Equilibrium constants for the formation of protonated methanol dimers via adsorption of gaseous methanol onto adsorbed methanol monomers, determined from kinetic studies of methanol dehydration to dimethyl ether (433 K), were also higher on H-USY than CD-HUSY (by a factor of 2.1). These larger constants predominantly reflect stronger dispersive interactions in H-USY, consistent with its smaller supercage voids that result from the occlusion of void space by extraframework Al (Alex) residues. These findings appear to clarify enduring controversies about the mechanistic interpretation of the effects of Na+ and Alex species on the catalytic reactivity of FAU zeolites. They also illustrate the need to normalize rates by the number of active sites instead of more convenient but less accurate structural proxies for such sites.

  10. PURDUE UNIVERSITY ULTRAFAST OPTICS & OPTICAL FIBER COMMUNICATIONS LABORATORYA.M. Weiner Andrew M. Weiner, Jason McKinney*, and Shijun Xiao

    E-Print Network [OSTI]

    Purdue University

    PURDUE UNIVERSITY ULTRAFAST OPTICS & OPTICAL FIBER COMMUNICATIONS LABORATORYA.M. Weiner Andrew M affiliation: Naval Research Labs #12;PURDUE UNIVERSITY ULTRAFAST OPTICS & OPTICAL FIBER COMMUNICATIONS bandwidth #12;PURDUE UNIVERSITY ULTRAFAST OPTICS & OPTICAL FIBER COMMUNICATIONS LABORATORYA.M. Weiner

  11. 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.

  12. Ultrafast Diagnostics for Electron Beams from Laser Plasma Accelerators

    E-Print Network [OSTI]

    Geddes, Cameron Guy Robinson

    Ultrafast Diagnostics for Electron Beams from Laser Plasma Accelerators N. H. Matlis, M. Bakeman, C key parameters of electron bunches from Laser Plasma Accelerators (LPAs). The diagnostics presented the ability to fine-tune and stabilize the electron beam parameters, however, is the ability to measure them

  13. 5D Data Storage by Ultrafast Laser Nanostructuring in Glass

    E-Print Network [OSTI]

    Anderson, Jim

    5D Data Storage by Ultrafast Laser Nanostructuring in Glass Jingyu Zhang* , Mindaugas Gecevicius-assembled form birefringence and retrieved in glass opening the era of unlimited lifetime data storage. © 2013 laser writing in glass were proposed for the polarization multiplexed optical memory, where

  14. ULTRAFAST RADIATION HEAT TRANSFER IN LASER TISSUE WELDING AND SOLDERING

    E-Print Network [OSTI]

    Guo, Zhixiong "James"

    , respectively. 1. INTRODUCTION The study of short-pulsed laser radiation transport and ultrafast matter­ radiation interactions is of great scientific and technological significance and is attracting increasing­9], to name a few. Due to the very short time duration of the radia- tion­matter interaction and transport

  15. Ultrafast gated intensifier design for laser fusion x-ray framing applications

    SciTech Connect (OSTI)

    Price, R.H.; Wiedwald, J.D.; Kalibjian, R.; Thomas, S.W.; Cook, W.M.

    1983-11-01

    A major challenge for laser fusion is the study of the symmetry and the hydrodynamic stability of imploding fuel capsules. Streaked x-radiography, in one space and one time dimension, does not provide sufficient information. Two (spatial) dimensional frames of 10 to 100 ps duration are required with good image quality, minimum geometrical distortion (approximately 1%), dynamic range greater than 1000 and greater than 200 x 200 pixels. A gated transmission line imager (TLI) can meet these requirements with frame times between 30 and 100 ps. An instrument of this type is now being developed. Progress on this instrument including theory of operation, ultrafast pulse generation and propagation, component integration, and high resolution phosphor screen development are presented.

  16. Light-control of the ultrafast demagnetization pathway in an antiferromagnetic insulator

    E-Print Network [OSTI]

    Sala, Vera G; Miller, Timothy A; Viola, Daniele; Luppi, Elenora; Véniard, Valérie; Cerullo, Giulio; Wall, Simon

    2015-01-01

    Ultrafast demagnetization is a complex process involving strong coupling between electronic, spin, and structural degrees of freedom which is dependent on the type of magnetic order and band structure. Controlling these interactions is key for developing magnetic devices that can fully exploit femto-magnetism. Here we show that energy and polarization tunable femtosecond light pulses can be used to control the demagnetization pathway in the antiferromagnetic insulator Cr2O3. We visualize how the demagnetization dynamics depends on the pump photon energy using transient second harmonic spectroscopy. This enables us to monitor changes to the magnetic and crystalline symmetry, revealing the key role played by phonons in the demagnetization process. The phonon symmetry can be selected through the colour and polarization of the pump pulse, providing control over the demagnetization process, which could lead to faster and more efficient control of magnetic order.

  17. 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 femtosecond detection speed. The femtosecond cooperative magnetic phenomena presented here further our understanding of Mn-hole correlations in III-V dilute magnetic semiconductors, and may well represent universal principles of a large class of carrier-mediated ferromagnetic materials. Thus they offer perspectives for future terahertz (1012 Hz) speed"spintronic" functional devices.

  18. C60,Bromobenzene Solvate: Crystallographic and Thermochemical Studies and Their Relationship to C60 Solubility in Bromobenzene

    E-Print Network [OSTI]

    C60,Bromobenzene Solvate: Crystallographic and Thermochemical Studies and Their Relationship to C60 observed with fractional populations of 0.71 and 0.29. The enthalpy of solution of pure C60 in bromobenzene was determined to be solH[C60(s)] ) -11.5 ( 2.0 kJ/mol. The enthalpy of solution of the solvated crystal was sol

  19. Theoretical oxidation state analysis of Ru-(bpy){sub 3}: Influence of water solvation and Hubbard correction in first-principles calculations

    SciTech Connect (OSTI)

    Reeves, Kyle G. [Department of Chemistry, University of North Carolina at Chapel Hill, North Carolina 27599-3290 (United States); Kanai, Yosuke, E-mail: ykanai@unc.edu [Department of Chemistry, University of North Carolina at Chapel Hill, North Carolina 27599-3290 (United States); Condensed Matter and Materials Division, Lawrence Livermore National Laboratory, California, 94550 (United States)

    2014-07-14

    Oxidation state is a powerful concept that is widely used in chemistry and materials physics, although the concept itself is arguably ill-defined quantum mechanically. In this work, we present impartial comparison of four, well-recognized theoretical approaches based on Lowdin atomic orbital projection, Bader decomposition, maximally localized Wannier function, and occupation matrix diagonalization, for assessing how well transition metal oxidation states can be characterized. Here, we study a representative molecular complex, tris(bipyridine)ruthenium. We also consider the influence of water solvation through first-principles molecular dynamics as well as the improved electronic structure description for strongly correlated d-electrons by including Hubbard correction in density functional theory calculations.

  20. ULTRACAM - an ultra-fast, triple-beam CCD camera

    E-Print Network [OSTI]

    Vik Dhillon; Tom Marsh; the ULTRACAM team

    2001-10-01

    ULTRACAM is an ultra-fast, triple-beam CCD camera which has been designed to study one of the few remaining unexplored regions of observational parameter space - high temporal resolution. The camera will see first light in Spring 2002, at a total cost of GBP 300 k, and will be used on 2-m, 4-m and 8-m class telescopes to study astrophysics on the fastest timescales.

  1. Ultrafast all-optical manipulation of interfacial magnetoelectric coupling

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal designUltrafast Transformations in

  2. Ultrafast Photo-Induced Charge Transfer Unveiled by Two-Dimensional Electronic Spectroscopy

    E-Print Network [OSTI]

    Bixner, Oliver; Mancal, Tomas; Hauer, Juergen; Milota, Franz; Fischer, Michael; Pugliesi, Igor; Bradler, Maximilian; Schmid, Walther; Riedle, Eberhard; Kauffmann, Harald F; Christensson, Niklas

    2012-01-01

    The interaction of exciton and charge transfer (CT) states plays a central role in photo-induced CT processes in chemistry, biology and physics. In this work, we use a combination of two-dimensional electronic spectroscopy (2D-ES), pump-probe measurements and quantum chemistry to investigate the ultrafast CT dynamics in a lutetium bisphthalocyanine dimer in different oxidation states. It is found that in the anionic form, the combination of strong CT-exciton interaction and electronic asymmetry induced by a counter-ion enables CT between the two macrocycles of the complex on a 30 fs timescale. Following optical excitation, a chain of electron and hole transfer steps gives rise to characteristic cross-peak dynamics in the electronic 2D spectra, and we monitor how the excited state charge density ultimately localizes on the macrocycle closest to the counter-ion within 100 fs. A comparison with the dynamics in the radical species further elucidates how CT states modulate the electronic structure and tune fs-reac...

  3. Ultrafast laser ablation ICP-MS: role of spot size, laser fluence, and repetition rate in signal intensity

    E-Print Network [OSTI]

    Harilal, S. S.

    Ultrafast laser ablation ICP-MS: role of spot size, laser fluence, and repetition rate in signal,a Richard E. Russob and Ahmed Hassaneina Ultrafast laser ablation inductively coupled plasma mass system. Though ultrafast laser ablation sample introduction provides better accuracy and precision

  4. Water dynamics in large and small reverse micelles: From two ensembles to collective behavior

    E-Print Network [OSTI]

    Fayer, Michael D.

    Water dynamics in large and small reverse micelles: From two ensembles to collective behavior David July 2009 The dynamics of water in Aerosol-OT reverse micelles are investigated with ultrafast infrared spectroscopy of the hydroxyl stretch. In large reverse micelles, the dynamics of water are separable into two

  5. Report on Ngai et al.: Change of Caged Dynamics at Tg in hydrated proteins found after suppressing the methyl group rotation contribution"

    E-Print Network [OSTI]

    Doster, Wolfgang

    neutron scattering data of solvated proteins, the solvent is now restricted to hydration water: The authors belong to the elastic neutron scattering community, which intends to explain protein dynamics of dynamic information. The full dynamic information derivable from neutron scattering experiments

  6. Molecular Dynamics Simulation of Nafion Oligomer Solvation in Equimolar Methanol-Water Mixture

    E-Print Network [OSTI]

    Muzzio, Fernando J.

    chains determines the unique sieving properties of the ionomer membranes. When exposed to water or other and diffusivity of methane and carbon dioxide in Nafion membranes and demonstrated its applicability to gas in the bulk. 1. Introduction Solid ionomer membranes are widely used in liquid and gas separations,1,2 water

  7. 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 strength. Additionally, the H-bond interactions between protolyzable surface oxygen groups and water were found to be stronger than those between bulk water molecules at all temperatures investigated in our CMD simulations (25, 150 and 250 C). Comparison with the protonation scheme previously determined for the (110) surface of isostructural cassiterite ({alpha}-SnO{sub 2}) reveals that the greater extent of H-bonding on the latter surface, and in particular between water and the terminal hydroxyl group (Sn-OH) results in the predicted protonation constant for that group being lower than for the bridged oxygen (Sn-O-Sn), while the reverse is true for the rutile (110) surface. These results demonstrate the importance of H-bond structure in dictating surface protonation behavior, and that explicit use of this solvation structure within the refined MUSIC model framework results in predicted surface protonation constants that are also consistent with a variety of other experimental and computational data.

  8. RADIATION HEAT TRANSFER IN TISSUE WELDING AND SOLDERING WITH ULTRAFAST LASERS

    E-Print Network [OSTI]

    Guo, Zhixiong "James"

    RADIATION HEAT TRANSFER IN TISSUE WELDING AND SOLDERING WITH ULTRAFAST LASERS Kyunghan Kim to incorporate transient radiation heat transfer in tissue welding and soldering with use of ultrafast lasers are performed between laser welding and laser soldering. The use of solder is found to substantially enhance

  9. A pulsed electron gun for ultrafast electron diffraction at surfaces A. Janzen,a

    E-Print Network [OSTI]

    von der Linde, D.

    A pulsed electron gun for ultrafast electron diffraction at surfaces A. Janzen,a B. Krenzer, O The construction of a pulsed electron gun for ultrafast reflection high-energy electron diffraction experiments describe the construction of an elec- tron gun used in RHEED experiments at crystal surfaces

  10. Hydrogen Bond Migration between Molecular Sites Observed with Ultrafast 2D IR Chemical Exchange Spectroscopy

    E-Print Network [OSTI]

    Fayer, Michael D.

    Hydrogen Bond Migration between Molecular Sites Observed with Ultrafast 2D IR Chemical ExchangeVed: January 12, 2010 Hydrogen-bonded complexes between phenol and phenylacetylene are studied using ultrafast hydrogen bonding acceptor sites (phenyl or acetylene) that compete for hydrogen bond donors in solution

  11. J. Phys. Chem. 1994, 98, 5113-5111 5773 Free Energy of Solvation, Interaction, and Binding of Arbitrary Charge Distributions Imbedded in

    E-Print Network [OSTI]

    Jayaram, Bhyravabotla

    J. Phys. Chem. 1994, 98, 5113-5111 5773 Free Energy of Solvation, Interaction, and Binding in a continuum solvent. Background Attempts seeking analytical solutions to the hydration free energies solvation free energies of arbitrary charge distributions with an overall spherical symmetry. This theory

  12. Calculation of Solvation Free Energies of Charged Solutes Using Mixed Cluster/Continuum Vyacheslav S. Bryantsev, Mamadou S. Diallo,, and William A. Goddard III*,

    E-Print Network [OSTI]

    Goddard III, William A.

    Calculation of Solvation Free Energies of Charged Solutes Using Mixed Cluster/Continuum Models methodologies make systematic errors in the computed free energies because of the incorrect accounting consideration. We analyze two different thermodynamic cycles for calculating the solvation free energies

  13. Ultrafast laser control of backward superfluorescence towards standoff sensing

    SciTech Connect (OSTI)

    Ariunbold, Gombojav O. [Texas A and M University, College Station, Texas 77843 (United States); National University of Mongolia, Ulaanbaatar 210646 (Mongolia); Baylor University, Waco, Texas 76798 (United States); Sautenkov, Vladimir A. [Texas A and M University, College Station, Texas 77843 (United States); Joint Institute for High Temperatures, Russian Academy of Sciences, Moscow 125412 (Russian Federation); P. N. Lebedev Physical Institute, Russian Academy of Sciences, Moscow 119991 (Russian Federation); Rostovtsev, Yuri V. [University of North Texas, Denton, Texas 76203 (United States); Scully, Marlan O. [Texas A and M University, College Station, Texas 77843 (United States); Baylor University, Waco, Texas 76798 (United States); Princeton University, Princeton, New Jersey 08544 (United States)

    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)

  14. 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.

  15. Ultrafast Shock Initiation of Exothermic Chemistry in Hydrogen Peroxide

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfateSciTechtail.Theory of rare Kaon and(Conference) |Article) |Fe(phen) 2 (NCS) 2Ultrafast Probes

  16. Ultrafast Shock Initiation of Exothermic Chemistry in Hydrogen Peroxide

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfateSciTechtail.Theory of rare Kaon and(Conference) |Article) |Fe(phen) 2 (NCS) 2Ultrafast

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

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design andBiofuelsUltrafast Core-Hole

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

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal designUltrafast Transformations inmixture of

  19. Acid strength and solvation effects on methylation, hydride transfer, and isomerization rates during catalytic homologation of C1 species

    E-Print Network [OSTI]

    Iglesia, Enrique

    Acid strength and solvation effects on methylation, hydride transfer, and isomerization rates,b, a Department of Chemical and Biomolecular Engineering, University of California at Berkeley, USA b Division, FAU, MFI) via methylation and hydride transfer steps that favor isobutane and triptane formation

  20. Efficient Monte Carlo sampling for long molecular chains using local moves, tested on a solvated lipid bilayer

    E-Print Network [OSTI]

    Mezei, Mihaly

    An improved acceptance criterion for local move Monte Carlo method in which trial steps change only sevenEfficient Monte Carlo sampling for long molecular chains using local moves, tested on a solvated, New York University, New York, New York 10029 Received 20 February 2002; accepted 27 November 2002

  1. Temperature and Length Scale Dependence of Solvophobic Solvation in a Single-site Water-like Liquid

    E-Print Network [OSTI]

    John R. Dowdle; Sergey V. Buldyrev; H. Eugene Stanley; Pablo G. Debenedetti; Peter J. Rossky

    2012-11-01

    The temperature and length scale dependence of solvation properties of spherical hard solvophobic solutes is investigated in the Jagla liquid, a simple liquid that consists of particles interacting via a spherically symmetric potential combining a hard core repulsion and a longer ranged soft core interaction, yet exhibits water-like anomalies. The results are compared with equivalent calculations for a model of a typical atomic liquid, the Lennard-Jones (LJ) potential, and with predictions for hydrophobic solvation in water using the cavity equation of state and the extended simple point charge (SPC/E) model. We find that the Jagla liquid captures the qualitative thermodynamic behavior of hydrophobic hydration as a function of temperature for both small and large length scale solutes. In particular, for both the Jagla liquid and water, we observe temperature-dependent enthalpy and entropy of solvation for all solute sizes as well as a negative solvation entropy for sufficiently small solutes at low temperature. The results suggest that, compared to a simple liquid, it is the presence of a second thermally accessible repulsive energy scale, acting to increasingly favor larger separations for decreasing temperature, that is the essential characteristic of a liquid that favors low-density, open structures and models hydrophobic hydration, and that it is the presence of this second energy scale that leads to the similarity in the behavior of water and the Jagla liquid. The implications of the temperature and length scale dependence of solvation free energies in water-like liquids are explored with a simple model for the aggregation of solvophobic solutes. We show how aggregate stability depends upon the size of the aggregate and the size of its constituent solutes, and we relate this dependence to cold-induced destabilization phenomena such as the cold-induced denaturation of proteins.

  2. Time-resolved spectroscopy of CI and CII line emissions from an ultrafast laser induced solid graphite plasma

    SciTech Connect (OSTI)

    N, Smijesh, E-mail: smiju5247@gmail.com [Lasers and Nonlinear optics lab, Department of Physics, National Institute of Technology Calicut, Kozhikode - 673 601 India and Raman Research Institute, Sadashivanagar, Bangalore 560080 (India); K, Chandrasekharan, E-mail: csk@nitc.ac.in [Lasers and Nonlinear optics lab, Department of Physics, National Institute of Technology Calicut, Kozhikode - 673 601 (India); Philip, Reji, E-mail: reij@rri.res.in [Raman Research Institute, Sadashivanagar, Bangalore 560080 (India)

    2014-10-15

    We present an experimental characterization of the evolution dynamics of CI and CII lines in an ultrafast laser produced graphite plasma under various ambient conditions. Fast and slow components are observed in the temporal evolution of CI transition at 658.7 nm (3p{sup 1}P - 4d{sup 1}P{sup 0}) and CII transition at 426.7 nm (3d {sup 2}D - 4f {sup 2}F{sup 0}). Fast peak is due to the recombination of fast ions species with electrons, found to have an increase in velocity upon increasing the ambient pressure. Whereas the slow peaks in both cases can be the results of slow ions or slow neutrals in the plume.

  3. 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.

  4. 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.

  5. 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 m 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

  6. Solvation studies on anion radicals of alkyl nitrobenzene derivatives in acetonitrile-alkyl alcohol solvent mixtures at 25 p0 sC 

    E-Print Network [OSTI]

    Chu, William Wen-Chen

    1970-01-01

    the coef- ficients al through a& 1 and Kl through K& for the formula (1) 1 2K1 1 + a3K1K2D2 ''' + t+1 I a (1) 1 + K1Dl K1K2 2 + ~ + K1K2' 'KS where a is the experimentally measured nitrogen hyperfine constant. Dl through D are functions of activities... of solvation complexes Rl through R&+i. Kl through K are equilibrium constants of solvation steps for i = '1 through s, e. q. step 1 through step s. is the number of solvation steps. Usually we apply a least squares approximation to determine...

  7. Substrate-induced microstructure effects on the dynamics of the photo-induced metal

    E-Print Network [OSTI]

    Rossi, Enrico

    Substrate-induced microstructure effects on the dynamics of the photo-induced metal­ insulator investigate the differences in the dynamics of the ultrafast photo-induced metal­insulator transition (MIT­electron interactions play the critical role, and a Peierls instability of the lattice [9­12]. There are numerous

  8. Reweighted ensemble dynamics simulations: theory, improvement, and application

    E-Print Network [OSTI]

    Linchen Gong; Xin Zhou; Zhong-Can Ou-Yang

    2015-02-22

    Based on multiple parallel short molecular dynamics simulation trajectories, we designed the reweighted ensemble dynamics (RED) method to more efficiently sample complex (biopolymer) systems, and to explore their hierarchical metastable states. Here we further present an improvement to depress statistical errors of the RED and we discuss a few keys in practical application of the RED, provides schemes on selection of basis functions, determination of free parameter in the RED. We illustrate the application of the improvements in two toy models and in the solvated alanine dipeptide. The results show the RED enable to capture the topology of multiple-state transition networks, to detect the diffusion-like dynamical behavior in entropy-dominated system, and to identify solvent effects in the solvated peptides. The illustrations serve as general applications of the RED in more complex biopolymer systems.

  9. 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.

  10. Studies of third-order nonlinearities in materials and devices for ultrafast lasers

    E-Print Network [OSTI]

    Gopinath, Juliet Tara, 1976-

    2005-01-01

    Recent developments in telecommunications, frequency metrology, and medical imaging have motivated research in ultrafast optics. Demand exists for broadband components and sources as well as highly nonlinear fibers and ...

  11. Ultrafast Laser Induced Thermo-Elasto-Visco-Plastodynamics in Single Crystalline Silicon 

    E-Print Network [OSTI]

    Qi, Xuele

    2011-02-22

    A comprehensive model for describing the fundamental mechanism dictating the interaction of ultrafast laser pulse with single crystalline silicon wafer is formulated. The need for establishing the feasibility of employing lasers of subpicosecond...

  12. Electromagnetically-driven ultra-fast tool servos for diamond turning

    E-Print Network [OSTI]

    Lu, Xiaodong, Ph. D. Massachusetts Institute of Technology

    2005-01-01

    This thesis presents the design, implementation, and control of a new class of fast tool servos (FTS). The primary thesis contributions include the design and experimental demonstration of: novel ultra-fast electromagnetic ...

  13. Electron Pulse Compression with a Practical Reflectron Design for Ultrafast Electron Diffraction

    E-Print Network [OSTI]

    Wang, Yihua

    Ultrafast electron diffraction (UED) is a powerful method for studying time-resolved structural changes. Currently, space-charge-induced temporal broadening prevents obtaining high-brightness electron pulses with sub-100 ...

  14. Two photon luminescence from quantum dots using broad and narrowband ultrafast laser pulses 

    E-Print Network [OSTI]

    Balasubramanian, Haribhaskar

    2008-10-10

    Nonlinear optical microscopy (NLOM) offers many advantages when imaging intact biological samples. By using ultrafast lasers in the near infrared and two photon excitation (TPE), signal production is limited to the focal volume and provides...

  15. Ultrafast optical switching of three-dimensional Si inverse opal photonic band gap crystals

    E-Print Network [OSTI]

    Vos, Willem L.

    Ultrafast optical switching of three-dimensional Si inverse opal photonic band gap crystals Tijmen on three-dimensional photonic band gap crystals. Switching the Si inverse opal is achieved by optically

  16. Precise and ultrafast molecular sieving through graphene oxide membranes

    E-Print Network [OSTI]

    Joshi, R K; Wang, F C; Kravets, V G; Su, Y; Grigorieva, I V; Wu, H A; Geim, A K; Nair, R R

    2014-01-01

    There has been intense interest in filtration and separation properties of graphene-based materials that can have well-defined nanometer pores and exhibit low frictional water flow inside them. Here we investigate molecular permeation through graphene oxide laminates. They are vacuum-tight in the dry state but, if immersed in water, act as molecular sieves blocking all solutes with hydrated radii larger than 4.5A. Smaller ions permeate through the membranes with little impedance, many orders of magnitude faster than the diffusion mechanism can account for. We explain this behavior by a network of nanocapillaries that open up in the hydrated state and accept only species that fit in. The ultrafast separation of small salts is attributed to an 'ion sponge' effect that results in highly concentrated salt solutions inside graphene capillaries.

  17. Precise and ultrafast molecular sieving through graphene oxide membranes

    E-Print Network [OSTI]

    R. K. Joshi; P. Carbone; F. C. Wang; V. G. Kravets; Y. Su; I. V. Grigorieva; H. A. Wu; A. K. Geim; R. R. Nair

    2014-01-14

    There has been intense interest in filtration and separation properties of graphene-based materials that can have well-defined nanometer pores and exhibit low frictional water flow inside them. Here we investigate molecular permeation through graphene oxide laminates. They are vacuum-tight in the dry state but, if immersed in water, act as molecular sieves blocking all solutes with hydrated radii larger than 4.5A. Smaller ions permeate through the membranes with little impedance, many orders of magnitude faster than the diffusion mechanism can account for. We explain this behavior by a network of nanocapillaries that open up in the hydrated state and accept only species that fit in. The ultrafast separation of small salts is attributed to an 'ion sponge' effect that results in highly concentrated salt solutions inside graphene capillaries.

  18. 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.

  19. 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.

  20. Semiclassical molecular dynamics simulations of ultrafast photodissociation dynamics associated with the Chappuis band of ozone

    E-Print Network [OSTI]

    Miller, William H.

    with the Chappuis band of ozone Victor S. Batista and William H. Millera) Department of Chemistry, University A ) of ozone following photoexcitation of the molecule in the gas phase with visible light. Our algorithm and recurrence events, as well as an interpretation of experimental studies of the Chappuis band of ozone

  1. Co-nonsolvency of PNiPAM at the transition between solvation mechanisms

    E-Print Network [OSTI]

    Irmgard Bischofberger; Davide C. E. Calzolari; Veronique Trappe

    2014-10-28

    We investigate the co-nonsolvency of poly-N-isopropyl acrylamide (PNiPAM) in different water-alcohol mixtures and show that this phenomenon is due to two distinct solvation contributions governing the phase behavior of PNiPAM in the water-rich and alcohol-rich regime respectively. While hydrophobic hydration is the predominant contribution governing the phase behavior of PNiPAM in the water-rich regime, the mixing contributions governing the phase behavior of classical polymer solutions determine the phase behavior of PNiPAM in the alcohol-rich regime. This is evidenced by distinct scaling relations denoting the energetic state of the aqueous medium as a key parameter for the phase behavior of PNiPAM in the water-rich regime, while the volume fractions of respectively water, alcohol and PNiPAM become relevant parameters in the alcohol-rich regime. Adding alcohol to water decreases the energetics of the aqueous medium, which gradually suppresses hydrophobic hydration, while adding water to alcohol decreases the solvent quality. Consequently, PNiPAM is insoluble in the intermediate range of solvent composition, where neither hydrophobic hydration nor the mixing contributions prevail. This accounts for the co-nonsolvency phenomenon observed for PNiPAM in water-alcohol mixtures.

  2. Theory of Solvation-Controlled Reactions in Stimuli-Responsive Nanoreactors

    E-Print Network [OSTI]

    Angioletti-Uberti, Stefano; Ballauff, Matthias; Dzubiella, Joachim

    2015-01-01

    Metallic nanoparticles embedded in stimuli-responsive polymers can be regarded as nanoreactors since their catalytic activity can be changed within wide limits: the physicochemical properties of the polymer network can be tuned and switched by external parameters, e.g. temperature or pH, and thus allows a selective control of reactant mobility and concentration close to the reaction site. Based on a combination of Debye's model of diffusion through an energy landscape and a two-state model for the polymer, here we develop an analytical expression for the observed reaction rate constant $k_{\\rm obs}$. Our formula shows an exponential dependence of this rate on the solvation free enthalpy change $\\Delta \\bar{G}_{\\rm sol}$, a quantity which describes the partitioning of the reactant in the network versus bulk. Thus, changes in $\\Delta \\bar{G}_{\\rm sol}$, and not in the diffusion coefficient, will be the decisive factor affecting the reaction rate in most cases. A comparison with recent experimental data on switc...

  3. Quantitative comparison of fuel spray images obtained using ultrafast coherent and incoherent double-pulsed illumination

    E-Print Network [OSTI]

    Purwar, Harsh; Idlahcen, Saïd; Rozé, Claude; Blaisot, Jean-Bernard; Ménard, Thibault

    2015-01-01

    We present a quantitative comparison between the high-pressure fuel spray images obtained experimentally using classical imaging with coherent and incoherent ultrafast illuminations recorded using a compatible CMOS camera. The ultrafast, incoherent illumination source was extracted from the supercontinuum generated by tightly focusing the femtosecond laser pulses in water. The average velocity maps computed using time-correlated image-pairs and spray edge complexity computed using the average curvature scale space maps are compared for the spray images obtained with the two illumination techniques and also for the numerically simulated spray using the coupled volume of fluid and level set method for interface tracking (direct numerical simulation or DNS). The spray images obtained with supercontinuum-derived, incoherent, ultrafast illumination are clearer, since the artifacts arising due to laser speckles and multiple diffraction effects are largely reduced and show a better correlation with the DNS results.

  4. 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.

  5. 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.

  6. 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.

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

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design andBiofuelsUltrafast Core-HoleUltrafast

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

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design andBiofuelsUltrafastUltrafast

  9. InVited Feature Article Water Dynamics and Proton Transfer in Nafion Fuel Cell Membranes

    E-Print Network [OSTI]

    Fayer, Michael D.

    InVited Feature Article Water Dynamics and Proton Transfer in Nafion Fuel Cell Membranes David E is the most widely used polyelectrolyte membrane in fuel cells. Ultrafast infrared spectroscopy of the O but has since become the most commonly used membrane separator in polymer electrolyte membrane fuel cells

  10. Ultrafast Spectroscopy of CdSe Nanocrystals: Morphological and Environmental Effects on Nonradiative and Nonadiabatic Relaxation

    E-Print Network [OSTI]

    Xu, Xianfan

    Ultrafast Spectroscopy of CdSe Nanocrystals: Morphological and Environmental Effects of various morpholo- gies has been demonstrated in CdSe, such as quantum dots (QDs),3 quantum rods (QRs),4 devices and technologies have come to fruition, for example, nanocrystal solar cells (NCSC),7 lasers,8

  11. HARMONIC CASCADE FEL DESIGNS FOR LUX, A FACILTY FOR ULTRAFAST X-RAY SCIENCE

    E-Print Network [OSTI]

    Wurtele, Jonathan

    HARMONIC CASCADE FEL DESIGNS FOR LUX, A FACILTY FOR ULTRAFAST X-RAY SCIENCE J. Corlett, W. Fawley. We also discuss lattice considerations pertinent to harmonic cascade FELs, somesensitivity studies. While much of this effort has been concentrated upon SASE-based FEL's, there is an alternative "harmonic

  12. Optical Deflection and Temporal Characterization of an Ultrafast Laser-Produced Electron Beam

    E-Print Network [OSTI]

    Umstadter, Donald

    Optical Deflection and Temporal Characterization of an Ultrafast Laser-Produced Electron Beam) The interaction of a laser-produced electron beam with an ultraintense laser pulse in free space is studied. We show that the optical pulse with a0 0:5 imparts momentum to the electron beam, causing it to deflect

  13. 1 Copyright 2007 by ASME THE ROLE OF THERMAL EXCITATION OF D BAND ELECTRONS IN ULTRAFAST

    E-Print Network [OSTI]

    Zhigilei, Leonid V.

    1 Copyright © 2007 by ASME THE ROLE OF THERMAL EXCITATION OF D BAND ELECTRONS IN ULTRAFAST LASER://www.faculty.virginia.edu/CompMat/ ABSTRACT The temperature dependences of the electron heat capacity and electron-phonon coupling factor for noble (Cu) and transition (Pt) metals are investigated based on the electron density of states (DOS

  14. Large and ultrafast third-order optical nonlinearity of heteroleptic triple-decker

    E-Print Network [OSTI]

    Huang, Yanyi

    Large and ultrafast third-order optical nonlinearity of heteroleptic triple-decker Abstract The third-order optical nonlinearity of two triple-decker mixed phthalocyaninato and porphyrinato investigated for several homoleptic double- decked diphthalocyanines [8,9]. One interesting property

  15. Ultrafast conversions between hydrogen bonded structures in liquid water observed by femtosecond x-ray spectroscopy

    E-Print Network [OSTI]

    Ultrafast conversions between hydrogen bonded structures in liquid water observed by femtosecond x the first femtosecond soft x-ray spectroscopy in liquids, enabling the observation of changes in hydrogen, characteristic x-ray absorption changes monitor the conversion of strongly hydrogen-bonded water structures

  16. Metastable phase formation in the Au-Si system via ultrafast nanocalorimetry

    E-Print Network [OSTI]

    Allen, Leslie H.

    Metastable phase formation in the Au-Si system via ultrafast nanocalorimetry M. Zhang, J. G. Wen, M://jap.aip.org/features/most_downloaded Information for Authors: http://jap.aip.org/authors #12;Metastable phase formation in the Au-Si system via of Materials Science and Engineering and Coordinated Science Laboratory, University of Illinois at Urbana

  17. 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.

  18. Generation of mega-electron-volt electron beams by an ultrafast intense laser pulse

    E-Print Network [OSTI]

    Umstadter, Donald

    Generation of mega-electron-volt electron beams by an ultrafast intense laser pulse Xiaofang Wang filamentation and beam breakup. These results suggest an approach for generating a beam of femtosecond, Me-intensity lasers has made it pos- sible to study extreme physics on a tabletop. Among the studies, the generation

  19. Ultrafast Photovoltaic Response in Ferroelectric Nanolayers Dan Daranciang,1,2,3

    E-Print Network [OSTI]

    Ultrafast Photovoltaic Response in Ferroelectric Nanolayers Dan Daranciang,1,2,3 Matthew J direct coupling to its intrinsic photovoltaic response. Using time-resolved x- ray scattering nanometer-scale domains of alternating polarization that minimize the free energy of the system [3

  20. Ultra-Fast Absorption of Amorphous Pure Drug Aerosols Via Deep Lung Inhalation

    E-Print Network [OSTI]

    Rabinowitz, Joshua D.

    Ultra-Fast Absorption of Amorphous Pure Drug Aerosols Via Deep Lung Inhalation JOSHUA D. RABINOWITZ. A promising means of accelerating drug action is through rapid systemic drug administration via deep lung inhalation. The speed of pulmonary drug absorption depends on the site of aerosol deposition within the lung

  1. Ultrafast-based projection-reconstruction three-dimensional nuclear magnetic resonance spectroscopy

    E-Print Network [OSTI]

    Frydman, Lucio

    Ultrafast-based projection-reconstruction three-dimensional nuclear magnetic resonance spectroscopy Eriks Kupce Varian Ltd., 28 Manor Road, Walton-on-Thames, Surrey KT12 2QF, United Kingdom Lucio Frydmana the accelerated acquisition of multidimensional nuclear magnetic resonance nD NMR spectra. Among the methods

  2. Rough interfaces, accurate predictions: The necessity of capillary modes in a minimal model of nanoscale hydrophobic solvation

    E-Print Network [OSTI]

    Suriyanarayanan Vaikuntanathan; Grant M Rotskoff; Alexander Hudson; Phillip Geissler

    2015-10-26

    Modern theories of the hydrophobic effect highlight its dependence on length scale, emphasizing in particular the importance of interfaces that emerge in the vicinity of sizable hydrophobes. We recently showed that a faithful treatment of such nanoscale interfaces requires careful attention to the statistics of capillary waves, with significant quantitative implications for the calculation of solvation thermodynamics. Here we show that a coarse-grained lattice model in the spirit of those pioneered by Chandler and coworkers, when informed by this understanding, can capture a broad range of hydrophobic behaviors with striking accuracy. Specifically, we calculate probability distributions for microscopic density fluctuations that agree very well with results of atomistic simulations, even many standard deviations from the mean, and even for probe volumes in highly heterogeneous environments. This accuracy is achieved without adjustment of free parameters, as the model is fully specified by well-known properties of liquid water. As illustrative examples of its utility, we characterize the free energy profile for a solute crossing the air-water interface, and compute the thermodynamic cost of evacuating the space between extended nanoscale surfaces. Together, these calculations suggest that a highly reduced model for aqueous solvation can serve as the basis for efficient multiscale modeling of spatial organization driven by hydrophobic and interfacial forces.

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

    Office of Scientific and Technical Information (OSTI)

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

  4. 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...

  5. 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.

  6. Tunable spin wave dynamics in two-dimensional Ni80Fe20 nanodot lattices by varying dot shape

    E-Print Network [OSTI]

    Otani, Yoshichika

    .1063/1.4890088] Potential applications of nanomagnets1 in magnetic data storage,2,3 memory,4 and logic5,6 devices as well in the ferromagnetic nanostructures. The ever increasing demand of miniaturization and speed of devices offers-chip microwave communi- cation devices attracted interest into the ultrafast magnetiza- tion dynamics

  7. Vibrational Spectra of Water Solutions of Azoles from QM/MM Calculations: Effects of Solvation

    E-Print Network [OSTI]

    Guidoni, Leonardo

    the decomposition of the vibrational density of states of the gas phase and solution dynamics. The calculated shifts the structural and dynamical aspects of water solutions. X-ray as well as neutron diffraction are the main source and electronic structure of the molecule.1 We expect therefore that also its vibrational properties could

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

    SciTech Connect (OSTI)

    Mabuchi, Takuya, E-mail: mabuchi@nanoint.ifs.tohoku.ac.jp [Graduate School of Engineering, Tohoku University, Sendai, Miyagi 980-8577 (Japan); Tokumasu, Takashi [Institute of Fluid Science, Tohoku University, Sendai, Miyagi 980-8577 (Japan)

    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.

  9. Quantum mechanical/molecular mechanical/continuum style solvation model: Second order Møller-Plesset perturbation theory

    SciTech Connect (OSTI)

    Thellamurege, Nandun M.; Si, Dejun; Cui, Fengchao; Li, Hui, E-mail: hli4@unl.edu [Department of Chemistry, University of Nebraska-Lincoln, Lincoln, Nebraska 68588 (United States)] [Department of Chemistry, University of Nebraska-Lincoln, Lincoln, Nebraska 68588 (United States)

    2014-05-07

    A combined quantum mechanical/molecular mechanical/continuum (QM/MM/C) style second order Møller-Plesset perturbation theory (MP2) method that incorporates induced dipole polarizable force field and induced surface charge continuum solvation model is established. The Z-vector method is modified to include induced dipoles and induced surface charges to determine the MP2 response density matrix, which can be used to evaluate MP2 properties. In particular, analytic nuclear gradient is derived and implemented for this method. Using the Assisted Model Building with Energy Refinement induced dipole polarizable protein force field, the QM/MM/C style MP2 method is used to study the hydrogen bonding distances and strengths of the photoactive yellow protein chromopore in the wild type and the Glu46Gln mutant.

  10. 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 positive. As a result, the turn-on loss at low current is quite low, and the turn-off loss at low current is relatively high. The phenomenon was verified with junction capacitance measurement along with the dv/dt calculation. Under 2-kV test condition, the turn-on and turn-off losses at 25-A is about 3 and 9 mJ, respectively. As compared to a 4.5-kV, 60-A rated IGBT, which has turn-on and turn-off losses about 25 and 20 mJ under similar test condition, the SGTO shows significant switching loss reduction. The switching loss depends on the switching frequency, but under hard-switching condition, the SGTO is favored to the IGBT device. The only concern is during low current turn-on condition, there is a voltage bump that can translate to significant power loss and associated heat. The reason for such a current bump is not known from this study. It is necessary that the device manufacturer perform though test and provide the answer so the user can properly apply SGTO in pulse-width-modulated (PWM) converter and inverter applications.

  11. 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.

  12. Ultrafast Charge Separation and Nongeminate Electron-Hole Recombination in Organic Photovoltaics

    E-Print Network [OSTI]

    Samuel L Smith; Alex W Chin

    2014-06-04

    The mechanism of electron-hole separation in organic solar cells is currently hotly debated. Recent experimental work suggests that these charges can separate on extremely short timescales (<100 fs). This can be understood in terms of delocalised transport within fullerene aggregates, which is thought to emerge on short timescales before vibronic relaxation induces polaron formation. However, in the optimal heterojunction morphology, electrons and holes will often re-encounter each other before reaching the electrodes. If such charges trap and cannot separate, then device efficiency will suffer. Here we extend the theory of ultrafast charge separation to incorporate polaron formation, and find that the same delocalised transport used to explain ultrafast charge separation can account for the suppression of nongeminate recombination in the best devices.

  13. Time of flight emission spectroscopy of laser produced nickel plasma: Short-pulse and ultrafast excitations

    SciTech Connect (OSTI)

    Smijesh, N.; Chandrasekharan, K. [Laser and Nonlinear Optics Laboratory, Department of Physics, National Institute of Technology Calicut, Calicut 673601 (India); Joshi, Jagdish C.; Philip, Reji, E-mail: reji@rri.res.in [Ultrafast and Nonlinear Optics Lab, Light and Matter Physics Group, Raman Research Institute, Bangalore 560080 (India)

    2014-07-07

    We report the experimental investigation and comparison of the temporal features of short-pulse (7 ns) and ultrafast (100 fs) laser produced plasmas generated from a solid nickel target, expanding into a nitrogen background. When the ambient pressure is varied in a large range of 10??Torr to 10²Torr, the plume intensity is found to increase rapidly as the pressure crosses 1 Torr. Time of flight (TOF) spectroscopy of emission from neutral nickel (Ni I) at 361.9 nm (3d?(²D) 4p ? 3d?(²D) 4s transition) reveals two peaks (fast and slow species) in short-pulse excitation and a single peak in ultrafast excitation. The fast and slow peaks represent recombined neutrals and un-ionized neutrals, respectively. TOF emission from singly ionized nickel (Ni II) studied using the 428.5 nm (3p?3d?(³P) 4s? 3p?3d? 4s) transition shows only a single peak for either excitation. Velocities of the neutral and ionic species are determined from TOF measurements carried out at different positions (i.e., at distances of 2 mm and 4 mm, respectively, from the target surface) on the plume axis. Measured velocities indicate acceleration of neutrals and ions, which is caused by the Coulomb pull of the electrons enveloping the plume front in the case of ultrafast excitation. Both Coulomb pull and laser-plasma interaction contribute to the acceleration in the case of short-pulse excitation. These investigations provide new information on the pressure dependent temporal behavior of nickel plasmas produced by short-pulse and ultrafast laser pulses, which have potential uses in applications such as pulsed laser deposition and laser-induced nanoparticle generation.

  14. 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}.

  15. Multidiagnostic analysis of ultrafast laser ablation of metals with pulse pair irradiation

    SciTech Connect (OSTI)

    Amoruso, S.; Bruzzese, R. [Dipartimento di Scienze Fisiche, Universita degli Studi di Napoli Federico II, Complesso Universitario di Monte S. Angelo, Via Cintia, I-80126 Napoli (Italy); CNR-SPIN, Complesso Universitario di Monte S. Angelo, Via Cintia, I-80126 Napoli (Italy); Wang, X. [CNR-SPIN, Complesso Universitario di Monte S. Angelo, Via Cintia, I-80126 Napoli (Italy); O'Connell, G.; Lunney, J. G. [School of Physics, Trinity College-Dublin, Dublin 2 (Ireland)

    2010-12-01

    Copper targets are irradiated in the ablation regime by pairs of equal, time-delayed collinear laser pulses separated on a timescale going from {approx_equal}2 ps to {approx_equal}2 ns. The ablation plume is characterized by ion probe diagnostic, fast imaging, and temporally and spatially resolved optical emission spectroscopy. The variation in the ablation efficiency with the delay between the pulses is analyzed by measuring the ablation crater profile with a contact profilometer. The second laser pulse modifies the characteristics of the plasma plume produced by the first pulse and the ablation efficiency. The different mechanisms involved in double pulse ultrafast laser ablation are identified and discussed. The experimental findings are interpreted in the frame of a simple model of the interaction of the second pulse with the nascent ablation plume produced by the first pulse. This model yields consistent and quantitative agreement with the experimental findings predicting the observed experimental trends of the ablation depth reduction and ion yield increase with the delay between the pulses, as well as the characteristic timescale of the observed changes. The possibility of controlling the characteristics of the plumes produced during ultrafast laser ablation via an efficient coupling of the energy of the second pulse to the various ablation components produced by the first pulse is of particular interest in ultrafast pulsed laser deposition and microprobe analyses of materials.

  16. Synthesis, Characterization, and Ultrafast Dynamics of Metal, Metal Oxide, and Semiconductor Nanomaterials

    E-Print Network [OSTI]

    Wheeler, Damon Andreas

    2013-01-01

    for Lasing and Solar Energy Conversion. The Journal ofoptical detectors, solar energy conversion, sensors, andwith a maximum solar energy conversion efficiency of 14-

  17. Synthesis, Characterization, and Ultrafast Dynamics of Metal, Metal Oxide, and Semiconductor Nanomaterials

    E-Print Network [OSTI]

    Wheeler, Damon Andreas

    2013-01-01

    Microscopy (EM), and PL Measurements UV-Vis spectra of theMicroscopy, and ICP-OES Measurements UV-Vis spectra of theMicroscopy (EM), UV-Vis, and Raman Measurements….242

  18. Ultrafast Magnetization Dynamics of SrRuO3 Thin Films

    SciTech Connect (OSTI)

    Langner, Matthew C

    2009-05-19

    Itinerant ferromagnet SrRuO3 has drawn interest from physicists due to its unusual transport and magnetic properties as well as from engineers due to its low resistivity and good lattice-matching to other oxide materials. The exact electronic structure remains a mystery, as well as details of the interactions between magnetic and electron transport properties. This thesis describes the use of time-resolved magneto-optical Kerr spectroscopy to study the ferromagnetic resonance of SrRuO3 thin films, where the ferromagnetic resonance is initiated by a sudden change in the easy axis direction in response to a pump pulse. The rotation of the easy axis is induced by laser heating, taking advantage of a temperature-dependent easy axis direction in SrRuO3 thin films. By measuring the change in temperature of the magnetic system in response to the laser pulse, we find that the specific heat is dominated by magnons up to unusually high temperature, ~;;100 K, and thermal diffusion is limited by a boundary resistance between the film and the substrate that is not consistent with standard phonon reflection and scattering models. We observe a high FMR frequency, 250 GHz, and large Gilbert damping parameter, alpha ~;; 1, consistent with strong spin-orbit coupling. We observe a time-dependent change in the easy axis direction on a ps time-scale, and we find that parameters associated with the change in easy axis, as well as the damping parameter, have a non-monotonic temperature dependence similar to that observed in anomalous Hall measurements.

  19. Real-Time Observation of Cuprates Structural Dynamics by Ultrafast Electron Crystallography

    E-Print Network [OSTI]

    Carbone, F.

    The phonon-mediated attractive interaction between carriers leads to the Cooper pair formation in conventional superconductors. Despite decades of research, the glue holding Cooper pairs in high-temperature superconducting ...

  20. Broadband electromagnetic response and ultrafast dynamics of few-layer epitaxial graphene

    E-Print Network [OSTI]

    Choi, Hyunyong

    2010-01-01

    of few-layer epitaxial graphene H. Choi, 1 F. Borondics, 2a con?r- mation of graphene’s unusual electrodynamics. ThisLett. 96, 256802 (2006). graphene THz/IR SiC FIG. 1: (Color

  1. Ultrafast Strong-Field Vibrational Dynamics Studied by Femtosecond Extreme-Ultraviolet Transient Absorption Spectroscopy

    E-Print Network [OSTI]

    Hosler, Erik Robert

    2013-01-01

    Expansion of this technique to the attosecond regime may facilitate detection of correlated electronic and nuclear

  2. Ultrafast dynamics in helium nanodroplets probed by femtosecond time-resolved EUV photoelectron imaging

    E-Print Network [OSTI]

    Kornilov, Oleg

    2010-01-01

    production of atomic 1s4p and 1s5p states, and an angular distribution that is similar to that of isolated helium

  3. Synthesis, Characterization, and Ultrafast Dynamics of Metal, Metal Oxide, and Semiconductor Nanomaterials

    E-Print Network [OSTI]

    Wheeler, Damon Andreas

    2013-01-01

    in hematite derived from goethite. 1979, 29, Li, D. ; Teoh,of Anion Adsorption on Goethite. 1987, 51, 54-56. (126)Amorphous Silica, and Goethite Surfaces. (136) Thimsen, E. ;

  4. Ultrafast Carrier Dynamics in Exfoliated and Functionalized Calcium Niobate Nanosheets in Water and Methanol

    E-Print Network [OSTI]

    Osterloh, Frank

    and Methanol Elizabeth C. Carroll, Owen C. Compton, Dorte Madsen, Frank E. Osterloh, and Delmar S. Larsen-order kinetics on a sub-nanosecond time scale that depended on the nanosheet size. Methanol was used and methanol solutions. Methanol is known as an efficient sacrificial electron donor for layered metal oxide

  5. Synthesis, Characterization, and Ultrafast Dynamics of Metal, Metal Oxide, and Semiconductor Nanomaterials

    E-Print Network [OSTI]

    Wheeler, Damon Andreas

    2013-01-01

    R. ; Mao, S. S. Energy & Environmental Science A perspectiveDurrant, J. R. Energy & Environmental Science CorrelatingGratzel, M. Energy & Environmental Science Cathodic shift in

  6. Synthesis, Characterization, and Ultrafast Dynamics of Metal, Metal Oxide, and Semiconductor Nanomaterials

    E-Print Network [OSTI]

    Wheeler, Damon Andreas

    2013-01-01

    Solar Absorption for Photocatalysis with Black Hydrogenatedof physical Chemistry C Photocatalysis of Ag-Loaded TiO 2Lu, G. ; Yates, J. T. , Photocatalysis on TiO2 Surfaces:

  7. Synthesis, Characterization, and Ultrafast Dynamics of Metal, Metal Oxide, and Semiconductor Nanomaterials

    E-Print Network [OSTI]

    Wheeler, Damon Andreas

    2013-01-01

    study using atomic layer deposition," Journal Of PhysicalArrays Formed by Atomic Layer Deposition. 2011, 115, 9498-Cells Prepared by Atomic Layer Deposition. 2011, 27, 461-

  8. Ultrafast carrier dynamics in microcrystalline silicon probed by time-resolved terahertz spectroscopy

    E-Print Network [OSTI]

    Ku?el, Petr

    the results of optical-pump­terahertz probe experiments applied to a set of thin-film microcrys- talline range of potential applications not only in the solar cell industry, but also in the technology we report on optical pump-terahertz probe OPTP experiments with a series of thin microcrys- talline

  9. Ultrafast relaxation dynamics of hot optical phonons in graphene Haining Wang,1,a

    E-Print Network [OSTI]

    Afshari, Ehsan

    on silicon carbide substrates and by chemical vapor deposition on nickel substrates. In the first few hundred lifetime in carbon nanotubes via time- resolved Raman anti-Stokes spectroscopy was performed by Song et al-SiC wafers by thermal decomposition epitaxial growth9 and also by chemical vapor deposition CVD on nickel.10

  10. Ultrafast X-ray study of dense-liquid-jet flow dynamics using structure-tracking

    E-Print Network [OSTI]

    Loss, Daniel

    in the human body8 to industrial liquid sprays9 , and to the control of air pollution by dust particles10 into a combustion chamber. A key to successfully make the combustion cleaner and more efficient is a full

  11. Ultrafast dynamics of hot electrons and holes in copper: Excitation, energy relaxation, and transport effects

    E-Print Network [OSTI]

    Wolf, Martin

    , and transport effects E. Knoesel, A. Hotzel, and M. Wolf Fritz-Haber-Institut der MPG, Faradayweg 4-6, D-14195 calculation, a simulation of the ballistic transport effect and its implication on the observed electron process for a hot electron is scattering with a ``cold'' elec- tron below the Fermi level, because

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

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfateSciTechtail.Theory of rare Kaon and(Conference) |Article) | SciTechArticle) |Report)| SciTech

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

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfateSciTechtail.Theory of rare Kaon and(Conference) |Article) | SciTechArticle) |Report)| SciTech|

  14. 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.

  15. 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

  16. Single Photon Subradiance:Quantum control of spontaneous emission and ultrafast readout

    E-Print Network [OSTI]

    Marlan O. Scully

    2015-05-12

    Recent work has shown that collective single photon emission from an ensemble of resonate two-level atoms is a rich field of study. For example single photon superradiance from an extended ensemble yields enhanced directional spontaneous emission; and when the effects of the collective Lamb shift are included it becomes even more interesting. The present paper addresses the flip side of superradiance, i.e., subradiance. Single photon subradiant states are potentially stable against collective spontaneous emission and can have ultrafast readout. In particular, it is shown how many atom collective effects can be used to control emission by preparing and switching between subradiant and superradiant states.

  17. 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.

  18. Measurements of Ionic Structure in Shock Compressed Lithium Hydride from Ultrafast X-Ray Thomson Scattering

    SciTech Connect (OSTI)

    Kritcher, A. L. [L-399, Lawrence Livermore National Laboratory, P.O. Box 808, Livermore, California 94551 (United States); Department of Nuclear Engineering, University of California Berkeley, Berkeley, California 94709 (United States); Neumayer, P.; Doeppner, T.; Landen, O. L.; Glenzer, S. H. [L-399, Lawrence Livermore National Laboratory, P.O. Box 808, Livermore, California 94551 (United States); Brown, C. R. D. [Department of Physics, Imperial College, London SW7 2AZ (United Kingdom); AWE plc., Aldermaston, Reading, RG7 4PR (United Kingdom); Davis, P. [L-399, Lawrence Livermore National Laboratory, P.O. Box 808, Livermore, California 94551 (United States); Department of Physics, University of California Berkeley, Berkeley, California 94709 (United States); Falcone, R. W.; Lee, H. J. [Department of Physics, University of California Berkeley, Berkeley, California 94709 (United States); Gericke, D. O.; Vorberger, J.; Wuensch, K. [CFSA, Department of Physics, University of Warwick, Coventry CV4 7AL (United Kingdom); Gregori, G. [Department of Physics, Oxford University, Oxford OX1 3PU (United Kingdom); Holst, B.; Redmer, R. [Universitaet Rostock, Institut fuer Physik, D-18051 Rostock (Germany); Morse, E. C. [Department of Nuclear Engineering, University of California Berkeley, Berkeley, California 94709 (United States); Pelka, A.; Roth, M. [Institut fuer Kernphysik, Technische Universitaet Darmstadt, Darmstadt (Germany)

    2009-12-11

    We present the first ultrafast temporally, spectrally, and angularly resolved x-ray scattering measurements from shock-compressed matter. The experimental spectra yield the absolute elastic and inelastic scattering intensities from the measured density of free electrons. Laser-compressed lithium-hydride samples are well characterized by inelastic Compton and plasmon scattering of a K-alpha x-ray probe providing independent measurements of temperature and density. The data show excellent agreement with the total intensity and structure when using the two-species form factor and accounting for the screening of ion-ion interactions.

  19. An ultrafast phase-change logic device driven by melting processes

    E-Print Network [OSTI]

    Loke, D.; Skelton, J. M.; Wang, W. J.; Lee, T. H.; Zhao, R.; Chong, T. C.; Elliott, S. R.

    2014-09-02

    augmented-wave (PAW) method (36), with the Perdew-Burke-Ernzerhof (PBE) exchange-correlation functional (37), was used. The GST models were simulated in cubic supercells with periodic boundary conditions. The plane-wave energy cutoff was 174.98 eV. All... /device structures are developed with a higher number of resistance levels and resistance-level combinations (11,14). 6 The GST cells have been shown to exhibit ultra-fast Boolean algebraic operations via boosting the energy delivered by electrical...

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

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfateSciTechtail.Theory of rare Kaon and(Conference) |Article) |Fe(phen) 2 (NCS) 2Ultrafast Probes for

  1. Controlling Graphene Ultrafast Hot Carrier Response from Metal-like to Semiconductor-like by Electrostatic Gating

    E-Print Network [OSTI]

    Zettl, Alex

    with dry nitrogen during the measurement. Sample preparation We grow single layer graphene on copper foil1 Controlling Graphene Ultrafast Hot Carrier Response from Metal-like to Semiconductor electro-optic sampling.2 The focused THz beam at our graphene sample has a diameter of 1 mm. For optical

  2. Ultrafast Microfluidic Mixer and Freeze-Quenching Yu Lin, Gary J. Gerfen, Denis L. Rousseau, and Syun-Ru Yeh*

    E-Print Network [OSTI]

    Yeh, Syun-Ru

    Ultrafast Microfluidic Mixer and Freeze-Quenching Device Yu Lin, Gary J. Gerfen, Denis L. Rousseau fluids. To overcome these problems, we have designed and tested a novel microfluidic silicon mixer. The mixed-solution jet, with a cross section of 10 µm × 100 µm, exits from the microfluidic silicon mixer

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

    DOE Patents [OSTI]

    Liu, Ping (Denver, CO); Tracy, C. Edwin (Golden, CO); Pitts, J. Roland (Lakewood, CO); Lee, Se-Hee (Lakewood, CO)

    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.

  4. Hydrogen Bond Switching among Flavin and Amino Acid Side Chains in the BLUF Photoreceptor Observed by Ultrafast Infrared Spectroscopy

    E-Print Network [OSTI]

    van Stokkum, Ivo

    Hydrogen Bond Switching among Flavin and Amino Acid Side Chains in the BLUF Photoreceptor Observed hydrogen-bond network with nearby amino acid side chains, including a highly conserved tyrosine and glutamine. The participation of particular amino acid side chains in the ultrafast hydrogen-bond switching

  5. Modeling and Technologies of Ultrafast Fiber Lasers Brandon G. Bale, Oleg G. Okhitnikov, and Sergei K. Turitsyn

    E-Print Network [OSTI]

    Turitsyn, Sergei K.

    for simplicity, maintenance, and reliability, however, have not been met by conventional ultrafast technology with reliable and cost- effective components, which makes suitably designed fiber lasers real contenders many alignment issues, it also distributes heat generated by optical pumping over the length

  6. Solvent-Dependent Molecular Structure of Ionic Species Directly Measured by Ultrafast X-Ray Solution Scattering

    E-Print Network [OSTI]

    Ihee, Hyotcherl

    Solvent-Dependent Molecular Structure of Ionic Species Directly Measured by Ultrafast X often play important roles in chemical reactions occurring in water and other solvents, but it has been elusive to determine the solvent-dependent molecular structure with atomic resolution. The triiodide ion

  7. Controlling Graphene Ultrafast Hot Carrier Response from Metal-like to Semiconductor-like by Electrostatic Gating

    E-Print Network [OSTI]

    Zettl, Alex

    1 Controlling Graphene Ultrafast Hot Carrier Response from Metal-like to Semiconductor electro-optic sampling.2 The focused THz beam at our graphene sample has a diameter of 1 mm. For optical between optical pump and THz probe. We use ion-gel gating to control the carrier concentration in graphene

  8. Controlling Graphene Ultrafast Hot Carrier Response from Metal-like to Semiconductor-like by Electrostatic Gating

    E-Print Network [OSTI]

    Wang, Feng

    Controlling Graphene Ultrafast Hot Carrier Response from Metal-like to Semiconductor neutral graphene but decreases in highly doped graphene. We show that this transition from semiconductor graphene upon optical excitation. We observe that the photoinduced terahertz absorption increases in charge

  9. PUBLISHED ONLINE: 10 JANUARY 2010 | DOI: 10.1038/NPHYS1498 Ultrafast energy transfer between water molecules

    E-Print Network [OSTI]

    Loss, Daniel

    -called water dimer). This intermolecular coulombic decay leads to an ejection of a low-energy electron from and leads to dissociation of the water dimer into two H2O+ ions. As electrons of low energy (0.7-20 eV) haveLETTERS PUBLISHED ONLINE: 10 JANUARY 2010 | DOI: 10.1038/NPHYS1498 Ultrafast energy transfer

  10. Ultrafast UV Pump/IR Probe Studies of C-H Activation in Linear, Cyclic, and Aryl Hydrocarbons

    E-Print Network [OSTI]

    Harris, Charles B.

    Ultrafast UV Pump/IR Probe Studies of C-H Activation in Linear, Cyclic, and Aryl Hydrocarbons, cyclic, and aromatic hydrocarbon solvents on a femtosecond to microsecond time scale. These results have revealed that the structure of the hydrocarbon substrate affects the final C-H bond activation step, which

  11. A 64-channel personal computer based image reconstruction system and applications in single echo acquisition magnetic resonance elastography and ultra-fast magnetic resonance imaging. 

    E-Print Network [OSTI]

    Yallapragada, Naresh

    2009-05-15

    Emerging technologies in parallel magnetic resonance imaging (MRI) with massive receiver arrays have paved the way for ultra-fast imaging at increasingly high frame rates. With the increase in the number of receiver channels ...

  12. 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.

  13. Ultra-fast heralded single photon source based on telecom technology

    E-Print Network [OSTI]

    Lutfi Arif Ngah; Olivier Alibart; Laurent Labonté; Virginia D'Auria; Sébastien Tanzilli

    2014-12-17

    The realization of an ultra-fast source of heralded single photons emitted at the wavelength of 1540 nm is reported. The presented strategy is based on state-of-the-art telecom technology, combined with off-the-shelf fiber components and waveguide non-linear stages pumped by a 10 GHz repetition rate laser. The single photons are heralded at a rate as high as 2.1 MHz with a heralding efficiency of 42%. Single photon character of the source is inferred by measuring the second-order autocorrelation function. For the highest heralding rate, a value as low as 0.023 is found. This not only proves negligible multi-photon contributions but also represents the best measured value reported to date for heralding rates in the MHz regime. These prime performances, associated with a device-like configuration, are key ingredients for both fast and secure quantum communication protocols.

  14. Phonon-Assisted Ultrafast Charge Separation in a Realistic PCBM Aggregate

    E-Print Network [OSTI]

    Samuel L. Smith; Alex W. Chin

    2014-06-25

    Organic solar cells must separate strongly bound electron-hole pairs into free charges. This is achieved at interfaces between electron donor and acceptor organic semiconductors. The most popular electron acceptor is the fullerene derivative PCBM. Electron-hole separation has been observed on femtosecond timescales, which is incompatible with conventional Marcus theories of organic transport. In this work we show that ultrafast charge transport in PCBM arises from its broad range of electronic eigenstates, provided by the presence of three closely spaced delocalised bands near the LUMO level. Vibrational fluctuations enable rapid transitions between these bands, which drives an electron transport of $\\sim$3 nm within 100 fs. All this is demonstrated within a realistic tight binding Hamiltonian containing transfer integrals no larger than 8 meV.

  15. 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.

  16. 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.

  17. Broadly, independent-tunable, dual-wavelength mid-infrared ultrafast optical parametric oscillator

    E-Print Network [OSTI]

    Jin, Yuwei; Harren, Frans J M; Mandon, Julien

    2015-01-01

    We demonstrate a two-crystal mid-infrared dual-wavelength optical parametric oscillator, synchronously pumped by a high power femtosecond Yb:fiber laser. The singly-resonant ring cavity, containing two periodically poled lithium niobate crystals, is capable of generating two synchronized idler wavelengths, independently tunable over 30 THz in the 2.9 - 4.2 {\\mu}m wavelength region, due to the cascaded quadratic nonlinear effect. The independent tunability of the two idlers makes the optical parametric oscillator a promising source for ultrafast pulse generation towards the THz wavelength region, based on different frequency generation. In addition, the observed frequency doubled idler within the crystal indicates the possibility to realize a broadband optical self-phase locking between pump, signal, idler and higher order generated parametric lights.

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

    SciTech Connect (OSTI)

    Lee, Chao-Kuei, E-mail: chuckcklee@yahoo.com [Department of Photonics, National Sun-Yat-Sen University, Kaohsiung 80400, Taiwan (China); Lin, Yuan-Yao [Department of Electrical Engineering, Institute of Photonics Technologies, National Tsing Hua University, Hsinchu 30010, Taiwan (China); Lin, Sung-Hui [Department of Photonics, National Chiao Tung University, Hsinchu 30010, Taiwan (China); Lin, Gong-Ru [Department of Electrical Engineering, Graduate Institute of Photonics and Optoelectronics, National Taiwan University, No. 1, Roosevelt Road, Sec. 4, Taipei 10617, Taiwan (China); Pan, Ci-Ling [Department of Photonics, National Chiao Tung University, Hsinchu 30010, Taiwan (China); Department of Physics, National Tsing Hwa University, Hsinchu 30010, Taiwan (China)

    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.

  19. Frequency modulated few-cycle optical pulse trains induced controllable ultrafast coherent population oscillations in three-level atomic systems

    E-Print Network [OSTI]

    Parvendra Kumar; Amarendra K. Sarma

    2012-11-16

    We report a study on the ultrafast coherent population oscillations (UCPO) in two level atoms induced by the frequency modulated few-cycle optical pulse train. The phenomenon of UCPO is investigated by numerically solving the optical Bloch equations beyond the rotating wave approximation. We demonstrate that the quantum state of the atoms and the frequency of UCPO may be controlled by controlling the number of pulses in the pulse trains and the pulse repetition time respectively. Moreover, the robustness of the population inversion against the variation of the laser pulse parameters is also investigated. The proposed scheme may be useful for the creation of atoms in selected quantum state for desired time duration and may have potential applications in ultrafast optical switching.

  20. Frequency modulated few-cycle optical pulse trains induced controllable ultrafast coherent population oscillations in three-level atomic systems

    E-Print Network [OSTI]

    Kumar, Parvendra

    2012-01-01

    We report a study on the ultrafast coherent population oscillations (UCPO) in sodium atoms induced by the frequency modulated few-cycle optical pulse trains. The phenomenon of UCPO is investigated by numerically solving the appropriate density matrix equations beyond the rotating wave approximation. We demonstrate that the quantum state of the atoms and the frequency of UCPO may be controlled by controlling the number of pulses in the pulse trains and the pulse repetition time respectively. Moreover, the robustness of population transfer against the variation of laser pulse parameters is also investigated. The proposed scheme may be useful for the creation of atomic beam in selected quantum state for desired time duration and may have potential applications in ultrafast optical switching.

  1. Quantum Chemical Analysis of the Excited State Dynamics of Hydrated Electrons

    E-Print Network [OSTI]

    P. O. J. Scherer; Sighart F. Fischer

    2006-02-01

    Quantum calculations are performed for an anion water cluster representing the first hydration shell of the solvated electron in solution. The absorption spectra from the ground state, the instant excited states and the relaxed excited states are calculated including CI-SD interactions. Analytic expressions for the nonadiabatic relaxation are presented. It is shown that the 50fs dynamics recently observed after s->p excitation is best accounted for if it is identified with the internal conversion, preceded by an adiabatic relaxation within the excited p state. In addition, transient absorptions found in the infrared are qualitatively reproduced by these calculations .

  2. 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.

  3. Velocity measurements in the near field of a diesel fuel injector by ultrafast imagery

    E-Print Network [OSTI]

    Sedarsky, David; Blaisot, Jean-Bernard; Rozé, Claude

    2013-01-01

    This paper examines the velocity profile of fuel issuing from a high-pressure single-orifice diesel injector. Velocities of liquid structures were determined from time-resolved ultrafast shadow images, formed by an amplified two-pulse laser source coupled to a double-frame camera. A statistical analysis of the data over many injection events was undertaken to map velocities related to spray formation near the nozzle outlet as a function of time after start of injection. These results reveal a strong asymmetry in the liquid profile of the test injector, with distinct fast and slow regions on opposite sides of the orifice. Differences of ~100 m/s can be observed between the 'fast' and 'slow' sides of the jet, resulting in different atomization conditions across the spray. On average, droplets are dispersed at a greater distance from the nozzle on the 'fast' side of the flow, and distinct macrostructure can be observed under the asymmetric velocity conditions. The changes in structural velocity and atomization b...

  4. On the presence of ultra-fast outflows in the WAX sample of Seyfert galaxies

    E-Print Network [OSTI]

    Tombesi, Francesco

    2014-01-01

    The study of winds in active galactic nuclei (AGN) is of utmost importance as they may provide the long sought-after link between the central black hole and the host galaxy, establishing the AGN feedback. Recently, Laha et al. (2014) reported the X-ray analysis of a sample of 26 Seyferts observed with XMM-Newton, which are part of the so-called warm absorbers in X-rays (WAX) sample. They claim the non-detection of Fe K absorbers indicative of ultra-fast outflows (UFOs) in four observations previously analyzed by Tombesi et al. (2010). They mainly impute the Tombesi et al. detections to an improper modeling of the underlying continuum in the E=4-10 keV band. We therefore re-address here the robustness of these detections and we find that the main reason for the claimed non-detections is likely due to their use of single events only spectra, which reduces the total counts by 40%. Performing a re-analysis of the data in the whole E=0.3-10 keV energy band using their models and spectra including also double event...

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

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

    Dai, Yang [Shanghai Inst. of Space Power Sources, Shanghai (China); Zhu, Yimei [Brookhaven National Lab. (BNL), Upton, NY (United States); Cai, Sendan [Shanghai Inst. of Space Power Sources, Shanghai (China); Wu, Lijun [Brookhaven National Lab. (BNL), Upton, NY (United States); Yang, Weijing [Shanghai Inst. of Space Power Sources, Shanghai (China); Xie, Jingying [Shanghai Inst. of Space Power Sources, Shanghai (China); Shanghai Engineering Center for Power and Energy Storage Systems, Shanghai (China); Wen, Wen [BL14B1 Shanghai Synchrotron Radiation Facility, Shanghai (China); Zheng, Jin-Cheng [Xiamen Univ., Xiamen (China); Zheng, Yi [Shanghai Inst. of Space Power Sources, Shanghai (China)

    2014-01-01

    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.

  6. 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.

  7. 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 ?m 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

  8. 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

  9. 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.

  10. Time-resolved X-ray diffraction study of ultra-fast structural dynamics in laser-excited solids

    E-Print Network [OSTI]

    von der Linde, D.

    bent Si (311)-crystal to form a monochromatic, 1:1 image of the plasma that was generated-ray pulse width of about (300 ± 50) fs. 3. Transient Thermo-Acoustic Effects Additional insight

  11. Direct observation of ultrafast many-body electron dynamics in a strongly-correlated ultracold Rydberg gas

    E-Print Network [OSTI]

    Takei, Nobuyuki; Genes, Claudiu; Pupillo, Guido; Goto, Haruka; Koyasu, Kuniaki; Chiba, Hisashi; Weidemüller, Matthias; Ohmori, Kenji

    2015-01-01

    Many-body interactions govern a variety of important quantum phenomena ranging from superconductivity and magnetism in condensed matter to solvent effects in chemistry. Understanding those interactions beyond mean field is a holy grail of modern sciences. AMO physics with advanced laser technologies has recently emerged as a new platform to study quantum many-body systems. One of its latest developments is the study of long-range interactions among ultracold particles to reveal the effects of many-body correlations. Rydberg atoms distinguish themselves by their large dipole moments and tunability of dipolar interactions. Most of ultracold Rydberg experiments have been performed with narrow-band lasers in the Rydberg blockade regime. Here we demonstrate an ultracold Rydberg gas in a complementary regime, where electronic coherence is created using a broadband picosecond laser pulse, thus circumventing the Rydberg blockade to induce strong many-body correlations. The effects of long-range Rydberg interactions h...

  12. Ultrafast chemical dynamics of atoms and molecules studied by femtosecond time-resolved extreme ultraviolet transient absorption spectroscopy

    E-Print Network [OSTI]

    Lin, Ming-Fu

    2013-01-01

    increase rate of the green powers. The NIR powers of thedue to a decrease of the green power. Before sending anyposition, very low green power should be used to prevent

  13. Ultrafast Dynamics of the Low-Lying 3 MLCT States of [Ru(bpy)2(dppp2)]2+

    E-Print Network [OSTI]

    Turro, Claudia

    for artificial photosynthesis.1 The detailed understanding of the initial steps after the absorption of a photon

  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. 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 Å around the uranium atom, whereas the hydrogen atoms of water are distributed around the uranium atom with the major peak at around 3.0 Å. 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.

  16. Ultrafast pump-probe force microscopy with nanoscale resolution Junghoon Jahng, Jordan Brocious, Dmitry A. Fishman, Steven Yampolsky, Derek Nowak, Fei Huang, Vartkess

    E-Print Network [OSTI]

    Potma, Eric Olaf

    Ultrafast pump-probe force microscopy with nanoscale resolution Junghoon Jahng, Jordan Brocious and reconfigurable setup for all-terahertz time-resolved pump-probe spectroscopy Rev. Sci. Instrum. 83, 053107 (2012); 10.1063/1.4717732 Femtosecond time-resolved optical pump-probe spectroscopy at kilohertz

  17. Ultrafast Electron Diffraction with Spatiotemporal Resolution of Atomic Motion This article has been downloaded from IOPscience. Please scroll down to see the full text article.

    E-Print Network [OSTI]

    Cao, Jianming

    of contents for this issue, or go to the journal homepage for more Home Search Collections Journals About lattice motions in an aluminium thin-film, trigged by ultrafast laser heating, have been observed- ing sub-picosecond pulses containing a few thousands of particles per pulse. Under this low source

  18. 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.

  19. Transition from ultrafast laser photo-electron emission to space charge limited current in a 1D gap

    E-Print Network [OSTI]

    Yangjie Liu; L. K. Ang

    2014-08-21

    A one-dimensional (1D) model has been constructed to study the transition of the time-dependent ultrafast laser photo-electron emission from a flat metallic surface to the space charge limited (SCL) current, including the effect of non-equilibrium laser heating on metals at the ultrafast time scale. At a high laser field, it is found that the space charge effect cannot be ignored and the SCL current emission is reached at a lower value predicted by a short pulse SCL current model that assumed a time-independent emission process. The threshold of the laser field to reach the SCL regime is determined over a wide range of operating parameters. The calculated results agree well with particle-in-cell (PIC) simulation. It is found that the space charge effect is more important for materials with lower work function like tungsten (4.4 eV) as compared to gold (5.4 eV). However for a flat surface, both materials will reach the space charge limited regime at the sufficiently high laser field such as $>$ 5 GV/m with a laser pulse length of tens to one hundred femtoseconds.

  20. 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.

  1. Sodium Chloride interaction with solvated and crystalline cellulose : sodium ion affects the tetramer and fibril in aqueous solution

    E-Print Network [OSTI]

    Bellesia, Giovanni

    2013-01-01

    Inorganic salts are a natural component of biomass which have a significant effect on the product yields from a variety of biomass conversion processes. Understanding their effect on biomass at the microscopic level can help discover their mechanistic role. We present a study of the effect of aqueous sodium chloride (NaCl) on the largest component of biomass, cellulose, focused on the thermodynamic and structural effect of a sodium ion on the cellulose tetramer, and fibril. Replica exchange molecular dynamics simulations of a cellulose tetramer reveal a number of preferred cellulose-Na contacts and bridging positions. Large scale MD simulations on a model cellulose fibril find that Na+ perturbs the hydroxymethyl rotational state population and consequently disrupts the "native" hydrogen bonding network.

  2. 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.

  3. 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.

  4. 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.

  5. Ultrafast single-electron transfer in coupled quantum dots driven by a few-cycle chirped pulse

    SciTech Connect (OSTI)

    Yang, Wen-Xing, E-mail: wenxingyang2@126.com [Department of Physics, Southeast University, Nanjing 210096 (China); Institute of Photonics Technologies, National Tsing-Hua University, Hsinchu 300, Taiwan (China); Chen, Ai-Xi [Department of Applied Physics, School of Basic Science, East China Jiaotong University, Nanchang 330013 (China); Bai, Yanfeng [Department of Physics, Southeast University, Nanjing 210096 (China); Lee, Ray-Kuang [Institute of Photonics Technologies, National Tsing-Hua University, Hsinchu 300, Taiwan (China)

    2014-04-14

    We theoretically study the ultrafast transfer of a single electron between the ground states of a coupled double quantum dot (QD) structure driven by a nonlinear chirped few-cycle laser pulse. A time-dependent Schrödinger equation without the rotating wave approximation is solved numerically. We demonstrate numerically the possibility to have a complete transfer of a single electron by choosing appropriate values of chirped rate parameters and the intensity of the pulse. Even in the presence of the spontaneous emission and dephasing processes of the QD system, high-efficiency coherent transfer of a single electron can be obtained in a wide range of the pulse parameters. Our results illustrate the potential to utilize few-cycle pulses for the excitation in coupled quantum dot systems through the nonlinear chirp parameter control, as well as a guidance in the design of experimental implementation.

  6. Electron-ion relaxation time dependent signal enhancement in ultrafast double-pulse laser-induced breakdown spectroscopy

    SciTech Connect (OSTI)

    Harilal, S. S.; Diwakar, P. K.; Hassanein, A. [Center for Materials Under Extreme Environment, School of Nuclear Engineering, Purdue University, West Lafayette, Indiana 47907 (United States)] [Center for Materials Under Extreme Environment, School of Nuclear Engineering, Purdue University, West Lafayette, Indiana 47907 (United States)

    2013-07-22

    We investigated the emission properties of collinear double-pulse compared to single-pulse ultrafast laser induced breakdown spectroscopy. Our results showed that the significant signal enhancement noticed in the double pulse scheme is strongly correlated to the characteristic electron-ion relaxation time and hence to the inter-pulse delays. Spectroscopic excitation temperature analysis showed that the improvement in signal enhancement is caused by the delayed pulse efficient reheating of the pre-plume. The signal enhancement is also found to be related to the upper excitation energy of the selected lines, i.e., more enhancement noticed for lines originating from higher excitation energy levels, indicating reheating is the major mechanism behind the signal improvement.

  7. Vibronic coupling explains the ultrafast carotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters

    E-Print Network [OSTI]

    Perlík, Václav; Cranston, Laura J; Cogdell, Richard J; Lincoln, Craig N; Savolainen, Janne; Šanda, František; Man?al, Tomáš; Hauer, Jürgen

    2015-01-01

    The initial energy transfer in photosynthesis occurs between the light-harvesting pigments and on ultrafast timescales. We analyze the carotenoid to bacteriochlorophyll energy transfer in LH2 Marichromatium purpuratum as well as in an artificial light-harvesting dyad system by using transient grating and two-dimensional electronic spectroscopy with 10 fs time resolution. We find that F\\"orster-type models reproduce the experimentally observed 60 fs transfer times, but overestimate coupling constants, which leads to a disagreement with both linear absorption and electronic 2D-spectra. We show that a vibronic model, which treats carotenoid vibrations on both electronic ground and excited state as part of the system's Hamiltonian, reproduces all measured quantities. Importantly, the vibronic model presented here can explain the fast energy transfer rates with only moderate coupling constants, which are in agreement with structure based calculations. Counterintuitively, the vibrational levels on the carotenoid el...

  8. Water-Stable, Hydroxamate Anchors for Functionalization of TiO{sub 2} Surfaces with Ultrafast Interfacial Electron Transfer

    SciTech Connect (OSTI)

    McNamara, W. R.; Milot, R. L.; Song, H.; Snoeberger III, R. C.; Batista, Victor S.; Schmuttenmaer, C. A.; Brudvig, Gary W.; Crabtree, Robert H.

    2010-01-01

    A novel class of derivatized hydroxamic acid linkages for robust sensitization of TiO{sub 2} nanoparticles (NPs) under various aqueous conditions is described. The stability of linkages bound to metal oxides under various conditions is important in developing photocatalytic cells which incorporate transition metal complexes for solar energy conversion. In order to compare the standard carboxylate anchor to hydroxamates, two organic dyes differing only in anchoring groups were synthesized and attached to TiO{sub 2} NPs. At acidic, basic, and close to neutral pH, hydroxamic acid linkages resist detachment compared to the labile carboxylic acids. THz spectroscopy was used to compare ultrafast interfacial electron transfer (IET) into the conduction band of TiO{sub 2} for both linkages and found similar IET characteristics. Observable electron injection and stronger binding suggest that hydroxamates are a suitable class of anchors for designing water stable molecules for functionalizing TiO{sub 2}.

  9. System and method for ultrafast optical signal detecting via a synchronously coupled anamorphic light pulse encoded laterally

    DOE Patents [OSTI]

    Heebner, John E. (Livermore, CA)

    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.

  10. 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

  11. 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.; Störmer, 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.

  12. Characterization and quantification of the role of coherence in ultrafast quantum biological experiments using quantum master equations, atomistic simulations, and quantum process tomography

    E-Print Network [OSTI]

    Rebentrost, Patrick; Yuen-Zhou, Joel; Aspuru-Guzik, Alán

    2010-01-01

    Long-lived electronic coherences in various photosynthetic complexes at cryogenic and room temperature have generated vigorous efforts both in theory and experiment to understand their origins and explore their potential role to biological function. The ultrafast signals resulting from the experiments that show evidence for these coherences result from many contributions to the molecular polarization. Quantum process tomography (QPT) was conceived in the context of quantum information processing to characterize and understand general quantum evolution of controllable quantum systems, for example while carrying out quantum computational tasks. We introduce our QPT method for ultrafast experiments, and as an illustrative example, apply it to a simulation of a two-chromophore subsystem of the Fenna-Matthews-Olson photosynthetic complex, which was recently shown to have long-lived quantum coherences. Our Fenna-Matthews-Olson model is constructed using an atomistic approach to extract relevant parameters for the s...

  13. 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

  14. Sandia Energy - Scattering Dynamics

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

    Scattering Dynamics Home Transportation Energy Predictive Simulation of Engines Combustion Chemistry Chemical Dynamics Scattering Dynamics Scattering DynamicsAshley...

  15. Correlated dynamics of the motion of proton-hole wave-packets in a photoionized water cluster

    E-Print Network [OSTI]

    Li, Zheng; Vendrell, Oriol; Santra, Robin

    2012-01-01

    We explore the correlated dynamics of an electron-hole and a proton after ionization of a protonated water cluster by extreme ultra-violet (XUV) light. An ultrafast decay mechanism is found in which the proton--hole dynamics after the ionization are driven by electrostatic repulsion and involve a strong coupling between the nuclear and electronic degrees of freedom. We describe the system by a quantum-dynamical approach and show that non-adiabatic effects are a key element of the mechanism by which electron and proton repel each other and become localized at opposite sides of the cluster. Based on the generality of the decay mechanism, similar effects may be expected for other ionized systems featuring hydrogen bonds.

  16. 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.

  17. Fano resonance control in a photonic crystal structure and its application to ultrafast switching

    SciTech Connect (OSTI)

    Yu, Yi, E-mail: yiyu@fotonik.dtu.dk; Heuck, Mikkel; Hu, Hao; Xue, Weiqi; Peucheret, Christophe; Chen, Yaohui; Oxenløwe, Leif Katsuo; Yvind, Kresten; Mørk, Jesper [DTU Fotonik, Technical University of Denmark, DK-2800 Kongens Lyngby (Denmark)

    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.

  18. Ultrafast crystalline-to-amorphous phase transition in Ge{sub 2}Sb{sub 2}Te{sub 5} chalcogenide alloy thin film using single-shot imaging spectroscopy

    SciTech Connect (OSTI)

    Takeda, Jun, E-mail: jun@ynu.ac.jp; Oba, Wataru; Minami, Yasuo; Katayama, Ikufumi [Department of Physics, Graduate School of Engineering, Yokohama National University, Yokohama 240-8501 (Japan); Saiki, Toshiharu [Graduate School of Science and Technology, Keio University, Yokohama 223-8522 (Japan)

    2014-06-30

    We have observed an irreversible ultrafast crystalline-to-amorphous phase transition in Ge{sub 2}Sb{sub 2}Te{sub 5} chalcogenide alloy thin film using broadband single-shot imaging spectroscopy. The absorbance change that accompanied the ultrafast amorphization was measured via single-shot detection even for laser fluences above the critical value, where a permanent amorphized mark was formed. The observed rise time to reach the amorphization was found to be ?130–200 fs, which was in good agreement with the half period of the A{sub 1} phonon frequency in the octahedral GeTe{sub 6} structure. This result strongly suggests that the ultrafast amorphization can be attributed to the rearrangement of Ge atoms from an octahedral structure to a tetrahedral structure. Finally, based on the dependence of the absorbance change on the laser fluence, the stability of the photoinduced amorphous phase is discussed.

  19. NuSTAR Reveals Relativistic Reflection But No Ultra-Fast Outflow In The Quasar PG 1211+143

    E-Print Network [OSTI]

    Zoghbi, A; Walton, D J; Harrison, F A; Fabian, A C; Reynolds, C S; Boggs, S E; Christensen, F E; Craig, W; Hailey, C J; Stern, D; Zhang, W W

    2015-01-01

    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' (or, 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 UFO's show 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,...

  20. 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.

  1. 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.

  2. Dynamic Reconstruction

    E-Print Network [OSTI]

    Horn, Berthold Klaus Paul

    Dynamic reconstruction is a method for generating images or image sequences from data obtained using moving radiation detection systems. While coded apertures are used as examples of the underlying information collection ...

  3. From gyroscopic to thermal motion: a crossover in the dynamics of molecular superrotors

    E-Print Network [OSTI]

    Milner, A A; Rezaiezadeh, K; Milner, V

    2015-01-01

    Localized heating of a gas by intense laser pulses leads to interesting acoustic, hydrodynamic and optical effects with numerous applications in science and technology, including controlled wave guiding and remote atmosphere sensing. Rotational excitation of molecules can serve as the energy source for raising the gas temperature. Here, we study the dynamics of energy transfer from the molecular rotation to heat. By optically imaging a cloud of molecular superrotors, created with an optical centrifuge, we experimentally identify two separate and qualitatively different stages of its evolution. The first non-equilibrium "gyroscopic" stage is characterized by the modified optical properties of the centrifuged gas - its refractive index and optical birefringence, owing to the ultrafast directional molecular rotation, which survives tens of collisions. The loss of rotational directionality is found to overlap with the release of rotational energy to heat, which triggers the second stage of thermal expansion. The ...

  4. Semiclassical molecular dynamics simulations of excited state double-proton transfer in 7-azaindole dimers

    SciTech Connect (OSTI)

    Guallar, V.; Batista, V.S.; Miller, W.H. [Department of Chemistry, University of California, and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)] [Department of Chemistry, University of California, and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)

    1999-05-01

    An {ital ab initio} excited state potential energy surface is constructed for describing excited state double proton transfer in the tautomerization reaction of photo-excited 7-azaindole dimers, and the ultrafast dynamics is simulated using the semiclassical (SC) initial value representation (IVR). The potential energy surface, determined in a reduced dimensionality, is obtained at the CIS level of quantum chemistry, and an approximate version of the SC-IVR approach is introduced which scales {ital linearly} with the number of degrees of freedom of the molecular system. The accuracy of this approximate SC-IVR approach is verified by comparing our semiclassical results with full quantum mechanical calculations. We find that proton transfer usually occurs during the first intermonomer symmetric-stretch vibration, about 100 fs after photoexcitation of the system, and produces an initial 15 percent population decay of the reactant base-pair, which is significantly reduced by isotopic substitution. {copyright} {ital 1999 American Institute of Physics.} thinsp

  5. 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

  6. 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

    Multiferroic materials have attracted much interest in the past decade, due not only to their novel device applications, but also their manifestations of coupling and interactions between different order parameters (particularly electric polarization and magnetic order). Recently, much attention has been focused on perovskite manganites, RMnO{sub 3} (R = rare earth ions), due to the discovery of a large magnetoelectric effect in these materials. The first member of this family to be discovered was TbMnO{sub 3} (TMO), which is now well established as a typical magnetoelectric multiferroic. Extensive experimental and theoretical studies have already been done on single crystal TMO (SC-TMO). In brief, SC-TMO, with a distorted orthorhombic perovskite structure, has an antiferromagnetic (AFM) phase transition at T{sub N} {approx}40 K with sinusoidally ordered Mn moments. Below T{sub FE} {approx} 28 K, ferroelectric (FE) order develops owing to the appearance of cycloidal spiral spin structure. In contrast, there are relatively few reports describing the properties of TMO thin films (typically grown on SrTiO{sub 3} (STO) substrates). In general, thin films can enable new functionality in materials, as their physical parameters can be changed by modifying their structure via strain imposed by the substrate. Strain in particular has the potential to directly couple FE and FM orders, which is very rare. This could benefit electronic device applications by providing low power consumption, high speed operation, and greater electric/magnetic field controllability. Previous investigations of magnetic properties in TMO films revealed an unexpected ferromagnetic (FM) order, in contrast to SC-TMO. However, several important questions regarding these films are still unanswered for instance: (1) What mechanism induces FM order? (2) Can FM, sinusoidal AFM and spiral AFM (or FE) orders coexist? (3) Can FM order be coupled to FE order? To fully understand these unique materials, 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.

  7. Excited State Structural Dynamics of Carotenoids and ChargeTransfer Systems

    SciTech Connect (OSTI)

    Van Tassle, Aaron Justin

    2006-09-01

    This dissertation describes the development andimplementation of a visible/near infrared pump/mid-infrared probeapparatus. Chapter 1 describes the background and motivation ofinvestigating optically induced structural dynamics, paying specificattention to solvation and the excitation selection rules of highlysymmetric molecules such as carotenoids. Chapter 2 describes thedevelopment and construction of the experimental apparatus usedthroughout the remainder of this dissertation. Chapter 3 will discuss theinvestigation of DCM, a laser dye with a fluorescence signal resultingfrom a charge transfer state. By studying the dynamics of DCM and of itsmethyl deuterated isotopomer (an otherwise identical molecule), we areable to investigate the origins of the charge transfer state and provideevidence that it is of the controversial twisted intramolecular (TICT)type. Chapter 4 introduces the use of two-photon excitation to the S1state, combined with one-photon excitation to the S2 state of thecarotenoid beta-apo-8'-carotenal. These 2 investigations show evidencefor the formation of solitons, previously unobserved in molecular systemsand found only in conducting polymers Chapter 5 presents an investigationof the excited state dynamics of peridinin, the carotenoid responsiblefor the light harvesting of dinoflagellates. This investigation allowsfor a more detailed understanding of the importance of structuraldynamics of carotenoids in light harvesting.

  8. Update on Electrolyte Modeling with Emphasis on Low Temperature...

    Energy Savers [EERE]

    Regions (subtask low temperature performance) Linking Ion Solvation and Lithium Battery Electrolyte Properties Molecular dynamics simulation studies of electrolytes...

  9. Molecular Simulations of Electrolytes and Electrolyte/Electrode...

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

    electrode interfaces Molecular dynamics simulation studies of electrolytes and electrolyteelectrode interfaces Linking Ion Solvation and Lithium Battery Electrolyte Properties...

  10. Nonlinear ultrafast dynamics of high temperature YBa[subscript 2]Cu[subscript 3]O[subscript 7-?] superconductors probed with THz pump / THz probe spectroscopy

    E-Print Network [OSTI]

    Grady, Nathaniel K.

    High power THz pulses induce near transparency in superconductive YBCO thin films below the critical temperature. THz pump/THz probe measurements reveal a decay of the induced transparency on the time scale of a few picoseconds.

  11. Ultrafast dynamics of strong-field dissociative ionization of CH2Br2 probed by femtosecond soft x-ray transient absorption spectroscopy

    E-Print Network [OSTI]

    Loh, Zhi-Heng; Leone, Stephen R.

    2008-01-01

    M. Lezius, V. Blanchet, D. M. Rayner, D. M. Villeneuve, A.I. V. Litvinyuk, K. F. Lee, D. M. Rayner, M. Spanner, D. M.F. Lee, P. W. Dooley, D. M. Rayner, D. M. Villeneuve, and P.

  12. 7216 J. Phys. Chem. 1993,97, 7216-7221 Ultrafast Electronic Deactivation and Vibrational Dynamics of Photoexcited Uranium(IV)

    E-Print Network [OSTI]

    Girolami, Gregory S.

    of Photoexcited Uranium(IV) Porphyrin Sandwich Complexes Osman Bilse1,t Stanley N. Milam,* Gregory S. Girolami

  13. 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.

  14. Reversibility, Water-Mediated Switching, and Directed Cell Dynamics

    E-Print Network [OSTI]

    J. C. Phillips

    2008-03-02

    Reversible switching of the complex network dynamics of proteins is mimicked in selected network glasses and compacted small carbohydrate molecules. Protein transitions occur on long time scales ~ us -ms, evocative of the exponentially large viscosities found in glass-forming supercooled liquids just above the glass transition; in searching for mechanisms for reversibly slowed "geared activation", Kauzmann was led from proteins to glasses. I show here that selected network glasses and small carbohydrate molecules can be used to model such transitions, and elucidate in particular some universal aspects of tandem repeats. The human ankyrin tandem repeat D34, with a superhelical "coiled spring" structure which has 426 residues, folds reversibly and plastically. Such molecules are too large for present transition-state numerical simulations, currently limited to ~ 100 residues solvated by ~ 3000 water molecules for times ~ ns. The transition states of D34 exhibit a surprisingly simple collective ("geared") pattern when studied by fluorescence near its center, in samples modified mutageneously along its 12 helical repeats. One can understand this "plastic" pattern by taking advantage of a symmetric 45-atom carbohydrate molecular bridge to "cross over" from proteins to inorganic network glasses. There one easily identifies gears, and can show that the collective pattern is the signature of nonlocal, water-mediated [hydro(phobic/philic)] switching. Details of the transition patterns emerge from analyzing the amino acid alpha helical repeat sequences with water-only hydrophobicity scales. Freezing and melting of monolayer water films at physiological temperatures can enable ankyrin repeats to direct cell dynamics in muscles, membranes and cytoskeletons.

  15. 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.

  16. Hierarchical Dynamic Models

    E-Print Network [OSTI]

    Penny, Will

    Hierarchical Dynamic Models Will Penny OU Processes Embedding OU(2) process Dynamic Models Hierarchical Dynamic Models Will Penny 26th May 2011 #12;Hierarchical Dynamic Models Will Penny OU Processes Dynamic Models Will Penny OU Processes Embedding OU(2) process Dynamic Models Generalised coordinates

  17. Nonadiabatic ab initio molecular dynamics of photoisomerization in bridged azobenzene

    SciTech Connect (OSTI)

    Gao Aihua; Li Bin; Zhang Peiyu; Han Keli [State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China)

    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.

  18. Coherent exciton dynamics in the presence of underdamped vibrations

    E-Print Network [OSTI]

    Arend G. Dijkstra; Chen Wang; Jianshu Cao; Graham R. Fleming

    2014-12-22

    Recent ultrafast optical experiments show that excitons in large biological light-harvesting complexes are coupled to molecular vibration modes. These high-frequency vibrations will not only affect the optical response, but also drive the exciton transport. Here, using a model dimer system, the frequency of the underdamped vibration is shown to have a strong effect on the exciton dynamics such that quantum coherent oscillations in the system can be present even in the case of strong noise. Two mechanisms are identified to be responsible for the enhanced transport efficiency: critical damping due to the tunable effective strength of the coupling to the bath, and resonance coupling where the vibrational frequency coincides with the energy gap in the system. The interplay of these two mechanisms determines parameters responsible for the most efficient transport, and these optimal control parameters are comparable to those in realistic light-harvesting complexes. Interestingly, oscillations in the excitonic coherence at resonance are suppressed in comparison to the case of an off-resonant vibration.

  19. 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.

  20. Ultrafast neutron detector

    DOE Patents [OSTI]

    Wang, Ching L. (Livermore, CA)

    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.

  1. 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.

  2. Photoinduced Excited State Electron Transfer at Liquid/Liquid Interfaces

    E-Print Network [OSTI]

    Cooper, Jason K; Benjamin, Ilan

    2014-01-01

    of Coumarin- 314 at the Water/Air Interface. J. Phys. Chem.Solvation of Coumarin 314 at Water/Air Interfaces AontainingSolvation Dynamics at the Air/Water Interface with Time-

  3. Electronic Relaxation Dynamics in Coupled Metal Nanoparticles

    E-Print Network [OSTI]

    Scherer, Norbert F.

    that takes into account two competing phenomena: electron inelastic surface scattering (ISS), which tends the ultrafast response to optical excitation. For example, they have promise as optical switches and as sources of hot electrons for photoelectrochemical processes, including solar energy conversion or organic waste

  4. Sandia Energy - Chemical Dynamics

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

    Chemical Dynamics Home Transportation Energy Predictive Simulation of Engines Combustion Chemistry Chemical Dynamics Chemical DynamicsAshley Otero2015-10-28T02:45:37+00:00...

  5. Bright, Coherent, Ultrafast Soft X-Ray Harmonics Spanning the Water Window from a Tabletop Light Source

    E-Print Network [OSTI]

    M. C. Chen; P. Arpin; T. Popmintchev; M. Gerrity; B. Zhang; M. Seaberg; M. M. Murnane; H. C. Kapteyn

    2010-06-20

    We demonstrate fully phase matched high-order harmonic generation with emission spanning the water window spectral region important for bio- and nano-imaging and a breadth of materials and molecular dynamics studies. We also generate the broadest bright coherent bandwidth (~300eV) to date obtained from any light source, small or large. The harmonic photon flux at 0.5 keV is 10^3 higher than demonstrated previously, making it possible for the first time to demonstrate spatial coherence in the water window. The continuum emission is consistent with a single attosecond burst, that extends bright attosecond pulses into the soft x-ray region.

  6. 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 = 1–6, 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 carbon–oxygen covalent bond compared to EC-. In ab initio molecular dynamics (AIMD) simulations of EC- solvated in liquid EC, large fluctuations in the carbonyl carbon–oxygen 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.

  7. Mesoscale Structures at Complex Fluid-Fluid Interfaces: a Novel Lattice Boltzmann / Molecular Dynamics Coupling

    E-Print Network [OSTI]

    Marcello Sega; Mauro Sbragaglia; Sofia Sergeevna Kantorovich; Alexey Olegovich Ivanov

    2014-02-19

    Complex fluid-fluid interfaces featuring mesoscale structures with adsorbed particles are key components of newly designed materials which are continuously enriching the field of soft matter. Simulation tools which are able to cope with the different scales characterizing these systems are fundamental requirements for efficient theoretical investigations. In this paper we present a novel simulation method, based on the approach of Ahlrichs and D\\"unweg [Ahlrichs and D\\"unweg, Int. J. Mod. Phys. C, 1998, 9, 1429], that couples the "Shan-Chen" multicomponent Lattice Boltzmann technique to off-lattice molecular dynamics to simulate efficiently complex fluid-fluid interfaces. We demonstrate how this approach can be used to study a wide class of challenging problems. Several examples are given, with an accent on bicontinuous phases formation in polyelectrolyte solutions and ferrofluid emulsions. We also show that the introduction of solvation free energies in the particle-fluid interaction unveils the hidden, multiscale nature of the particle-fluid coupling, allowing to treat symmetrically (and interchangeably) the on-lattice and off-lattice components of the system.

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

    Office of Scientific and Technical Information (OSTI)

    be obtained from a Raman spectroscopic evaluation of electrolytes containing the LiPF6 salt and aprotic solvents. Of particular note is the overlap of the Raman bands for both...

  9. Electrolyte Solvation and Ionic Association. V. Acetonitrile...

    Office of Scientific and Technical Information (OSTI)

    V. Acetonitrile-Lithium Bis(fluorosulfonyl)imide (LiFSI) Mixtures Electrolytes with the salt lithium bis(fluorosulfonyl)imide (LiFSI) have been evaluated relative to comparable...

  10. 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...

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

    Office of Scientific and Technical Information (OSTI)

    States Language: English Subject: coordination; crystal structure; ionic association; lithium; Raman Word Cloud More Like This Full Text Journal Articles DOI: 10.1021jp5046782...

  12. The Microscopic Linear Dynamics

    E-Print Network [OSTI]

    Penny, Will

    The Microscopic Brain Will Penny Linear Dynamics Exponentials Matrix Exponential Eigendecomposition References The Microscopic Brain Will Penny 7th April 2011 #12;The Microscopic Brain Will Penny Linear;The Microscopic Brain Will Penny Linear Dynamics Exponentials Matrix Exponential Eigendecomposition

  13. Categorical Introduction to Dynamical Systems Symbolic Dynamical Systems

    E-Print Network [OSTI]

    Kahng, Byung-Jay

    Categorical Introduction to Dynamical Systems Symbolic Dynamical Systems Symbolic Embedding Examples Results Embeddings in Symbolic Dynamical Systems Jonathan Jaquette Swarthmore College July 22, 2009 Jonathan Jaquette Embeddings in Symbolic Dynamical Systems #12;Categorical Introduction

  14. Intramolecular and nonlinear dynamics

    SciTech Connect (OSTI)

    Davis, M.J. [Argonne National Laboratory, IL (United States)

    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.

  15. Introduction Dynamical properties of (-)-transformation Dynamical properties of

    E-Print Network [OSTI]

    /04/2010 Digital expansions, dynamics and tilings, Aussois Dynamical properties of the (-)-transformation 1/17 #12 of (-)-transformation Digital expansions, dynamics and tilings, Aussois Dynamical properties of the (-)-transformation 2/17 #12;Introduction Dynamical properties of (-)-transformation Introduction Digital expansions, dynamics

  16. Dynamics of femtosecond laser absorption of fused silica in the ablation regime

    SciTech Connect (OSTI)

    Lebugle, M., E-mail: lebugle@lp3.univ-mrs.fr; Sanner, N.; Varkentina, N.; Sentis, M.; Utéza, O. [Aix Marseille Université, CNRS, LP3 UMR 7341, 13288 Marseille (France)

    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.

  17. Femtosecond surface plasmon interferometry with gold nanostructures

    E-Print Network [OSTI]

    Temnov, Vasily V.

    We measure the ultrafast electron dynamics in gold via ultrafast surface plasmon interferometry. A new plasmonic microinterferometer with tilted slit-groove pair is used to unambiguously determine changes of real and ...

  18. 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?.

  19. Dynamic Instruction Fusion

    E-Print Network [OSTI]

    Lee, Ian

    2012-01-01

    SANTA CRUZ DYNAMIC INSTRUCTION FUSION A thesis submitted in4 2.2 Instruction Fusion & Complex10 3.1 Fusion Selection

  20. Elliptical Galaxy Dynamics

    E-Print Network [OSTI]

    David Merritt

    1998-11-06

    A review of elliptical galaxy dynamics, with a focus on nonintegrable models. Topics covered include torus construction; modelling axisymmetric galaxies; triaxiality; collisionless relaxation; and collective instabilities.

  1. Electromagnetic Wave Dynamics in

    E-Print Network [OSTI]

    Kaiser, Robin

    Mesoscopic Electromagnetic Wave Dynamics in Ultracold Atomic Gases Robin Kaiser and Mark D. Havey Mesoscopic Electromagnetic Wave Dynamics in Ultracold Atomic Gases #12;39 E xperimental developments permit in the transport proper- ties of electromagnetic radiation in strongly scattering random media. Even in weakly

  2. Skyrmion Dynamics for Spintronic Devices

    E-Print Network [OSTI]

    Liu, Yizhou

    2013-01-01

    Skyrmion Dynamics for Spintronic Devices A Thesis submittedSkyrmion Dynamics for Spintronic Devices by Yizhou Liua candidate for future spintronic devices. However, Skyrmion

  3. Dynamic Positioning Simulator Dynamic Positioning Simulator

    E-Print Network [OSTI]

    Vuik, Kees

    to the ocean floor, without using anchors accomplished by two or more propulsive devices controlled by inputs Dynamic Positioning: No tugboats needed; Offshore set-up is quick; Power saving; Precision situations more on Ship: Wind Force Fw = 1 2 air V 2 rw CXw (rw )AT 1 2 air V 2 rw CYw (rw )AL Mw = 1 2 air V 2 rw CMw (rw

  4. 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. At present this is done using liquid electrolytes that are flammable-a serious...

  5. Ultrafast Transformations in Superionic Nanocrystals

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

    no longer had to travel through a vacuum in fragile glass tubes to create or process electrical signals. Instead, they moved within a solid material, and logic switches could...

  6. Ultrafast Transformations in Superionic Nanocrystals

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

    of solid-state electronics represented a major upgrade over the use of mechanical switches and vacuum tubes. Devices incorporating solid-state electronics could be smaller,...

  7. Ultrafast X-ray Sources

    SciTech Connect (OSTI)

    George Neil

    2010-04-19

    Since before the scattering of X-rays off of DNA led to the first understanding of the double helix structure, sources of X-rays have been an essential tool for scientists examining the structure and interactions of matter. The resolution of a microscope is proportional to the wavelength of light so x-rays can see much finer structures than visible light, down to single atoms. In addition, the energy of X-rays is resonant with the core atomic levels of atoms so with appropriate wavelengths the placement of specific atoms in a large molecule can be determined. Over 10,000 scientists use synchrotron sources, storage rings of high energy electrons, each year worldwide. As an example of such use, virtually every picture of a protein or drug molecule that one sees in the scientific press is a reconstruction based on X-ray scattering of synchrotron light from the crystallized form of that molecule. Unfortunately those pictures are static and proteins work through configuration (shape) changes in response to energy transfer. To understand how biological systems work requires following the energy flow to these molecules and tracking how shape changes drive their interaction with other molecules. We'd like to be able to freeze the action of these molecules at various steps along the way with an X-ray strobe light. How fast does it have to be? To actually get a picture of a molecule in a fixed configuration requires X-ray pulses as short as 30 femtoseconds (1/30 of a millionth of a millionth of a second). To capture the energy flow through changes in electronic levels requires a faster strobe, less than 1 femtosecond! And to acquire such information in smaller samples with higher accuracy demands brighter and brighter X-rays. Unfortunately modern synchrotrons (dubbed 3rd Generation Light Sources) cannot deliver such short bright pulses of X-rays. An entirely new approach is required, linear-accelerator (linac-)-based light sources termed 4th or Next Generation Light Sources (NGLSs). Although NGLSs will not displace synchrotrons from their role they do offer exciting new capabilities which can be understood from the physics of the light production in each device.

  8. 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.

  9. 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,...

  10. Ultrafast Transformations in Superionic Nanocrystals

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

    pathways determining how these materials switch and the new functional properties that emerge at the nanoscale are largely unknown and unexplored. Researchers have recently carried...

  11. Ultrafast Transformations in Superionic Nanocrystals

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

    level. Depiction of the copper sulfide superionic state with copper in blue and sulfur in yellow. Image credit: Greg StewartSLAC National Accelerator Laboratory. In...

  12. Ultrafast Transformations in Superionic Nanocrystals

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity ofkandz-cm11 Outreach Home RoomPreservationBio-Inspired SolarAbout /Two0 - 19 Publications 1.Design » Design

  13. Ultrafast Transformations in Superionic Nanocrystals

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity ofkandz-cm11 Outreach Home RoomPreservationBio-Inspired SolarAbout /Two0 - 19 Publications 1.Design »

  14. Ultrafast Transformations in Superionic Nanocrystals

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effectWorking With WIPPfinal design

  15. LUSI :: LCLS Ultrafast Science Instruments

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power Administration would likeUniverseIMPACTThousand CubicResource andfirstDevice UW Madison LineTransitionLUG

  16. Quasistatic dynamical systems

    E-Print Network [OSTI]

    Neil Dobbs; Mikko Stenlund

    2015-04-08

    We introduce the notion of a quasistatic dynamical system, which generalizes that of an ordinary dynamical system. Quasistatic dynamical systems are inspired by the namesake processes in thermodynamics, which are idealized processes where the observed system transforms (infinitesimally) slowly due to external influence, tracing out a continuous path of thermodynamic equilibria over an (infinitely) long time span. Time-evolution of states under a quasistatic dynamical system is entirely deterministic, but choosing the initial state randomly renders the process a stochastic one. In the prototypical setting where the time-evolution is specified by strongly chaotic maps on the circle, we obtain a description of the statistical behaviour as a stochastic diffusion process, under surprisingly mild conditions on the initial distribution, by solving a well-posed martingale problem. We also consider various admissible ways of centering the process, with the curious conclusion that the "obvious" centering suggested by the initial distribution sometimes fails to yield the expected diffusion.

  17. Dynamics of Nanoconfined Acetonitrile

    E-Print Network [OSTI]

    Norton, Cassandra

    2011-04-27

    components of interest in the simulations are the diffusion coefficients and reorientational correlation times, two dynamical constants of a given system, and the causes of the magnitudes and variability of each is explored. The acetonitrile molecules...

  18. Nanoindentation Under Dynamic Conditions

    E-Print Network [OSTI]

    Wheeler, Jeffrey M

    2009-05-22

    and in analysis of the resulting data. Recent development has enabled investigation of materials under several dynamic conditions. The palladium-hydrogen system has a large miscibility gap, where the palladium lattice rapidly expands to form a hydrogen-rich ?...

  19. Photochemical reaction dynamics

    SciTech Connect (OSTI)

    Moore, B.C. [Lawrence Berkeley Laboratory, Livermore, CA (United States)

    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.

  20. 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.

  1. 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.

  2. The Dynamical Discrete Web

    E-Print Network [OSTI]

    L. R. G. Fontes; C. M. Newman; K. Ravishankar; E. Schertzer

    2007-04-20

    The dynamical discrete web (DDW), introduced in recent work of Howitt and Warren, is a system of coalescing simple symmetric one-dimensional random walks which evolve in an extra continuous dynamical parameter s. The evolution is by independent updating of the underlying Bernoulli variables indexed by discrete space-time that define the discrete web at any fixed s. In this paper, we study the existence of exceptional (random) values of s where the paths of the web do not behave like usual random walks and the Hausdorff dimension of the set of such exceptional s. Our results are motivated by those about exceptional times for dynamical percolation in high dimension by H\\"aggstrom, Peres and Steif, and in dimension two by Schramm and Steif. The exceptional behavior of the walks in DDW is rather different from the situation for dynamical random walks of Benjamini, H\\"aggstrom, Peres and Steif. In particular, we prove that there are exceptional values of s for which the walk from the origin S^s(n) has limsup S^s(n)/\\sqrt n \\leq K with a nontrivial dependence of the Hausdorff dimension on K. We also discuss how these and other results extend to the dynamical Brownian web, a natural scaling limit of DDW. The scaling limit is the focus of a paper in preparation; it was studied by Howitt and Warren and is related to the Brownian net of Sun and Swart.

  3. Dynamical laser spike processing

    E-Print Network [OSTI]

    Shastri, Bhavin J; Tait, Alexander N; Rodriguez, Alejandro W; Wu, Ben; Prucnal, Paul R

    2015-01-01

    Novel materials and devices in photonics have the potential to revolutionize optical information processing, beyond conventional binary-logic approaches. Laser systems offer a rich repertoire of useful dynamical behaviors, including the excitable dynamics also found in the time-resolved "spiking" of neurons. Spiking reconciles the expressiveness and efficiency of analog processing with the robustness and scalability of digital processing. We demonstrate that graphene-coupled laser systems offer a unified low-level spike optical processing paradigm that goes well beyond previously studied laser dynamics. We show that this platform can simultaneously exhibit logic-level restoration, cascadability and input-output isolation---fundamental challenges in optical information processing. We also implement low-level spike-processing tasks that are critical for higher level processing: temporal pattern detection and stable recurrent memory. We study these properties in the context of a fiber laser system, but the addit...

  4. Statistics of football dynamics

    E-Print Network [OSTI]

    Mendes, R S; Anteneodo, C

    2007-01-01

    We investigate the dynamics of football matches. Our goal is to characterize statistically the temporal sequence of ball movements in this collective sport game, searching for traits of complex behavior. Data were collected over a variety of matches in South American, European and World championships throughout 2005 and 2006. We show that the statistics of ball touches presents power-law tails and can be described by $q$-gamma distributions. To explain such behavior we propose a model that provides information on the characteristics of football dynamics. Furthermore, we discuss the statistics of duration of out-of-play intervals, not directly related to the previous scenario.

  5. 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.

  6. Protein Dynamics and Biocatalysis

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power Administration wouldMass mapSpeedingProgramExemptionsProtein Dynamics Hit the Big Screen Protein Dynamics

  7. Introduction to Accelerated Molecular Dynamics

    SciTech Connect (OSTI)

    Perez, Danny [Los Alamos National Laboratory

    2012-07-10

    Molecular Dynamics is the numerical solution of the equations of motion of a set of atoms, given an interatomic potential V and some boundary and initial conditions. Molecular Dynamics is the largest scale model that gives unbiased dynamics [x(t),p(t)] in full atomistic detail. Molecular Dynamics: is simple; is 'exact' for classical dynamics (with respect to a given V); can be used to compute any (atomistic) thermodynamical or dynamical properties; naturally handles complexity -- the system does the right thing at the right time. The physics derives only from the interatomic potential.

  8. Speeding up dynamic compilation: concurrent and parallel dynamic compilation 

    E-Print Network [OSTI]

    Bohm, Igor

    2013-07-02

    The main challenge faced by a dynamic compilation system is to detect and translate frequently executed program regions into highly efficient native code as fast as possible. To efficiently reduce dynamic compilation ...

  9. Dynamic Systems, Measurement,

    E-Print Network [OSTI]

    Singhose, William

    Journal of Dynamic Systems, Measurement, and Control Technical Briefs Remote Vibration Control for Flexible Beams Subject to Harmonic Disturbances Shang-Teh Wu Department of Mechanical Engineering, National at the boundary are required in the control algorithm, which emulates the behavior of a set of mechanical spring

  10. LABORATORY VI ROTATIONAL DYNAMICS

    E-Print Network [OSTI]

    Minnesota, University of

    Lab VI - 1 LABORATORY VI ROTATIONAL DYNAMICS So far this semester, you have been asked to think kinematics. OBJECTIVES: Successfully completing this laboratory should enable you to: · Use linear kinematics in a laboratory on earth, before launching the satellite. EQUIPMENT You will use an apparatus that spins

  11. NEWS & VIEWS Glass dynamics

    E-Print Network [OSTI]

    Weeks, Eric R.

    NEWS & VIEWS Glass dynamics Diverging views on glass transition Gregory B. mc.mckenna@ttu.edu T he glass transition is one of the most intriguing phenomena in the world of soft condensed matter. Despite decades of study, many aspects of the behaviour of glass-forming liquids remain elusive

  12. Dynamical transition, hydrophobic interface, and the temperature dependence of electrostatic fluctuations in proteins

    E-Print Network [OSTI]

    Matyushov, Dmitry

    fluctuations in proteins David N. LeBard and Dmitry V. Matyushov Center for Biological Physics, Arizona State the redox state of the protein, is related to the formation of the hydrophobic protein-water interface, allowing large-amplitude collective fluctuations of the water density in the protein's first solvation

  13. Molecular Dynamics Simulations of a Set of Isoniazid Derivatives Bound to

    E-Print Network [OSTI]

    Ferreira, Márcia M. C.

    13084-971, POB 6154, Brazil 2 Laboratory of Molecular Modeling and Design (M/C-781), College of Pharmacy was used to calculate the solvation energy of the lowest-energy conformation obtained from each MDS. Structural parameters as well as binding energy contributions were considered in this analysis

  14. Shared and Dynamic Libraries on Hopper

    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...

  15. Tools for dynamic model development

    E-Print Network [OSTI]

    Schaber, Spencer Daniel

    2014-01-01

    For this thesis, several tools for dynamic model development were developed and analyzed. Dynamic models can be used to simulate and optimize the behavior of a great number of natural and engineered systems, from the ...

  16. 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.

  17. 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.

  18. Nonlinear chemical dynamics Francesc Sagusa

    E-Print Network [OSTI]

    Epstein, Irving R.

    Nonlinear chemical dynamics Francesc Saguésa and Irving R. Epsteinb a Departament de Química Física March 2003 The interdisciplinary field of nonlinear chemical dynamics has grown significantly in breadth an overview of some of the key results of nonlinear chemical dynamics, with emphasis on those areas most

  19. ANALYSING DYNAMIC FUNCTION SCHEDULING DECISIONS

    E-Print Network [OSTI]

    Harrison, Michael

    , University of York, York YO10 5DD, UK Abstract: Function allocation, as a process used in the construction, the notion of dynamic function allocation becomes increasingly desirable where in certain situations of dynamic function allocation that reflects typical work activity where the dynamic scheduling of activities

  20. 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.

  1. Beam Dynamics for ARIA

    SciTech Connect (OSTI)

    Ekdahl, Carl August Jr. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    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.

  2. Dynamical impurity problems

    SciTech Connect (OSTI)

    Emery, V.J. [Brookhaven National Lab., Upton, NY (United States); Kivelson, S.A. [California Univ., Los Angeles, CA (United States). Dept. of Physics

    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. Dynamical Methods in Algebra Dynamical Methods in Algebra [1] Dynamical Methods in Algebra

    E-Print Network [OSTI]

    Coquand, Thierry

    Dynamical Methods in Algebra Dynamical Methods in Algebra [1] Dynamical Methods in Algebra We present a possible realisation of Hilbert's program for (some part of) abstract algebra G in number theory) that cannot be eliminated Surprisingly this is not the case for abstract algebra 1 #12

  4. 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

    Funded by the DOE grant (i) we continued to study and analyze the atomistic detail of the electron transfer (ET) across the chromophore-TiO2 interface in Gratzel cell systems for solar hydrogen production. (ii) We extensively investigated the nature of photoexcited states and excited state dynamics in semiconductor quantum dots (QD) designed for photovoltaic applications. (iii) We continued a newly initiated research direction focusing on excited state properties and electron-phonon interactions in nanoscale carbon materials. Over the past year, the results of the DOE funded research were summarized in 3 review articles. 12 original manuscripts were written. The research results were reported in 28 invited talks at conferences and university seminars. 20 invitations were accepted for talks in the near future. 2 symposia at national and international meetings have being organized this year on topics closely related to the DOE funded project, and 2 more symposia have been planned for the near future. We summarized the insights into photoinduced dynamics of semiconductor QDs, obtained from our time-domain ab initio studies. QDs exhibit both molecular and bulk properties. Unlike either bulk or molecular materials, QD properties can be modified continuously by changing QD shape and size. However, the chemical and physical properties of molecular and bulk materials often contradict each other, which can lead to differing viewpoints about the behavior of QDs. For example, the molecular view suggests strong electron-hole and charge-phonon interactions, as well as slow energy relaxation due to mismatch between electronic energy gaps and phonon frequencies. In contrast, the bulk view advocates that the kinetic energy of quantum confinement is greater than electron-hole interactions, that charge-phonon coupling is weak, and that the relaxation through quasi-continuous bands is rapid. By synthesizing the bulk and molecular viewpoints, we clarified the controversies and 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 excitations. Conduction and valence band transitions that are not available in neutral NCs dominate

  5. Hamiltonian Dynamics of Preferential Attachment

    E-Print Network [OSTI]

    Zuev, Konstantin; Krioukov, Dmitri

    2015-01-01

    Prediction and control of network dynamics are grand-challenge problems in network science. The lack of understanding of fundamental laws driving the dynamics of networks is among the reasons why many practical problems of great significance remain unsolved for decades. Here we study the dynamics of networks evolving according to preferential attachment, known to approximate well the large-scale growth dynamics of a variety of real networks. We show that this dynamics is Hamiltonian, thus casting the study of complex networks dynamics to the powerful canonical formalism, in which the time evolution of a dynamical system is described by Hamilton's equations. We derive the explicit form of the Hamiltonian that governs network growth in preferential attachment. This Hamiltonian turns out to be nearly identical to graph energy in the configuration model, which shows that the ensemble of random graphs generated by preferential attachment is nearly identical to the ensemble of random graphs with scale-free degree d...

  6. Symmetries in open quantum dynamics

    E-Print Network [OSTI]

    Thomas F. Jordan

    2014-08-20

    Simple examples are used to introduce and examine a Heisenberg picture of symmetries of open quantum dynamics that can be described by unitary operators. When the symmetries are for Hamiltonian dynamics of an entire system, and the spectrum of the Hamiltonian operator has a lower bound, the symmetry operators commute with the Hamiltonian operator. An example shows that symmetry operators need not commute with the Hamiltonian operator when the spectrum of the Hamiltonian does not have a lower bound. There are many more symmetries that are only for the open dynamics of a subsystem and are described by unitary operators that do not commute with the Hamiltonian for the dynamics of the entire system. Examples show how these symmetries alone can reveal properties of the dynamics and reduce what needs to be done to work out the dynamics. A symmetry of the open dynamics of a subsystem can imply properties of the dynamics for the entire system that are not implied by the symmetries of the dynamics of the entire system. The symmetries are generally not related to constants of the motion for the open dynamics of the subsystem. There are symmetries of the open dynamics of a subsystem that depend only on the dynamics. In the simplest examples, these are also symmetries of the dynamics of the entire system. There are many more symmetries, of a new kind, that also depend on correlations, or absence of correlations, between the subsystem and the rest of the entire system, or on the state of the rest of the entire system. Symmetries that depend on correlations generally cannot be seen in the Schr\\"{o}dinger picture as symmetries of dynamical maps of density matrices for the subsystem.

  7. Dynamics of Motivations

    E-Print Network [OSTI]

    Knoll, Jörn

    ) - Upot, f mean field = C(f(x, p, t)) Collision Term = p2 2m - Upot(x, p) dp1dp2dp3 d d (1 - f)f1(1 - f2, t)) Collision Term = p2 2m - Upot(x, p) dp1dp2dp3 d d (1 - f)f1(1 - f2)f3 + loss term. Voskresensky1,3 1GSI 2Kurchatov Inst. (Moscow) 3Moscow Ins. for Physics and Engineering #12;Dynamics

  8. Jets, Lifts and Dynamics

    E-Print Network [OSTI]

    O?ul Esen; Hasan Gümral

    2010-11-03

    We show that complete cotangent lifts of vector fields, their decomposition into vertical representative and holonomic part provide a geometrical framework underlying Eulerian equations of continuum mechanics. We discuss Euler equations for ideal incompressible fluid and Vlasov equations of plasma dynamics in connection with the lifts of divergence-free and Hamiltonian vector fields, respectively. As a further application, we obtain kinetic equations of particles moving with the flow of contact vector fields both from Lie-Poisson reductions and with the techniques of present framework.

  9. Dynamic Transfer Limits Study

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power Administration would like submit theCovalentLaboratory |Sectorfor $1.14 Per1-ENuclearDynamic Switching

  10. Dynamic Bertrand Oligopoly

    SciTech Connect (OSTI)

    Ledvina, Andrew, E-mail: aledvina@princeton.edu; Sircar, Ronnie, E-mail: sircar@princeton.ed [Princeton University, ORFE Department (United States)

    2011-02-15

    We study continuous time Bertrand oligopolies in which a small number of firms producing similar goods compete with one another by setting prices. We first analyze a static version of this game in order to better understand the strategies played in the dynamic setting. Within the static game, we characterize the Nash equilibrium when there are N players with heterogeneous costs. In the dynamic game with uncertain market demand, firms of different sizes have different lifetime capacities which deplete over time according to the market demand for their good. We setup the nonzero-sum stochastic differential game and its associated system of HJB partial differential equations in the case of linear demand functions. We characterize certain qualitative features of the game using an asymptotic approximation in the limit of small competition. The equilibrium of the game is further studied using numerical solutions. We find that consumers benefit the most when a market is structured with many firms of the same relative size producing highly substitutable goods. However, a large degree of substitutability does not always lead to large drops in price, for example when two firms have a large difference in their size.

  11. Los Alamos Dynamics Summer School

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

    School Los Alamos Dynamics Summer School Overview Contact Institute Director Charles Farrar (505) 663-5330 Email Professional Staff Assistant Jutta Kayser (505) 663-5649 Email...

  12. Dynamically Responsive Infrared Window Coatings

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

    Dynamically Responsive Infrared Window Coatings 2015 Building Technologies Office Peer Review Dr. Kyle J. Alvine, kyle.alvine@pnnl.gov Pacific Northwest National Laboratory 21C...

  13. Algorithms for dynamical overlap fermions

    E-Print Network [OSTI]

    Stefan Schaefer

    2006-09-28

    An overview of the current status of algorithmic approaches to dynamical overlap fermions is given. In particular the issue of changing the topological sector is discussed.

  14. Nuclear Matter and Nuclear Dynamics

    E-Print Network [OSTI]

    M Colonna

    2009-02-26

    Highlights on the recent research activity, carried out by the Italian Community involved in the "Nuclear Matter and Nuclear Dynamics" field, will be presented.

  15. 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 to solvent evaporation. These effects become more important as cluster size increases. In addition, differences in timescale and mechanism are observed between clusters of Ar, which binds to I{sup -} and I{sub 2}{sup -} rather weakly, and CO{sub 2}, whose large quadruple moment allows substantially stronger binding to these anions.

  16. 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.

  17. Quasifission dynamics in TDHF

    E-Print Network [OSTI]

    Umar, A S; Simenel, C

    2015-01-01

    For light and medium mass systems the capture cross-section may be considered to be the same as that for complete fusion, whereas for heavy systems leading to superheavy formations the evaporation residue cross-section is dramatically reduced due to the quasifission (QF) and fusion-fission processes thus making the capture cross-section to be essentially the sum of these two cross-sections, with QF occurring at a much shorter time-scale. Consequently, quasifission is the primary reaction mechanism that limits the formation of superheavy nuclei. Within the last few years the time-dependent Hartree-Fock (TDHF) approach has been utilized for studying the dynamics of quasifission. The study of quasifission is showing a great promise to provide insight based on very favorable comparisons with experimental data. In this article we will focus on the TDHF calculations of quasifission observables for the $^{48}$Ca+$^{249}$Bk system.

  18. Dynamical Yukawa Couplings

    E-Print Network [OSTI]

    Rodrigo Alonso

    2013-07-07

    The matter content of the Standard Model admits a global symmetry due to the generational structure of the spectrum respected by all interactions except for fermion couplings to the Higgs doublet. This symmetry is identified as the largest possible global symmetry of the free theory and extended to the case of massive neutrinos. The violation of such symmetry is then assumed dynamical and the value of the Yukawa couplings is fixed by a variational principle. This ansatz yields compelling results: Quark Yukawas naturally accommodate hierarchical masses and small mixing whereas Lepton Yukawas exhibit a hierarchical pattern for charged leptons and simultaneously degeneracy in the neutrino sector correlated with large mixing and Majorana phases. The difference in the mixing patterns of Quark and Leptons in this scheme stem from the Dirac vs Majorana nature of fermions.

  19. Hamiltonian Dynamics of Preferential Attachment

    E-Print Network [OSTI]

    Konstantin Zuev; Fragkiskos Papadopoulos; Dmitri Krioukov

    2015-04-29

    Prediction and control of network dynamics are grand-challenge problems in network science. The lack of understanding of fundamental laws driving the dynamics of networks is among the reasons why many practical problems of great significance remain unsolved for decades. Here we study the dynamics of networks evolving according to preferential attachment, known to approximate well the large-scale growth dynamics of a variety of real networks. We show that this dynamics is Hamiltonian, thus casting the study of complex networks dynamics to the powerful canonical formalism, in which the time evolution of a dynamical system is described by Hamilton's equations. We derive the explicit form of the Hamiltonian that governs network growth in preferential attachment. This Hamiltonian turns out to be nearly identical to graph energy in the configuration model, which shows that the ensemble of random graphs generated by preferential attachment is nearly identical to the ensemble of random graphs with scale-free degree distributions. In other words, preferential attachment generates nothing but random graphs with power-law degree distribution. The extension of the developed canonical formalism for network analysis to richer geometric network models with non-degenerate groups of symmetries may eventually lead to a system of equations describing network dynamics at small scales.

  20. Dynamic Coupling Measurement for Object-

    E-Print Network [OSTI]

    Bae, Doo-Hwan

    Dynamic Coupling Measurement for Object- Oriented Software Dynamic Coupling Measurement for Object- Oriented SoftwareErik Arisholm, Lionel C. Briand, Audun Foyen IEEE Transaction on Software Engineering/2)Introduction (1/2) Extensive research related to quality of OO software has performed Define structural metrics

  1. Status of dynamical ensemble generation

    E-Print Network [OSTI]

    Chulwoo Jung

    2010-01-06

    I give an overview of current and future plans of dynamical QCD ensemble generation activities. A comparison of simulation cost between different discretizations is made. Recent developments in techniques and algorithms used in QCD dynamical simulations, especially mass reweighting, are also discussed.

  2. Dynamics and Equilibria Sergiu Hart

    E-Print Network [OSTI]

    Naor, Moni

    Dynamics and Equilibria Sergiu Hart Presidential Address, GAMES 2008 (July 2008) Revised and Expanded (November 2009) Revised (2010, 2011, 2012, 2013) SERGIU HART c 2008 ­ p. #12;DYNAMICS AND EQUILIBRIA Sergiu Hart Center for the Study of Rationality Dept of Economics Dept of Mathematics The Hebrew

  3. Attosecond Probing of Vibrational Dynamics with High-Harmonic Generation Manfred Lein*

    E-Print Network [OSTI]

    Lein, Manfred

    ; published 11 February 2005) The numerical solution of the time-dependent Schro¨dinger equation for vibrating hydrogen molecules in few-cycle laser pulses shows that high-harmonic generation is sensitive to the laser.80.Rv The laser-based measurement of ultrafast processes in atoms and molecules has recently advanced

  4. FEATURE ARTICLE Femtosecond Studies of Electron Dynamics at Dielectric-Metal Interfaces

    E-Print Network [OSTI]

    Harris, Charles B.

    of Chemistry, UniVersity of California, Berkeley, California 94720, and Chemical Sciences DiVision, E. O. Lawrence Berkeley National Laboratory, Berkeley, California 94720 ReceiVed: September 30, 1998 Ultrafast transport properties across an interface requires the knowledge of the energies, spatial extent

  5. chsm.Rev. 1992. 92.463-480 463 Dynamical Solvent Effects on Activated Electron-Transfer Reactions

    E-Print Network [OSTI]

    Turro, Nicholas J.

    influencesexerted by the solvating environment upon the kinetics of electron- transfer (ET)proteases, either solvent influences upon AG' attributed to the reactionfree energy, AGO, whereas the former describesthe only mildly by the "slow" nuclear solvent modes. In addition to such energetic factors, however, one

  6. Real-time dynamics for interactive environments 

    E-Print Network [OSTI]

    Timchenko, Alexander Nikolai

    2009-05-15

    . Two primary dynamic behaviors are explored: rigid body dynamics and articulated dynamics. A generalized collision response model is built for rigid bodies and articulated structures which can be adapted to other types of behaviors. The framework...

  7. Dynamics of neural cryptography

    SciTech Connect (OSTI)

    Ruttor, Andreas; Kinzel, Wolfgang; Kanter, Ido [Institut fuer Theoretische Physik, Universitaet Wuerzburg, Am Hubland, 97074 Wuerzburg (Germany); Minerva Center and Department of Physics, Bar Ilan University, Ramat Gan 52900 (Israel)

    2007-05-15

    Synchronization of neural networks has been used for public channel protocols in cryptography. In the case of tree parity machines the dynamics of both bidirectional synchronization and unidirectional learning is driven by attractive and repulsive stochastic forces. Thus it can be described well by a random walk model for the overlap between participating neural networks. For that purpose transition probabilities and scaling laws for the step sizes are derived analytically. Both these calculations as well as numerical simulations show that bidirectional interaction leads to full synchronization on average. In contrast, successful learning is only possible by means of fluctuations. Consequently, synchronization is much faster than learning, which is essential for the security of the neural key-exchange protocol. However, this qualitative difference between bidirectional and unidirectional interaction vanishes if tree parity machines with more than three hidden units are used, so that those neural networks are not suitable for neural cryptography. In addition, the effective number of keys which can be generated by the neural key-exchange protocol is calculated using the entropy of the weight distribution. As this quantity increases exponentially with the system size, brute-force attacks on neural cryptography can easily be made unfeasible.

  8. 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.

  9. Fractal dynamics of earthquakes

    SciTech Connect (OSTI)

    Bak, P.; Chen, K. [Brookhaven National Lab., Upton, NY (United States). Dept. of Physics

    1995-05-01

    Many objects in nature, from mountain landscapes to electrical breakdown and turbulence, have a self-similar fractal spatial structure. It seems obvious that to understand the origin of self-similar structures, one must understand the nature of the dynamical processes that created them: temporal and spatial properties must necessarily be completely interwoven. This is particularly true for earthquakes, which have a variety of fractal aspects. The distribution of energy released during earthquakes is given by the Gutenberg-Richter power law. The distribution of epicenters appears to be fractal with dimension D {approx} 1--1.3. The number of after shocks decay as a function of time according to the Omori power law. There have been several attempts to explain the Gutenberg-Richter law by starting from a fractal distribution of faults or stresses. But this is a hen-and-egg approach: to explain the Gutenberg-Richter law, one assumes the existence of another power-law--the fractal distribution. The authors present results of a simple stick slip model of earthquakes, which evolves to a self-organized critical state. Emphasis is on demonstrating that empirical power laws for earthquakes indicate that the Earth`s crust is at the critical state, with no typical time, space, or energy scale. Of course the model is tremendously oversimplified; however in analogy with equilibrium phenomena they do not expect criticality to depend on details of the model (universality).

  10. Computational fluid dynamic applications

    SciTech Connect (OSTI)

    Chang, S.-L.; Lottes, S. A.; Zhou, C. Q.

    2000-04-03

    The rapid advancement of computational capability including speed and memory size has prompted the wide use of computational fluid dynamics (CFD) codes to simulate complex flow systems. CFD simulations are used to study the operating problems encountered in system, to evaluate the impacts of operation/design parameters on the performance of a system, and to investigate novel design concepts. CFD codes are generally developed based on the conservation laws of mass, momentum, and energy that govern the characteristics of a flow. The governing equations are simplified and discretized for a selected computational grid system. Numerical methods are selected to simplify and calculate approximate flow properties. For turbulent, reacting, and multiphase flow systems the complex processes relating to these aspects of the flow, i.e., turbulent diffusion, combustion kinetics, interfacial drag and heat and mass transfer, etc., are described in mathematical models, based on a combination of fundamental physics and empirical data, that are incorporated into the code. CFD simulation has been applied to a large variety of practical and industrial scale flow systems.

  11. Laser Driven Dynamic Loading of Condensed Matter

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

    Laser Driven Dynamic Loading of Condensed Matter Laser Driven Dynamic Loading of Condensed Matter Advanced diagnostics of experiments covering many orders of magnitude in strain...

  12. 16.07 Dynamics, Fall 2004

    E-Print Network [OSTI]

    Peraire, Jaume

    Dynamics starts with fundamentals of Newtonian mechanics. Further topics include kinematics, particle dynamics, motion relative to accelerated reference frames, work and energy, impulse and momentum, systems of particles ...

  13. Proceedings of the Seventeenth DOE Solar Photochemistry Research Conference

    SciTech Connect (OSTI)

    Not Available

    1993-12-31

    The Seventeenth DOE Solar Photochemistry Research Conference sponsored by the Division of Chemical Sciences, Office of Basic Energy Sciences, is being held June 6--10, 1993, at Cragun`s Lodge and Conference Center, Brainerd, Minnesota The meeting is hosted this year by the Ames Laboratory of Iowa State University. The purpose of the meeting is to foster cooperation, collaboration, and exchange of current research ideas among grantees and contractors of the DOE Division of Chemical Sciences engaged in fundamental research on solar photochemical energy conversion. This conference provides a special opportunity for interaction among investigators from diverse traditional chemistry disciplines who share the common good of providing the knowledge and concepts needed for production of low cost fuels and chemicals or electricity by photochemical conversion of solar energy. Our special guest plenary lecturer is Professor Graham Fleming, of the University of Chicago, who will speak on ultrafast spectroscopic studies of molecular dynamics in the condensed phase. The remaining presentations on Monday will feature further investigations of ultrafast phenomena in solvation, electron transfer, and charge separation at interfaces. These will lead into the topical sessions which follow on photosynthesis, molecular models, photoinduced charge transfer in homogeneous and heterogeneous solutions, inorganic photochemistry, and photoelectrochemistry. As an added feature, the photoelectrochemistry session will include six short introductory lectures for the benefit of nonspecialists on outstanding issues and problems in that field. In this volume may be found a copy of the program, the abstracts of 28 formal presentations and 59 posters, as well as an address listing of the 114 participants.

  14. Connecting curves for dynamical systems

    E-Print Network [OSTI]

    R. Gilmore; Jean-Marc Ginoux; Timothy Jones; C. Letellier; U. S. Freitas

    2010-03-08

    We introduce one dimensional sets to help describe and constrain the integral curves of an $n$ dimensional dynamical system. These curves provide more information about the system than the zero-dimensional sets (fixed points) do. In fact, these curves pass through the fixed points. Connecting curves are introduced using two different but equivalent definitions, one from dynamical systems theory, the other from differential geometry. We describe how to compute these curves and illustrate their properties by showing the connecting curves for a number of dynamical systems.

  15. 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.

  16. Gas-phase chemical dynamics

    SciTech Connect (OSTI)

    Weston, R.E. Jr.; Sears, T.J.; Preses, J.M. [Brookhaven National Laboratory, Upton, NY (United States)

    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.

  17. Essays in dynamic general equilibrium

    E-Print Network [OSTI]

    Cao, Dân (Dân Vu?)

    2010-01-01

    This thesis consists of three chapters studying dynamic economies in general equilibrium. The first chapter considers an economy in business cycles with potentially imperfect financial markets. The second chapter investigates ...

  18. Abstract Machines for Dynamic Computation 

    E-Print Network [OSTI]

    Walton, Christopher D

    In this thesis we address the challenges associated with the provision of dynamic software architectures. These are systems in which programs are constructed from separately compiled units with a facility for the replacement ...

  19. Mantle dynamics in the Mediterranean

    E-Print Network [OSTI]

    Faccenna, Claudio

    The Mediterranean offers a unique opportunity to study the driving forces of tectonic deformation within a complex mobile belt. Lithospheric dynamics are affected by slab rollback and collision of two large, slowly moving ...

  20. Dynamical Mutation of Dark Energy

    E-Print Network [OSTI]

    L. R. Abramo; R. C. Batista; L. Liberato; R. Rosenfeld

    2008-01-03

    We discuss the intriguing possibility that dark energy may change its equation of state in situations where large dark energy fluctuations are present. We show indications of this dynamical mutation in some generic models of dark energy.

  1. Dynamical mutation of dark energy

    SciTech Connect (OSTI)

    Abramo, L. R.; Batista, R. C. [Instituto de Fisica, Universidade de Sao Paulo, CP 66318, 05315-970, Sao Paulo (Brazil); Liberato, L.; Rosenfeld, R. [Instituto de Fisica Teorica, Universidade Estadual Paulista, R. Pamplona 145, 01405-900, Sao Paulo (Brazil)

    2008-03-15

    We discuss the intriguing possibility that dark energy may change its equation of state in situations where large dark energy fluctuations are present. We show indications of this dynamical mutation in some generic models of dark energy.

  2. Qubit dynamics under alternating controls

    E-Print Network [OSTI]

    Aiello, Clarice Demarchi

    2014-01-01

    In this thesis, we discuss two problems of quantum dynamics in the presence of alternating controls. Alternating controls arise in many protocols designed to extend the duration over which a qubit is a useful computational ...

  3. Nonlinear dynamics of hysteretic oscillators 

    E-Print Network [OSTI]

    Shekhawat, Ashivni

    2009-05-15

    The dynamic response and bifurcations of a harmonic oscillator with a hysteretic restoring force and sinusoidal excitation are investigated. A multilinear model of hysteresis is presented. A hybrid system approach is used to formulate and study...

  4. 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.

  5. Peak mass and dynamical friction

    E-Print Network [OSTI]

    A. Del Popolo; M. Gambera

    1995-06-09

    We show how the results given by several authors relatively to the mass of a density peak are changed when small scale substructure induced by dynamical friction are taken into account. The peak mass obtained is compared to the result of Peacock \\& Heavens (1990) and to the peak mass when dynamical friction is absent to show how these effects conspire to reduce the mass accreted by the peak.

  6. Dynamical Crossover in Supercritical Water

    E-Print Network [OSTI]

    Yu. D. Fomin; V. N. Ryzhov; E. N. Tsiok; V. V. Brazhkin

    2015-02-10

    Dynamical crossover in water is studied by means of computer simulation. The crossover temperature is calculated from the behavior of velocity autocorrelation functions. The results are compared with experimental data. It is shown that the qualitative behavior of the dynamical crossover line is similar to the melting curve behavior. Importantly, the crossover line belongs to experimentally achievable $(P,T)$ region which stimulates the experimental investigation in this field.

  7. Dynamic Tides in Close Binaries

    E-Print Network [OSTI]

    B. Willems

    2005-11-10

    The basic theory of dynamic tides in close binaries is reviewed. Particular attention is paid to resonances between dynamic tides and free oscillation modes and to the role of the apsidal-motion rate in probing the internal structure of binary components. The discussed effects are generally applicable to stars across the entire Hertzsprung-Russell diagram, including the binary OB-stars discussed at this meeting.

  8. Role of solvation in pressure-induced helix stabilization

    E-Print Network [OSTI]

    Best, Robert B; Mittal, Jeetain

    2015-01-01

    In contrast to the well-known destabilization of globular proteins by high pressure, re- cent work has shown that pressure stabilizes the formation of isolated {\\alpha}-helices. However all simulations to date have obtained a qualitatively opposite result within the experimen- tal pressure range. We show that using a protein force field (Amber03w) parametrized in conjunction with an accurate water model (TIP4P/2005) recovers the correct pressure- dependence and an overall stability diagram for helix formation similar to that from experi- ment; on the other hand, we confirm that using TIP3P water results in a very weak pressure destabilization of helices. By carefully analyzing the contributing factors, we show that this is not merely a consequence of different peptide conformations sampled using TIP3P. Rather, there is a critical role for the solvent itself in determining the dependence of total system volume (peptide and solvent) on helix content. Helical peptide structures exclude a smaller volume to water,...

  9. Role of solvation in pressure-induced helix stabilization

    E-Print Network [OSTI]

    Robert B. Best; Cayla Miller; Jeetain Mittal

    2015-03-12

    In contrast to the well-known destabilization of globular proteins by high pressure, re- cent work has shown that pressure stabilizes the formation of isolated {\\alpha}-helices. However all simulations to date have obtained a qualitatively opposite result within the experimen- tal pressure range. We show that using a protein force field (Amber03w) parametrized in conjunction with an accurate water model (TIP4P/2005) recovers the correct pressure- dependence and an overall stability diagram for helix formation similar to that from experi- ment; on the other hand, we confirm that using TIP3P water results in a very weak pressure destabilization of helices. By carefully analyzing the contributing factors, we show that this is not merely a consequence of different peptide conformations sampled using TIP3P. Rather, there is a critical role for the solvent itself in determining the dependence of total system volume (peptide and solvent) on helix content. Helical peptide structures exclude a smaller volume to water, relative to non-helical structures with both the water models, but the total system volume for helical conformations is higher than non-helical conformations with TIP3P water at low to intermediate pressures, in contrast to TIP4P/2005 water. Our results further emphasize the importance of using an accurate water model to study protein folding under conditions away from standard temperature and pressure.

  10. Linking Ion Solvation and Lithium Battery Electrolyte Properties...

    Broader source: Energy.gov (indexed) [DOE]

    Nonfluorinated (or Partially Fluorinated) Anions for Lithium Salts and Ionic Liquids for Lithium Battery Electrolytes Inexpensive, Nonfluorinated (or Partially Fluorinated) Anions...

  11. Drag reduction and solvation in polymer solutions Witold Brostow*1

    E-Print Network [OSTI]

    North Texas, University of

    with low MDF for: oil well operations; crude oil trans- port; fire fighting; high sewer throughput; irrigation; hydrotransport of solids; marine applications; and bio- medical applications including in a variety of applications1, 2) : oil well operations,crude oil transport, fire fighting,increasing sewer

  12. The Solvation and Dissociation of 4Benzylaniline Hydrochloride in Chlorobenzene

    E-Print Network [OSTI]

    Miller, Alice

    , John M. Winfield, David Adam, Alice A. Miller, Robert H. Carr,§ Archie Eaglesham,§ and David Lennon

  13. 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...

  14. Diversity of felodipine solvates: structure and physicochemical properties

    E-Print Network [OSTI]

    Surov, Artem O.; Solanko, Katarzyna A.; Bond, Andrew D.; Bauer-Brandl, Annette; Perlovich, German L.

    2015-04-20

    312) equipped with a hot stage and Microstat 100 temperature controller. The microscope images were recorded with an Altami CMOS digital camera using Altami Studio image capture software. The samples were heated over a temperature range of 25–170°C... are expected to be less stable with respect to their Fel-Fel interactions. The transformation from the “back-40 to-back” to the “side-on” arrangement occurs at certain value of Vvdw for the solvent molecule, which is apparently large enough to stabilize...

  15. Lithium Diisopropylamide Solvated by Hexamethylphosphoramide: Substrate-Dependent

    E-Print Network [OSTI]

    Collum, David B.

    the Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell UniVersity, Ithaca, New York 14853. In Encyclopedia of Reagents for Organic Synthesis; Paquette, L. A., Ed.; Wiley: New York, 1995; Vol. 4, pp 2668

  16. Oscillatory Solvation Forces: A Comparison of Theory and

    E-Print Network [OSTI]

    Attard, Phil

    Department of Applied Mathematics, Research School of Physical Sciences and Engineering, Australian National of the molecular detail it pro­ vides about the behaviour of surfaces and fluids, but also because the measurements on mechan­ ical springs and optical interferometry [28]. Improvements on this basic design have been made

  17. Hydration, Solvation and Hydrolysis of Multicharged Metal Ions

    E-Print Network [OSTI]

    to a dimer, [Th2 (2 -OH)2 (H2 O)12 ]6+ , then to a tetramer, [Th4 (2 - OH)8 (H2 O)16 ]8+ , and finally. Coordinated water looses the protons in two steps, first with the formation of the dimer and tetramer to a dimer, then to a tetramer, [Cr4 (2 -OH)2 (-OH)4 (OH)n (H2 O)12-n ](6-n)+ with increasing pH from 0 to 3

  18. Accurate Evaluation of Charge Asymmetry in Aqueous Solvation

    E-Print Network [OSTI]

    Mukhopadhyay, Abhishek; Onufriev, Alexey V

    2015-01-01

    Charge hydration asymmetry (CHA) -- a characteristic dependence of hydration free energy on the sign of the solute charge -- quantifies the asymmetric response of water to electric field at microscopic level. Accurate estimates of CHA are critical for understanding of hydration effects ubiquitous in chemistry and biology. However, measuring hydration energies of charged species is fraught with significant difficulties, which lead to unacceptably large (up to 300 %) variation in the available estimates of the CHA effect. We circumvent these difficulties by developing a framework which allows us to extract and accurately estimate the intrinsic propensity of water to exhibit CHA from accurate experimental hydration free energies of neutral polar molecules. Specifically, from a set of 504 small molecules we identify two pairs that are analogous, with respect to CHA, to the K+/F- pair -- a classical probe for the effect. We use these "CHA-conjugate" molecule pairs to quantify the intrinsic charge-asymmetric respon...

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

    Office of Scientific and Technical Information (OSTI)

    low andor high temperature performance, lifetime, safety, etc. which is achievable. The development within this project of a "looking glass" into the molecular interactions...

  20. 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...

  1. Solvation Effects on Free Energy Surface of Polyalanine

    E-Print Network [OSTI]

    G. Gokoglu; H. Arkin; E. Akturk; T. Celik

    2007-03-22

    We have simulated 10-residue polyalanine chain by multicanonical method to visualize the 3D topographic picture of the free energy landscape over the whole range of temperatures, hence to show the funnel along the folding pathway exhaustively. We have simulated and compared the system in vacuo and in solvent, and examined the changes in the free energy landscape due to the solvent effects, which are taken into account by commonly used model Accessible Surface Area.

  2. Electrolyte Solvation and Ionic Association. V. Acetonitrile-Lithium

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfate Reducing(Journal Article) | SciTech(Journal Article) |ContinuumPhotoactive

  3. Electrolyte Solvation and Ionic Association. VI. Acetonitrile-Lithium Salt

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfate Reducing(Journal Article) | SciTech(Journal Article) |ContinuumPhotoactiveMixtures: Highly

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

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfate Reducing(Journal Article) |production at aSciTech ConnectW49B (Journal(TechnicalElectrolyte

  5. Solvate Structures and Computational/Spectroscopic Characterization of

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfateSciTechtail. (Conference)Feedback System in the CERNimmobilize spent

  6. Structural Interactions within Lithium Salt Solvates: Acyclic Carbonates

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfateSciTechtail. (Conference)Feedback System inStatus of theSciTech Connect Book: Structuraland

  7. Linking Ion Solvation and Lithium Battery Electrolyte Properties |

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Home Page on Google Bookmark EERE: Alternative Fuels Data Center Home Page on Delicious RankADVANCED MANUFACTURING OFFICE INDUSTRIALU.S.Leadership on CleanUp GeorgiaLinac CoherentGeneration

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

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power Administration would likeUniverse (Journal Article) | SciTechSubmittedEcologistand9, 2013Electrolyte Properties

  9. Event-driven multithreaded dynamic optimization

    E-Print Network [OSTI]

    Zhang, Weifeng

    2006-01-01

    Speci?c Optimizations . . . . . . . . . . . . . F.3. Trace Optimization Overhead . . . . . . . . . . . . . . .Dynamic Optimization . . . . . . .B. Optimizations with the

  10. Dynamic models for nonstationary signal segmentation

    E-Print Network [OSTI]

    Penny, Will

    Dynamic models for nonstationary signal segmentation William D. Penny and Stephen J. Roberts w.penny

  11. Simple Dynamic Gasifier Model That Runs in Aspen Dynamics

    SciTech Connect (OSTI)

    Robinson, P.J.; Luyben, W.L. [Lehigh University, Bethlehem, PA (United States). Dept. of Chemical Engineering

    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.

  12. Ab-Initio Molecular Dynamics

    E-Print Network [OSTI]

    Thomas D. Kühne

    2013-03-26

    Computer simulation methods, such as Monte Carlo or Molecular Dynamics, are very powerful computational techniques that provide detailed and essentially exact information on classical many-body problems. With the advent of ab-initio molecular dynamics, where the forces are computed on-the-fly by accurate electronic structure calculations, the scope of either method has been greatly extended. This new approach, which unifies Newton's and Schr\\"odinger's equations, allows for complex simulations without relying on any adjustable parameter. This review is intended to outline the basic principles as well as a survey of the field. Beginning with the derivation of Born-Oppenheimer molecular dynamics, the Car-Parrinello method and the recently devised efficient and accurate Car-Parrinello-like approach to Born-Oppenheimer molecular dynamics, which unifies best of both schemes are discussed. The predictive power of this novel second-generation Car-Parrinello approach is demonstrated by a series of applications ranging from liquid metals, to semiconductors and water. This development allows for ab-initio molecular dynamics simulations on much larger length and time scales than previously thought feasible.

  13. Ab-Initio Molecular Dynamics

    E-Print Network [OSTI]

    Kühne, Thomas D

    2012-01-01

    Computer simulations and molecular dynamics in particular, is a very powerful method to provide detailed and essentially exact informations of classical many-body problems. With the advent of \\textit{ab-initio} molecular dynamics, where the forces are computed on-the-fly by accurate electronic structure calculations, the scope of either method has been greatly extended. This new approach, which unifies Newton's and Schr\\"odinger's equations, allows for complex simulations without relying on any adjustable parameter. This review is intended to outline the basic principles as well as a survey of the field. Beginning with the derivation of Born-Oppenheimer molecular dynamics, the Car-Parrinello method as well as novel hybrid scheme that unifies best of either approach are discussed. The predictive power is demonstrated by a series of applications ranging from insulators to semiconductors and even metals in condensed phases.

  14. Natural Dynamics for Combinatorial Optimization

    E-Print Network [OSTI]

    Ovchinnikov, Igor V

    2015-01-01

    Stochastic and or natural dynamical systems (DSs) are dominated by sudden nonlinear processes such as neuroavalanches, gamma-ray bursts, solar flares, earthquakes etc. that exhibit scale-free statistics. These behaviors also occur in many nanosystems. On phase diagrams, these DSs belong to a finite-width phase that separates the phases of thermodynamic equilibrium and ordinary chaotic dynamics, and that is known under such names as intermittency, noise-induced chaos, and self-organized criticality. Within the recently formulated approximation-free cohomological theory of stochastic differential equations, the noise-induced chaos can be roughly interpreted as a noise-induced overlap between regular (integrable) and chaotic (non-integrable) deterministic dynamics so that DSs in this phase inherit the properties of the both. Here, we analyze this unique set of properties and conclude that such DSs must be the most efficient natural optimizers. Based on this understanding, we propose the method of the natural dyn...

  15. Dynamics of Triaxial Stellar Systems

    E-Print Network [OSTI]

    David Merritt

    1996-11-11

    Recent work on the dynamics of triaxial stellar systems is reviewed. The motion of boxlike orbits in realistic triaxial potentials is generically stochastic. The degree to which the stochasticity manifests itself in the dynamics depends on the chaotic mixing timescale, which is a small multiple of the crossing time in triaxial models with steep cusps or massive central singularities. Low-luminosity ellipticals, which have the steepest cusps and the shortest dynamical times, are less likely than bright ellipticals to have strongly triaxial shapes. The observational evidence for triaxiality is reviewed; departures from axisymmetry in early-type galaxies are often found to be associated with evidence of recent interactions or with the presence of a bar.

  16. Plasticity of metal wires in torsion: molecular dynamics and dislocation dynamics simulations

    E-Print Network [OSTI]

    Cai, Wei

    Plasticity of metal wires in torsion: molecular dynamics and dislocation dynamics simulations-4040 Abstract The orientation dependent plasticity in metal nanowires is investigated using molecular dynamics metal wires controls the mechanisms of plastic deformation. For wires oriented along 110 , dislocations

  17. 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.

  18. Theoretical studies of combustion dynamics

    SciTech Connect (OSTI)

    Bowman, J.M. [Emory Univ., Atlanta, GA (United States)

    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.

  19. Statistics as a dynamical attractor

    E-Print Network [OSTI]

    Michail Zak

    2012-08-30

    It is demonstrated that any statistics can be represented by an attractor of the solution to a corresponding systen of ODE coupled with its Liouville equation. Such a non-Newtonian representation allows one to reduce foundations of statistics to better established foundations of ODE. In addition to that, evolution to the attractor reveals possible micro-mechanisms driving random events to the final distribution of the corresponding statistical law. Special attention is concentrated upon the power law and its dynamical interpretation: it is demonstrated that the underlying dynamics supports a " violent reputation" of the power law statistics.

  20. Dynamics of Protein Hydration Water

    E-Print Network [OSTI]

    M. Wolf; S. Emmert; R. Gulich; P. Lunkenheimer; A. Loidl

    2014-12-08

    We present the frequency- and temperature-dependent dielectric properties of lysozyme solutions in a broad concentration regime, measured at subzero temperatures and compare the results with measurements above the freezing point of water and on hydrated lysozyme powder. Our experiments allow examining the dynamics of unfreezable hydration water in a broad temperature range including the so-called No Man's Land (160 - 235 K). The obtained results prove the bimodality of the hydration shell dynamics and are discussed in the context of the highly-debated fragile-to-strong transition of water.