Krykunov, Mykhaylo; Seth, Mike; Ziegler, Tom [Department of Chemistry, University of Calgary, University Drive 2500, Calgary, Alberta T2N 1N4 (Canada)] [Department of Chemistry, University of Calgary, University Drive 2500, Calgary, Alberta T2N 1N4 (Canada)
2014-05-14T23:59:59.000Z
We have applied the relaxed and self-consistent extension of constricted variational density functional theory (RSCF-CV-DFT) for the calculation of the lowest charge transfer transitions in the molecular complex X-TCNE between X = benzene and TCNE = tetracyanoethylene. Use was made of functionals with a fixed fraction (?) of Hartree-Fock exchange ranging from ? = 0 to ? = 0.5 as well as functionals with a long range correction (LC) that introduces Hartree-Fock exchange for longer inter-electronic distances. A detailed comparison and analysis is given for each functional between the performance of RSCF-CV-DFT and adiabatic time-dependent density functional theory (TDDFT) within the Tamm-Dancoff approximation. It is shown that in this particular case, all functionals afford the same reasonable agreement with experiment for RSCF-CV-DFT whereas only the LC-functionals afford a fair agreement with experiment using TDDFT. We have in addition calculated the CT transition energy for X-TCNE with X = toluene, o-xylene, and naphthalene employing the same functionals as for X = benzene. It is shown that the calculated charge transfer excitation energies are in as good agreement with experiment as those obtained from highly optimized LC-functionals using adiabatic TDDFT. We finally discuss the relation between the optimization of length separation parameters and orbital relaxation in the RSCF-CV-DFT scheme.
Kevin Leung; Susan B. Rempe; Peter A. Schultz; Eduardo M. Sproviero; Victor S. Batista; Michael E. Chandross; Craig J. Medforth
2006-10-26T23:59:59.000Z
We apply Density Functional Theory (DFT) and the DFT+U technique to study the adsorption of transition metal porphine molecules on atomistically flat Au(111) surfaces. DFT calculations using the Perdew-Burke-Ernzerhof (PBE) exchange correlation functional correctly predict the palladium porphine (PdP) low-spin ground state. PdP is found to adsorb preferentially on gold in a flat geometry, not in an edgewise geometry, in qualitative agreement with experiments on substituted porphyrins. It exhibits no covalent bonding to Au(111), and the binding energy is a small fraction of an eV. The DFT+U technique, parameterized to B3LYP predicted spin state ordering of the Mn d-electrons, is found to be crucial for reproducing the correct magnetic moment and geometry of the isolated manganese porphine (MnP) molecule. Adsorption of Mn(II)P on Au(111) substantially alters the Mn ion spin state. Its interaction with the gold substrate is stronger and more site-specific than PdP. The binding can be partially reversed by applying an electric potential, which leads to significant changes in the electronic and magnetic properties of adsorbed MnP, and ~ 0.1 Angstrom, changes in the Mn-nitrogen distances within the porphine macrocycle. We conjecture that this DFT+U approach may be a useful general method for modeling first row transition metal ion complexes in a condensed-matter setting.
Burns, Lori A [ORNL; Sherrill, David [Georgia Institute of Technology; Vazquez-Mayagoitia, Alvaro [ORNL; Sumpter, Bobby G [ORNL
2011-01-01T23:59:59.000Z
A systematic study of techniques for treating non-covalent interactions within the computationally efficient density functional theory (DFT) framework is presented through comparison to benchmark-quality evaluations of binding strength com- piled for molecular complexes of diverse size and nature. In particular, the effi- cacy of functionals deliberately crafted to encompass long-range forces, a posteri- ori DFT+dispersion corrections (DFT-D2 and DFT-D3), and exchange-hole dipole moment (XDM) theory is assessed against a large collection (469 energy points) of reference interaction energies at the CCSD(T) level of theory extrapolated to the estimated complete basis set limit. The established S22 and JSCH test sets of minimum-energy structures, as well as collections of dispersion-bound (NBC10) and hydrogen-bonded (HBC6) dissociation curves and a pairwise decomposition of a protein-ligand reaction site (HSG), comprise the chemical systems for this work. From evaluations of accuracy, consistency, and efficiency for PBE-D, BP86-D, B97-D, PBE0-D, B3LYP-D, B970-D, M05-2X, M06-2X, B97X-D, B2PLYP-D, XYG3, and B3LYP-XDM methodologies, it is concluded that distinct, often contrasting, groups of these elicit the best performance within the accessible double- or robust triple- basis set regimes and among hydrogen-bonded or dispersion-dominated complexes. For overall results, M05-2X, B97-D3, and B970-D2 yield superior values in conjunc- tion with aug-cc-pVDZ, for a mean absolute deviation of 0.41 0.49 kcal/mol, and B3LYP-D3, B97-D3, B97X-D, and B2PLYP-D3 dominate with aug-cc-pVTZ, af- fording, together with XYG3/6-311+G(3df,2p), a mean absolute deviation of 0.33 0.38 kcal/mol.
Error Analysis in Nuclear Density Functional Theory
Nicolas Schunck; Jordan D. McDonnell; Jason Sarich; Stefan M. Wild; Dave Higdon
2014-07-11T23:59:59.000Z
Nuclear density functional theory (DFT) is the only microscopic, global approach to the structure of atomic nuclei. It is used in numerous applications, from determining the limits of stability to gaining a deep understanding of the formation of elements in the universe or the mechanisms that power stars and reactors. The predictive power of the theory depends on the amount of physics embedded in the energy density functional as well as on efficient ways to determine a small number of free parameters and solve the DFT equations. In this article, we discuss the various sources of uncertainties and errors encountered in DFT and possible methods to quantify these uncertainties in a rigorous manner.
Jain, Anubhav, Ph.D. Massachusetts Institute of Technology
2011-01-01T23:59:59.000Z
This thesis relates to the emerging field of high-throughput density functional theory (DFT) computation for materials design and optimization. Although highthroughput DFT is a promising new method for materials discovery, ...
Charge transport, configuration interaction and Rydberg states under density functional theory
Cheng, Chiao-Lun
2008-01-01T23:59:59.000Z
Density functional theory (DFT) is a computationally efficient formalism for studying electronic structure and dynamics. In this work, we develop DFT-based excited-state methods to study electron transport, Rydberg excited ...
Density Functional Theory (DFT) Simulated Annealing (SA)
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Bjørnstad, Ottar Nordal
Stability of titanium oxide phases in Kohn-Sham density functional theory A well known problem of stability of titanium oxide phases at room temperature. That is, anatase instead of rutile is predicted as the room temperature phase for titanium oxide. In this work we try to establish the reasons
Yeo, Sang Chul
Ammonia (NH[subscript 3]) nitridation on an Fe surface was studied by combining density functional theory (DFT) and kinetic Monte Carlo (kMC) calculations. A DFT calculation was performed to obtain the energy barriers ...
Progress at the interface of wave-function and density-functional theories
Gidopoulos, Nikitas I. [ISIS, Rutherford Appleton Laboratory, STFC, Didcot, OX11 0QX, Oxon (United Kingdom)
2011-04-15T23:59:59.000Z
The Kohn-Sham (KS) potential of density-functional theory (DFT) emerges as the minimizing effective potential in a variational scheme that does not involve fixing the unknown single-electron density. Using Rayleigh Schroedinger (RS) perturbation theory (PT), we construct ab initio approximations for the energy difference, the minimization of which determines the KS potential directly - thereby bypassing DFT's traditional algorithm to search for the density that minimizes the total energy. From second-order RS PT, we obtain variationally stable energy differences to be minimized, solving the severe problem of variational collapse of orbital-dependent exchange-correlation functionals based on second-order RS PT.
Rabani, Eran
Communication: Embedded fragment stochastic density functional theory Daniel Neuhauser, Roi Baer (2014) Communication: Embedded fragment stochastic density functional theory Daniel Neuhauser,1,a) RoiÂ18 Recently, we formulated KS-DFT as a statistical theory in which the electron density is determined from
Density functional theory based generalized effective fragment potential method
Nguyen, Kiet A., E-mail: kiet.nguyen@wpafb.af.mil, E-mail: ruth.pachter@wpafb.af.mil [Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433 (United States); UES, Inc., Dayton, Ohio 45432 (United States); Pachter, Ruth, E-mail: kiet.nguyen@wpafb.af.mil, E-mail: ruth.pachter@wpafb.af.mil [Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433 (United States); Day, Paul N. [Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433 (United States); General Dynamics Information Technology, Inc., Dayton, Ohio 45431 (United States)
2014-06-28T23:59:59.000Z
We present a generalized Kohn-Sham (KS) density functional theory (DFT) based effective fragment potential (EFP2-DFT) method for the treatment of solvent effects. Similar to the original Hartree-Fock (HF) based potential with fitted parameters for water (EFP1) and the generalized HF based potential (EFP2-HF), EFP2-DFT includes electrostatic, exchange-repulsion, polarization, and dispersion potentials, which are generated for a chosen DFT functional for a given isolated molecule. The method does not have fitted parameters, except for implicit parameters within a chosen functional and the dispersion correction to the potential. The electrostatic potential is modeled with a multipolar expansion at each atomic center and bond midpoint using Stone's distributed multipolar analysis. The exchange-repulsion potential between two fragments is composed of the overlap and kinetic energy integrals and the nondiagonal KS matrices in the localized molecular orbital basis. The polarization potential is derived from the static molecular polarizability. The dispersion potential includes the intermolecular D3 dispersion correction of Grimme et al. [J. Chem. Phys. 132, 154104 (2010)]. The potential generated from the CAMB3LYP functional has mean unsigned errors (MUEs) with respect to results from coupled cluster singles, doubles, and perturbative triples with a complete basis set limit (CCSD(T)/CBS) extrapolation, of 1.7, 2.2, 2.0, and 0.5 kcal/mol, for the S22, water-benzene clusters, water clusters, and n-alkane dimers benchmark sets, respectively. The corresponding EFP2-HF errors for the respective benchmarks are 2.41, 3.1, 1.8, and 2.5 kcal/mol. Thus, the new EFP2-DFT-D3 method with the CAMB3LYP functional provides comparable or improved results at lower computational cost and, therefore, extends the range of applicability of EFP2 to larger system sizes.
Propagation of uncertainties in the nuclear DFT models
Markus Kortelainen
2014-09-04T23:59:59.000Z
Parameters of the nuclear density functional theory (DFT) models are usually adjusted to experimental data. As a result they carry certain theoretical error, which, as a consequence, carries out to the predicted quantities. In this work we address the propagation of theoretical error, within the nuclear DFT models, from the model parameters to the predicted observables. In particularly, the focus is set on the Skyrme energy density functional models.
Subsystem real-time Time Dependent Density Functional Theory
Krishtal, Alisa; Pavanello, Michele
2015-01-01T23:59:59.000Z
We present the extension of Frozen Density Embedding (FDE) theory to real-time Time Dependent Density Functional Theory (rt-TDDFT). FDE a is DFT-in-DFT embedding method that allows to partition a larger Kohn-Sham system into a set of smaller, coupled Kohn-Sham systems. Additional to the computational advantage, FDE provides physical insight into the properties of embedded systems and the coupling interactions between them. The extension to rt-TDDFT is done straightforwardly by evolving the Kohn-Sham subsystems in time simultaneously, while updating the embedding potential between the systems at every time step. Two main applications are presented: the explicit excitation energy transfer in real time between subsystems is demonstrated for the case of the Na$_4$ cluster and the effect of the embedding on optical spectra of coupled chromophores. In particular, the importance of including the full dynamic response in the embedding potential is demonstrated.
Density Functional Resonance Theory of Unbound Electronic Systems
Daniel L. Whitenack; Adam Wasserman
2011-06-20T23:59:59.000Z
Density Functional Resonance Theory (DFRT) is a complex-scaled version of ground-state Density Functional Theory (DFT) that allows one to calculate the resonance energies and lifetimes of metastable anions. In this formalism, the exact energy and lifetime of the lowest-energy resonance of unbound systems is encoded into a complex "density" that can be obtained via complex-coordinate scaling. This complex density is used as the primary variable in a DFRT calculation just as the ground-state density would be used as the primary variable in DFT. As in DFT, there exists a mapping of the N-electron interacting system to a Kohn-Sham system of N non-interacting particles in DFRT. This mapping facilitates self consistent calculations with an initial guess for the complex density, as illustrated with an exactly-solvable model system. Whereas DFRT yields in principle the exact resonance energy and lifetime of the interacting system, we find that neglecting the complex-correlation contribution leads to errors of similar magnitude to those of standard scattering close-coupling calculations under the bound-state approximation.
Kummel, Andrew C.
A density functional theory study of the correlation between analyte basicity, ZnPc adsorption Received 4 January 2009; accepted 27 April 2009; published online 28 May 2009 Density functional theory DFT of their electron donating ability or Lewis basicity. With the exception of the most basic analyte investigated
Density functional theory study of mercury adsorption on metal surfaces
Steckel, J.A.
2008-01-01T23:59:59.000Z
Density functional theory #1;DFT#2; calculations are used to characterize the interaction of mercury with copper, nickel, palladium, platinum, silver, and gold surfaces. Mercury binds relatively strongly to all the metal surfaces studied, with binding energies up to #3;1 eV for Pt and Pd. DFT calculations underestimate the energy of adsorption with respect to available experimental data. Plane-wave DFT results using the local density approximation and the Perdew-Wang 1991 and Perdew-Burke-Ernzerhof parametrizations of the generalized gradient approximation indicate that binding of mercury at hollow sites is preferred over binding at top or bridge sites. The interaction with mercury in order of increasing reactivity over the six metals studied is Ag #1;Au#1;Cu#1;Ni#1;Pt#1;Pd. Binding is stronger on the #1;001#2; faces of the metal surfaces, where mercury is situated in fourfold hollow sites as opposed to the threefold hollow sites on #1;111#2; faces. In general, mercury adsorption leads to decreases in the work function; adsorbate-induced work function changes are particularly dramatic on Pt.
Density Functional Theory investigations of titanium gamma-surfaces and stacking faults
Benoit, Magali; Morillo, Joseph
2015-01-01T23:59:59.000Z
Properties of hcp-Ti such as elastic constants, stacking faults and gamma-surfaces are computed using Density Functional Theory (DFT) and two central force Embedded Atom interaction Models (EAM). The results are compared to previously published calculations and to predicting models. Their implications on the plastic properties of hcp-Ti are discussed.
Solovyeva, Alisa [Gorlaeus Laboratories, Leiden Institute of Chemistry, Leiden University, P.O. Box 9502, 2300 RA Leiden (Netherlands); Technical University Braunschweig, Institute for Physical and Theoretical Chemistry, Hans-Sommer-Str. 10, 38106 Braunschweig (Germany); Pavanello, Michele [Gorlaeus Laboratories, Leiden Institute of Chemistry, Leiden University, P.O. Box 9502, 2300 RA Leiden (Netherlands); Neugebauer, Johannes [Technical University Braunschweig, Institute for Physical and Theoretical Chemistry, Hans-Sommer-Str. 10, 38106 Braunschweig (Germany)
2012-05-21T23:59:59.000Z
Subsystem density-functional theory (DFT) is a powerful and efficient alternative to Kohn-Sham DFT for large systems composed of several weakly interacting subunits. Here, we provide a systematic investigation of the spin-density distributions obtained in subsystem DFT calculations for radicals in explicit environments. This includes a small radical in a solvent shell, a {pi}-stacked guanine-thymine radical cation, and a benchmark application to a model for the special pair radical cation, which is a dimer of bacteriochlorophyll pigments, from the photosynthetic reaction center of purple bacteria. We investigate the differences in the spin densities resulting from subsystem DFT and Kohn-Sham DFT calculations. In these comparisons, we focus on the problem of overdelocalization of spin densities due to the self-interaction error in DFT. It is demonstrated that subsystem DFT can reduce this problem, while it still allows to describe spin-polarization effects crossing the boundaries of the subsystems. In practical calculations of spin densities for radicals in a given environment, it may thus be a pragmatic alternative to Kohn-Sham DFT calculations. In our calculation on the special pair radical cation, we show that the coordinating histidine residues reduce the spin-density asymmetry between the two halves of this system, while inclusion of a larger binding pocket model increases this asymmetry. The unidirectional energy transfer in photosynthetic reaction centers is related to the asymmetry introduced by the protein environment.
Ceder, Gerbrand
We compare the accuracy of conventional semilocal density functional theory (DFT), the DFT+U method, and the Heyd-Scuseria-Ernzerhof (HSE06) hybrid functional for structural parameters, redox reaction energies, and formation ...
Quantification of Uncertainties in Nuclear Density Functional theory
N. Schunck; J. D. McDonnell; D. Higdon; J. Sarich; S. Wild
2014-09-17T23:59:59.000Z
Reliable predictions of nuclear properties are needed as much to answer fundamental science questions as in applications such as reactor physics or data evaluation. Nuclear density functional theory is currently the only microscopic, global approach to nuclear structure that is applicable throughout the nuclear chart. In the past few years, a lot of effort has been devoted to setting up a general methodology to assess theoretical uncertainties in nuclear DFT calculations. In this paper, we summarize some of the recent progress in this direction. Most of the new material discussed here will be be published in separate articles.
Tuning Range-Separated Density Functional Theory for Photocatalytic Water Splitting Systems
Bokareva, Olga S; Bokarev, Sergey I; Kühn, Oliver
2015-01-01T23:59:59.000Z
We discuss the applicability of long-range separated density functional theory (DFT) to the prediction of electronic transitions of a particular photocatalytic system based on an Ir(III) photosensitizer (IrPS). Special attention is paid to the charge-transfer properties which are of key importance for the photoexcitation dynamics, but and cannot be correctly described by means of conventional DFT. The optimization of the range-separation parameter is discussed for IrPS including its complexes with electron donors and acceptors used in photocatalysis. Particular attention is paid to the problems arising for a description of medium effects by a polarizable continuum model.
Time Dependent Density Functional Theory An introduction
Botti, Silvana
Time Dependent Density Functional Theory An introduction Francesco Sottile LSI, Ecole Polytechnique (ETSF) Time Dependent Density Functional Theory Palaiseau, 7 February 2012 1 / 32 #12;Outline 1 Frontiers 4 Perspectives and Resources Francesco Sottile (ETSF) Time Dependent Density Functional Theory
Bankura, Arindam; DiStasio, Robert A; Swartz, Charles W; Klein, Michael L; Wu, Xifan
2015-01-01T23:59:59.000Z
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...
Temperature Dependent Magnon-Phonon Coupling in bcc Fe from Theory and Experiment
Tai, Yu-Chong
- actions in bcc Fe. Parameter-free electronic structure calculations like den- sity functional theory (DFT moments (DLM) molecular dynamics [1], magnetic empirical poten- tials [2
Batista, Victor S. (Yale University, New Haven, CT); Chandross, Michael Evan; Leung, Kevin; Sporviero, Eduardo (Yale University, New Haven, CT); Schultz, Peter Andrew; Rempe, Susan B.
2005-06-01T23:59:59.000Z
We apply density functional theory (DFT) and the DFT+U technique to study the adsorption of transition metal porphine molecules on atomistically flat Au(111) surfaces. DFT calculations using the Perdew?Burke?Ernzerhof exchange correlation functional correctly predict the palladium porphine (PdP) low-spin ground state. PdP is found to adsorb preferentially on gold in a flat geometry, not in an edgewise geometry, in qualitative agreement with experiments on substituted porphyrins. It exhibits no covalent bonding to Au(111), and the binding energy is a small fraction of an electronvolt. The DFT+U technique, parametrized to B3LYP-predicted spin state ordering of the Mn d-electrons, is found to be crucial for reproducing the correct magnetic moment and geometry of the isolated manganese porphine (MnP) molecule. Adsorption of Mn(II)P on Au(111) substantially alters the Mn ion spin state. Its interaction with the gold substrate is stronger and more site-specific than that of PdP. The binding can be partially reversed by applying an electric potential, which leads to significant changes in the electronic and magnetic properties of adsorbed MnP and 0.1 {angstrom} changes in the Mn-nitrogen distances within the porphine macrocycle. We conjecture that this DFT+U approach may be a useful general method for modeling first-row transition metal ion complexes in a condensed-matter setting.
Wide range equation of state for fluid hydrogen from density functional theory
Wang, Cong; Zhang, Ping [Institute of Applied Physics and Computational Mathematics, P.O. Box 8009, Beijing 100088 (China) [Institute of Applied Physics and Computational Mathematics, P.O. Box 8009, Beijing 100088 (China); Center for Applied Physics and Technology, Peking University, Beijing 100871 (China)
2013-09-15T23:59:59.000Z
Wide range equation of state (EOS) for liquid hydrogen is ultimately obtained by combining two kinds of density functional theory (DFT) molecular dynamics simulations, namely, first-principles molecular dynamics simulations and orbital-free molecular dynamics simulations. Specially, the present introduction of short cutoff radius pseudopotentials enables the EOS to be available in the range from 9.82 × 10{sup ?4} to 1.347 × 10{sup 3} g/cm{sup 3} and up to 5 × 10{sup 7} K. By comprehensively comparing with various attainable experimental and theoretical data, we derive the conclusion that our DFT-EOS can be readily and reliably applied to hydrodynamic simulations of the inertial confinement fusion.
Fast plane wave density functional theory molecular dynamics calculations on multi-GPU machines
Jia, Weile, E-mail: jiawl@sccas.cn [Supercomputing Center, Computer Network Information Center, Chinese Academy of Sciences, No. 4 South 4th Street, ZhongGuanCun, Beijing 100190 (China) [Supercomputing Center, Computer Network Information Center, Chinese Academy of Sciences, No. 4 South 4th Street, ZhongGuanCun, Beijing 100190 (China); University of Chinese Academy of Sciences, Beijing (China); Fu, Jiyun, E-mail: fujy@sccas.cn [Supercomputing Center, Computer Network Information Center, Chinese Academy of Sciences, No. 4 South 4th Street, ZhongGuanCun, Beijing 100190 (China) [Supercomputing Center, Computer Network Information Center, Chinese Academy of Sciences, No. 4 South 4th Street, ZhongGuanCun, Beijing 100190 (China); University of Chinese Academy of Sciences, Beijing (China); Cao, Zongyan, E-mail: zycao@sccas.cn [Supercomputing Center, Computer Network Information Center, Chinese Academy of Sciences, No. 4 South 4th Street, ZhongGuanCun, Beijing 100190 (China)] [Supercomputing Center, Computer Network Information Center, Chinese Academy of Sciences, No. 4 South 4th Street, ZhongGuanCun, Beijing 100190 (China); Wang, Long, E-mail: wangl@sccas.cn [Supercomputing Center, Computer Network Information Center, Chinese Academy of Sciences, No. 4 South 4th Street, ZhongGuanCun, Beijing 100190 (China)] [Supercomputing Center, Computer Network Information Center, Chinese Academy of Sciences, No. 4 South 4th Street, ZhongGuanCun, Beijing 100190 (China); Chi, Xuebin, E-mail: chi@sccas.cn [Supercomputing Center, Computer Network Information Center, Chinese Academy of Sciences, No. 4 South 4th Street, ZhongGuanCun, Beijing 100190 (China)] [Supercomputing Center, Computer Network Information Center, Chinese Academy of Sciences, No. 4 South 4th Street, ZhongGuanCun, Beijing 100190 (China); Gao, Weiguo, E-mail: wggao@fudan.edu.cn [School of Mathematical Sciences, Fudan University, 220 Handan Road, Shanghai 200433 (China) [School of Mathematical Sciences, Fudan University, 220 Handan Road, Shanghai 200433 (China); MOE Key Laboratory of Computational Physical Sciences, Fudan University, Shanghai (China); Wang, Lin-Wang, E-mail: lwwang@lbl.gov [Material Science Division, Lawrence Berkeley National Laboratory, One Cyclotron Road Mail Stop 50F Berkeley, CA 94720 (United States)] [Material Science Division, Lawrence Berkeley National Laboratory, One Cyclotron Road Mail Stop 50F Berkeley, CA 94720 (United States)
2013-10-15T23:59:59.000Z
Plane wave pseudopotential (PWP) density functional theory (DFT) calculation is the most widely used method for material simulations, but its absolute speed stagnated due to the inability to use large scale CPU based computers. By a drastic redesign of the algorithm, and moving all the major computation parts into GPU, we have reached a speed of 12 s per molecular dynamics (MD) step for a 512 atom system using 256 GPU cards. This is about 20 times faster than the CPU version of the code regardless of the number of CPU cores used. Our tests and analysis on different GPU platforms and configurations shed lights on the optimal GPU deployments for PWP-DFT calculations. An 1800 step MD simulation is used to study the liquid phase properties of GaInP.
Uncertainty Quantification for Nuclear Density Functional Theory...
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Arindam Bankura; Biswajit Santra; Robert A. DiStasio Jr.; Charles W. Swartz; Michael L. Klein; Xifan Wu
2015-03-25T23:59:59.000Z
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.
Time Dependent Density Functional Theory An Introduction
Botti, Silvana
Time Dependent Density Functional Theory An Introduction Francesco Sottile Laboratoire des Solides) Belfast, 29 Jun 2007 Time Dependent Density Functional Theory Francesco Sottile #12;Intro Formalism Linear Response Formalism 3 TDDFT in practice: The ALDA: Achievements and Shortcomings 4 Resources Time
Jacek Dobaczewski Density functional theory and energy
Dobaczewski, Jacek
in Poland per voivodship Energy density functional 245 647 Price voivodship functional 654 763 295 580Jacek Dobaczewski Density functional theory and energy density functionals in nuclear physics Jacek://www.fuw.edu.pl/~dobaczew/Stellenbosch/dobaczewski_lecture.pdf Home page: http://www.fuw.edu.pl/~dobaczew/ #12;Jacek Dobaczewski Nuclear Structure Energy scales
SCALING RELATIONS IN DENSITY FUNCTIONAL THEORY AND
Burke, Kieron
are being made to apply DFT to systems of bio- logical interest that would otherwise be unfeasible with traditional wavefunction methods. Although much of present research in DFT development focuses on an extension to the study of models for organometallic catalysts used in the dehydrogenation of alkanes to form alkenes
Ferromagnetism in GaN: Gd: A density functional theory study
Stevenson, Cynthia; Stevenson, Cynthia
2008-02-04T23:59:59.000Z
First principle calculations of the electronic structure and magnetic interaction of GaN:Gd have been performed within the Generalized Gradient Approximation (GGA) of the density functional theory (DFT) with the on-site Coulomb energy U taken into account (also referred to as GGA+U). The ferromagnetic p-d coupling is found to be over two orders of magnitude larger than the s-d exchange coupling. The experimental colossal magnetic moments and room temperature ferromagnetism in GaN:Gd reported recently are explained by the interaction of Gd 4f spins via p-d coupling involving holes introduced by intrinsic defects such as Ga vacancies.
Verma, Prakash; Bartlett, Rodney J., E-mail: bartlett@ufl.edu [Quantum Theory Project, University of Florida, Gainesville, Florida 32611 (United States)
2014-05-14T23:59:59.000Z
This paper's objective is to create a “consistent” mean-field based Kohn-Sham (KS) density functional theory (DFT) meaning the functional should not only provide good total energy properties, but also the corresponding KS eigenvalues should be accurate approximations to the vertical ionization potentials (VIPs) of the molecule, as the latter condition attests to the viability of the exchange-correlation potential (V{sub XC}). None of the prominently used DFT approaches show these properties: the optimized effective potential V{sub XC} based ab initio dft does. A local, range-separated hybrid potential cam-QTP-00 is introduced as the basis for a “consistent” KS DFT approach. The computed VIPs as the negative of KS eigenvalue have a mean absolute error of 0.8 eV for an extensive set of molecule's electron ionizations, including the core. Barrier heights, equilibrium geometries, and magnetic properties obtained from the potential are in good agreement with experiment. A similar accuracy with less computational efforts can be achieved by using a non-variational global hybrid variant of the QTP-00 approach.
Burke, Kieron
Semiclassical Origins of Density Functionals Peter Elliott, Donghyung Lee, Attila Cangi, and Kieron world of pure density functional theory (DFT), i.e., Thomas-Fermi (TF) and related theories
Functional Integration for Quantum Field Theory
J. LaChapelle
2006-10-16T23:59:59.000Z
The functional integration scheme for path integrals advanced by Cartier and DeWitt-Morette is extended to the case of fields. The extended scheme is then applied to quantum field theory. Several aspects of the construction are discussed.
Santra, Biswajit; Tkatchenko, Alexandre; Alfè, Dario; Slater, Ben; Michaelides, Angelos; Car, Roberto; Scheffler, Matthias
2013-01-01T23:59:59.000Z
Density-functional theory (DFT) has been widely used to study water and ice for at least 20 years. However, the reliability of different DFT exchange-correlation (xc) functionals for water remains a matter of considerable debate. This is particularly true in light of the recent development of DFT based methods that account for van der Waals (vdW) dispersion forces. Here, we report a detailed study with several xc functionals (semi-local, hybrid, and vdW inclusive approaches) on ice Ih and six proton ordered phases of ice. Consistent with our previous study [Phys. Rev. Lett. 107, 185701 (2011)] which showed that vdW forces become increasingly important at high pressures, we find here that all vdW inclusive methods considered improve the relative energies and transition pressures of the high-pressure ice phases compared to those obtained with semi-local or hybrid xc functionals. However, we also find that significant discrepancies between experiment and the vdW inclusive approaches remain in the cohesive proper...
Biswajit Santra; Ji?í Klimeš; Alexandre Tkatchenko; Dario Alfè; Ben Slater; Angelos Michaelides; Roberto Car; Matthias Scheffler
2014-08-14T23:59:59.000Z
Density-functional theory (DFT) has been widely used to study water and ice for at least 20 years. However, the reliability of different DFT exchange-correlation (xc) functionals for water remains a matter of considerable debate. This is particularly true in light of the recent development of DFT based methods that account for van der Waals (vdW) dispersion forces. Here, we report a detailed study with several xc functionals (semi-local, hybrid, and vdW inclusive approaches) on ice Ih and six proton ordered phases of ice. Consistent with our previous study [Phys. Rev. Lett. 107, 185701 (2011)] which showed that vdW forces become increasingly important at high pressures, we find here that all vdW inclusive methods considered improve the relative energies and transition pressures of the high-pressure ice phases compared to those obtained with semi-local or hybrid xc functionals. However, we also find that significant discrepancies between experiment and the vdW inclusive approaches remain in the cohesive properties of the various phases, causing certain phases to be absent from the phase diagram. Therefore, room for improvement in the description of water at ambient and high pressures remains and we suggest that because of the stern test the high pressure ice phases pose they should be used in future benchmark studies of simulation methods for water.
Van der Waals density-functional theory study for bulk solids with BCC, FCC, and diamond structures
Park, Jinwoo; Hong, Suklyun
2015-01-01T23:59:59.000Z
Proper inclusion of van der Waals (vdW) interactions in theoretical simulations based on standard density functional theory (DFT) is crucial to describe the physics and chemistry of systems such as organic and layered materials. Many encouraging approaches have been proposed to combine vdW interactions with standard approximate DFT calculations. Despite many vdW studies, there is no consensus on the reliability of vdW methods. To help further development of vdW methods, we have assessed various vdW functionals through the calculation of structural prop- erties at equilibrium, such as lattice constants, bulk moduli, and cohesive energies, for bulk solids, including alkali, alkali-earth, and transition metals, with BCC, FCC, and diamond structures as the ground state structure. These results provide important information for the vdW-related materials research, which is essential for designing and optimizing materials systems for desired physical and chemical properties.
About density functional theory interpretation
Kirill Koshelev
2015-05-28T23:59:59.000Z
Two forms of relativistic density functional are derived from Dirac equation. Based on their structure analysis model of split electron is proposed. In this model electric charge and mass of electron behave like two point-like particles. It is shown that two electrons obeying this model cannot occupy the same quantum state. Empirical verification of the model is discussed.
Magnetic fields and density functional theory
Salsbury Jr., Freddie
1999-02-01T23:59:59.000Z
A major focus of this dissertation is the development of functionals for the magnetic susceptibility and the chemical shielding within the context of magnetic field density functional theory (BDFT). These functionals depend on the electron density in the absence of the field, which is unlike any other treatment of these responses. There have been several advances made within this theory. The first of which is the development of local density functionals for chemical shieldings and magnetic susceptibilities. There are the first such functionals ever proposed. These parameters have been studied by constructing functionals for the current density and then using the Biot-Savart equations to obtain the responses. In order to examine the advantages and disadvantages of the local functionals, they were tested numerically on some small molecules.
Hexakis(4-phormylphenoxy)cyclotriphosphazene: X-ray and DFT-calculated structures
Albayrak, Cigdem, E-mail: calbayrak@sinop.edu.tr; Kosar, Basak [Sinop University, Faculty of Education (Turkey); Odabasoglu, Mustafa [Pamukkale University, Chemical Technology Program (Turkey); Bueyuekguengoer, Orhan [Ondokuz Mayis University, Faculty of Arts and Sciences (Turkey)
2010-12-15T23:59:59.000Z
The crystal structure of hexakis(4-phormylphenoxy)cyclotriphosphazene is determined by using X-ray diffraction and then the molecular structure is investigated with density functional theory (DFT). X-Ray study shows that the title compound has C-H-{pi} interaction with phosphazene ring. The molecules in the unit cell are packed with Van der Waals and dipole-dipole interactions and the molecules are packed in zigzag shaped. Optimized molecular geometry is calculated with DFT at B3LYP/6-311G(d,p) level. The results from both experimental and theoretical calculations are compared in this study.
Density Functional Theory Study of Oxygen Reduction Activity...
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Density Functional Theory Study of Oxygen Reduction Activity on Ultrathin Platinum Nanotubes. Density Functional Theory Study of Oxygen Reduction Activity on Ultrathin Platinum...
A Density Functional Theory Study of Formaldehyde Adsorption...
Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)
Density Functional Theory Study of Formaldehyde Adsorption on Ceria. A Density Functional Theory Study of Formaldehyde Adsorption on Ceria. Abstract: Molecular adsorption of...
Density functional theory for carbon dioxide crystal
Chang, Yiwen; Mi, Jianguo, E-mail: mijg@mail.buct.edu.cn; Zhong, Chongli [State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029 (China)
2014-05-28T23:59:59.000Z
We present a density functional approach to describe the solid?liquid phase transition, interfacial and crystal structure, and properties of polyatomic CO{sub 2}. Unlike previous phase field crystal model or density functional theory, which are derived from the second order direct correlation function, the present density functional approach is based on the fundamental measure theory for hard-sphere repulsion in solid. More importantly, the contributions of enthalpic interactions due to the dispersive attractions and of entropic interactions arising from the molecular architecture are integrated in the density functional model. Using the theoretical model, the predicted liquid and solid densities of CO{sub 2} at equilibrium triple point are in good agreement with the experimental values. Based on the structure of crystal-liquid interfaces in different planes, the corresponding interfacial tensions are predicted. Their respective accuracies need to be tested.
Fragment Approach to Constrained Density Functional Theory Calculations using Daubechies Wavelets
Ratcliff, Laura E; Mohr, Stephan; Deutsch, Thierry
2015-01-01T23:59:59.000Z
In a recent paper we presented a linear scaling Kohn-Sham density functional theory (DFT) code based on Daubechies wavelets, where a minimal set of localized support functions is optimized in situ and therefore adapted to the chemical properties of the molecular system. Thanks to the systematically controllable accuracy of the underlying basis set, this approach is able to provide an optimal contracted basis for a given system: accuracies for ground state energies and atomic forces are of the same quality as an uncontracted, cubic scaling approach. This basis set offers, by construction, a natural subset where the density matrix of the system can be projected. In this paper we demonstrate the flexibility of this minimal basis formalism in providing a basis set that can be reused as-is, i.e. without reoptimization, for charge-constrained DFT calculations within a fragment approach. Support functions, represented in the underlying wavelet grid, of the template fragments are roto-translated with high numerical p...
Density functional theory study of (OCS)2^-
Bilalbegovic, G
2007-01-01T23:59:59.000Z
The structural and electronic properties of the carbonyl sulfide dimer anion are calculated using density functional theory within a pseudopotential method. Three geometries are optimized and investigated: C2v and C2 symmetric, as well as one asymmetric structure. A distribution of an excess charge in three isomers are studied by the Hirshfeld method. In an asymmetric (OCS)2^- isomer the charge is not equally divided between the two moieties, but it is distributed as OCS^{-0.6} OCS^{-0.4}. Low-lying excitation levels of three isomers are compared using the time-dependent density functional theory in the Casida approach.
On the cosmological mass function theory
A. Del Popolo
2006-09-06T23:59:59.000Z
This paper provides, from one side, a review of the theory of the cosmological mass function from a theoretical point of view, starting from the seminal paper of Press & Shechter (1974) to the last developments (Del Popolo & Gambera (1998, 1999), Sheth & Tormen 1999 (ST), Sheth, Mo & Tormen 2001 (ST1), Jenkins et al. 2001 (J01), Shet & Tormen 2002 (ST2), Del Popolo 2002a, Yagi et al. 2004 (YNY)), and from another side some improvements on the multiplicity function models in literature. ...
Goddard III, William A.
activity of the proposed materials by density functional theory (DFT). Quantum mechanics was applied for automotive applications, sta- tionary/portable power supply, and as a component of hybrid energy systems1 reaction (HOR) at the anode.8 ORR mechanisms and electronic structures of ORR catalysts are widely
A COMPLEXITY THEORY OF CONSTRUCTIBLE FUNCTIONS AND ...
2014-09-30T23:59:59.000Z
in the new definitions are constructible functions on Rn or Cn. We define .... representation theory and algebraic geometry can be made to bear on this subject .... of the zeros of a polynomial system P = {P1,...,Pn} ? C[X1,...,Xn], in terms ... applied areas such as signal processing and data analysis [4], but to our knowledge.
Density Functional Theory Models for Radiation Damage
Density Functional Theory Models for Radiation Damage S.L. Dudarev EURATOM/CCFE Fusion Association and informative as the most advanced experimental techniques developed for the observation of radiation damage investigation and assessment of radiation damage effects, offering new insight into the origin of temperature
Adsorption of silver dimer on graphene - A DFT study
Kaur, Gagandeep, E-mail: gaganj1981@yahoo.com [Department of Physics and Centre of Advanced Studies in Physics, Panjab University, Chandigarh-160014, India and Chandigarh Engineering College, Landran, Mohali-140307, Punjab (India); Gupta, Shuchi [Department of Physics and Centre of Advanced Studies in Physics, Panjab University, Chandigarh-160014, India and University Institute of Engineering and Technology, Panjab University, Chandigarh -160014 (India); Rani, Pooja; Dharamvir, Keya [Department of Physics and Centre of Advanced Studies in Physics, Panjab University, Chandigarh-160014 (India)
2014-04-24T23:59:59.000Z
We performed a systematic density functional theory (DFT) study of the adsorption of silver dimer (Ag{sub 2}) on graphene using SIESTA (Spanish Initiative for Electronic Simulations with Thousands of Atoms) package, in the generalized gradient approximation (GGA). The adsorption energy, geometry, and charge transfer of Ag2-graphene system are calculated. The minimum energy configuration for a silver dimer is parallel to the graphene sheet with its two atoms directly above the centre of carbon-carbon bond. The negligible charge transfer between the dimer and the surface is also indicative of a weak bond. The methodology demonstrated in this paper may be applied to larger silver clusters on graphene sheet.
Thermally-assisted-occupation density functional theory with generalized-gradient approximations
Chai, Jeng-Da, E-mail: jdchai@phys.ntu.edu.tw [Department of Physics, Center for Theoretical Sciences, and Center for Quantum Science and Engineering, National Taiwan University, Taipei 10617, Taiwan (China)] [Department of Physics, Center for Theoretical Sciences, and Center for Quantum Science and Engineering, National Taiwan University, Taipei 10617, Taiwan (China)
2014-05-14T23:59:59.000Z
We extend the recently proposed thermally-assisted-occupation density functional theory (TAO-DFT) [J.-D. Chai, J. Chem. Phys. 136, 154104 (2012)] to generalized-gradient approximation (GGA) exchange-correlation density functionals. Relative to our previous TAO-LDA (i.e., the local density approximation to TAO-DFT), the resulting TAO-GGAs are significantly superior for a wide range of applications, such as thermochemistry, kinetics, and reaction energies. For noncovalent interactions, TAO-GGAs with empirical dispersion corrections are shown to yield excellent performance. Due to their computational efficiency for systems with strong static correlation effects, TAO-LDA and TAO-GGAs are applied to study the electronic properties (e.g., the singlet-triplet energy gaps, vertical ionization potentials, vertical electron affinities, fundamental gaps, and symmetrized von Neumann entropy) of acenes with different number of linearly fused benzene rings (up to 100), which is very challenging for conventional electronic structure methods. The ground states of acenes are shown to be singlets for all the chain lengths studied here. With the increase of acene length, the singlet-triplet energy gaps, vertical ionization potentials, and fundamental gaps decrease monotonically, while the vertical electron affinities and symmetrized von Neumann entropy (i.e., a measure of polyradical character) increase monotonically.
Schwinger functions in noncommutative quantum field theory
Dorothea Bahns
2009-08-31T23:59:59.000Z
It is shown that the $n$-point functions of scalar massive free fields on the noncommutative Minkowski space are distributions which are boundary values of analytic functions. Contrary to what one might expect, this construction does not provide a connection to the popular traditional Euclidean approach to noncommutative field theory (unless the time variable is assumed to commute). Instead, one finds Schwinger functions with twistings involving only momenta that are on the mass-shell. This explains why renormalization in the traditional Euclidean noncommutative framework crudely differs from renormalization in the Minkowskian regime.
Silvestrelli, Pier Luigi; Ambrosetti, Alberto [Dipartimento di Fisica e Astronomia, Università di Padova, via Marzolo 8, I–35131 Padova, Italy and DEMOCRITOS National Simulation Center of the Italian Istituto Officina dei Materiali (IOM) of the Italian National Research Council (CNR), Trieste (Italy)] [Dipartimento di Fisica e Astronomia, Università di Padova, via Marzolo 8, I–35131 Padova, Italy and DEMOCRITOS National Simulation Center of the Italian Istituto Officina dei Materiali (IOM) of the Italian National Research Council (CNR), Trieste (Italy)
2014-03-28T23:59:59.000Z
The Density Functional Theory (DFT)/van der Waals-Quantum Harmonic Oscillator-Wannier function (vdW-QHO-WF) method, recently developed to include the vdW interactions in approximated DFT by combining the quantum harmonic oscillator model with the maximally localized Wannier function technique, is applied to the cases of atoms and small molecules (X=Ar, CO, H{sub 2}, H{sub 2}O) weakly interacting with benzene and with the ideal planar graphene surface. Comparison is also presented with the results obtained by other DFT vdW-corrected schemes, including PBE+D, vdW-DF, vdW-DF2, rVV10, and by the simpler Local Density Approximation (LDA) and semilocal generalized gradient approximation approaches. While for the X-benzene systems all the considered vdW-corrected schemes perform reasonably well, it turns out that an accurate description of the X-graphene interaction requires a proper treatment of many-body contributions and of short-range screening effects, as demonstrated by adopting an improved version of the DFT/vdW-QHO-WF method. We also comment on the widespread attitude of relying on LDA to get a rough description of weakly interacting systems.
Higher-order adaptive finite-element methods for Kohn–Sham density functional theory
Motamarri, P. [Department of Mechanical Engineering, University of Michigan, Ann Arbor, MI 48109 (United States)] [Department of Mechanical Engineering, University of Michigan, Ann Arbor, MI 48109 (United States); Nowak, M.R. [Department of Electrical Engineering, University of Michigan, Ann Arbor, MI 48109 (United States)] [Department of Electrical Engineering, University of Michigan, Ann Arbor, MI 48109 (United States); Leiter, K.; Knap, J. [U.S. Army Research Labs, Aberdeen Proving Ground, Aberdeen, MD 21001 (United States)] [U.S. Army Research Labs, Aberdeen Proving Ground, Aberdeen, MD 21001 (United States); Gavini, V., E-mail: vikramg@umich.edu [Department of Mechanical Engineering, University of Michigan, Ann Arbor, MI 48109 (United States)
2013-11-15T23:59:59.000Z
We present an efficient computational approach to perform real-space electronic structure calculations using an adaptive higher-order finite-element discretization of Kohn–Sham density-functional theory (DFT). To this end, we develop an a priori mesh-adaption technique to construct a close to optimal finite-element discretization of the problem. We further propose an efficient solution strategy for solving the discrete eigenvalue problem by using spectral finite-elements in conjunction with Gauss–Lobatto quadrature, and a Chebyshev acceleration technique for computing the occupied eigenspace. The proposed approach has been observed to provide a staggering 100–200-fold computational advantage over the solution of a generalized eigenvalue problem. Using the proposed solution procedure, we investigate the computational efficiency afforded by higher-order finite-element discretizations of the Kohn–Sham DFT problem. Our studies suggest that staggering computational savings—of the order of 1000-fold—relative to linear finite-elements can be realized, for both all-electron and local pseudopotential calculations, by using higher-order finite-element discretizations. On all the benchmark systems studied, we observe diminishing returns in computational savings beyond the sixth-order for accuracies commensurate with chemical accuracy, suggesting that the hexic spectral-element may be an optimal choice for the finite-element discretization of the Kohn–Sham DFT problem. A comparative study of the computational efficiency of the proposed higher-order finite-element discretizations suggests that the performance of finite-element basis is competing with the plane-wave discretization for non-periodic local pseudopotential calculations, and compares to the Gaussian basis for all-electron calculations to within an order of magnitude. Further, we demonstrate the capability of the proposed approach to compute the electronic structure of a metallic system containing 1688 atoms using modest computational resources, and good scalability of the present implementation up to 192 processors.
Functional Keldysh theory of spin torques
Duine, R. A.; Nunez, A. S.; Sinova, Jairo; MacDonald, A. H.
2007-01-01T23:59:59.000Z
Functional Keldysh theory of spin torques R. A. Duine,1,* A. S. N??ez, 2,? Jairo Sinova,3,? and A. H. MacDonald4,? 1Institute for Theoretical Physics, Utrecht University, Leuvenlaan 4, 3584 CE Utrecht, The Netherlands 2Instituto de F?sica, PUCV... #1;Received 15 March 2007; published 18 June 2007#2; We present a microscopic treatment of current-induced torques and thermal fluctuations in itinerant ferro- magnets based on a functional formulation of the Keldysh formalism. We find...
Nuclear fission in covariant density functional theory
A. V. Afanasjev; H. Abusara; P. Ring
2013-09-12T23:59:59.000Z
The current status of the application of covariant density functional theory to microscopic description of nuclear fission with main emphasis on superheavy nuclei (SHN) is reviewed. The softness of SHN in the triaxial plane leads to an emergence of several competing fission pathes in the region of the inner fission barrier in some of these nuclei. The outer fission barriers of SHN are considerably affected both by triaxiality and octupole deformation.
Density Functional Theory Studies of the Electronic Structure...
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Theory Studies of the Electronic Structure of Solid State Actinide Oxides. Density Functional Theory Studies of the Electronic Structure of Solid State Actinide Oxides. Abstract:...
Near surface stoichiometry in UO2: A density functional theory study
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Yu, Jianguo; Valderrama, Billy; Henderson, Hunter B.; Manuel, Michele V.; Allen, Todd
2015-08-01T23:59:59.000Z
The mechanisms of oxygen stoichiometry variation in UO2 at different temperature and oxygen partial pressure are important for understanding the dynamics of microstructure in these crystals. However, very limited experimental studies have been performed to understand the atomic structure of UO2 near surface and defect effects of near surface on stoichiometry in which the system can exchange atoms with the external reservoir. In this study, the near (110) surface relaxation and stoichiometry in UO2 have been studied with density functional theory (DFT) calculations. On the basis of the point-defect model (PDM), a general expression for the near surface stoichiometric variationmore »is derived by using DFT total-energy calculations and atomistic thermodynamics, in an attempt to pin down the mechanisms of oxygen exchange between the gas environment and defected UO2. By using the derived expression, it is observed that, under poor oxygen conditions, the stoichiometry of near surface is switched from hyperstoichiometric at 300 K with a depth around 3 nm to near-stoichiometric at 1000 K and hypostoichiometric at 2000 K. Furthermore, at very poor oxygen concentrations and high temperatures, our results also suggest that the bulk of the UO2 prefers to be hypostoichiometric, although the surface is near-stoichiometric.« less
Mixing of equations of state for xenon-deuterium using density functional theory
Magyar, Rudolph J.; Mattsson, Thomas R. [Sandia National Laboratories, Albuquerque, New Mexico 87185 (United States)
2013-03-15T23:59:59.000Z
We report on a theoretical study of equation of state (EOS) properties of fluid and dense plasma mixtures of xenon and deuterium to explore and illustrate the basic physics of the mixing of a light element with a heavy element. Accurate EOS models are crucial to achieve high-fidelity hydrodynamics simulations of many high-energy-density phenomena, for example inertial confinement fusion and strong shock waves. While the EOS is often tabulated for separate species, the equation of state for arbitrary mixtures is generally not available, requiring properties of the mixture to be approximated by combining physical properties of the pure systems. Density functional theory (DFT) at elevated-temperature is used to assess the thermodynamics of the xenon-deuterium mixture at different mass ratios. The DFT simulations are unbiased as to elemental species and therefore provide comparable accuracy when describing total energies, pressures, and other physical properties of mixtures as they do for pure systems. The study focuses on addressing the accuracy of different mixing rules in the temperature range 1000-40 000 K for pressures between 100 and 600 GPa (1-6 Mbar), thus, including the challenging warm dense matter regime of the phase diagram. We find that a mix rule taking into account pressure equilibration between the two species performs very well over the investigated range.
Near Surface Stoichiometry in UO 2 : A Density Functional Theory Study
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Yu, Jianguo; Valderrama, Billy; Henderson, Hunter B.; Manuel, Michele V.; Allen, Todd
2015-01-01T23:59:59.000Z
The mechanisms of oxygen stoichiometry variation in UO2at different temperature and oxygen partial pressure are important for understanding the dynamics of microstructure in these crystals. However, very limited experimental studies have been performed to understand the atomic structure of UO2near surface and defect effects of near surface on stoichiometry in which the system can exchange atoms with the external reservoir. In this study, the near (110) surface relaxation and stoichiometry in UO2have been studied with density functional theory (DFT) calculations. On the basis of the point-defect model (PDM), a general expression for the near surface stoichiometric variation is derived bymore »using DFT total-energy calculations and atomistic thermodynamics, in an attempt to pin down the mechanisms of oxygen exchange between the gas environment and defected UO2. By using the derived expression, it is observed that, under poor oxygen conditions, the stoichiometry of near surface is switched from hyperstoichiometric at 300?K with a depth around 3?nm to near-stoichiometric at 1000?K and hypostoichiometric at 2000?K. Furthermore, at very poor oxygen concentrations and high temperatures, our results also suggest that the bulk of the UO2prefers to be hypostoichiometric, although the surface is near-stoichiometric.« less
Maeta, Takahiro [Graduate School of System Engineering, Okayama Prefectural University, 111 Kuboki, Soja, Okayama 719-1197 (Japan); GlobalWafers Japan Co., Ltd., Higashikou, Seirou-machi, Kitakanbara-gun, Niigata 957-0197 (Japan); Sueoka, Koji [Department of Communication Engineering, Okayama Prefectural University, 111 Kuboki, Soja, Okayama 719-1197 (Japan)
2014-08-21T23:59:59.000Z
Ge-based substrates are being developed for applications in advanced nano-electronic devices because of their higher intrinsic carrier mobility than Si. The stability and diffusion mechanism of impurity atoms in Ge are not well known in contrast to those of Si. Systematic studies of the stable sites of 2nd to 6th row element impurity atoms in Ge crystal were undertaken with density functional theory (DFT) and compared with those in Si crystal. It was found that most of the impurity atoms in Ge were stable at substitutional sites, while transition metals in Si were stable at interstitial sites and the other impurity atoms in Si were stable at substitutional sites. Furthermore, DFT calculations were carried out to clarify the mechanism responsible for the diffusion of impurity atoms in Ge crystals. The diffusion mechanism for 3d transition metals in Ge was found to be an interstitial-substitutional diffusion mechanism, while in Si this was an interstitial diffusion mechanism. The diffusion barriers in the proposed diffusion mechanisms in Ge and Si were quantitatively verified by comparing them to the experimental values in the literature.
Mehdi Farzanehpour; I. V. Tokatly
2015-06-29T23:59:59.000Z
We use analytic (current) density-potential maps of time-dependent (current) density functional theory (TD(C)DFT) to inverse engineer analytically solvable time-dependent quantum problems. In this approach the driving potential (the control signal) and the corresponding solution of the Schr\\"odinger equation are parametrized analytically in terms of the basic TD(C)DFT observables. We describe the general reconstruction strategy and illustrate it with a number of explicit examples. First we consider the real space one-particle dynamics driven by a time-dependent electromagnetic field and recover, from the general TDDFT reconstruction formulas, the known exact solution for a driven oscillator with a time-dependent frequency. Then we use analytic maps of the lattice TD(C)DFT to control quantum dynamics in a discrete space. As a first example we construct a time-dependent potential which generates prescribed dynamics on a tight-binding chain. Then our method is applied to the dynamics of spin-1/2 driven by a time dependent magnetic field. We design an analytic control pulse that transfers the system from the ground to excited state and vice versa. This pulse generates the spin flip thus operating as a quantum NOT gate.
Electronic Structure via Potential Functional Approximations Attila Cangi,1
Burke, Kieron
Elliott,2 Kieron Burke,1 and E. K. U. Gross3 1 Department of Chemistry, University of California, 1102 of density-functional theory (DFT), suggested by Thomas [1] and Fermi [2] (TF) and made formally exact
Krishtal, Alisa; Genova, Alessandro; Pavanello, Michele
2015-01-01T23:59:59.000Z
Subsystem Density-Functional Theory (DFT) is an emerging technique for calculating the electronic structure of complex molecular and condensed phase systems. In this topical review, we focus on some recent advances in this field related to the computation of condensed phase systems, their excited states, and the evaluation of many-body interactions between the subsystems. As subsystem DFT is in principle an exact theory, any advance in this field can have a dual role. One is the possible applicability of a resulting method in practical calculations. The other is the possibility of shedding light on some quantum-mechanical phenomenon which is more easily treated by subdividing a supersystem into subsystems. An example of the latter is many-body interactions. In the discussion, we present some recent work from our research group as well as some new results, casting them in the current state-of-the-art in this review as comprehensively as possible.
Symmetry energy in nuclear density functional theory
W. Nazarewicz; P. -G. Reinhard; W. Satula; D. Vretenar
2013-07-22T23:59:59.000Z
The nuclear symmetry energy represents a response to the neutron-proton asymmetry. In this survey we discuss various aspects of symmetry energy in the framework of nuclear density functional theory, considering both non-relativistic and relativistic self-consistent mean-field realizations side-by-side. Key observables pertaining to bulk nucleonic matter and finite nuclei are reviewed. Constraints on the symmetry energy and correlations between observables and symmetry-energy parameters, using statistical covariance analysis, are investigated. Perspectives for future work are outlined in the context of ongoing experimental efforts.
Kanematsu, Yusuke; Tachikawa, Masanori [Quantum Chemistry Division, Yokohama City University, Seto 22-2, Kanazawa-ku, Yokohama 236-0027 (Japan)] [Quantum Chemistry Division, Yokohama City University, Seto 22-2, Kanazawa-ku, Yokohama 236-0027 (Japan)
2014-04-28T23:59:59.000Z
We have developed the multicomponent hybrid density functional theory [MC-(HF+DFT)] method with polarizable continuum model (PCM) for the analysis of molecular properties including both nuclear quantum effect and solvent effect. The chemical shifts and H/D isotope shifts of the picolinic acid N-oxide (PANO) molecule in chloroform and acetonitrile solvents are applied by B3LYP electron exchange-correlation functional for our MC-(HF+DFT) method with PCM (MC-B3LYP/PCM). Our MC-B3LYP/PCM results for PANO are in reasonable agreement with the corresponding experimental chemical shifts and isotope shifts. We further investigated the applicability of our method for acetylacetone in several solvents.
Kornobis, Karina; Wong, Bryan M; Lodowski, Piotr; Jaworska, Maria; Andruniów, Tadeusz; Rudd, Kenneth; Kozlowski, Pawel M; 10.1021/jp110914y
2011-01-01T23:59:59.000Z
Time-dependent density functional theory (TD-DFT) and correlated ab initio methods have been applied to the electronically excited states of vitamin B12 (cyanocobalamin or CNCbl). Different experimental techniques have been used to probe the excited states of CNCbl, revealing many issues that remain poorly understood from an electronic structure point of view. Due to its efficient scaling with size, TD-DFT emerges as one of the most practical tools that can be used to predict the electronic properties of these fairly complex molecules. However, the description of excited states is strongly dependent on the type of functional used in the calculations. In the present contribution, the choice of a proper functional for vitamin B12 was evaluated in terms of its agreement with both experimental results and correlated ab initio calculations. Three different functionals, i.e. B3LYP, BP86, and LC-BLYP, were tested. In addition, the effect of relative contributions of DFT and HF to the exchange-correlation functional ...
Local pressure of confined fluids inside nanoslit pores -- A density functional theory prediction
F. Heidari; G. A. Mansoori; E. Keshavarzi
2013-07-18T23:59:59.000Z
In this work, the local pressure of fluids confined inside nanoslit pores is predicted within the framework of the density functional theory. The Euler-Lagrange equation in the density functional theory of statistical mechanics is used to obtain the force balance equation which leads to a general equation to predict the local normal component of the pressure tensor. Our approach yields a general equation for predicting the normal pressure of confined fluids and it satisfies the exact bulk thermodynamics equation when the pore width approaches infinity. As two basic examples, we report the solution of the general equation for hard-sphere (HS) and Lennard-Jones (LJ) fluids confined between two parallel-structureless hard walls. To do so, we use the modified fundamental measure theory (mFMT) to obtain the normal pressure for hard-sphere confined fluid and mFMT incorporated with the Rosenfeld perturbative DFT for the LJ fluid. Effects of different variables including pore width, bulk density and temperature on the behavior of normal pressure are studied and reported. Our predicted results show that in both HS and LJ cases the confined fluids normal pressure has an oscillatory behavior and the number of oscillations increases with bulk density and temperature. The oscillations also become broad and smooth with pore width at a constant temperature and bulk density. In comparison with the HS confined fluid, the values of normal pressure for the LJ confined fluid as well as its oscillations at all distances from the walls are less profound.
Theoretical Chemistry Theory, Computation, and
Gherman, Benjamin F.
1 23 Theoretical Chemistry Accounts Theory, Computation, and Modeling ISSN 1432-881X Volume 128). In order to explore the origin of this preference, density functional theory (DFT) calculations have been-terminus of nascent eubacterial proteins during protein synthesis [14]. As PDF is essential for bacterial survival
Band terminations in density functional theory
A. V. Afanasjev
2009-02-01T23:59:59.000Z
The analysis of the terminating bands has been performed in the relativistic mean field framework. It was shown that nuclear magnetism provides an additional binding to the energies of the specific configuration and this additional binding increases with spin and has its {\\it maximum} exactly at the terminating state. This suggests that the terminating states can be an interesting probe of the time-odd mean fields {\\it provided that other effects can be reliably isolated.} Unfortunately, a reliable isolation of these effects is not that simple: many terms of the density functional theories contribute into the energies of the terminating states and the deficiencies in the description of those terms affect the result. The recent suggestion \\cite{ZSW.05} that the relative energies of the terminating states in the $N \
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Tawa, G.J.; Martin, R.L.; Pratt, L.R.; Russo, T.V. [Los Alamos National Lab., NM (United States)] [Los Alamos National Lab., NM (United States)
1996-02-01T23:59:59.000Z
Electrostatic solvation free energies are calculated using a self consistent reaction field (SCRF) procedure that combines a continuum dielectric model of the solvent with both Hartree-Fock (HF) and density functional theory (DFT) for the solute. Several molecules are studied in aqueous solution. They comprise three groups: nonpolar neutral, polar neutral, and ionic. The calculated values of {Delta}G{sup e1} are sensitive to the atomic radii used to define the solute molecular surface, particularly to the value of the hydrogen radius. However, the values of {Delta}G{sup e1} exhibit reasonable correlation with experiment when a previously determined, physically motivated set of atomic radii were used to define the van der Waals surface of the solute. The standard deviation between theory and experiment is 2.51 kcal/mol for HF and 2.21 kcal/mol for DFT for the 14 molecules examined. The errors with HF or DFT are similar. The relative difference between the calculated values of {Delta}G{sup e1} and experiment is largest for nonpolar neutral molecules, intermediate for polar neutral molecules, and smallest for ions. This is consistent with the expected relative importance of nonelectrostatic contributions to the free energy that are omitted in the model. 92 refs., 4 figs., 6 tabs.
Mehmood, F.; Pachter, R., E-mail: ruth.pachter@us.af.mil [Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433 (United States)
2014-04-28T23:59:59.000Z
In this work, density functional theory (DFT) calculations have been used to investigate chemical sensing on surfaces of single-layer MoS{sub 2} and graphene, considering the adsorption of the chemical compounds triethylamine, acetone, tetrahydrofuran, methanol, 2,4,6-trinitrotoluene, o-nitrotoluene, o-dichlorobenzene, and 1,5-dicholoropentane. Physisorption of the adsorbates on free-standing surfaces was analyzed in detail for optimized material structures, considering various possible adsorption sites. Similar adsorption characteristics for the two surface types were demonstrated, where inclusion of a correction to the DFT functional for London dispersion was shown to be important to capture interactions at the interface of molecular adsorbate and surface. Charge transfer analyses for adsorbed free-standing surfaces generally demonstrated very small effects. However, charge transfer upon inclusion of the underlying SiO{sub 2} substrate rationalized experimental observations for some of the adsorbates considered. A larger intrinsic response for the electron-donor triethylamine adsorbed on MoS{sub 2} as compared to graphene was demonstrated, which may assist in devising chemical sensors for improved sensitivity.
Sussman, Joel L.
Taiyuan Road, Shanghai 200031, P. R. China, and Departments of Structural Biology and Neurobiology, NH4 + always tilts toward the carbon-carbon bond rather than toward the heteroatom or the carbon
The vacuum state functional of interacting string field theory
A. Ilderton
2005-06-21T23:59:59.000Z
We show that the vacuum state functional for both open and closed string field theories can be constructed from the vacuum expectation values it must generate. The method also applies to quantum field theory and as an application we give a diagrammatic description of the equivalance between Schrodinger and covariant repreresentations of field theory.
Soderlind, P; Wolfer, W
2007-07-27T23:59:59.000Z
Spin and orbital and electron correlations are known to be important when treating the high-temperature {delta} phase of plutonium within the framework of density-functional theory (DFT). One of the more successful attempts to model {delta}-Pu within this approach has included condensed-matter generalizations of Hund's three rules for atoms, i.e., spin polarization, orbital polarization, and spin-orbit coupling. Here they perform a quantitative analysis of these interactions relative rank for the bonding and electronic structure in {delta}-Pu within the DFT model. The result is somewhat surprising in that spin-orbit coupling and orbital polarization are far more important than spin polarization for a realistic description of {delta}-Pu. They show that these orbital correlations on their own, without any formation of magnetic spin moments, can account for the low atomic density of the {delta} phase with a reasonable equation-of-state. In addition, this unambiguously non-magnetic (NM) treatment produces a one-electron spectra with resonances close to the Fermi level consistent with experimental valence band photoemission spectra.
I. A. Shkrob
2006-07-25T23:59:59.000Z
Density functional theory (DFT) is used to rationalize magnetic parameters of hydrated electron trapped in alkaline glasses as observed using Electron Paramagnetic Resonance (EPR) and Electron Spin Echo Envelope Modulation (ESEEM) spectroscopies. To this end, model water cluster anions (n=4-8 and n=20,24) that localize the electron internally are examined. It is shown that EPR parameters of such water anions (such as hyperfine coupling tensors of H/D nuclei in the water molecules) are defined mainly by the cavity size and the coordination number of the electron; the water molecules in the second solvation shell play a relatively minor role. An idealized model of hydrated electron (that is usually attributed to L. Kevan) in which six hydroxyl groups arranged in an octahedral pattern point towards the common center is shown to provide the closest match to the experimental parameters, such as isotropic and anisotropic hyperfine coupling constants for the protons (estimated from ESEEM), the second moment of the EPR spectra, and the radius of gyration. The salient feature of these DFT models is the significant transfer (10-20%) of spin density into the frontal O 2p orbitals of water molecules. Spin bond polarization involving these oxygen orbitals accounts for small, negative hyperfine coupling constants for protons in hydroxyl groups that form the electron-trapping cavity. In Part 2, these results are generalized for more realistic geometries of core anions obtained using a dynamic one-electron mixed qunatum/classical molecular dynamics model.
A COMPLEXITY THEORY OF CONSTRUCTIBLE FUNCTIONS AND ...
2014-09-30T23:59:59.000Z
Sep 30, 2014 ... Primary 14P10, 14P25; Secondary 68W30. Key words and phrases. constructible functions, constructible sheaves, polynomial hierarchy,.
Ensemble density variational methods with self- and ghost-interaction-corrected functionals
Pastorczak, Ewa [Institute of Applied Radiation Chemistry, Faculty of Chemistry, Lodz University of Technology, ul. Wroblewskiego 15, 93-590 Lodz (Poland)] [Institute of Applied Radiation Chemistry, Faculty of Chemistry, Lodz University of Technology, ul. Wroblewskiego 15, 93-590 Lodz (Poland); Pernal, Katarzyna, E-mail: pernalk@gmail.com [Institute of Physics, Lodz University of Technology, ul. Wolczanska 219, 90-924 Lodz (Poland)] [Institute of Physics, Lodz University of Technology, ul. Wolczanska 219, 90-924 Lodz (Poland)
2014-05-14T23:59:59.000Z
Ensemble density functional theory (DFT) offers a way of predicting excited-states energies of atomic and molecular systems without referring to a density response function. Despite a significant theoretical work, practical applications of the proposed approximations have been scarce and they do not allow for a fair judgement of the potential usefulness of ensemble DFT with available functionals. In the paper, we investigate two forms of ensemble density functionals formulated within ensemble DFT framework: the Gross, Oliveira, and Kohn (GOK) functional proposed by Gross et al. [Phys. Rev. A 37, 2809 (1988)] alongside the orbital-dependent eDFT form of the functional introduced by Nagy [J. Phys. B 34, 2363 (2001)] (the acronym eDFT proposed in analogy to eHF – ensemble Hartree-Fock method). Local and semi-local ground-state density functionals are employed in both approaches. Approximate ensemble density functionals contain not only spurious self-interaction but also the so-called ghost-interaction which has no counterpart in the ground-state DFT. We propose how to correct the GOK functional for both kinds of interactions in approximations that go beyond the exact-exchange functional. Numerical applications lead to a conclusion that functionals free of the ghost-interaction by construction, i.e., eDFT, yield much more reliable results than approximate self- and ghost-interaction-corrected GOK functional. Additionally, local density functional corrected for self-interaction employed in the eDFT framework yields excitations energies of the accuracy comparable to that of the uncorrected semi-local eDFT functional.
Optimal Transportation Theory with Repulsive Costs
Simone Di Marino; Augusto Gerolin; Luca Nenna
2015-06-15T23:59:59.000Z
This paper intents to present the state of art and recent developments of the optimal transportation theory with many marginals for a class of repulsive cost functions. We introduce some aspects of the Density Functional Theory (DFT) from a mathematical point of view, and revisit the theory of optimal transport from its perspective. Moreover, in the last three sections, we describe some recent and new theoretical and numerical results obtained for the Coulomb cost, the repulsive harmonic cost and the determinant cost.
Efficient Real-Time Time-Dependent Density Functional Theory...
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Efficient Real-Time Time-Dependent Density Functional Theory Method and its Application to a Collision of an Ion with a 2D Material This content will become publicly available on...
Constrained Density-Functional Theory--Configuration Interaction
Kaduk, Benjamin James
2012-01-01T23:59:59.000Z
In this thesis, I implemented a method for performing electronic structure calculations, "Constrained Density Functional Theory-- Configuration Interaction" (CDFT-CI), which builds upon the computational strengths of Density ...
A Classical Density-Functional Theory for Describing Water Interfaces
Jessica Hughes; Eric Krebs; David Roundy
2012-08-31T23:59:59.000Z
We develop a classical density functional for water which combines the White Bear fundamental-measure theory (FMT) functional for the hard sphere fluid with attractive interactions based on the Statistical Associating Fluid Theory (SAFT-VR). This functional reproduces the properties of water at both long and short length scales over a wide range of temperatures, and is computationally efficient, comparable to the cost of FMT itself. We demonstrate our functional by applying it to systems composed of two hard rods, four hard rods arranged in a square and hard spheres in water.
Preface: Special Topic on Advances in Density Functional Theory
Yang, Weitao [Department of Chemistry and Department of Physics, Duke University, Durham, North Carolina 27708 (United States)] [Department of Chemistry and Department of Physics, Duke University, Durham, North Carolina 27708 (United States)
2014-05-14T23:59:59.000Z
This Special Topic Issue on the Advances in Density Functional Theory, published as a celebration of the fifty years of density functional theory, contains a retrospective article, a perspective article, and a collection of original research articles that showcase recent theoretical advances in the field. It provides a timely discussion reflecting a cross section of our understanding, and the theoretical and computational developments, which have significant implications in broad areas of sciences and engineering.
Test Functions Space in Noncommutative Quantum Field Theory
M. Chaichian; M. Mnatsakanova; A. Tureanu; Yu. Vernov
2008-07-26T23:59:59.000Z
It is proven that the $\\star$-product of field operators implies that the space of test functions in the Wightman approach to noncommutative quantum field theory is one of the Gel'fand-Shilov spaces $S^{\\beta}$ with $\\beta test functions smears the noncommutative Wightman functions, which are in this case generalized distributions, sometimes called hyperfunctions. The existence and determination of the class of the test function spaces in NC QFT is important for any rigorous treatment in the Wightman approach.
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Liu, Jin; Adamska, Lyudmyla; Doorn, Stephen K.; Tretiak, Sergei
2015-05-14T23:59:59.000Z
Conformational structure and the electronic properties of various electronic excitations in cycloparaphenylenes (CPPs) are calculated using hybrid Density Functional Theory (DFT). The results demonstrate that wavefunctions of singlet and triplet excitons as well as the positive and negative polarons remain fully delocalized in CPPs. In contrast, these excitations in larger CPP molecules become localized on several phenyl rings, which are locally planarized, while the undeformed ground state geometry is preserved on the rest of the hoop. As evidenced by the measurements of bond-length alternation and dihedral angles, localized regions show stronger hybridization between neighboring bonds and thus enhanced electronic communication.more »This effect is even more significant in the smaller hoops, where phenyl rings have strong quinoid character in the ground state. Thus, upon excitation, electron–phonon coupling leads to the self-trapping of the electronic wavefunction and release of energy from fractions of an eV up to two eVs, depending on the type of excitation and the size of the hoop. The impact of such localization on electronic and optical properties of CPPs is systematically investigated and compared with the available experimental measurements.« less
Density functional theory and optimal transportation with Coulomb cost
Codina Cotar; Gero Friesecke; Claudia Klüppelberg
2011-04-04T23:59:59.000Z
We present here novel insight into exchange-correlation functionals in density functional theory, based on the viewpoint of optimal transport. We show that in the case of two electrons and in the semiclassical limit, the exact exchange-correlation functional reduces to a very interesting functional of novel form, which depends on an optimal transport map $T$ associated with a given density $\\rho$. Since the above limit is strongly correlated, the limit functional yields insight into electron correlations. We prove the existence and uniqueness of such an optimal map for any number of electrons and each $\\rho$, and determine the map explicitly in the case when $\\rho$ is radially symmetric.
Improved association in a classical density functional theory for water
Eric J. Krebs; Jeff B. Schulte; David Roundy
2013-09-07T23:59:59.000Z
We present a modification to our recently published SAFT-based classical density functional theory for water. We have recently developed and tested a functional for the averaged radial distribution function at contact of the hard-sphere fluid that is dramatically more accurate at interfaces than earlier approximations. We now incorporate this improved functional into the association term of our free energy functional for water, improving its description of hydrogen bonding. We examine the effect of this improvement by studying two hard solutes: a hard hydrophobic rod and a hard sphere. The improved functional leads to a moderate change in the density profile and a large decrease in the number of hydrogen bonds broken in the vicinity of the solutes.We present a modification to our recently published SAFT-based classical density functional theory for water. We have recently developed and tested a functional for the averaged radial distribution function at contact of the hard-sphere fluid that is dramatically more accurate at interfaces than earlier approximations. We now incorporate this improved functional into the association term of our free energy functional for water, improving its description of hydrogen bonding. We examine the effect of this improvement by studying two hard solutes: a hard hydrophobic rod and a hard sphere. The improved functional leads to a moderate change in the density profile and a large decrease in the number of hydrogen bonds broken in the vicinity of the solutes.
(E)-2-[(2-Bromophenylimino)methyl]-5-methoxyphenol: X-ray and DFT-calculated structures
Kosar, B., E-mail: bkosar@omu.edu.tr; Albayrak, C. [Sinop University, Faculty of Education (Turkey); Odabasoglu, M. [Pamukkale University, Chemistry Program (Turkey); Bueyuekguengoer, O. [Ondokuz Mayis University, Faculty of Arts and Sciences (Turkey)
2010-12-15T23:59:59.000Z
The crystal structure of (E)-2-[(2-Bromophenylimino)methyl]-5-methoxyphenol is determined by using X-ray diffraction and then the molecular structure is investigated with density functional theory (DFT). X-Ray study shows that the title compound has a strong intramolecular O-H-N hydrogen bond and three dimensional crystal structure is primarily determined by C-H-{pi} and weak van der Waals interactions. The strong O-H-N bond is an evidence of the preference for the phenol-imine tautomeric form in the solid state. Optimized molecular geometry is calculated with DFT at the B3LYP/6-31G(d,p) level. The IR spectra of compound were recorded experimentally and calculated to compare with each other. The results from both experiment and theoretical calculations are compared in this study.
Saldin, Dilano
, University of Wisconsin Milwaukee, Milwaukee, WI 53211, USA 4 National Energy Technology Laboratory and Low Energy Electron Diffraction Joanna James1 , Dilano K. Saldin2 , T. Zheng3 , W. T. Tysoe3 Theory (DFT) calculations have played a key role in the growing list of surface species whose structure
Density functional theory for self-bound systems
Nir Barnea
2007-11-06T23:59:59.000Z
The density functional theory is extended to account for self-bound systems. To this end the Hohenberg-Kohn theorem is formulated for the intrinsic density and a Kohn-Sham like procedure for an $N$--body system is derived using the adiabatic approximation to account for the center of mass motion.
Monte Carlo tests of Orbital-Free Density Functional Theory
D. I. Palade
2014-12-12T23:59:59.000Z
The relationship between the exact kinetic energy density in a quantum system in the frame of Density Functional Theory and the semiclassical functional expression for the same quantity is investigated. The analysis is performed with Monte Carlo simulations of the Kohn-Sham potentials. We find that the semiclassical form represents the statistical expectation value of the quantum nature. Based on the numerical results, we propose an empirical correction to the existing functional and an associated method to improve the Orbital-Free results.
Addressing spectroscopic quality of covariant density functional theory
A. V. Afanasjev
2014-09-17T23:59:59.000Z
The spectroscopic quality of covariant density functional theory has been accessed by analyzing the accuracy and theoretical uncertainties in the description of spectroscopic observables. Such analysis is first presented for the energies of the single-particle states in spherical and deformed nuclei. It is also shown that the inclusion of particle-vibration coupling improves the description of the energies of predominantly single-particle states in medium and heavy-mass spherical nuclei. However, the remaining differences between theory and experiment clearly indicate missing physics and missing terms in covariant energy density functionals. The uncertainties in the predictions of the position of two-neutron drip line sensitively depend on the uncertainties in the prediction of the energies of the single-particle states. On the other hand, many spectroscopic observables in well deformed nuclei at ground state and finite spin only weakly depend on the choice of covariant energy density functional.
Multi-time wave functions for quantum field theory
Petrat, Sören, E-mail: petrat@math.lmu.de [Mathematisches Institut, Ludwig-Maximilians-Universität, Theresienstr. 39, 80333 München (Germany); Tumulka, Roderich, E-mail: tumulka@math.rutgers.edu [Department of Mathematics, Rutgers University, 110 Frelinghuysen Road, Piscataway, NJ 08854-8019 (United States)
2014-06-15T23:59:59.000Z
Multi-time wave functions such as ?(t{sub 1},x{sub 1},…,t{sub N},x{sub N}) have one time variable t{sub j} for each particle. This type of wave function arises as a relativistic generalization of the wave function ?(t,x{sub 1},…,x{sub N}) of non-relativistic quantum mechanics. We show here how a quantum field theory can be formulated in terms of multi-time wave functions. We mainly consider a particular quantum field theory that features particle creation and annihilation. Starting from the particle–position representation of state vectors in Fock space, we introduce multi-time wave functions with a variable number of time variables, set up multi-time evolution equations, and show that they are consistent. Moreover, we discuss the relation of the multi-time wave function to two other representations, the Tomonaga–Schwinger representation and the Heisenberg picture in terms of operator-valued fields on space–time. In a certain sense and under natural assumptions, we find that all three representations are equivalent; yet, we point out that the multi-time formulation has several technical and conceptual advantages. -- Highlights: •Multi-time wave functions are manifestly Lorentz-covariant objects. •We develop consistent multi-time equations with interaction for quantum field theory. •We discuss in detail a particular model with particle creation and annihilation. •We show how multi-time wave functions are related to the Tomonaga–Schwinger approach. •We show that they have a simple representation in terms of operator valued fields.
Relativistic density functional theory for finite nuclei and neutron stars
J. Piekarewicz
2015-02-05T23:59:59.000Z
The main goal of the present contribution is a pedagogical introduction to the fascinating world of neutron stars by relying on relativistic density functional theory. Density functional theory provides a powerful--and perhaps unique--framework for the calculation of both the properties of finite nuclei and neutron stars. Given the enormous densities that may be reached in the core of neutron stars, it is essential that such theoretical framework incorporates from the outset the basic principles of Lorentz covariance and special relativity. After a brief historical perspective, we present the necessary details required to compute the equation of state of dense, neutron-rich matter. As the equation of state is all that is needed to compute the structure of neutron stars, we discuss how nuclear physics--particularly certain kind of laboratory experiments--can provide significant constrains on the behavior of neutron-rich matter.
Zanatta, G.; Gottfried, C. [Departamento de Bioquímica, Universidade Federal do Rio Grande do Sul, 90035-003 Porto Alegre-RS (Brazil)] [Departamento de Bioquímica, Universidade Federal do Rio Grande do Sul, 90035-003 Porto Alegre-RS (Brazil); Silva, A. M. [Universidade Estadual do Piauí, 64260-000 Piripiri-Pi (Brazil)] [Universidade Estadual do Piauí, 64260-000 Piripiri-Pi (Brazil); Caetano, E. W. S., E-mail: ewcaetano@gmail.com [Instituto de Educação, Ciência e Tecnologia do Ceará, 60040-531 Fortaleza-CE (Brazil)] [Instituto de Educação, Ciência e Tecnologia do Ceará, 60040-531 Fortaleza-CE (Brazil); Sales, F. A. M.; Freire, V. N. [Departamento de Física, Universidade Federal do Ceará, Caixa Postal 6030, 60455-760 Fortaleza-CE (Brazil)] [Departamento de Física, Universidade Federal do Ceará, Caixa Postal 6030, 60455-760 Fortaleza-CE (Brazil)
2014-03-28T23:59:59.000Z
Results of optical absorption measurements are presented together with calculated structural, electronic, and optical properties for the anhydrous monoclinic L-asparagine crystal. Density functional theory (DFT) within the generalized gradient approximation (GGA) including dispersion effects (TS, Grimme) was employed to perform the calculations. The optical absorption measurements revealed that the anhydrous monoclinic L-asparagine crystal is a wide band gap material with 4.95 eV main gap energy. DFT-GGA+TS simulations, on the other hand, produced structural parameters in very good agreement with X-ray data. The lattice parameter differences ?a, ?b, ?c between theory and experiment were as small as 0.020, 0.051, and 0.022 Å, respectively. The calculated band gap energy is smaller than the experimental data by about 15%, with a 4.23 eV indirect band gap corresponding to Z???? and Z???? transitions. Three other indirect band gaps of 4.30 eV, 4.32 eV, and 4.36 eV are assigned to ?3 ???, ?1 ???, and ?2 ??? transitions, respectively. ?-sol computations, on the other hand, predict a main band gap of 5.00 eV, just 50 meV above the experimental value. Electronic wavefunctions mainly originating from O 2p–carboxyl, C 2p–side chain, and C 2p–carboxyl orbitals contribute most significantly to the highest valence and lowest conduction energy bands, respectively. By varying the lattice parameters from their converged equilibrium values, we show that the unit cell is less stiff along the b direction than for the a and c directions. Effective mass calculations suggest that hole transport behavior is more anisotropic than electron transport, but the mass values allow for some charge mobility except along a direction perpendicular to the molecular layers of L-asparagine which form the crystal, so anhydrous monoclinic L-asparagine crystals could behave as wide gap semiconductors. Finally, the calculations point to a high degree of optical anisotropy for the absorption and complex dielectric function, with more structured curves for incident light polarized along the 100 and 101 directions.
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Yamaoka, Hitoshi; Jarrige, Ignace; Schwier, Eike F.; Arita, Masashi; Shimada, Kenya; Tsujii, Naohito; Jiang, Jian; Hayashi, Hirokazu; Iwasawa, Hideaki; Namatame, Hirofumi; et al
2015-03-01T23:59:59.000Z
The electronic structure of Ce?Pd??X? (X = Si, Ge) has been studied using detailed density functional theory (DFT) calculations and high-resolution photoelectron spectroscopy (PES) measurements. The orbital decomposition of the electronic structure by DFT calculations indicates that Ce atoms at the (8c) site surrounded by 16 Pd atoms have a more localized nature and a tendency to be magnetic. Ce atoms in the (4a) site surrounded by 12 Pd and 6 X atoms, on the other, show only a negligible magnetic moment. In the photoemission valence-band spectra we observe a strong f? (Ce??) component with a small fraction of f¹more »(Ce³?) component. The spectral weight of f¹ component near the Fermi level Ce?Pd??Si? is stronger than that for Ce?Pd??Ge? at the 4d-4f resonance, suggesting stronger c-f hybridization in the former. This may hint to the origin of the large electronic specific coefficient of Ce?Pd??Si? compared to Ce?Pd??Ge?.« less
Adam P. Hughes; Uwe Thiele; Andrew J. Archer
2015-01-28T23:59:59.000Z
The contribution to the free energy for a film of liquid of thickness $h$ on a solid surface, due to the interactions between the solid-liquid and liquid-gas interfaces is given by the binding potential, $g(h)$. The precise form of $g(h)$ determines whether or not the liquid wets the surface. Note that differentiating $g(h)$ gives the Derjaguin or disjoining pressure. We develop a microscopic density functional theory (DFT) based method for calculating $g(h)$, allowing us to relate the form of $g(h)$ to the nature of the molecular interactions in the system. We present results based on using a simple lattice gas model, to demonstrate the procedure. In order to describe the static and dynamic behaviour of non-uniform liquid films and drops on surfaces, a mesoscopic free energy based on $g(h)$ is often used. We calculate such equilibrium film height profiles and also directly calculate using DFT the corresponding density profiles for liquid drops on surfaces. Comparing quantities such as the contact angle and also the shape of the drops, we find good agreement between the two methods. We also study in detail the effect on $g(h)$ of truncating the range of the dispersion forces, both those between the fluid molecules and those between the fluid and wall. We find that truncating can have a significant effect on $g(h)$ and the associated wetting behaviour of the fluid.
Descriptions of carbon isotopes within the energy density functional theory
Ismail, Atef [Fundamental and Applied Sciences Department, Universiti Teknologi PETRONAS, Bandar Seri Iskandar, 31750 Tronoh, Perak, Malaysia and Department of Physics, Al-Azhar University, 71524 Assiut (Egypt); Cheong, Lee Yen; Yahya, Noorhana [Fundamental and Applied Sciences Department, Universiti Teknologi PETRONAS, Bandar Seri Iskandar, 31750 Tronoh, Perak (Malaysia); Tammam, M. [Department of Physics, Al-Azhar University, 71524 Assiut (Egypt)
2014-10-24T23:59:59.000Z
Within the energy density functional (EDF) theory, the structure properties of Carbon isotopes are systematically studied. The shell model calculations are done for both even-A and odd-A nuclei, to study the structure of rich-neutron Carbon isotopes. The EDF theory indicates the single-neutron halo structures in {sup 15}C, {sup 17}C and {sup 19}C, and the two-neutron halo structures in {sup 16}C and {sup 22}C nuclei. It is also found that close to the neutron drip-line, there exist amazing increase in the neutron radii and decrease on the binding energies BE, which are tightly related with the blocking effect and correspondingly the blocking effect plays a significant role in the shell model configurations.
Particle-vibration coupling within covariant density functional theory
E. Litvinova; P. Ring; V. Tselyaev
2007-05-08T23:59:59.000Z
Covariant density functional theory, which has so far been applied only within the framework of static and time dependent mean field theory is extended to include Particle-Vibration Coupling (PVC) in a consistent way. Starting from a conventional energy functional we calculate the low-lying collective vibrations in Relativistic Random Phase Approximation (RRPA) and construct an energy dependent self-energy for the Dyson equation. The resulting Bethe-Salpeter equation in the particle-hole ($ph$) channel is solved in the Time Blocking Approximation (TBA). No additional parameters are used and double counting is avoided by a proper subtraction method. The same energy functional, i.e. the same set of coupling constants, generates the Dirac-Hartree single-particle spectrum, the static part of the residual $ph$-interaction and the particle-phonon coupling vertices. Therefore a fully consistent description of nuclear excited states is developed. This method is applied for an investigation of damping phenomena in the spherical nuclei with closed shells $^{208}$Pb and $^{132}$Sn. Since the phonon coupling terms enrich the RRPA spectrum with a multitude of $ph\\otimes$phonon components a noticeable fragmentation of the giant resonances is found, which is in full agreement with experimental data and with results of the semi-phenomenological non-relativistic approach.
A Self-Consistent Hubbard U Density-Functional Theory Approach...
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Self-Consistent Hubbard U Density-Functional Theory Approach to the Addition-Elimination Reactions of Hydrocarbons on Bare FeO A Self-Consistent Hubbard U Density-Functional Theory...
DFT Investigation of Osmium Terpyridinyl Complexes as Potential Optical Limiting Materials
Alok, Shashwat
2015-01-01T23:59:59.000Z
The development of optical power limiting materials is important to protect individuals or materials from intense laser irradiation. The photophysical behavior of Os(II) polypyridinyl complexes having aromatic hydrocarbon terpyridyl ligands has received considerable attention as systems exhibiting intramolecular energy transfer to yield a long excited states lifetime. Here we present a focused discussion to illustrate the photophysical behavior of transition metal complexes with modified terpyridyl ligands, utilizing density functional theory. Our DFT studies of the excited state behavior of Os(II) complexes containing pyrene-vinylene derived terpyridine (pyr-v-tpy) ligands can be applied to the development of optical limiting materials controlling the laser power at longer wavelength range.
Desnavi, Sameerah, E-mail: sameerah-desnavi@zhcet.ac.in [Department of Electronic Engineering, ZHCET, Aligarh Muslim University, Aligarh-202002 (India); Chakraborty, Brahmananda; Ramaniah, Lavanya M. [High Pressure and Synchrotron Radiation Physics Division, Bhabha Atomic Research Centre, Mumbai-400085 (India)
2014-04-24T23:59:59.000Z
The electronic structure and hydrogen storage capability of Yttrium-doped grapheme has been theoretically investigated using first principles density functional theory (DFT). Yttrium atom prefers the hollow site of the hexagonal ring with a binding energy of 1.40 eV. Doping by Y makes the system metallic and magnetic with a magnetic moment of 2.11 ?{sub B}. Y decorated graphene can adsorb up to four hydrogen molecules with an average binding energy of 0.415 eV. All the hydrogen atoms are physisorbed with an average desorption temperature of 530.44 K. The Y atoms can be placed only in alternate hexagons, which imply a wt% of 6.17, close to the DoE criterion for hydrogen storage materials. Thus, this system is potential hydrogen storage medium with 100% recycling capability.
Daubechies wavelets for linear scaling density functional theory
Mohr, Stephan [Institut für Physik, Universität Basel, Klingelbergstr. 82, 4056 Basel (Switzerland); Univ. Grenoble Alpes, INAC-SP2M, F-38000 Grenoble, France and CEA, INAC-SP2M, F-38000 Grenoble (France); Ratcliff, Laura E.; Genovese, Luigi; Caliste, Damien; Deutsch, Thierry [Univ. Grenoble Alpes, INAC-SP2M, F-38000 Grenoble, France and CEA, INAC-SP2M, F-38000 Grenoble (France); Boulanger, Paul [Univ. Grenoble Alpes, INAC-SP2M, F-38000 Grenoble, France and CEA, INAC-SP2M, F-38000 Grenoble (France); Institut Néel, CNRS and Université Joseph Fourier, B.P. 166, 38042 Grenoble Cedex 09 (France); Goedecker, Stefan [Institut für Physik, Universität Basel, Klingelbergstr. 82, 4056 Basel (Switzerland)
2014-05-28T23:59:59.000Z
We demonstrate that Daubechies wavelets can be used to construct a minimal set of optimized localized adaptively contracted basis functions in which the Kohn-Sham orbitals can be represented with an arbitrarily high, controllable precision. Ground state energies and the forces acting on the ions can be calculated in this basis with the same accuracy as if they were calculated directly in a Daubechies wavelets basis, provided that the amplitude of these adaptively contracted basis functions is sufficiently small on the surface of the localization region, which is guaranteed by the optimization procedure described in this work. This approach reduces the computational costs of density functional theory calculations, and can be combined with sparse matrix algebra to obtain linear scaling with respect to the number of electrons in the system. Calculations on systems of 10?000 atoms or more thus become feasible in a systematic basis set with moderate computational resources. Further computational savings can be achieved by exploiting the similarity of the adaptively contracted basis functions for closely related environments, e.g., in geometry optimizations or combined calculations of neutral and charged systems.
Jackson, Virgil E.; Gutowski, Keith E.; Dixon, David A.
2013-09-12T23:59:59.000Z
The structures, vibrational frequencies and energetics of anhydrous and hydrated complexes of UO2 2+ with the phosphate anions H2PO4 ?, HPO4 2?, and PO4 3? were predicted at the density functional theory (DFT) and MP2 molecular orbital theory levels as isolated gas phase species and in aqueous solution by using self-consistent reaction field (SCRF) calculations with different solvation models. The geometries and vibrational frequencies of the major binding modes for these complexes are compared to experiment where possible and good agreement is found. The uranyl moiety is nonlinear in many of the complexes, and the coordination number (CN) 5 in the equatorial plane is the predominant binding motif. The phosphates are found to bind in both monodentate and bidentate binding modes depending on the charge and the number of water molecules. The SCRF calculations were done with a variety of approaches, and different SCRF approaches were found to be optimal for different reaction types. The acidities of HxPO4 3?x in HxPO4 3?x(H2O)4, x = 0?3 complexes were calculated with different SCRF models and compared to experiment. Phosphate anions can displace water molecules from the first solvation shell at the uranyl exothermically. The addition of water molecules can cause the bonding of H2PO4 ? and HPO4 2? to change from bidentate to monodentate exothermically while maintaining CN 5. The addition of water can generate monodentate structures capable of cross-linking to other uranyl phosphates to form the types of structures found in the solid state. [UO2(HPO4)(H2O)3] is predicted to be a strong base in the gas phase and in aqueous solution. It is predicted to be a much weaker acid than H3PO4 in the gas phase and in solution.
Phonons and related crystal properties from density-functional perturbation theory
Wu, Zhigang
-Functional Perturbation Theory 516 A. Lattice dynamics from electronic-structure theory 516 B. Density-functional theory July 2001) This article reviews the current status of lattice-dynamical calculations in crystals, using specialized topics are treated, including the implementation for metals, the calculation of the response
Self-interaction corrections in density functional theory
Tsuneda, Takao, E-mail: ttsuneda@yamanashi.ac.jp [Fuel Cell Nanomaterials Center, University of Yamanashi, Kofu 400-0021 (Japan)] [Fuel Cell Nanomaterials Center, University of Yamanashi, Kofu 400-0021 (Japan); Hirao, Kimihiko [Computational Chemistry Unit, RIKEN Advanced Institute for Computational Science, Kobe, Hyogo 650-0047 (Japan)] [Computational Chemistry Unit, RIKEN Advanced Institute for Computational Science, Kobe, Hyogo 650-0047 (Japan)
2014-05-14T23:59:59.000Z
Self-interaction corrections for Kohn-Sham density functional theory are reviewed for their physical meanings, formulations, and applications. The self-interaction corrections get rid of the self-interaction error, which is the sum of the Coulomb and exchange self-interactions that remains because of the use of an approximate exchange functional. The most frequently used self-interaction correction is the Perdew-Zunger correction. However, this correction leads to instabilities in the electronic state calculations of molecules. To avoid these instabilities, several self-interaction corrections have been developed on the basis of the characteristic behaviors of self-interacting electrons, which have no two-electron interactions. These include the von Weizsäcker kinetic energy and long-range (far-from-nucleus) asymptotic correction. Applications of self-interaction corrections have shown that the self-interaction error has a serious effect on the states of core electrons, but it has a smaller than expected effect on valence electrons. This finding is supported by the fact that the distribution of self-interacting electrons indicates that they are near atomic nuclei rather than in chemical bonds.
Lao, Ka Un; Herbert, John M., E-mail: herbert@chemistry.ohio-state.edu [Department of Chemistry and Biochemistry, The Ohio State University, Columbus, Ohio 43210 (United States)
2014-01-28T23:59:59.000Z
The performance of second-order symmetry-adapted perturbation theory (SAPT) calculations using Kohn-Sham (KS) orbitals is evaluated against benchmark results for intermolecular interactions. Unlike previous studies of this “SAPT(KS)” methodology, the present study uses non-empirically tuned long-range corrected (LRC) functionals for the monomers. The proper v{sub xc} (r)?0 asymptotic limit is achieved by tuning the range separation parameter in order to satisfy the condition that the highest occupied KS energy level equals minus the molecule's ionization energy, for each monomer unit. Tests for He{sub 2}, Ne{sub 2}, and the S22 and S66 data sets reveal that this condition is important for accurate prediction of the non-dispersion components of the energy, although errors in SAPT(KS) dispersion energies remain unacceptably large. In conjunction with an empirical dispersion potential, however, the SAPT(KS) method affords good results for S22 and S66, and also accurately predicts the whole potential energy curve for the sandwich isomer of the benzene dimer. Tuned LRC functionals represent an attractive alternative to other asymptotic corrections that have been employed in density-functional-based SAPT calculations, and we recommend the use of tuned LRC functionals in both coupled-perturbed SAPT(DFT) calculations and dispersion-corrected SAPT(KS) calculations.
Ye, Jingyun; Liu, Changjun; Mei, Donghai; Ge, Qingfeng
2014-08-01T23:59:59.000Z
Methanol synthesis from CO2 hydrogenation on Pd4/In2O3 has been investigated using density functional theory (DFT) and microkinetic modeling. In this study, three possible routes in the reaction network of CO2 + H2 ? CH3OH + H2O have been examined. Our DFT results show that the HCOO route competes with the RWGS route whereas a high activation barrier kinetically blocks the HCOOH route. DFT results also suggest that H2COO* + H* ? H2CO* +OH* and cis-COOH* + H* ?CO* + H2O* are the rate limiting steps in the HCOO route and the RWGS route, respectively. Microkinetic modeling results demonstrate that the HCOO route is the dominant reaction route for methanol synthesis from CO2 hydrogenation. We found that the activation of H adatom on the small Pd cluster and the presence of H2O on the In2O3 substrate play important roles in promoting the methanol synthesis. The hydroxyl adsorbed at the interface of Pd4/In2O3 induces the transformation of the supported Pd4 cluster from a butterfly structure into a tetrahedron structure. This important structure change not only indicates the dynamical nature of the supported nanoparticle catalyst structure during the reaction but also shifts the final hydrogenation step from H2COH to CH3O.
Supplementary data for "Relativistic density functional theory modeling of plutonium and
Titov, Anatoly
Supplementary data for "Relativistic density functional theory modeling of plutonium and americium equilibrium geometries of plutonium and americium oxide molecules (standard .xyz files separated by empty
Liu Li; Li Yue; Farrar, James M. [Department of Chemistry, University of Rochester, Rochester, New York 14627 (United States)
2005-09-01T23:59:59.000Z
The reactions between O{sup -} and C{sub 2}H{sub 2} have been studied using the crossed-beam technique and density-functional theory (DFT) calculations in the collision energy range from 0.35 to 1.5 eV (34-145 kJ/mol). Both proton transfer and C-O bond formation are observed. The proton transfer channel forming C{sub 2}H{sup -} is the dominant pathway. The center-of-mass flux distributions of the C{sub 2}H{sup -} product ions are highly asymmetric, with maxima close to the velocity and direction of the precursor acetylene beam, characteristic of direct reactions. The reaction quantitatively transforms the entire reaction exothermicity into internal excitation of the products, consistent with mixed energy release in which the proton is transferred in a configuration in which both the breaking and the forming bonds are extended. The C-O bond formation channel producing HC{sub 2}O{sup -} displays a distinctive kinematic picture in which the product distribution switches from predominantly forward scattering with a weak backward peak to sideways scattering as the collision energy increases. At low collision energies, the reaction occurs through an intermediate that lives a significant fraction of a rotational period. The asymmetry in the distribution leads to a lifetime estimate of 600 fs, in reasonable agreement with DFT calculations showing that hydrogen-atom migration is rate limiting. At higher collision energies, the sideways-scattered products arise from repulsive energy release from a bent transition state.
Meng, Da; Zheng, Bin; Lin, Guang; Sushko, Maria L.
2014-08-29T23:59:59.000Z
We have developed efficient numerical algorithms for the solution of 3D steady-state Poisson-Nernst-Planck equations (PNP) with excess chemical potentials described by the classical density functional theory (cDFT). The coupled PNP equations are discretized by finite difference scheme and solved iteratively by Gummel method with relaxation. The Nernst-Planck equations are transformed into Laplace equations through the Slotboom transformation. Algebraic multigrid method is then applied to efficiently solve the Poisson equation and the transformed Nernst-Planck equations. A novel strategy for calculating excess chemical potentials through fast Fourier transforms is proposed which reduces computational complexity from O(N2) to O(NlogN) where N is the number of grid points. Integrals involving Dirac delta function are evaluated directly by coordinate transformation which yields more accurate result compared to applying numerical quadrature to an approximated delta function. Numerical results for ion and electron transport in solid electrolyte for Li ion batteries are shown to be in good agreement with the experimental data and the results from previous studies.
Department for Analysis and Computational Number Theory Additive functions and number systems
Department for Analysis and Computational Number Theory Additive functions and number systems systems April 7, 2010 1 / 35 #12;Department for Analysis and Computational Number Theory Outline Number and Computational Number Theory Number systems Let R be an integral domain, b R, and N = {n1, . . . , nm} R
Basic Theory in Construction of Boolean Functions with Maximum Possible Annihilator Immunity
International Association for Cryptologic Research (IACR)
Basic Theory in Construction of Boolean Functions with Maximum Possible Annihilator Immunity #3. In this paper we present a construction keeping in mind the basic theory of annihilator immunity the basic theory. Most importantly, the cryptographic properties of our constructions, such as nonlinearity
Basic Theory in Construction of Boolean Functions with Maximum Possible Annihilator Immunity
International Association for Cryptologic Research (IACR)
Basic Theory in Construction of Boolean Functions with Maximum Possible Annihilator Immunity Deepak present a construction keeping in mind the basic theory of annihilator immunity. This construction immunity that comes from the basic theory. Most importantly, the cryptographic properties of our
Electronvibration coupling in time-dependent density-functional theory: Application to benzene
Bertsch George F.
Electronvibration coupling in time-dependent density-functional theory: Application to benzene G://jcp.aip.org/about/rights_and_permissions #12;Electronvibration coupling in time-dependent density-functional theory: Application to benzene G for electronvibration coupling, we apply it to the optical properties of the * transitions in benzene
Density-Functional Theory and Quantum Chemistry Studies on "dry" and "wet"
Alavi, Ali
Density-Functional Theory and Quantum Chemistry Studies on "dry" and "wet" NaCl(001) vorgelegt von essential role as a food preserva- tive. However, many fundamental physical and chemical properties of Na), and defects on NaCl(001) surfaces have been examined with density-functional theory within the plane
Klaas J. H. Giesbertz
2015-06-16T23:59:59.000Z
A theorem for the invertibility of arbitrary response functions is presented under the following conditions: the time-dependence of the potentials should be Laplace transformable and the initial state should be a ground state, though it might be degenerate. This theorem provides a rigorous foundation for all density-functional-like theories in the time-dependent linear response regime. Especially for time-dependent one-body reduced density matrix (1RDM) functional theory this is an important step forward, since a solid foundation has currently been lacking. The theorem is equally valid for static response functions in the non-degenerate case, so can be used to characterize the uniqueness of the potential in the ground state version of the corresponding density-functional-like theory. Such a classification of the uniqueness of the non-local potential in ground state 1RDM functional theory has been lacking for decades. With the aid of presented invertibility theorem presented here, a complete classification of the non-uniqueness of the non-local potential in 1RDM functional theory can be given for the first time.
Liu Li; Li Yue; Farrar, James M. [Department of Chemistry, University of Rochester, Rochester, New York 14627 (United States)
2006-03-28T23:59:59.000Z
The proton transfer reaction between OH{sup -} and C{sub 2}H{sub 2}, the sole reactive process observed over the collision energy range from 0.37 to 1.40 eV, has been studied using the crossed beam technique and density-functional theory (DFT) calculations. The center of mass flux distributions of the product C{sub 2}H{sup -} ions at three different energies are highly asymmetric, characteristic of a direct process occurring on a time scale much less than a rotational period of any transient intermediate. The maxima in the flux distributions correspond to product velocities and directions close to those of the precursor acetylene reactants. The reaction quantitatively transforms the entire exothermicity into internal excitation of the products, consistent with an energy release motif in which the proton is transferred early, in a configuration in which the forming bond is extended. This picture is supported by DFT calculations showing that the first electrostatically bound intermediate on the reaction pathway is the productlike C{sub 2}H{sup -}{center_dot}H{sub 2}O species. Most of the incremental translational energy in the two higher collision energy experiments appears in product translational energy, and provides an example of induced repulsive energy release characteristic of the heavy+light-heavy mass combination.
Time-dependent Internal DFT formalism and Kohn-Sham scheme
J. Messud
2009-11-05T23:59:59.000Z
We generalize to the time-dependent case the stationary Internal DFT / Kohn-Sham formalism presented in Ref. [14]. We prove that, in the time-dependent case, the internal properties of a self-bound system (as an atomic nuclei) are all defined by the internal one-body density and the initial state. We set-up a time-dependent Internal Kohn-Sham scheme as a practical way to compute the internal density. The main difference with the traditional DFT / Kohn-Sham formalism is the inclusion of the center-of-mass correlations in the functional.
Moreira, E. [Departamento de Fisica Teorica e Experimental, Universidade Federal do Rio Grande do Norte, 59072-970 Natal-RN (Brazil); Henriques, J.M. [Centro de Educacao e Saude, Universidade Federal de Campina Grande, Campus Cuite, 58175-000 Cuite-PB (Brazil); Azevedo, D.L. [Departamento de Fisica, Universidade Federal do Maranhao, Centro de Ciencias Exatas e Tecnologia, 65085-580 Sao Luis-MA (Brazil); Departamento de Fisica Teorica e Experimental, Universidade Federal do Rio Grande do Norte, 59072-970 Natal-RN (Brazil); Caetano, E.W.S., E-mail: ewcaetano@gmail.co [Instituto Federal de Educacao, Ciencia e Tecnologia do Ceara, Av. 13 de Maio, 2081, Benfica, 60040-531 Fortaleza-CE (Brazil); Freire, V.N. [Departamento de Fisica, Universidade Federal do Ceara, Centro de Ciencias, Caixa Postal 6030, Campus do Pici, 60455-760 Fortaleza-CE (Brazil); Albuquerque, E.L. [Departamento de Biofisica e Farmacologia, Universidade Federal do Rio Grande do Norte, 59072-970 Natal-RN (Brazil)
2011-04-15T23:59:59.000Z
Orthorhombic SrSnO{sub 3} was investigated using density functional theory (DFT) considering both the local density and generalized gradient approximations, LDA and GGA, respectively. The electronic band structure, density of states, complex dielectric function, optical absorption, and the infrared and Raman spectra were computed. Calculated lattice parameters are close to the experimental measurements, and an indirect band gap E(S{yields}{Gamma})=1.97eV (2.27 eV) was obtained within the GGA (LDA) level of calculation. Effective masses for holes and electrons were estimated, being very anisotropic in comparison with similar results for orthorhombic CaSnO{sub 3}. The complex dielectric function and the optical absorption of SrSnO{sub 3} were shown to be sensitive to the plane of polarization of the incident light. The infrared spectrum between 100 and 600 cm{sup -1} was obtained, with its main peaks being assigned, and a nice agreement between experimental and theoretical peaks of the Raman spectrum of orthorhombic SrSnO{sub 3} was achieved. -- Graphical abstract: Orthorhombic SrSnO{sub 3}: a view of the unit cell (left) and plots showing the calculated and experimental Raman spectra (right). Display Omitted Research highlights: {yields} We have performed DFT calculations on orthorhombic SrSnO{sub 3} crystals, obtaining their structural, electronical and optical properties. {yields} An indirect band gap was obtained, and anisotropic effective masses were found for both electrons and holes. {yields} The complex dielectric function and the optical absorption of SrSnO{sub 3} were shown to be very sensitive to the plane of polarization of the incident light. {yields} The infrared spectrum between 100 and 600 cm{sup -1} was obtained, with its main peaks being assigned, and a nice agreement between experimental and theoretical peaks of the Raman spectrum was achieved.
A proximal gradient method for ensemble density functional theory
Michael Ulbrich
2015-04-23T23:59:59.000Z
Apr 23, 2015 ... Although the widely used self-consistent field iteration method can be extended to solve the minimization of the total energy functional with ...
Element orbitals for Kohn-Sham density functional theory
Lin, Lin; Ying, Lexing
2012-05-08T23:59:59.000Z
We present a method to discretize the Kohn-Sham Hamiltonian matrix in the pseudopotential framework by a small set of basis functions automatically contracted from a uniform basis set such as planewaves. Each basis function is localized around an element, which is a small part of the global domain containing multiple atoms. We demonstrate that the resulting basis set achieves meV accuracy for 3D densely packed systems with a small number of basis functions per atom. The procedure is applicable to insulating and metallic systems.
Green function identities in Euclidean quantum field theory
G. Sardanashvily
2006-04-01T23:59:59.000Z
Given a generic Lagrangian system of even and odd fields, we show that any infinitesimal transformation of its classical Lagrangian yields the identities which Euclidean Green functions of quantum fields satisfy.
Joint inversion of receiver function and ambient noise based on Bayesian theory
van der Hilst, Robert D.
In this study, we present a method for the joint inversion of receiver function and ambient noise based on Bayesian inverse theory (Tarantola, 1987, 2005). The nonlinear inversion method of the complex spectrum ratio of ...
Semiparametric functional data analysis for longitudinal/clustered data: theory and application
Hu, Zonghui
2006-04-12T23:59:59.000Z
: Statistics iii ABSTRACT Semiparametric Functional Data Analysis for Longitudinal/Clustered Data: Theory and Application. (December 2004) Zonghui Hu, B.S., Dalian University of Technology, Dalian, P.R.China; M.S., Dalian University of Technology, Dalian, P...
The three point function in Liouville and $\\mathcal{N}=1$ Super Liouville Theory
Tupia, Martín D Arteaga
2015-01-01T23:59:59.000Z
In this dissertation we present some basic features about Liouville and $\\mathcal{N}=1$ Super Liouville Theory, and focus in the computation of their three point functions. Additionally, we include an introduction to Conformal Field Theories (CFT) and Supersymmetry, which are the basic tools of the present research.
The three point function in Liouville and $\\mathcal{N}=1$ Super Liouville Theory
Martín D. Arteaga Tupia
2015-08-20T23:59:59.000Z
In this dissertation we present some basic features about Liouville and $\\mathcal{N}=1$ Super Liouville Theory, and focus in the computation of their three point functions. Additionally, we include an introduction to Conformal Field Theories (CFT) and Supersymmetry, which are the basic tools of the present research.
Partition Functions of Superconformal Chern-Simons Theories from Fermi Gas Approach
Sanefumi Moriyama; Tomoki Nosaka
2014-08-14T23:59:59.000Z
We study the partition function of three-dimensional ${\\mathcal N}=4$ superconformal Chern-Simons theories of the circular quiver type, which are natural generalizations of the ABJM theory, the worldvolume theory of M2-branes. In the ABJM case, it was known that the perturbative part of the partition function sums up to the Airy function as $Z(N)=e^{A}C^{-1/3}\\mathrm{Ai}[C^{-1/3}(N-B)]$ with coefficients $C$, $B$ and $A$ and that for the non-perturbative part the divergences coming from the coefficients of worldsheet instantons and membrane instantons cancel among themselves. We find that many of the interesting properties in the ABJM theory are extended to the general superconformal Chern-Simons theories. Especially, we find an explicit expression of $B$ for general ${\\mathcal N}=4$ theories, a conjectural form of $A$ for a special class of theories, and cancellation in the non-perturbative coefficients for the simplest theory next to the ABJM theory.
Improving the orbital-free density functional theory description of covalent materials
Carter, Emily A.
, Los Angele, Los Angeles, California 90095-1569 and Department of Mechanical and Aerospace Engineering-free-electron-like metals such as Al and its alloys, OF-DFT employing the WGC KEDF produces bulk properties in good
Nakata, Ayako; Tsuneda, Takao; Hirao, Kimihiko [Advanced Science Institute, RIKEN, Wako 351-0198 (Japan); CREST, Japan Science and Technology Agency, Kawaguchi 332-0012 (Japan)
2011-12-14T23:59:59.000Z
A long-range corrected (LC) time-dependent density functional theory (TDDFT) incorporating relativistic effects with spin-orbit couplings is presented. The relativistic effects are based on the two-component zeroth-order regular approximation Hamiltonian. Before calculating the electronic excitations, we calculated the ionization potentials (IPs) of alkaline metal, alkaline-earth metal, group 12 transition metal, and rare gas atoms as the minus orbital (spinor) energies on the basis of Koopmans' theorem. We found that both long-range exchange and spin-orbit coupling effects are required to obtain Koopmans' IPs, i.e., the orbital (spinor) energies, quantitatively in DFT calculations even for first-row transition metals and systems containing large short-range exchange effects. We then calculated the valence excitations of group 12 transition metal atoms and the Rydberg excitations of rare gas atoms using spin-orbit relativistic LC-TDDFT. We found that the long-range exchange and spin-orbit coupling effects significantly contribute to the electronic spectra of even light atoms if the atoms have low-lying excitations between orbital spinors of quite different electron distributions.
Silvestrelli, Pier Luigi
2015-01-01T23:59:59.000Z
The DFT/vdW-WF2s1 method, recently developed to include the van der Waals interactions in the Density Functional Theory and describe adsorption processes on metal surfaces by taking metal-screening effects into account, is applied to the case of the interaction of Xe and graphene with a transition-metal surface, namely Ni(111). In general the adsorption of rare-gas atoms on metal surfaces is important because is prototypical for physisorption processes. Moreover, the interaction of graphene with Ni(111) is of particular interest for practical applications (efficient and large-scale production of high-quality graphene) and, from a theoretical point of view, is particularly challenging, since it can be described by a delicate interplay between chemisorption and physisorption processes. The first-principles simulation of transition metals require particular care also because they can be viewed as intermediate systems between simple metals and insulating crystals. Even in these cases the method performs well as d...
U?ur, Gökay [Department of Physics, Faculty of Science, Gazi University, 06500 Ankara (Turkey); Candan, Abdullah [Central Research and Practice Laboratory (AH?LAB), Ahi Evran University, 40100 K?r?ehir (Turkey)
2014-10-06T23:59:59.000Z
First-principle calculations of structural, electronic, elastic and phonon properties of SnMg{sub 2}O{sub 4}, SnZn{sub 2}O{sub 4} and SnCd{sub 2}O{sub 4} compounds are presented, using the pseudo-potential plane waves approach based on density functional theory (DFT) within the generalized gradient approximation (GGA). The computed ground state structural parameters, i.e. lattice constants, internal free parameter and bulk modulus are in good agreement with the available theoretical results. Our calculated elastic constants are indicative of stability of SnX{sub 2}O{sub 4} (X=Mg, Zn, Cd) compounds in the spinel structure. The partial density of states (PDOS) of these compounds is in good agreement with the earlier ab-initio calculations. The phonon dispersion relations were calculated using the direct method. Phonon dispersion results indicate that SnZn{sub 2}O{sub 4} is dynamically stable, while SnMg{sub 2}O{sub 4} and SnCd{sub 2}O{sub 4} are unstable.
Likos, Christos N.
Density-functional theory of freezing of quantum liquids at zero temperature using exact liquid-functional theory to study the freezing of superfluid 4 He, charged bosons, and charged fermions at zero temperature-functional theory of freezing that involve linear response, all fail to correctly describe the crystalliza- tion
Alavi, Ali
On the accuracy of density-functional theory exchange-correlation functionals for H bonds in small for hydro- gen H bonds? What is the best exchange-correlation xc functional for treating H bonds? Questions
Uncertainty Quantification for Nuclear Density Functional Theory and
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:1 First Use of Energy for All Purposes (Fuel and Nonfuel), 2002; Level:5 TablesExports to3,1,50022,3,,0,,6,1,SeparationConnect1.08]Te[subscriptM-PACEResponses tocorrection.Theory (Conference) | SciTech
Uncertainty Quantification for Nuclear Density Functional Theory and
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:1 First Use of Energy for All Purposes (Fuel and Nonfuel), 2002; Level:5 TablesExports to3,1,50022,3,,0,,6,1,SeparationConnect1.08]Te[subscriptM-PACEResponses tocorrection.Theory (Conference) | SciTechInformation Content
Uncertainty Quantification for Nuclear Density Functional Theory and
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:1 First Use of Energy for All Purposes (Fuel and Nonfuel), 2002; Level:5 TablesExports to3,1,50022,3,,0,,6,1,SeparationConnect1.08]Te[subscriptM-PACEResponses tocorrection.Theory (Conference) | SciTechInformation
A Theory of Linear Fractional Transformations of Rational Functions
Reiter, Harold
functions, we say that g g if g = ax+b cx+d -1 g ax+b cx+d , where a b c d = 0. For practical purposes ax+b cx+d = ax + b, a linear function, our methods yield a large number of first level invariants and n i=0 Aixi and n i=0 Bixi have no roots in common. Also, g g if g = ax+b cx+d -1 g ax+b cx
Smoothness of the Gap Function in the BCS-Bogoliubov Theory of Superconductivity
Shuji Watanabe
2010-06-07T23:59:59.000Z
We deal with the gap equation in the BCS-Bogoliubov theory of superconductivity, where the gap function is a function of the temperature $T$ only. We show that the squared gap function is of class $C^2$ on the closed interval $[\\,0,\\,T_c\\,]$. Here, $T_c$ stands for the transition temperature. Furthermore, we show that the gap function is monotonically decreasing on $[0,\\,T_c]$ and obtain the behavior of the gap function at $T=T_c$. We mathematically point out some more properties of the gap function.
Function group approach to unconstrained Hamiltonian Yang-Mills theory
Antti Salmela
2005-09-07T23:59:59.000Z
Starting from the temporal gauge Hamiltonian for classical pure Yang-Mills theory with the gauge group SU(2) a canonical transformation is initiated by parametrising the Gauss law generators with three new canonical variables. The construction of the remaining variables of the new set proceeds through a number of intermediate variables in several steps, which are suggested by the Poisson bracket relations and the gauge transformation properties of these variables. The unconstrained Hamiltonian is obtained from the original one by expressing it in the new variables and then setting the Gauss law generators to zero. This Hamiltonian turns out to be local and it decomposes into a finite Laurent series in powers of the coupling constant.
The Gaussian Radial Basis Function Method for Plasma Kinetic Theory
Hirvijoki, Eero; Belli, Emily; Embréus, Ola
2015-01-01T23:59:59.000Z
A fundamental macroscopic description of a magnetized plasma is the Vlasov equation supplemented by the nonlinear inverse-square force Fokker-Planck collision operator [Rosenbluth et al., Phys. Rev., 107, 1957]. The Vlasov part describes advection in a six-dimensional phase space whereas the collision operator involves friction and diffusion coefficients that are weighted velocity-space integrals of the particle distribution function. The Fokker-Planck collision operator is an integro-differential, bilinear operator, and numerical discretization of the operator is far from trivial. In this letter, we describe a new approach to discretize the entire kinetic system based on an expansion in Gaussian Radial Basis functions (RBFs). This approach is particularly well-suited to treat the collision operator because the friction and diffusion coefficients can be analytically calculated. Although the RBF method is known to be a powerful scheme for the interpolation of scattered multidimensional data, Gaussian RBFs also...
Theory and Application of Linear Supply Function Equilibrium in Electricity Markets
Baldick, Ross
Theory and Application of Linear Supply Function Equilibrium in Electricity Markets Ross Baldick Department of Electrical and Computer Engineering, The University of Texas at Austin, 1 University Station C equilibrium (SFE) model of interaction in an electricity market. We assume a linear demand function
DiLabio, Gino A., E-mail: Gino.DiLabio@nrc.ca [National Institute for Nanotechnology, National Research Council of Canada, 11421 Saskatchewan Drive, Edmonton, Alberta T6G 2M9 (Canada); Department of Chemistry, University of British Columbia, Okanagan, 3333 University Way, Kelowna, British Columbia V1V 1V7 (Canada); Koleini, Mohammad [National Institute for Nanotechnology, National Research Council of Canada, 11421 Saskatchewan Drive, Edmonton, Alberta T6G 2M9 (Canada) [National Institute for Nanotechnology, National Research Council of Canada, 11421 Saskatchewan Drive, Edmonton, Alberta T6G 2M9 (Canada); Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta T6G 2V4 (Canada)
2014-05-14T23:59:59.000Z
Dispersion-correcting potentials (DCPs) are atom-centered Gaussian functions that are applied in a manner that is similar to effective core potentials. Previous work on DCPs has focussed on their use as a simple means of improving the ability of conventional density-functional theory methods to predict the binding energies of noncovalently bonded molecular dimers. We show in this work that DCPs developed for use with the LC-?PBE functional along with 6-31+G(2d,2p) basis sets are capable of simultaneously improving predicted noncovalent binding energies of van der Waals dimer complexes and covalent bond dissociation enthalpies in molecules. Specifically, the DCPs developed herein for the C, H, N, and O atoms provide binding energies for a set of 66 noncovalently bonded molecular dimers (the “S66” set) with a mean absolute error (MAE) of 0.21 kcal/mol, which represents an improvement of more than a factor of 10 over unadorned LC-?PBE/6-31+G(2d,2p) and almost a factor of two improvement over LC-?PBE/6-31+G(2d,2p) used in conjunction with the “D3” pairwise dispersion energy corrections. In addition, the DCPs reduce the MAE of calculated X-H and X-Y (X,Y = C, H, N, O) bond dissociation enthalpies for a set of 40 species from 3.2 kcal/mol obtained with unadorned LC-?PBE/6-31+G(2d,2p) to 1.6 kcal/mol. Our findings demonstrate that broad improvements to the performance of DFT methods may be achievable through the use of DCPs.
Molecular Density Functional Theory for water with liquid-gas coexistence and correct pressure
Jeanmairet, Guillaume; Sergiievskyi, Volodymyr; Borgis, Daniel
2015-01-01T23:59:59.000Z
The solvation of hydrophobic solutes in water is special because liquid and gas are almost at coexistence. In the common hypernetted chain approximation to integral equations, or equivalently in the homogenous reference fluid of molecular density functional theory, coexistence is not taken into account. Hydration structures and energies of nanometer-scale hydrophobic solutes are thus incorrect. In this article, we propose a bridge functional that corrects this thermodynamic inconsistency by introducing a metastable gas phase for the homogeneous solvent. We show how this can be done by a third order expansion of the functional around the bulk liquid density that imposes the right pressure and the correct second order derivatives. Although this theory is not limited to water, we apply it to study hydrophobic solvation in water at room temperature and pressure and compare the results to all-atom simulations. With this correction, molecular density functional theory gives, at a modest computational cost, quantita...
Fluid - solid transition in simple systems using density functional theory
Atul S. Bharadwaj; Yashwant Singh
2014-11-24T23:59:59.000Z
A free energy functional for a crystal proposed by Singh and Singh (Europhysics Letters \\textbf{88}, 16005 (2009)) which contains both the symmetry-conserved and symmetry-broken parts of the direct pair correlation function has been used to investigate the fluid-solid transition in systems interacting via purely repulsive WCA Lennard - Jones (RLJ) potential and the full Lennard - Jones (LJ) potential. The results found for freezing parameters for the fluid - face centred cubic (fcc) crystal transition are in very good agreement with simulation results. It is shown that although the contribution made by the symmetry broken part to the grand thermodynamic potential at the freezing point is small compared to that of the symmetry conserving part, its role is crucial in stabilizing the crystalline structure and on values of freezing parameters. The effect of attractive part of the LJ potential on the freezing parameters is found to be small, confirming the view that the fluid - solid transition is primarily determined by the repulsive part of the potential.
Minasian, Stefan G.; Keith, Jason M.; Batista, Enrique R.; Boland, Kevin S.; Clark, David L.; Conradson, Steven D.; Kozimor, Stosh A.; Martin, Richard L.; Schwarz, Daniel E.; Shuh, David K.; Wagner, Gregory L.; Wilkerson, Marianne P.; Wolfsberg, Laura E.; Yang, Ping
2012-03-09T23:59:59.000Z
Chlorine K-edge X-ray absorption spectroscopy (XAS) and ground-state and time-dependent hybrid density functional theory (DFT) were used to probe electronic structure for O{sub h}-MCl{sub 6}{sup 2-}(M = Ti, Zr, Hf, U) and C{sub 4v}-UOCl{sub 5}{sup -}, and to determine the relative contributions of valence 3d, 4d, 5d, 6d, and 5f orbitals in M-Cl bonding. Spectral interpretations were guided by time-dependent DFT calculated transition energies and oscillator strengths, which agree well with the experimental XAS spectra. The data provide new spectroscopic evidence for the involvement of both 5f and 6d orbitals in actinide-ligand bonding in UCl{sub 6}{sup 2-}. For the MCl{sub 6}{sup 2-}, where transitions into d orbitals of t{sub 2g} symmetry are spectroscopically resolved for all four complexes, the experimentally determined Cl 3p character per M-Cl bond increases from 8.3(4)% (TiCl{sub 6}{sup 2-}) to 10.3(5)% (ZrCl{sub 6}{sup 2-}), 12(1)% (HfCl{sub 6}{sup 2-}), and 26 18(1)% (UCl{sub 6}{sup 2-}). Chlorine K-edge XAS spectra of UOCl{sub 5}{sup -} provide additional insights into the transition assignments by 27 lowering the symmetry to C{sub 4v}, where five pre-edge transitions into both 5f and 6d orbitals are observed. For UCl{sub 6}{sup 2-}, the XAS data 28 suggest that orbital mixing associated with the U 5f orbitals is considerably lower than that of the U 6d orbitals. For both UCl{sub 6}{sup 2-}29 and UOCl{sub 5}{sup -}, the ground-state DFT calculations predict a larger 5f contribution to bonding than is determined experimentally. 30 These findings are discussed in the context of conventional theories of covalent bonding for d- and f-block metal complexes.
Glueball Wave Functions in U(1) Lattice Gauge Theory
Mushtaq Loan; Yi Ying
2006-06-26T23:59:59.000Z
Standard Monte Carlo simulations have been performed for 3-dimensional U(1) lattice gauge model on improved lattices to measure the wavefunction and size of the scalar and the tensor glueballs. Our results show the radii of ~ 0.60 and ~ 1.12 in the units of string tension, or ~0.28 and ~0.52 fm, for the scalar and tensor glueballs, respectively. At finite temperature we see clear evidence of the deconfined phase, and the transition appears to be similar to that of the two-dimensional XY model as expected from universality arguments. Preliminary results show no significant changes in the glueball wave functions and the masses in the deconfined phase.
Effective field theory for dilute fermions with pairing
Furnstahl, R.J. [Department of Physics, Ohio State University, Columbus, OH 43210 (United States)], E-mail: furnstahl.1@osu.edu; Hammer, H.-W. [Helmholtz-Institut fuer Strahlen- und Kernphysik (Theorie), Universitaet Bonn, Nussallee 14-16, D-53115 Bonn (Germany)], E-mail: hammer@itkp.uni-bonn.de; Puglia, S.J. [SBIG PLC, Berkeley Square House, London W1J 6BR (United Kingdom)], E-mail: spuglia@sbiguk.com
2007-11-15T23:59:59.000Z
Effective field theory (EFT) methods for a uniform system of fermions with short-range, natural interactions are extended to include pairing correlations, as part of a program to develop a systematic Kohn-Sham density functional theory (DFT) for medium and heavy nuclei. An effective action formalism for local composite operators leads to a free-energy functional that includes pairing by applying an inversion method order by order in the EFT expansion. A consistent renormalization scheme is demonstrated for the uniform system through next-to-leading order, which includes induced-interaction corrections to pairing.
Boccia, A.; Lanzilotto, V.; Marrani, A. G.; Zanoni, R. [Dipartimento di Chimica, Universita degli Studi di Roma ''La Sapienza'', piazzale Aldo Moro 5, I-00185 Rome (Italy); Stranges, S. [Dipartimento di Chimica, Universita degli Studi di Roma ''La Sapienza'', piazzale Aldo Moro 5, I-00185 Rome (Italy); IOM-CNR, Laboratorio TASC, I-34149 Basovizza, Trieste (Italy); Alagia, M. [IOM-CNR, Laboratorio TASC, I-34149 Basovizza, Trieste (Italy); Fronzoni, G.; Decleva, P. [Dipartimento di Scienze Chimiche, Universita di Trieste, Via L. Giorgieri 1, I-34127 Trieste, Italy and IOM-CNR Democritos, Trieste (Italy)
2012-04-07T23:59:59.000Z
We present the results of an experimental and theoretical investigation of monosubstituted ethyl-, vinyl-, and ethynyl-ferrocene (EtFC, VFC, and EFC) free molecules, obtained by means of synchrotron-radiation based C 1s photoabsorption (NEXAFS) and photoemission (C 1s XPS) spectroscopies, and density functional theory (DFT) calculations. Such a combined study is aimed at elucidating the role played by the C-C bond unsaturation degree of the substituent on the electronic structure of the ferrocene derivatives. Such substituents are required for molecular chemical anchoring onto relevant surfaces when ferrocenes are used for molecular electronics hybrid devices. The high resolution C 1s NEXAFS spectra exhibit distinctive features that depend on the degree of unsaturation of the hydrocarbon substituent. The theoretical approach to consider the NEXAFS spectrum made of three parts allowed to disentangle the specific contribution of the substituent group to the experimental spectrum as a function of its unsaturation degree. C 1s IEs were derived from the experimental data analysis based on the DFT calculated IE values for the different carbon atoms of the substituent and cyclopentadienyl (Cp) rings. Distinctive trends of chemical shifts were observed for the substituent carbon atoms and the substituted atom of the Cp ring along the series of ferrocenes. The calculated IE pattern was rationalized in terms of initial and final state effects influencing the IE value, with special regard to the different mechanism of electron conjugation between the Cp ring and the substituent, namely the {sigma}/{pi} hyperconjugation in EtFC and the {pi}-conjugation in VFC and EFC.
Simple regularization scheme for multi-reference density functional theories
Wojciech Satula; Jacek Dobaczewski
2014-07-03T23:59:59.000Z
Background: Extensions of single-reference (SR) energy-density-functionals (EDFs) to multi-reference (MR) applications involve using the generalized Wick theorem (GWT), which leads to singular energy kernels that cannot be properly integrated to restore symmetries, unless the EDFs are generated by true interactions. Purpose: We propose a new method to regularize the MR EDFs, which is based on using auxiliary quantities obtained by multiplying the kernels with appropriate powers of overlaps. Methods: Regularized matrix elements of two-body interactions are obtained by integrating the auxiliary quantities and then solving simple linear equations. Results: We implement the new regularization method within the self-consistent Skyrme-Hartree-Fock approach and we perform a proof-of-principle angular-momentum projection (AMP) of states in odd-odd nucleus 26Al. We show that for EDFs generated by true interactions, our regularization method gives results identical to those obtained within the standard AMP procedure. We also show that for EDFs that do not correspond to true interactions, it gives stable and converging results that are different than unstable and non-converging standard AMP values. Conclusions: The new regularization method proposed in this work may provide us with a relatively inexpensive and efficient tool to generalize SR EDFs to MR applications, thus allowing for symmetry restoration and configuration mixing performed for typical nuclear EDFs, which most often do not correspond to true interactions.
Telnov, Dmitry A.; Chu, Shih-I
2000-12-13T23:59:59.000Z
In the framework of the Floquet formulation of time-dependent density functional theory we present several exact relations involving different parts of the quasienergy functional. These relations hold when the exact densities ...
Kozimor, Stosh A.; Yang, Ping; Batista, Enrique R.; Boland, Kevin S.; Burns, Carol J.; Clark, David L.; Conradson, Steven D.; Martin, Richard L.; Wikerson, Marianne P.; Wolfsberg, Laura E.
2009-09-02T23:59:59.000Z
We describe the use of Cl K-edge X-ray Absorption Spectroscopy (XAS) and both ground state and time-dependent hybrid density functional theory (DFT) to probe electronic structure and determine the degree of orbital mixing in M-Cl bonds for (C5Me5)2MCl2 (M = Ti, 1; Zr, 2; Hf, 3; Th, 4; and U, 5), where we can directly compare a class of structurally similar compounds for d- and f-elements. We report direct experimental evidence for covalency in M-Cl bonding, including actinides, and offer insight into the relative roles of the valence f- and dorbitals in these systems. The Cl K-edge XAS data for the group IV transition metals, 1 – 3, show slight decreases in covalency in M-Cl bonding with increasing principal quantum number, in the order Ti > Zr > Hf. The percent Cl 3p character per M-Cl bond was experimentally determined to be 25, 23, and 22% per M-Cl bond for 1-3, respectively. For actinides, we find a shoulder on the white line for (C5Me5)2ThCl2, 4, and distinct, but weak pre-edge features for 2 (C5Me5)2UCl2, 5. The percent Cl 3p character in Th-Cl bonds in 4 was determined to be 14 %, with high uncertainty, while the U-Cl bonds in 5 contains 9 % Cl 3p character. The magnitudes of both values are approximately half what was observed for the transition metal complexes in this class of bent metallocene dichlorides. Using the hybrid DFT calculations as a guide to interpret the experimental Cl K-edge XAS, these experiments suggest that when evaluating An- Cl bonding, both 5f- and 6d-orbitals should be considered. For (C5Me5)2ThCl2, the calculations and XAS indicate that the 5f- and 6d-orbitals are nearly degenerate and heavily mixed. In contrast, the 5f- and 6d-orbitals in (C5Me5)2UCl2 are no longer degenerate, and fall in two distinct energy groupings. The 5f-orbitals are lowest in energy and split into a 5-over-2 pattern with the high lying U 6d-orbitals split in a 4-over-1 pattern, the latter of which is similar to the dorbital splitting in group IV transition metal (C5R5)2MCl2 (R = H, Me) compounds. Time dependent-DFT (TD-DFT) was used to calculate the energies and intensities of Cl 1s transitions into empty metal based orbitals containing Cl 3p character, and provide simulated Cl K-edge XAS spectra for 1 - 4. However, for 5, which has two unpaired electrons, analogous information was obtained from transition dipole calculations using ground state Kohn-Sham orbitals. The simulations provide additional confidence in the interpretation of spectra based on ground state calculations. Overall, this study demonstrates that Cl K-edge XAS and DFT calculations represent powerful tools that can be used to evaluate electronic structure and covalency in actinide metal-ligand bonding. In addition, these results provide a framework that can be used in future studies to evaluate actinide covalency in compounds that contain transuranic elements.
Geometry of Spin and Spin^c structures in the M-theory partition function
Hisham Sati
2012-04-01T23:59:59.000Z
We study the effects of having multiple Spin structures on the partition function of the spacetime fields in M-theory. This leads to a potential anomaly which appears in the eta-invariants upon variation of the Spin structure. The main source of such spaces are manifolds with nontrivial fundamental group, which are also important in realistic models. We extend the discussion to the Spin^c case and find the phase of the partition function, and revisit the quantization condition for the C-field in this case. In type IIA string theory in ten dimensions, the mod 2 index of the Dirac operator is the obstruction to having a well-defined partition function. We geometrically characterize manifolds with and without such an anomaly and extend to the case of nontrivial fundamental group. The lift to KO-theory gives the alpha-invariant, which in general depends on the Spin structure. This reveals many interesting connection to positive scalar curvature manifolds and constructions related to the Gromov-Lawson-Rosenberg conjecture. In the twelve-dimensional theory bounding M-theory, we study similar geometric questions, including choices of metrics and obtaining elements of K-theory in ten dimensions by pushforward in K-theory on the disk fiber. We interpret the latter in terms of the families index theorem for Dirac operators on the M-theory circle and disk. This involves superconnections, eta-forms, and infinite-dimensional bundles, and gives elements in Deligne cohomology in lower dimensions. We illustrate our discussion with many examples throughout.
Four-point correlation function of stress-energy tensors in N=4 superconformal theories
Korchemsky, G P
2015-01-01T23:59:59.000Z
We derive the explicit expression for the four-point correlation function of stress-energy tensors in four-dimensional N=4 superconformal theory. We show that it has a remarkably simple and suggestive form allowing us to predict a large class of four-point correlation functions involving the stress-energy tensor and other conserved currents. We then apply the obtained results on the correlation functions to computing the energy-energy correlations, which measure the flow of energy in the final states created from the vacuum by a source. We demonstrate that they are given by a universal function independent of the choice of the source. Our analysis relies only on N=4 superconformal symmetry and does not use the dynamics of the theory.
Qian Zhao; Bao Yuan Sun; Wen Hui Long
2014-11-23T23:59:59.000Z
The isospin coupling-channel decomposition of the potential energy density functional is carried out within the covariant density functional theory, and their isospin and density dependence in particular the influence on the symmetry energy is studied. It is found that both isospin-singlet and isospin-triplet components of the potential energy play the dominant role in deciding the symmetry energy, especially when the Fock diagram is introduced. The results illustrate a quite different mechanism to the origin of the symmetry energy from the microscopic Brueckner-Hartree-Fock theory, and demonstrate the importance of the Fork diagram in the CDF theory, especially from the isoscalar mesons, in the isospin properties of the in-medium nuclear force at high density.
A Density Functional Theory Study of Hydrogen Adsorption in MOF-5 Tim Mueller and Gerbrand Ceder*
Ceder, Gerbrand
. The effect of the framework on the physical structure and electronic structure of the organic linker initio molecular dynamics in the generalized gradient approximation to density functional theory, and calculations indicate that the sites with the strongest interaction with hydrogen are located near the Zn4O
Relativistic density functional theory modeling of plutonium and americium higher oxide molecules
Titov, Anatoly
Relativistic density functional theory modeling of plutonium and americium higher oxide molecules of plutonium and americium higher oxide molecules Andréi Zaitsevskii,1,2,a) Nikolai S. Mosyagin,2,3 Anatoly V of plutonium and americium higher oxide molecules (actinide oxidation states VI through VIII) by two
The Rise of Solitons in Sine-Gordon Field Theory: From Jacobi Amplitude to Gudermannian Function
Leonardo Mondaini
2014-11-20T23:59:59.000Z
We show how the famous soliton solution of the classical sine-Gordon field theory in $(1+1)$-dimensions may be obtained as a particular case of a solution expressed in terms of the Jacobi amplitude, which is the inverse function of the incomplete elliptic integral of the first kind.
Electronvibration coupling in time-dependent density-functional theory: Application to benzene
Bertsch George F.
Electronvibration coupling in time-dependent density-functional theory: Application to benzene G for electronvibration coupling, we apply it to the optical properties of the * transitions in benzene with the electronic excitations. In this work, we have chosen the benzene model for an exploratory study
Relative stability of nanosized wurtzite and graphitic ZnO from density functional theory
Melnik, Roderick
Relative stability of nanosized wurtzite and graphitic ZnO from density functional theory Bin Wen to determine the relative stability of wurtzite and graphitic phases of ZnO nanostructures. Our results the threshold number, the relative stability of the wurtzite phase is observed. Finally, we discuss
Freezing of 4 He and its liquid-solid interface from density functional theory
Caupin, Frédéric
Freezing of 4 He and its liquid-solid interface from density functional theory F. Ancilotto,1 M of the method that accurately describes the solid phase and the freezing transition of liquid 4 He at zero phenomenon of crystallization waves, i.e., melting-freezing waves which can easily propagate on the liquid
Linear Algebraic Calculation of Green's function for Large-Scale Electronic Structure Theory
Hoshi, Takeo
Linear Algebraic Calculation of Green's function for Large-Scale Electronic Structure Theory R (Dated: March 2, 2006) A linear algebraic method named the shifted conjugate-orthogonal-conjugate-gradient method is introduced for large-scale electronic structure calculation. The method gives an iterative
Gautam, P.; Gautam, D.; Chaudhary, R. P., E-mail: rpchaudhary65@gmail.com [Sant Longowal Institute of Engineering and Technology, Department of Chemistry (India)
2013-12-15T23:59:59.000Z
The title compound N-(4-acetyl-5,5-dimethyl-4,5-dihydro-1,3,4-thiadiazol-2-yl)acetamide (III) was obtained from the reaction of 2-(propan-2-ylidene)hydrazinecarbothioamide (II) with acetic anhydride instead of formation of the desired thiosemcarbazide derivative of Meldrum acid. The structures of II and III were established by elemental analysis, IR, NMR, Mass and X-ray crystallographic studies. II crystallizes in triclinic system, sp. gr. P-bar1 Z = 2; III crystallizes in the monoclinic system, sp. gr. P2{sub 1}/c, Z = 8. Density functional theory (DFT) calculations have been carried out for III. {sup 1}H and {sup 13}C NMR of III has been calculated and correlated with experimental results.
Correlation functions of the energy-momentum tensor in SU(2) gauge theory at finite temperature
Huebner, K; Pica, C
2008-01-01T23:59:59.000Z
We calculate correlation functions of the energy-momentum tensor in the vicinity of the deconfinement phase transition of (3+1)-dimensional SU(2) gauge theory and discuss their critical behavior in the vicinity of the second order deconfinement transition. We show that correlation functions of the trace of the energy momentum tensor diverge uniformly at the critical point in proportion to the specific heat singularity. Correlation functions of the pressure, on the other hand, stay finite at the critical point. We discuss the consequences of these findings for the analysis of transport coefficients, in particular the bulk viscosity, in the vicinity of a second order phase transition point.
Senjean, Bruno; Jensen, Hans Jørgen Aa; Fromager, Emmanuel
2015-01-01T23:59:59.000Z
The computation of excitation energies in range-separated ensemble density-functional theory (DFT) is discussed. The latter approach is appealing as it enables the rigorous formulation of a multi-determinant state-averaged DFT method. In the exact theory, the short-range density functional, that complements the long-range wavefunction-based ensemble energy contribution, should vary with the ensemble weights even when the density is held fixed. This weight dependence ensures that the range-separated ensemble energy varies linearly with the ensemble weights. When the (weight-independent) ground-state short-range exchange-correlation functional is used in this context, curvature appears thus leading to an approximate weight-dependent excitation energy. In order to obtain unambiguous approximate excitation energies, we simply propose to interpolate linearly the ensemble energy between equiensembles. It is shown that such a linear interpolation method (LIM) effectively introduces weight dependence effects. LIM has...
P. H. -L. Sit; Matteo Cococcioni; Nicola Marzari
2007-01-12T23:59:59.000Z
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.
Carter, Emily A.
2012-01-01T23:59:59.000Z
, Princeton, New Jersey 08544, USA Emily A. Carter Departments of Mechanical and Aerospace Engineering. However, OF-DFT Ag-Al alloy properties differ substantially from those predicted by KS-DFT using nonlocal is that when the system contains many different elements, such as in complex metal alloys, it becomes difficult
Dynamical density functional theory for the diffusion of injected Brownian particles
H. Löwen; M. Heinen
2014-09-08T23:59:59.000Z
While the theory of diffusion of a single Brownian particle in confined geometries is well-established by now, we discuss here the theoretical framework necessary to generalize the theory of diffusion to dense suspensions of strongly interacting Brownian particles. Dynamical density functional theory (DDFT) for classical Brownian particles represents an ideal tool for this purpose. After outlining the basic ingredients to DDFT we show that it can be readily applied to flowing suspensions with time-dependent particle sources. Particle interactions lead to considerable layering in the mean density profiles, a feature that is absent in the trivial case of noninteracting, freely diffusing particles. If the particle injection rate varies periodically in time with a suitable frequency, a resonance in the layering of the mean particle density profile is predicted.
The three-loop beta function in SU(N) lattice gauge theories
B. Alles; A. Feo; H. Panagopoulos
1996-09-11T23:59:59.000Z
We calculate the third coefficient of the lattice $\\beta$ function in pure Yang-Mills theory. We make use of a computer code for solving perturbation theory analytically on the lattice. We compute the divergent integrals by using a method based on a Taylor expansion of the integrand in powers of the external momenta in $4 - \\epsilon$ dimensions. Our results are in agreement with a previous calculation by M. L\\"uscher and P. Weisz where the authors used a different technique. We also show how this new coefficient modifies the scaling function on the lattice in both the standard and energy schemes. In particular we show that asymptotic scaling is extremely well achieved in the energy scheme.
Computationally efficient double hybrid density functional theory using dual basis methods
Byrd, Jason N
2015-01-01T23:59:59.000Z
We examine the application of the recently developed dual basis methods of Head-Gordon and co-workers to double hybrid density functional computations. Using the B2-PLYP, B2GP-PLYP, DSD-BLYP and DSD-PBEP86 density functionals, we assess the performance of dual basis methods for the calculation of conformational energy changes in C$_4$-C$_7$ alkanes and for the S22 set of noncovalent interaction energies. The dual basis methods, combined with resolution-of-the-identity second-order M{\\o}ller-Plesset theory, are shown to give results in excellent agreement with conventional methods at a much reduced computational cost.
A density functional theory study of electric potential saturation: planar geometry
Gabriel Tellez; Emmanuel Trizac
2003-08-01T23:59:59.000Z
We investigate the possibility of electrostatic potential saturation, which may lead to the phenomenon of effective charge saturation. The system under study is a uniformly charged infinite plane immersed in an arbitrary electrolyte made up of several micro-species. To describe the electric double layer, we use a generic density functional theory in which the local micro-ionic density profiles are arbitrary functions of the local electrostatic potential. A necessary and sufficient condition is obtained for saturation, whereby the electrostatic potential created by the plane becomes independent of its bare charge, provided the latter is large enough.
Steam Reforming on Transition-metal Carbides from Density-functional Theory
Vojvodic, Aleksandra
2012-05-11T23:59:59.000Z
A screening study of the steam reforming reaction on clean and oxygen covered early transition-metal carbides surfaces is performed by means of density-functional theory calculations. It is found that carbides provide a wide spectrum of reactivities, from too reactive via suitable to too inert. Several molybdenum-based systems are identified as possible steam reforming catalysts. The findings suggest that carbides provide a playground for reactivity tuning, comparable to the one for pure metals.
Density functional theory of freezing for soft interactions in two dimensions
Sven van Teeffelen; Christos N. Likos; Norman Hoffmann; Hartmut Löwen
2006-04-18T23:59:59.000Z
A density functional theory of two-dimensional freezing is presented for a soft interaction potential that scales as inverse cube of particle distance. This repulsive potential between parallel, induced dipoles is realized for paramagnetic colloids on an interface, which are additionally exposed to an external magnetic field. An extended modified weighted density approximation which includes correct triplet correlations in the liquid state is used. The theoretical prediction of the freezing transition is in good agreement with experimental and simulation data.
Lee, Jui-Che; Lin, Shiang-Tai
2015-01-01T23:59:59.000Z
The exciton binding energy, the energy required to dissociate an excited electron-hole pair into free charge carriers, is one of the key factors to the optoelectronic performance of organic materials. However, it remains unclear whether modern quantum-mechanical calculations, mostly based on Kohn-Sham density functional theory (KS-DFT) and time-dependent density functional theory (TDDFT), are reliably accurate for exciton binding energies. In this study, the exciton binding energies and related optoelectronic properties (e.g., the ionization potentials, electron affinities, fundamental gaps, and optical gaps) of 121 small- to medium-sized molecules are calculated using KS-DFT and TDDFT with various density functionals. Our KS-DFT and TDDFT results are compared with those calculated using highly accurate CCSD and EOM-CCSD methods, respectively. The omegaB97, omegaB97X, and omegaB97X-D functionals are shown to generally outperform (with a mean absolute error of 0.36 eV) other functionals for the properties inve...
Dynamic density functional theory of protein adsorption on polymer-coated nanoparticles
Angioletti-Uberti, Stefano; Dzubiella, Joachim
2014-01-01T23:59:59.000Z
We present a theoretical model for the description of the adsorption kinetics of globular proteins onto charged core-shell microgel particles based on Dynamic Density Functional Theory (DDFT). This model builds on a previous description of protein adsorption thermodynamics [Yigit \\textit{et al}, Langmuir 28 (2012)], shown to well interpret the available calorimetric experimental data of binding isotherms. In practice, a spatially-dependent free-energy functional including the same physical interactions is built, and used to study the kinetics via a generalised diffusion equation. To test this model, we apply it to the case study of Lysozyme adsorption on PNIPAM coated nanoparticles, and show that the dynamics obtained within DDFT is consistent with that extrapolated from experiments. We also perform a systematic study of the effect of various parameters in our model, and investigate the loading dynamics as a function of proteins' valence and hydrophobic adsorption energy, as well as their concentration and th...
Large-order perturbation theory for the electromagnetic current-current correlation function
Brown, L.S.; Yaffe, L.G.; Zhai, C. (Department of Physics, FM-15, University of Washington, Seattle, Washington 98195 (United States))
1992-11-15T23:59:59.000Z
The constraints imposed by asymptotic freedom and analyticity on the large-order behavior of perturbation theory for the electromagnetic current-current correlation function are examined. By suitably applying the renormalization group, the coefficients of the asymptotic expansion in the deep Euclidean region may be expressed explicitly in terms of the perturbative coefficients of the Minkowski space discontinuity (the {ital R} ratio in {ital e}{sup +}{ital e{minus}} scattering). This relation yields a generic'' prediction for the large-order behavior of the Euclidean perturbation series and suggests the presence of nonperturbative 1/{ital q}{sup 2} correction in the Euclidean correlation function. No such generic'' prediction can be made for the physically measurable {ital R} ratio. A novel functional method is developed to obtain these results.
Boyer, Edmond
case in which coupled cluster theory is used to obtain the density and excitation energies for benchmark and highly accurate studies, they are still too demanding for standard applications. Another
Analytic cubic and quartic force fields using density-functional theory
Ringholm, Magnus; Gao, Bin; Thorvaldsen, Andreas J.; Ruud, Kenneth [Centre for Theoretical and Computational Chemistry (CTCC), Department of Chemistry, University of Tromsø—The Arctic University of Norway, 9037 Tromsø (Norway)] [Centre for Theoretical and Computational Chemistry (CTCC), Department of Chemistry, University of Tromsø—The Arctic University of Norway, 9037 Tromsø (Norway); Jonsson, Dan [Centre for Theoretical and Computational Chemistry (CTCC), Department of Chemistry, University of Tromsø—The Arctic University of Norway, 9037 Tromsø (Norway) [Centre for Theoretical and Computational Chemistry (CTCC), Department of Chemistry, University of Tromsø—The Arctic University of Norway, 9037 Tromsø (Norway); High Performance Computing Group, University of Tromsø—The Arctic University of Norway, 9037 Tromsø (Norway); Bast, Radovan [Theoretical Chemistry and Biology, School of Biotechnology, Royal Institute of Technology, AlbaNova University Center, S-10691 Stockholm, Sweden and PDC Center for High Performance Computing, Royal Institute of Technology, S-10044 Stockholm (Sweden)] [Theoretical Chemistry and Biology, School of Biotechnology, Royal Institute of Technology, AlbaNova University Center, S-10691 Stockholm, Sweden and PDC Center for High Performance Computing, Royal Institute of Technology, S-10044 Stockholm (Sweden); Ekström, Ulf; Helgaker, Trygve [Center for Theoretical and Computational Chemistry (CTCC), Department of Chemistry, University of Oslo, P.O. Box 1033, Blindern, 0315 Oslo (Norway)] [Center for Theoretical and Computational Chemistry (CTCC), Department of Chemistry, University of Oslo, P.O. Box 1033, Blindern, 0315 Oslo (Norway)
2014-01-21T23:59:59.000Z
We present the first analytic implementation of cubic and quartic force constants at the level of Kohn–Sham density-functional theory. The implementation is based on an open-ended formalism for the evaluation of energy derivatives in an atomic-orbital basis. The implementation relies on the availability of open-ended codes for evaluation of one- and two-electron integrals differentiated with respect to nuclear displacements as well as automatic differentiation of the exchange–correlation kernels. We use generalized second-order vibrational perturbation theory to calculate the fundamental frequencies of methane, ethane, benzene, and aniline, comparing B3LYP, BLYP, and Hartree–Fock results. The Hartree–Fock anharmonic corrections agree well with the B3LYP corrections when calculated at the B3LYP geometry and from B3LYP normal coordinates, suggesting that the inclusion of electron correlation is not essential for the reliable calculation of cubic and quartic force constants.
Qiang Zhao; Jian Min Dong; Jun Ling Song; Wen Hui Long
2014-07-23T23:59:59.000Z
Half-life of proton radioactivity of spherical proton emitters is studied within the scheme of covariant density functional (CDF) theory, and for the first time the potential barrier that prevents the emitted proton is extracted with the similarity renormalization group (SRG) method, in which the spin-orbit potential along with the others that turn out to be non-negligible can be derived automatically. The spectroscopic factor that is significant is also extracted from the CDF calculations. The estimated half-lives are found in good agreement with the experimental values, which not only confirms the validity of the CDF theory in describing the proton-rich nuclei, but also indicates the prediction power of present approach to calculate the half-lives and in turn to extract the structural information of proton emitters.
Correlation of Theory and Function in Well-Defined Bimetallic Electrocatalysts - Final Report
Crooks, Richard M.
2014-06-05T23:59:59.000Z
The objective of this research proposal was to correlate the structure of nanoparticles that are comprised of ~100-200 atoms to their electrocatalytic function. This objective was based on the growing body of evidence suggesting that catalytic properties can be tailored through controlled synthesis of nanoparticles. What has been missing from many of these studies, and what we are contributing, is a model catalyst that is sufficiently small, structurally well-defined, and well-characterized that its function can be directly predicted by theory. Specifically, our work seeks to develop a fundamental and detailed understanding of the relationship between the structure of nanoscopic oxygen-reduction catalysts and their function. We assembled a team with expertise in theory, synthesis, and advanced characterization methods to address the primary objective of this project. We anticipated the outcomes of the study to be: (1) a better theoretical understanding of how nanoparticle structure affects catalytic properties; (2) the development of advanced, in-situ and ex-situ, atomic-scale characterization methods that are appropriate for particles containing about 100 atoms; and (3) improved synthetic methods that produce unique nanoparticle structures that can be used to test theoretical predictions. During the project period, we have made excellent progress on all three fronts.
Cornaton, Yann; Jensen, Hans Jørgen Aa; Fromager, Emmanuel
2013-01-01T23:59:59.000Z
An alternative separation of short-range exchange and correlation energies is used in the framework of second-order range-separated density-functional perturbation theory. This alternative separation was initially proposed by Toulouse et al. [Theor. Chem. Acc. 114, 305 (2005)] and relies on a long-range interacting wavefunction instead of the non-interacting Kohn-Sham one. When second-order corrections to the density are neglected, the energy expression reduces to a range-separated double-hybrid (RSDH) type of functional, RSDHf, where "f" stands for "full-range integrals" as the regular full-range interaction appears explicitly in the energy expression when expanded in perturbation theory. In contrast to usual RSDH functionals, RSDHf describes the coupling between long- and short-range correlations as an orbital-dependent contribution. Calculations on the first four noble-gas dimers show that this coupling has a significant effect on the potential energy curves in the equilibrium region, improving the accurac...
Free-energy functional of the electronic potential for Schrödinger-Poisson theory
Vikram Jadhao; Kaushik Mitra; Francisco J. Solis; Monica Olvera de la Cruz
2014-12-15T23:59:59.000Z
In the study of model electronic device systems where electrons are typically under confinement, a key obstacle is the need to iteratively solve the coupled Schr\\"{o}dinger-Poisson (SP) equation. It is possible to bypass this obstacle by adopting a variational approach and obtaining the solution of the SP equation by minimizing a functional. Further, using molecular dynamics methods that treat the electronic potential as a dynamical variable, the functional can be minimized on the fly in conjunction with the update of other dynamical degrees of freedom leading to considerable reduction in computational costs. But such approaches require access to a true free-energy functional, one that evaluates to the equilibrium free energy at its minimum. In this paper, we present a variational formulation of the Schr\\"{o}dinger-Poisson (SP) theory with the needed free-energy functional of the electronic potential. We apply our formulation to semiconducting nanostructures and provide the expression of the free-energy functional for narrow channel quantum wells where the local density approximation yields accurate physics and for the case of wider channels where Thomas-Fermi approximation is valid.
Free Energy Calculations of Crystalline Hard Sphere Complexes Using Density Functional Theory
Gunawardana, K. G. S. H. [Ames Lab., Ames, IA (United States); Song, Xueyu [Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States). Department of Chemistry
2014-12-22T23:59:59.000Z
Recently developed fundamental measure density functional theory (FMT) is used to study binary hard sphere (HS) complexes in crystalline phases. By comparing the excess free energy, pressure and phase diagram, we show that the fundamental measure functional yields good agreements to the available simulation results of AB, AB_{2} and AB_{13} crystals. Additionally, we use this functional to study the HS models of five binary crystals, Cu_{5}Zr(C15_{b}), Cu_{51}Zr_{14}(?), Cu_{10}Zr_{7}(?), CuZr(B2) and CuZr_{2} (C11_{b}), which are observed in the Cu-Zr system. The FMT functional gives well behaved minimum for most of the hard sphere crystal complexes in the two dimensional Gaussian space, namely a crystalline phase. However, the current version of FMT functional (white Bear) fails to give a stable minimum for the structure Cu_{10}Zr_{7}(?). We argue that the observed solid phases for the HS models of the Cu-Zr system are true thermodynamic stable phases and can be used as a reference system in perturbation calculations.
Free Energy Calculations of Crystalline Hard Sphere Complexes Using Density Functional Theory
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Gunawardana, K. G. S. H.; Song, Xueyu
2014-12-22T23:59:59.000Z
Recently developed fundamental measure density functional theory (FMT) is used to study binary hard sphere (HS) complexes in crystalline phases. By comparing the excess free energy, pressure and phase diagram, we show that the fundamental measure functional yields good agreements to the available simulation results of AB, AB2 and AB13 crystals. Additionally, we use this functional to study the HS models of five binary crystals, Cu5Zr(C15b), Cu51Zr14(?), Cu10Zr7(?), CuZr(B2) and CuZr2 (C11b), which are observed in the Cu-Zr system. The FMT functional gives well behaved minimum for most of the hard sphere crystal complexes in the two dimensional Gaussian space,more »namely a crystalline phase. However, the current version of FMT functional (white Bear) fails to give a stable minimum for the structure Cu10Zr7(?). We argue that the observed solid phases for the HS models of the Cu-Zr system are true thermodynamic stable phases and can be used as a reference system in perturbation calculations.« less
Growth mechanism of atomic layer deposition of zinc oxide: A density functional theory approach
Afshar, Amir; Cadien, Kenneth C., E-mail: kcadien@ualberta.ca [Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta T6G 2V4 (Canada)
2013-12-16T23:59:59.000Z
Atomic layer deposition of zinc oxide (ZnO) using diethylzinc (DEZ) and water is studied using density functional theory. The reaction pathways between the precursors and ZnO surface sites are discussed. Both reactions proceed by the formation of intermediate complexes on the surface. The Gibbs free energy of the formation of these complexes is positive at temperatures above ?120?°C and ?200?°C for DEZ and water half-reactions, respectively. Spectroscopic ellipsometry results show that the growth per cycle changes at approximately the same temperatures.
Song, Xueyu
online 18 July 2008 Free energies and correlation functions of liquid and solid hard-sphere HS mixtures theory the free energies of solid and liquid Lennard-Jones LJ mixtures are obtained from correlation, Chandler, and Andersen WCA Refs. 5 and 6 perturbation theory, the free energy is separated into two parts
Firoozabadi, Abbas
representa- tion of various intermolecular interactions e.g., short-range repulsions, van der Waals- ing of hydrocarbons, N2, CO2, H2S, and sometimes water, DFT at the current stage only exhibits very
Orbital-free density functional theory of out-of-plane charge screening in graphene
Jianfeng Lu; Vitaly Moroz; Cyrill B. Muratov
2015-06-30T23:59:59.000Z
We propose a density functional theory of Thomas-Fermi-Dirac-von Weizs\\"acker type to describe the response of a single layer of graphene resting on a dielectric substrate to a point charge or a collection of charges some distance away from the layer. We formulate a variational setting in which the proposed energy functional admits minimizers, both in the case of free graphene layers and under back-gating. We further provide conditions under which those minimizers are unique and correspond to configurations consisting of inhomogeneous density profiles of charge carrier of only one type. The associated Euler-Lagrange equation for the charge density is also obtained, and uniqueness, regularity and decay of the minimizers are proved under general conditions. In addition, a bifurcation from zero to non-zero response at a finite threshold value of the external charge is proved.
Sun, Shih-Jye [Department of Applied Physics, National University of Kaohsiung, Kaohsiung 811, Taiwan (China); Lin, Ken-Huang; Li, Jia-Yun [Department of Mechanical and Electro-Mechanical Engineering, National Sun Yat-Sen University, Kaohsiung 804, Taiwan (China); Ju, Shin-Pon, E-mail: jushin-pon@mail.nsysu.edu.tw [Department of Mechanical and Electro-Mechanical Engineering, National Sun Yat-Sen University, Kaohsiung 804, Taiwan (China); Department of Medicinal and Applied Chemistry, Kaohsiung Medical University, Kaohsiung 807, Taiwan (China)
2014-10-07T23:59:59.000Z
The simulated annealing basin-hopping method incorporating the penalty function was used to predict the lowest-energy structures for ultrathin tungsten nanowires and nanotubes of different sizes. These predicted structures indicate that tungsten one-dimensional structures at this small scale do not possess B.C.C. configuration as in bulk tungsten material. In order to analyze the relationship between multi-shell geometries and electronic transfer, the electronic and structural properties of tungsten wires and tubes including partial density of state and band structures which were determined and analyzed by quantum chemistry calculations. In addition, in order to understand the application feasibility of these nanowires and tubes on nano-devices such as field emitters or chemical catalysts, the electronic stability of these ultrathin tungsten nanowires was also investigated by density functional theory calculations.
Quasi-particle energy spectra in local reduced density matrix functional theory
Lathiotakis, Nektarios N. [Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, Vass. Constantinou 48, GR-11635 Athens (Greece); Helbig, Nicole [Peter-Grünberg Institut and Institute for Advanced Simulation, Forschungszentrum Jülich, D-52425 Jülich (Germany); Rubio, Angel [Nano-Bio Spectroscopy Group and ETSF Scientific Development Centre, Dpto. Física de Materiales, Universidad del País Vasco, CFM CSIC-UPV/EHU-MPC and DIPC, Av. Tolosa 72, E-20018 San Sebastián (Spain); Gidopoulos, Nikitas I. [Department of Physics, Durham University, South Road, Durham DH1 3LE (United Kingdom)
2014-10-28T23:59:59.000Z
Recently, we introduced [N. N. Lathiotakis, N. Helbig, A. Rubio, and N. I. Gidopoulos, Phys. Rev. A 90, 032511 (2014)] local reduced density matrix functional theory (local RDMFT), a theoretical scheme capable of incorporating static correlation effects in Kohn-Sham equations. Here, we apply local RDMFT to molecular systems of relatively large size, as a demonstration of its computational efficiency and its accuracy in predicting single-electron properties from the eigenvalue spectrum of the single-particle Hamiltonian with a local effective potential. We present encouraging results on the photoelectron spectrum of molecular systems and the relative stability of C{sub 20} isotopes. In addition, we propose a modelling of the fractional occupancies as functions of the orbital energies that further improves the efficiency of the method useful in applications to large systems and solids.
Orbital-free density functional theory of out-of-plane charge screening in graphene
Jianfeng Lu; Vitaly Moroz; Cyrill B. Muratov
2014-05-20T23:59:59.000Z
We propose a density functional theory of Thomas-Fermi-Dirac-von Weizs\\"acker type to describe the response of a single layer of graphene resting on a dielectric substrate to a point charge or a collection of point charges some distance away from the layer. We formulate a variational setting in which the proposed energy functional admits minimizers, both in the case of free graphene layers and under back-gating. We further provide conditions under which those minimizers are unique and correspond to configurations consisting of inhomogeneous density profiles of charge carrier of only one type. The associated Euler-Lagrange equation for the charge density is also obtained, and uniqueness, regularity and decay of the minimizers are proved under general conditions. In addition, a bifurcation from zero to non-zero response at a finite threshold value of the external charge is proved.
Building A Universal Nuclear Energy Density Functional (UNEDF)
Carlson, Joe, Los Alamos National Laboratory, Los Alamos, NM; Furnstahl, Dick, Ohio State University, Columbus, OH; Horoi, Mihai, Central Michigan University, Mount Pleasant, MI; Lusk, Rusty, Argonne National Laboratory, Argonne, IL; Nazarewicz, Witek, University of Tennessee, Knoxville, TN; Ng, Esmond, Berkeley National Laboratory, Berkeley, CA; Thompson, Ian, Lawrence Livermore National Laboratory, Livermore, CA; Vary, James, Iowa State University, Ames, Iowa
2012-09-30T23:59:59.000Z
During the period of Dec. 1 2006 â?? Jun. 30, 2012, the UNEDF collaboration carried out a comprehensive study of all nuclei, based on the most accurate knowledge of the strong nuclear interaction, the most reliable theoretical approaches, the most advanced algorithms, and extensive computational resources, with a view towards scaling to the petaflop platforms and beyond. The long-term vision initiated with UNEDF is to arrive at a comprehensive, quantitative, and unified description of nuclei and their reactions, grounded in the fundamental interactions between the constituent nucleons. We seek to replace current phenomenological models of nuclear structure and reactions with a well-founded microscopic theory that delivers maximum predictive power with well-quantified uncertainties. Specifically, the mission of this project has been three-fold: first, to find an optimal energy density functional (EDF) using all our knowledge of the nucleonic Hamiltonian and basic nuclear properties; second, to apply the EDF theory and its extensions to validate the functional using all the available relevant nuclear structure and reaction data; third, to apply the validated theory to properties of interest that cannot be measured, in particular the properties needed for reaction theory. The main physics areas of UNEDF, defined at the beginning of the project, were: ab initio structure; ab initio functionals; DFT applications; DFT extensions; reactions.
J. D. McDonnell; N. Schunck; D. Higdon; J. Sarich; S. M. Wild; W. Nazarewicz
2015-01-15T23:59:59.000Z
Statistical tools of uncertainty quantification can be used to assess the information content of measured observables with respect to present-day theoretical models; to estimate model errors and thereby improve predictive capability; to extrapolate beyond the regions reached by experiment; and to provide meaningful input to applications and planned measurements. To showcase new opportunities offered by such tools, we make a rigorous analysis of theoretical statistical uncertainties in nuclear density functional theory using Bayesian inference methods. By considering the recent mass measurements from the Canadian Penning Trap at Argonne National Laboratory, we demonstrate how the Bayesian analysis and a direct least-squares optimization, combined with high-performance computing, can be used to assess the information content of the new data with respect to a model based on the Skyrme energy density functional approach. Employing the posterior probability distribution computed with a Gaussian process emulator, we apply the Bayesian framework to propagate theoretical statistical uncertainties in predictions of nuclear masses, two-neutron dripline, and fission barriers. Overall, we find that the new mass measurements do not impose a constraint that is strong enough to lead to significant changes in the model parameters. The example discussed in this study sets the stage for quantifying and maximizing the impact of new measurements with respect to current modeling and guiding future experimental efforts, thus enhancing the experiment-theory cycle in the scientific method.
R. L. Mkrtchyan
2014-10-29T23:59:59.000Z
We show that partition function of Chern-Simons theory on three-sphere with classical and exceptional groups (actually on the whole corresponding lines in Vogel's plane) can be represented as ratio of respectively triple and double sine functions (last function is essentially a modular quantum dilogarithm). The product representation of sine functions gives Gopakumar-Vafa structure form of partition function, which in turn gives a corresponding integer invariants of manifold after geometrical transition. In this way we suggest to extend gauge/string duality to exceptional groups, although one still have to resolve few problems. In both classical and exceptional cases an additional terms, non-perturbative w.r.t. the string coupling constant, appear. The full universal partition function of Chern-Simons theory on three-sphere is shown to be the ratio of quadruple sine functions. We also briefly discuss the matrix model for exceptional line.
Kozimor, S.A.; Yang, P.; Batista, E.R.; Boland, K.S.; Burns, C.J.; Christensen, C.N.; Clark, D.L.; Conradson, S.D.; Hay, P.J.; Lezama, J.S.; Martin, R.L.; Schwarz, D.E.; Wilkerson, M.P.; Wolfsberg, L.E.
2009-05-20T23:59:59.000Z
For 3-5d transition-metal ions, the (C{sub 5}R{sub 5}){sub 2}MCl{sub 2} (R = H, Me for M = Ti, Zr, Hf) bent metallocenes represent a series of compounds that have been central in the development of organometallic chemistry and homogeneous catalysis. Here, we evaluate how changes in the principal quantum number for the group IV (C{sub 5}H{sub 5}){sub 2}MCl{sub 2} (M = Ti, Zr, Hf; 1-3, respectively) complexes affects the covalency of M-Cl bonds through application of Cl K-edge X-ray Absorption Spectroscopy (XAS). Spectra were recorded on solid samples dispersed as a thin film and encapsulated in polystyrene matrices to reliably minimize problems associated with X-ray self-absorption. The data show that XAS pre-edge intensities can be quantitatively reproduced when analytes are encapsulated in polystyrene. Cl K-edge XAS data show that covalency in M-Cl bonding changes in the order Ti > Zr > Hf and demonstrates that covalency slightly decreases with increasing principal quantum number in 1-3. The percent Cl 3p character was experimentally determined to be 26, 23, and 18% per M-Cl bond in the thin-film samples for 1-3 respectively and was indistinguishable from the polystyrene samples, which analyzed as 25, 25, and 19% for 1-3, respectively. To aid in interpretation of Cl K-edge XAS, 1-3 were also analyzed by ground-state and time-dependent density functional theory (TD-DFT) calculations. The calculated spectra and percent chlorine character are in close agreement with the experimental observations, and show 20, 18, and 17% Cl 3p character per M-Cl bond for 1-3, respectively. Polystyrene matrix encapsulation affords a convenient method to safely contain radioactive samples to extend our studies to include actinide elements, where both 5f and 6d orbitals are expected to play a role in M-Cl bonding and where transition assignments must rely on accurate theoretical calculations.
Complex-energy approach to sum rules within nuclear density functional theory
Nobuo Hinohara; Markus Kortelainen; Witold Nazarewicz; Erik Olsen
2015-01-28T23:59:59.000Z
The linear response of the nucleus to an external field contains unique information about the effective interaction, correlations, and properties of its excited states. To characterize the response, it is useful to use its energy-weighted moments, or sum rules. By comparing computed sum rules with experimental values, the information content of the response can be utilized in the optimization process of the nuclear Hamiltonian or EDF. But the additional information comes at a price: compared to the ground state, computation of excited states is more demanding. To establish an efficient framework to compute sum rules of the response that is adaptable to the optimization of the nuclear EDF and large-scale surveys of collective strength, we have developed a new technique within the complex-energy FAM based on the QRPA. To compute sum rules, we carry out contour integration of the response function in the complex-energy plane. We benchmark our results against the conventional matrix formulation of the QRPA theory, the Thouless theorem for the energy-weighted sum rule, and the dielectric theorem for the inverse energy-weighted sum rule. We demonstrate that calculated sum-rule values agree with those obtained from the matrix formulation of the QRPA. We also discuss the applicability of both the Thouless theorem about the energy-weighted sum rule and the dielectric theorem for the inverse energy-weighted sum rule to nuclear density functional theory in cases when the EDF is not based on a Hamiltonian. The proposed sum-rule technique based on the complex-energy FAM is a tool of choice when optimizing effective interactions or energy functionals. The method is very efficient and well-adaptable to parallel computing. The FAM formulation is especially useful when standard theorems based on commutation relations involving the nuclear Hamiltonian and external field cannot be used.
Alavi, Ali
Coupled cluster benchmarks of water monomers and dimers extracted from density-functional theory functionals in simulations of liquid water, water monomers and dimers were extracted from a PBE simulation liquid water: The importance of monomer deformations Biswajit Santra,1 Angelos Michaelides,1,2,a
Raghunathan, Shampa; Nest, Mathias [Theoretische Chemie, TU Muenchen, Lichtenbergstr. 4, 85747 Garching (Germany)
2012-02-14T23:59:59.000Z
Explicitly time-dependent density functional theory (TDDFT) is a formally exact theory, which can treat very large systems. However, in practice it is used almost exclusively in the adiabatic approximation and with standard ground state functionals. Therefore, if combined with coherent control theory, it is not clear which control tasks can be achieved reliably, and how this depends on the functionals. In this paper, we continue earlier work in order to establish rules that answer these questions. Specifically, we look at the creation of wave packets by ultrashort laser pulses that contain several excited states. We find that (i) adiabatic TDDFT only works if the system is not driven too far from the ground state, (ii) the permanent dipole moments involved should not differ too much, and (iii) these results are independent of the functional used. Additionally, we find an artifact that produces fluence-dependent excitation energies.
Dynamic density functional theory of protein adsorption on polymer-coated nanoparticles
Stefano Angioletti-Uberti; Matthias Ballauff; Joachim Dzubiella
2014-07-30T23:59:59.000Z
We present a theoretical model for the description of the adsorption kinetics of globular proteins onto charged core-shell microgel particles based on Dynamic Density Functional Theory (DDFT). This model builds on a previous description of protein adsorption thermodynamics [Yigit \\textit{et al}, Langmuir 28 (2012)], shown to well interpret the available calorimetric experimental data of binding isotherms. In practice, a spatially-dependent free-energy functional including the same physical interactions is built, and used to study the kinetics via a generalised diffusion equation. To test this model, we apply it to the case study of Lysozyme adsorption on PNIPAM coated nanoparticles, and show that the dynamics obtained within DDFT is consistent with that extrapolated from experiments. We also perform a systematic study of the effect of various parameters in our model, and investigate the loading dynamics as a function of proteins' valence and hydrophobic adsorption energy, as well as their concentration and that of the nanoparticles. Although we concentrated here on the case of adsorption for a single protein type, the model's generality allows to study multi-component system, providing a reliable instrument for future studies of competitive and cooperative adsorption effects often encountered in protein adsorption experiments.
Prediction of Iron K-Edge Absorption Spectra Using Time-Dependent Density Functional Theory
George, S.DeBeer; Petrenko, T.; Neese, F.
2009-05-14T23:59:59.000Z
Iron K-edge X-ray absorption pre-edge features have been calculated using a time-dependent density functional approach. The influence of functional, solvation, and relativistic effects on the calculated energies and intensities has been examined by correlation of the calculated parameters to experimental data on a series of 10 iron model complexes, which span a range of high-spin and low-spin ferrous and ferric complexes in O{sub h} to T{sub d} geometries. Both quadrupole and dipole contributions to the spectra have been calculated. We find that good agreement between theory and experiment is obtained by using the BP86 functional with the CP(PPP) basis set on the Fe and TZVP one of the remaining atoms. Inclusion of solvation yields a small improvement in the calculated energies. However, the inclusion of scalar relativistic effects did not yield any improved correlation with experiment. The use of these methods to uniquely assign individual spectral transitions and to examine experimental contributions to backbonding is discussed.
Sako, Akifumi; Suzuki, Toshiya [Department of Mathematics, Faculty of Science and Technology, Keio University, 3-14-1 Hiyoshi, Kohoku-ku, Yokohama 223-8522 (Japan); Department of Physics, Faculty of Science, Ochanomizu University, 2-1-1 Otsuka, Bunkyo-ku, Tokyo 112-8610 (Japan)
2006-01-15T23:59:59.000Z
We investigate cohomological gauge theories in noncommutative R{sup 2D}. We show that vacuum expectation values of the theories do not depend on noncommutative parameters, and the large noncommutative parameter limit is equivalent to the dimensional reduction. As a result of these facts, we show that a partition function of a cohomological theory defined in noncommutative R{sup 2D} and a partition function of a cohomological field theory in R{sup 2D+2} are equivalent if they are connected through dimensional reduction. Therefore, we find several partition functions of supersymmetric gauge theories in various dimensions are equivalent. Using this technique, we determine the partition function of the N=4 U(1) gauge theory in noncommutative R{sup 4}, where its action does not include a topological term. The result is common among (8-dim, N=2), (6-dim, N=2), (2-dim, N=8) and the IKKT matrix model given by their dimensional reduction to 0-dim.
Fattebert, J; Law, R J; Bennion, B; Lau, E Y; Schwegler, E; Lightstone, F C
2009-04-24T23:59:59.000Z
We evaluate the accuracy of density functional theory quantum calculations of biomolecular subsystems using a simple electrostatic embedding scheme. Our scheme is based on dividing the system of interest into a primary and secondary subsystem. A finite difference discretization of the Kohn-Sham equations is used for the primary subsystem, while its electrostatic environment is modeled with a simple one-electron potential. Force-field atomic partial charges are used to generate smeared Gaussian charge densities and to model the secondary subsystem. We illustrate the utility of this approach with calculations of truncated dipeptide chains. We analyze quantitatively the accuracy of this approach by calculating atomic forces and comparing results with fullQMcalculations. The impact of the choice made in terminating dangling bonds at the frontier of the QM region is also investigated.
Mussard, Bastien; Ángyán, János G
2015-01-01T23:59:59.000Z
Analytical forces have been derived in the Lagrangian framework for several random phase approximation (RPA) correlated total energy methods based on the range separated hybrid (RSH) approach, which combines a short-range density functional approximation for the short-range exchange-correlation energy with a Hartree-Fock-type long-range exchange and RPA long-range correlation. The RPA correlation energy has been expressed as a ring coupled cluster doubles (rCCD) theory. The resulting analytical gradients have been implemented and tested for geometry optimization of simple molecules and intermolecular charge transfer complexes, where intermolecular interactions are expected to have a non-negligible effect even on geometrical parameters of the monomers.
Yao, J M; Hagino, K; Ring, P; Meng, J
2014-01-01T23:59:59.000Z
We report a systematic study of nuclear matrix elements (NMEs) in neutrinoless double-beta decays with state-of-the-art beyond mean-field covariant density functional theory. The dynamic effects of particle-number and angular-momentum conservations as well as quadrupole shape fluctuations are taken into account with projections and generator coordinate method for both initial and final nuclei. The full relativistic transition operator is adopted to calculate the NMEs which are found to be consistent with the results of previous beyond non-relativistic mean-field calculation based on a Gogny force with the exception of $^{150}$Nd. Our study shows that the total NMEs can be well approximated by the pure axial-vector coupling term, the calculation of which is computationally much cheaper than that of full terms.
Time-odd mean fields in covariant density functional theory I. Non-rotating systems
A. V. Afanasjev; H. Abusara
2010-10-09T23:59:59.000Z
Time-odd mean fields (nuclear magnetism) are analyzed in the framework of covariant density functional theory (CDFT). It is shown that they always provide additional binding to the binding energies of odd-mass nuclei. This additional binding only weakly depends on the RMF parametrization reflecting good localization of the properties of time-odd mean fields in CDFT. The underlying microscopic mechanism is discussed in detail. Time-odd mean fields affect odd-even mass differences. However, our analysis suggests that the modifications of the strength of pairing correlations required to compensate for their effects are modest. In contrast, time-odd mean fields have profound effect on the properties of odd-proton nuclei in the vicinity of proton-drip line. Their presence can modify the half-lives of proton-emitters (by many orders of magnitude in light nuclei) and affect considerably the possibilities of their experimental observation.
Jeanmairet, Guillaume; Levesque, Maximilien; Rotenberg, Benjamin; Borgis, Daniel
2014-01-01T23:59:59.000Z
We report here how the hydration of complex surfaces can be efficiently studied thanks to recent advances in classical molecular density functional theory. This is illustrated on the example of the pyrophylite clay. After presenting the most recent advances, we show that the strength of this implicit method is that (i) it is in quantitative or semi-quantitative agreement with reference all-atoms simulations (molecular dynamics here) for both the solvation structure and energetics, and that (ii) the computational cost is two to three orders of magnitude less than in explicit methods. The method remains imperfect, in that it locally overestimates the polarization of water close to hydrophylic sites of the clay. The high numerical efficiency of the method is illustrated and exploited to carry a systematic study of the electrostatic and van der Waals components of the surface-solvant interactions within the most popular force field for clays, CLAYFF. Hydration structure and energetics are found to weakly depend u...
Green's function method for single-particle resonant states in relativistic mean field theory
T. T. Sun; S. Q. Zhang; Y. Zhang; J. N. Hu; J. Meng
2014-09-30T23:59:59.000Z
Relativistic mean field theory is formulated with the Green's function method in coordinate space to investigate the single-particle bound states and resonant states on the same footing. Taking the density of states for free particle as a reference, the energies and widths of single-particle resonant states are extracted from the density of states without any ambiguity. As an example, the energies and widths for single-neutron resonant states in $^{120}$Sn are compared with those obtained by the scattering phase-shift method, the analytic continuation in the coupling constant approach, the real stabilization method and the complex scaling method. Excellent agreements are found for the energies and widths of single-neutron resonant states.
Steam reforming on transition-metal carbides from density-functional theory
Vojvodic, Aleksandra
2009-01-01T23:59:59.000Z
A screening study of the steam reforming reaction (CH_4 + H_2O -> CO + 3H_2) on early transition-metal carbides (TMC's) is performed by means of density-functional theory calculations. The set of considered surfaces includes the alpha-Mo_2C(100) surfaces, the low-index (111) and (100) surfaces of TiC, VC, and delta-MoC, and the oxygenated alpha-Mo_2C(100) and TMC(111) surfaces. It is found that carbides provide a wide spectrum of reactivities towards the steam reforming reaction, from too reactive via suitable to too inert. The reactivity is discussed in terms of the electronic structure of the clean surfaces. Two surfaces, the delta-MoC(100) and the oxygen passivated alpha-Mo_2C(100) surfaces, are identified as promising steam reforming catalysts. These findings suggest that carbides provide a playground for reactivity tuning, comparable to the one for pure metals.
Green's function multiple-scattering theory with a truncated basis set: An augmented-KKR formalism
Alam, Aftab [Indian Institute of Technology Bombay; Khan, Suffian N [Ames Laboratory; Smirnov, A V [Ames Laboratory; Nicholson, D M [Oak Ridge National Laboratory; Johnson, Duane D [Ames Laboratory
2014-11-01T23:59:59.000Z
The Korringa-Kohn-Rostoker (KKR) Green's function, multiple-scattering theory is an efficient site-centered, electronic-structure technique for addressing an assembly of N scatterers. Wave functions are expanded in a spherical-wave basis on each scattering center and indexed up to a maximum orbital and azimuthal number Lmax=(l,m)max, while scattering matrices, which determine spectral properties, are truncated at Ltr=(l,m)tr where phase shifts ?l>ltr are negligible. Historically, Lmax is set equal to Ltr, which is correct for large enough Lmax but not computationally expedient; a better procedure retains higher-order (free-electron and single-site) contributions for Lmax>Ltr with ?l>ltr set to zero [X.-G. Zhang and W. H. Butler, Phys. Rev. B 46, 7433 (1992)]. We present a numerically efficient and accurate augmented-KKR Green's function formalism that solves the KKR equations by exact matrix inversion [R3 process with rank N(ltr+1)2] and includes higher-L contributions via linear algebra [R2 process with rank N(lmax+1)2]. The augmented-KKR approach yields properly normalized wave functions, numerically cheaper basis-set convergence, and a total charge density and electron count that agrees with Lloyd's formula. We apply our formalism to fcc Cu, bcc Fe, and L10 CoPt and present the numerical results for accuracy and for the convergence of the total energies, Fermi energies, and magnetic moments versus Lmax for a given Ltr.
Sussman, Joel L.
Theoretical Insight into the Interactions of TMA-Benzene and TMA-Pyrrole with B3LYP Density theoretical investigation of the tetramethylammonium(TMA)-benzene and TMA-pyrrole complexes has been performed density in the 5 6 aromatic system of pyrrole is larger than that in the 6 6 system of benzene
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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:1 First Use of Energy for All Purposes (Fuel and Nonfuel), 2002; Level:5 TablesExports(Journal Article)41clothThe Bonneville Power Administration wouldDecember 2014 National SecurityDelegations,Central Park in,000
Chu, Shih-I
Time-dependent density-functional theory for strong-field multiphoton processes: Application 1997 We present a self-interaction-free time-dependent density-functional theory TDDFT. The theory is based on the extension of the time-dependent Kohn-Sham formalism. The time-dependent exchange
Maranzana, Andrea, E-mail: andrea.maranzana@unito.it, E-mail: anna.giordana@hotmail.com, E-mail: vincenzo.barone@sns.it, E-mail: mauro.causa@unina.it, E-mail: mipavone@unina.it; Giordana, Anna, E-mail: andrea.maranzana@unito.it, E-mail: anna.giordana@hotmail.com, E-mail: vincenzo.barone@sns.it, E-mail: mauro.causa@unina.it, E-mail: mipavone@unina.it; Indarto, Antonius, E-mail: antonius.indarto@che.itb.ac.id; Tonachini, Glauco, E-mail: glauco.tonachini@unito.it [Dipartimento di Chimica, Università di Torino, Corso Massimo D’Azeglio 48, I-10125 Torino (Italy)] [Dipartimento di Chimica, Università di Torino, Corso Massimo D’Azeglio 48, I-10125 Torino (Italy); Barone, Vincenzo, E-mail: andrea.maranzana@unito.it, E-mail: anna.giordana@hotmail.com, E-mail: vincenzo.barone@sns.it, E-mail: mauro.causa@unina.it, E-mail: mipavone@unina.it [Scuola Normale Superiore, Piazza dei Cavalieri 7, I-56126, Pisa (Italy)] [Scuola Normale Superiore, Piazza dei Cavalieri 7, I-56126, Pisa (Italy); Causà, Mauro, E-mail: andrea.maranzana@unito.it, E-mail: anna.giordana@hotmail.com, E-mail: vincenzo.barone@sns.it, E-mail: mauro.causa@unina.it, E-mail: mipavone@unina.it [Dipartimento di Ingegneria Chimica, dei Materiali e della Produzione Industriale, Università di Napoli “Federico II,” Via Cintia, 80126 Napoli (Italy)] [Dipartimento di Ingegneria Chimica, dei Materiali e della Produzione Industriale, Università di Napoli “Federico II,” Via Cintia, 80126 Napoli (Italy); Pavone, Michele, E-mail: andrea.maranzana@unito.it, E-mail: anna.giordana@hotmail.com, E-mail: vincenzo.barone@sns.it, E-mail: mauro.causa@unina.it, E-mail: mipavone@unina.it [Dipartimento di Scienze Chimiche, Università di Napoli “Federico II,” Complesso Universitario di Monte Sant’Angelo, Via Cintia, I-80126 Napoli (Italy)] [Dipartimento di Scienze Chimiche, Università di Napoli “Federico II,” Complesso Universitario di Monte Sant’Angelo, Via Cintia, I-80126 Napoli (Italy)
2013-12-28T23:59:59.000Z
Our purpose is to identify a computational level sufficiently dependable and affordable to assess trends in the interaction of a variety of radical or closed shell unsaturated hydro-carbons A adsorbed on soot platelet models B. These systems, of environmental interest, would unavoidably have rather large sizes, thus prompting to explore in this paper the performances of relatively low-level computational methods and compare them with higher-level reference results. To this end, the interaction of three complexes between non-polar species, vinyl radical, ethyne, or ethene (A) with benzene (B) is studied, since these species, involved themselves in growth processes of polycyclic aromatic hydrocarbons (PAHs) and soot particles, are small enough to allow high-level reference calculations of the interaction energy ?E{sub AB}. Counterpoise-corrected interaction energies ?E{sub AB} are used at all stages. (1) Density Functional Theory (DFT) unconstrained optimizations of the A?B complexes are carried out, using the B3LYP-D, ?B97X-D, and M06-2X functionals, with six basis sets: 6-31G(d), 6-311 (2d,p), and 6-311++G(3df,3pd); aug-cc-pVDZ and aug-cc-pVTZ; N07T. (2) Then, unconstrained optimizations by Møller-Plesset second order Perturbation Theory (MP2), with each basis set, allow subsequent single point Coupled Cluster Singles Doubles and perturbative estimate of the Triples energy computations with the same basis sets [CCSD(T)//MP2]. (3) Based on an additivity assumption of (i) the estimated MP2 energy at the complete basis set limit [E{sub MP2/CBS}] and (ii) the higher-order correlation energy effects in passing from MP2 to CCSD(T) at the aug-cc-pVTZ basis set, ?E{sub CC-MP}, a CCSD(T)/CBS estimate is obtained and taken as a computational energy reference. At DFT, variations in ?E{sub AB} with basis set are not large for the title molecules, and the three functionals perform rather satisfactorily even with rather small basis sets [6-31G(d) and N07T], exhibiting deviation from the computational reference of less than 1 kcal mol{sup ?1}. The zero-point vibrational energy corrected estimates ?(E{sub AB}+ZPE), obtained with the three functionals and the 6-31G(d) and N07T basis sets, are compared with experimental D{sub 0} measures, when available. In particular, this comparison is finally extended to the naphthalene and coronene dimers and to three ??? associations of different PAHs (R, made by 10, 16, or 24 C atoms) and P (80 C atoms)
Hydration of gas-phase ytterbium ion complexes studied by experiment and theory
Rutkowski, Philip X; Michelini, Maria C.; Bray, Travis H.; Russo, Nino; Marcalo, Joaquim; Gibson, John K.
2011-02-11T23:59:59.000Z
Hydration of ytterbium (III) halide/hydroxide ions produced by electrospray ionization was studied in a quadrupole ion trap mass spectrometer and by density functional theory (DFT). Gas-phase YbX{sub 2}{sup +} and YbX(OH){sup +} (X = OH, Cl, Br, or I) were found to coordinate from one to four water molecules, depending on the ion residence time in the trap. From the time dependence of the hydration steps, relative reaction rates were obtained. It was determined that the second hydration was faster than both the first and third hydrations, and the fourth hydration was the slowest; this ordering reflects a combination of insufficient degrees of freedom for cooling the hot monohydrate ion and decreasing binding energies with increasing hydration number. Hydration energetics and hydrate structures were computed using two approaches of DFT. The relativistic scalar ZORA approach was used with the PBE functional and all-electron TZ2P basis sets; the B3LYP functional was used with the Stuttgart relativistic small-core ANO/ECP basis sets. The parallel experimental and computational results illuminate fundamental aspects of hydration of f-element ion complexes. The experimental observations - kinetics and extent of hydration - are discussed in relationship to the computed structures and energetics of the hydrates. The absence of pentahydrates is in accord with the DFT results, which indicate that the lowest energy structures have the fifth water molecule in the second shell.
Herbert, Allan Jerome
1969-01-01T23:59:59.000Z
THE EMPIRICAL RELEVANCE OP THE DEFINITION OP WEALTH AS APPLIED TO THE THEORY OF THE CONSUMPTION FUNCTION A Thesis by ALI AN JEROME HEBERT Submitted to the Graduate College of Texas ASM University in Partial fulfillment of the requirement... for the degree of MASTER OF SCIENCE Ma l96 9 year Maj or Sub)set Economics THE EMPIRICAL RELEVANCE OF THE DEFINITION OF HEALTH AS APPLIED TO THE THEORY OF THE CONSUMPTION FUNCTION A Thesis by ALLAN JEROME HEBERT Approved as to style and content by: a...
Vijayakumar, M.; Hu, Jian Z.
2013-10-15T23:59:59.000Z
To analyze the lithium ion interaction with realistic graphene surfaces, we carried out dispersion corrected DFT-D3 studies on graphene with common point defects and chemisorbed oxygen containing functional groups along with defect free graphene surface. Our study reveals that, the interaction between lithium ion (Li+) and graphene is mainly through the delocalized ? electron of pure graphene layer. However, the oxygen containing functional groups pose high adsorption energy for lithium ion due to the Li-O ionic bond formation. Similarly, the point defect groups interact with lithium ion through possible carbon dangling bonds and/or cation-? type interactions. Overall these defect sites render a preferential site for lithium ions compared with pure graphene layer. Based on these findings, the role of graphene surface defects in lithium battery performance were discussed.
The spacetime of double field theory: Review, remarks, and outlook
Hohm, Olaf
We review double field theory (DFT) with emphasis on the doubled spacetime and its generalized coordinate transformations, which unify diffeomorphisms and b-field gauge transformations. We illustrate how the composition ...
Paris-Sud XI, Université de
2089 Fourth-order coherence-function theory of laser-induced molecular reorientational grating mécanisme de formation du réseau de population. Abstract. 2014 We have employed fourth-order coherence proposed to distinguish molecular reorientational grating from thermal grating. We then apply the fourth
Boyer, Edmond
Dynamical mean-field theory using Wannier functions: A flexible route to electronic structure materials with different degrees of structural and electronic complexity, SrVO3 and BaVS3, are investigated calculations of strongly correlated materials F. Lechermann,1,2, * A. Georges,1 A. Poteryaev,1 S. Biermann,1 M
Rappe, Andrew M.
Effect of substituting of S for O: The sulfide perovskite BaZrS3 investigated with density-principles density functional theory calculations to investigate the ground-state structure of sulfide perovskite Ba s : 71.15.Mb, 77.84. s I. INTRODUCTION The flexible structure of ABX3 X=O, S perovskites lends itself
Song, Xueyu
density functional theory. The equilibrium interfacial density profiles and interfacial free energies were of density profile. We found that the average interfacial free energy is about 0.78, which is in reasonable of the crystal-melt interface is the interfacial free energy. Experimentally, this quantity can be extracted from
Uranium (VI)Bis(imido) chalcogenate complexes:synthesis and density functional theory analysis
Spencer, Liam P [Los Alamos National Laboratory; Batista, Enrique R [Los Alamos National Laboratory; Boncella, James M [Los Alamos National Laboratory; Yang, Ping [Los Alamos National Laboratory; Scott, Brian L [Los Alamos National Laboratory
2009-01-01T23:59:59.000Z
Bis(imido) uranium(VI) trans- and cis-dichalcogenate complexes with the general formula U(NtBu)2(EAr)2(OPPh3)2 (EAr = O-2-tBuC6H4, SPh, SePh, TePh) and U(NtBu)2(EAr)2(R2bpy) (EAr = SPh, SePh, TePh) (R2bpy = 4,4'-disubstituted-2,2'-bipyridyl, R = Me, tBu) have been prepared. This family of complexes includes the first reported monodentate selenolate and tellurolate complexes of uranium(VI). Density functional theory calculations show that covalent interactions in the U-E bond increase in the trans-dichalcogenate series U(NtBu)2(EAr)2(OPPh3)2 as the size of the chalcogenate donor increases and that both 5f and 6d orbital participation is important in the M-E bonds of U-S, U-Se, and U-Te complexes.
Complex-energy approach to sum rules within nuclear density functional theory
Hinohara, Nobuo; Nazarewicz, Witold; Olsen, Erik
2015-01-01T23:59:59.000Z
The linear response of the nucleus to an external field contains unique information about the effective interaction, correlations, and properties of its excited states. To characterize the response, it is useful to use its energy-weighted moments, or sum rules. By comparing computed sum rules with experimental values, the information content of the response can be utilized in the optimization process of the nuclear Hamiltonian or EDF. But the additional information comes at a price: compared to the ground state, computation of excited states is more demanding. To establish an efficient framework to compute sum rules of the response that is adaptable to the optimization of the nuclear EDF and large-scale surveys of collective strength, we have developed a new technique within the complex-energy FAM based on the QRPA. To compute sum rules, we carry out contour integration of the response function in the complex-energy plane. We benchmark our results against the conventional matrix formulation of the QRPA theory...
Density functional theory investigation of 3d, 4d, and 5d 13-atom metal clusters
Piotrowski, Mauricio J.; Piquini, Paulo; Da Silva, Juarez L. F. [Departamento de Fisica, Universidade Federal de Santa Maria, Santa Maria 97105-900, RS (Brazil); Instituto de Fisica de Sao Carlos, Universidade de Sao Paulo, Cx. Postal 369, Sao Carlos 13560-970, SP (Brazil)
2010-04-15T23:59:59.000Z
The knowledge of the atomic structure of clusters composed by few atoms is a basic prerequisite to obtain insights into the mechanisms that determine their chemical and physical properties as a function of diameter, shape, surface termination, as well as to understand the mechanism of bulk formation. Due to the wide use of metal systems in our modern life, the accurate determination of the properties of 3d, 4d, and 5d metal clusters poses a huge problem for nanoscience. In this work, we report a density functional theory study of the atomic structure, binding energies, effective coordination numbers, average bond lengths, and magnetic properties of the 3d, 4d, and 5d metal (30 elements) clusters containing 13 atoms, M{sub 13}. First, a set of lowest-energy local minimum structures (as supported by vibrational analysis) were obtained by combining high-temperature first-principles molecular-dynamics simulation, structure crossover, and the selection of five well-known M{sub 13} structures. Several new lower energy configurations were identified, e.g., Pd{sub 13}, W{sub 13}, Pt{sub 13}, etc., and previous known structures were confirmed by our calculations. Furthermore, the following trends were identified: (i) compact icosahedral-like forms at the beginning of each metal series, more opened structures such as hexagonal bilayerlike and double simple-cubic layers at the middle of each metal series, and structures with an increasing effective coordination number occur for large d states occupation. (ii) For Au{sub 13}, we found that spin-orbit coupling favors the three-dimensional (3D) structures, i.e., a 3D structure is about 0.10 eV lower in energy than the lowest energy known two-dimensional configuration. (iii) The magnetic exchange interactions play an important role for particular systems such as Fe, Cr, and Mn. (iv) The analysis of the binding energy and average bond lengths show a paraboliclike shape as a function of the occupation of the d states and hence, most of the properties can be explained by the chemistry picture of occupation of the bonding and antibonding states.
Vukmirovic, Nenad
2010-01-01T23:59:59.000Z
Petersilka, Density Functional Theory (Springer, New York,Quantum Dots: Theory Nenad Vukmirovi´ and Lin-Wang Wang cdensity functional theory; electronic structure; empirical
Ferrero, Alejandro
2015-01-01T23:59:59.000Z
We analyze the $\\beta$-functions of Yukawa and electromagnetic theories with Lorentz violation (LV) and propose an alternative method to find the scale dependence of the different fields that parametrize such violations. The method of solution consists of decomposing a family of parameters into their irreducible representations and thus generating a group of subfamilies that obey the same symmetries and transformation rules. This method allows us to decouple the differential equations describing the $\\beta$-functions and find out if whether they are positive or not. For a set of parameters describing a Lorentz-violating theory, we expect their associated $\\beta$-functions to be nonnegative or, otherwise, their scale dependence to be weak enough. These conditions rely on the fact that asymptotically-free parameters can leave high imprints of LV at low energies, which are ruled out by observations. Besides imposing some constrains on the coefficients that describe LV, this method can be used to extract irreleva...
Magnetism in undoped ZnS studied from density functional theory
Xiao, Wen-Zhi, E-mail: xiaowenzhi@hnu.edu.cn, E-mail: llwang@hun.edu.cn; Rong, Qing-Yan; Xiao, Gang [Department of Physics and Mathematics, Hunan Institute of Engineering, Xiangtan 411104 (China); Wang, Ling-ling, E-mail: xiaowenzhi@hnu.edu.cn, E-mail: llwang@hun.edu.cn [School of Physics and Microelectronics and Key Lab for Micro-Nano Physics and Technology of Hunan Province, Hunan University, Changsha 410082 (China); Meng, Bo [College of Physics and Electronic Engineering, Caili University, Kaili 556011 (China)
2014-06-07T23:59:59.000Z
The magnetic property induced by the native defects in ZnS bulk, thin film, and quantum dots are investigated comprehensively based on density functional theory within the generalized gradient approximation + Hubbard U (GGA?+?U) approach. We find the origin of magnetism is closely related to the introduction of hole into ZnS systems. The relative localization of S-3p orbitals is another key to resulting in unpaired p-electron, due to Hund's rule. For almost all the ZnS systems under study, the magnetic moment arises from the S-dangling bonds generated by Zn vacancies. The charge-neutral Zn vacancy, Zn vacancy in 1? charge sate, and S vacancy in the 1+ charge sate produce a local magnetic moment of 2.0, 1.0, and 1.0??{sub B}, respectively. The Zn vacancy in the neutral and 1? charge sates are the important cause for the ferromagnetism in ZnS bulk, with a Curie temperature (T{sub C}) above room temperature. For ZnS thin film with clean (111) surfaces, the spins on each surface are ferromagnetically coupled but antiferromagnetically coupled between two surfaces, which is attributable to the internal electric field between the two polar (111) surfaces of the thin film. Only surface Zn vacancies can yield local magnetic moment for ZnS thin film and quantum dot, which is ascribed to the surface effect. Interactions between magnetic moments on S-3p states induced by hole-doping are responsible for the ferromagnetism observed experimentally in various ZnS samples.
Welden, Alicia Rae; Zgid, Dominika
2015-01-01T23:59:59.000Z
One-body Green's function theories implemented on the real frequency axis offer a natural formalism for the unbiased theoretical determination of quasiparticle spectra in molecules and solids. Self-consistent Green's function methods employing the imaginary axis formalism on the other hand can benefit from the iterative implicit resummation of higher order diagrams that are not included when only the first iteration is performed. Unfortunately, the imaginary axis Green's function does not give direct access to the desired quasiparticle spectra, which undermines its utility. To this end we investigate how reliably one can calculate quasiparticle spectra from the Extended Koopmans' Theorem (EKT) applied to the imaginary time Green's function in a second order approximation (GF2). We find that EKT in conjunction with GF2 yields IPs and EAs that systematically underestimate experimental and accurate coupled-cluster reference values for a variety of molecules and atoms. This establishes that the EKT allows one to ...
Landscape of the exact energy functional
Cohen, Aron J
2015-01-01T23:59:59.000Z
One of the great challenges of electronic structure theory is the search for the exact functional of density functional theory (DFT). Its existence is undoubted but it is hard to even conceptualize it as it is a surface in a massively multidimensional space. However, the asymmetric two-site Hubbard model has a two-dimensional universe of density matrices and the exact functional simply becomes a function of two variables whose landscape can be calculated, visualized and explored. This one unique surface contains all the possible physics of any system in this universe. A walk on this landscape, moved to the angle of any one-electron Hamiltonian, gives a valley whose minimum is the exact total energy. We show concrete examples of pure-state density matrices that are not v-representable due to the underlying non-convex nature of the exact functional. Using the Perdew, Parr, Levy and Balduz extension to fractional ensembles we calculate the exact functional for all numbers of electrons. The derivative discontinui...
DFT --Das Future Tool ``Das Future Tool'' was the title of the group T-shirt1 that we
Ziegler, Tom
TRIBUTE DFT -- Das Future Tool ``Das Future Tool'' was the title of the group T-shirt1 that we had and considered it just another semi-empirical method.2 Tom, however, realized that DFT was ``Das Future Tool
Density Functional Theory for Protein Transfer Free Energy Eric A. Mills and Steven S. Plotkin*
Plotkin, Steven S.
-solvation" repulsive force at larger distances. 1. INTRODUCTION Proteins fold and function in the crowded environment different that the conditions for protein folding are generally mutually exclusive between the two milieu environment on protein folding, stability, and function. Accurately accounting for the effects of the cell
Free-energy functionals of the electrostatic potential for Poisson-Boltzmann theory
Vikram Jadhao; Francisco J. Solis; Monica Olvera de la Cruz
2013-09-26T23:59:59.000Z
In simulating charged systems, it is often useful to treat some ionic components of the system at the mean-field level and solve the Poisson-Boltzmann (PB) equation to get their respective density profiles. The numerically intensive task of solving the PB equation at each step of the simulation can be bypassed using variational methods that treat the electrostatic potential as a dynamic variable. But such approaches require the access to a true free-energy functional; a functional that not only provides the correct solution of the PB equation upon extremization, it also evaluates to the true free energy of the system at its minimum. Moreover, the numerical efficiency of such procedures is further enhanced if the free-energy functional is local and is expressed in terms of the electrostatic potential. Existing PB functionals of the electrostatic potential, while possessing the local structure, are not free-energy functionals. We present a variational formulation with a local free-energy functional of the potential. In addition, we also construct a nonlocal free-energy functional of the electrostatic potential. These functionals are suited for employment in simulation schemes based on the ideas of dynamical optimization.
Fayer, Michael D.
(CO2) as a function of density from low density (well below the critical density) to high density ethane, carbon dioxide, and fluoroform as a function of density at two temperatures are presented of input information on the SCF properties obtained from the fluids' equations of state and other tabulated
Interaction energies of monosubstituted benzene dimers via nonlocal density functional theory
T. Thonhauser; Aaron Puzder; David C. Langreth
2005-09-15T23:59:59.000Z
We present density-functional calculations for the interaction energy of monosubstituted benzene dimers. Our approach utilizes a recently developed fully nonlocal correlation energy functional, which has been applied to the pure benzene dimer and several other systems with promising results. The interaction energy as a function of monomer distance was calculated for four different substituents in a sandwich and two T-shaped configurations. In addition, we considered two methods for dealing with exchange, namely using the revPBE generalized gradient functional as well as full Hartree-Fock. Our results are compared with other methods, such as Moller-Plesset and coupled-cluster calculations, thereby establishing the usefulness of our approach. Since our density-functional based method is considerably faster than other standard methods, it provides a computational inexpensive alternative, which is of particular interest for larger systems where standard calculations are too expensive or infeasible.
G. Chechin; D. Ryabov; S. Shcherbinin
2015-02-27T23:59:59.000Z
Some exact interactions between vibrational modes in systems with discrete symmetry can be described by the theory of the bushes of nonlinear normal modes (NNMs) [G.M. Chechin, V.P. Sakhnenko. Physica D 117, 43 (1998)]. Each bush represents a dynamical object conserving the energy of the initial excitation. Existence of bushes of NNMs is ensured by some group-theoretical selection rules. In [G.M. Chechin, et al. Int. J. Non-Linear Mech. 38, 1451 (2003)], existence and stability of the bushes of vibrational modes in the simple octahedral model of mass points interacting via Lennard-Jones potential were investigated. In the present paper, we study these dynamical objects by the density functional theory in SF6 molecule which possesses the same symmetry and structure. We have fully confirmed the results previously obtained in the framework of the group theoretical approach and have found some new properties of the bushes of NNMs.
V. Dorvilien; C. N. Patra; L. B. Bhuiyan; C. W. Outhwaite
2013-12-17T23:59:59.000Z
The structure of cylindrical double layers is studied using a modified Poisson Boltzmann theory and the density functional approach. In the model double layer, the electrode is a cylindrical polyion that is infinitely long, impenetrable, and uniformly charged. The polyion is immersed in a sea of equi-sized rigid ions embedded in a dielectric continuum. An in-depth comparison of the theoretically predicted zeta potentials, the mean electrostatic potentials, and the electrode-ion singlet density distributions is made with the corresponding Monte Carlo simulation data. The theories are seen to be consistent in their predictions that include variations in ionic diameters, electrolyte concentrations, and electrode surface charge densities, and are also capable of well reproducing some new and existing Monte Carlo results.
The Theory of Functional Forms of the Consumer Demand System and its Application
Usui, Ikuyasu
2010-01-25T23:59:59.000Z
This dissertation studies the consumer demand system focusing on its functional forms in the theoretical aspect and the empirical aspect. The theoretical part investigates the regularity property of the consumer demand ...
Jorge L. deLyra
2015-03-24T23:59:59.000Z
A correspondence between arbitrary Fourier series and certain analytic functions on the unit disk of the complex plane is established. The expression of the Fourier coefficients is derived from the structure of complex analysis. The orthogonality and completeness relations of the Fourier basis are derived in the same way. It is shown that the limiting function of any Fourier series is also the limit to the unit circle of an analytic function in the open unit disk. An alternative way to recover the original real functions from the Fourier coefficients, which works even when the Fourier series are divergent, is thus presented. The convergence issues are discussed up to a certain point. Other possible uses of the correspondence established are pointed out.
Of energy and the economy : theory and evidence for their functional relationship
Chang, Vincent H. (Vincent Hua-Cheng)
2007-01-01T23:59:59.000Z
This paper offers a set of explicit functional relationships that link energy and the economy. Despite the reliance on energy permeating the whole economy, no such complete relationships had been presented before. How ...
Ahmadi, Amir Ali
2008-01-01T23:59:59.000Z
Lyapunov's direct method, which is based on the existence of a scalar function of the state that decreases monotonically along trajectories, still serves as the primary tool for establishing stability of nonlinear systems. ...
Aliaga Salazar, James Wilson
2009-06-02T23:59:59.000Z
. In this study, we are mainly interested in developing a computational framework for the analysis of plate structures comprised of composite or functionally graded materials (FGM) with embedded or surface mounted piezoelectric sensors/actuators. These systems...
Aliaga Salazar, James Wilson
2009-06-02T23:59:59.000Z
Smart materials are very important because of their potential applications in the biomedical, petroleum and aerospace industries. They can be used to build systems and structures that self-monitor to function and adapt to new operating conditions...
Impaired Theory Of Mind for Moral Judgment in High-Functioning Autism
Moran, Joseph M.
High-functioning autism (ASD) is characterized by real-life difficulties in social interaction; however, these individuals often succeed on laboratory tests that require an understanding of another person's beliefs and ...
Jorge L. deLyra
2015-05-04T23:59:59.000Z
The results presented in this paper are refinements of some results presented in a previous paper. Three such refined results are presented. The first one relaxes one of the basic hypotheses assumed in the previous paper, and thus extends the results obtained there to a wider class of real functions. The other two relate to a closer examination of the issue of the representability of real functions by their Fourier coefficients. As was shown in the previous paper, in many cases one can recover the real function from its Fourier coefficients even if the corresponding Fourier series diverges almost everywhere. In such cases we say that the real function is still representable by its Fourier coefficients. Here we establish a very weak condition on the Fourier coefficients that ensures the representability of the function by those coefficients. In addition to this, we show that any real function that is absolutely integrable can be recovered almost everywhere from, and hence is representable by, its Fourier coefficients, regardless of whether or not its Fourier series converges. Interestingly, this also provides proof for a conjecture proposed in the previous paper.
Mariana Kirchbach; Andreas Wirzba
1996-11-01T23:59:59.000Z
The generating functional of heavy baryon chiral perturbation theory at order O(Q^2) in the mean field approximation (with a pseudoscalar source coupling which is consistent with the PCAC-Ward identities on the current quark level) has been exploited to derive Migdal's in--medium pion propagator. It is shown that the prediction for the density dependence of the quark condensate obtained on the composite hadron level by embedding PCAC within the framework of Migdal's approach to finite Fermi systems is identical to that resulting from QCD.
Kirchbach, M; Kirchbach, Mariana; Wirzba, Andreas
1996-01-01T23:59:59.000Z
The generating functional of heavy baryon chiral perturbation theory at order {\\cal O}(Q^2) in the mean field approximation (with a pseudoscalar source coupling which is consistent with the PCAC-Ward identities on the current quark level) has been exploited to derive Migdal's in--medium pion propagator. It is shown that the prediction for the density dependence of the quark condensate obtained on the composite hadron level by embedding PCAC within the framework of Migdal's approach to finite Fermi systems is identical to that resulting from QCD.
L. B. Bhuiyan; D. Henderson; S. Soko?owski
2012-07-13T23:59:59.000Z
A recently proposed local second contact value theorem [Henderson D., Boda D., J. Electroanal. Chem., 2005, 582, 16] for the charge profile of an electric double layer is used in conjunction with the existing Monte Carlo data from the literature to assess the contact behavior of the electrode-ion distributions predicted by the density functional theory. The results for the contact values of the co- and counterion distributions and their product are obtained for the symmetric valency, restricted primitive model planar double layer for a range of electrolyte concentrations and temperatures. Overall, the theoretical results satisfy the second contact value theorem reasonably well, the agreement with the simulations being semi-quantitative or better. The product of the co- and counterion contact values as a function of the electrode surface charge density is qualitative with the simulations with increasing deviations at higher concentrations.
Volodymyr P. Sergiievskyi; Guillaume Jeanmairet; Maximilien Levesque; Daniel Borgis
2014-06-11T23:59:59.000Z
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.
Hetero-twin formation during growth of nano-scale Al-TiN composites - experimental and DFT studies
Bhattacharyya, Dhriti [Los Alamos National Laboratory; Liu, Xiang - Yang [Los Alamos National Laboratory; Hoagland, Richard G [Los Alamos National Laboratory; Misra, Amit [Los Alamos National Laboratory; Genc, A [MSE, OSU; Fraser, H L [MSE, OSU
2009-01-01T23:59:59.000Z
It is well known that high stacking fault energy metals such as Al do not form either growth twins or mechanical twins easily. Although mechanical twins in nanocrystalline Al have been observed under certain conditions, growth twins have never been observed. In this work, the authors report for the first time, through transmission electron microscopy (TEM), that Al layers, when deposited on TiN layers, tend to grow in a twin relationship to both the TiN layer and the underlying Al layer. The TiN layers assume the orientation of the Al layers below. Calculations using density functional theory (DFT) show that nitrogen termination in the {l_brace}111{r_brace} growth plane of the TiN layers favors the growth of twin oriented Al layers over these TiN layers. This finding provides a way to create a twin-modulated structure in Al with the inclusion of intermediate nm-scale layer of an ionic solid such as TiN. Al metal is resistant to twinning, as it has a high stacking fault energy (SFE) of > 150 mJ/m. Although twins have been observed in nano-scale grains of Al, and predicted by molecular dynamics (MD) simulations in conditions when the nanoscale grains are plastically deformed, no process or phenomenon has been reported yet in which the deposition of an intermediate layer of a different material phase causes the subsequent layer of Al to be deposited in the twin orientation. The authors show in this paper that it is possible to form Al layers in twin orientation to each other across polar TiN layers, if these are grown so that both the Al and TiN layers have a {l_brace}111{r_brace} surface as their growth front. Since the deposition of Al and TiN layers is used in the formation of diffusion barriers, and the mechanical properties of these nanoscale multilayers are also seen to be exceptional, it is important to investigate and understand their structure at the nanometer length scale, and thence to be able to control it. Moreover, these findings point out a method of introducing nano-scale twins in high SFE materials in general, and can potentially improve the properties of nano-layered materials.
Communication: Self-interaction correction with unitary invariance in density functional theory
Pederson, Mark R., E-mail: mark.pederson@science.doe.gov [Office of Basic Energy Sciences, SC22.1, U.S. Department of Energy, Washington, DC 20585 (United States); Department of Chemistry, Johns Hopkins University, Baltimore, Maryland 21218 (United States); Ruzsinszky, Adrienn [Department of Physics, Temple University, Philadelphia, Pennsylvania 19122 (United States)] [Department of Physics, Temple University, Philadelphia, Pennsylvania 19122 (United States); Perdew, John P. [Department of Physics, Temple University, Philadelphia, Pennsylvania 19122 (United States) [Department of Physics, Temple University, Philadelphia, Pennsylvania 19122 (United States); Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122 (United States)
2014-03-28T23:59:59.000Z
Standard spin-density functionals for the exchange-correlation energy of a many-electron ground state make serious self-interaction errors which can be corrected by the Perdew-Zunger self-interaction correction (SIC). We propose a size-extensive construction of SIC orbitals which, unlike earlier constructions, makes SIC computationally efficient, and a true spin-density functional. The SIC orbitals are constructed from a unitary transformation that is explicitly dependent on the non-interacting one-particle density matrix. When this SIC is applied to the local spin-density approximation, improvements are found for the atomization energies of molecules.
Beylkin, Gregory
Multiresolution quantum chemistry in multiwavelet bases: Analytic derivatives for Hartree An efficient and accurate analytic gradient method is presented for HartreeFock and density functional differential equations. In this paper, we extend the approach to include computation of analytic derivatives
Bochevarov, Arteum D.
We report the performance of eight density functionals (B3LYP, BPW91, OLYP, O3LYP, M06, M06-2X, PBE, and SVWN5) in two Gaussian basis sets (Wachters and Partridge-1 on iron atoms; cc-pVDZ on the rest of atoms) for prediction ...
Mukamel, Shaul
for superconductors Oleg Berman1, * and Shaul Mukamel1,2, 1 Department of Chemistry, University of Rochester, Box-temperature superconductors. The temperature of the Kosterlitz- Thouless transition to the two-dimensional superfluidity for the ground-state wave function of superconductors predicts a gap in the spectrum1 originating from
On the Design of Loss Functions for Classification: theory, robustness to outliers, and SavageBoost
Vasconcelos, Nuno M.
state-of-the-art classifier design algorithms, including SVMs, boosting, and logistic regression, de literature. We show that the two problems are identical, and probability elicitation can be seen as a reverse, not the case for the reverse progression: it is shown that any functional form of the minimum conditio
On the Design of Loss Functions for Classification: theory, robustness to outliers, and SavageBoost
Vasconcelos, Nuno M.
stateoftheart classifier design algorithms, including SVMs, boosting, and logistic regression, de literature. We show that the two problems are identical, and probability elicitation can be seen as a reverse, not the case for the reverse progression: it is shown that any functional form
Desheng Li
2010-05-26T23:59:59.000Z
In this paper we first construct smooth Morse-Lyapunov functions of attractors for nonsmooth dynamical systems. Then we prove that all open attractor neighborhoods of an attractor have the same homotopy type. Based on this basic fact we finally introduce the concept of critical group for Morse sets of an attractor and establish Morse inequalities and equations.
The Fourier transform solution for the Green's function of monoenergetic neutron transport theory
Barry D. ganapol
2014-03-17T23:59:59.000Z
Nearly 45 years ago, Ken Case published his seminal paper on the singular eigenfunction solution for the Green's function of the monoenergetic neutron transport equation with isotropic scattering. Previously, the solution had been obtained by Fourier transform. While it is apparent the two had to be equivalent, a convincing equivalence proof for general anisotropic scattering remained a challenge until now.
L. C. T. Brito; H. G. Fargnoli; A. P. Baêta Scarpelli; Marcos Sampaio; M. C. Nemes
2009-03-12T23:59:59.000Z
We show that to n loop order the divergent content of a Feynman amplitude is spanned by a set of basic (logarithmically divergent) integrals which need not be evaluated. Only the coefficients of the basic divergent integrals are necessary to determine renormalization group functions. Relations between these coefficients of different loop orders are derived.
Wilkins, John
Comparison of screened hybrid density functional theory to diffusion Monte Carlo in calculations of total energies of silicon phases and defects Enrique R. Batista,1, * Jochen Heyd,2 Richard G. Hennig,3 for the prediction of defect properties using the Heyd-Scuseria-Ernzerhof HSE screened-exchange hybrid functional
Non-Gaussian halo mass function and non-spherical halo collapse: theory vs. simulations
Achitouv, Ixandra E.; Corasaniti, Pier Stefano, E-mail: Ixandra.Achitouv@obspm.fr, E-mail: Pier-Stefano.Corasaniti@obspm.fr [Laboratoire Univers et Théories (LUTh), UMR 8102 CNRS, Observatoire de Paris, Université Paris Diderot, 5 Place Jules Janssen, 92190 Meudon (France)
2012-02-01T23:59:59.000Z
The mass distribution of dark matter halos is a sensitive probe of primordial non-Gaussianity (NG). We derive an analytical formula of the halo mass function by perturbatively computing excursion set path-integrals for a non-Gaussian density field with non-vanishing skewness, f{sub NL}. We assume a stochastic barrier model which captures the main features of the ellipsoidal collapse of halos. Contrary to previous results based on extensions of the Press-Schechter formalism to NG initial conditions, we find that the non-spherical collapse of halos directly alter the signature of primordial NG. This points toward a potential degeneracy between the effect of primordial non-Gaussianity and that of non-linear halo collapse. The inferred mass function is found to be in remarkable agreement with N-body simulations of NG local type. Deviations are well within numerical uncertainties for all values of f{sub NL}{sup loc} in the range of validity of the perturbative calculation (|f{sub nl}{sup loc}|?<200). Moreover, the comparison with simulation results suggests that for |f{sub NL}|?>30 the non-linear collapse of halos, as described by our barrier model, strongly deviates from that of Gaussian initial conditions. This is not surprising since the effect of non-linear gravitational processes may be altered by initially large NG. Hence, in the lack of prior theoretical knowledge, halo collapse model parameters should be included in statistical halo mass function data analysis which aim to constrain the signature of primordial NG.
Perfetti, Christopher M [ORNL] [ORNL; Martin, William R [University of Michigan] [University of Michigan; Rearden, Bradley T [ORNL] [ORNL; Williams, Mark L [ORNL] [ORNL
2012-01-01T23:59:59.000Z
This study introduced three approaches for calculating the importance weighting function for Contributon and CLUTCH eigenvalue sensitivity coefficient calculations, and compared them in terms of accuracy and applicability. The necessary levels of mesh refinement and mesh convergence for obtaining accurate eigenvalue sensitivity coefficients were determined through two parametric studies, and the results of these studies suggest that a sufficiently-accurate mesh for calculating eigenvalue sensitivity coefficients can be obtained for the Contributon and CLUTCH methods with only a small increase in problem runtime.
Towards time-dependent current-density-functional theory in the non-linear regime
Escartín, J. M.; Vincendon, M.; Romaniello, P.; Dinh, P. M.; Reinhard, P.-G.; Suraud, E.
2015-02-27T23:59:59.000Z
? ? Im [???(r, t)???(r, t)] ? q mc AS(r, t) ?(r, t) , (2b) and are independent of the gauge chosen to represent the electromagnetic potentials. A. The Vignale-Kohn functional in real time Up to second order in spatial derivatives, under the basic... that, while treat- ing the memory instantaneously in time, maintains the dissipating effects of the VK approximation. We have demonstrated the capabilities of the method by apply- ing it to Mg, Ca and Na2 whereby we are modeling a short laser pulse...
A density functional theory model of mechanically activated silyl ester hydrolysis
Pill, Michael F.; Schmidt, Sebastian W. [Department of Applied Sciences and Mechatronics, Munich University of Applied Sciences, Lothstr. 34, 80335 Munich (Germany) [Department of Applied Sciences and Mechatronics, Munich University of Applied Sciences, Lothstr. 34, 80335 Munich (Germany); Institut für Physikalische Chemie, Christian-Albrechts-Universität zu Kiel, Olshausenstraße 40, 24098 Kiel (Germany); Center for Nanoscience (CeNS), Geschwister-Scholl-Platz 1, 80539 Munich (Germany); Beyer, Martin K. [Institut für Physikalische Chemie, Christian-Albrechts-Universität zu Kiel, Olshausenstraße 40, 24098 Kiel (Germany) [Institut für Physikalische Chemie, Christian-Albrechts-Universität zu Kiel, Olshausenstraße 40, 24098 Kiel (Germany); Institut für Ionenphysik und Angewandte Physik, Leopold-Franzens-Universität Innsbruck, Technikerstraße 25, 6020 Innsbruck (Austria); Clausen-Schaumann, Hauke [Department of Applied Sciences and Mechatronics, Munich University of Applied Sciences, Lothstr. 34, 80335 Munich (Germany) [Department of Applied Sciences and Mechatronics, Munich University of Applied Sciences, Lothstr. 34, 80335 Munich (Germany); Center for Nanoscience (CeNS), Geschwister-Scholl-Platz 1, 80539 Munich (Germany); Kersch, Alfred, E-mail: akersch@hm.edu [Department of Applied Sciences and Mechatronics, Munich University of Applied Sciences, Lothstr. 34, 80335 Munich (Germany)] [Department of Applied Sciences and Mechatronics, Munich University of Applied Sciences, Lothstr. 34, 80335 Munich (Germany)
2014-01-28T23:59:59.000Z
To elucidate the mechanism of the mechanically activated dissociation of chemical bonds between carboxymethylated amylose (CMA) and silane functionalized silicon dioxide, we have investigated the dissociation kinetics of the bonds connecting CMA to silicon oxide surfaces with density functional calculations including the effects of force, solvent polarizability, and pH. We have determined the activation energies, the pre-exponential factors, and the reaction rate constants of candidate reactions. The weakest bond was found to be the silyl ester bond between the silicon and the alkoxy oxygen atom. Under acidic conditions, spontaneous proton addition occurs close to the silyl ester such that neutral reactions become insignificant. Upon proton addition at the most favored position, the activation energy for bond hydrolysis becomes 31 kJ?mol{sup ?1}, which agrees very well with experimental observation. Heterolytic bond scission in the protonated molecule has a much higher activation energy. The experimentally observed bi-exponential rupture kinetics can be explained by different side groups attached to the silicon atom of the silyl ester. The fact that different side groups lead to different dissociation kinetics provides an opportunity to deliberately modify and tune the kinetic parameters of mechanically activated bond dissociation of silyl esters.
The Spacetime of Double Field Theory: Review, Remarks, and Outlook
Olaf Hohm; Dieter Lust; Barton Zwiebach
2014-10-30T23:59:59.000Z
We review double field theory (DFT) with emphasis on the doubled spacetime and its generalized coordinate transformations, which unify diffeomorphisms and b-field gauge transformations. We illustrate how the composition of generalized coordinate transformations fails to associate. Moreover, in dimensional reduction, the O(d,d) T-duality transformations of fields can be obtained as generalized diffeomorphisms. Restricted to a half-dimensional subspace, DFT includes `generalized geometry', but is more general in that local patches of the doubled space may be glued together with generalized coordinate transformations. Indeed, we show that for certain T-fold backgrounds with non-geometric fluxes, there are generalized coordinate transformations that induce, as gauge symmetries of DFT, the requisite O(d,d;Z) monodromy transformations. Finally we review recent results on the \\alpha' extension of DFT which, reduced to the half-dimensional subspace, yields intriguing modifications of the basic structures of generalized geometry.
Wopperer, P; Reinhard, P -G; Suraud, E
2014-01-01T23:59:59.000Z
Various ways to analyze the dynamical response of clusters and molecules to electromagnetic perturbations exist. Particularly rich information can be obtained from measuring the properties of electrons emitted in the course of the excitation dynamics. Such an analysis of electron signals covers total ionization, Photo-Electron Spectra, Photoelectron Angular Distributions, and ideally combined PES/PAD, with a long history in molecular physics, also increasingly used in cluster physics. Recent progress in the design of new light sources (high intensity and/or frequency, ultra short pulses) opens new possibilities for measurements and thus has renewed the interest on the analysis of dynamical scenarios through these observables, well beyond a simple access to a density of states. This, in turn, has motivated many theoretical investigations of the dynamics of electronic emission for molecules and clusters. A theoretical tool of choice is here Time-Dependent Density Functional Theory (TDDFT) propagated in real tim...
K. Hagino; J. M. Yao
2015-04-15T23:59:59.000Z
We describe low-lying collective excitations of atomic nuclei with the multi-reference covariant density functional theory, and combine them with coupled-channels calculations for heavy-ion fusion reactions at energies around the Coulomb barrier. To this end, we use the calculated transition strengths among several collective states as inputs to the coupled-channels calculations. This approach provides a natural way to describe anharmonic multi-phonon excitations as well as a deviation of rotational excitations from a simple rigid rotor. We apply this method to subbarrier fusion reactions of $^{58}$Ni+$^{58}$Ni, $^{58}$Ni+$^{60}$Ni and $^{40}$Ca+$^{58}$Ni systems. We find that the effect of anharmonicity tends to smear the fusion barrier distributions, better reproducing the experimental data compared to the calculations in the harmonic oscillator limit.
Huang, S. [Center for Theoretical Physics, Laboratory for Nuclear Science Department of Physics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 (United States)] [Center for Theoretical Physics, Laboratory for Nuclear Science Department of Physics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 (United States); [Department of Physics, FM-15, University of Washington, Seattle, Washington 98195 (United States); Lissia, M. [Center for Theoretical Physics, Laboratory for Nuclear Science Department of Physics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 (United States)] [Center for Theoretical Physics, Laboratory for Nuclear Science Department of Physics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 (United States); [Istituto Nazionale di Fisica Nucleare, via Ada Negri 18, I-09127 Cagliari (Italy); [Dipartimento di Fisica dell` Universita di Cagliari I-09124 Cagliari (Italy)
1995-07-15T23:59:59.000Z
Within the framework of the operator product expansion and the renormalization group equation, we show that the temperature and chemical potential dependence of the zeroth moment of a spectral function (SF) is completely determined by the one-loop structure in an asymptotically free theory, and in particular in QCD. Logarithmic corrections are found to play an essential role in the derivation. This exact result constrains the shape of SF`s, and implies striking effects near phase transitions. Phenomenological parametrizations of the SF, often used in applications such as the analysis of lattice QCD data or QCD sum rule calculations at finite temperature and baryon density, must satisfy these constraints. We also explicitly illustrate in detail the exact sum rule in the Gross-Neveu model.
Andreas Härtel; Mathijs Janssen; Sela Samin; René van Roij
2015-03-06T23:59:59.000Z
Capacitive mixing (CAPMIX) and capacitive deionization (CDI) are promising candidates for harvesting clean, renewable energy and for the energy efficient production of potable water, respectively. Both CAPMIX and CDI involve water-immersed porous carbon (supercapacitors) electrodes at voltages of the order of hundreds of millivolts, such that counter-ionic packing is important for the electric double layer (EDL) which forms near the surface of these porous materials. Thus, we propose a density functional theory (DFT) to model the EDL, where the White-Bear mark II fundamental measure theory functional is combined with a mean-field Coulombic and a mean spherical approximation-type correction to describe the interplay between dense packing and electrostatics, in good agreement with molecular dynamics simulations. We discuss the concentration-dependent potential rise due to changes in the chemical potential in capacitors in the context of an over-ideal theoretical description and its impact on energy harvesting and water desalination. Compared to less elaborate mean-field models our DFT calculations reveal a higher work output for blue-energy cycles and a higher energy demand for desalination cycles.
Tong, Xiao-Min; Chu, Shih-I
1998-01-01T23:59:59.000Z
We present a self-interaction-free time-dependent density-functional theory (TDDFT) for nonperturbative treatment of multiphoton processes of many-electron atomic systems in intense laser fields. The theory is based on the ...
Li, Xiaozhou; Bond, Andrew D.; Johansson, Kristoffer E.; Van de Streek, Jacco, E-mail: jacco.vandestreek@sund.ku.dk [Department of Pharmacy, University of Copenhagen, Universitetsparken 2, Copenhagen DK-2100 (Denmark)
2014-08-01T23:59:59.000Z
The crystal structure of (Z)-N-(5-ethyl-2,3-di-hydro-1,3,4-thiadiazol-2-ylidene) -4-methylbenzenesulfonamide contains an imine tautomer, rather than the previously reported amine tautomer. The tautomers can be distinguished using dispersion-corrected density functional theory calculations and by comparison of calculated and measured {sup 13}C solid-state NMR spectra. The crystal structure of the title compound, C{sub 11}H{sub 13}N{sub 3}O{sub 2}S{sub 2}, has been determined previously on the basis of refinement against laboratory powder X-ray diffraction (PXRD) data, supported by comparison of measured and calculated {sup 13}C solid-state NMR spectra [Hangan et al. (2010 ?). Acta Cryst. B66, 615–621]. The mol@@ecule is tautomeric, and was reported as an amine tautomer [systematic name: N-(5-ethyl-1,3,4-thia@@diazol-2-yl)-p-toluene@@sulfonamide], rather than the correct imine tautomer. The protonation site on the mol@@ecule’s 1,3,4-thia@@diazole ring is indicated by the inter@@molecular contacts in the crystal structure: N—H?O hydrogen bonds are established at the correct site, while the alternative protonation site does not establish any notable inter molecular inter@@actions. The two tautomers provide essentially identical Rietveld fits to laboratory PXRD data, and therefore they cannot be directly distinguished in this way. However, the correct tautomer can be distinguished from the incorrect one by previously reported qu@@anti@@tative criteria based on the extent of structural distortion on optimization of the crystal structure using dispersion-corrected density functional theory (DFT-D) calculations. Calculation of the {sup 13}C SS-NMR spectrum based on the correct imine tautomer also provides considerably better agreement with the measured {sup 13}C SS-NMR spectrum.
Morzan, Uriel N.; Ramírez, Francisco F.; Scherlis, Damián A., E-mail: damian@qi.fcen.uba.ar, E-mail: mcgl@qb.ffyb.uba.ar [Departamento de Química Inorgánica, Analítica y Química Física/INQUIMAE, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Ciudad Universitaria, Pab. II, Buenos Aires (C1428EHA) (Argentina); Oviedo, M. Belén; Sánchez, Cristián G. [Departamento de Matemática y Física, Facultad de Ciencias Químicas, INFIQC, Universidad Nacional de Córdoba, Ciudad Universitaria, X5000HUA Córdoba (Argentina)] [Departamento de Matemática y Física, Facultad de Ciencias Químicas, INFIQC, Universidad Nacional de Córdoba, Ciudad Universitaria, X5000HUA Córdoba (Argentina); Lebrero, Mariano C. González, E-mail: damian@qi.fcen.uba.ar, E-mail: mcgl@qb.ffyb.uba.ar [Instituto de Química y Fisicoquímica Biológicas, IQUIFIB, CONICET (Argentina)] [Instituto de Química y Fisicoquímica Biológicas, IQUIFIB, CONICET (Argentina)
2014-04-28T23:59:59.000Z
This article presents a time dependent density functional theory (TDDFT) implementation to propagate the Kohn-Sham equations in real time, including the effects of a molecular environment through a Quantum-Mechanics Molecular-Mechanics (QM-MM) hamiltonian. The code delivers an all-electron description employing Gaussian basis functions, and incorporates the Amber force-field in the QM-MM treatment. The most expensive parts of the computation, comprising the commutators between the hamiltonian and the density matrix—required to propagate the electron dynamics—, and the evaluation of the exchange-correlation energy, were migrated to the CUDA platform to run on graphics processing units, which remarkably accelerates the performance of the code. The method was validated by reproducing linear-response TDDFT results for the absorption spectra of several molecular species. Two different schemes were tested to propagate the quantum dynamics: (i) a leap-frog Verlet algorithm, and (ii) the Magnus expansion to first-order. These two approaches were confronted, to find that the Magnus scheme is more efficient by a factor of six in small molecules. Interestingly, the presence of iron was found to seriously limitate the length of the integration time step, due to the high frequencies associated with the core-electrons. This highlights the importance of pseudopotentials to alleviate the cost of the propagation of the inner states when heavy nuclei are present. Finally, the methodology was applied to investigate the shifts induced by the chemical environment on the most intense UV absorption bands of two model systems of general relevance: the formamide molecule in water solution, and the carboxy-heme group in Flavohemoglobin. In both cases, shifts of several nanometers are observed, consistently with the available experimental data.
Diebold, Ulrike
-terminated TiO2 rutile (011)-1 Â 1 surface shows an undulated surface topography with exposed two-fold O (O2cThe 2 Â 1 reconstruction of the rutile TiO2(011) surface: A combined density functional theory, X for publication 28 October 2008 Available online 5 November 2008 Keywords: Titanium dioxide Surface reconstruction
Gherman, Benjamin F.
and the Applicability of Density Functional Theory for Fuel Cell Modeling Nathan E. Schultz, Benjamin F. Gherman Form: August 18, 2006 Electrode poisoning by CO is a major concern in fuel cells. As interest. Introduction Several of the most successful fuel cell applications use a Pt anode as a catalyst
Final Technical Report for DE-SC0001878 [Theory and Simulation of Defects in Oxide Materials
Chelikowsky, James R. [University of Texas at Austin] [University of Texas at Austin
2014-04-14T23:59:59.000Z
We explored a wide variety of oxide materials and related problems, including materials at the nanoscale and generic problems associated with oxide materials such as the development of more efficient computational tools to examine these materials. We developed and implemented methods to understand the optical and structural properties of oxides. For ground state properties, our work is predominantly based on pseudopotentials and density functional theory (DFT), including new functionals and going beyond the local density approximation (LDA): LDA+U. To study excited state properties (quasiparticle and optical excitations), we use time dependent density functional theory, the GW approach, and GW plus Bethe-Salpeter equation (GW-BSE) methods based on a many-body Green function approaches. Our work focused on the structural, electronic, optical and magnetic properties of defects (such as oxygen vacancies) in hafnium oxide, titanium oxide (both bulk and clusters) and related materials. We calculated the quasiparticle defect states and charge transition levels of oxygen vacancies in monoclinic hafnia. we presented a milestone G0W0 study of two of the crystalline phases of dye-sensitized TiO{sub 2} clusters. We employed hybrid density functional theory to examine the electronic structure of sexithiophene/ZnO interfaces. To identify the possible effect of epitaxial strain on stabilization of the ferromagnetic state of LaCoO{sub 3} (LCO), we compare the total energy of the magnetic and nonmagnetic states of the strained theoretical bulk structure.
Rabindra Nath Das
2007-01-16T23:59:59.000Z
The linear non homogeneous singular integral equation (LNSIE)derived from the nonlinear non homogeneous integral eauation (NNIE)of Chandrsasekhar's H- functions is considered here to develop a new form of H - functions.The Plemelj's formulae are applied to that equation to determine a new linear non homogeneous integral equation(LNIE)for H- functions in complex plane . The analytic properties of this new linear integral equation are assessed and compared with known linear integral equations satisfied by H- functions. The Cauchy integral formulae in complex plane are used to obtain this form of H- functions not dependent on H- function in the integral . This new form of H-function is represented as a simple integral in terms of known functions both for conservative and non conservative cases. This is identical with the form of H- functions derived by this author by application of Wiener HOpf technique. The equivalence of application of the theory of linear singular integral equation in Riemann Hilbert Problem and of the technique of Wiener- Hopf in linear integral in representing the H- functions is therefore eatablished .This new form may be used for solving the problems of radiative transfer in anisotropic and non coherent scattering by the method of Laplace Transform and Wiener -Hopf technique.
TjT^f'Dft Ris#-R-442 Department of Reactor
Tf tf 4 otgiooRfc ©TjT^f'Dft Ris#-R-442 iK Department of Reactor Technology Annual Progress Report-R-442 DEPARTMENT OF REACTOR TECHNOLOGY ANNUAL PROGRESS REPORT 1 January - 31 December 1980 Abstract. The activities of the Department of Reactor Tech- nology at Riso during 1980 are described. The work is presented
Density functional theory study of first-layer adsorption of ZrO2 and HfO2 on Ge(100)
Kummel, Andrew C.
Density functional theory study of first-layer adsorption of ZrO2 and HfO2 on Ge(100) T.J. Grassman on the Ge(100)-4 Â 2 surface. Surface binding geometries of metal-down (OMGe) and oxygen-down (M OGe) were considered, including both adsorbate and displacement geometries of MOGe. Calculated enthalpies
A. Mironov; A. Zabrodin
1992-01-08T23:59:59.000Z
Using the finite-size effects the scaling dimensions and correlation functions of the main operators in continuous and lattice models of 1d spinless Bose-gas with pairwise interaction of rather general form are obtained. The long-wave properties of these systems can be described by the Gaussian model with central charge $c=1$. The disorder operators of the extended Gaussian model are found to correspond to some non-local operators in the {\\it XXZ} Heisenberg antiferromagnet. Just the same approach is applicable to fermionic systems. Scaling dimensions of operators and correlation functions in the systems of interacting Fermi-particles are obtained. We present a universal treatment for $1d$ systems of different kinds which is independent of the exact integrability and gives universal expressions for critical exponents through the thermodynamic characteristics of the system.
Song, Xueyu
perturbation theory. The free energies of the liquid and solid phases are computed using the fundamental to compute free energies of liquid and solid mixtures and, hence, to study alloy phase behaviors an effective hard-sphere HS system. The free energy is, thus, separated into two parts: one of them is the free
Revisiting HgCl2: A Solution- and Solid-State 199Hg NMR and ZORA-DFT Computational Study
Taylor, Robert E; Carver, Colin T; Larsen, Ross E; Dmitrenko, Olga; Bai, Shi; Dybowski, Cecil
2009-01-01T23:59:59.000Z
7 (1997), 333-336. [26] R. E. Taylor, Concepts Magn. Reson.DFT Computational Study R. E. Taylor 1 *, Colin T. Carver2522 USA *Corresponding author: R. E. Taylor Email address:
DFT-MD approach to TiO2/liquid interface systems for photocatalysis and dye-sensitised solar cell
Katsumoto, Shingo
DFT-MD approach to TiO2/liquid interface systems for photocatalysis and dye-sensitised solar cell- namics (MD) analysis of TiO2/solution in- terfaces related to photocatalysis and dye- sensitized solar
Arghavani Nia, Borhan, E-mail: b.arghavani@gmail.com [Department of Physics, Kermanshah Branch, Islamic Azad University, Kermanshah (Iran, Islamic Republic of); Sedighi, Matin [Department of Physics, Kermanshah Branch, Islamic Azad University, Kermanshah (Iran, Islamic Republic of); Shahrokhi, Masoud [Young Researchers and Elite Club, Kermanshah Branch, Islamic Azad University, Kermanshah (Iran, Islamic Republic of); Moradian, Rostam [Nano-Science and Nano-Technology Research Center, Razi University, Kermanshah (Iran, Islamic Republic of); Computational Physics Science Research Laboratory, Department of Nano-Science, Institute for Studies in Theoretical Physics and Mathematics (IPM), P.O. Box 19395-1795, Tehran (Iran, Islamic Republic of)
2013-11-15T23:59:59.000Z
A density functional theory study of structural, electronical and optical properties of Ca{sub 3}Sb{sub 2} compound in hexagonal and cubic phases is presented. In the exchange–correlation potential, generalized gradient approximation (PBE-GGA) has been used to calculate lattice parameters, bulk modulus, cohesive energy, dielectric function and energy loss spectra. The electronic band structure of this compound has been calculated using the above two approximations as well as another form of PBE-GGA, proposed by Engle and Vosko (EV-GGA). It is found that the hexagonal phase of Ca{sub 3}Sb{sub 2} has an indirect gap in the ??N direction; while in the cubic phase there is a direct-gap at the ? point in the PBE-GGA and EV-GGA. Effects of applying pressure on the band structure of the system studied and optical properties of these systems were calculated. - Graphical abstract: A density functional theory study of structural, electronic and optical properties of Ca{sub 3}Sb{sub 2} compound in hexagonal and cubic phases is presented. Display Omitted - Highlights: • Physical properties of Ca{sub 3}Sb{sub 2} in hexagonal and cubic phases are investigated. • It is found that the hexagonal phase is an indirect gap semiconductor. • Ca{sub 3}Sb{sub 2} is a direct-gap semiconductor at the ? point in the cubic phase. • By increasing pressure the semiconducting band gap and anti-symmetry gap are decreased.
Electromagnetic Theory 1 /56 Electromagnetic Theory
Bicknell, Geoff
Electromagnetic Theory 1 /56 Electromagnetic Theory Summary: · Maxwell's equations · EM Potentials · Equations of motion of particles in electromagnetic fields · Green's functions · Lienard-Weichert potentials · Spectral distribution of electromagnetic energy from an arbitrarily moving charge #12;Electromagnetic
Chu, Shih-I; Chu, Xi
2001-01-17T23:59:59.000Z
We present a self-interaction-free time-dependent density-functional theory (TDDFT) for nonperturbative treatment of multiphoton processes of many-electron molecular systems in intense laser fields. The time-dependent ...
Chu, Xi; Chu, Shih-I
2001-11-14T23:59:59.000Z
We present a time-dependent density-functional theory (TDDFT) with proper asymptotic long-range potential for nonperturbative treatment of multiphoton processes of many-electron molecular systems in intense laser fields. ...
Chu, Shih-I; Telnov, Dmitry A.
2009-04-03T23:59:59.000Z
We present a time-dependent density-functional-theory approach for the ab initio study of the effect of correlated multielectron responses on the multiphoton ionization (MPI) of diatomic molecules N2, O2, and F2 in intense ...
Fahleson, Tobias; Norman, Patrick, E-mail: panor@ifm.liu.se [Department of Physics, Chemistry and Biology, Linköping University, SE-581 83 Linköping (Sweden); Coriani, Sonia, E-mail: coriani@units.it [Dipartimento di Scienze Chimiche e Farmaceutiche, Università degli Studi di Trieste, I-34127 Trieste (Italy); Rizzo, Antonio, E-mail: rizzo@ipcf.cnr.it [CNR - Consiglio Nazionale delle Ricerche, Istituto per i Processi Chimico Fisici (IPCF-CNR), UOS di Pisa, I-56124 Pisa (Italy); Rikken, Geert L. J. A., E-mail: geert.rikken@lncmi.cnrs.fr [Laboratoire National des Champs Magnétiques Intenses, UPR3228, CNRS/INSA/UJF/UPS, Toulouse and Grenoble (France)
2013-11-21T23:59:59.000Z
We report on the results of a systematic ab initio study of the Jones birefringence of noble gases, of furan homologues, and of monosubstituted benzenes, in the gas phase, with the aim of analyzing the behavior and the trends within a list of systems of varying size and complexity, and of identifying candidates for a combined experimental/theoretical study of the effect. We resort here to analytic linear and nonlinear response functions in the framework of time-dependent density functional theory. A correlation is made between the observable (the Jones constant) and the atomic radius for noble gases, or the permanent electric dipole and a structure/chemical reactivity descriptor as the para Hammett constant for substituted benzenes.
Afshar, Mahdi [Department of Physics, Iran University of Science and Technology, Tehran (Iran, Islamic Republic of)] [Department of Physics, Iran University of Science and Technology, Tehran (Iran, Islamic Republic of); Sargolzaei, Mohsen [Department of Chemistry, Shahrood University of Technology, Shahrood (Iran, Islamic Republic of)] [Department of Chemistry, Shahrood University of Technology, Shahrood (Iran, Islamic Republic of)
2013-11-15T23:59:59.000Z
We have demonstrated electronic structure and magnetic properties of Cu{sub 3}, Ag{sub 3} and Au{sub 3} trimers using a full potential local orbital method in the framework of relativistic density functional theory. We have also shown that the non-relativistic generalized gradient approximation for the exchange-correlation energy functional gives reliable magnetic properties in coinage metal trimers compared to experiment. In addition we have indicated that the spin-orbit coupling changes the structure and magnetic properties of gold trimer while the structure and magnetic properties of copper and silver trimers are marginally affected. A significant orbital moment of 0.21?{sub B} was found for most stable geometry of the gold trimer whereas orbital magnetism is almost quenched in the copper and silver trimers.
Berland, Kristian [Chalmers University of Technology, Sweden] [Chalmers University of Technology, Sweden; Arter, Calvin A [Wake Forest University, Winston-Salem] [Wake Forest University, Winston-Salem; Cooper, Valentino R [ORNL] [ORNL; Lee, Dr. Kyuho [Lawrence Berkeley National Laboratory (LBNL)] [Lawrence Berkeley National Laboratory (LBNL); Lundqvist, Prof. Bengt I. [Chalmers University of Technology, Sweden] [Chalmers University of Technology, Sweden; Schroder, Prof. Elsebeth [Chalmers University of Technology, Sweden] [Chalmers University of Technology, Sweden; Thonhauser, Prof. Timo [Wake Forest University, Winston-Salem] [Wake Forest University, Winston-Salem; Hyldgaard, Per [Chalmers University of Technology, Sweden] [Chalmers University of Technology, Sweden
2014-01-01T23:59:59.000Z
The theoretical description of sparse matter attracts much interest, in particular for those groundstate properties that can be described by density functional theory (DFT). One proposed approach, the van der Waals density functional (vdW-DF) method, rests on strong physical foundations and offers simple yet accurate and robust functionals. A very recent functional within this method called vdW-DF-cx [K. Berland and P. Hyldgaard, Phys. Rev. B, in print] stands out in its attempt to use an exchange energy derived from the same plasmon-based theory from which the nonlocal correlation energy was derived. Encouraged by its good performance for solids, layered materials, and aromatic molecules, we apply it to several systems that are characterized by competing interactions. These include the ferroelectric response in PbTiO3, the adsorption of small molecules within metal-organic frameworks (MOFs), the graphite/diamond phase transition, and the adsorption of an aromaticmolecule on the Ag(111) surface. Our results indicate that vdW-DF-cx is overall well suited to tackle these challenging systems. In addition to being a competitive density functional for sparse matter, the vdW-DF-cx construction presents a more robust general purpose functional that could be applied to a range of materials problems with a variety of competing interactions.
S. A. Larin; M. Moennigmann; M. Stroesser; V. Dohm
1997-11-07T23:59:59.000Z
We present an analytic five-loop calculation for the additive renormalization constant A(u,epsilon) and the associated renormalization-group function B(u) of the specific heat of the O(n) symmetric phi^4 theory within the minimal subtraction scheme. We show that this calculation does not require new five-loop integrations but can be performed on the basis of the previous five-loop calculation of the four-point vertex function combined with an appropriate identification of symmetry factors of vacuum diagrams. We also determine the amplitude functions of the specific heat in three dimensions for n=1,2,3 above T_c and for n=1 below T_c up to five-loop order. Accurate results are obtained from Borel resummations of B(u) for n=1,2,3 and of the amplitude functions for n=1. Previous conjectures regarding the smallness of the resummed higher-order contributions are confirmed. Borel resummed universal amplitude ratios A^+/A^- and a_c^+/a_c^- are calculated for n=1.
Kaufman-Osborn, Tobin [Materials Science and Engineering Program, University of California, San Diego, La Jolla, California 92093 (United States); Chagarov, Evgueni A. [Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92093 (United States); Kummel, Andrew C., E-mail: akummel@ucsd.edu [Materials Science and Engineering Program, University of California, San Diego, La Jolla, California 92093 (United States); Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92093 (United States)
2014-05-28T23:59:59.000Z
Passivation, functionalization, and atomic layer deposition nucleation via H{sub 2}O{sub 2}(g) and trimethylaluminum (TMA) dosing was studied on the clean Ge(100) surface at the atomic level using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). Chemical analysis of the surface was performed using x-ray photoelectron spectroscopy, while the bonding of the precursors to the substrate was modeled with density functional theory (DFT). At room temperature, a saturation dose of H{sub 2}O{sub 2}(g) produces a monolayer of a mixture of –OH or –O species bonded to the surface. STS confirms that H{sub 2}O{sub 2}(g) dosing eliminates half-filled dangling bonds on the clean Ge(100) surface. Saturation of the H{sub 2}O{sub 2}(g) dosed Ge(100) surface with TMA followed by a 200?°C anneal produces an ordered monolayer of thermally stable Ge–O–Al bonds. DFT models and STM simulations provide a consistent model of the bonding configuration of the H{sub 2}O{sub 2}(g) and TMA dosed surfaces. STS verifies the TMA/H{sub 2}O{sub 2}/Ge surface has an unpinned Fermi level with no states in the bandgap demonstrating the ability of a Ge–O–Al monolayer to serve as an ideal template for further high-k deposition.
Duality Symmetric String and M-Theory
David S. Berman; Daniel C. Thompson
2014-12-09T23:59:59.000Z
We review recent developments in duality symmetric string theory. We begin with the world sheet doubled formalism which describes strings in an extended space time with extra coordinates conjugate to winding modes. This formalism is T-duality symmetric and can accommodate non-geometric T-fold backgrounds which are beyond the scope of Riemannian geometry. Vanishing of the conformal anomaly of this theory can be interpreted as a set of spacetime equations for the background fields. These equations follow from an action principle that has been dubbed Double Field Theory (DFT). We review the aspects of generalised geometry relevant for DFT. We outline recent extensions of DFT and explain how, by relaxing the so-called strong constraint with a Scherk Schwarz ansatz, one can obtain backgrounds that simultaneously depend on both the regular and T-dual coordinates. This provides a purely geometric higher dimensional origin to gauged supergravities that arise from non-geometric compactification. We then turn to M-theory and describe recent progress in formulating an E_{n(n)} U-duality covariant description of the dynamics. We describe how spacetime may be extended to accommodate coordinates conjugate to brane wrapping modes and the construction of generalised metrics in this extend space that unite the bosonic fields of supergravity into a single object. We review the action principles for these theories and their novel gauge symmetries. We also describe how a Scherk Schwarz reduction can be applied in the M-theory context and the resulting relationship to the embedding tensor formulation of maximal gauged supergravities.
Spencer, Liam P.; Yang, Ping; Minasian, Stefan G.; Jilek, Robert E.; Batista, Enrique R.; Boland, Kevin S.; Boncella, James M.; Conradson, S. D.; Clark, David L.; Hayton, Trevor W.; Kozimor, Stosh A.; Martin, Richard L.; MacInnes, Molly M.; Olson, Angela C.; Scott, Brian L.; Shuh, D. K.; Wilkerson, Marianne P.
2013-02-13T23:59:59.000Z
Synthetic routes to salts containing uranium bisimido tetrahalide anions [U(NR)(2)X-4](2-) (X = Cl-, Br-) and non-coordinating NEt4+ and PPh4+ countercations are reported. In general, these compounds can be prepared from U(NR)(2)I-2(THF)(x) (x = 2 and R = 'Bu, Ph; x = 3 and R = Me) upon addition of excess halide. In addition to providing stable coordination complexes with Cl-, the [U(NMe)(2)](2 +) cation also reacts with Br- to form stable [NEt4](2)[U(NMe)(2)Br-4] complexes. These materials were used as a platform to compare electronic structure and bonding in [U(NR)(2)](2+) with [UO2](2+). Specifically, Cl K-edge X-ray absorption spectroscopy (XAS) and both ground-state and time-dependent hybrid density functional theory (DFT and TDDFT) were used to probe U-Cl bonding interactions in [PPh4](2)[U((NBu)-Bu-t)(2)Cl-4] and [PPh4](2)[UO2Cl4]. The DFT and XAS results show the total amount of Cl 3p character mixed with the U 5f orbitals was roughly 7-10% per U-Cl bond for both compounds, which shows that moving from oxo to imido has little effect on orbital mixing between the U 5f and equatorial Cl 3p orbitals. The results are presented in the context of recent Cl K-edge XAS and DFT studies on other hexavalent uranium chloride systems with fewer oxo or imido ligands.
DFT study on cysteine adsorption mechanism on Au(111) and Au(110)
Buimaga-Iarinca, Luiza; Floare, Calin G.; Calborean, Adrian; Turcu, Ioan [National Institute for Research and Development of Isotopic and Molecular Technologies, 65-103 Donath, 400293 Cluj-Napoca (Romania)] [National Institute for Research and Development of Isotopic and Molecular Technologies, 65-103 Donath, 400293 Cluj-Napoca (Romania)
2013-11-13T23:59:59.000Z
Periodic density functional theory calculations were used to investigate relevant aspects of adsorption mechanisms of cysteine dimers in protonated form on Au(111) and Au(110) surfaces. The projected densities of states are explicitly discussed for all main chemical groups of cysteine, i.e. the amino group (NH2), the thiol group (SH) and the carboxylic group (COOH) to identify differences in adsorption mechanism. Special emphasis is put on the analysis of changes in the electronic structure of molecules adsorbed on Au(111) and Au(110) surfaces as well as the accompanying charge transfer mechanisms at molecule-substrate interaction.
Cox, Stephen J.; Michaelides, Angelos, E-mail: angelos.michaelides@ucl.ac.uk [Thomas Young Centre and London Centre for Nanotechnology, 17–19 Gordon Street, London WC1H 0AH (United Kingdom) [Thomas Young Centre and London Centre for Nanotechnology, 17–19 Gordon Street, London WC1H 0AH (United Kingdom); Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ (United Kingdom); Towler, Michael D. [Department of Earth Sciences, University College London Gower Street, London WC1E 6BT (United Kingdom) [Department of Earth Sciences, University College London Gower Street, London WC1E 6BT (United Kingdom); Theory of Condensed Matter Group, Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, Cambridge CB3 0HE (United Kingdom); Alfè, Dario [Thomas Young Centre and London Centre for Nanotechnology, 17–19 Gordon Street, London WC1H 0AH (United Kingdom) [Thomas Young Centre and London Centre for Nanotechnology, 17–19 Gordon Street, London WC1H 0AH (United Kingdom); Department of Earth Sciences, University College London Gower Street, London WC1E 6BT (United Kingdom)
2014-05-07T23:59:59.000Z
High quality reference data from diffusion Monte Carlo calculations are presented for bulk sI methane hydrate, a complex crystal exhibiting both hydrogen-bond and dispersion dominated interactions. The performance of some commonly used exchange-correlation functionals and all-atom point charge force fields is evaluated. Our results show that none of the exchange-correlation functionals tested are sufficient to describe both the energetics and the structure of methane hydrate accurately, while the point charge force fields perform badly in their description of the cohesive energy but fair well for the dissociation energetics. By comparing to ice I{sub h}, we show that a good prediction of the volume and cohesive energies for the hydrate relies primarily on an accurate description of the hydrogen bonded water framework, but that to correctly predict stability of the hydrate with respect to dissociation to ice I{sub h} and methane gas, accuracy in the water-methane interaction is also required. Our results highlight the difficulty that density functional theory faces in describing both the hydrogen bonded water framework and the dispersion bound methane.
Rabindra Nath Das
2007-02-22T23:59:59.000Z
In Radiative transfer, the intensities of radiation from the bounding faces of finite slab are obtained in terms of X- and Y- functions of Chandrasekhar . Those are non linear non homogeneous coupled integral equations . Those non linear integral equations are meromorphically extended to the complex plane to get linear non homogeneous coupled integral equations. Those linear integral equations are converted to linear singular integral equations with. linear constraints . Those singular integral equations are then transformed to non homogeneous Riemann Hilbert Problems. Solutions of those Riemann Hilbert Problems are obtained using the theory of linear singular integral equations to decouple those X- and Y- functions. New forms of linear non homogeneous decoupled integral equations are derived for X- and Y- function separately with new linear constraints. Those new decoupled integral equations are transformed into linear singular integral equations to get two new separate non homogeneous Riemann Hilbert problems and to find solutions in terms of one known N- function and five new unknown functions in complex plane . All five functions are represented in terms of N-functions using the theory of contour integration >. Those X- and Y- functions are finally expressed in terms of that N - function and also in terms of H- functions of Chandrasekhar and of integrals in Cauchy principal value sense in the complex plane and real plane. both for conservative and non conservative cases . The H - functions for semi infinite atmosphere are derived as a limiting case from the expression of X- function of finite atmosphere.
Salciccioli, Michael; Yu, Weiting; Barteau, Mark A; Chen, Jingguang; Vlachos, Dion G.
2011-05-25T23:59:59.000Z
Understanding and controlling bond-breaking sequences of oxygenates on transition metal catalysts can greatly impact the utilization of biomass feedstocks for fuels and chemicals. The decomposition of ethylene glycol, as the simplest representative of biomass-derived polyols, was studied via density functional theory (DFT) calculations to identify the differences in reaction pathways between Pt and the more active Ni/Pt bimetallic catalyst. Comparison of the computed transition states indicated three potentially feasible paths from ethylene glycol to C1 oxygenated adsorbates on Pt. While not important on Pt, the pathway to 1,2-dioxyethylene (OCH?CH?O) is favored energetically on the Ni/Pt catalyst. Temperature-programmed desorption (TPD) experiments were conducted with deuterated ethylene glycols for comparison with DFT results. These experiments confirmed that decomposition of ethylene glycol on Pt proceeds via initial O–H bond cleavage, followed by C–H and the second O–H bond cleavages, whereas on the Ni/Pt surface, both O–H bonds are cleaved initially. The results are consistent with vibrational spectra and indicate that tuning of the catalyst surface can selectively control bond breaking. Finally, the significant mechanistic differences in decomposition of polyols compared to that of monoalcohols and hydrocarbons serve to identify general trends in bond scission sequences.
J. M. Yao; L. S. Song; K. Hagino; P. Ring; J. Meng
2015-01-29T23:59:59.000Z
We report a systematic study of nuclear matrix elements (NMEs) in neutrinoless double-beta decays with a state-of-the-art beyond mean-field covariant density functional theory. The dynamic effects of particle-number and angular-momentum conservations as well as quadrupole shape fluctuations are taken into account with projections and generator coordinate method for both initial and final nuclei. The full relativistic transition operator is adopted to calculate the NMEs. The present systematic studies show that in most of the cases there is a much better agreement with the previous non-relativistic calculation based on the Gogny force than in the case of the nucleus $^{150}$Nd found in Song et al. [Phys. Rev. C 90, 054309 (2014)]. In particular, we find that the total NMEs can be well approximated by the pure axial-vector coupling term with a considerable reduction of the computational effort.
Duan, Yuhua; Zhang, Bo; Sorescu, Dan C.; Johnson, Karl; Majzoub, Eric H; Luebke, David R.
2012-07-01T23:59:59.000Z
The structural, electronic, phonon dispersion and thermodynamic properties of MHCO3 (M D Li, Na, K) solids were investigated using density functional theory. The calculated bulk properties for both their ambient and the high-pressure phases are in good agreement with available experimental measurements. Solid phase LiHCO3 has not yet been observed experimentally. We have predicted several possible crystal structures for LiHCO3 using crystallographic database searching and prototype electrostatic ground state modeling. Our total energy and phonon free energy .FPH/ calculations predict that LiHCO3 will be stable under suitable conditions of temperature and partial pressures of CO2 and H2O. Our calculations indicate that the HCO 3 groups in LiHCO3 and NaHCO3 form an infinite chain structure through O#1; #1; #1;H#1; #1; #1;O hydrogen bonds. In contrast, the HCO 3 anions form dimers, .HCO 3 /2, connected through double hydrogen bonds in all phases of KHCO3. Based on density functional perturbation theory, the Born effective charge tensor of each atom type was obtained for all phases of the bicarbonates. Their phonon dispersions with the longitudinal optical–transverse optical splitting were also investigated. Based on lattice phonon dynamics study, the infrared spectra and the thermodynamic properties of these bicarbonates were obtained. Over the temperature range 0–900 K, the FPH and the entropies (S) of MHCO3 (M D Li, Na, K) systems vary as FPH.LiHCO3/ > FPH.NaHCO3/ > FPH.KHCO3/ and S.KHCO3/ > S.NaHCO3/ > S.LiHCO3/, respectively, in agreement with the available experimental data. Analysis of the predicted thermodynamics of the CO2 capture reactions indicates that the carbonate/bicarbonate transition reactions for Na and K could be used for CO2 capture technology, in agreement with experiments.
Kawaguchi, Yoshizo [Research Institute for Innovation in Sustainable Chemistry, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki 305-8565 (Japan); Electronics and Photonics Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki 305-8568 (Japan); Sasaki, Fumio; Mochizuki, Hiroyuki [Electronics and Photonics Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki 305-8568 (Japan); Ishitsuka, Tomoaki; Tomie, Toshihisa [Research Institute of Instrumentation Frontier, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki 305-8568 (Japan); Ootsuka, Teruhisa [Nanoelectronics Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki 305-8568 (Japan); Watanabe, Shuji [Graduate School of Science and Engineering, Yamagata University, 1-4-12, Kojirakawa, Yamagata 990-8560 (Japan); Nanosystem Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki 305-8568 (Japan); Shimoi, Yukihiro [Nanosystem Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki 305-8568 (Japan); Yamao, Takeshi; Hotta, Shu [Department of Macromolecular Science and Engineering, Graduate School of Science and Technology, Kyoto Institute of Technology, Matsugasaki, Sakyo-ku, Kyoto 606-8585 (Japan)
2013-02-28T23:59:59.000Z
We have investigated electronic states in the valence electron bands for the thin films of three thiophene/phenylene co-oligomer (TPCO) compounds, 2,5-bis(4-biphenylyl)thiophene (BP1T), 1,4-bis(5-phenylthiophen-2-yl)benzene (AC5), and 1,4-bis{l_brace}5-[4-(trifluoromethyl)phenyl]thiophen-2-yl{r_brace}benzene (AC5-CF{sub 3}), by using extreme-UV excited photoelectron spectroscopy (EUPS). By comparing both EUPS spectra and secondary electron spectra between AC5 and AC5-CF{sub 3}, we confirm that CF{sub 3} substitution to AC5 deepens valence states by 2 eV, and increases the ionization energy by 3 eV. From the cut-off positions of secondary electron spectra, the work functions of AC5, AC5-CF{sub 3}, and BP1T are evaluated to be 3.8 eV, 4.8 eV, and 4.0 eV, respectively. We calculate molecular orbital (MO) energy levels by the density functional theory and compare results of calculations with those of experiments. Densities of states obtained by broadening MO levels well explain the overall features of experimental EUPS spectra of three TPCOs.
The DFT+Umol method and its application to the adsorption of CO on platinum model clusters
Soini, Thomas M.; Krüger, Sven [Department Chemie and Catalysis Research Center, Technische Universität München, 85747 Garching (Germany)] [Department Chemie and Catalysis Research Center, Technische Universität München, 85747 Garching (Germany); Rösch, Notker, E-mail: roesch@mytum.de [Department Chemie and Catalysis Research Center, Technische Universität München, 85747 Garching (Germany) [Department Chemie and Catalysis Research Center, Technische Universität München, 85747 Garching (Germany); Institute of High Performance Computing, Agency for Science, Technology and Research, 1 Fusionopolis Way, No. 16-16 Connexis, Singapore 138632 (Singapore)
2014-05-07T23:59:59.000Z
Semi-local DFT approximations are well-known for their difficulty with describing the correct site preference for the adsorption of CO molecules on (111) surfaces of several late transition metals. To address this problem originating from a residual self-interaction in the CO LUMO, we present the DFT+Umol approach which generalizes the empirical DFT+U correction to fragment molecular orbitals. This correction is applied to examine CO adsorption energies at various sites on the (111) facets of cuboctahedral clusters Pt{sub m}(CO){sub 8} (m = 79, 140, 225). The DFT+Umol correction leaves the electronic ground state of metal clusters, in particular their d-band structure, essentially unchanged, affecting almost exclusively the energy of the CO LUMO. As a result, that correction is significantly stronger for complexes at hollow sites, hence increases the propensity for adsorption at top sites. We also analyze competing edge effects on the (111) facets of the cluster models.
Chemisorption of (CHx and C2Hy) Hydrocarbons on Pt(111) Clusters and Surfaces from DFT Studies
Goddard III, William A.
Chemisorption of (CHx and C2Hy) Hydrocarbons on Pt(111) Clusters and Surfaces from DFT Studies Timo that these hydrocarbons all bind covalently (-bonds) to the surface, in agreement with the studies by Kua and Goddard on small Pt clusters. In nearly every case the structure of the adsorbed hydrocarbon achieves a saturated
Rocca, Jorge J.
Partial Oxidation of Propylene Catalyzed by VO3 Clusters: A Density Functional Theory Study Zhe are carried out to investigate partial oxidation of propylene over neutral VO3 clusters. CdC bond cleavage of propylene with VO3 at room temperature. Formation of hydrogen transfer products H2O + VO2C3H4, CH2d
Paris-Sud XI, Université de
functional theory of f-band metals : lanthanum, cerium and thorium C1 ) D. Glotzel Institut fur cérium et du thorium à l'aide de la méthode « linear muffin tin orbital » (LMTO) et de l'approximation de centered cubic lanthanum, cerium and thorium have been performed using the linear muffin tin orbital (LMTO
Xue, H. T.; Tang, F. L., E-mail: tfl03@mails.tsinghua.edu.cn [State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals, Department of Materials Science and Engineering, Lanzhou University of Technology, Lanzhou 730050 (China); Science and Technology on Surface Engineering Laboratory, Lanzhou Institute of Physics, Lanzhou 730000 (China); Lu, W. J.; Li, X. K.; Zhang, Y. [State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals, Department of Materials Science and Engineering, Lanzhou University of Technology, Lanzhou 730050 (China); Feng, Y. D. [Science and Technology on Surface Engineering Laboratory, Lanzhou Institute of Physics, Lanzhou 730000 (China)
2014-08-07T23:59:59.000Z
The phase diagram of the CuInSe{sub 2}-CuGaSe{sub 2} pseudobinary system was determined using a combination of special quasirandom structure approach, ab initio density functional theory calculations, and thermodynamic modelling. It is shown that the CuIn{sub 1?x}Ga{sub x}Se{sub 2} solution phase has a tendency to phase separation at low temperature. The calculated consolute temperature is 485?K. It is found that both the binodal and spinodal curves are significantly asymmetric and on both curves there are a local maximum and a local minimum, which have not been reported in the previous studies. Our phase diagram can well explain the finding that the inhomogeneity of CuIn{sub 0.25}Ga{sub 0.75}Se{sub 2} is higher than that of CuIn{sub 0.75}Ga{sub 0.25}Se{sub 2} at the same temperature, while the previous phase diagrams cannot. Hence, our phase diagram should be more reliable and applicable.
Liu Li; Martin, Courtney; Farrar, James M. [Department of Chemistry, University of Rochester, Rochester, New York 14627 (United States)
2006-10-07T23:59:59.000Z
The reactions between OH{sup +}({sup 3}{sigma}{sup -}) and C{sub 2}H{sub 2} have been studied using crossed ion and molecular beams and density functional theory calculations. Both charge transfer and proton transfer channels are observed. Products formed by carbon-carbon bond cleavage analogous to those formed in the isoelectronic O({sup 3}P)+C{sub 2}H{sub 2} reaction, e.g., {sup 3}CH{sub 2}+HCO{sup +}, are not observed. The center of mass flux distributions of both product ions at three different energies are highly asymmetric, with maxima close to the velocity and direction of the precursor acetylene beam, characteristic of direct reactions. The internal energy distributions of the charge transfer products are independent of collision energy and are peaked at the reaction exothermicity, inconsistent with either the existence of favorable Franck-Condon factors or energy resonance. In proton transfer, almost the entire reaction exothermicity is transformed into product internal excitation, consistent with mixed energy release in which the proton is transferred with both the breaking and forming bonds extended. Most of the incremental translational energy in the two higher-energy experiments appears in product translational energy, providing an example of induced repulsive energy release.
Minezawa, Noriyuki, E-mail: minezawa@fukui.kyoto-u.ac.jp [Fukui Institute for Fundamental Chemistry, Kyoto University, Sakyo-ku, Kyoto 606-8103 (Japan)
2014-10-28T23:59:59.000Z
Examining photochemical processes in solution requires understanding the solvent effects on the potential energy profiles near conical intersections (CIs). For that purpose, the CI point in solution is determined as the crossing between nonequilibrium free energy surfaces. In this work, the nonequilibrium free energy is described using the combined method of linear-response free energy and collinear spin-flip time-dependent density functional theory. The proposed approach reveals the solvent effects on the CI geometries of stilbene in an acetonitrile solution and those of thymine in water. Polar acetonitrile decreases the energy difference between the twisted minimum and twisted-pyramidalized CI of stilbene. For thymine in water, the hydrogen bond formation stabilizes significantly the CI puckered at the carbonyl carbon atom. The result is consistent with the recent simulation showing that the reaction path via this geometry is open in water. Therefore, the present method is a promising way of identifying the free-energy crossing points that play an essential role in photochemistry of solvated molecules.
Javaid, Saqib [EMMG, Physics Division, PINSTECH, P.O. Nilore, Islamabad (Pakistan); National Centre of Physics, Islamabad (Pakistan); Javed Akhtar, M., E-mail: javedakhtar6@gmail.com [EMMG, Physics Division, PINSTECH, P.O. Nilore, Islamabad (Pakistan)
2014-07-14T23:59:59.000Z
We have investigated the behavior of orthoferrite LaFeO{sub 3} at ambient conditions and under pressure using DFT (generalized gradient approximation (GGA))?+?U approach. Ground state electronic (band gap) and magnetic properties are considerably improved due to the Hubbard correction. Moreover, the experimentally observed pressure-driven phase transition, namely, the simultaneous occurrence of spin crossover, isostructural volume collapse, and drastic reduction in electrical resistance (electronic phase transition) is nicely described by GGA?+?U calculations. In particular, despite a sharp drop in resistance, a small band gap still remains in the low spin state indicating an insulator to semiconductor phase transition, in good agreement with the experiments but in contrast to GGA, which predicts metallic behavior in low spin state. We discuss the origin of variation in electronic structure of LaFeO{sub 3} in low spin state as obtained from GGA to GGA?+?U methods. These results emphasize the importance of correlation effects in describing the pressure-driven phase transition in LaFeO{sub 3} and other rare-earth orthoferrites.
Baer, Marcel D.; Kuo, I-F W.; Tobias, Douglas J.; Mundy, Christopher J.
2014-07-17T23:59:59.000Z
The propensities of the water self ions, H3O+ and OH- , for the air-water interface has implications for interfacial acid-base chemistry. Despite numerous experimental and computational studies, no consensus has been reached on the question of whether or not H3O+ and/or OH- prefer to be at the water surface or in the bulk. Here we report a molecular dynamics simulation study of the bulk vs. interfacial behavior of H3O+ and OH- that employs forces derived from density functional theory with a generalized gradient approximation exchangecorrelation functional (specifically, BLYP) and empirical dispersion corrections. We computed the potential of mean force (PMF) for H3O+ as a function of the position of the ion in a 215-molecule water slab. The PMF is flat, suggesting that H3O+ has equal propensity for the air-water interface and the bulk. We compare the PMF for H3O+ to our previously computed PMF for OH- adsorption, which contains a shallow minimum at the interface, and we explore how differences in solvation of each ion at the interface vs. the bulk are connected with interfacial propensity. We find that the solvation shell of H3O+ is only slightly dependent on its position in the water slab, while OH- partially desolvates as it approaches the interface, and we examine how this difference in solvation behavior is manifested in the electronic structure and chemistry of the two ions. DJT was supported by National Science Foundation grant CHE-0909227. CJM was supported by the U.S. Department of Energy‘s (DOE) Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences. Pacific Northwest National Laboratory (PNNL) is operated for the Department of Energy by Battelle. The potential of mean force required resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DEAC05-00OR22725. The remaining simulations and analysis used resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. at at Lawrence Berkeley National Laboratory. MDB is grateful for the support of the Linus Pauling Distinguished Postdoctoral Fellowship Program at PNNL.
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Al-Hamdani, Yasmine S.; Alfè, Dario; von Lilienfeld, O. Anatole; Michaelides, Angelos
2014-10-22T23:59:59.000Z
Density functional theory (DFT) studies of weakly interacting complexes have recently focused on the importance of van der Waals dispersion forces, whereas the role of exchange has received far less attention. Here, by exploiting the subtle binding between water and a boron and nitrogen doped benzene derivative (1,2-azaborine) we show how exact exchange can alter the binding conformation within a complex. Benchmark values have been calculated for three orientations of the water monomer on 1,2-azaborine from explicitly correlated quantum chemical methods, and we have also used diffusion quantum Monte Carlo. For a host of popular DFT exchange-correlation functionals we showmore »that the lack of exact exchange leads to the wrong lowest energy orientation of water on 1,2-azaborine. As such, we suggest that a high proportion of exact exchange and the associated improvement in the electronic structure could be needed for the accurate prediction of physisorption sites on doped surfaces and in complex organic molecules. Meanwhile to predict correct absolute interaction energies an accurate description of exchange needs to be augmented by dispersion inclusive functionals, and certain non-local van der Waals functionals (optB88- and optB86b-vdW) perform very well for absolute interaction energies. Through a comparison with water on benzene and borazine (B?N?H?) we show that these results could have implications for the interaction of water with doped graphene surfaces, and suggest a possible way of tuning the interaction energy.« less
Al-Hamdani, Yasmine S.; Michaelides, Angelos, E-mail: angelos.michaelides@ucl.ac.uk [Thomas Young Centre and London Centre for Nanotechnology, 17–19 Gordon Street, London WC1H 0AH (United Kingdom); Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ (United Kingdom); Alfè, Dario [Thomas Young Centre and London Centre for Nanotechnology, 17–19 Gordon Street, London WC1H 0AH (United Kingdom); Department of Earth Sciences, University College London, Gower Street, London WC1E 6BT (United Kingdom); Lilienfeld, O. Anatole von [Institute of Physical Chemistry, Department of Chemistry, University of Basel, Klingelbergstrasse 80, CH-4056 Basel (Switzerland); Argonne National Laboratories, 9700 S. Cass Avenue, Lemont, Illinois 60439 (United States)
2014-11-14T23:59:59.000Z
Density functional theory (DFT) studies of weakly interacting complexes have recently focused on the importance of van der Waals dispersion forces, whereas the role of exchange has received far less attention. Here, by exploiting the subtle binding between water and a boron and nitrogen doped benzene derivative (1,2-azaborine) we show how exact exchange can alter the binding conformation within a complex. Benchmark values have been calculated for three orientations of the water monomer on 1,2-azaborine from explicitly correlated quantum chemical methods, and we have also used diffusion quantum Monte Carlo. For a host of popular DFT exchange-correlation functionals we show that the lack of exact exchange leads to the wrong lowest energy orientation of water on 1,2-azaborine. As such, we suggest that a high proportion of exact exchange and the associated improvement in the electronic structure could be needed for the accurate prediction of physisorption sites on doped surfaces and in complex organic molecules. Meanwhile to predict correct absolute interaction energies an accurate description of exchange needs to be augmented by dispersion inclusive functionals, and certain non-local van der Waals functionals (optB88- and optB86b-vdW) perform very well for absolute interaction energies. Through a comparison with water on benzene and borazine (B{sub 3}N{sub 3}H{sub 6}) we show that these results could have implications for the interaction of water with doped graphene surfaces, and suggest a possible way of tuning the interaction energy.
Pisani, Pablo
2015-01-01T23:59:59.000Z
We present a pedagogical exposition of some applications of functional methods in quantum field theory: we use heat-kernel and zeta-function techniques to study the Casimir effect, the pair production in strong electric fields, quantum fields at finite temperature and beta-functions for a self-interacting scalar field, QED and pure Yang-Mills theories. The more recent application to the UV/IR mixing phenomenon in noncommutative theories is also discussed in this framework.
Pablo Pisani
2015-05-16T23:59:59.000Z
We present a pedagogical exposition of some applications of functional methods in quantum field theory: we use heat-kernel and zeta-function techniques to study the Casimir effect, the pair production in strong electric fields, quantum fields at finite temperature and beta-functions for a self-interacting scalar field, QED and pure Yang-Mills theories. The more recent application to the UV/IR mixing phenomenon in noncommutative theories is also discussed in this framework.
Mutombo, P.; Romanyuk, O., E-mail: romanyuk@fzu.cz [Institute of Physics, Academy of Sciences of the Czech Republic, Cukrovarnická 10, 16200 Prague (Czech Republic)
2014-05-28T23:59:59.000Z
The atomic structures of non-polar GaN(101{sup ¯}0),?(112{sup ¯}0) and semipolar GaN(202{sup ¯}1),?(202{sup ¯}1{sup ¯}) surfaces were studied using ab initio calculations within density functional theory. The bulk-like truncated (1?×?1) structure with buckled Ga-N or Ga-Ga dimers was found stable on the non-polar GaN(101{sup ¯}0) surface in agreement with previous works. Ga-N heterodimers were found energetically stable on the GaN(112{sup ¯}0)-(1?×?1) surface. The formation of vacancies and substitution site defects was found unfavorable for non-polar GaN surfaces. Semipolar GaN(202{sup ¯}1)-(1?×?1) surface unit cells consist of non-polar (101{sup ¯}0) and semipolar (101{sup ¯}1) nano-facets. The (101{sup ¯}1) nano-facets consist of two-fold coordinated atoms, which form N-N dimers within a (2?×?1) surface unit cell on a GaN(202{sup ¯}1) surface. Dimers are not formed on the GaN(202{sup ¯}1{sup ¯}) surface. The stability of the surfaces with single (101{sup ¯}0) or (101{sup ¯}1) nano-facets was analyzed. A single non-polar (101{sup ¯}0)-(1?×?1) nano-facet was found stable on the GaN(202{sup ¯}1) surface, but unstable on the GaN(202{sup ¯}1{sup ¯}) surface. A single (101{sup ¯}1) nano-facet was found unstable. Semipolar GaN surfaces with (202{sup ¯}1) and (202{sup ¯}1{sup ¯}) polarity can be stabilized with a Ga overlayer at Ga-rich experimental conditions.
X-ray diffraction, spectroscopic and DFT studies of 1-(4-bromophenyl)-3,5-diphenylformazan
Tezcan, H., E-mail: habibe@gazi.edu.tr [Gazi University, Department of Chemistry, Faculty of Education (Turkey); Tokay, N. [Hacettepe University, Department of Chemistry, Faculty of Science (Turkey); Alpaslan, G. [Giresun University, Department of Medical Services and Techniques, Vocational School of Health Services (Turkey); Erdönmez, A. [Ondokuz May?s University, Department of Physics, Faculty of Science and Art (Turkey)
2013-12-15T23:59:59.000Z
The crystal structure of 1-(4-bromophenyl)-3,5-diphenylformazan was determined by X-ray single crystal diffraction technique. The crystals are orthorhombic, a = 23.0788(9), b = 7.9606(3), c = 18.6340(12) Å, Z = 8, sp. gr. Pbca, R{sub 1} = 0.074. The structure was also examined using the density-functional theory. Its structure stability, and frontier molecular orbital components were discussed and the results were compared with X-ray and spectral results. The maximum absorbtion peaks of the UV-vis spectrum of the compound have been calculated using the time-dependent density-functional theory. It was found a good agreement between the calculated and experimental maximum absorption wavelength.
Interfacial Properties and Design of Functional Energy Materials
Sumpter, Bobby G [ORNL] [ORNL; Liang, Liangbo [ORNL] [ORNL; Nicolai, Adrien [Rensselaer Polytechnic Institute (RPI)] [Rensselaer Polytechnic Institute (RPI); Meunier, V. [Rensselaer Polytechnic Institute (RPI)] [Rensselaer Polytechnic Institute (RPI)
2014-01-01T23:59:59.000Z
The vital importance of energy to society continues to demand a relentless pursuit of energy responsive materials that can bridge fundamental chemical structures at the molecular level and achieve improved functionality, such as efficient energy conversion/storage/transmission, over multiple length scales. This demand can potentially be realized by harnessing the power of self-assembly a spontaneous process where molecules or much larger entities form ordered aggregates as a consequence of predominately non-covalent (weak) interactions. Self-assembly is the key to bottom-up design of molecular devices, because the nearly atomic-level control is very difficult to realize in a top-down, e.g., lithographic approach. However, while function (e.g., charge mobility) in simple systems such as single crystals can often be predicted, predicting the function of the great variety of self-assembled molecular architectures is complicated by the lack of understanding and control over nanoscale interactions, mesoscale architectures, and macroscale (long-range) order. To establish a foundation toward delivering practical solutions, it is critical to develop an understanding of the chemical and physical mechanisms responsible for the self-assembly of molecular and hybrid materials on various substrates. Typically molecular self-assembly involves poorly understood non-covalent intermolecular and substrate-molecule interactions compounded by local and/or collective influences from the substrate atomic lattice (symmetry and/or topological features) and electronic structure. Thus, progress towards unraveling the underlying physicochemical processes that control the structure and macroscopic physical, mechanical, electrical, and transport properties of materials increasingly requires tight integration of theory, modeling and simulation with precision synthesis, advanced experimental characterization, and device measurements. In this mode, theory and simulation can greatly accelerate the process of materials discovery by providing atomic level understanding of physicochemical phenomena and for making predictions of trends. In particular, this approach can provide understanding, prediction and exploration of new materials and conditions before they are realized in the lab, to illuminate connections between experimental observations, and help identify new materials for targeted synthesis. Toward this end, Density Functional Theory (DFT) can provide a suitable computational framework for investigating the inter- and intramolecular bonding, molecular conformation, charge and spin configurations that are intrinsic to self-assembly of molecules on substrates. This Account highlights recent advances in using an integrated approach based on DFT and scanning probe microscopy [STM(s), AFM] to study/develop electronic materials formed from the self-assembly of molecules into supramolecular or polymeric architectures on substrates. Here it is the interplay between molecular interactions and surface electrons that is used to control the final architecture and subsequent bulk properties of the two-dimensional patterns/assemblies. Indeed a rich variety of functional energy materials become possible.
Statistical mechanical theory for steady state systems. VII. Nonlinear theory
Attard, Phil
Statistical mechanical theory for steady state systems. VII. Nonlinear theory Phil Attard School May 2007; published online 2 July 2007 The second entropy theory for nonequilibrium thermodynamics explicitly as a type of the Green-Kubo equilibrium time correlation function. The theory is illustrated
DFT modeling of adsorption onto uranium metal using large-scale parallel computing
Davis, N.; Rizwan, U. [Department of Nuclear, Plasma, and Radiological Engineering, University of Illinois at Urbana-Champaign, Urbana, IL (United States)
2013-07-01T23:59:59.000Z
There is a dearth of atomistic simulations involving the surface chemistry of 7-uranium which is of interest as the key fuel component of a breeder-burner stage in future fuel cycles. Recent availability of high-performance computing hardware and software has rendered extended quantum chemical surface simulations involving actinides feasible. With that motivation, data for bulk and surface 7-phase uranium metal are calculated in the plane-wave pseudopotential density functional theory method. Chemisorption of atomic hydrogen and oxygen on several un-relaxed low-index faces of 7-uranium is considered. The optimal adsorption sites (calculated cohesive energies) on the (100), (110), and (111) faces are found to be the one-coordinated top site (8.8 eV), four-coordinated center site (9.9 eV), and one-coordinated top 1 site (7.9 eV) respectively, for oxygen; and the four-coordinated center site (2.7 eV), four-coordinated center site (3.1 eV), and three-coordinated top2 site (3.2 eV) for hydrogen. (authors)
Screened Hybrid and DFT + U Studies of the Structural, Electronic, and Optical Properties of U3O8
Wen, Xiaodong; Martin, Richard L.; Scuseria, Gustavo E.; Rudin, Sven P.; Batista, Enrique R.; Burrell, Anthony K.
2012-11-26T23:59:59.000Z
A systematic comparison of the structures and electronic and optical properties of U3O8 in the c2mm, P¯62m, and P21/m structures (the ?, ?, and ? phases, respectively) is performed using density functional theory + U (PBE + U) and the Heyd–Scuseria–Ernzerhof screened hybrid functional (HSE). The relationship between the semiconducting C2mm phase of U3O8 and the high temperature, metallic P¯62m phase is explored in more detail. Our calculated results show that the HSE functional gives a better description of the electronic and optical properties when compared with available experimental data for the ? and ? phases, but neither approach does particularly well for the high pressure ? phase.
Efficient Pulse-Doppler Processing and Ambiguity Functions of Nonuniform Coherent Pulse Trains
Nehorai, Arye
Efficient Pulse-Doppler Processing and Ambiguity Functions of Nonuniform Coherent Pulse Trains Lafayette, Indiana 47907 Email: {srasool, mrb}@purdue.edu Abstract--We propose a DFT based pulse Doppler processing receiver for staggered pulse trains. The proposed receiver is a simple extension of traditional
Water and Carbon Dioxide Adsorption at Olivine Surfaces. | EMSL
Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)
and Carbon Dioxide Adsorption at Olivine Surfaces. Water and Carbon Dioxide Adsorption at Olivine Surfaces. Abstract: Plane-wave density functional theory (DFT) calculations were...
The microscopic features of heterogeneous ice nucleation may affect the macroscopic
Alavi, Ali
sciences,17,18 along with the food and transport industries. Whereas experiments aimed at measuring the ice functional theory (DFT) c
Molecular simulations studies of gas adsorption in metal–organic frameworks
Chen, Linjiang
2014-06-30T23:59:59.000Z
Using computational tools ranging from molecular simulations – including both Monte Carlo and molecular dynamics methods – to quantum mechanical (QM) calculations (primarily at density functional theory (DFT) level), ...
Chu, Iek-Heng; Cheng, Hai-Ping
2013-01-01T23:59:59.000Z
We have studied the energetics, electronic structure, optical excitation, and electron relaxation of dinitromethane molecules (CH$_{2}$N$_{2}$O$_{4}$) adsorbed on semiconducting carbon nanotubes (CNTs) of chiral index (n,0) (n=7, 10, 13, 16, 19). Using first-principles density functional theory (DFT) with generalized gradient approximations and van der Waals corrections, we have calculated adsorption energies of dinitropentylpyrene, in which the dinitromethane is linked to the pyrene via an aliphatic chain, on a CNT. A 75.26 kJ/mol binding energy has been found, which explains why such aliphatic chain-pyrene units can be and have been used in experiments to bind functional molecules to CNTs. The calculated electronic structures show that the dinitromethane introduces a localized state inside the band gap of CNT systems of n=10, 13, 16 and 19; such a state can trap an electron when the CNT is photoexcited. We have therefore investigated the dynamics of intra-band relaxations using the reduced density matrix fo...
Theory of nodal s±-wave pairing symmetry in the Pu-based 115 superconductor family
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Das, Tanmoy; Zhu, Jian -Xin; Graf, Matthias J.
2015-02-27T23:59:59.000Z
The spin-fluctuation mechanism of superconductivity usually results in the presence of gapless or nodal quasiparticle states in the excitation spectrum. Nodal quasiparticle states are well established in copper-oxide, and heavy-fermion superconductors, but not in iron-based superconductors. Here, we study the pairing symmetry and mechanism of a new class of plutonium-based high-Tc superconductors and predict the presence of a nodal s?? wave pairing symmetry in this family. Starting from a density-functional theory (DFT) based electronic structure calculation we predict several three-dimensional (3D) Fermi surfaces in this 115 superconductor family. We identify the dominant Fermi surface “hot-spots” in the inter-band scattering channel,more »which are aligned along the wavevector Q = (?, ?, ?), where degeneracy could induce sign-reversal of the pairing symmetry. Our calculation demonstrates that the s?? wave pairing strength is stronger than the previously thought d-wave pairing; and more importantly, this pairing state allows for the existence of nodal quasiparticles. Finally, we predict the shape of the momentum- and energy-dependent magnetic resonance spectrum for the identification of this pairing symmetry.« less
Kim, Inkoo; Lee, Yoon Sup, E-mail: yslee@kaist.edu [Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701 (Korea, Republic of)
2014-10-28T23:59:59.000Z
We report the formulation and implementation of KRCASPT2, a two-component multi-configurational second-order perturbation theory based on Kramers restricted complete active space self-consistent field (KRCASSCF) reference function, in the framework of the spin-orbit relativistic effective core potential. The zeroth-order Hamiltonian is defined as the sum of nondiagonal one-electron operators with generalized two-component Fock matrix elements as scalar factors. The Kramers symmetry within the zeroth-order Hamiltonian is maintained via the use of a state-averaged density, allowing a consistent treatment of degenerate states. The explicit expressions are derived for the matrix elements of the zeroth-order Hamiltonian as well as for the perturbation vector. The use of a fully variational reference function and nondiagonal operators in relativistic multi-configurational perturbation theory is reported for the first time. A series of initial calculations are performed on the ionization potential and excitation energies of the atoms of the 6p-block; the results display a significant improvement over those from KRCASSCF, showing a closer agreement with experimental results. Accurate atomic properties of the superheavy elements of the 7p-block are also presented, and the electronic structures of the low-lying excited states are compared with those of their lighter homologues.
Functionalized Graphene Nanoroads for Quantum Well Device. |...
Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)
Nanoroads for Quantum Well Device. Functionalized Graphene Nanoroads for Quantum Well Device. Abstract: Using density functional theory, a series of calculations of structural and...
Battenfeld, Ingo
2008-01-01T23:59:59.000Z
This thesis presents Topological Domain Theory as a powerful and flexible framework for denotational semantics. Topological Domain Theory models a wide range of type constructions and can interpret many computational features. Furthermore, it has...We begin by describing the categories of Topological Domain Theory, and their categorical structure. In particular, we recover the basic constructions of domain theory, such as products, function spaces, fixed points and recursive types, in the context of Topological Domain Theory....As a central contribution, we give a detailed account of how computational effects can be modelled in Topological Domain Theory. Following recent work of Plotkin and Power, who proposed to construct effect monads via free algebra functors, this is done by showing that free algebras for a large class of parametrised equational theories exist in Topological Domain Theory. These parametrised equational theories are expressive enough to generate most of the standard examples of effect monads. Moreover, the free algebras in Topological Domain Theory are obtained by an explicit inductive construction, using only basic topological and set-theoretical principles....We also give a comparison of Topological and Classical Domain Theory. The category of omega-continuous dcpos embeds into Topological Domain Theory, and we prove that this embedding preserves the basic domain-theoretic constructions in most cases. We show that the classical powerdomain constructions on omega-continuous dcpos, including the probabilistic powerdomain, can be recovered in Topological Domain Theory....Finally, we give a synthetic account of Topological Domain Theory. We show that Topological Domain Theory is a specific model of Synthetic Domain Theory in the realizability topos over Scott's graph model. We give internal characterisations of the categories of Topological Domain Theory in this realizability topos, and prove the corresponding categories to be internally complete and weakly small. This enables us to show that Topological Domain Theory can model the polymorphic lambda-calculus, and to obtain a richer collection of free algebras than those constructed earlier....In summary, this thesis shows that Topological Domain Theory supports a wide range of semantic constructions, including the standard domain-theoretic constructions, computational effects and polymorphism, all within a single setting....
Baik, Mu-Hyun
1,2-CF bond activation of perfluoroarenes and alkylidene isomers of titanium. DFT analysis of the CeF bond activation pathway and rotation of the titanium alkylidene moiety José G. Andino, Hongjun Received in revised form 26 July 2011 Accepted 27 July 2011 Keywords: Alkylidene Titanium CeF bond
Herbert, John
-Functional Description of the 1 La State in Polycyclic Aromatic Hydrocarbons: Charge-Transfer Character in Disguise? Ryan aromatic hydrocarbons (PAHs) includes two singlet excited states that are often denoted 1 La and 1 Lb. Time operator into short- and long-range components.8,15,21À23 While conventional TD-DFT's propensity
Morse Theory One of the most cited
Landweber, Laura
Morse Theory J. Milnor One of the most cited books in mathemat- ics, John Milnor's expo- sition of Morse theory has been the most impor- tant book on the subject for more than forty years. Morse theory for Advanced Study, and Princeton published his Topological Methods in the Theory of Functions of a Complex
Frank Discussion of the Status of Ground-state Orbital-free DFT
Karasiev, Valentin V
2015-01-01T23:59:59.000Z
F.E. Harris has been a significant partner in our work on orbital-free density functional approximations for use in ab initio molecular dynamics. Here we mention briefly the essential progress on single-point functionals since our original paper (2006). Then we focus on the advantages and limitations of generalized gradient approximation (GGA) non-interacting kinetic-energy functionals. We reconsider the constraints provided by near-origin conditions in atomic-like systems and their relationship to regularized versus physical external potentials. Then we seek the best empirical GGA for the non-interacting KE for a modest-sized set of molecules with a well-defined near-origin behavior of their densities. The search is motivated by a desire for insight into GGA limitations and for a target for constraint-based development.
Boolean Theory laws proof Number Theory Character Theory
Hehner, Eric C.R.
Review Boolean Theory laws proof Number Theory Character Theory Bunches Sets Strings Lists for loop 1/109 #12;Review Boolean Theory laws proof Number Theory Character Theory Bunches Sets Strings with exit for loop 2/109 #12;Review Boolean Theory laws proof Number Theory Character Theory Bunches Sets
Oeiras, R. Y.; Silva, E. Z. da [Institute of Physics “Gleb Wataghin”, University of Campinas-Unicamp, 13083-859 Campinas, SP (Brazil)] [Institute of Physics “Gleb Wataghin”, University of Campinas-Unicamp, 13083-859 Campinas, SP (Brazil)
2014-04-07T23:59:59.000Z
Carbon linear atomic chains attached to graphene have experimentally been produced. Motivated by these results, we study the nature of the carbon bonds in these nanowires and how it affects their electrical properties. In the present study we investigate chains with different numbers of atoms and we observe that nanowires with odd number of atoms present a distinct behavior than the ones with even numbers. Using graphene nanoribbons as leads, we identify differences in the quantum transport of the chains with the consequence that even and odd numbered chains have low and high electrical conduction, respectively. We also noted a dependence of current with the wire size. We study this unexpected behavior using a combination of first principles calculations and simple models based on chemical bond theory. From our studies, the electrons of carbon nanowires present a quasi-free electron behavior and this explains qualitatively the high electrical conduction and the bond lengths with unexpected values for the case of odd nanowires. Our study also allows the understanding of the electric conduction dependence with the number of atoms and their parity in the chain. In the case of odd number chains a proposed ?-bond (MpB) model describes unsaturated carbons that introduce a mobile ?-bond that changes dramatically the structure and transport properties of these wires. Our results indicate that the nature of bonds plays the main role in the oscillation of quantum electrical conduction for chains with even and odd number of atoms and also that nanowires bonded to graphene nanoribbons behave as a quasi-free electron system, suggesting that this behavior is general and it could also remain if the chains are bonded to other materials.
Vo, Trinh; Allmen, Paul von; Huang, Chen-Kuo; Ma, James; Bux, Sabah; Fleurial, Jean-Pierre [Jet Propulsion Laboratory, California Institute of Technology, Pasadena, California 91109 (United States)
2014-10-07T23:59:59.000Z
The electronic properties and Seebeck coefficients of Ce{sub 3}Te{sub 4} and La{sub 3}Te{sub 4} are computed using Density Functional Theory with on-site Coulomb interaction correction. We found that the Seebeck coefficients of Ce{sub 3}Te{sub 4} and La{sub 3}Te{sub 4} are almost equal at temperatures larger than the Curie temperature of Ce{sub 3}Te{sub 4}, and in good agreement with the measurements reported by May et al. [Phys. Rev. B 86, 035135 (2012)]. At temperatures below the Curie temperature, the Seebeck coefficient of Ce{sub 3}Te{sub 4} increases due to the ferromagnetic ordering, which leads the f-electron of Ce to contribute to the Seebeck coefficient in the relevant range of electron concentration.
Discontinuous Lyapunov Functions for Nonasymptotic Stability Analysis
Paris-Sud XI, Université de
Discontinuous Lyapunov Functions for Nonasymptotic Stability Analysis A. Polyakov Inria Lille of discontinuous control systems using discontinuous Lyapunov functions. Elements of Filippov theory of generalized derivatives and non-smooth Lyapunov functions are considered. The generalized Lyapunov theorems
Boolean Theory laws proof Number Theory Character Theory
Hehner, Eric C.R.
construction induction Recursive Program Definition construction induction Theory Design and Implementation Definition construction induction Theory Design and Implementation data theory program theory Data Recursive Data Definition construction induction Recursive Program Definition construction induction Theory
DFT+U Study of CeO2 and Its Native Defects
Huang, Bolong; Gillen, Roland; Robertson, John
2014-10-14T23:59:59.000Z
in solid state fuel cells2, as a catalyst3-6, as a high-dielectric constant gate oxide7, and in resistance random access memories (ReRAM)8. Many properties of CeO2 are determined by its intrinsic defects9-23 and the unusual behavior of the semi-core Ce 4f... averaging scheme46 for spin- orbital coupling effect. The RRKJ method is chosen as optimization of pseudopotentials47. The PBE functional was chosen for PBE+U calculations with a kinetic cutoff energy of 750eV, which expands the valence electrons states...
DFT+U Study of Polaronic Conduction in Li2O2 and Li2CO3: Implications for Li-Air Batteries
Thygesen, Kristian
DFT+U Study of Polaronic Conduction in Li2O2 and Li2CO3: Implications for Li-Air Batteries J. M-air batteries are known to be Li2O2 and residual Li2CO3. Recent experiments indicate that the charge transport through these materials is the main limiting factor for the battery performance. It has been also shown
Makrlik, Emanuel [Czech University of Life Sciences, Prague, Kamy´cká; Toman, Petr [Institute of Macromolecular Chemistry, Prague; Vanura, Petr [Institute of Chemical Technology, Prague, Czech Republic; Moyer, Bruce A [ORNL
2013-01-01T23:59:59.000Z
From extraction experiments and c-activity measurements, the extraction constant corresponding to the equilibrium Cs+ (aq) + I (aq) + 1 (org),1Cs+ (org) + I (org) taking place in the two-phase water-phenyltrifluoromethyl sulfone (abbrev. FS 13) system (1 = calix[4]arene-bis(t-octylbenzo-18-crown-6); aq = aqueous phase, org = FS 13 phase) was evaluated as logKex (1Cs+, I) = 2.1 0.1. Further, the stability constant of the 1Cs+ complex in FS 13 saturated with water was calculated for a temperature of 25 C: log borg (1Cs+) = 9.9 0.1. Finally, by using quantum mechanical DFT calculations, the most probable structure of the cationic complex species 1Cs+ was derived. In the resulting 1Cs+ complex, the central cation Cs+ is bound by eight bond interactions to six oxygen atoms of the respective 18-crown-6 moiety and to two carbons of the corresponding two benzene rings of the parent ligand 1 via cation p interaction.
2015-03-12T23:59:59.000Z
Cellar theory. A. Eremenko. March 12, 2015. The temperature on the Earth surface at a given place experiences roughly speaking periodic fluctuation, daily and ...
Quantum theory Bohrification: topos theory and quantum theory
Spitters, Bas
Quantum theory Bohrification: topos theory and quantum theory Bas Spitters Domains XI, 9/9/2014 Bas Spitters Bohrification: topos theory and quantum theory #12;Quantum theory Point-free Topology The axiom, Krein-Millman, Alaoglu, Hahn-Banach, Gelfand, Zariski, ... Bas Spitters Bohrification: topos theory
Computational Benchmarking in Biomimetic Nickel, Copper, and Iron Complexes
Brothers, Scott Michael
2012-02-14T23:59:59.000Z
that might define catalytic efficiency of enzymes can be addressed by theory. Density functional theory, or DFT, has been developed as an in silico tool to complement and interpret crystallographic and spectroscopic results or to make predictions...
Walsh, Timothy Francis; Reese, Garth M.; Bhardwaj, Manoj Kumar
2004-08-01T23:59:59.000Z
This manual describes the theory behind many of the constructs in Salinas. For a more detailed description of how to use Salinas , we refer the reader to Salinas, User's Notes. Many of the constructs in Salinas are pulled directly from published material. Where possible, these materials are referenced herein. However, certain functions in Salinas are specific to our implementation. We try to be far more complete in those areas. The theory manual was developed from several sources including general notes, a programer-notes manual, the user's notes and of course the material in the open literature.
Green functions and Macdonald functions associated to complex reflection groups
Shoj, Toshiaki
Green functions and Macdonald functions associated to complex reflection groups Toshiaki Shoji Department of Mathematics Science University of Tokyo Noda, Chiba 2788510, Japan 1. Introduction 1.1. Green functions are introduced by J.A. Green [G] in 1955, in connection with the representation theory of general
Theory and applications of Bessel functions
Wasson, William Albert
1949-01-01T23:59:59.000Z
negat1ve integer. Then equations (1-2) are equivalent to d=& ~ C=(. '=C~= . -=o, I 3 C, = ? C, ? art(&u+~V c ? 0" c. &si g~(yt. K)('C+W ~) "Cu+i) C () C'. I Cv+') (IC=], 2, 3, " ~~* K! I (v+ tc+i) Thus a formal solut1on of Bessel's equation 1...s y=y C?X' = P ("?X"' K p'f AA' ( ? I) Q / cv+)w (xI (~q . . . ) K! p(v+z~i) wh1ch takes a simpler form if we further choose the arb1, trary I C to be Then we have the particular formal / (u+i) ~ solution P tLK Z (x/=Z /xX h-3 K! / P+K I...
Theory and applications of Bessel functions
Wasson, William Albert
1949-01-01T23:59:59.000Z
fferential operator VV dA~ + X ~X +( v')' Ant1cipating termwise =x dif f erent1abili ty, QK (&+ k) X K=o (?(+&~) (w+w-i) x K=o K=o p (p (y+g)(d+w-i) X y (?(ate) y K=o o(+K+ Q. ~+wE qQ?X g?v x V~QL?X = g (e ? u )x + L p(d+i) ? A/X q Q (g. L(&+ ?J... ? v j + 6?) 8' This will vanish 1dentically if and only if C. (& -~') I(~pl) p 9 = 0 g gs(~q P jy( = O (g=. . . ' ) These equations are satisfied in particular if d=& ) (l 2) C, = O) (', (av+K) K ~ (" = 0 (v=&, &, + Now assume that V ia not a...
Density-Functional Theory for Complex Fluids
Wu, Jianzhong
. This generic methodology is built upon a mathematical theorem that states, for an equilibrium system at a given modeling of the microscopic struc- tures and phase behavior of soft-condensed matter. The methodol- ogy to the one-body density profile Grand potential: the free energy of an open system at fixed volume
Density functional theory study of acetaldehyde hydrodeoxygenation...
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hydroxyls, which can recombine into a water molecule weakly bound at the Mo site. A terminal oxygen (Ot) defect site thus forms after water desorption. CH3CHO adsorbs at the...
Functional Keldysh theory of spin torques
Duine, R. A.; Nunez, A. S.; Sinova, Jairo; MacDonald, A. H.
2007-01-01T23:59:59.000Z
that to first order in the applied electric field, the usual form of thermal fluctuations via a phenomenological stochastic magnetic field holds. DOI: 10.1103/PhysRevB.75.214420 PACS number#1;s#2;: 72.25.Pn, 72.15.Gd I. INTRODUCTION Phenomena related... is the effective field and #1; the Gilbert damping constant. The co- efficients #1; and #2; are dissipative in the sense that they relate quantities that are even under time reversal to quantities that are odd under time reversal.30,31 The observation that both...
Hilbert Spaces of Entire Functions
squares of entire functions on the whole reai axis to mean squares on a. Sequence of real ... transformation admits an integral representation in terms of its invariant ... theory of special functions, a subject which is very oid in relation to most of modern ... The book presumes a knowledge of Hilbert space and analytic function.
Quantum Field Theory and Representation Theory
Woit, Peter
Quantum Field Theory and Representation Theory Peter Woit woit@math.columbia.edu Department of Mathematics Columbia University Quantum Field Theory and Representation Theory p.1 #12;Outline of the talk · Quantum Mechanics and Representation Theory: Some History Quantum Field Theory and Representation Theory
Smooth Field Theories and Homotopy Field Theories
Wilder, Alan Cameron
2011-01-01T23:59:59.000Z
1 . . . . . . . . 4 Categories of Field Theories 4.1 Functorto super symmetric field theories. CRM Proceedings and0-dimensional super symmetric field theories. preprint 2008.
On Conformal Field Theory and Number Theory
Huang, An
2011-01-01T23:59:59.000Z
Frontiers in Number Theory, Physics, and Ge- ometry II. (Witten, Quantum Field Theory, Crassmannians, and AlgebraicJ. Polchinski, String Theory, Vol. 1, Cambridge Univ.
Covariant Hamiltonian Field Theory
Jürgen Struckmeier; Andreas Redelbach
2012-05-22T23:59:59.000Z
A consistent, local coordinate formulation of covariant Hamiltonian field theory is presented. Whereas the covariant canonical field equations are equivalent to the Euler-Lagrange field equations, the covariant canonical transformation theory offers more general means for defining mappings that preserve the form of the field equations than the usual Lagrangian description. It is proved that Poisson brackets, Lagrange brackets, and canonical 2-forms exist that are invariant under canonical transformations of the fields. The technique to derive transformation rules for the fields from generating functions is demonstrated by means of various examples. In particular, it is shown that the infinitesimal canonical transformation furnishes the most general form of Noether's theorem. We furthermore specify the generating function of an infinitesimal space-time step that conforms to the field equations.
Bevir, Mark
2013-01-01T23:59:59.000Z
Marsh, eds. , The State: Theory and Issues. Basingstoke, UK:Passion,” Administra- tive Theory & Praxis 18 (1996), 97–?Public Administration Theory,” Administrative Theory &
Arithmetical Functions : Infinite Products
Garimella Rama Murthy
2012-11-26T23:59:59.000Z
In this technical report, certain interesting classification of arithmetical functions is proposed. The notion of additively decomposable and multiplicatively decomposable arithmetical functions is proposed. The concepts of arithmetical polynomials and arithmetical power series are introduced. Using these concepts, an interesting Theorem relating arithmetical power series and infinite products has been proved. Also arithmetical polynomials are related to probabilistic number theory. Furthermore some results related to the Waring problem are discussed.
Mathematical quantization of Hamiltonian field theories
A. V. Stoyanovsky
2015-02-04T23:59:59.000Z
We define the renormalized evolution operator of the Schr\\"odinger equation in the infinite dimensional Weyl-Moyal algebra during a time interval for a wide class of Hamiltonians depending on time. This leads to a mathematical definition of quantum field theory $S$-matrix and Green functions. We show that for renormalizable field theories, our theory yields the renormalized perturbation series of perturbative quantum field theory. All the results are based on the Feynman graph series technique.
Classical Theorems in Noncommutative Quantum Field Theory
M. Chaichian; M. Mnatsakanova; A. Tureanu; Yu. Vernov
2006-12-12T23:59:59.000Z
Classical results of the axiomatic quantum field theory - Reeh and Schlieder's theorems, irreducibility of the set of field operators and generalized Haag's theorem are proven in SO(1,1) invariant quantum field theory, of which an important example is noncommutative quantum field theory. In SO(1,3) invariant theory new consequences of generalized Haag's theorem are obtained. It has been proven that the equality of four-point Wightman functions in two theories leads to the equality of elastic scattering amplitudes and thus the total cross-sections in these theories.
Riemann zeta function and quantum chaos
Eugene Bogomolny
2007-08-30T23:59:59.000Z
A brief review of recent developments in the theory of the Riemann zeta function inspired by ideas and methods of quantum chaos is given.
Theta-functions on noncommutative tori
Albert Schwarz
2001-07-25T23:59:59.000Z
Ordinary theta-functions can be considered as holomorphic sections of line bundles over tori. We show that one can define generalized theta-functions as holomorphic elements of projective modules over noncommutative tori (theta-vectors). The theory of these new objects is not only more general, but also much simpler than the theory of ordinary theta-functions. It seems that the theory of theta-vectors should be closely related to Manin's theory of quantized theta-functions, but we don't analyze this relation.
Building a Universal Nuclear Energy Density Functional
Bertulani, Carlos A. [Texas A& M Univ., Commerce, TX (United States)
2014-09-10T23:59:59.000Z
This grant had two components: Density functional theory and pairing and Nuclear reactions. This final report summarizes the activities for this SciDAC-2 project.
Holographic Quenches and Fermionic Spectral Functions
N. Callebaut; B. Craps; F. Galli; D. C. Thompson; J. Vanhoof; J. Zaanen; Hongbao Zhang
2014-11-04T23:59:59.000Z
Using holographic methods we investigate the behaviour of fermionic spectral functions of strongly coupled 2+1 dimensional field theories as both temperature and chemical potential are quenched.
A New Glauber Theory based on Multiple Scattering Theory
Masanobu Yahiro; Kosho Minomo; Kazuyuki Ogata; Mitsuji Kawai
2008-09-26T23:59:59.000Z
Glauber theory for nucleus-nucleus scattering at high incident energies is reformulated so as to become applicable also for the scattering at intermediate energies. We test validity of the eikonal and adiabatic approximations used in the formulation, and discuss the relation between the present theory and the conventional Glauber calculations with either the empirical nucleon-nucleon profile function or the modified one including the in-medium effect.
ORAL QUAL SYLLABUS: SET THEORY; ERGODIC THEORY
ORAL QUAL SYLLABUS: SET THEORY; ERGODIC THEORY SAMUEL COSKEY Set Theory. #15; Basic set theory's theorem { there exists an Aronsajn tree { Shanin's root system lemma (#2;2) #15; Descriptive set theory of set theory (Jech 12,13) { Mostowski's collapsing theorem { relativization and absolute formulas { re
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the Fock matrix is constructed and then diagonalized. To build the Fock matrix, Fast Fourier Transforms are used to tranform orbitals from the plane wave basis ( where the...
David J. Gross; Washington Taylor
2001-06-27T23:59:59.000Z
We describe the ghost sector of cubic string field theory in terms of degrees of freedom on the two halves of a split string. In particular, we represent a class of pure ghost BRST operators as operators on the space of half-string functionals. These BRST operators were postulated by Rastelli, Sen, and Zwiebach to give a description of cubic string field theory in the closed string vacuum arising from condensation of a D25-brane in the original tachyonic theory. We find a class of solutions for the ghost equations of motion using the pure ghost BRST operators. We find a vanishing action for these solutions, and discuss possible interpretations of this result. The form of the solutions we find in the pure ghost theory suggests an analogous class of solutions in the original theory on the D25-brane with BRST operator Q_B coupling the matter and ghost sectors.
Quantum Field Theory of Fluids
Ben Gripaios; Dave Sutherland
2015-04-23T23:59:59.000Z
The quantum theory of fields is largely based on studying perturbations around non-interacting, or free, field theories, which correspond to a collection of quantum-mechanical harmonic oscillators. The quantum theory of an ordinary fluid is `freer', in the sense that the non-interacting theory also contains an infinite collection of quantum-mechanical free particles, corresponding to vortex modes. By computing a variety of correlation functions at tree- and loop-level, we give evidence that a quantum perfect fluid can be consistently formulated as a low-energy, effective field theory. We speculate that the quantum behaviour is radically different to both classical fluids and quantum fields, with interesting physical consequences for fluids in the low temperature regime.
Yuhua Duan
2012-01-01T23:59:59.000Z
Alkali metal zirconates could be used as solid sorbents for CO{sub 2} capture. The structural, electronic, and phonon properties of Na{sub 2}ZrO{sub 3}, K{sub 2}ZrO{sub 3}, Na{sub 2}CO{sub 3}, and K{sub 2}CO{sub 3} are investigated by combining the density functional theory with lattice phonon dynamics. The thermodynamics of CO{sub 2} absorption/desorption reactions of these two zirconates are analyzed. The calculated results show that their optimized structures are in a good agreement with experimental measurements. The calculated band gaps are 4.339 eV (indirect), 3.641 eV (direct), 3.935 eV (indirect), and 3.697 eV (direct) for Na{sub 2}ZrO{sub 3}, K{sub 2}ZrO{sub 3}, Na{sub 2}CO{sub 3}, and K{sub 2}CO{sub 3}, respectively.The calculated phonon dispersions and phonon density of states for M{sub 2}ZrO{sub 3} and M{sub 2}CO{sub 3} (M = K, Na, Li) revealed that from K to Na to Li, their frequency peaks are shifted to high frequencies due to the molecular weight decreased from K to Li. From the calculated reaction heats and relationships of free energy change versus temperatures and CO{sub 2} pressures of the M{sub 2}ZrO{sub 3} (M = K, Na, Li) reacting with CO{sub 2}, we found that the performance of Na{sub 2}ZrO{sub 3} capturing CO{sub 2} is similar to that of Li{sub 2}ZrO{sub 3} and is better than that of K{sub 2}ZrO{sub 3}. Therefore, Na{sub 2}ZrO{sub 3} and Li{sub 2}ZrO{sub 3} are good candidates of high temperature CO{sub 2} sorbents and could be used for post combustion CO{sub 2} capture technologies.
Mathematical niche theory Mathematical niche theory
Meszéna, Géza
Mathematical niche theory Mathematical niche theory G´eza Mesz´ena1 Gy¨orgy Barab´as2 KalleUniversity of Turku MMEE 2011, Groningen #12;Mathematical niche theory Outline 1 Introduction 2 Core theory 3 Ways of niche segragation 4 Controversies #12;Mathematical niche theory Introduction Why are there so
Quiver gauge theories and integrable lattice models
Junya Yagi
2015-06-30T23:59:59.000Z
We discuss connections between certain classes of supersymmetric quiver gauge theories and integrable lattice models from the point of view of topological quantum field theories (TQFTs). The relevant classes include 4d $\\mathcal{N} = 1$ theories known as brane box and brane tilling models, 3d $\\mathcal{N} = 2$ and 2d $\\mathcal{N} = (2,2)$ theories obtained from them by compactification, and 2d $\\mathcal{N} = (0,2)$ theories closely related to these theories. We argue that their supersymmetric indices carry structures of TQFTs equipped with line operators, and as a consequence, are equal to the partition functions of lattice models. The integrability of these models follows from the existence of extra dimension in the TQFTs, which emerges after the theories are embedded in M-theory. The Yang-Baxter equation expresses the invariance of supersymmetric indices under Seiberg duality and its lower-dimensional analogs.
Instanton Effects in Orbifold ABJM Theory
Masazumi Honda; Sanefumi Moriyama
2014-06-28T23:59:59.000Z
We study the partition function of the orbifold ABJM theory on $S^3$, which is the $\\mathcal{N}=4$ necklace quiver Chern-Simons-matter theory with alternating levels, in the Fermi gas formalism. We find that the grand potential of the orbifold ABJM theory is expressed explicitly in terms of that of the ABJM theory. As shown previously, the ABJM grand potential consists of the naive but primary non-oscillatory term and the subsidiary infinitely-replicated oscillatory terms. We find that the subsidiary oscillatory terms of the ABJM theory actually give a non-oscillatory primary term of the orbifold ABJM theory. Also, interestingly, the perturbative part in the ABJM theory results in a novel instanton contribution in the orbifold theory. We also present a physical interpretation for the non-perturbative instanton effects.
Walsh, Timothy Francis; Reese, Garth M.; Bhardwaj, Manoj Kumar
2011-11-01T23:59:59.000Z
Salinas provides a massively parallel implementation of structural dynamics finite element analysis, required for high fidelity, validated models used in modal, vibration, static and shock analysis of structural systems. This manual describes the theory behind many of the constructs in Salinas. For a more detailed description of how to use Salinas, we refer the reader to Salinas, User's Notes. Many of the constructs in Salinas are pulled directly from published material. Where possible, these materials are referenced herein. However, certain functions in Salinas are specific to our implementation. We try to be far more complete in those areas. The theory manual was developed from several sources including general notes, a programmer notes manual, the user's notes and of course the material in the open literature.
Physics 221B: Solution to HW # 8 Quantum Field Theory
Murayama, Hitoshi
Physics 221B: Solution to HW # 8 Quantum Field Theory 1) Bosonic Grand-Partition Function The solution to this problem is outlined clearly in the beginning of the lecture notes `Quantum Field Theory II
A Naturally Renormalized Quantum Field Theory
S. Rouhani; M. V. Takook
2006-07-07T23:59:59.000Z
It was shown that quantum metric fluctuations smear out the singularities of Green's functions on the light cone [1], but it does not remove other ultraviolet divergences of quantum field theory. We have proved that the quantum field theory in Krein space, {\\it i.e.} indefinite metric quantization, removes all divergences of quantum field theory with exception of the light cone singularity [2,3]. In this paper, it is discussed that the combination of quantum field theory in Krein space together with consideration of quantum metric fluctuations, results in quantum field theory without any divergences.
Conjugate flow action functionals
Venturi, Daniele, E-mail: daniele-venturi@brown.edu [Division of Applied Mathematics, Brown University, Rhode Island 02912 (United States)] [Division of Applied Mathematics, Brown University, Rhode Island 02912 (United States)
2013-11-15T23:59:59.000Z
We present a new general framework to construct an action functional for a non-potential field theory. The key idea relies on representing the governing equations relative to a diffeomorphic flow of curvilinear coordinates which is assumed to be functionally dependent on the solution field. Such flow, which will be called the conjugate flow, evolves in space and time similarly to a physical fluid flow of classical mechanics and it can be selected in order to symmetrize the Gâteaux derivative of the field equations with respect to suitable local bilinear forms. This is equivalent to requiring that the governing equations of the field theory can be derived from a principle of stationary action on a Lie group manifold. By using a general operator framework, we obtain the determining equations of such manifold and the corresponding conjugate flow action functional. In particular, we study scalar and vector field theories governed by second-order nonlinear partial differential equations. The identification of transformation groups leaving the conjugate flow action functional invariant could lead to the discovery of new conservation laws in fluid dynamics and other disciplines.
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Theory and Software Home People Science Highlights Publications Seminars & Meetings Opportunities Advisory Committee Theory and Software Group (X-ray Science Division) The Theory...
Bevir, Mark
2013-01-01T23:59:59.000Z
Management and Organization Theory: From Panopticon toand covering both organization theory and changing patternsTrust in Organizations: Frontiers of Theory and Research (
Smooth Field Theories and Homotopy Field Theories
Wilder, Alan Cameron
2011-01-01T23:59:59.000Z
CHAPTER 3. FIELD THEORIES Definition 3.2.1. A smooth fielda ’top down’ definition of field theories. Taking as ourin the following. Definition A field theory is a symmetric
Thomson, James D.
allocation theory is that an organism's reproductive success, through either male or female function, can in that function. The shapes of these curves determine what patterns of resource allocation can be evolutionarily and female function. Sex allocation theory matured rapidly through the efforts of Charnov 55(1979, 1982
De Branges spaces and Krein's theory of entire operators
Luis O. Silva; Julio H. Toloza
2015-06-23T23:59:59.000Z
This work presents a contemporary treatment of Krein's entire operators with deficiency indices $(1,1)$ and de Branges' Hilbert spaces of entire functions. Each of these theories played a central role in the research of both renown mathematicians. Remarkably, entire operators and de Branges spaces are intimately connected and the interplay between them has had an impact in both spectral theory and the theory of functions. This work exhibits the interrelation between Krein's and de Branges' theories by means of a functional model and discusses recent developments, giving illustrations of the main objects and applications to the spectral theory of difference and differential operators.
Computer Stochastics in Scalar Quantum Field Theory
C. B. Lang
1993-12-01T23:59:59.000Z
This is a series of lectures on Monte Carlo results on the non-perturbative, lattice formulation approach to quantum field theory. Emphasis is put on 4D scalar quantum field theory. I discuss real space renormalization group, fixed point properties and logarithmic corrections, partition function zeroes, the triviality bound on the Higgs mass, finite size effects, Goldstone bosons and chiral perturbation theory, and the determination of scattering phase shifts for some scalar models.
Control of a highly flexible rotating beam: theory and experiments
Chang, Pei-Ming
1990-01-01T23:59:59.000Z
state of art control methodologies that include (i) classical proportional plus derivative (PD) control (ii) Linear Quadratic Regulator (LQR) (iii) servomechanism theory (iv) Lyapunov theory and (v) quantitative feedback theory (QFT), (3... Functions CHAPTER III . CONTROL THEORY 6 7 7 10 15 16 17 25 27 3. 1 Collocated PD Control 3. 2 Linear State Feedback Control 3. 3 Robust Servo-Mechanism Theory 3. 4 Robust Control Synthesized by Lyapunov's Second Method 3. 5 Quantitative...
Modified Fourier expansions: theory, construction and applications
Adcock, Ben
2010-10-12T23:59:59.000Z
Modified Fourier expansions present an alternative to more standard algorithms for the approximation of nonperiodic functions in bounded domains. This thesis addresses the theory of such expansions, their effective construction and computation...
Pizza into Java: Translating theory into practice
Wadler, Philip
Pizza into Java: Translating theory, Pizza is a strict superset of Java that incorporatesothreehigher-order function* *s, and ideas from.algebraic data types. Pizza is defined by translation into Java andPcompilesiintozza attempts to make
A Count of Classical Field Theory Graphs
Gordon Chalmers
2005-07-28T23:59:59.000Z
A generating function is derived that counts the number of diagrams in an arbitrary scalar field theory. The number of graphs containing any number $n_j$ of $j$-point vertices is given. The count is also used to obtain the number of classical graphs in gauge theory and gravity.
Effective Field Theory for Top Quark Physics
Cen Zhang; Scott Willenbrock
2010-08-18T23:59:59.000Z
Physics beyond the standard model can affect top-quark physics indirectly. We describe the effective field theory approach to describing such physics, and contrast it with the vertex-function approach that has been pursued previously. We argue that the effective field theory approach has many fundamental advantages and is also simpler.
Exciton/Charge-transfer Electronic Couplings in Organic Semiconductors
Difley, Seth
Charge transfer (CT) states and excitons are important in energy conversion processes that occur in organic light emitting devices (OLEDS) and organic solar cells. An ab initio density functional theory (DFT) method for ...
Orondo, Peter Omondi
2012-01-01T23:59:59.000Z
We provide a first principles analysis of the physics and thermodynamics of interstitial hydrogen in metal. By utilizing recent advances in Density Functional Theory (DFT) to get state energies of the metal-hydrogen system, ...
A Polarizable QM/MM Explicit Solvent Model for Computational Electrochemistry in Water
Wang, Lee-Ping
We present a quantum mechanical/molecular mechanical (QM/MM) explicit solvent model for the computation of standard reduction potentials E[subscript 0]. The QM/MM model uses density functional theory (DFT) to model the ...
CO[subscript 2] hydrogenation to formic acid on Ni(111)
Peng, Guowen
Periodic, self-consistent, density functional theory (DFT) calculations are employed to study CO[subscript 2] hydrogenation on Ni(111). CO[subscript 2] hydrogenation with H adsorbed on the surface and with H absorbed in ...
Understanding mechanisms for C-H bond activation
Vastine, Benjamin Alan
2009-05-15T23:59:59.000Z
The results from density functional theory (DFT) studies into C–H bond activation, hydrogen transfer, and alkyne–to–vinylidene isomerization are presented in this work. The reaction mechanism for the reductive elimination ...
Forbus, Kenneth D.
- tem called CARNOT that explains steady-flow thermodynamic cycles ranging in complexity from four to 24 of thermodynamic cycles. We have implemented this theory in a system called CARNOT that takes as input a schematic of the more interesting results from other cycles CARNOT currently solves. We conclude with a dis- cussion
Equivalence Relations in Set Theory, Computation Theory and Complexity Theory
Equivalence Relations in Set Theory, Computation Theory and Complexity Theory Denable Equivalence-preserving transformations Unitary equivalence of unitary operators Conformal equivalence of Riemann surfaces These are analytic (1 1 with parameters) equivalence relations on Polish spaces (think of the reals) #12;Equivalence
Giannozzi, Paolo
, in the case of dye-sensitized solar cells (DSSC),2 the D - A system is rep- resented by a D organic dye competitive with thin- film inorganic solar cells. However, large-scale applications still suffer of a low processes at the core of the solar cell functioning:13 (i) optical absorption induced by solar light
E. Minguzzi
2009-09-04T23:59:59.000Z
Every time function on spacetime gives a (continuous) total preordering of the spacetime events which respects the notion of causal precedence. The problem of the existence of a (semi-)time function on spacetime and the problem of recovering the causal structure starting from the set of time functions are studied. It is pointed out that these problems have an analog in the field of microeconomics known as utility theory. In a chronological spacetime the semi-time functions correspond to the utilities for the chronological relation, while in a K-causal (stably causal) spacetime the time functions correspond to the utilities for the K^+ relation (Seifert's relation). By exploiting this analogy, we are able to import some mathematical results, most notably Peleg's and Levin's theorems, to the spacetime framework. As a consequence, we prove that a K-causal (i.e. stably causal) spacetime admits a time function and that the time or temporal functions can be used to recover the K^+ (or Seifert) relation which indeed turns out to be the intersection of the time or temporal orderings. This result tells us in which circumstances it is possible to recover the chronological or causal relation starting from the set of time or temporal functions allowed by the spacetime. Moreover, it is proved that a chronological spacetime in which the closure of the causal relation is transitive (for instance a reflective spacetime) admits a semi-time function. Along the way a new proof avoiding smoothing techniques is given that the existence of a time function implies stable causality, and a new short proof of the equivalence between K-causality and stable causality is given which takes advantage of Levin's theorem and smoothing techniques.
Effective Hamiltonian Constraint from Group Field Theory
Etera R. Livine; Daniele Oriti; James P. Ryan
2011-04-28T23:59:59.000Z
Spinfoam models provide a covariant formulation of the dynamics of loop quantum gravity. They are non-perturbatively defined in the group field theory (GFT) framework: the GFT partition function defines the sum of spinfoam transition amplitudes over all possible (discretized) geometries and topologies. The issue remains, however, of explicitly relating the specific form of the group field theory action and the canonical Hamiltonian constraint. Here, we suggest an avenue for addressing this issue. Our strategy is to expand group field theories around non-trivial classical solutions and to interpret the induced quadratic kinematical term as defining a Hamiltonian constraint on the group field and thus on spin network wave functions. We apply our procedure to Boulatov group field theory for 3d Riemannian gravity. Finally, we discuss the relevance of understanding the spectrum of this Hamiltonian operator for the renormalization of group field theories.
Random wave functions and percolation
E. Bogomolny; C. Schmit
2007-08-31T23:59:59.000Z
Recently it was conjectured that nodal domains of random wave functions are adequately described by critical percolation theory. In this paper we strengthen this conjecture in two respects. First, we show that, though wave function correlations decay slowly, a careful use of Harris' criterion confirms that these correlations are unessential and nodal domains of random wave functions belong to the same universality class as non critical percolation. Second, we argue that level domains of random wave functions are described by the non-critical percolation model.
Group field theories generating polyhedral complexes
Johannes Thürigen
2015-06-28T23:59:59.000Z
Group field theories are a generalization of matrix models which provide both a second quantized reformulation of loop quantum gravity as well as generating functions for spin foam models. While states in canonical loop quantum gravity, in the traditional continuum setting, are based on graphs with vertices of arbitrary valence, group field theories have been defined so far in a simplicial setting such that states have support only on graphs of fixed valency. This has led to the question whether group field theory can indeed cover the whole state space of loop quantum gravity. In this contribution based on [1] I present two new classes of group field theories which satisfy this objective: i) a straightforward, but rather formal generalization to multiple fields, one for each valency and ii) a simplicial group field theory which effectively covers the larger state space through a dual weighting, a technique common in matrix and tensor models. To this end I will further discuss in some detail the combinatorial structure of the complexes generated by the group field theory partition function. The new group field theories do not only strengthen the links between the mentioned quantum gravity approaches but, broadening the theory space of group field theories, they might also prove useful in the investigation of renormalizability.
Introduction to Control & Optimal control theory Maria Soledad Aronna
Moreira, Carlos Gustavo
Introduction to Control & Optimal control theory MarÂ´ia Soledad Aronna IMPA, Estrada Dona Castorina 110, 22460-320 Rio de Janeiro - RJ, Brazil November 17, 2014 Control theory deals with ordinary interval of time. Optimal control theory studies situations in which one associates a cost functional
Composite Photon Theory Versus Elementary Photon Theory
Walton A. Perkins
2015-03-02T23:59:59.000Z
The purpose of this paper is to show that the composite photon theory measures up well against the Standard Model's elementary photon theory. This is done by comparing the two theories area by area. Although the predictions of quantum electrodynamics are in excellent agreement with experiment (as in the anomalous magnetic moment of the electron), there are some problems, such as the difficulty in describing the electromagnetic field with the four-component vector potential because the photon has only two polarization states. In most areas the two theories give similar results, so it is impossible to rule out the composite photon theory. Pryce's arguments in 1938 against a composite photon theory are shown to be invalid or irrelevant. Recently, it has been realized that in the composite theory the antiphoton does not interact with matter because it is formed of a neutrino and an antineutrino with the wrong helicity. This leads to experimental tests that can determine which theory is correct.
Chu, Shih-I; Carrera, Juan J.
2009-06-17T23:59:59.000Z
stabilized narrow-band continuous-wave #1;cw#2; laser used for the actual spectroscopy. However, suitable narrow-band-width cw sources rarely exist at high frequencies #3;10#4;, such as vacuum-ultraviolet #1;vuv#2; and extreme-ultraviolet #1;xuv#2; radiations...;. If the high-frequency comb laser can be generated successfully, there will be a number of applications such as vuv-xuv holography, nanolithography, x-ray atomic clocks, and for the testing of fundamental theories such as quantum electrodynamics. However...
Some convolution products in Quantum Field Theory
Herintsitohaina Ratsimbarison
2006-12-05T23:59:59.000Z
This paper aims to show constructions of scale dependence and interaction on some probabilistic models which may be revelant for renormalization theory in Quantum Field Theory. We begin with a review of the convolution product's use in the Kreimer-Connes formalism of perturbative renormalization. We show that the Wilson effective action can be obtained from a convolution product propriety of regularized Gaussian measures on the space of fields. Then, we propose a natural C*-algebraic framework for scale dependent field theories which may enhance the conceptual approach to renormalization theory. In the same spirit, we introduce a probabilistic construction of interacting theories for simple models and apply it for quantum field theory by defining a partition function in this setting.
Appropriating Theory Bonnie Nardi
Nardi, Bonnie
Appropriating Theory Bonnie Nardi forthcoming in D. Sonnenwald, ed. Theory Development in Information: Reflecting on the Process. Austin in this volume concern the development of new theory. I want to take a slightly
David J. Gross; Washington Taylor
2001-06-04T23:59:59.000Z
We describe projection operators in the matter sector of Witten's cubic string field theory using modes on the right and left halves of the string. These projection operators represent a step towards an analytic solution of the equations of motion of the full string field theory, and can be used to construct Dp-brane solutions of the string field theory when the BRST operator Q is taken to be pure ghost, as suggested in the recent conjecture by Rastelli, Sen and Zwiebach. We show that a family of solutions related to the sliver state are rank one projection operators on the appropriate space of half-string functionals, and we construct higher rank projection operators corresponding to configurations of multiple D-branes.
LATTICE GAUGE THEORY 1 Lattice Gauge Theory
Creutz, Michael
a crucial tool for the quantum field the- orist. Applied to the formalism of lattice gauge theory, numerical simulations are providing fundamental quantitative information about the interactions of quarksLATTICE GAUGE THEORY 1 Lattice Gauge Theory Michael Creutz Supercomputers have recently become
John H. Schwarz
1998-09-01T23:59:59.000Z
Superstring theory, and a recent extension called M theory, are leading candidates for a quantum theory that unifies gravity with the other forces. As such, they are certainly not ordinary quantum field theories. However, recent duality conjectures suggest that a more complete definition of these theories can be provided by the large N limits of suitably chosen U(N) gauge theories associated to the asymptotic boundary of spacetime.
Improved methodology for refolding functional TGF-beta Superfamily ligands
Shumaker, Stephanie D.
2009-01-01T23:59:59.000Z
C. M. ; Mechanisms of Protein Folding 2000, 1, 1-28. 11.structure is critical to protein folding and function. Welandscape theory of protein folding asserts that evolution
Correlation of Structure and Function of Zinc Metalloproteins...
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of Structure and Function of Zinc Metalloproteins Via a Combined NMRMolecular Theory Approach Investigative Team: NMR: Andrew S. Lipton - PI (PNNL) and Paul D. Ellis...
Redundant axioms in the definition of Bregman functions
Jan 22, 2002 ... REDUNDANT AXIOMS IN THE DEFINITION OF BREGMAN ...... some new results on the theory of Bregman functions, Mathematics of ...
Quantum Optimal Control Theory
J. Werschnik; E. K. U. Gross
2007-07-12T23:59:59.000Z
The control of quantum dynamics via specially tailored laser pulses is a long-standing goal in physics and chemistry. Partly, this dream has come true, as sophisticated pulse shaping experiments allow to coherently control product ratios of chemical reactions. The theoretical design of the laser pulse to transfer an initial state to a given final state can be achieved with the help of quantum optimal control theory (QOCT). This tutorial provides an introduction to QOCT. It shows how the control equations defining such an optimal pulse follow from the variation of a properly defined functional. We explain the most successful schemes to solve these control equations and show how to incorporate additional constraints in the pulse design. The algorithms are then applied to simple quantum systems and the obtained pulses are analyzed. Besides the traditional final-time control methods, the tutorial also presents an algorithm and an example to handle time-dependent control targets.
Quantum Optimal Control Theory
G. H. Gadiyar
1994-05-10T23:59:59.000Z
The possibility of control of phenomena at microscopic level compatible with quantum mechanics and quantum field theory is outlined. The theory could be used in nanotechnology.
BNL | CFN: Theory & Computation
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Theory and Computation Contact: Mark Hybertsen Advances in theory, numerical algorithms and computational capabilities have enabled an unprecedented opportunity for fundamental...
Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)
Dark Matter Theory Dark Matter Theory Understanding discoveries at the Energy, Intensity, and Cosmic Frontiers Get Expertise Rajan Gupta (505) 667-7664 Email Bruce Carlsten (505)...
On higher spin partition functions
M. Beccaria; A. A. Tseytlin
2015-06-05T23:59:59.000Z
We observe that the partition function of the set of all free massless higher spins s=0,1,2,3,... in flat space is equal to one: the ghost determinants cancel against the "physical" ones or, equivalently, the (regularized) total number of degrees of freedom vanishes. This reflects large underlying gauge symmetry and suggests analogy with supersymmetric or topological theory. The Z=1 property extends also to the AdS background, i.e. the 1-loop vacuum partition function of Vasiliev theory is equal to 1 (assuming a particular regularization of the sum over spins); this was noticed earlier as a consistency requirement for the vectorial AdS/CFT duality. We find that Z=1 is also true in the conformal higher spin theory (with higher-derivative d^{2s} kinetic terms) expanded near flat or conformally flat S^4 background. We also consider the partition function of free conformal theory of symmetric traceless rank s tensor field which has 2-derivative kinetic term but only scalar gauge invariance in flat 4d space. This non-unitary theory has a Weyl-invariant action in curved background and corresponds to "partially massless" field in AdS_5. We discuss in detail the special case of s=2 (or "conformal graviton"), compute the corresponding conformal anomaly coefficients and compare them with previously found expressions for generic representations of conformal group in 4 dimensions.
Advanced Analysis: Skeleton notes 1. Fourier Theory
Davies, Christopher
Advanced Analysis: Skeleton notes 1. Fourier Theory The Fourier series of a function f() on [-, ] is - anein , where an = an(f) = 1 2 - f()e-in d. The Fourier transform of a function f(x) on R is the function ^f() = 1 2 - f(x)e-ix dx, and the Fourier inversion formula is f(x) = - f()eix d. One circle
The paleoclassical interpretation of quantum theory
I. Schmelzer
2015-06-30T23:59:59.000Z
This interpretation establishes a completely classical ontology -- only the classical trajectory in configuration space -- and interprets the wave function as describing incomplete information (in form of a probability flow) about this trajectory. This combines basic ideas of de Broglie-Bohm theory and Nelsonian stochastics about the trajectory with a Bayesian interpretation of the wave function. Various objections are considered and discussed. In particular a regularity principle for the zeros of the wave function allows to meet the Wallstrom objection.
Theory of rheology in confinement
Artem A. Aerov; Matthias Krüger
2014-12-12T23:59:59.000Z
The viscosity of fluids is generally understood in terms of kinetic mechanisms, i.e., particle collisions, or thermodynamic ones as imposed through structural distortions upon e.g. applying shear. Often the former is less relevant, and (damped) Brownian particles are considered good fluid model systems. We formulate a general theoretical approach for rheology in confinement, based on the many particle diffusion equation, evaluated via classical density functional theory. We discuss the viscosity for the situation of two parallel walls in relative motion as a function of wall-to-wall distance.
Marcos Marino; Pavel Putrov
2012-03-14T23:59:59.000Z
The partition function on the three-sphere of many supersymmetric Chern-Simons-matter theories reduces, by localization, to a matrix model. We develop a new method to study these models in the M-theory limit, but at all orders in the 1/N expansion. The method is based on reformulating the matrix model as the partition function of an ideal Fermi gas with a non-trivial, one-particle quantum Hamiltonian. This new approach leads to a completely elementary derivation of the N^{3/2} behavior for ABJM theory and N=3 quiver Chern-Simons-matter theories. In addition, the full series of 1/N corrections to the original matrix integral can be simply determined by a next-to-leading calculation in the WKB or semiclassical expansion of the quantum gas, and we show that, for several quiver Chern-Simons-matter theories, it is given by an Airy function. This generalizes a recent result of Fuji, Hirano and Moriyama for ABJM theory. It turns out that the semiclassical expansion of the Fermi gas corresponds to a strong coupling expansion in type IIA theory, and it is dual to the genus expansion. This allows us to calculate explicitly non-perturbative effects due to D2-brane instantons in the AdS background.
Alternative analysis to perturbation theory
J. Martinez-Carranza; F. Soto-Eguibar; H. Moya-Cessa
2011-10-04T23:59:59.000Z
We develop an alternative approach to time independent perturbation theory in non-relativistic quantum mechanics. The method developed has the advantage to provide in one operation the correction to the energy and to the wave function, additionally we can analyze the time evolution of the system. To verify our results, we apply our method to the harmonic oscillator perturbed by a quadratic potential. An alternative form of the Dyson series, in matrix form instead of integral form, is also obtained.
Washington Taylor
2006-06-28T23:59:59.000Z
This elementary introduction to string field theory highlights the features and the limitations of this approach to quantum gravity as it is currently understood. String field theory is a formulation of string theory as a field theory in space-time with an infinite number of massive fields. Although existing constructions of string field theory require expanding around a fixed choice of space-time background, the theory is in principle background-independent, in the sense that different backgrounds can be realized as different field configurations in the theory. String field theory is the only string formalism developed so far which, in principle, has the potential to systematically address questions involving multiple asymptotically distinct string backgrounds. Thus, although it is not yet well defined as a quantum theory, string field theory may eventually be helpful for understanding questions related to cosmology in string theory.
Resurgent functions and splitting problems
Sauzin, David
2006-01-01T23:59:59.000Z
The present text is an introduction to \\'Ecalle's theory of resurgent functions and alien calculus, in connection with problems of exponentially small separatrix splitting. An outline of the resurgent treatment of Abel's equation for resonant dynamics in one complex variable is included. The emphasis is on examples of nonlinear difference equations, as a simple and natural way of introducing the concepts.
Interpolating function and Stokes Phenomena
Masazumi Honda; Dileep P. Jatkar
2015-04-28T23:59:59.000Z
When we have two expansions of physical quantity around two different points in parameter space, we can usually construct a family of functions, which interpolates the both expansions. In this paper we study analytic structures of such interpolating functions and discuss their physical implications. We propose that the analytic structures of the interpolating functions provide information on analytic property and Stokes phenomena of the physical quantity, which we approximate by the interpolating functions. We explicitly check our proposal for partition functions of zero-dimensional $\\varphi^4$ theory and Sine-Gordon model. In the zero dimensional Sine-Gordon model, we compare our result with a recent result from resurgence analysis. We also comment on construction of interpolating function in Borel plane.
Interpolating function and Stokes Phenomena
Honda, Masazumi
2015-01-01T23:59:59.000Z
When we have two expansions of physical quantity around two different points in parameter space, we can usually construct a family of functions, which interpolates the both expansions. In this paper we study analytic structures of such interpolating functions and discuss their physical implications. We propose that the analytic structures of the interpolating functions provide information on analytic property and Stokes phenomena of the physical quantity, which we approximate by the interpolating functions. We explicitly check our proposal for partition functions of zero-dimensional $\\varphi^4$ theory and Sine-Gordon model. In the zero dimensional Sine-Gordon model, we compare our result with a recent result from resurgence analysis. We also comment on construction of interpolating function in Borel plane.
Bivariate lognormal density function
Schreyer, Glenn William
1972-01-01T23:59:59.000Z
. H. Matis and. Dr. C. K. Chui. TABLE OF CONTENTS CHAPTER Page I INTRODUCTION 1. 1 Current Status of' the Theory 1. 2 Aims of' the investigation 1. 3 Possible Applications 1 3 3 II THE PARA|%TER ESTIMATION 2. 1 Problem Description 2. 2... The Estimates RELATED PROBLHMS 3. 1 Missing Data Problem 5 1. 4 1. 6 16 3, 1. 1 Method. of Mm~ imum Likelihood 3. 1, 2 Smith-Hocking Procedure 17 19 IV 3. 2 The Hs. zard. Function MONTE CARLO STUDY 4. 1 The Simulation Problem 4. 2 The Simulation...
Bevir, Mark
2013-01-01T23:59:59.000Z
direct interference. Proponents of governability theory stress the resources the state has at its disposal
Introduction to Information Theory
Belohlavek, Radim
Introduction to Information Theory and Its Applications Radim Belohl´avek Dept. Computer Science providing introduction to Information Theory. Radim Belohl´avek, Introduction to Information Theory and Its Applications 1 #12;Information Theory: What and Why · information: one of key terms in our society
Zhang, Shuzhong
Introduction Theory of CAMNS Practical realization of CAMNS Simulation results & Conclusions Blind Separation of Non-negative Sources using Convex Analysis: Theory and Methods Wing-Kin (Ken) Ma Dept Blind Separation of Non-negative Sources using Convex Analysis: Theory and #12;Introduction Theory
Introduction Classical Field Theory
Baer, Christian
Introduction Classical Field Theory Locally Covariant Quantum Field Theory Renormalization Time evolution Conclusions and outlook Locality and Algebraic Structures in Field Theory Klaus Fredenhagen IIÂ¨utsch and Pedro Lauridsen Ribeiro) Klaus Fredenhagen Locality and Algebraic Structures in Field Theory #12
Mardirossian, Narbe; Head-Gordon, Martin, E-mail: mhg@cchem.berkeley.edu [Department of Chemistry, University of California, Berkeley and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)] [Department of Chemistry, University of California, Berkeley and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)
2014-05-14T23:59:59.000Z
The limit of accuracy for semi-empirical generalized gradient approximation (GGA) density functionals is explored by parameterizing a variety of local, global hybrid, and range-separated hybrid functionals. The training methodology employed differs from conventional approaches in 2 main ways: (1) Instead of uniformly truncating the exchange, same-spin correlation, and opposite-spin correlation functional inhomogeneity correction factors, all possible fits up to fourth order are considered, and (2) Instead of selecting the optimal functionals based solely on their training set performance, the fits are validated on an independent test set and ranked based on their overall performance on the training and test sets. The 3 different methods of accounting for exchange are trained both with and without dispersion corrections (DFT-D2 and VV10), resulting in a total of 491 508 candidate functionals. For each of the 9 functional classes considered, the results illustrate the trade-off between improved training set performance and diminished transferability. Since all 491 508 functionals are uniformly trained and tested, this methodology allows the relative strengths of each type of functional to be consistently compared and contrasted. The range-separated hybrid GGA functional paired with the VV10 nonlocal correlation functional emerges as the most accurate form for the present training and test sets, which span thermochemical energy differences, reaction barriers, and intermolecular interactions involving lighter main group elements.
V.3K(1)-Local Homotopy Theory, Iwasawa Theory
V.3K(1)-Local Homotopy Theory, Iwasawa Theory and Algebraic K-Theory Stephen A. Mitchell* 3.3 K(1)-local Homotopy Theory............................................................. 965 -Adic K-Theory ................................................................. 968 K(1)-Localization
Quantum statistical correlations in thermal field theories: Boundary effective theory
Bessa, A. [Escola de Ciencias e Tecnologia, Universidade Federal do Rio Grande do Norte, Caixa Postal 1524, 59072-970, Natal, RN (Brazil); Instituto de Fisica, Universidade de Sao Paulo, Caixa Postal 66318, 05315-970, Sao Paulo, SP (Brazil); Brandt, F. T. [Instituto de Fisica, Universidade de Sao Paulo, Caixa Postal 66318, 05315-970, Sao Paulo, SP (Brazil); Carvalho, C. A. A. de; Fraga, E. S. [Instituto de Fisica, Universidade Federal do Rio de Janeiro, Caixa Postal 68528, 21941-972, Rio de Janeiro, RJ (Brazil)
2010-09-15T23:59:59.000Z
We show that the one-loop effective action at finite temperature for a scalar field with quartic interaction has the same renormalized expression as at zero temperature if written in terms of a certain classical field {phi}{sub c}, and if we trade free propagators at zero temperature for their finite-temperature counterparts. The result follows if we write the partition function as an integral over field eigenstates (boundary fields) of the density matrix element in the functional Schroedinger field representation, and perform a semiclassical expansion in two steps: first, we integrate around the saddle point for fixed boundary fields, which is the classical field {phi}{sub c}, a functional of the boundary fields; then, we perform a saddle-point integration over the boundary fields, whose correlations characterize the thermal properties of the system. This procedure provides a dimensionally reduced effective theory for the thermal system. We calculate the two-point correlation as an example.
Super-renormalizable & Finite Gravitational Theories
Leonardo Modesto; Leslaw Rachwal
2014-07-30T23:59:59.000Z
We hereby introduce and extensively study a class of non-polynomial higher derivative theories of gravity that realize a ultraviolet (UV) completion of Einstein general relativity. These theories are unitary (ghost free) and at most only one-loop divergences survive. The outcome is a class of theories super-renormalizable in even dimension and finite in odd dimension. Moreover, we explicitly prove in D=4 that there exists an extension of the theory that is completely finite and all the beta functions vanish even at one-loop. These results can be easily extended in extra dimensions and it is likely that the higher dimensional theory can be made finite too. Therefore we have the possibility for "finite quantum gravity" in any dimension.
ABJ Theory in the Higher Spin Limit
Shinji Hirano; Masazumi Honda; Kazumi Okuyama; Masaki Shigemori
2015-04-27T23:59:59.000Z
We study the conjecture made by Chang, Minwalla, Sharma, and Yin on the duality between the N=6 Vasiliev higher spin theory on AdS_4 and the N=6 Chern-Simons-matter theory, so-called ABJ theory, with gauge group U(N) x U(N+M). Building on our earlier results on the ABJ partition function, we develop the systematic 1/M expansion, corresponding to the weak coupling expansion in the higher spin theory, and compare the leading 1/M correction, with our proposed prescription, to the one-loop free energy of the N=6 Vasiliev theory. We find an agreement between the two sides up to an ambiguity that appears in the bulk one-loop calculation.
Noncommutative Quantization for Noncommutative Field Theory
Yasumi Abe
2006-07-06T23:59:59.000Z
We present a new procedure for quantizing field theory models on a noncommutative spacetime. The new quantization depends on the noncommutative parameter explicitly and reduces to the canonical quantization in the commutative limit. It is shown that a quantum field theory constructed by the new quantization yeilds exactly the same correlation functions as those of the commutative field theory, that is, the noncommutative effects disappear completely after quantization. This implies, for instance, that by using the new quantization, the noncommutativity can be incorporated in the process of quantization, rahter than in the action as conventionally done.
Three approaches to classical thermal field theory
Gozzi, E., E-mail: gozzi@ts.infn.it [Department of Physics, University of Trieste, Strada Costiera 11, Miramare - Grignano, 34151 Trieste (Italy); INFN, Sezione di Trieste (Italy); Penco, R., E-mail: rpenco@syr.edu [Department of Physics, Syracuse University, Syracuse, NY 13244-1130 (United States)
2011-04-15T23:59:59.000Z
Research Highlights: > Classical thermal field theory admits three equivalent path integral formulations. > Classical Feynman rules can be derived for all three formulations. > Quantum Feynman rules reduce to classical ones at high temperatures. > Classical Feynman rules become much simpler when superfields are introduced. - Abstract: In this paper we study three different functional approaches to classical thermal field theory, which turn out to be the classical counterparts of three well-known different formulations of quantum thermal field theory: the closed-time path (CTP) formalism, the thermofield dynamics (TFD) and the Matsubara approach.
Splines and Linear Control Theory Zhimin Zhang, John Tomlinson and Clyde Martin
Zhang, Zhimin
Splines and Linear Control Theory Zhimin Zhang, John Tomlinson and Clyde Martin Department and the linear control theory has been analyzed. We show that spline functions can be constructed naturally from the control theory. By establishing a framework based on control theory, we provide a simple and systematic
Mesoscopic theory of the viscoelasticity of polymers
S. M. Chitanvis
1999-01-26T23:59:59.000Z
We have advanced our previous static theory of polymer entanglement involving an extended Cahn-Hilliard functional, to include time-dependent dynamics. We go beyond the Gaussian approximation, to the one-loop level, to compute the frequency dependent storage and loss moduli of the system. The three parameters in our theory are obtained by fitting to available experimental data on polystyrene melts of various chain lengths. This provides a physical representation of the parameters in terms of the chain length of the system. We discuss the importance of the various terms in our energy functional with respect to their contribution to the viscoelastic response of the polymeric system.
Söderlind, P. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Landa, A. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Turchi, P. E. A. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
2014-10-01T23:59:59.000Z
In a recent paper, Xie et al. [Phys. Rev. B 88, 235128 (2013)], report that the density-functional theory (DFT) with the so-called DFT plus Hubbard U (DFT+U) modification improves energetics, volumes, and formation enthalpies over the standard form of DFT for uranium metal and U-Zr alloys. Also, spin-orbit coupling (SOC) was argued to advance the aforementioned properties in these systems. We demonstrate, contrarily, that neither the Hubbard U approach nor SOC is necessary for a correct description of uranium metal and U-Zr alloys. We further illustrate that the combination of DFT+U and SOC in the projector augmented-wave calculations by Xie et al. results in unrealistically large volume expansions, particularly for ?-U, in stark contrast to all previous calculations for elemental uranium. This in turn may also explain why the DFT+U with SOC model predicts negative enthalpy of mixing in the U-Zr alloy system contradicting conventional DFT as well as one of the main features of the experimental U-Zr phase diagram. The assertion by Xie et al. that DFT+U is an improvement over DFT for these systems is illustrated to be incorrect.
Green Functions of Relativistic Field Equations
Ying-Qiu Gu
2006-12-20T23:59:59.000Z
In this paper, we restudy the Green function expressions of field equations. We derive the explicit form of the Green functions for the Klein-Gordon equation and Dirac equation, and then estimate the decay rate of the solution to the linear equations. The main motivation of this paper is to show that: (1). The formal solutions of field equations expressed by Green function can be elevated as a postulate for unified field theory. (2). The inescapable decay of the solution of linear equations implies that the whole theory of the matter world should include nonlinear interaction.
Generalized Quantum Theory and Mathematical Foundations of Quantum Field Theory
Maroun, Michael Anthony
2013-01-01T23:59:59.000Z
The Unique Status of Condensed Matter Theory . . . . . . . .of a Satisfactory Theory . . . . . . . . . . . . BasicThe Generalized Quantum Theory The Postulates and Philosophy
Exact results on ABJ theory and the refined topological string
Masazumi Honda; Kazumi Okuyama
2014-07-22T23:59:59.000Z
We study the partition function of the ABJ theory, which is the N=6 superconformal Chern-Simons matter theory with gauge group U(N)xU(N+M) and Chern-Simons levels (k,-k). We exactly compute the ABJ partition function on a three sphere for various k, M and N via the Fermi gas approach. By using these exact data, we show that the ABJ partition function is completely determined by the refined topological string on local P^1 x P^1, including membrane instanton effects in the M-theory dual.
Tom Banks
1999-11-10T23:59:59.000Z
This is a series of lectures on M Theory for cosmologists. After summarizing some of the main properties of M Theory and its dualities I show how it can be used to address various fundamental and phenomenological issues in cosmology.
Henderson, Leah
2010-01-01T23:59:59.000Z
This thesis consists of three papers on the nature of scientific theories and inference. In many cases, scientific theories can be regarded as organized into hierarchies, with higher levels sometimes called 'paradigms', ...
Covariant Noncommutative Field Theory
Estrada-Jimenez, S. [Licenciaturas en Fisica y en Matematicas, Facultad de Ingenieria, Universidad Autonoma de Chiapas Calle 4a Ote. Nte. 1428, Tuxtla Gutierrez, Chiapas (Mexico); Garcia-Compean, H. [Departamento de Fisica, Centro de Investigacion y de Estudios Avanzados del IPN P.O. Box 14-740, 07000 Mexico D.F., Mexico and Centro de Investigacion y de Estudios Avanzados del IPN, Unidad Monterrey Via del Conocimiento 201, Parque de Investigacion e Innovacion Tecnologica (PIIT) Autopista nueva al Aeropuerto km 9.5, Lote 1, Manzana 29, cp. 66600 Apodaca Nuevo Leon (Mexico); Obregon, O. [Instituto de Fisica de la Universidad de Guanajuato P.O. Box E-143, 37150 Leon Gto. (Mexico); Ramirez, C. [Facultad de Ciencias Fisico Matematicas, Universidad Autonoma de Puebla, P.O. Box 1364, 72000 Puebla (Mexico)
2008-07-02T23:59:59.000Z
The covariant approach to noncommutative field and gauge theories is revisited. In the process the formalism is applied to field theories invariant under diffeomorphisms. Local differentiable forms are defined in this context. The lagrangian and hamiltonian formalism is consistently introduced.
Eisenstein Series in String Theory
N. A. Obers; B. Pioline
2000-03-01T23:59:59.000Z
We discuss the relevance of Eisenstein series for representing certain G(Z)-invariant string theory amplitudes which receive corrections from BPS states only. The Eisenstein series are constructed using G(Z)-invariant mass formulae and are manifestly invariant modular functions on the symmetric space K\\G(R) of non-compact type, with K the maximal compact subgroup of G(R). In particular, we show how Eisenstein series of the T-duality group SO(d,d,Z) can be used to represent one- and g-loop amplitudes in compactified string theory. We also obtain their non-perturbative extensions in terms of the Eisenstein series of the U-duality group E_{d+1(d+1)}(Z).
Thomson, James D.
allocation theory is that an organism's reproductive success, through either male or female function, can in that function. The shapes of these curves determine what patterns of resource allocation can be evolutionarily and female pathways, to the amount of resources it invested in male and female function. Sex allocation
Topological quantum field theories
Albert Schwarz
2000-11-29T23:59:59.000Z
Following my plenary lecture on ICMP2000 I review my results concerning two closely related topics: topological quantum field theories and the problem of quantization of gauge theories. I start with old results (first examples of topological quantum field theories were constructed in my papers in late seventies) and I come to some new results, that were not published yet.
New second derivative theories of gravity for spherically symmetric spacetimes
Rakesh Tibrewala
2015-03-17T23:59:59.000Z
We present new second derivative, generally covariant theories of gravity for spherically symmetric spacetimes (general covariance is in the $t-r$ plane) belonging to the class where the spherically symmetric Einstein-Hilbert theory is modified by the presence of $g_{\\theta\\theta}$ dependent functions. In $3+1$ dimensional vacuum spacetimes there is three-fold infinity of freedom in constructing such theories as revealed by the presence of three arbitrary $g_{\\theta\\theta}$ dependent functions in the Hamiltonian (matter Hamiltonian also has the corresponding freedom). This result is not a contradiction to the theorem of Hojman et. al. [1] which is applicable to the full theory whereas the above conclusion is for symmetry reduced sector of the theory (which has a much reduced phase space). In the full theory where there are no special symmetries, the result of Hojman et. al. will continue to hold. In the process we also show that theories where the constraint algebra is deformed by the presence of $g_{\\theta\\theta}$ dependent functions - as is the case in the presence of inverse triad corrections in loop quantum gravity - can always be brought to the form where they obey the standard (undeformed) constraint algebra by performing a suitable canonical transformation. We prove that theories obtained after performing canonical transformation are inequivalent to the symmetry reduced general relativity and that the resulting theories fall within the purview of the theories mentioned above.
Evolution of the coupling constant in SU(2) lattice gauge theory with two adjoint fermions
Ari J. Hietanen; Kari Rummukainen; Kimmo Tuominen
2009-11-24T23:59:59.000Z
We measure the evolution of the coupling constant using the Schroedinger functional method in the lattice formulation of SU(2) gauge theory with two massless Dirac fermions in the adjoint representation. We observe strong evidence for an infrared fixed point, where the theory becomes conformal. We measure the continuum beta-function and the coupling constant as a function of the energy scale.
Gauge theories on noncommutative spaces
Albert Schwarz
2000-11-29T23:59:59.000Z
I review my results about noncommutative gauge theories and about the relation of these theories to M(atrix) theory following my lecture on ICMP 2000.
Higher Auslander-Reiten Theory
West, Jacob
2015-01-01T23:59:59.000Z
Linearly Com- pact Rings. Applications. , Category Theory,Homology Theory and their Applications II. Lecture Notes in1977), 519– , Representation Theory of Artin Algebras VI: A
Limit theory for overfit models
Calhoun, Grayson Ford
2009-01-01T23:59:59.000Z
theory. . . . . . . . . . . . . . . . . . . . . . . . .1.2 Asymptotic Theory and Main Results . . . . . . . . .Chapter 2 Limit theory for comparing over?t models out-of-
Review: Theories of Sustainable Development
Laberge, Yves
2015-01-01T23:59:59.000Z
Review: Theories of Sustainable Development Edited By JudithTheories of Sustainable Development. Abingdon: Routledge,Routledge Studies in Sustainable Development. Theories of
Theorizing Practice and Practicing Theory
Feldman, Martha S; Orlikowski, Wanda J
2011-01-01T23:59:59.000Z
Practice and Practicing Theory Organization Science 22(5),Practice and Practicing Theory Organization Science 22(5),Practice and Practicing Theory Organization Science 22(5),
Variational methods for field theories
Ben-Menahem, S.
1986-09-01T23:59:59.000Z
Four field theory models are studied: Periodic Quantum Electrodynamics (PQED) in (2 + 1) dimensions, free scalar field theory in (1 + 1) dimensions, the Quantum XY model in (1 + 1) dimensions, and the (1 + 1) dimensional Ising model in a transverse magnetic field. The last three parts deal exclusively with variational methods; the PQED part involves mainly the path-integral approach. The PQED calculation results in a better understanding of the connection between electric confinement through monopole screening, and confinement through tunneling between degenerate vacua. This includes a better quantitative agreement for the string tensions in the two approaches. Free field theory is used as a laboratory for a new variational blocking-truncation approximation, in which the high-frequency modes in a block are truncated to wave functions that depend on the slower background modes (Boron-Oppenheimer approximation). This ''adiabatic truncation'' method gives very accurate results for ground-state energy density and correlation functions. Various adiabatic schemes, with one variable kept per site and then two variables per site, are used. For the XY model, several trial wave functions for the ground state are explored, with an emphasis on the periodic Gaussian. A connection is established with the vortex Coulomb gas of the Euclidean path integral approach. The approximations used are taken from the realms of statistical mechanics (mean field approximation, transfer-matrix methods) and of quantum mechanics (iterative blocking schemes). In developing blocking schemes based on continuous variables, problems due to the periodicity of the model were solved. Our results exhibit an order-disorder phase transition. The transfer-matrix method is used to find a good (non-blocking) trial ground state for the Ising model in a transverse magnetic field in (1 + 1) dimensions.
II.2K-Theory and Intersection Theory
II.2K-Theory and Intersection Theory Henri Gillet 2.1 Introduction.3 K-Theory and Intersection Multiplicities ......................................... 253 Serre's tor Groups .............................................. 259 Higher Rational Equivalence and Milnor K-Theory
Sociology: Computational Organization Theory Sociology: Computational Organization Theory
Sadeh, Norman M.
Sociology: Computational Organization Theory Sociology: Computational Organization Theory Kathleen; organization theory; organizational learning; social networks; expert systems Citation: Kathleen Carley, 1994, "Sociology: Computational Organization Theory." Social Science Computer Review, 12(4): 611-624. #12;Sociology
Exact Results in Supersymmetric Gauge Theories
Saulius Valatka
2014-12-31T23:59:59.000Z
In this thesis we discuss supersymmetric gauge theories, focusing on exact results achieved using methods of integrability. For the larger portion of the thesis we study the N=4 super Yang-Mills theory in the planar limit, a recurring topic being the Konishi anomalous dimension, which is roughly the analogue for the mass of the proton in quantum chromodynamics. The N=4 supersymmetric Yang-Mills theory is known to be integrable in the planar limit, which opens up a wealth of techniques one can employ in order to find results in this limit valid at any value of the coupling. We begin with perturbation theory where the integrability of the theory first manifests itself. Here we showcase the first exact result, the so-called slope function, which is the linear small spin expansion coefficient of the generalized Konishi anomalous dimension. We then move on to exact results mainly achieved using the novel quantum spectral curve approach, the method allowing one to find scaling dimensions of operators at arbitrary values of the coupling. As an example we find the second coefficient in the small spin expansion after the slope, which we call the curvature function. This allows us to extract non-trivial information about the Konishi operator. Methods of integrability are also applicable to other supersymmetric gauge theories such as ABJM, which in fact shares many similarities with N=4 super Yang-Mills. We briefly review these parallel developments in the last chapter of the thesis.
John H. Schwarz
1995-03-20T23:59:59.000Z
A brief review of the status of duality symmetries in string theory is presented. The evidence is accumulating rapidly that an enormous group of duality symmetries, including perturbative T dualities and non-perturbative S-dualities, underlies string theory. It is my hope that an understanding of these symmetries will suggest the right way to formulate non-perturbative string theory. Whether or not this hope is realized, it has already been demonstrated that this line of inquiry leads to powerful new tools for understanding gauge theories and new evidence for the uniqueness of string theory, as well as deep mathematical results.
Bootstrapping Fuzzy Scalar Field Theory
Christian Saemann
2015-04-13T23:59:59.000Z
We describe a new way of rewriting the partition function of scalar field theory on fuzzy complex projective spaces as a solvable multitrace matrix model. This model is given as a perturbative high-temperature expansion. At each order, we present an explicit analytic expression for most of the arising terms; the remaining terms are computed explicitly up to fourth order. The method presented here can be applied to any model of hermitian matrices. Our results confirm constraints previously derived for the multitrace matrix model by Polychronakos. A further implicit expectation about the shape of the multitrace terms is however shown not to be true.
Active Oxygen Vacancy Site for Methanol Synthesis from CO2 Hydrogenation on In2O3(110): A DFT Study
Ye, Jingyun; Liu, Changjun; Mei, Donghai; Ge, Qingfeng
2013-06-03T23:59:59.000Z
Methanol synthesis from CO2 hydrogenation on the defective In2O3(110) surface with surface oxygen vacancies has been investigated using periodic density functional theory calculations. The relative stabilities of six possible surface oxygen vacancies numbered from Ov1 to Ov6 on the perfect In2O3(110) surface were examined. The calculated oxygen vacancy formation energies show that the D1 surface with the Ov1 defective site is the most thermodynamically favorable while the D4 surface with the Ov4 defective site is the least stable. Two different methanol synthesis routes from CO2 hydrogenation over both D1 and D4 surfaces were studied and the D4 surface was found to be more favorable for CO2 activation and hydrogenation. On the D4 surface, one of the O atoms of the CO2 molecule fills in the Ov4 site upon adsorption. Hydrogenation of CO2 to HCOO on the D4 surface is both thermodynamically and kinetically favorable. Further hydrogenation of HCOO involves both forming the C-H bond and breaking the C-O bond, resulting in H2CO and hydroxyl. The HCOO hydrogenation is slightly endothermic with an activation barrier of 0.57 eV. A high barrier of 1.14 eV for the hydrogenation of H2CO to H3CO indicates that this step is the rate-limiting step in the methanol synthesis on the defective In2O3(110) surface. We gratefully acknowledge the supports from the National Natural Science Foundation of China (#20990223) and from US Department of Energy, Basic Energy Science program (DE-FG02-05ER46231). D. Mei was supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. The computations were performed in part using the Molecular Science Computing Facility in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), which is a U.S. Department of Energy national scientific user facility located at Pacific Northwest National Laboratory in Richland, Washington. PNNL is a multiprogram national laboratory operated for DOE by Battelle.
Non-Lagrangian Theories from Brane Junctions
Ling Bao; Vladimir Mitev; Elli Pomoni; Masato Taki; Futoshi Yagi
2013-11-08T23:59:59.000Z
In this article we use 5-brane junctions to study the 5D T_N SCFTs corresponding to the 5D N=1 uplift of the 4D N=2 strongly coupled gauge theories, which are obtained by compactifying N M5 branes on a sphere with three full punctures. Even though these theories have no Lagrangian description, by using the 5-brane junctions proposed by Benini, Benvenuti and Tachikawa, we are able to derive their Seiberg-Witten curves and Nekrasov partition functions. We cross-check our results with the 5D superconformal index proposed by Kim, Kim and Lee. Through the AGTW correspondence, we discuss the relations between 5D superconformal indices and n-point functions of the q-deformed W_N Toda theories.
Network Security Validation Using Game Theory
Mavronicolas, Marios
1 Network Security Validation Using Game Theory Vicky Papadopoulou and Andreas Gregoriades Computer.papadopoulou,a.gregoriades}@euc.ac.cy Abstract: Non-functional requirements (NFR) such as network security recently gained widespread attention the immunity property of the distributed systems that depended on these networks. Security requirements
Modular bootstrap in Liouville field theory
Leszek Hadasz; Zbigniew Jaskolski; Paulina Suchanek
2009-11-22T23:59:59.000Z
The modular matrix for the generic 1-point conformal blocks on the torus is expressed in terms of the fusion matrix for the 4-point blocks on the sphere. The modular invariance of the toric 1-point functions in the Liouville field theory with DOZZ structure constants is proved.
MULTIVARIATE OUTLYINGNESS FUNCTIONS MAHALANOBIS TYPE OUTLYINGNESS FUNCTIONS
Serfling, Robert
OUTLINE MULTIVARIATE OUTLYINGNESS FUNCTIONS MAHALANOBIS TYPE OUTLYINGNESS FUNCTIONS ADDITION MULTIVARIATE OUTLYINGNESS FUNCTIONS MAHALANOBIS TYPE OUTLYINGNESS FUNCTIONS ADDITION AND REPLACEMENT BREAKDOWN Criterion Robert Serfling NONPARAMETRIC OUTLIER IDENTIFICATION #12;OUTLINE MULTIVARIATE OUTLYINGNESS
Magnetism Theory Group / POSTECH Magnetism Theory Group / POSTECH
Min, Byung Il
Magnetism Theory Group / POSTECH #12;Magnetism Theory Group / POSTECH #12;Magnetism Theory Group / POSTECH #12;Magnetism Theory Group / POSTECH #12;Magnetism Theory Group / POSTECH J.H . Park et al. #12;'s of FeinCsm e tal The chargeandorbitalordering geom etryin YB a C o 2 O 5 S. K. Kwon etal .Magnetism Theory
Spin-Statistics Correlations in Various Noncommutative Field Theories
Rahul Srivastava
2013-09-01T23:59:59.000Z
In this thesis we study field theories written on a particular model of noncommutative spacetime, the Groenewold-Moyal (GM) plane. We start with briefly reviewing the novel features of field theories on GM plane e.g. the $\\ast$-product, restoration of Poincar\\'e-Hopf symmetry and twisted commutation relations. We then discuss our work on renormalization of field theories on GM plane. We show that any generic noncommutative theory involving pure matter fields with polynomial interactions, is a renormalizable theory if the analogous commutative theory is renormalizable. We further show that all such noncommutative theories will have same fixed points and $\\beta$-functions for the couplings, as that of the analogous commutative theory. The unique feature of these field theories is the twisted statistics obeyed by the particles. Motivated by it, we look at the possibility of twisted statistics by deforming internal symmetries instead of spacetime symmetries. We construct two different twisted theories which can be viewed as internal symmetry analogue of the GM plane and dipole field theories which arise in the low energy limit of certain string configurations. We further study their various properties like the issue of causality and the scattering formalism. Having studied the mathematical properties of noncommutative and twisted internal symmetries we move on to discuss their potential phenomenological signatures. We first discuss the noncommutative thermal correlation functions and show that because of the twisted statistics, all correlation functions except two-point function get modified. Finally we discuss the modifications in Hanbury-Brown Twiss (HBT) correlation functions due to twisted statistics on GM plane and the potential of observing signatures of noncommutativity by doing a HBT correlation experiment with Ultra High Energy Cosmic Rays (UHECRs).
Viscosity, Black Holes, and Quantum Field Theory
D. T. Son; A. O. Starinets
2007-07-11T23:59:59.000Z
We review recent progress in applying the AdS/CFT correspondence to finite-temperature field theory. In particular, we show how the hydrodynamic behavior of field theory is reflected in the low-momentum limit of correlation functions computed through a real-time AdS/CFT prescription, which we formulate. We also show how the hydrodynamic modes in field theory correspond to the low-lying quasinormal modes of the AdS black p-brane metric. We provide a proof of the universality of the viscosity/entropy ratio within a class of theories with gravity duals and formulate a viscosity bound conjecture. Possible implications for real systems are mentioned.
Renormalization of Noncommutative Quantum Field Theories
Amilcar R. de Queiroz; Rahul Srivastava; Sachindeo Vaidya
2013-02-14T23:59:59.000Z
We report on a comprehensive analysis of the renormalization of noncommutative \\phi^4 scalar field theories on the Groenewold-Moyal (GM) plane. These scalar field theories are twisted Poincar\\'e invariant. Our main results are that these scalar field theories are renormalizable, free of UV/IR mixing, possess the same fixed points and \\beta-functions for the couplings as their commutative counterparts. We also argue that similar results hold true for any generic noncommutative field theory with polynomial interactions and involving only pure matter fields. A secondary aim of this work is to provide a comprehensive review of different approaches for the computation of the noncommutative S-matrix: noncommutative interaction picture and noncommutative LSZ formalism.
Noncommutative Deformations of Wightman Quantum Field Theories
Harald Grosse; Gandalf Lechner
2008-08-26T23:59:59.000Z
Quantum field theories on noncommutative Minkowski space are studied in a model-independent setting by treating the noncommutativity as a deformation of quantum field theories on commutative space. Starting from an arbitrary Wightman theory, we consider special vacuum representations of its Weyl-Wigner deformed counterpart. In such representations, the effect of the noncommutativity on the basic structures of Wightman theory, in particular the covariance, locality and regularity properties of the fields, the structure of the Wightman functions, and the commutative limit, is analyzed. Despite the nonlocal structure introduced by the noncommutativity, the deformed quantum fields can still be localized in certain wedge-shaped regions, and may therefore be used to compute noncommutative corrections to two-particle S-matrix elements.
Rigorous results in space-space noncommutative quantum field theory
M. N. Mnatsakanova; Yu. S. Vernov
2006-12-19T23:59:59.000Z
The axiomatic approach based on Wightman functions is developed in noncommutative quantum field theory. We have proved that the main results of the axiomatic approach remain valid if the noncommutativity affects only the spatial variables.
On the excursion theory for linear diffusions Paavo Salminen
Paris-Sud XI, Université de
in the canonical space C of continuous functions : R+ R+. Let Ct := {(s) : s t} denote the smallest -algebra awarded the 1st Gauss prize, by offering some discussion and illustration of K It^o's excursion theory
PCT Theorem in Field Theory on Noncommutative Space
Namit Mahajan
2003-07-29T23:59:59.000Z
The PCT theorem is shown to be valid in quantum field theory formulated on noncommutative spacetime by exploiting the properties of the Wightman functions defined in such a set up.
Theory of light-harvesting in photosynthesis: from structure...
Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)
Theory of light-harvesting in photosynthesis: from structure to function May 17, 2011 at 3pm36-428 Thomas Renger Johannes Kepler Universitat -Linz, Austria renger2 abstract In...
Chen, Jiale [Institute of Plasma Physics, Chinese Academy of Sciences, Hefei 230031 (China) [Institute of Plasma Physics, Chinese Academy of Sciences, Hefei 230031 (China); Center for Magnetic Fusion Theory, Chinese Academy of Sciences, Hefei (China); Gao, Zhe [Department of Engineering Physics, Tsinghua University, Beijing 100084 (China) [Department of Engineering Physics, Tsinghua University, Beijing 100084 (China); Center for Magnetic Fusion Theory, Chinese Academy of Sciences, Hefei (China)
2013-08-15T23:59:59.000Z
The second-order velocity distribution function was calculated from the second-order rf kinetic theory [Jaeger et al., Phys. Plasmas 7, 641 (2000)]. However, the nonresonant ponderomotive force in the radial direction derived from the theory is inconsistent with that from the fluid theory. The inconsistency arises from that the multiple-timescale-separation assumption fails when the second-order Vlasov equation is directly integrated along unperturbed particle orbits. A slowly ramped wave field including an adiabatic turn-on process is applied in the modified kinetic theory in this paper. Since this modification leads only to additional reactive/nonresonant response relevant with the secular resonant response from the previous kinetic theory, the correct nonresonant ponderomotive force can be obtained while all the resonant moments remain unchanged.
Finding True Beliefs: Applying Rank-Dependent Expected Utility Theory
Chen, Yiling
-making that incorporates probability weighting and non-linear utility functions, to the analysis of the quadratic scoringFinding True Beliefs: Applying Rank-Dependent Expected Utility Theory to Proper Scoring Rules-value maximizers. Thus, we apply rank-dependent expected utility theory, a more general model of decision
Shear viscosity of the $\\Phi^4$ theory from classical simulation
Homor, M M
2015-01-01T23:59:59.000Z
Shear viscosity of the classical $\\Phi^4$ theory is measured using classical microcanonical simulation. To calculate the Kubo formula, we measure the energy-momentum tensor correlation function, and apply the Green-Kubo relation. Being a classical theory, the results depend on the cutoff which should be chosen in the range of the temperature. Comparison with experimentally accessible systems is also performed.
Shear viscosity of the $?^4$ theory from classical simulation
M. M. Homor; A. Jakovac
2015-05-05T23:59:59.000Z
Shear viscosity of the classical $\\Phi^4$ theory is measured using classical microcanonical simulation. To calculate the Kubo formula, we measure the energy-momentum tensor correlation function, and apply the Green-Kubo relation. Being a classical theory, the results depend on the cutoff which should be chosen in the range of the temperature. Comparison with experimentally accessible systems is also performed.
Fourier Analysis, Distribution Theory, and Wavelets Bengt Ove Turesson1
Nair, M.Thamban
Fourier Analysis, Distribution Theory, and Wavelets Bengt Ove Turesson1 March 13, 2012 1 . . . . . . . . . . . . . . . . . . . . . . . . . . 13 II Fourier Series 14 2 L1 -theory for Fourier Series 15 2.1 Function Spaces . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15 2.2 Fourier Series and Fourier Coefficients . . . . . . . . . . . . . . . . . 15 2.3 Trigonometric
A Goldstone Theorem in Thermal Relativistic Quantum Field Theory
Christian D. Jaekel; Walter F. Wreszinski
2010-06-01T23:59:59.000Z
We prove a Goldstone Theorem in thermal relativistic quantum field theory, which relates spontaneous symmetry breaking to the rate of space-like decay of the two-point function. The critical rate of fall-off coincides with that of the massless free scalar field theory. Related results and open problems are briefly discussed.
A review on SUSY gauge theories on $S^3$
Kazuo Hosomichi
2015-07-04T23:59:59.000Z
This is the 9th article in the collection of reviews "Exact results on N=2 supersymmetric gauge theories", ed. J.Teschner. We review the exact computations in 3D N=2 supersymmetric gauge theories on the round or squashed $S^3$ and the relation between 3D partition functions and 4D superconformal indices.
Noncommutative Dipole Field Theories
K. Dasgupta; M. M. Sheikh-Jabbari
2002-02-05T23:59:59.000Z
Assigning an intrinsic constant dipole moment to any field, we present a new kind of associative star product, the dipole star product, which was first introduced in [hep-th/0008030]. We develop the mathematics necessary to study the corresponding noncommutative dipole field theories. These theories are sensible non-local field theories with no IR/UV mixing. In addition we discuss that the Lorentz symmetry in these theories is ``softly'' broken and in some particular cases the CP (and even CPT) violation in these theories may become observable. We show that a non-trivial dipole extension of N=4, D=4 gauge theories can only be obtained if we break the SU(4) R (and hence super)-symmetry. Such noncommutative dipole extensions, which in the maximal supersymmetric cases are N=2 gauge theories with matter, can be embedded in string theory as the theories on D3-branes probing a smooth Taub-NUT space with three form fluxes turned on or alternatively by probing a space with R-symmetry twists. We show the equivalences between the two approaches and also discuss the M-theory realization.
$S$-duality in Vafa-Witten theory for non-simply laced gauge groups
Siye Wu
2008-02-14T23:59:59.000Z
Vafa-Witten theory is a twisted N=4 supersymmetric gauge theory whose partition functions are the generating functions of the Euler number of instanton moduli spaces. In this paper, we recall quantum gauge theory with discrete electric and magnetic fluxes and review the main results of Vafa-Witten theory when the gauge group is simply laced. Based on the transformations of theta functions and their appearance in the blow-up formulae, we propose explicit transformations of the partition functions under the Hecke group when the gauge group is non-simply laced. We provide various evidences and consistency checks.
Topological Field Theory Amplitudes for $A_{N-1}$ Fibration
Iqbal, Amer; Qureshi, Babar A; Shabbir, Khurram; Shehper, Muhammad A
2015-01-01T23:59:59.000Z
We study the partition function ${\\cal N}=1$ 5D $U(N)$ gauge theory with $g$ adjoint hypermultiplets and show that for massless adjoint hypermultiplets it is equal to the partition function of a two dimensional topological field on a genus $g$ Riemann surface. We describe the topological field theory by its amplitudes associated with cap, propagator and pair of pants. These basic amplitudes are open topological string amplitudes associated with certain Calabi-Yau threefolds in the presence of Lagrangian branes.
Theory and Modeling of Weakly Bound/Physisorbed Materials
by physisorption: CNT, fullerenes, carbon aerogels Doping, Decorating, Charging · Accuracy of Methods: DFT, QMC CNT may have increased absorption3 · Carbon aerogels4 have exhibited 5 wt% for high surface areas, ~1
Lucien Hardy
2013-03-06T23:59:59.000Z
We discuss how to reconstruct quantum theory from operational postulates. In particular, the following postulates are consistent only with for classical probability theory and quantum theory. Logical Sharpness: There is a one-to-one map between pure states and maximal effects such that we get unit probability. This maximal effect does not give probability equal to one for any other pure state. Information Locality: A maximal measurement is effected on a composite system if we perform maximal measurements on each of the components. Tomographic Locality: The state of a composite system can be determined from the statistics collected by making measurements on the components. Permutability: There exists a reversible transformation on any system effecting any given permutation of any given maximal set of distinguishable states for that system. Sturdiness: Filters are non-flattening. To single out quantum theory we need only add any requirement that is inconsistent with classical probability theory and consistent with quantum theory.
Mesoscopic theory for inhomogeneous mixtures
A. Ciach
2010-10-22T23:59:59.000Z
Mesoscopic density functional theory for inhomogeneous mixtures of sperical particles is developed in terms of mesoscopic volume fractions by a systematic coarse-graining procedure starting form microscopic theory. Approximate expressions for the correlation functions and for the grand potential are obtained for weak ordering on mesoscopic length scales. Stability analysis of the disordered phase is performed in mean-field approximation (MF) and beyond. MF shows existence of either a spinodal or a $\\lambda$-surface on the volume-fractions - temperature phase diagram. Separation into homogeneous phases or formation of inhomogeneous distribution of particles occurs on the low-temperature side of the former or the latter surface respectively, depending on both the interaction potentials and the size ratios between particles of different species. Beyond MF the spinodal surface is shifted, and the instability at the $\\lambda$-surface is suppressed by fluctuations. We interpret the $\\lambda$-surface as a borderline between homogeneous and inhomogeneous (containing clusters or other aggregates) structure of the disordered phase. For two-component systems explicit expressions for the MF spinodal and $\\lambda$-surfaces are derived. Examples of interaction potentials of simple form are analyzed in some detail, in order to identify conditions leading to inhomogeneous structures.
Automated Lattice Perturbation Theory
Monahan, Christopher
2014-11-01T23:59:59.000Z
I review recent developments in automated lattice perturbation theory. Starting with an overview of lattice perturbation theory, I focus on the three automation packages currently "on the market": HiPPy/HPsrc, Pastor and PhySyCAl. I highlight some recent applications of these methods, particularly in B physics. In the final section I briefly discuss the related, but distinct, approach of numerical stochastic perturbation theory.
Theory Modeling and Simulation
Shlachter, Jack [Los Alamos National Laboratory
2012-08-23T23:59:59.000Z
Los Alamos has a long history in theory, modeling and simulation. We focus on multidisciplinary teams that tackle complex problems. Theory, modeling and simulation are tools to solve problems just like an NMR spectrometer, a gas chromatograph or an electron microscope. Problems should be used to define the theoretical tools needed and not the other way around. Best results occur when theory and experiments are working together in a team.
Krokhin, Arkadii [Univ. of North Texas, Denton, TX (United States)
2014-04-18T23:59:59.000Z
New applications of the theory of homogenization for heterogeneous metamaterials, in particular for acoustic cloaking and for design and engineering of tunable phononic crystal.
*D. J. Kelleher
2011-09-30T23:59:59.000Z
Spectral Graph Theory. *D. J. Kelleher2. 2Department of Mathematics. University of Connecticut. UConn— SIGMA Seminar — Fall 2011. D. J. Kelleher. Spectral ...
Theory of Relaxor Ferroelectrics
Guzman-Verri, Gian Giacomo
2012-01-01T23:59:59.000Z
Theory of Thermal Neutron Scattering: the Use of Neutronsdetermined from neutron scattering. [39] A symmetry analysis9, 10] Only recently neutron scattering experiments have
Constructive Quantum Field Theory
Giovanni Gallavotti
2005-10-04T23:59:59.000Z
A review of the renormalization group approach to the proof of non perturbative ultraviolet stability in scalar field theories in dimension d=2,3.
Bevir, Mark
2013-01-01T23:59:59.000Z
Trentmann, “The Modern Genealogy of the Consumer: Meanings,2007. Biebricher, T. “Genealogy and Governmentality. ”of Political Theory: The Genealogy of an American Vocation.