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
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
Uncertainty Quantification for Nuclear Density Functional Theory...
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Uncertainty Quantification for Nuclear Density Functional Theory and Information Content of New Measurements Citation Details In-Document Search This content will become publicly...
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.
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
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.
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.
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...
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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 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.
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.
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
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.
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.
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:...
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 \
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 ...
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...
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.
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 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.
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.
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.
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.
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.
Density functional theory of freezing: Analysis of crystal density
Laird, Brian Bostian; McCoy, John D.; Haymet, A. D. J.
1987-09-01T23:59:59.000Z
the natural variables are temperature, chemical potential, and volume. The pressures are set equal by varying the liquid density until the grand thermodynamic potential, flO = - pV /kT, of the solid phase equals that of the liquid phase. It should... with temperature T, volume V, and chemical potential J.L. The particles interact via a potential energy U(rl, ... ,rn ) and feel an external single particle potential ifJ (r). Defining a dimen sionless single particle effective potential by u (r) = pJ.L - pif...
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.
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.
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.
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.
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...
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.
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.
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.
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.
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
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.
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.
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.
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
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
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
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.
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 ...
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.
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
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.
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.
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.
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.
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
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
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.
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.
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.
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
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.
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 ...
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.
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
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.
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.
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.
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.
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
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
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.
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
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.
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.
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.
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...
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...
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.
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.
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.
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.
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.
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...
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
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
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...
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.
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.
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.
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
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.
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.
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.
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
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
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
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.
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
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.
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.
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.
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.
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 ...
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.
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.
Laboratory Density Functionals
B. G. Giraud
2007-07-26T23:59:59.000Z
We compare several definitions of the density of a self-bound system, such as a nucleus, in relation with its center-of-mass zero-point motion. A trivial deconvolution relates the internal density to the density defined in the laboratory frame. This result is useful for the practical definition of density functionals.
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.
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.
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.
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...
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 ...
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...
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.
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
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...
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.
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.
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
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.
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
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.
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...
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
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.
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.
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.
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.
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.
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.
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...
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
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.
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
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.
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.
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 ...
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.
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
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.
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 ...
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.
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.
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.
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.
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 ...
Chu, Shih-I
2013-01-01T23:59:59.000Z
-correlation potential which proved accurate in calculations of unperturbed electronic structure of Ar. Calculations is, not including dynamic response of the electron density) differ significantly from those obtained [24]. Electronic structure of atoms and molecules can be encoded in the HHG signal; the latter may
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
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
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.
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.
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.
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.
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.
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.
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.
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.
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
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.
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.
Building a Universal Nuclear Energy Density Functional
Carlson, Joe A. [Michigan State University; Furnstahl, Dick; Horoi, Mihai; Lust, Rusty; Nazaewicc, Witek; Ng, Esmond; Thompson, Ian; Vary, James
2012-12-30T23:59:59.000Z
During the period of Dec. 1 2006 – 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.
Nuclear Energy Density Functionals Constrained by Low-Energy QCD
Dario Vretenar
2008-02-06T23:59:59.000Z
A microscopic framework of nuclear energy density functionals is reviewed, which establishes a direct relation between low-energy QCD and nuclear structure, synthesizing effective field theory methods and principles of density functional theory. Guided by two closely related features of QCD in the low-energy limit: a) in-medium changes of vacuum condensates, and b) spontaneous breaking of chiral symmetry; a relativistic energy density functional is developed and applied in studies of ground-state properties of spherical and deformed nuclei.
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...
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.
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
Javier, Alnald Caintic
2013-08-05T23:59:59.000Z
(111)-(3 x 3)-C6H6 adlayer at 0.3 V. Bias voltage: 100 mV; tunneling current: 30 nA??. 68 Figure 25 High-resolution EC-STM image of the Pd(111)-c(2?3 x 3)-rect-C6H6 adlattice at 0.55 V. Bias voltage: 120 mV; tunneling current: 30 nA?.. 69... potential (?) of a system of interacting electrons is determined uniquely by the ground-state electron density (?) and thus suggest that all properties of a system derived from solving the Schr?dinger equation can be determined using ? [68]. Since...
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
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.
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.
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.
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.
Computing spectral densities in finite temperature field theory
Jeon, S. (Physics Department FM-15, University of Washington, Seattle, Washington 98195 (United States))
1993-05-15T23:59:59.000Z
Convenient Cutkosky-like diagrammatic rules for computing the spectral densities of arbitrary two-point correlation functions in finite temperature field theory are derived. The approach is based on an explicit analytic continuation of imaginary-time Feynman diagrams. The application of this method to the perturbative evaluation of transport coefficients is briefly discussed.
Effective Field Theory and Finite Density Systems
R. J. Furnstahl; G. Rupak; T. Schaefer
2008-01-04T23:59:59.000Z
This review gives an overview of effective field theory (EFT) as applied at finite density, with a focus on nuclear many-body systems. Uniform systems with short-range interactions illustrate the ingredients and virtues of many-body EFT and then the varied frontiers of EFT for finite nuclei and nuclear matter are surveyed.
Instabilities in the Nuclear Energy Density Functional
M. Kortelainen; T. Lesinski
2010-02-05T23:59:59.000Z
In the field of Energy Density Functionals (EDF) used in nuclear structure and dynamics, one of the unsolved issues is the stability of the functional. Numerical issues aside, some EDFs are unstable with respect to particular perturbations of the nuclear ground-state density. The aim of this contribution is to raise questions about the origin and nature of these instabilities, the techniques used to diagnose and prevent them, and the domain of density functions in which one should expect a nuclear EDF to be stable.
The density of states approach for the simulation of finite density quantum field theories
K. Langfeld; B. Lucini; A. Rago; R. Pellegrini; L. Bongiovanni
2015-03-02T23:59:59.000Z
Finite density quantum field theories have evaded first principle Monte-Carlo simulations due to the notorious sign-problem. The partition function of such theories appears as the Fourier transform of the generalised density-of-states, which is the probability distribution of the imaginary part of the action. With the advent of Wang-Landau type simulation techniques and recent advances, the density-of-states can be calculated over many hundreds of orders of magnitude. Current research addresses the question whether the achieved precision is high enough to reliably extract the finite density partition function, which is exponentially suppressed with the volume. In my talk, I review the state-of-play for the high precision calculations of the density-of-states as well as the recent progress for obtaining reliable results from highly oscillating integrals. I will review recent progress for the $Z_3$ quantum field theory for which results can be obtained from the simulation of the dual theory, which appears to free of a sign problem.
The density of states approach for the simulation of finite density quantum field theories
Langfeld, K; Rago, A; Pellegrini, R; Bongiovanni, L
2015-01-01T23:59:59.000Z
Finite density quantum field theories have evaded first principle Monte-Carlo simulations due to the notorious sign-problem. The partition function of such theories appears as the Fourier transform of the generalised density-of-states, which is the probability distribution of the imaginary part of the action. With the advent of Wang-Landau type simulation techniques and recent advances, the density-of-states can be calculated over many hundreds of orders of magnitude. Current research addresses the question whether the achieved precision is high enough to reliably extract the finite density partition function, which is exponentially suppressed with the volume. In my talk, I review the state-of-play for the high precision calculations of the density-of-states as well as the recent progress for obtaining reliable results from highly oscillating integrals. I will review recent progress for the $Z_3$ quantum field theory for which results can be obtained from the simulation of the dual theory, which appears to fr...
Stretched hydrogen molecule from a constrained-search density-functional perspective
Valone, Steven M [Los Alamos National Laboratory; Levy, Mel [DIKE UNIV.
2009-01-01T23:59:59.000Z
Constrained-search density functional theory gives valuable insights into the fundamentals of density functional theory. It provides exact results and bounds on the ground- and excited-state density functionals. An important advantage of the theory is that it gives guidance in the construction of functionals. Here they engage constrained search theory to explore issues associated with the functional behavior of 'stretched bonds' in molecular hydrogen. A constrained search is performed with familiar valence bond wavefunctions ordinarily used to describe molecular hydrogen. The effective, one-electron hamiltonian is computed and compared to the corresponding uncorrelated, Hartree-Fock effective hamiltonian. Analysis of the functional suggests the need to construct different functionals for the same density and to allow a competition among these functions. As a result the correlation energy functional is composed explicitly of energy gaps from the different functionals.
Nuclear Energy Density Functionals: What do we really know?
Bulgac, Aurel; Jin, Shi
2015-01-01T23:59:59.000Z
We present the simplest nuclear energy density functional (NEDF) to date, determined by only 4 significant phenomenological parameters, yet capable of fitting measured nuclear masses with better accuracy than the Bethe-Weizs\\"acker mass formula, while also describing density structures (charge radii, neutron skins etc.) and time-dependent phenomena (induced fission, giant resonances, low energy nuclear collisions, etc.). The 4 significant parameters are necessary to describe bulk nuclear properties (binding energies and charge radii); an additional 2 to 3 parameters have little influence on the bulk nuclear properties, but allow independent control of the density dependence of the symmetry energy and isovector excitations, in particular the Thomas-Reiche-Kuhn sum rule. This Hohenberg-Kohn-style of density functional theory successfully realizes Weizs\\"acker's ideas and provides a computationally tractable model for a variety of static nuclear properties and dynamics, from finite nuclei to neutron stars, where...
BUILDING A UNIVERSAL NUCLEAR ENERGY DENSITY FUNCTIONAL (UNEDF...
Office of Scientific and Technical Information (OSTI)
Technical Report: BUILDING A UNIVERSAL NUCLEAR ENERGY DENSITY FUNCTIONAL (UNEDF) Citation Details In-Document Search Title: BUILDING A UNIVERSAL NUCLEAR ENERGY DENSITY FUNCTIONAL...
Nuclear Physics A 770 (2006) 131 Relativistic nuclear energy density functional
Weise, Wolfram
2006-01-01T23:59:59.000Z
Nuclear Physics A 770 (2006) 131 Relativistic nuclear energy density functional constrained by low 10 February 2006 Available online 3 March 2006 Abstract A relativistic nuclear energy density Keywords: Relativistic mean field; Density functional theory; Nuclear structure; Chiral dynamics; QCD sum
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 ...
Time-dependent density-functional studies on strength functions in neutron-rich nuclei
Shuichiro Ebata; Tsunenori Inakura; Takashi Nakatsukasa
2013-02-08T23:59:59.000Z
The electric dipole (E1) strength functions have been systematically calculated based on the time-dependent density functional theory (TDDFT), using the finite amplitude method and the real-time approach to the TDDFT with pairing correlations. The low-energy E1 strengths in neutron-rich isotopes show peculiar behaviors, such as sudden enhancement and reduction, as functions of the neutron numbers.They seem to be due to the interplay between the neutron shell effect and the deformation effect.
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.
Irradiation-Induced Magnetism in Graphite: A Density Functional Study P. O. Lehtinen,1
Krasheninnikov, Arkady V.
Irradiation-Induced Magnetism in Graphite: A Density Functional Study P. O. Lehtinen,1 A. S. Foster October 2004) Recent experiments indicate that proton irradiation triggers ferromagnetism in originally the origin of irradiation-induced magnetism, we have performed spin-polarized density functional theory
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.
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.
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
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...
Density Functional Theory (DFT) Simulated Annealing (SA)
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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.
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.
Moyal's Characteristic Function, the Density Matrix and von Neumann's Idempotent
Basil J. Hiley
2014-08-25T23:59:59.000Z
In the Wigner-Moyal approach to quantum mechanics, we show that Moyal's starting point, the characteristic function $M(\\tau,\\theta)=\\int \\psi^{*}(x)e^{i(\\tau {\\hat p}+\\theta{\\hat x})}\\psi(x)dx$, is essentially the primitive idempotent used by von Neumann in his classic paper "Die Eindeutigkeit der Schr\\"odingerschen Operatoren". This paper provides the original proof of the Stone-von Neumann equation. Thus the mathematical structure Moyal develops is simply a re-expression of what is at the heart of quantum mechanics and reproduces exactly the results of the quantum formalism. The "distribution function" $F(X,P,t)$ is simply the quantum mechanical density matrix expressed in an $( X,P)$-representation, where $X$ and $P$ are the mean co-ordinates of a cell structure in phase space. The whole approach therefore clearly has little to do with classical statistical theories but is a consequence of a non-commutative nature of the theory.
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)
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.
M. Oettel; S. Goerig; A. Haertel; H. Loewen; M. Radu; T. Schilling
2010-09-03T23:59:59.000Z
We perform a comparative study of the free energies and the density distributions in hard sphere crystals using Monte Carlo simulations and density functional theory (employing Fundamental Measure functionals). Using a recently introduced technique (Schilling and Schmid, J. Chem. Phys 131, 231102 (2009)) we obtain crystal free energies to a high precision. The free energies from Fundamental Measure theory are in good agreement with the simulation results and demonstrate the applicability of these functionals to the treatment of other problems involving crystallization. The agreement between FMT and simulations on the level of the free energies is also reflected in the density distributions around single lattice sites. Overall, the peak widths and anisotropy signs for different lattice directions agree, however, it is found that Fundamental Measure theory gives slightly narrower peaks with more anisotropy than seen in the simulations. Among the three types of Fundamental Measure functionals studied, only the White Bear II functional (Hansen-Goos and Roth, J. Phys.: Condens. Matter 18, 8413 (2006)) exhibits sensible results for the equilibrium vacancy concentration and a physical behavior of the chemical potential in crystals constrained by a fixed vacancy concentration.
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.
The Hubbard Dimer: A density functional case study of a many-body problem
Carrascal, Diego; Smith, Justin C; Burke, Kieron
2015-01-01T23:59:59.000Z
This review explains the relationship between density functional theory and strongly correlated models using the simplest possible example, the two-site Hubbard model. The relationship to traditional quantum chemistry is included. Even in this elementary example, where the exact ground-state energy and site occupations can be found analytically, there is much to be explained in terms of the underlying logic and aims of Density Functional Theory. Although the usual solution is analytic, the density functional is given only implicitly. We overcome this difficulty using the Levy-Lieb construction to create a parametrization of the exact function with negligible errors. The symmetric case is most commonly studied, but we find a rich variation in behavior by including asymmetry, as strong correlation physics vies with charge-transfer effects. We explore the behavior of the gap and the many-body Green's function, demonstrating the `failure' of the Kohn-Sham method to reproduce the fundamental gap. We perform benchm...
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
Density functional and neutron diffraction studies of lithium polymer electrolytes.
Baboul, A. G.
1998-06-26T23:59:59.000Z
The structure of PEO doped with lithium perchlorate has been determined using neutron diffraction on protonated and deuterated samples. The experiments were done in the liquid state. Preliminary analysis indicates the Li-O distance is about 2.0 {angstrom}. The geometries of a series of gas phase lithium salts [LiCF{sub 3}SO{sub 3}, Li(CF{sub 3}SO{sub 2}){sub 2}N, Li(CF{sub 3}SO{sub 2}){sub 2}CH, LiClO{sub 4}, LiPF{sub 6}, LiAsF{sub 6}] used in polymer electrolytes have been optimized at B3LYP/6-31G(d) density functional level of theory. All local minima have been identified. For the triflate, imide, methanide, and perchlorate anions, the lithium cation is coordinated to two oxygens and have binding energies of ca 141 kcal/mol at the B3LYP/6-311+G(3df,2p)/B3LYP/6-31G* level of theory. For the hexafluoroarsenate and hexafluorophosphate the lithium cation is coordinated to three oxygens and have binding energies of ca. 136 kcal/mol.
Lutsker, Vitalij; Niehaus, Thomas A
2015-01-01T23:59:59.000Z
Bridging the gap between first principles methods and empirical schemes, the density functional based tight-binding method (DFTB) has become a versatile tool in predictive atomistic simulations over the past years. One of the major restrictions of this method is the limitation to local or gradient corrected exchange-correlation functionals. This excludes the important class of hybrid or long-range corrected functionals, which are advantageous in thermochemistry, as well as in the computation of vibrational, photoelectron and optical spectra. The present work provides a detailed account of the implementation of DFTB for a long-range corrected functional in generalized Kohn-Sham theory. We apply the method to a set of organic molecules and compare ionization potentials and electron affinities with the original DFTB method and higher level theory. The new scheme cures the significant overpolarization in electric fields found for local DFTB, which parallels the functional dependence in first principles density fu...
Roberto Peverati; Donald G. Truhlar
2013-09-06T23:59:59.000Z
Kohn-Sham density functional theory is in principle an exact formulation of quantum mechanical electronic structure theory, but in practice we have to rely on approximate exchange-correlation (xc) functionals. The objective of our work has been to design an xc functional with broad accuracy across as wide an expanse of chemistry and physics as possible, leading-as a long-range goal-to a functional with good accuracy for all problems, i.e., a universal functional. To guide our path toward that goal and to measure our progress, we have developed-building on earlier work in our group-a set of databases of reference data for a variety of energetic and structural properties in chemistry and physics. These databases include energies of molecular processes such as atomization, complexation, proton addition, and ionization; they also include molecular geometries and solid-state lattice constants, chemical reaction barrier heights, and cohesive energies and band gaps of solids. For the present paper we gather many of these databases into four comprehensive databases, two with 384 energetic data for chemistry and solid-state physics and another two with 68 structural data for chemistry and solid-state physics, and we test 2 wave function methods and 77 density functionals (12 Minnesota meta functionals and 65 others) in a consistent way across this same broad set of data. We especially highlight the Minnesota density functionals, but the results have broader implications in that one may see the successes and failures of many kinds of density functionals when they are all applied to the same data. Therefore the results provide a status report on the quest for a universal functional.
Density-matrix functionals for pairing in mesoscopic superconductors
Denis Lacroix; Guillaume Hupin
2010-09-03T23:59:59.000Z
A functional theory based on single-particle occupation numbers is developed for pairing. This functional, that generalizes the BCS approach, directly incorporates corrections due to particle number conservation. The functional is benchmarked with the pairing Hamiltonian and reproduces perfectly the energy for any particle number and coupling.
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.
Song, Xueyu
Calculations of free energies in liquid and solid phases: Fundamental measure density, a theoretical description of the free energies and correlation functions of hard-sphere (HS) liquid and solid-Chandler-Andersen perturbation theory, free energies of liquid and solid phases with many interaction potentials can be obtained
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.
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.
Kinetic Theory for Binary Granular Mixtures at Low-Density
Vicente Garzo
2007-04-10T23:59:59.000Z
Many features of granular media can be modelled as a fluid of hard spheres with {\\em inelastic} collisions. Under rapid flow conditions, the macroscopic behavior of grains can be described through hydrodynamic equations. At low-density, a fundamental basis for the derivation of the hydrodynamic equations and explicit expressions for the transport coefficients appearing in them is provided by the Boltzmann kinetic theory conveniently modified to account for inelastic binary collisions. The goal of this chapter is to give an overview of the recent advances made for binary granular gases by using kinetic theory tools. Some of the results presented here cover aspects such as transport properties, energy nonequipartition, instabilities, segregation or mixing, non-Newtonian behavior, .... In addition, comparison of the analytical results with those obtained from Monte Carlo and molecular dynamics simulations is also carried out, showing the reliability of kinetic theory to describe granular flows even for strong dissipation.
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
Probability distribution functions in the finite density lattice QCD
S. Ejiri; Y. Nakagawa; S. Aoki; K. Kanaya; H. Saito; T. Hatsuda; H. Ohno; T. Umeda
2012-12-04T23:59:59.000Z
We study the phase structure of QCD at high temperature and density by lattice QCD simulations adopting a histogram method. We try to solve the problems which arise in the numerical study of the finite density QCD, focusing on the probability distribution function (histogram). As a first step, we investigate the quark mass dependence and the chemical potential dependence of the probability distribution function as a function of the Polyakov loop when all quark masses are sufficiently large, and study the properties of the distribution function. The effect from the complex phase of the quark determinant is estimated explicitly. The shape of the distribution function changes with the quark mass and the chemical potential. Through the shape of the distribution, the critical surface which separates the first order transition and crossover regions in the heavy quark region is determined for the 2+1-flavor case.
Relativistic Nuclear Energy Density Functionals: adjusting parameters to binding energies
T. Niksic; D. Vretenar; P. Ring
2008-09-08T23:59:59.000Z
We study a particular class of relativistic nuclear energy density functionals in which only nucleon degrees of freedom are explicitly used in the construction of effective interaction terms. Short-distance (high-momentum) correlations, as well as intermediate and long-range dynamics, are encoded in the medium (nucleon density) dependence of the strength functionals of an effective interaction Lagrangian. Guided by the density dependence of microscopic nucleon self-energies in nuclear matter, a phenomenological ansatz for the density-dependent coupling functionals is accurately determined in self-consistent mean-field calculations of binding energies of a large set of axially deformed nuclei. The relationship between the nuclear matter volume, surface and symmetry energies, and the corresponding predictions for nuclear masses is analyzed in detail. The resulting best-fit parametrization of the nuclear energy density functional is further tested in calculations of properties of spherical and deformed medium-heavy and heavy nuclei, including binding energies, charge radii, deformation parameters, neutron skin thickness, and excitation energies of giant multipole resonances.
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. ...
Binding Energies in Benzene Dimers: Nonlocal Density Functional Calculations
Aaron Puzder; Maxime Dion; David C. Langreth
2005-09-15T23:59:59.000Z
The interaction energy and minimum energy structure for different geometries of the benzene dimer has been calculated using the recently developed nonlocal correlation energy functional for calculating dispersion interactions. The comparison of this straightforward and relatively quick density functional based method with recent calculations can elucidate how the former, quicker method might be exploited in larger more complicated biological, organic, aromatic, and even infinite systems such as molecules physisorbed on surfaces, and van der Waals crystals.
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.
Calibrating Speed-Density Functions for ff SMesoscopic Traffic Simulation
Bertini, Robert L.
. (1999), Tavana & Mahmassani (2000), Wang & Papageorgiou (2005), Antoniou et al. (2007) #12;Case Studies) supply #12;Case Studies (contd.) · DynaMIT speed-density function form · Performance measures ( )= - S i pointsdataofnumber speed)(count,simulated : : S iy #12;Case Studies (contd.) · Methodology Large
Probability Density Function Estimation Using Orthogonal Forward Regression
Chen, Sheng
Probability Density Function Estimation Using Orthogonal Forward Regression S. Chen, X. Hong and C estimation is formulated as a regression problem and the orthogonal forward regression tech- nique is adopted procedure. Two examples are used to demonstrate the ability of this regression- based approach
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.
Attarian Shandiz, M., E-mail: mohammad.attarianshandiz@mail.mcgill.ca; Gauvin, R. [Department of Materials Engineering, McGill University, Montreal, Quebec H3A 0C5 (Canada)
2014-10-28T23:59:59.000Z
The temperature and pressure dependency of the volume plasmon energy of solids was investigated by density functional theory calculations. The volume change of crystal is the major factor responsible for the variation of valence electron density and plasmon energy in the free electron model. Hence, to introduce the effect of temperature and pressure for the density functional theory calculations of plasmon energy, the temperature and pressure dependency of lattice parameter was used. Also, by combination of the free electron model and the equation of state based on the pseudo-spinodal approach, the temperature and pressure dependency of the plasmon energy was modeled. The suggested model is in good agreement with the results of density functional theory calculations and available experimental data for elements with the free electron behavior.
Understanding Kernel Ridge Regression: Common behaviors from simple functions to density functionals
Vu, Kevin; Li, Li; Rupp, Matthias; Chen, Brandon F; Khelif, Tarek; Müller, Klaus-Robert; Burke, Kieron
2015-01-01T23:59:59.000Z
Accurate approximations to density functionals have recently been obtained via machine learning (ML). By applying ML to a simple function of one variable without any random sampling, we extract the qualitative dependence of errors on hyperparameters. We find universal features of the behavior in extreme limits, including both very small and very large length scales, and the noise-free limit. We show how such features arise in ML models of density functionals.
Ab Initio Derivation of Model Energy Density Functionals
Dobaczewski, J
2015-01-01T23:59:59.000Z
I propose a simple and manageable method that allows for deriving coupling constants of model energy density functionals (EDFs) directly from ab initio calculations performed for finite fermion systems. A proof-of-principle application allows for linking properties of finite nuclei, determined by using the nuclear nonlocal Gogny functional, to the coupling constants of the quasilocal Skyrme functional. The method does not rely on properties of infinite fermion systems but on the ab initio calculations in finite systems. It also allows for quantifying merits of different model EDFs in describing the ab initio results.
Ab Initio Derivation of Model Energy Density Functionals
J. Dobaczewski
2015-07-07T23:59:59.000Z
I propose a simple and manageable method that allows for deriving coupling constants of model energy density functionals (EDFs) directly from ab initio calculations performed for finite fermion systems. A proof-of-principle application allows for linking properties of finite nuclei, determined by using the nuclear nonlocal Gogny functional, to the coupling constants of the quasilocal Skyrme functional. The method does not rely on properties of infinite fermion systems but on the ab initio calculations in finite systems. It also allows for quantifying merits of different model EDFs in describing the ab initio results.
Measuring the entanglement of analogue Hawking radiation by the density-density correlation function
Steinhauer, Jeff
2015-01-01T23:59:59.000Z
We theoretically study the entanglement of Hawking radiation emitted by an analogue black hole. We find that this entanglement can be measured by the experimentally accessible density-density correlation function, which only requires standard imaging techniques. It is seen that the high energy tail of the distribution of Hawking radiation should be entangled, whereas the low energy part is not. This confirms a previous numerical study. The full Peres-Horodecki criterion is considered, but a significant simplification is found in the stationary, homogeneous case. Our method applies to systems which are sufficiently cold that the thermal phonons can be neglected.
Generalized second law at linear order for actions that are functions of Lovelock densities
Sudipta Sarkar; Aron C. Wall
2015-05-19T23:59:59.000Z
In this article we consider the second law of black holes (and other causal horizons) in theories where the gravitational action is an arbitrary function of the Lovelock densities. We show that there exists an entropy which increases locally, for linearized perturbations to regular Killing horizons. In addition to a classical increase theorem, we also prove a generalized second law for semiclassical, minimally-coupled matter fields.
New theory of superconductivity. Method of equilibrium density matrix
Boris Bondarev
2013-09-22T23:59:59.000Z
A new variational method for studying the equilibrium states of an interacting particles system has been proposed. The statistical description of the system is realized by means of a density matrix. This method is used for description of conduction electrons in metals. An integral equation for the electron distribution function over wave vectors has been obtained. The solutions of this equation have been found for those cases where the single-particle Hamiltonian and the electron interaction Hamiltonian can be approximated by a quite simple expression. It is shown that the distribution function at temperatures below the critical value possesses previously unknown features which allow to explain the superconductivity of metals and presence of a gap in the energy spectrum of superconducting electrons.
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...
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...
Measuring the Density Fluctuation From the Cluster Gas Mass Function
Kazuhiro Shimasaku
1997-01-27T23:59:59.000Z
We investigate the gas mass function of clusters of galaxies to measure the density fluctuation spectrum on cluster scales. The baryon abundance confined in rich clusters is computed from the gas mass function and compared with the mean baryon density in the universe which is predicted by the Big Bang Nucleosynthesis. This baryon fraction and the slope of the gas mass function put constraints on $\\sigma_8$, the rms linear fluctuation on scales of $8h^{-1}\\Mpc$, and the slope of the fluctuation spectrum, where $h$ is the Hubble constant in units of 100 $\\kms \\oMpc$. We find $\\sigma_8 = 0.80 \\pm 0.15$ and $n \\sim -1.5$ for $0.5 \\le h \\le 0.8$, where we assume that the density spectrum is approximated by a power law on cluster scales: $\\sigma(r) \\propto r^{-{3+n\\over{2}}}$. Our value of $\\sigma_8$ is independent of the density parameter, $\\Omega_0$, and thus we can estimate $\\Omega_0$ by combining $\\sigma_8$ obtained in this study with those from $\\Omega_0$-dependent analyses to date. We find that $\\sigma_8(\\Omega_0)$ derived from the cluster abundance such as the temperature function gives $\\Omega_0 \\sim 0.5$ while $\\sigma_8(\\Omega_0)$ measured from the peculiar velocity field of galaxies gives $\\Omega_0 \\sim 0.2-1$, depending on the technique used to analyze peculiar velocity data. Constraints are also derived for open, spatially flat, and tilted Cold Dark Matter models and for Cold + Hot Dark Matter models.
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
Peverati, Roberto
2012-01-01T23:59:59.000Z
Kohn-Sham density functional theory is in principle an exact formulation of quantum mechanical electronic structure theory, but in practice we have to rely on approximate exchange-correlation (xc) functionals. The objective of our work has been to design an xc functional with broad accuracy across as wide an expanse of chemistry and physics as possible, leading-as a long-range goal-to a functional with good accuracy for all problems, i.e., a universal functional. To guide our path toward that goal and to measure our progress, we have developed-building on earlier work in our group-a set of databases of reference data for a variety of energetic and structural properties in chemistry and physics. These databases include energies of molecular processes such as atomization, complexation, proton addition, and ionization; they also include molecular geometries and solid-state lattice constants, chemical reaction barrier heights, and cohesive energies and band gaps of solids. For the present paper we gather many of ...
Level densities of nickel isotopes: microscopic theory versus experiment
M. Bonett-Matiz; Abhishek Mukherjee; Y. Alhassid
2013-05-01T23:59:59.000Z
We apply a spin-projection method to calculate microscopically the level densities of a family of nickel isotopes $^{59-64}$Ni using the shell model Monte Carlo approach in the complete $pfg_{9/2}$ shell. Accurate ground-state energies of the odd-mass nickel isotopes, required for the determination of excitation energies, are determined using the Green's function method recently introduced to circumvent the odd particle-number sign problem. Our results are in excellent agreement with recent measurements based on proton evaporation spectra and with level counting data at low excitation energies. We also compare our results with neutron resonance data, assuming equilibration of parity and a spin-cutoff model for the spin distribution at the neutron binding energy, and find good agreement with the exception of $^{63}$Ni.
Loops and Power Counting in the High Density Effective Field Theory
Thomas Schaefer
2003-10-15T23:59:59.000Z
We introduce the high density effective theory of QCD. We discuss, in particular, the problem of developing a consistent power counting scheme.
Power-law tails in probability density functions of molecular cloud column density
Brunt, Chris
2015-01-01T23:59:59.000Z
Power-law tails are often seen in probability density functions (PDFs) of molecular cloud column densities, and have been attributed to the effect of gravity. We show that extinction PDFs of a sample of five molecular clouds obtained at a few tenths of a parsec resolution, probing extinctions up to A$_{{\\mathrm{V}}}$ $\\sim$ 10 magnitudes, are very well described by lognormal functions provided that the field selection is tightly constrained to the cold, molecular zone and that noise and foreground contamination are appropriately accounted for. In general, field selections that incorporate warm, diffuse material in addition to the cold, molecular material will display apparent core+tail PDFs. The apparent tail, however, is best understood as the high extinction part of a lognormal PDF arising from the cold, molecular part of the cloud. We also describe the effects of noise and foreground/background contamination on the PDF structure, and show that these can, if not appropriately accounted for, induce spurious ...
Gong, Xingao
A density-functional study of small titanium clusters S. H. Wei Department of Physics, Xiangtan-functional theory with a local spin density approximation. We find that the inner-shells (3s3p) of the titanium atom of titanium clusters, Ti7 is found to be a magic cluster, which is in good agreement with the experimental
Building a Universal Nuclear Energy Density Functional (UNEDF): SciDAC-2 Project
Carlson, Joe; Furnstahl, Dick; Lusk, Rusty; Nazarewicz, Witek; Ng, Esmond; Thompson, Ian; Vary, James
2012-06-30T23:59:59.000Z
An understanding of the properties of atomic nuclei is crucial for a complete nuclear theory, for element formation, for properties of stars, and for present and future energy and defense applications. During the period of Dec. 1, 2006 - 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; and third, to apply the validated theory to properties of interest that cannot be measured, in particular the properties needed for reaction theory.
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...
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...
Theory and Computation | Center for Functional Nanomaterials
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George, Steven C.
Short Communication Automated computation of functional vascular density using laser speckle Laser Institute and Medical Clinic, University of California, Irvine, CA 92697, USA c Edwards: Laser speckle imaging Functional vascular density Dorsal window chamber Blood flow We report
Dipole polarizability of 120Sn and nuclear energy density functionals
T. Hashimoto; A. M. Krumbholz; P. -G. Reinhard; A. Tamii; P. von Neumann-Cosel; T. Adachi; N. Aoi; C. A. Bertulani; H. Fujita; Y. Fujita; E. Ganio?lu; K. Hatanaka; C. Iwamoto; T. Kawabata; N. T. Khai; A. Krugmann; D. Martin; H. Matsubara; K. Miki; R. Neveling; H. Okamura; H. J. Ong; I. Poltoratska; V. Yu. Ponomarev; A. Richter; H. Sakaguchi; Y. Shimbara; Y. Shimizu; J. Simonis; F. D. Smit; G. Süsoy; J. H. Thies; T. Suzuki; M. Yosoi; J. Zenihiro
2015-03-28T23:59:59.000Z
The electric dipole strength distribution in 120Sn between 5 and 22 MeV has been determined at RCNP Osaka from a polarization transfer analysis of proton inelastic scattering at E_0 = 295 MeV and forward angles including 0{\\deg}. Combined with photoabsorption data an electric dipole polarizability alpha_D(120Sn) = 8.93(36) fm^3 is extracted. The correlation of this value with alpha_D for 208Pb serves as a test of energy density functionals (EDFs). The majority of models based on Skyrme interactions can describe the data while relativistic approaches fail. The accuracy of the experimental results provides important constraints on the static isovector properties of EDFs used to predict symmetry energy parameters and the neutron skin thickness of nuclei.
Cohen, Doron
of the survival probability is manifestly related to the parametric theory of the local density of states LDOS necessitates a generalization of the theory regarding survival probability 11 . In Sec. III we re- mindQuantum irreversibility, perturbation independent decay, and the parametric theory of the local
Zhang, Ping; Zhao, Xian-Geng
2010-01-01T23:59:59.000Z
Plutonium dioxide is of high technological importance in nuclear fuel cycle and is particularly crucial in long-term storage of Pu-based radioactive waste. Using first-principles density-functional theory, in this paper we systematically study the structural, electronic, mechanical, thermodynamic properties, and pressure induced structural transition of PuO$_{2}$. To properly describe the strong correlation in the Pu $5f$ electrons, the local density approximation$+U$ and the generalized gradient approximation$+U$ theoretical formalisms have been employed. We optimize the $U$ parameter in calculating the total energy, lattice parameters, and bulk modulus at the nonmagnetic, ferromagnetic, and antiferromagnetic configurations for both ground state fluorite structure and high pressure cotunnite structure. The best agreement with experiments is obtained by tuning the effective Hubbard parameter $U$ at around 4 eV within the LDA$+U$ approach. After carefully testing the validity of the ground state, we further in...
Mao, James X.; Lee, Anita S.; Kitchin, John R.; Nulwala, Hunaid B; Luebke, David R.; Damodaran, Krishnan
2013-04-24T23:59:59.000Z
Density Functional Theory is used to investigate a weakly coordinating room-temperature ionic liquid, 1-ethyl-3-methyl imidazolium tetracyanoborate ([Emim]{sup +}[TCB]{sup -}). Four locally stable conformers of the ion pair were located. Atoms-in-molecules (AIM) and electron density analysis indicated the existence of several hydrogen bonds. Further investigation through the Natural Bond Orbital (NBO) and Natural Energy Decomposition Analysis (NEDA) calculations provided insight into the origin of interactions in the [Emim]{sup +}[TCB]{sup -} ion pair. Strength of molecular interactions in the ionic liquid was correlated with frequency shifts of the characteristic vibrations of the ion pair. Harmonic vibrations of the ion pair were also compared with the experimental Raman and Infrared spectra. Vibrational frequencies were assigned by visualizing displacements of atoms around their equilibrium positions and through Potential Energy Distribution (PED) analysis.
Cosmic density and velocity fields in Lagrangian perturbation theory
Mikel Susperregi; Thomas Buchert
1997-08-04T23:59:59.000Z
A first- and second-order relation between cosmic density and peculiar-velocity fields is presented. The calculation is purely Lagrangian and it is derived using the second-order solutions of the Lagrange-Newton system obtained by Buchert & Ehlers. The procedure is applied to two particular solutions given generic initial conditions. In this approach, the continuity equation yields a relation between the over-density and peculiar-velocity fields that automatically satisfies Euler's equation because the orbits are derived from the Lagrange-Newton system. This scheme generalizes some results obtained by Nusser et al. (1991) in the context of the Zel'dovich approximation. As opposed to several other reconstruction schemes, in this approach it is not necessary to truncate the expansion of the Jacobian given by the continuity equation in order to calculate a first- or second-order expression for the density field. In these previous schemes, the density contrast given by (a) the continuity equation and (b) Euler's equation are mutually incompatible. This inconsistency arises as a consequence of an improper handling of Lagrangian and Eulerian coordinates in the analysis. Here, we take into account the fact that an exact calculation of the density is feasible in the Lagrangian picture and therefore an accurate and consistent description is obtained.
Parameterizing deep convection using the assumed probability density function method
Storer, R. L. [Univ. of Wisconsin - Milwaukee, Milwaukee, WI (United States); Griffin, B. M. [Univ. of Wisconsin - Milwaukee, Milwaukee, WI (United States); Höft, J. [Univ. of Wisconsin - Milwaukee, Milwaukee, WI (United States); Weber, J. K. [Univ. of Wisconsin - Milwaukee, Milwaukee, WI (United States); Raut, E. [Univ. of Wisconsin - Milwaukee, Milwaukee, WI (United States); Larson, V. E. [Univ. of Wisconsin - Milwaukee, Milwaukee, WI (United States); Wang, M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)] (ORCID:000000029179228X); Rasch, P. J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
2015-01-01T23:59:59.000Z
Due to their coarse horizontal resolution, present-day climate models must parameterize deep convection. This paper presents single-column simulations of deep convection using a probability density function (PDF) parameterization. The PDF parameterization predicts the PDF of subgrid variability of turbulence, clouds, and hydrometeors. That variability is interfaced to a prognostic microphysics scheme using a Monte Carlo sampling method.The PDF parameterization is used to simulate tropical deep convection, the transition from shallow to deep convection over land, and midlatitude deep convection. These parameterized single-column simulations are compared with 3-D reference simulations. The agreement is satisfactory except when the convective forcing is weak. The same PDF parameterization is also used to simulate shallow cumulus and stratocumulus layers. The PDF method is sufficiently general to adequately simulate these five deep, shallow, and stratiform cloud cases with a single equation set. This raises hopes that it may be possible in the future, with further refinements at coarse time step and grid spacing, to parameterize all cloud types in a large-scale model in a unified way.
Parameterizing deep convection using the assumed probability density function method
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Storer, R. L.; Griffin, B. M.; Höft, J.; Weber, J. K.; Raut, E.; Larson, V. E.; Wang, M.; Rasch, P. J.
2015-01-01T23:59:59.000Z
Due to their coarse horizontal resolution, present-day climate models must parameterize deep convection. This paper presents single-column simulations of deep convection using a probability density function (PDF) parameterization. The PDF parameterization predicts the PDF of subgrid variability of turbulence, clouds, and hydrometeors. That variability is interfaced to a prognostic microphysics scheme using a Monte Carlo sampling method.The PDF parameterization is used to simulate tropical deep convection, the transition from shallow to deep convection over land, and midlatitude deep convection. These parameterized single-column simulations are compared with 3-D reference simulations. The agreement is satisfactory except when the convective forcing is weak.more »The same PDF parameterization is also used to simulate shallow cumulus and stratocumulus layers. The PDF method is sufficiently general to adequately simulate these five deep, shallow, and stratiform cloud cases with a single equation set. This raises hopes that it may be possible in the future, with further refinements at coarse time step and grid spacing, to parameterize all cloud types in a large-scale model in a unified way.« less
Theory of reduced superfluid density in underdoped cuprate superconductors
Lee, Wei-Cheng; Sinova, Jairo; Burkov, A. A.; Joglekar, Yogesh; MacDonald, A. H.
2008-01-01T23:59:59.000Z
-doping fraction x is very small, superconduc- tivity which appears when x exceeds a minimum value ?0.1, and a maximum Tc in optimally doped materials with x ?0.2. In the underdoped regime, the superconducting tran- sition temperature is limited by phase... accounted for by theories5 in which superconductivity is due to the condensation of Coo- per pairs formed from holes in a doped Mott insulator.6 Theories which start with this view must still explain the fact that ? vanishes at a nonzero value of x...
Tests of second-generation and third-generation density functionals for thermochemical kineticsy
Truhlar, Donald G
Tests of second-generation and third-generation density functionals for thermochemical kineticsy January 2004 We report tests of second- and third-generation density functionals, for pure density of these methods is tested against each other as well as against first- generation methods (BP86, BLYP, PW91, B3PW
NT@UW-15-05 Nuclear Energy Density Functionals: What do we really know?
NT@UW-15-05 Nuclear Energy Density Functionals: What do we really know? Aurel Bulgac,1, Michael Mc2814, USA (Dated: July 1, 2015) We present the simplest nuclear energy density functional (NEDF) to date nuclear properties, but allow independent control of the density dependence of the symmetry energy
Cosmological status of Lagrangian theory of density perturbations
V. Strokov
2006-12-14T23:59:59.000Z
We show that hydrodynamical and field approaches in theory of cosmological scalar perturbations are equivalent for a single medium. We also give relations between notations introduced by V. Lukash, J. Bardeen, J. Bardeen et al. and G. Chibisov and V. Mukhanov.
Quantum Mechanics as a Classical Theory XVI: Positive-Definite Densities
L. S. F. Olavo
1997-04-02T23:59:59.000Z
In this paper we will turn our attention to the problem of obtaining phase-space probability density functions. We will show that it is possible to obtain functions which assume only positive values over all its domain of definition.
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.
Sandia Energy - Statistical Mechanics with Density Functional Theory
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Comments on: Statistical Mechanics with Density Functional Theory Accuracy
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Density Functional Theory-Based Database Development and CALPHAD Automation
Chen, Long-Qing
model usually follows the following sequences: collecting the thermochemical and phase boundary data be provided by first-principles calculation typically include: (I) the enthalpy of formation, the relative
Element orbitals for Kohn-Sham density functional theory
Lin, Lin
2013-01-01T23:59:59.000Z
ranging from 128 atoms to 4394 atoms. ing C and H as sparseranging from 128 atoms to 4394 atoms. The length of thefor 128 atoms to 98.8 a.u. for 4394 atoms. The number of
Thermal Density Functional Theory in Context Aurora Pribram-Jones,
Burke, Kieron
.3. Consequences 4 III.2.4. Extension to degenerate ground states 4 III.3. Kohn-Sham scheme 5 III.3.1. Exchange [1], and the various methods for modeling it are di- verse [2Â4]. The field includes enormous with useful accuracy. It is important to understand, from the outset, that the logic and methodology of KS
Mass Spectrometry and Density Functional Theory Characterizations of DNA Modifications
Williams, Renee Therese
2012-01-01T23:59:59.000Z
intrinsic reaction coordinate (IRC) methods. Energy maximafound, optimization QST IRC R P LST Figure 1.3 Illustrationreaction coordinate (IRC) methods, where R represents the
The Materials Project: Combining Density Functional Theory Calculations
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Density Functional Theory Approach to Nuclear Fission (Conference) |
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Density Functional Theory Approach to Nuclear Fission (Conference) |
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Density functional theory study of the structural, electronic, lattice
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Density functional theory study of the structural, electronic, lattice
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,Separation 23TribalInformationConference:(JournalTowards a Climate-Specific Test:theSciTechdynamical,
Mass Spectrometry and Density Functional Theory Characterizations of DNA Modifications
Williams, Renee Therese
2012-01-01T23:59:59.000Z
Containing 1,2-GpG, 1,2-ApG, and 1,3-GpXpG CisplatinODNs) containing a 1,2-GpG, 1,2-ApG, or 1,3-GpXpG cisplatinODNs containing a 1,2-GpG, 1,2-ApG or 1,3-GpXpG intrastrand
Maps of current density using density-functional methods A. Soncini,1,a
Helgaker, Trygve
, University of Durham, South Road, Durham DH1 3LE, United Kingdom Received 22 May 2008; accepted 17 July 2008 are compared and integration of the current densities to yield shielding constants is performed. In general of induced current density in molecules. © 2008 American Institute of Physics. DOI: 10.1063/1.2969104 I
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.
Berland, Kristian [Microtechnology and Nanoscience, MC2, Chalmers University of Technology, SE-412 96 Göteborg (Sweden) [Microtechnology and Nanoscience, MC2, Chalmers University of Technology, SE-412 96 Göteborg (Sweden); Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States); Arter, Calvin A.; Thonhauser, T. [Department of Physics, Wake Forest University, Winston-Salem, North Carolina 27109 (United States)] [Department of Physics, Wake Forest University, Winston-Salem, North Carolina 27109 (United States); Cooper, Valentino R. [Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831-6114 (United States)] [Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831-6114 (United States); Lee, Kyuho [Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States) [Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States); Department of Chemical and Biomolecular Engineering, University of California, Berkeley, California 94720 (United States); Lundqvist, Bengt I. [Department of Applied Physics, Chalmers University of Technology, SE-412 96 Göteborg (Sweden)] [Department of Applied Physics, Chalmers University of Technology, SE-412 96 Göteborg (Sweden); Schröder, Elsebeth; Hyldgaard, Per [Microtechnology and Nanoscience, MC2, Chalmers University of Technology, SE-412 96 Göteborg (Sweden)] [Microtechnology and Nanoscience, MC2, Chalmers University of Technology, SE-412 96 Göteborg (Sweden)
2014-05-14T23:59:59.000Z
The theoretical description of sparse matter attracts much interest, in particular for those ground-state properties that can be described by density functional theory. 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 89, 035412 (2014)] 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 PbTiO{sub 3}, the adsorption of small molecules within metal-organic frameworks, the graphite/diamond phase transition, and the adsorption of an aromatic-molecule 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.
On the breaking and restoration of symmetries within the nuclear energy density functional formalism
T. Duguet; J. Sadoudi
2010-10-19T23:59:59.000Z
We review the notion of symmetry breaking and restoration within the frame of nuclear energy density functional methods. We focus on key differences between wave-function- and energy-functional-based methods. In particular, we point to difficulties encountered within the energy functional framework and discuss new potential constraints on the underlying energy density functional that could make the restoration of broken symmetries better formulated within such a formalism. We refer to Ref.~\\cite{duguet10a} for details.
Sutton, Christopher; Gray, Matthew T.; Brunsfeld, Max; Parrish, Robert M.; Sherrill, C. David; Sears, John S.; Brédas, Jean-Luc, E-mail: jean-luc.bredas@chemistry.gatech.edu, E-mail: thomas.koerzdoerfer@uni-potsdam.de [School of Chemistry and Biochemistry and Center for Computational Molecular Science and Technology, Georgia Institute of Technology, Atlanta, Georgia 30332 (United States)] [School of Chemistry and Biochemistry and Center for Computational Molecular Science and Technology, Georgia Institute of Technology, Atlanta, Georgia 30332 (United States); Körzdörfer, Thomas, E-mail: jean-luc.bredas@chemistry.gatech.edu, E-mail: thomas.koerzdoerfer@uni-potsdam.de [School of Chemistry and Biochemistry and Center for Computational Molecular Science and Technology, Georgia Institute of Technology, Atlanta, Georgia 30332 (United States) [School of Chemistry and Biochemistry and Center for Computational Molecular Science and Technology, Georgia Institute of Technology, Atlanta, Georgia 30332 (United States); Computational Chemistry, Institute of Chemistry, University of Potsdam, D-14476 Potsdam (Germany)
2014-02-07T23:59:59.000Z
We investigate the torsion potentials in two prototypical ?-conjugated polymers, polyacetylene and polydiacetylene, as a function of chain length using different flavors of density functional theory. Our study provides a quantitative analysis of the delocalization error in standard semilocal and hybrid density functionals and demonstrates how it can influence structural and thermodynamic properties. The delocalization error is quantified by evaluating the many-electron self-interaction error (MESIE) for fractional electron numbers, which allows us to establish a direct connection between the MESIE and the error in the torsion barriers. The use of non-empirically tuned long-range corrected hybrid functionals results in a very significant reduction of the MESIE and leads to an improved description of torsion barrier heights. In addition, we demonstrate how our analysis allows the determination of the effective conjugation length in polyacetylene and polydiacetylene chains.
ASSESSMENT OF THE PERFORMANCE OF SEVERAL DENSITY FUNCTIONALS
Adler, Joan
) Focus on exchange-correlation energy...............................................9 b) Considerations calculation method for the gap? .......................................23 CONCLUSION AND OUTLOOKS chemistry and physics world during the last decades. Nevertheless, like every theory, it contains some
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,.
Negative energy densities in integrable quantum field theories at one-particle level
Bostelmann, Henning
2015-01-01T23:59:59.000Z
We study the phenomenon of negative energy densities in quantum field theories with self-interaction. Specifically, we consider a class of integrable models (including the sinh-Gordon model) in which we investigate the expectation value of the energy density in one-particle states. In this situation, we classify the possible form of the stress-energy tensor from first principles. We show that one-particle states with negative energy density generically exist in non-free situations, and we establish lower bounds for the energy density (quantum energy inequalities). Demanding that these inequalities hold reduces the ambiguity in the stress-energy tensor, in some situations fixing it uniquely. Numerical results for the lowest spectral value of the energy density allow us to demonstrate how negative energy densities depend on the coupling constant and on other model parameters.
Negative energy densities in integrable quantum field theories at one-particle level
Henning Bostelmann; Daniela Cadamuro
2015-02-05T23:59:59.000Z
We study the phenomenon of negative energy densities in quantum field theories with self-interaction. Specifically, we consider a class of integrable models (including the sinh-Gordon model) in which we investigate the expectation value of the energy density in one-particle states. In this situation, we classify the possible form of the stress-energy tensor from first principles. We show that one-particle states with negative energy density generically exist in non-free situations, and we establish lower bounds for the energy density (quantum energy inequalities). Demanding that these inequalities hold reduces the ambiguity in the stress-energy tensor, in some situations fixing it uniquely. Numerical results for the lowest spectral value of the energy density allow us to demonstrate how negative energy densities depend on the coupling constant and on other model parameters.
Accurate Energies and Structures for Large Water Clusters Using the X3LYP Hybrid Density Functional
Goddard III, William A.
Accurate Energies and Structures for Large Water Clusters Using the X3LYP Hybrid Density FunctionalVed: June 9, 2004; In Final Form: August 10, 2004 We predict structures and energies of water clusters containing up to 19 waters with X3LYP, an extended hybrid density functional designed to describe
Reactions of Polycarbonate with Cyclohexene Oxide and Phosphites: A Density Functional Study
Reactions of Polycarbonate with Cyclohexene Oxide and Phosphites: A Density Functional Study J bisphenol A polycarbonate (BPA-PC). We describe density functional (DF) calculations of the reactions to organic molecules and polymers, focusing on bisphenol A polycarbonate (BPA-PC). BPA-PC is an important
Probability-density function for energy perturbations of isolated optical pulses
Lakoba, Taras I.
Probability-density function for energy perturbations of isolated optical pulses C. J. Mc to determine the probability-density function (PDF) for noise-induced energy perturbations of isolated (solitary) optical pulses in fiber communication systems. The analytical formula is consistent
A. V. Afanasjev
2015-08-22T23:59:59.000Z
The assessment of the global performance of the state-of-the-art covariant energy density functionals and related theoretical uncertainties in the description of ground state observables has recently been performed. Based on these results, the correlations between global description of binding energies and nuclear matter properties of covariant energy density functionals have been studied in this contribution.
Density functional simulations of Tebased phase change materials J. Akola 1,2
E*PCOS2008 Density functional simulations of Tebased phase change materials J. Akola 1,2 and R. O limitations of the theoretical methods are discussed. Key words: Phase change materials, density functional. This is extremely difficult in practice, and our first calculations on phase change materials were carried out
Statistical Image Modeling with the Magnitude Probability Density Function of Complex Wavelet
Oraintara, Soontorn
Statistical Image Modeling with the Magnitude Probability Density Function of Complex Wavelet the probability density function (pdf) of the magnitude of complex wavelet coefficients with the assump- tion Statistical image modeling in the wavelet domain is of inter- est in recent years due to the ability
Afanasjev, A V
2015-01-01T23:59:59.000Z
The assessment of the global performance of the state-of-the-art covariant energy density functionals and related theoretical uncertainties in the description of ground state observables has recently been performed. Based on these results, the correlations between global description of binding energies and nuclear matter properties of covariant energy density functionals have been studied in this contribution.
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.
Applications of Skyrme energy-density functional to fusion reactions spanning the fusion barriers
Min Liu; Ning Wang; Zhuxia Li; Xizhen Wu; Enguang Zhao
2006-01-25T23:59:59.000Z
The Skyrme energy density functional has been applied to the study of heavy-ion fusion reactions. The barriers for fusion reactions are calculated by the Skyrme energy density functional with proton and neutron density distributions determined by using restricted density variational (RDV) method within the same energy density functional together with semi-classical approach known as the extended semi-classical Thomas-Fermi method. Based on the fusion barrier obtained, we propose a parametrization of the empirical barrier distribution to take into account the multi-dimensional character of real barrier and then apply it to calculate the fusion excitation functions in terms of barrier penetration concept. A large number of measured fusion excitation functions spanning the fusion barriers can be reproduced well. The competition between suppression and enhancement effects on sub-barrier fusion caused by neutron-shell-closure and excess neutron effects is studied.
Effects of van der Waals Density Functional Corrections on Trends...
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are not noticeably different between the two classes of functionals, while on Cu(111), modest changes are seen in both the erpendicular distance and the orientation of the aromatic...
Uncertainty Quantification and Propagation in Nuclear Density Functional
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Shielding Effectiveness Density Theory for Carbon Fiber/ Nylon 6,6 Composites
Perger, Warren F.
resistivity (1/electrical conductivity) values for various materials are typically 1014 to 1017 for polymers to improving the electri- cal conductivity of a polymer is through the addition of a conductive filler materialShielding Effectiveness Density Theory for Carbon Fiber/ Nylon 6,6 Composites Jason M. Keith
United abominations: Density functional studies of heavy metal chemistry
Schoendorff, George
2012-04-02T23:59:59.000Z
Carbonyl and nitrile addition to uranyl (UO{sup 2}{sup 2+}) are studied. The competition between nitrile and water ligands in the formation of uranyl complexes is investigated. The possibility of hypercoordinated uranyl with acetone ligands is examined. Uranyl is studied with diactone alcohol ligands as a means to explain the apparent hypercoordinated uranyl. A discussion of the formation of mesityl oxide ligands is also included. A joint theory/experimental study of reactions of zwitterionic boratoiridium(I) complexes with oxazoline-based scorpionate ligands is reported. A computational study was done of the catalytic hydroamination/cyclization of aminoalkenes with zirconium-based catalysts. Techniques are surveyed for programming for graphical processing units (GPUs) using Fortran.
Takuya Kanazawa; Tilo Wettig
2014-09-28T23:59:59.000Z
We generalize QCD at asymptotically large isospin chemical potential to an arbitrary even number of flavors. We also allow for small quark chemical potentials, which stress the coincident Fermi surfaces of the paired quarks and lead to a sign problem in Monte Carlo simulations. We derive the corresponding low-energy effective theory in both $p$- and $\\epsilon$-expansion and quantify the severity of the sign problem. We construct the random matrix theory describing our physical situation and show that it can be mapped to a known random matrix theory at low baryon density so that new insights can be gained without additional calculations. In particular, we explain the Silver Blaze phenomenon at high isospin density. We also introduce stressed singular values of the Dirac operator and relate them to the pionic condensate. Finally we comment on extensions of our work to two-color QCD.
Extra-galactic high-energy transients: event rate densities and luminosity functions
Sun, Hui; Li, Zhuo
2015-01-01T23:59:59.000Z
Several types of extra-galactic high-energy transients have been discovered, which include high-luminosity and low-luminosity long-duration gamma-ray bursts (GRBs), short-duration GRBs, supernova shock breakouts (SBOs), and tidal disruption events (TDEs) without or with an associated relativistic jet. In this paper, we apply a unified method to systematically study the redshift-dependent event rate densities and the global luminosity functions (ignoring redshift evolution) of these transients. We introduce some empirical formulae for the redshift-dependent event rate densities for different types of transients, and derive the local specific event rate density, which also represents its global luminosity function. Long GRBs have a large enough sample to reveal features in the global luminosity function, which is best characterized as a triple power law. All the other transients are consistent with having a single power law luminosity function. The total event rate density depends on the minimum luminosity, and...
Towards a Microscopic Reaction Description Based on Energy Density Functionals
Nobre, G A; DIetrich, F S; Escher, J E; Thompson, I J; Dupuis, M; Terasaki, J; Engel, J
2011-09-26T23:59:59.000Z
A microscopic calculation of reaction cross sections for nucleon-nucleus scattering has been performed by explicitly coupling the elastic channel to all particle-hole excitations in the target and one-nucleon pickup channels. The particle-hole states may be regarded as doorway states through which the flux flows to more complicated configurations, and subsequently to long-lived compound nucleus resonances. Target excitations for {sup 40,48}Ca, {sup 58}Ni, {sup 90}Zr and {sup 144}Sm were described in a random-phase framework using a Skyrme functional. Reaction cross sections obtained agree very well with experimental data and predictions of a state-of-the-art fitted optical potential. Couplings between inelastic states were found to be negligible, while the pickup channels contribute significantly. The effect of resonances from higher-order channels was assessed. Elastic angular distributions were also calculated within the same method, achieving good agreement with experimental data. For the first time observed absorptions are completely accounted for by explicit channel coupling, for incident energies between 10 and 70 MeV, with consistent angular distribution results.
On oscillator-bath system: Exact propagator, Reduced density matrix and Green's function
A. Refaei; F. Kheirandish
2014-07-27T23:59:59.000Z
The exact form of quantum propagator of a quantum oscillator interacting with a bosonic bath consisting of $N$ distinguished quantum oscillators with different frequencies is obtained in the Heisenberg picture. Reduced density matrix for oscillator is obtained. The kernel or Green's function connecting the initial density matrix of the oscillator to the density matrix in an arbitrary time is obtained and its connection to Feynman-Vernon influence functional is discussed. Weak coupling regime and squared mean values for position, momentum and energy of the oscillator are obtained in equilibrium.
Helgaker, Trygve
Erratum: "Density-functional and electron correlated study of five linear birefringences.6 nm . The effect of electron correlation depends strongly on the functional, leading t
Global hybrids from the semiclassical atom theory satisfying the local density linear response
Fabiano, E; Cortona, P; Della Sala, F
2015-01-01T23:59:59.000Z
We propose global hybrid approximations of the exchange-correlation (XC) energy functional which reproduce well the modified fourth-order gradient expansion of the exchange energy in the semiclassical limit of many-electron neutral atoms and recover the full local density approximation (LDA) linear response. These XC functionals represent the hybrid versions of the APBE functional [Phys. Rev. Lett. 106, 186406, (2011)] yet employing an additional correlation functional which uses the localization concept of the correlation energy density to improve the compatibility with the Hartree-Fock exchange as well as the coupling-constant-resolved XC potential energy. Broad energetical and structural testings, including thermochemistry and geometry, transition metal complexes, non-covalent interactions, gold clusters and small gold-molecule interfaces, as well as an analysis of the hybrid parameters, show that our construction is quite robust. In particular, our testing shows that the resulting hybrid, including 20\\% o...
Comparative Density Functional Study of Methanol Decomposition on Cu4 and Co4 Clusters
Mehmood, Faisal; Greeley, Jeffrey P.; Zapol, Peter; Curtiss, Larry A.
2010-11-18T23:59:59.000Z
A density functional theory study of the decomposition of methanol on Cu4 and Co4 clusters is presented. The reaction intermediates and activation barriers have been determined for reaction steps to form H2 and CO. For both clusters, methanol decomposition initiated by C-H and O-H bond breaking was investigated. In the case of a Cu4 cluster, methanol dehydrogenation through hydroxymethyl (CH2OH), hydroxymethylene (CHOH), formyl (CHO), and carbon monoxide (CO) is found to be slightly more favorable. For a Co4 cluster, the dehydrogenation pathway through methoxy (CH3O) and formaldehyde (CH2O) is slightly more favorable. Each of these pathways results in formation of CO and H2. The Co cluster pathway is very favorable thermodynamically and kinetically for dehydrogenation. However, since CO binds strongly, it is likely to poison methanol decomposition to H2 and CO at low temperatures. In contrast, for the Cu cluster, CO poisoning is not likely to be a problem since it does not bind strongly, but the dehydrogenation steps are not energetically favorable. Pathways involving C-O bond cleavage are even less energetically favorable. The results are compared to our previous study of methanol decomposition on Pd4 and Pd8 clusters. Finally, all reaction energy changes and transition state energies, including those for the Pd clusters, are related in a linear, Broensted-Evans-Polanyi plot.
Tao, Jianmin [Los Alamos National Laboratory; Perdew, John P [TULANE UNIV; Staroverov, Viktor N [UNIV OF WESTERN ONTARIO; Scuseria, Gustavo E [RICE UNIV
2008-01-01T23:59:59.000Z
We construct a nonlocal density functional approximation with full exact exchange, while preserving the constraint-satisfaction approach and justified error cancellations of simpler semilocal functionals. This is achieved by interpolating between different approximations suitable for two extreme regions of the electron density. In a 'normal' region, the exact exchange-correlation hole density around an electron is semilocal because its spatial range is reduced by correlation and because it integrates over a narrow range to -1. These regions are well described by popular semilocal approximations (many of which have been constructed nonempirically), because of proper accuracy for a slowly-varying density or because of error cancellation between exchange and correlation. 'Abnormal' regions, where non locality is unveiled, include those in which exchange can dominate correlation (one-electron, nonuniform high-density, and rapidly-varying limits), and those open subsystems of fluctuating electron number over which the exact exchange-correlation hole integrates to a value greater than -1. Regions between these extremes are described by a hybrid functional mixing exact and semi local exchange energy densities locally (i.e., with a mixing fraction that is a function of position r and a functional of the density). Because our mixing fraction tends to 1 in the high-density limit, we employ full exact exchange according to the rigorous definition of the exchange component of any exchange-correlation energy functional. Use of full exact exchange permits the satisfaction of many exact constraints, but the nonlocality of exchange also requires balanced nonlocality of correlation. We find that this nonlocality can demand at least five empirical parameters (corresponding roughly to the four kinds of abnormal regions). Our local hybrid functional is perhaps the first accurate size-consistent density functional with full exact exchange. It satisfies other known exact constraints, including exactness for all one-electron densities, and provides an excellent, fit 1.0 the 223 molecular enthalpies of formation of the G3/99 set and the 42 reaction barrier heights of the BH42/03 set, improving both (but especially the latter) over most semilocal functionals and global hybrids. Exact constraints, physical insights, and paradigm examples hopefully suppress 'overfitting'.
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.
Yan, Xun-Wang [Beijing Computational Science Research Center, Beijing 100084 (China) [Beijing Computational Science Research Center, Beijing 100084 (China); Faculty of Physics and Electronic Technology, Hubei University, Wuhan 430062 (China); State Key Laboratory of Theoretical Physics, Institute of Theoretical Physics, Chinese Academy of Science, Beijing 100190, China and School of Physics and Electrical Engineering, Anyang Normal University, Henan 455000 (China); Huang, Zhongbing, E-mail: huangzb@hubu.edu.cn [Beijing Computational Science Research Center, Beijing 100084 (China) [Beijing Computational Science Research Center, Beijing 100084 (China); Faculty of Physics and Electronic Technology, Hubei University, Wuhan 430062 (China); Lin, Hai-Qing [Beijing Computational Science Research Center, Beijing 100084 (China)] [Beijing Computational Science Research Center, Beijing 100084 (China)
2013-11-28T23:59:59.000Z
By the first principle calculations based on the van der Waals density functional theory, we study the crystal structures and electronic properties of La-doped phenanthrene. Two stable atomic geometries of La{sub 1}phenanthrene are obtained by relaxation of atomic positions from various initial structures. The structure-I is a metal with two energy bands crossing the Fermi level, while the structure-II displays a semiconducting state with an energy gap of 0.15 eV, which has an energy gain of 0.42 eV per unit cell compared to the structure-I. The most striking feature of La{sub 1}phenanthrene is that La 5d electrons make a significant contribution to the total density of state around the Fermi level, which is distinct from potassium doped phenanthrene and picene. Our findings provide an important foundation for the understanding of superconductivity in La-doped phenanthrene.
Yao, Kun
2015-01-01T23:59:59.000Z
We demonstrate a convolutional neural network trained to reproduce the Kohn-Sham kinetic energy of hydrocarbons from electron density. The output of the network is used as a non-local correction to the conventional local and semi-local kinetic functionals. We show that this approximation qualitatively reproduces Kohn-Sham potential energy surfaces when used with conventional exchange correlation functionals. Numerical noise inherited from the non-linearity of the neural network is identified as the major challenge for the model. Finally we examine the features in the density learned by the neural network to anticipate the prospects of generalizing these models.
Cosmological Constant as Vacuum Energy Density of Quantum Field Theories on Noncommutative Spacetime
Xiao-Jun Wang
2004-12-15T23:59:59.000Z
We propose a new approach to understand hierarchy problem for cosmological constant in terms of considering noncommutative nature of space-time. We calculate that vacuum energy density of the noncommutative quantum field theories in nontrivial background, which admits a smaller cosmological constant by introducing an higher noncommutative scale $\\mu_{NC}\\sim M_p$. The result $\\rho_\\Lambda\\sim 10^{-6}\\Lambda_{SUSY}^8M_p^4/\\mu_{NC}^8$ yields cosmological constant at the order of current observed value for supersymmetry breaking scale at 10TeV. It is the same as Banks' phenomenological formula for cosmological constant.
Towards a strong-coupling theory of QCD at finite density
B. Bringoltz; B. Svetitsky
2002-09-02T23:59:59.000Z
We apply strong-coupling perturbation theory to the QCD lattice Hamiltonian. We begin with naive, nearest-neighbor fermions and subsequently break the doubling symmetry with next-nearest-neighbor terms. The effective Hamiltonian is that of an antiferromagnet with an added kinetic term for baryonic "impurities," reminiscent of the t-J model of high-T_c superconductivity. As a first step, we fix the locations of the baryons and make them static. Following analyses of the t-J model, we apply large-N methods to obtain a phase diagram in the (N_c,N_f) plane at zero temperature and baryon density. Next we study a simplified U(3) toy model, in which we add baryons to the vacuum. We use a coherent state formalism to write a path integral which we analyze with mean field theory, obtaining a phase diagram in the (n_B,T) plane.
Carbon species confined inside carbon nanotubes: A density functional study Yi Liu and R. O. Jones*
Carbon species confined inside carbon nanotubes: A density functional study Yi Liu and R. O. Jones of the energies, structures, and vibration frequencies of carbon chains, rings, graphitic sheets, bowls, cages, and tubes inside single-walled carbon nanotubes CNT's with different diameters. The calculated energies show
Density Functional Study of Polycarbonate. 2. Crystalline Analogs, Cyclic Oligomers dimer and tetramer of bisphenol A polycarbonate (BPA-PC), as well as for the isolated structural units- bonate molecules has led to many studies of this family of polymers. Bisphenol A polycarbonate (BPA
Density Functional Study of Reactions of Phenoxides with Polycarbonate P. Ballone and R. O. Jones*
Density Functional Study of Reactions of Phenoxides with Polycarbonate P. Ballone and R. O. Jones used to study the reactions of chains of bisphenol A polycarbonate (BPA-PC) with sodium phenoxide (Na of the reactions of phenol, LiOPh, and NaOPh with the cyclic tetramer of bisphenol A polycarbonate (BPA
Branching Reactions in Polycarbonate: A Density Functional Study J. Akola and R. O. Jones*
Branching Reactions in Polycarbonate: A Density Functional Study J. Akola and R. O. Jones* Institut on the properties of polymers, and bisphenol A polycarbonate (BPA-PC) is no exception. We describe here the results and rubbers, where the entire system may be viewed as a single cross-linked molecule.2 Polycarbonates (PC
Density Functional Study of Crystalline Analogs of Polycarbonates B. Montanari, P. Ballone, and R of Bisphenol A polycarbonate (BPA-PC) and for the isolated structural unit. The calculations are free of polycarbonate molecules has grown greatly in the past two decades due to a wide range of industrial applications
A Combined Density Functional and Monte Carlo Study of Polycarbonate R. O. Jones and P. Ballone[*
A Combined Density Functional and Monte Carlo Study of Polycarbonate R. O. Jones and P. Ballone and reactivity for organic systems closely related to bisphenol-A-polycarbonate(BPA- PC). The results provide a detailed description of polymers, using bisphenol A polycarbonate (BPA- PC) as an example
Juliano, Steven A.
: Coccinellidae) to Different Densities of Aphis fabae (Hemiptera: Aphididae) ROYA FARHADI,1 HOSSEIN ALLAHYARI,1 on Aphis fabae (Scolpoli) (Hemiptera: Aphididae) by estimating the functional responses of all stages, Aphis fabae, searching efÞciency, han- dling time Black bean aphid, Aphis fabae (Scolpoli) (Hemiptera
Douanla, Hermann Yonta
2011-01-01T23:59:59.000Z
Spectral asymptotics of linear periodic elliptic operators with indefinite (sign-changing) density function is investigated in perforated domains with the two-scale convergence method. The limiting behavior of positive and negative eigencouples depends crucially on whether the average of the weight over the solid part is positive, negative or equal to zero. We prove concise homogenization results in all three cases.
Hermann Yonta Douanla
2012-08-21T23:59:59.000Z
Spectral asymptotics of linear periodic elliptic operators with indefinite (sign-changing) density function is investigated in perforated domains with the two-scale convergence method. The limiting behavior of positive and negative eigencouples depends crucially on whether the average of the weight over the solid part is positive, negative or equal to zero. We prove concise homogenization results in all three cases.
LES/probability density function approach for the simulation of an ethanol spray flame
Raman, Venkat
an experimental pilot-stabilized ethanol spray flame. In this particular flame, droplet evaporation occurs awayLES/probability density function approach for the simulation of an ethanol spray flame Colin Heye a, Austin, TX 78712, United States b School of Aerospace, Mechanical and Mechatronic Engineering
A Framework to Determine the Probability Density Function for the Output Power of Wind Farms
Liberzon, Daniel
A Framework to Determine the Probability Density Function for the Output Power of Wind Farms Sairaj to the power output of a wind farm while factoring in the availability of the wind turbines in the farm availability model for the wind turbines, we propose a method to determine the wind-farm power output pdf
The 2dF Galaxy Redshift Survey: luminosity functions by density environment and galaxy type
Darren J. Croton; Glennys R. Farrar; Peder Norberg; Matthew Colless; John A. Peacock; I. K. Baldry; C. M. Baugh; J. Bland-Hawthorn; T. Bridges; R. Cannon; S. Cole; C. Collins; W. Couch; G. Dalton; R. De Propris; S. P. Driver; G. Efstathiou; R. S. Ellis; C. S. Frenk; K. Glazebrook; C. Jackson; O. Lahav; I. Lewis; S. Lumsden; S. Maddox; D. Madgwick; B. A. Peterson; W. Sutherland; K. Taylor
2005-02-08T23:59:59.000Z
We use the 2dF Galaxy Redshift Survey to measure the dependence of the bJ-band galaxy luminosity function on large-scale environment, defined by density contrast in spheres of radius 8h-1Mpc, and on spectral type, determined from principal component analysis. We find that the galaxy populations at both extremes of density differ significantly from that at the mean density. The population in voids is dominated by late types and shows, relative to the mean, a deficit of galaxies that becomes increasingly pronounced at magnitudes brighter than M_bJ-5log10h <-18.5. In contrast, cluster regions have a relative excess of very bright early-type galaxies with M_bJ-5log10h < -21. Differences in the mid to faint-end population between environments are significant: at M_bJ-5log10h=-18 early and late-type cluster galaxies show comparable abundances, whereas in voids the late types dominate by almost an order of magnitude. We find that the luminosity functions measured in all density environments, from voids to clusters, can be approximated by Schechter functions with parameters that vary smoothly with local density, but in a fashion which differs strikingly for early and late-type galaxies. These observed variations, combined with our finding that the faint-end slope of the overall luminosity function depends at most weakly on density environment, may prove to be a significant challenge for models of galaxy formation.
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.
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Smallwood, D.O.
1996-01-01T23:59:59.000Z
It is shown that the usual method for estimating the coherence functions (ordinary, partial, and multiple) for a general multiple-input! multiple-output problem can be expressed as a modified form of Cholesky decomposition of the cross-spectral density matrix of the input and output records. The results can be equivalently obtained using singular value decomposition (SVD) of the cross-spectral density matrix. Using SVD suggests a new form of fractional coherence. The formulation as a SVD problem also suggests a way to order the inputs when a natural physical order of the inputs is absent.
Dey, Debarshi
2010-01-01T23:59:59.000Z
2 1.2 Normal Distribution and Simple Linear5 1.3 Skew Normal Distribution andthe Standard Normal Density and Distribution Functions 3.1
T. Duguet; M. Bender; K. Bennaceur; D. Lacroix; T. Lesinski
2009-03-04T23:59:59.000Z
We discuss the origin of pathological behaviors that have been recently identified in particle-number-restoration calculations performed within the nuclear energy density functional framework. A regularization method that removes the problematic terms from the multi-reference energy density functional and which applies (i) to any symmetry restoration- and/or generator-coordinate-method-based configuration mixing calculation and (ii) to energy density functionals depending only on integer powers of the density matrices, was proposed in [D. Lacroix, T. Duguet, M. Bender, arXiv:0809.2041] and implemented for particle-number restoration calculations in [M. Bender, T. Duguet, D. Lacroix, arXiv:0809.2045]. In the present paper, we address the viability of non-integer powers of the density matrices in the nuclear energy density functional. Our discussion builds upon the analysis already carried out in [J. Dobaczewski \\emph{et al.}, Phys. Rev. C \\textbf{76}, 054315 (2007)]. First, we propose to reduce the pathological nature of terms depending on a non-integer power of the density matrices by regularizing the fraction that relates to the integer part of the exponent using the method proposed in [D. Lacroix, T. Duguet, M. Bender, arXiv:0809.2041]. Then, we discuss the spurious features brought about by the remaining fractional power. Finally, we conclude that non-integer powers of the density matrices are not viable and should be avoided in the first place when constructing nuclear energy density functionals that are eventually meant to be used in multi-reference calculations.
Application of nuclear density functionals to lepton number violating weak processes
Rodriguez, Tomas R.; Martinez-Pinedo, Gabriel [Technische Universitaet Darmstadt, Magdalenenstr. 12, D-64289, Darmstadt (Germany) and GSI Helmholtzzentrum fuer Schwerionenforschung, Plankstr. 1, D-64291 Darmstadt (Germany)
2012-10-20T23:59:59.000Z
We present an application of energy density functional methods with the Gogny interaction to the calculation of nuclear matrix elements (NME) for neutrinoless double beta decay and double electron capture. Beyond mean field effects have been included by particle number and angular momentum restoration and shape mixing within the generator coordinate method (GCM) framework. We analyze in detail the NME for {sup 116}Cd nucleus which is one of the most promising candidates to detect neutrinoless double beta decay.
Nuclear energy density functionals: What we can learn about/from their global performance?
Afanasjev, A. V.; Agbemava, S. E.; Ray, D. [Department of Physics and Astronomy, Mississippi State University, MS 39762 (United States); Ring, P. [Fakultät für Physik, Technische Universität München, D-85748 Garching (Germany)
2014-10-15T23:59:59.000Z
A short review of recent results on the global performance of covariant energy density functionals is presented. It is focused on an analysis of the accuracy of the description of physical observables of ground and excited states as well as to related theoretical uncertainties. In addition, a global analysis of pairing properties is presented and the impact of pairing on the position of two-neutron drip line is discussed.
Modeling nuclear weak-interaction processes with relativistic energy density functionals
Paar, N; Vale, D; Vretenar, D
2015-01-01T23:59:59.000Z
Relativistic energy density functionals have become a standard framework for nuclear structure studies of ground-state properties and collective excitations over the entire nuclide chart. We review recent developments in modeling nuclear weak-interaction processes: charge-exchange excitations and the role of isoscalar proton-neutron pairing, charged-current neutrino-nucleus reactions relevant for supernova evolution and neutrino detectors, and calculation of beta-decay rates for r-process nucleosynthesis.
Probing the finite density equation of state of QCD via resummed perturbation theory
Sylvain Mogliacci
2014-07-08T23:59:59.000Z
In this Ph.D. thesis, the primary goal is to present a recent investigation of the finite density thermodynamics of hot and dense quark-gluon plasma. As we are interested in a temperature regime, in which naive perturbation theory is known to lose its predictive power, we clearly need to use a refined approach. To this end, we adopt a resummed perturbation theory point of view and employ two different frameworks. We first use hard-thermal-loop perturbation theory (HLTpt) at leading order to obtain the pressure for nonvanishing quark chemical potentials, and next, inspired by dimensional reduction, resum the known four-loop weak coupling expansion for the quantity. We present and analyze our findings for various cumulants of conserved charges. This provides us with information, through correlations and fluctuations, on the degrees of freedom effectively present in the quark-gluon plasma right above the deconfinement transition. Moreover, we compare our results with state-of-the-art lattice Monte Carlo simulations as well as with a recent three-loop mass truncated HTLpt calculation. We obtain very good agreement between the two different perturbative schemes, as well as between them and lattice data, down to surprisingly low temperatures right above the phase transition. We also quantitatively test the convergence of an approximation, which is used in higher order loop calculations in HTLpt. This method based on expansions in mass parameters, is unavoidable beyond leading order, thus motivating our investigation. We find the ensuing convergence to be very fast, validating its use in higher order computations.
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.
Arianna Carbone; Arnau Rios; Artur Polls
2014-11-19T23:59:59.000Z
The properties of symmetric nuclear and pure neutron matter are investigated within an extended self-consistent Green's function method that includes the effects of three-body forces. We use the ladder approximation for the study of infinite nuclear matter and incorporate the three-body interaction by means of a density-dependent two-body force. This force is obtained via a correlated average over the third particle, with an in-medium propagator consistent with the many-body calculation we perform. We analyze different prescriptions in the construction of the average and conclude that correlations provide small modifications at the level of the density-dependent force. Microscopic as well as bulk properties are studied, focusing on the changes introduced by the density dependent two-body force. The total energy of the system is obtained by means of a modified Galitskii-Migdal-Koltun sum rule. Our results validate previously used uncorrelated averages and extend the availability of chirally motivated forces to a larger density regime.
Homogenization of Steklov spectral problems with indefinite density function in perforated domains
Douanla, Hermann Yonta
2011-01-01T23:59:59.000Z
The asymptotic behavior of second order self-adjoint elliptic Steklov eigenvalue problems with periodic rapidly oscillating coefficients and with indefinite (sign-changing) density function is investigated in periodically perforated domains. We prove that the spectrum of this problem is discrete and consists of two sequences, one tending to -{\\infty} and another towards +{\\infty}. The limiting behavior of positive and negative eigencouples depends crucially on whether the average of the weight over the surface of the reference hole is positive, negative or equal to zero. By means of the two-scale convergence method, we prove concise homogenization results in all three cases.
Homogenization of Steklov spectral problems with indefinite density function in perforated domains
Hermann Yonta Douanla
2012-08-21T23:59:59.000Z
The asymptotic behavior of second order self-adjoint elliptic Steklov eigenvalue problems with periodic rapidly oscillating coefficients and with indefinite (sign-changing) density function is investigated in periodically perforated domains. We prove that the spectrum of this problem is discrete and consists of two sequences, one tending to -{\\infty} and another to +{\\infty}. The limiting behavior of positive and negative eigencouples depends crucially on whether the average of the weight over the surface of the reference hole is positive, negative or equal to zero. By means of the two-scale convergence method, we investigate all three cases.
Energy Density Functional Study of Nuclear Matrix Elements for Neutrinoless {beta}{beta} Decay
Rodriguez, Tomas R. [GSI Helmholtzzentrum fuer Schwerionenforschung, D-64259 Darmstadt (Germany); Departamento de Fisica Teorica, Universidad Autonoma de Madrid, E-28049 Madrid (Spain); CEA, Irfu, SPhN, Centre de Saclay, F-911191 Gif-sur-Yvette (France); Martinez-Pinedo, Gabriel [GSI Helmholtzzentrum fuer Schwerionenforschung, D-64259 Darmstadt (Germany)
2010-12-17T23:59:59.000Z
We present an extensive study of nuclear matrix elements (NME) for the neutrinoless double-beta decay of the nuclei {sup 48}Ca, {sup 76}Ge, {sup 82}Se, {sup 96}Zr, {sup 100}Mo, {sup 116}Cd, {sup 124}Sn, {sup 128}Te, {sup 130}Te, {sup 136}Xe, and {sup 150}Nd based on state-of-the-art energy density functional methods using the Gogny D1S functional. Beyond-mean-field effects are included within the generating coordinate method with particle number and angular momentum projection for both initial and final ground states. We obtain a rather constant value for the NMEs around 4.7 with the exception of {sup 48}Ca and {sup 150}Nd, where smaller values are found. We analyze the role of deformation and pairing in the evaluation of the NME and present detailed results for the decay of {sup 150}Nd.
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...
K. Nomura; T. Niksic; T. Otsuka; N. Shimizu; D. Vretenar
2011-06-14T23:59:59.000Z
Microscopic energy density functionals (EDF) have become a standard tool for nuclear structure calculations, providing an accurate global description of nuclear ground states and collective excitations. For spectroscopic applications this framework has to be extended to account for collective correlations related to restoration of symmetries broken by the static mean field, and for fluctuations of collective variables. In this work we compare two approaches to five-dimensional quadrupole dynamics: the collective Hamiltonian for quadrupole vibrations and rotations, and the Interacting Boson Model. The two models are compared in a study of the evolution of non-axial shapes in Pt isotopes. Starting from the binding energy surfaces of $^{192,194,196}$Pt, calculated with a microscopic energy density functional, we analyze the resulting low-energy collective spectra obtained from the collective Hamiltonian, and the corresponding IBM-2 Hamiltonian. The calculated excitation spectra and transition probabilities for the ground-state bands and the $\\gamma$-vibration bands are compared to the corresponding sequences of experimental states.
Polycarbonate Simulations with a Density Functional Based Force Field P. Ballone, B. Montanari properties of molecules related to polycarbonate have been used to optimize the parameters describing dynamics simulations of crystalline, amorphous, and liquid polycarbonate systems. Applications include
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
Ad. R. Raduta; F. Gulminelli; M. Oertel
2014-09-15T23:59:59.000Z
We study the thermodynamical properties of compressed baryonic matter with strangeness within non-relativistic energy density functional models with a particular emphasis on possible phase transitions found earlier for a simple $n,p,e,\\Lambda$-mixture. The aim of the paper is twofold: I) examining the phase structure of the complete system, including the full baryonic octet and II) testing the sensitivity of the results to the model parameters. We find that, associated to the onset of the different hyperonic families, up to three separate strangeness-driven phase transitions may occur. Consequently, a large fraction of the baryonic density domain is covered by phase coexistence with potential relevance for (proto)-neutron star evolution. It is shown that the presence of a phase transition is compatible both with the observational constraint on the maximal neutron star mass, and with the present experimental information on hypernuclei. In particular we show that two solar mass neutron stars are compatible with important hyperon content. Still, the parameter space is too large to give a definitive conclusion of the possible occurrence of a strangeness driven phase transition, and further constraints from multiple-hyperon nuclei and/or hyperon diffusion data are needed.
Terminating states as a unique laboratory for testing nuclear energy density functional
M. Zalewski; W. Satula
2007-01-30T23:59:59.000Z
Systematic calculations of favored signature maximum-spin I_max and unfavored signature I_max - 1 terminating states for [f 7/2 ^ n] and [d 3/2 ^ (-1) f 7/2 ^ (n+1)] configurations (n denotes number of valence particles) in A ~ 44 mass region are presented. Following the result of Zdunczuk et al., Phys. Rev. C71 (2005) 024305 the calculations are performed using Skyrme energy density functional with empirical Landau parameters and slightly reduced spin-orbit strength. The aim is to identify and phenomenologically restore rotational symmetry broken by the Skyrme-Hartree-Fock solutions. In particular, it is shown that correlation energy due to symmetry restoration is absolutely crucial in order to reproduce energy splitting E(I_max) - E(I_max -1) in [f 7/2 ^ n] configurations but is relatively less important for [d 3/2 ^ (-1) f 7/2 ^ (n+1)] configurations.
P. W. Zhao; Z. P. Li; J. M. Yao; J. Meng
2010-11-11T23:59:59.000Z
A new parametrization PC-PK1 for the nuclear covariant energy density functional with nonlinear point-coupling interaction is proposed by fitting to observables for 60 selected spherical nuclei, including the binding energies, charge radii and empirical pairing gaps. The success of PC-PK1 is illustrated in its description for infinite nuclear matter and finite nuclei including the ground-state and low-lying excited states. Particularly, PC-PK1 improves the description for isospin dependence of binding energy along either the isotopic or the isotonic chains, which makes it more reliable for application in exotic nuclei. The predictive power of PC-PK1 is also illustrated for the nuclear low-lying excitation states in a five-dimensional collective Hamiltonian in which the parameters are determined by constrained calculations for triaxial shapes.
K. Nomura; R. Rodriguez-Guzman; L. M. Robledo; N. Shimizu
2012-08-23T23:59:59.000Z
We investigate the emergence and evolution of shape coexistence in the neutron-deficient Lead isotopes within the interacting boson model (IBM) plus configuration mixing with microscopic input based on the Gogny energy density functional (EDF). The microscopic potential energy surface obtained from the constrained self-consistent Hartree-Fock-Bogoliubov method employing the Gogny-D1M EDF is mapped onto the coherent-state expectation value of the configuration-mixing IBM Hamiltonian. In this way, the parameters of the IBM Hamiltonian are fixed for each of the three relevant configurations (spherical, prolate and oblate) associated to the mean field minima. Subsequent diagonalization of the Hamiltonian provides the excitation energy of the low-lying states and transition strengths among them. The model predictions for the $0^{+}$ level energies and evolving shape coexistence in the considered Lead chain are consistent both with experiment and with the indications of the Gogny-EDF energy surfaces.
Ning Wang; Xizhen Wu; Zhuxia Li; Min Liu; Werner Scheid
2006-09-18T23:59:59.000Z
The Skyrme energy-density functional approach has been extended to study the massive heavy-ion fusion reactions. Based on the potential barrier obtained and the parameterized barrier distribution the fusion (capture) excitation functions of a lot of heavy-ion fusion reactions are studied systematically. The average deviations of fusion cross sections at energies near and above the barriers from experimental data are less than 0.05 for 92% of 76 fusion reactions with $Z_1Z_2fusion reactions, for example, the $^{238}$U-induced reactions and $^{48}$Ca+$^{208}$Pb the capture excitation functions have been reproduced remarkable well. The influence of structure effects in the reaction partners on the capture cross sections are studied with our parameterized barrier distribution. Through comparing the reactions induced by double-magic nucleus $^{48}$Ca and by $^{32}$S and $^{35}$Cl, the 'threshold-like' behavior in the capture excitation function for $^{48}$Ca induced reactions is explored and an optimal balance between the capture cross section and the excitation energy of the compound nucleus is studied. Finally, the fusion reactions with $^{36}$S, $^{37}$Cl, $^{48}$Ca and $^{50}$Ti bombarding on $^{248}$Cm, $^{247,249}$Bk, $^{250,252,254}$Cf and $^{252,254}$Es, and as well as the reactions lead to the same compound nucleus with Z=120 and N=182 are studied further. The calculation results for these reactions are useful for searching for the optimal fusion configuration and suitable incident energy in the synthesis of superheavy nuclei.
Truhlar, Donald G
Tests of the RPBE, revPBE, -HCTHhyb, B97X-D, and MOHLYP density functional approximations and 29 density functional approximations are tested against two diverse databases, one with 18 bond energies Some tests of density functionals against the representa- tive databases have already been reported.2
Power Density Spectra of Gamma-Ray Burst Light Curves: Implications on Theory and Observation
Heon-Young Chang; Insu Yi
2001-01-02T23:59:59.000Z
We study the power density spectrum (PDS) of artificial light curves of observed gamma-ray bursts (GRBs). We investigate statistical properties of GRB light curves by comparing the reported characteristics in the PDSs of the observed GRBs with those that we model, and discuss implications on interpretations of the PDS analysis results. Results of PDS analysis of observed GRBs suggest that the averaged PDS of GRBs follows a power law over about two decades of frequency with the power law index, -5/3, and the distribution of individual power follows an exponential distribution. Though an attempt to identify the most sensitive physical parameter has been made on the basis of the internal shock model, we demonstrate that conclusions of this kind of approach should be derived with due care. It is indicative that the physical information extracted from the slope can be misleading. We show that the reported slope and the distribution can be reproduced by adjusting the sampling interval in the time domain for a given decaying timescale of individual pulse in a specific form of GRB light curves. In particular, given that the temporal feature is modeled by a two-sided exponential function, the power law behavior with the index of -5/3 and the exponential distribution of the observed PDS is recovered at the 64 ms trigger time scale when the decaying timescale of individual pulse is $\\sim 1$ second, provided that the pulse sharply rises. Another way of using the PDS analysis is an application of the same method to individual long bursts in order to examine a possible evolution of the decaying timescale in a single burst.
Spurious finite-size instabilities in nuclear energy density functionals: spin channel
Pastore, A; Davesne, D; Navarro, J
2015-01-01T23:59:59.000Z
It has been recently shown, that some Skyrme functionals can lead to non-converging results in the calculation of some properties of atomic nuclei. A previous study has pointed out a possible link between these convergence problems and the appearance of finite-size instabilities in symmetric nuclear matter (SNM) around saturation density. We show that the finite-size instabilities not only affect the ground state properties of atomic nuclei, but they can also influence the calculations of vibrational excited states in finite nuclei. We perform systematic fully-self consistent Random Phase Approximation (RPA) calculations in spherical doubly-magic nuclei. We employ several Skyrme functionals and vary the isoscalar and isovector coupling constants of the time-odd term $\\mathbf{s}\\cdot \\Delta \\mathbf{s}$ . We determine critical values of these coupling constants beyond which the RPA calculations do not converge because RPA the stability matrix becomes non-positive.By comparing the RPA calculations of atomic nucl...
Rodriguez-Guzman, R R
2015-01-01T23:59:59.000Z
Mean field calculations, based on the D1S, D1N and D1M parametrizations of the Gogny energy density functional, have been carried out to obtain the potential energy surfaces relevant to fission in several Ra isotopes with the neutron number 144 $\\le$ N $\\le$ 176. Inner and outer barrier heights as well as first and second isomer excitation energies are given. The existence of a well developed third minimum along the fission paths of Ra nuclei, is analyzed in terms of the energetics of the "fragments" defining such elongated configuration. The masses and charges of the fission fragments are studied as functions of the neutron number in the parent Ra isotope. The comparison between fission and $\\alpha$-decay half-lives, reveals that the former becomes faster for increasing neutron numbers. Though there exists a strong variance of the results with respect to the parameters used in the computation of the spontaneous fission rate, a change in tendency is observed at N=164 with a steady increase that makes heavier ...
Ghasemi, S Alireza; Saha, Santanu; Goedecker, Stefan
2015-01-01T23:59:59.000Z
Based on an analysis of the short range chemical environment of each atom in a system, standard machine learning based approaches to the construction of interatomic potentials aim at determining directly the central quantity which is the total energy. This prevents for instance an accurate description of the energetics of systems where long range charge transfer is important as well as of ionized systems. We propose therefore not to target directly with machine learning methods the total energy but an intermediate physical quantity namely the charge density, which then in turn allows to determine the total energy. By allowing the electronic charge to distribute itself in an optimal way over the system, we can describe not only neutral but also ionized systems with unprecedented accuracy. We demonstrate the power of our approach for both neutral and ionized NaCl clusters where charge redistribution plays a decisive role for the energetics. We are able to obtain chemical accuracy, i.e. errors of less than a mil...
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.
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.
A study of the observed areal distribution of rainfall as a function of the density of rain gages
Alvarez Bernal, Fernando
1969-01-01T23:59:59.000Z
. W. K. Henry A study was made of reported rainfall as a function of the density oi gages for several geographical areas including Tezas, Colombia, Guyana, Panama, Venezuela, and Ecuador--each having different terrain effects. Consideration..., and Panama areas using mean-monthly data. . . . . . . . . . . . , . . . . . . 40 Comparison of depth-area relations from different gage density for one storm in East Yegua basin Cl?niiydg I l. 'ITRC?'UCTTOK Those "!ho i:ork i!it/ raiuf all iiata know...
Coclite, Alessandro; De Palma, Pietro; Cutrone, Luigi
2013-01-01T23:59:59.000Z
Flamelet Progress Variable (FPV) combustion models allow the evaluation of all thermo chemical quantities in a reacting flow by computing only the mixture fraction Z and a progress variable C. When using such a method to predict a turbulent combustion in conjunction with a turbulence model, a probability density function (PDF) is required to evaluate statistical averages (e.g., Favre average) of chemical quantities. The choice of the PDF is a compromise between computational costs and accuracy level. The aim of this paper is to investigate the influence of the PDF choice and its modeling aspects in the simulation of non premixed turbulent combustion. Three different models are considered: the standard one, based on the choice of a beta distribution for Z and a Dirac distribution for C; a model employing a beta distribution for both Z and C; a third model obtained using a beta distribution for Z and the statistical most likely distribution (SMLD) for C. The standard model, although widely used, doesn't take in...
Development and evaluation of probability density functions for a set of human exposure factors
Maddalena, R.L.; McKone, T.E.; Bodnar, A.; Jacobson, J.
1999-06-01T23:59:59.000Z
The purpose of this report is to describe efforts carried out during 1998 and 1999 at the Lawrence Berkeley National Laboratory to assist the U.S. EPA in developing and ranking the robustness of a set of default probability distributions for exposure assessment factors. Among the current needs of the exposure-assessment community is the need to provide data for linking exposure, dose, and health information in ways that improve environmental surveillance, improve predictive models, and enhance risk assessment and risk management (NAS, 1994). The U.S. Environmental Protection Agency (EPA) Office of Emergency and Remedial Response (OERR) plays a lead role in developing national guidance and planning future activities that support the EPA Superfund Program. OERR is in the process of updating its 1989 Risk Assessment Guidance for Superfund (RAGS) as part of the EPA Superfund reform activities. Volume III of RAGS, when completed in 1999 will provide guidance for conducting probabilistic risk assessments. This revised document will contain technical information including probability density functions (PDFs) and methods used to develop and evaluate these PDFs. The PDFs provided in this EPA document are limited to those relating to exposure factors.
Density functional study of CaN mono and bilayer on Cu(001)
Zahedifar, Maedeh; Hashemifar, S. Javad, E-mail: hashemifar@cc.iut.ac.ir; Akbarzadeh, Hadi [Department of Physics, Isfahan University of Technology, Isfahan, 84156-83111 (Iran, Islamic Republic of)] [Department of Physics, Isfahan University of Technology, Isfahan, 84156-83111 (Iran, Islamic Republic of)
2014-01-15T23:59:59.000Z
Density functional - pseudopotential calculations are performed to provide first-principles insights into magnetic behaviour of bulk CaN and CaN monolayers on Cu(001) in the rock-salt (RS) and zinc-blende (ZB) structures. Our results indicate that both RS- and ZB-CaN exhibit half-metallic ferromagnetism originated from the incomplete 2p shell of the nitrogen ion. In contrast to the bulk CaN, the CaN monolayers on Cu(001) generally favor ZB structure. We argue that the more stable ZB-CaN thin films on Cu(001) are nonmagnetic, because of strong Cu-N bonding at the interface, while the less stable Ca terminated ZB-CaN thin films exhibit half-metallic ferromagnetism. The transition path between the high energy ferromagnetic and the stable nonmagnetic configurations of the ZB-CaN monolayer on Cu(001) are studied by using the nudged elastic band method. We observe a two stages transition and an activation barrier of about 1.18 eV in the minimum energy path of this transition.
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.
Mehmood, F.; Greeley, J.; Zapol, P.; Curtiss, L. A.
2010-08-12T23:59:59.000Z
A density functional theory study of the decomposition of methanol on Cu{sub 4} and Co{sub 4} clusters is presented. The reaction intermediates and activation barriers have been determined for reaction steps to form H{sub 2} and CO. For both clusters, methanol decomposition initiated by C-H and O-H bond breaking was investigated. In the case of a Cu{sub 4} cluster, methanol dehydrogenation through hydroxymethyl (CH{sub 2}OH), hydroxymethylene (CHOH), formyl (CHO), and carbon monoxide (CO) is found to be slightly more favorable. For a Co{sub 4} cluster, the dehydrogenation pathway through methoxy (CH{sub 3}O) and formaldehyde (CH{sub 2}O) is slightly more favorable. Each of these pathways results in formation of CO and H{sub 2}. The Co cluster pathway is very favorable thermodynamically and kinetically for dehydrogenation. However, since CO binds strongly, it is likely to poison methanol decomposition to H{sub 2} and CO at low temperatures. In contrast, for the Cu cluster, CO poisoning is not likely to be a problem since it does not bind strongly, but the dehydrogenation steps are not energetically favorable. Pathways involving C-O bond cleavage are even less energetically favorable. The results are compared to our previous study of methanol decomposition on Pd{sub 4} and Pd{sub 8} clusters. Finally, all reaction energy changes and transition state energies, including those for the Pd clusters, are related in a linear, Broensted?Evans?Polanyi plot.
Holmes, Sean T.; Dybowski, Cecil [Department of Chemistry and Biochemistry, University of Delaware, Newark, Delaware 19716 (United States); Iuliucci, Robbie J. [Department of Chemistry, Washington and Jefferson College, Washington, Pennsylvania 15301 (United States); Mueller, Karl T. [Department of Chemistry, Pennsylvania State University, University Park, Pennsylvania 16802 (United States); Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352 (United States)
2014-10-28T23:59:59.000Z
A quantum-chemical method for modeling solid-state nuclear magnetic resonance chemical-shift tensors by calculations on large symmetry-adapted clusters of molecules is demonstrated. Four hundred sixty five principal components of the {sup 13}C chemical-shielding tensors of 24 organic materials are analyzed. The comparison of calculations on isolated molecules with molecules in clusters demonstrates that intermolecular effects can be successfully modeled using a cluster that represents a local portion of the lattice structure, without the need to use periodic-boundary conditions (PBCs). The accuracy of calculations which model the solid state using a cluster rivals the accuracy of calculations which model the solid state using PBCs, provided the cluster preserves the symmetry properties of the crystalline space group. The size and symmetry conditions that the model cluster must satisfy to obtain significant agreement with experimental chemical-shift values are discussed. The symmetry constraints described in the paper provide a systematic approach for incorporating intermolecular effects into chemical-shielding calculations performed at a level of theory that is more advanced than the generalized gradient approximation. Specifically, NMR parameters are calculated using the hybrid exchange-correlation functional B3PW91, which is not available in periodic codes. Calculations on structures of four molecules refined with density plane waves yield chemical-shielding values that are essentially in agreement with calculations on clusters where only the hydrogen sites are optimized and are used to provide insight into the inherent sensitivity of chemical shielding to lattice structure, including the role of rovibrational effects.
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
Lobach, Ihar; Feranchuk, Ilya
2015-01-01T23:59:59.000Z
Linear theory of the parametric beam instability or the self-amplification of parametric x-ray radiation (PXR) from relativistic electrons in a crystal is considered taking into account finite emittance of the electron beam and absorption of the radiation. It is shown that these factors change essentially the estimation of threshold parameters of the electron bunches for the coherent X-ray generation. The boundary conditions for the linear theory of the effect is analyzed in details and it is shown that the grazing incidence diffraction geometry is optimal for the growth of instability. Numerical estimations of amplification and coherent photon yield in dependence on the electron current density are presented for the case of mm-thickness Si crystal and 100 MeV electrons. Possible improvements of the experimental scheme for optimization of the coherent radiation intensity are discussed.
Truhlar, Donald G
2009 The performance of the M06-L density functional has been tested for band gaps in seven,13 that is designed for main group thermo- chemistry, transition metal bonding, thermochemical kinet- ics in group-4, group 35, and metal oxide semiconductors. In Sec. II, we describe the test sets
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.
Testing Density Wave Theory with Resolved Stellar Populations around Spiral Arms in M81
Choi, Yumi; Williams, Benjamin F; Weisz, Daniel R; Skillman, Evan D; Fouesneau, Morgan; Dolphin, Andrew E
2015-01-01T23:59:59.000Z
Stationary density waves rotating at a constant pattern speed $\\Omega_{\\rm P}$ would produce age gradients across spiral arms. We test whether such age gradients are present in M81 by deriving the recent star formation histories (SFHs) of 20 regions around one of M81's grand-design spiral arms. For each region, we use resolved stellar populations to determine the SFH by modeling the observed color-magnitude diagram (CMD) constructed from archival Hubble Space Telescope (HST) F435W and F606W imaging. Although we should be able to detect systematic time delays in our spatially-resolved SFHs, we find no evidence of star formation propagation across the spiral arm. Our data therefore provide no convincing evidence for a stationary density wave with a single pattern speed in M81, and instead favor the scenario of kinematic spiral patterns that are likely driven by tidal interactions with the companion galaxies M82 and NGC 3077.
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
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.
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.
Nordlund, Dennis
2008-01-01T23:59:59.000Z
Structure Effects in Liquid Water studied by Photoelectronphotoelectron emission spectra of liquid water in comparisonwith gas-phase water, ice close to the melting point, low
Nordlund, Dennis; Odelius, Michael; Bluhm, Hendrik; Ogasawara, Hirohito; Pettersson, Lars G.M.; Nilsson, Anders
2008-04-29T23:59:59.000Z
We present valence photoelectron emission spectra of liquid water in comparison with gas-phase water, ice close to the melting point, low temperature amorphous and crystalline ice. All aggregation states have major electronic structure changes relative to the free molecule, with rehybridization and development of bonding and anti-bonding states accompanying the hydrogen bond formation. Sensitivity to the local structural order, most prominent in the shape and splitting of the occupied 3a{sub 1} orbital, is understood from the electronic structure averaging over various geometrical structures, and reflects the local nature of the orbital interaction.
Excited states and electron transfer in solution : models based on density functional theory
Kowalczyk, Timothy Daniel
2012-01-01T23:59:59.000Z
Our understanding of organic materials for solar energy conversion stands to benefit greatly from accurate, computationally tractable electronic structure methods for excited states. Here we apply two approaches based on ...
Li, Mo
materials of Li-ion batteries and cathode materials of proton exchange membrane (PEM) fuel cells charging and discharging. Experiment shows promising results [2]. As a cathode material in (PEM) fuel cells and geometrically optimized in a periodic repeating box. The box was made large enough to prevent self interaction
Dynamics of Charge-Transfer Processes with Time-Dependent Density Functional Theory
(organic, inorganic, and hybrids), photocatalysis, biomolecules in solvents, reactions at the interface
Density Functional Theory for High-Throughput Screening of Chemicals and Materials
Fu, Jia
2015-01-01T23:59:59.000Z
Celzard, A. ; Fierro, V. Energy & Fuels 2005, 19, 573. (140)Snurr, R. Q. ; Hupp, J. T. Energy & Environmental ScienceH. -K. ; Zhou, H. -C. Energy & Environmental Science 2013,
Structural motifs in oxidized graphene: A genetic algorithm study based on density functional theory
Gong, Xingao
of China 2National Renewable Energy Laboratory, Golden, Colorado 80401, USA Received 16 June 2010 running along the zigzag direction. In contrast, the ground-state phase with a slightly lower energy and the low-energy struc- tures of C1O will take place in the ground state. In addition, the electronic
Hirunsit, Pussana
2011-10-21T23:59:59.000Z
speeds corrosion and breakdown of cell components ?Complex electrolyte management ?Slow start-up Solid Oxide (SOFC) Solid zirconium oxide to which a small amount of Yttria is added 650 - 1000?C 5kW ? 3MW ?Auxiliary power...
Density Functional Theory for High-Throughput Screening of Chemicals and Materials
Fu, Jia
2015-01-01T23:59:59.000Z
organic compounds and gas storage capabilities in nanoporousof materials for gas storage has been rather limited becausefree energy and gas storage and transport properties in
van der Waals Corrected Density Functional Theory Calculations on Zeolitic Imidazolate Frameworks
Ray, Keith G.
2013-01-01T23:59:59.000Z
Organic Frame- works: Gas Storage, Separation and Catalysis,ZIF compounds for gas storage and separation applications.can be useful for gas storage applications, e.g. , CO 2 or H
Thygesen, Kristian
been demonstrated in an experiment by Bonn et al.,8 who were able to form carbon dioxide from carbon impossible because the carbon monoxide desorbs be- fore the carbon dioxide formation when the temperature. It is demonstrated that with the model we can extract several properties of the system, such as the presence
van der Waals Corrected Density Functional Theory Calculations on Zeolitic Imidazolate Frameworks
Ray, Keith G.
2013-01-01T23:59:59.000Z
structure, and carbon dioxide capture properties of zeoliticand carbon dioxide cap- ture properties of zeoliticCarbon dioxide’s liquid-vapor coexistence curve and critical properties
Joint Density-Functional Theory of Electrochemistry > Research Highlights >
Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)
AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE:1 First Use of Energy for All Purposes (Fuel and Nonfuel), 2002; Level:5 TablesExports(Journal Article) | SciTech Connect Journal Article: X-rayContract Documents PPPLHighlyResearchJobs About About Home OrganizationIn
Efficient Real-Time Time-Dependent Density Functional Theory Method and its
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,SeparationConnect Journal Article: Discrete phase space based(JournalApplication to a Collision of an Ion with
Structure, magnetism, and adhesion at Cr/Fe interfaces from density functional theory
Carter, Emily A.
Department of Mechanical and Aerospace Engineering and Program in Applied and Computational Mathematics, and corrosive blast gases [1]. Steel alone will erode rather quickly under these conditions and alloying
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
Li, Weixue
calculations Hai-Yan Su,1,2,3 Xin-He Bao,1,a and Wei-Xue Li1,2,b 1 State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People's Republic of China 2 Center for Theoretical and Computational Chemistry, Dalian Institute of Chemical Physics, Chinese Academy
A Hybrid Density Functional Theory for Solvation and Solvent-Mediated Interactions
Jin, Zhehui
2012-01-01T23:59:59.000Z
method, the major source of the free energy increase arisesfree energy of anions, are probably due to different sources
Density Functional Theory for High-Throughput Screening of Chemicals and Materials
Fu, Jia
2015-01-01T23:59:59.000Z
the compressed natural gas (CNG) at the same temperature andcompressed natural gas tank (CNG). According to this table,Compressed Natural Gas (CNG) 136 , involve either cryogenic
Density Functional Theory for High-Throughput Screening of Chemicals and Materials
Fu, Jia
2015-01-01T23:59:59.000Z
parameters for MOF-5, Cu-BTC and ZIF-8 were from universalMOF materials, MOF-5 129 and Cu-BTC 130 , again at roomFor methane adsorption in Cu-BTC, however, WDA-Y reproduces
Hirunsit, Pussana
2011-10-21T23:59:59.000Z
Pt-based alloy surfaces are used to catalyze the electrochemical oxygen reduction reaction (ORR), where molecular oxygen is converted into water on fuel cell electrodes. In this work, we address challenges due to the cost ...
Density Functional Theory for High-Throughput Screening of Chemicals and Materials
Fu, Jia
2015-01-01T23:59:59.000Z
Microporous and Mesoporous Materials 2001, (29) Occelli, M.Microporous and Mesoporous Materials 2012, (170) Ben, T. ;Zhou, H. -C. Chemistry of Materials 2010, (172) Yuan, D. ;
A. Staszczak; A. Baran; W. Nazarewicz
2012-08-06T23:59:59.000Z
Lifetimes of super-heavy (SH) nuclei are primarily governed by alpha decay and spontaneous fission (SF). Here we study the competing decay modes of even-even SH isotopes with 108 cold fusion" and "hot fusion" reactions. The region of long-lived SH nuclei is expected to be centered on $^{294}$Ds with a total half-life of ?1.5 days.
The scaling functions of the free energy density and its derivatives for the 3d O(4) model
Engels, Juergen
2011-01-01T23:59:59.000Z
We derive direct representations of the scaling functions of the 3d O(4) model which are relevant for comparisons to other models, in particular QCD. This is done in terms of expansions in the scaling variable z= t/h^{1/Delta}. The expansions around z=0 and the corresponding asymptotic ones for z --> +- infinity overlap such that no interpolation is needed. The expansion coefficients are determined numerically from the data of a previous high statistics simulation of the O(4) model on a three-dimensional lattice of linear extension L=120. From the scaling function of the magnetization we calculate the leading asymptotic coefficients of the scaling function of the free energy density. As a result we obtain the universal amplitude ratio A^+/A^-=1.84(4) for the specific heat. Comparing the scaling function of the energy density to the data we find the non-singular part of the energy density epsilon_{ns}(T) with high precision and at the same time excellent scaling properties.
The structure of mixed {sup 3}He-{sup 4}He droplets doped with OCS: A density functional approach
Leal, Antonio; Mateo, David; Pi, Martí; Barranco, Manuel [Departament ECM, Facultat de Física and IN2UB, Universitat de Barcelona, Diagonal 645, 08028 Barcelona (Spain)] [Departament ECM, Facultat de Física and IN2UB, Universitat de Barcelona, Diagonal 645, 08028 Barcelona (Spain); Navarro, Jesús [IFIC (CSIC-Universidad de Valencia), P.O. Box 22085, E-46071 Valencia (Spain)] [IFIC (CSIC-Universidad de Valencia), P.O. Box 22085, E-46071 Valencia (Spain)
2013-11-07T23:59:59.000Z
We have investigated the structure and energetics of mixed {sup 3}He-{sup 4}He droplets doped with a carbonyl sulfide molecule within a density functional approach considering a small but finite temperature of 0.1 K. The molecule is treated as an external field to which the helium droplet is attached. The energetics and appearance of these droplets are discussed for selected numbers of helium atoms, identifying the first magic numbers of the fermionic component.
J. Terasaki; J. Engel
2011-05-19T23:59:59.000Z
Although nuclear energy density functionals are determined primarily by fitting to ground state properties, they are often applied in nuclear astrophysics to excited states, usually through the quasiparticle random phase approximation (QRPA). Here we test the Skyrme functionals SkM* and SLy4 along with the self-consistent QRPA by calculating properties of low-lying vibrational states in a large number of well-deformed even-even rare-earth nuclei. We reproduce trends in energies and transition probabilities associated with gamma-vibrational states, but our results are not perfect and indicate the presences of multi-particle-hole correlations that are not included in the QRPA. The Skyrme functional SkM* performs noticeably better than SLy4. In a few nuclei, changes in the treatment of the pairing energy functional have a significant effect. The QRPA is less successful with "beta-vibrational" states than with the gamma-vibrational states.
Potassium permeation through the KcsA channel: a density functional study
Guidoni, Leonardo
; Streptomyces lividans; Ab initio electronic structure calculation; Ionic selectivity; Electronic polarization of the electronic structure for potassium permeation, we have here under- taken a first principles Density-Parrinello Molecular Dynamics [19] and hybrid CPMD/MM calculations [20]. Our investigation is carried out in two steps
ATP Hydrolysis in Water -A Density Functional Study J. Akola and R. O. Jones*
), which exists in millimolar range concentrations. Nucleotides play critical and diverse roles in cellular-dependent hydrolysis reaction. Two paths for ATP hydrolysis in water with Mg2+ are studied here using the density, and a dissociative reaction involving a scission of the terminal bridging P-O bond. The latter has an activation
Analysis of Multiple Scalar Large-Eddy Simulation/Probability Density Function Formulation
Raman, Venkat
in the spray flame. Filtered density uj Filtered velocity W Filtered evaporation source term ~P Filtered term in PDF transport equation G() Spray evaporation correction term in PDF transport equation d for Turbulent Spray Combustion C. R. Heye , H. Koo and V. Raman Department of Aerospace Engineering
Crystallization of polyethylene by modified weighted density approximation(MWDA)
Razeghizadeh, Alireza; Lavafpour, Farhad
2015-01-01T23:59:59.000Z
In this article, we use the modified weighted density approximation to study the crystallization of polyethylene. We also use a direct correlation function of polyethylene based on RISM theory. The free energy of a polyethylene is calculated using density functional theory. The crystallization and solid and liquid density are calculated and finally compared with the prism simulation and experimental results. That shown the result obtained by MWDA is in better agreement, compared with the experimental result than the prism.
Crystallization of polyethylene by modified weighted density approximation(MWDA)
Alireza Razeghizadeh; Vahdat Rafee; Farhad Lavafpour
2015-02-07T23:59:59.000Z
In this article, we use the modified weighted density approximation to study the crystallization of polyethylene. We also use a direct correlation function of polyethylene based on RISM theory. The free energy of a polyethylene is calculated using density functional theory. The crystallization and solid and liquid density are calculated and finally compared with the prism simulation and experimental results. That shown the result obtained by MWDA is in better agreement, compared with the experimental result than the prism.
Chu, Shih-I; Zhou, Zhongyuan
2005-02-28T23:59:59.000Z
A spin-dependent density-functional approach for the calculation of highly and multiply excited state of atomic system is proposed based on the localized Hartree-Fock density-functional method and Slater’s diagonal sum rule. In this approach...
E*PCOS2009 Density functional simulations of phase change materials: disordered phases of Ge8Sb2Te75.0Te17.7 (AIST). These represent two families used widely as phase change materials: pseudobinary and more flexible than those of Ag. Key words: Phase change materials, density functional calculations
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.
Tian Hao
2014-09-05T23:59:59.000Z
Tap density of a granular powder is often linked to the flowability via Carr Index that measures how tight a powder can be packed, under an assumption that more easily packed powders usually flow poorly. Understanding how particles are packed is important for revealing why a powder flows better than others. There are two types of empirical equations that were proposed to fit the experimental data of packing fractions vs. numbers of taps in literature: The inverse logarithmic and the stretched exponential. Using the rate process theory and the free volume concept, we obtain the tap density equations and they can be reducible to the two empirical equations currently widely used in literature. Our equations could potentially fit experimental data better with an additional adjustable parameter. The tapping amplitude and frequency, the weight of the granular materials, and the environment temperature are grouped into one parameter that weighs the pace of packing process. The current results, in conjunction with our previous findings, may imply that both dry(granular)and wet(colloidal and polymeric) particle systems are governed by the same physical mechanisms in term of the role of the free volume and how particles behave (a rate controlled process).
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.
Banik, Sarmistha [BITS Pilani, Hyderabad Campus, Hyderabad-500078 (India); Hempel, Matthias [Departement Physik, Universität Basel, Klingelbergstrasse 82, 4056 Basel (Switzerland); Bandyopadhyay, Debades [Astroparticle Physics and Cosmology Division, Saha Institute of Nuclear Physics, 1/AF Bidhannagar, Kolkata-700064 (India)
2014-10-01T23:59:59.000Z
We develop new hyperon equation of state (EoS) tables for core-collapse supernova simulations and neutron stars. These EoS tables are based on a density-dependent relativistic hadron field theory where baryon-baryon interaction is mediated by mesons, using the parameter set DD2 for nucleons. Furthermore, light and heavy nuclei along with interacting nucleons are treated in the nuclear statistical equilibrium model of Hempel and Schaffner-Bielich which includes excluded volume effects. Of all possible hyperons, we consider only the contribution of ?s. We have developed two variants of hyperonic EoS tables: in the np?? case the repulsive hyperon-hyperon interaction mediated by the strange ? meson is taken into account, and in the np? case it is not. The EoS tables for the two cases encompass a wide range of densities (10{sup –12} to ?1 fm{sup –3}), temperatures (0.1 to 158.48 MeV), and proton fractions (0.01 to 0.60). The effects of ? hyperons on thermodynamic quantities such as free energy per baryon, pressure, or entropy per baryon are investigated and found to be significant at higher densities. The cold, ?-equilibrated EoS (with the crust included self-consistently) results in a 2.1 M {sub ?} maximum mass neutron star for the np?? case, whereas that for the np? case is 1.95 M {sub ?}. The np?? EoS represents the first supernova EoS table involving hyperons that is directly compatible with the recently measured 2 M {sub ?} neutron stars.
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.
Berland, Kristian
2013-01-01T23:59:59.000Z
The adsorption of benzene and C60 on graphene and boron nitride (BN) is studied using density functional theory with the non-local correlation functional vdW-DF. By comparing these systems we can systematically investigate their adsorption nature and differences between the two functional versions vdW-DF1 and vdW-DF2. The bigger size of the C60 molecule makes it bind stronger to the surface than benzene, yet the interface between the molecules and the sheets are similar in nature. The binding separation is more sensitive to the exchange variant used in vdW-DF than to the correlation version. This result is related to the exchange and correlation components of the potential energy curve (PEC). We show that a moderate dipole forms for C60 on graphene, unlike for the other adsorption systems. We find that the corrugation is very sensitive to the variant or version of vdW-DF used, in particular the exchange. Further, we show that this sensitivity arise indirectly through the shift in binding separation caused by ...
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.
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
Freezing of a two dimensional fluid in to a crystalline phase : Density functional approach
Anubha Jaiswal; Swarn L. Singh; Yashwant Singh
2012-10-02T23:59:59.000Z
A free-energy functional for a crystal proposed by Singh and Singh (Europhys. Lett. {\\bf {88}}, 16005 (2009)) and which contains both the symmetry conserved and symmetry broken parts of the direct pair correlation function has been used to investigate the crystallization of a two-dimensional fluid. The results found for fluids interacting via the inverse power potential $ u(r)= \\epsilon ({\\sigma}/{r})^{n} $ for n= 3, 6 and 12 are in good agreement with experimental and simulation results. The contribution made by the symmetry broken part to the grand thermodynamic potential at the freezing point is found to increase with the softness of the potential. Our results explain why the Ramakrishnan-Yussouff (Phys. Rev. B {\\bf 19}, 2775 (1979)) free-energy functional gave good account of freezing transitions of hard-core potentials but failed for potentials that have soft core and/or attractive tail.
Tools for incorporating a D-wave contribution in Skyrme energy density functionals
P. Becker; D. Davesne; J. Meyer; A. Pastore; J. Navarro
2014-06-02T23:59:59.000Z
The possibility of adding a D-wave term to the standard Skyrme effective interaction has been widely considered in the past. Such a term has been shown to appear in the next-to-next-to-leading order of the Skyrme pseudo-potential. The aim of the present article is to provide the necessary tools to incorporate this term in a fitting procedure: first, a mean-field equation written in spherical symmetry in order to describe spherical nuclei and second, the response function to detect unphysical instabilities. With these tools it will be possible to build a new fitting procedure to determine the coupling constants of the new functional.
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.
Christian Iliadis; Richard Longland; Art Champagne; Alain Coc; Ryan Fitzgerald
2010-04-23T23:59:59.000Z
Numerical values of charged-particle thermonuclear reaction rates for nuclei in the A=14 to 40 region are tabulated. The results are obtained using a method, based on Monte Carlo techniques, that has been described in the preceding paper of this series (Paper I). We present a low rate, median rate and high rate which correspond to the 0.16, 0.50 and 0.84 quantiles, respectively, of the cumulative reaction rate distribution. The meaning of these quantities is in general different from the commonly reported, but statistically meaningless expressions, "lower limit", "nominal value" and "upper limit" of the total reaction rate. In addition, we approximate the Monte Carlo probability density function of the total reaction rate by a lognormal distribution and tabulate the lognormal parameters {\\mu} and {\\sigma} at each temperature. We also provide a quantitative measure (Anderson-Darling test statistic) for the reliability of the lognormal approximation. The user can implement the approximate lognormal reaction rate probability density functions directly in a stellar model code for studies of stellar energy generation and nucleosynthesis. For each reaction, the Monte Carlo reaction rate probability density functions, together with their lognormal approximations, are displayed graphically for selected temperatures in order to provide a visual impression. Our new reaction rates are appropriate for bare nuclei in the laboratory. The nuclear physics input used to derive our reaction rates is presented in the subsequent paper of this series (Paper III). In the fourth paper of this series (Paper IV) we compare our new reaction rates to previous results.
Universal Nuclear Energy Density Functional: Tools and Resources from the UNEDF SciDAC Collaboration
DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]
UNEDF supports the Low-Energy Nuclear Physics National HPC Initiative. There are approximately 3,000 known nuclei, most of them produced in the laboratory, with an additional 6,000 that could in principle still be created. An understanding of the properties of these elements is crucial for future energy and defense applications. The long-term vision of UNEF is to arrive at a comprehensive and unified description of nuclei and their reactions, grounded in the fundamental interactions between the constituent nucleons. It seeks 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.
Probability density functions for the variable solar wind near the solar cycle minimum
Vörös,; Leitner, M; Narita, Y; Consolini, G; Kovács, P; Tóth, A; Lichtenberger, J
2015-01-01T23:59:59.000Z
Unconditional and conditional statistics is used for studying the histograms of magnetic field multi-scale fluctuations in the solar wind near the solar cycle minimum in 2008. The unconditional statistics involves the magnetic data during the whole year 2008. The conditional statistics involves the magnetic field time series splitted into concatenated subsets of data according to a threshold in dynamic pressure. The threshold separates fast stream leading edge compressional and trailing edge uncompressional fluctuations. The histograms obtained from these data sets are associated with both large-scale (B) and small-scale ({\\delta}B) magnetic fluctuations, the latter corresponding to time-delayed differences. It is shown here that, by keeping flexibility but avoiding the unnecessary redundancy in modeling, the histograms can be effectively described by a limited set of theoretical probability distribution functions (PDFs), such as the normal, log-normal, kappa and logkappa functions. In a statistical sense the...
Venturi, D. [Division of Applied Mathematics, Brown University, Providence, RI 02912 (United States)] [Division of Applied Mathematics, Brown University, Providence, RI 02912 (United States); Karniadakis, G.E., E-mail: george_karniadakis@brown.edu [Division of Applied Mathematics, Brown University, Providence, RI 02912 (United States)
2012-08-30T23:59:59.000Z
By using functional integral methods we determine new evolution equations satisfied by the joint response-excitation probability density function (PDF) associated with the stochastic solution to first-order nonlinear partial differential equations (PDEs). The theory is presented for both fully nonlinear and for quasilinear scalar PDEs subject to random boundary conditions, random initial conditions or random forcing terms. Particular applications are discussed for the classical linear and nonlinear advection equations and for the advection-reaction equation. By using a Fourier-Galerkin spectral method we obtain numerical solutions of the proposed response-excitation PDF equations. These numerical solutions are compared against those obtained by using more conventional statistical approaches such as probabilistic collocation and multi-element probabilistic collocation methods. It is found that the response-excitation approach yields accurate predictions of the statistical properties of the system. In addition, it allows to directly ascertain the tails of probabilistic distributions, thus facilitating the assessment of rare events and associated risks. The computational cost of the response-excitation method is order magnitudes smaller than the one of more conventional statistical approaches if the PDE is subject to high-dimensional random boundary or initial conditions. The question of high-dimensionality for evolution equations involving multidimensional joint response-excitation PDFs is also addressed.
Rodriguez-Guzman, R
2014-01-01T23:59:59.000Z
The most recent parametrization D1M of the Gogny energy density functional is used to describe fission in the isotopes $^{232-280}$ Pu. We resort to the methodology introduced in our previous studies [Phys. Rev. C \\textbf{88}, 054325 (2013) and Phys. Rev. C \\textbf {89}, 054310 (2014)] to compute the fission paths, collective masses and zero point quantum corrections within the Hartree-Fock-Bogoliubov framework. The systematics of the spontaneous fission half-lives t$_{SF}$, masses and charges of the fragments in Plutonium isotopes is analyzed and compared with available experimental data. We also pay attention to isomeric states, the deformation properties of the fragments as well as to the competition between the spontaneous fission and $\\alpha$-decay modes. The impact of pairing correlations on the predicted t$_{SF}$ values is demonstrated with the help of calculations for $^{232-280}$Pu in which the pairing strengths of the Gogny-D1M energy density functional are modified by 5 $\\%$ and 10 $\\%$, respective...
R. Rodriguez-Guzman; L. M. Robledo
2014-05-27T23:59:59.000Z
The most recent parametrization D1M of the Gogny energy density functional is used to describe fission in the isotopes $^{232-280}$ Pu. We resort to the methodology introduced in our previous studies [Phys. Rev. C \\textbf{88}, 054325 (2013) and Phys. Rev. C \\textbf {89}, 054310 (2014)] to compute the fission paths, collective masses and zero point quantum corrections within the Hartree-Fock-Bogoliubov framework. The systematics of the spontaneous fission half-lives t$_{SF}$, masses and charges of the fragments in Plutonium isotopes is analyzed and compared with available experimental data. We also pay attention to isomeric states, the deformation properties of the fragments as well as to the competition between the spontaneous fission and $\\alpha$-decay modes. The impact of pairing correlations on the predicted t$_{SF}$ values is demonstrated with the help of calculations for $^{232-280}$Pu in which the pairing strengths of the Gogny-D1M energy density functional are modified by 5 $\\%$ and 10 $\\%$, respectively. We further validate the use of the D1M parametrization through the discussion of the half-lives in $^{242-262}$Fm. Our calculations corroborate that, though the uncertainties in the absolute values of physical observables are large, the Gogny-D1M Hartree-Fock-Bogoliubov framework still reproduces the trends with mass and/or neutron numbers and therefore represents a reasonable starting point to describe fission in heavy nuclear systems from a microscopic point of view.
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.
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.
An extended SMLD approach for presumed probability density function in flamelet combustion model
Coclite, Alessandro; De Palma, Pietro; Cutrone, Luigi
2013-01-01T23:59:59.000Z
This paper provides an extension of the standard flamelet progress variable (FPV) approach for turbulent combustion, applying the statistically most likely distribution (SMLD) framework to the joint PDF of the mixture fraction, Z, and the progress variable, C. In this way one does not need to make any assumption about the statistical correlation between Z and C and about the behaviour of the mixture fraction, as required in previous FPV models. In fact, for state-of-the-art models, with the assumption of very-fast-chemistry,Z is widely accepted to behave as a passive scalar characterized by a $\\beta$-distribution function. Instead, the model proposed here, evaluates the most probable joint distribution of Z and C without any assumption on their behaviour and provides an effective tool to verify the adequateness of widely used hypotheses, such as their statistical independence. The model is validated versus three well-known test cases, namely, the Sandia flames. The results are compared with those obtained by ...
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.
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.
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.
H. Mei; K. Hagino; J. M. Yao; T. Motoba
2015-04-20T23:59:59.000Z
We present a detailed formalism of the microscopic particle-rotor model for hypernuclear low-lying states based on a covariant density functional theory. In this method, the hypernuclear states are constructed by coupling a hyperon to low-lying states of the core nucleus, which are described by the generator coordinate method (GCM) with the particle number and angular momentum projections. We apply this method to study in detail the low-lying spectrum of $^{13}_{~\\Lambda}$C and $^{21}_{~\\Lambda}$Ne hypernuclei. We also briefly discuss the structure of $^{155}_{~~\\Lambda}$Sm as an example of heavy deformed hypernuclei. It is shown that the low-lying excitation spectrum with positive parity states of the hypernuclei, which are dominated by $\\Lambda$ hyperon in $s$-orbital coupled to the core states, are similar to that for the corresponding core states, while the electric quadrupole transition strength, $B(E2)$, from the 2$^+_1$ state to the ground state is reduced according to the mass number of the hypernuclei. Our study indicates that the energy splitting between the first 1/2$^-$ and 3/2$^-$ hypernuclear states is generally small for all the hypernuclei which we study. However, their configurations depend much on the properties of a core nucleus, in particular on the sign of deformation parameter. That is, the first $1/2^-$ and $3/2^-$ states in $^{13}_{~\\Lambda}$C are dominated by a single configuration with $\\Lambda$ particle in the $p$-wave orbits and thus providing good candidates for a study of the $\\Lambda$ spin-orbit splitting. On the other hand, those states in the other hypernuclei exhibit a large configuration mixing and thus their energy difference cannot be interpreted as the spin-orbit splitting for the $p$-orbits.
A. M. Sukhovoj; V. A. Khitrov
2010-09-24T23:59:59.000Z
From a comparison of the total gamma-spectra calculated for different functional dependencies of level density and radiative strength functions, there were obtained both their square root relative differences and analogous data for the used parameters. The analysis of these data showed that the total uncertainty in determination of gamma-spectra intensities which is necessary to obtain reliable values of parameters of cascade gamma-decay, most probably, must not exceed one percent.
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
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.
Yue Shi; J. Dobaczewski; P. T. Greenlees
2014-03-08T23:59:59.000Z
Nuclei in the $Z\\approx100$ mass region represent the heaviest systems where detailed spectroscopic information is experimentally available. Although microscopic-macroscopic and self-consistent models have achieved great success in describing the data in this mass region, a fully satisfying precise theoretical description is still missing. By using fine-tuned parametrizations of the energy density functionals, the present work aims at an improved description of the single-particle properties and rotational bands in the nobelium region. Such locally optimized parameterizations may have better properties when extrapolating towards the superheavy region. Skyrme-Hartree-Fock-Bogolyubov and Lipkin-Nogami methods were used to calculate the quasiparticle energies and rotational bands of nuclei in the nobelium region. Starting from the most recent Skyrme parametrization, UNEDF1, the spin-orbit coupling constants and pairing strengths have been tuned, so as to achieve a better agreement with the excitation spectra and odd-even mass differences in $^{251}$Cf and $^{249}$Bk. The quasiparticle properties of $^{251}$Cf and $^{249}$Bk were very well reproduced. At the same time, crucial deformed neutron and proton shell gaps open up at $N=152$ and $Z=100$, respectively. Rotational bands in Fm, No, and Rf isotopes, where experimental data are available, were also fairly well described. To help future improvements towards a more precise description, small deficiencies of the approach were carefully identified. In the $Z\\approx100$ mass region, larger spin-orbit strengths than those from global adjustments lead to improved agreement with data. Puzzling effects of particle-number restoration on the calculated moment of inertia, at odds with the experimental behaviour, require further scrutiny.
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.
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...
Bozkaya, U?ur, E-mail: ugur.bozkaya@atauni.edu.tr [Department of Chemistry, Atatürk University, Erzurum 25240, Turkey and Department of Chemistry, Middle East Technical University, Ankara 06800 (Turkey)
2014-09-28T23:59:59.000Z
General analytic gradient expressions (with the frozen-core approximation) are presented for density-fitted post-HF methods. An efficient implementation of frozen-core analytic gradients for the second-order Møller–Plesset perturbation theory (MP2) with the density-fitting (DF) approximation (applying to both reference and correlation energies), which is denoted as DF-MP2, is reported. The DF-MP2 method is applied to a set of alkanes, conjugated dienes, and noncovalent interaction complexes to compare the computational cost of single point analytic gradients with MP2 with the resolution of the identity approach (RI-MP2) [F. Weigend and M. Häser, Theor. Chem. Acc. 97, 331 (1997); R. A. Distasio, R. P. Steele, Y. M. Rhee, Y. Shao, and M. Head-Gordon, J. Comput. Chem. 28, 839 (2007)]. In the RI-MP2 method, the DF approach is used only for the correlation energy. Our results demonstrate that the DF-MP2 method substantially accelerate the RI-MP2 method for analytic gradient computations due to the reduced input/output (I/O) time. Because in the DF-MP2 method the DF approach is used for both reference and correlation energies, the storage of 4-index electron repulsion integrals (ERIs) are avoided, 3-index ERI tensors are employed instead. Further, as in case of integrals, our gradient equation is completely avoid construction or storage of the 4-index two-particle density matrix (TPDM), instead we use 2- and 3-index TPDMs. Hence, the I/O bottleneck of a gradient computation is significantly overcome. Therefore, the cost of the generalized-Fock matrix (GFM), TPDM, solution of Z-vector equations, the back transformation of TPDM, and integral derivatives are substantially reduced when the DF approach is used for the entire energy expression. Further application results show that the DF approach introduce negligible errors for closed-shell reaction energies and equilibrium bond lengths.
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
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.
A density functional theory study of atomic steps on stoichiometric rutile TiO{sub 2}(110)
Stausholm-Møller, Jess; Kristoffersen, Henrik Høgh; Martinez, Umberto; Hammer, Bjørk [Interdisciplinary Nanoscience Center (iNANO) and Department of Physics and Astronomy, Aarhus University, DK-8000 Aarhus C (Denmark)] [Interdisciplinary Nanoscience Center (iNANO) and Department of Physics and Astronomy, Aarhus University, DK-8000 Aarhus C (Denmark)
2013-12-21T23:59:59.000Z
We present a detailed theoretical study of the energetics of stoichiometric steps on the (110) surface of rutile TiO{sub 2}. Step structures running along the ?001?, ?11{sup ¯}1?, and ?11{sup ¯}0? directions including bulk-terminations and possible reconstructions have been considered. A robust method for extracting surface and step energies of vicinal surfaces, where the surface energies converge slowly with respect to slab thickness, is outlined and used. Based on the calculated step energies a 2D Wulff-construction is presented from which it can be concluded that in equilibrium only oxygen terminated steps running along the ?001? directions and reconstructed steps along the ?11{sup ¯}1? directions should be present. Finally it is found that under conditions of stoichiometry the reconstructed ?11{sup ¯}1? steps should be more than twice as abundant as oxygen terminated ?001? steps.
Ab initio density functional theory study of uranium solubility in Gd2Zr2O7 pyrochlore
Chen, Qing-yun; Meng, Chuan-min; Liao, Chang-zhong; Wang, Lie-lin; Xie, Hua; Lv, Hui-yi; Wu, Tao; Ji, Shi-yin; Huang, Yu-zhu
2015-01-01T23:59:59.000Z
In this study, an ab initio calculation is performed to investigate the uranium solubility in different sites of Gd2Zr2O7 pyrochlore. The Gd2Zr2O7 maintains its pyrochlore structure at low uranium dopant levels, and the lattice constants of Gd2(Zr2-yUy)O7 and (Gd2-yUy)Zr2O7 are generally expressed as being linearly related to the uranium content y. Uranium is found to be a preferable substitute for the B-site gadolinium atoms in cation-disordered Gd2Zr2O7 (where gadolinium and zirconium atoms are swapped) over the A-site gadolinium atoms in ordered Gd2Zr2O7 due to the lower total energy of (Gd2-yZry)(Zr2-yUy)O7. The theoretical findings present a reasonable explanation of recent experiment results.
Florian, Libisch
an accurate and efficient way to study properties of iso- lated defects in semiconductors. C 2015 AIP types of solid state materials and play important roles in engineering material properties. The presence of defects significantly affects the chemical, electrical, optical, and mechanical properties of the material
Truong, Thanh N.
-Bound Nitrogen during Combustion Alejandro Montoya,, Thanh N. Truong,*,§ and Adel F. Sarofim Department. The calculations were carried out to simulate combustion conditions resulting in the absence and presence and in stratospheric ozone depletion. One of the anthropogenic sources of N2O is the combustion of coal, particularly
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
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
Li, Weixue
of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China a b s t r
Li, Weixue
... surfaces Ming-Mei Yang State Key Laboratory Of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, China and Graduate School of the Chinese Academy of Sciences, Beijing 100039, China Xin-He Bao State Key Laboratory Of Catalysis, Dalian Institute of Chemical
Photovoltaic properties and size-pH phase stability of iron disulfide from density-functional theory
Sun, Ruoshi
2013-01-01T23:59:59.000Z
Despite its exceptional optical absorptivity, suitable band gap, and earth abundance, the low open-circuit voltage of pyrite FeS? has remained the biggest challenge preventing its use in photovoltaic devices. Two widely-accepted ...
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
Prepr. Pap.-Am. Chem. Soc., Div. Fuel Chem. 2004, 49 (2), xxxx DENSITY FUNCTIONAL THEORY STUDY OF
Truong, Thanh N.
OF CARBON-H2O REACTIONS DURING GASIFICATION WITH STEAM Juan F. Espinal,1 Fanor Mondragón,1 and Thanh N of Chemistry, University of Utah Salt Lake City, Utah, USA 84112 Introduction Carbon gasification is an alternative process to the combustion of coal since it produces less pollution and is more efficient
Truong, Thanh N.
are of particular importance to coal chemistry, such as those in coal gasification and combustion. Previous surface involved in the process of gasification and combustion has a turbostratic character where the adsorption of NO to illustrate the effects of the spin contamination because of its importance in coal
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...
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 ...
Chu, Shih-I
and structures PACS 85.65.+h Molecular electronic devices PACS 71.15.Pd Molecular dynamics calculations (Carr for electron transport dynamics in molecular devices Zhongyuan Zhou(a) and Shih-I Chu Department of Chemistry. The electron wave function is calculated by solving this equation in a finite P-space volume. This approach
Kim, Sejoong
We present a first-principles approach for inelastic quantum transport calculations based on maximally localized Wannier functions. Electronic-structure properties are obtained from density-functional theory in a plane-wave ...
Berland, Kristian [Chalmers University of Technology, Sweden; Cooper, Valentino R [ORNL; Langreth, David C. [Rutgers University; Schroder, Prof. Elsebeth [Chalmers University of Technology, Sweden; Chakarova-Kack, Svetla [Chalmers University of Technology, Sweden
2011-01-01T23:59:59.000Z
The adsorption of an adenine molecule on graphene is studied using a first-principles van der Waals functional (vdW-DF) [Dion et al., Phys. Rev. Lett. 92, 246401 (2004)]. The cohesive energy of an ordered adenine overlayer is also estimated. For the adsorption of a single molecule, we determine the optimal binding configuration and adsorption energy by translating and rotating the molecule. The adsorption energy for a single molecule of adenine is found to be 711 meV, which is close to the calculated adsorption energy of the similar-sized naphthalene. Based on the single molecular binding configuration, we estimate the cohesive energy of a two-dimensional ordered overlayer. We find a significantly stronger binding energy for the ordered overlayer than for single-molecule adsorption.
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
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.
Generalized Holographic Quantum Criticality at Finite Density
B. Goutéraux; E. Kiritsis
2013-01-23T23:59:59.000Z
We show that the near-extremal solutions of Einstein-Maxwell-Dilaton theories, studied in ArXiv:1005.4690, provide IR quantum critical geometries, by embedding classes of them in higher-dimensional AdS and Lifshitz solutions. This explains the scaling of their thermodynamic functions and their IR transport coefficients, the nature of their spectra, the Gubser bound, and regulates their singularities. We propose that these are the most general quantum critical IR asymptotics at finite density of EMD theories.
Duguet, T; Ebran, J -P; Lesinski, T; Somà, V
2015-01-01T23:59:59.000Z
This programmatic paper lays down the possibility to reconcile the necessity to resum many-body correlations into the energy kernel with the fact that safe multi-reference energy density functional (EDF) calculations cannot be achieved whenever the Pauli principle is not strictly enforced, as is for example the case when many-body correlations are parametrized under the form of empirical density dependencies. Our proposal is to exploit a newly developed ab initio many-body formalism to guide the construction of safe, explicitly correlated and systematically improvable parametrizations of the {\\it off-diagonal} energy and norm kernels that lie at the heart of the nuclear EDF method. The many-body formalism of interest relies on the concepts of symmetry breaking {\\it and} restoration that have made the fortune of the nuclear EDF method and is, as such, amenable to this guidance. After elaborating on our proposal, we briefly outline the project we plan to execute in the years to come.
T. Duguet; M. Bender; J. -P. Ebran; T. Lesinski; V. Somà
2015-02-12T23:59:59.000Z
This programmatic paper lays down the possibility to reconcile the necessity to resum many-body correlations into the energy kernel with the fact that safe multi-reference energy density functional (EDF) calculations cannot be achieved whenever the Pauli principle is not strictly enforced, as is for example the case when many-body correlations are parametrized under the form of empirical density dependencies. Our proposal is to exploit a newly developed ab initio many-body formalism to guide the construction of safe, explicitly correlated and systematically improvable parametrizations of the {\\it off-diagonal} energy and norm kernels that lie at the heart of the nuclear EDF method. The many-body formalism of interest relies on the concepts of symmetry breaking {\\it and} restoration that have made the fortune of the nuclear EDF method and is, as such, amenable to this guidance. After elaborating on our proposal, we briefly outline the project we plan to execute in the years to come.
Masao Iwamatsu; Yutaka Okabe
2010-06-11T23:59:59.000Z
The square-gradient density-functional model with triple-parabolic free energy, that was used previously to study the homogeneous bubble nucleation [J. Chem. Phys. 129, 104508 (2008)], is used to study the stability of the critical bubble nucleated within the bulk under-saturated stretched fluid. The stability of the bubble is studied by solving the Schr\\"odinger equation for the fluctuation. The negative eigenvalue corresponds to the unstable growing mode of the fluctuation. Our results show that there is only one negative eigenvalue whose eigenfunction represents the fluctuation that corresponds to the isotropically growing or shrinking nucleus. In particular, this negative eigenvalue survives up to the spinodal point. Therefore the critical bubble is not fractal or ramified near the spinodal.
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.
Rappe, Andrew M.
Hybrid density functional calculations of the band gap of GaxIn1-xN Xifan Wu,1 Eric J. Walter,2 Andrew M. Rappe,3 Roberto Car,1 and Annabella Selloni1 1Chemistry Department, Princeton University Recent theoretical work has provided evidence that hybrid functionals, which include a fraction of exact
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.
Takashima, A.; Onoe, J. [Department of Nuclear Engineering and Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology, O-okayama, Meguro, Tokyo 152-8550 (Japan); Nishii, T. [Technology Development Center, Electric Power Development Co., Ltd. (J-Power), Chigasaki, Kanagawa 253-0041 (Japan)
2010-08-15T23:59:59.000Z
We have examined the infrared (IR) spectra of electron-beam (EB) irradiated C{sub 60} films, using in situ IR spectroscopy in the temperature range of 60-300 K. The irradiation-time evolution of the IR spectra shows that two highly intense new peaks finally appear around 565 and 1340 cm{sup -1} when the EB-induced C{sub 60} polymerization was saturated. To determine the cross-linked structure of the polymer explicitly, we have compared the IR spectra with theoretical spectra obtained from the cross-linked structure of all C{sub 120} stable isomers derived from the general Stone-Wales (GSW) rearrangement, using first-principles density-functional calculations. Since each C{sub 120} isomer has the same cross-linked structure as that of its corresponding one-dimensional (1D) C{sub 60} polymer, the IR modes obtained from the cross-linked structure of C{sub 120} are close to those obtained from the corresponding 1D polymer. Comparison between the experimental and theoretical IR spectra suggests that the 1D peanut-shaped C{sub 60} polymer has a cross-linked structure roughly similar to that of the P08 peanut-shaped C{sub 120} isomer.
Ju, J.; Döpp, A.; Cros, B. [Laboratoire de Physique des Gaz et des Plasmas, CNRS-Université Paris-Sud, 91405 Orsay (France)] [Laboratoire de Physique des Gaz et des Plasmas, CNRS-Université Paris-Sud, 91405 Orsay (France); Svensson, K.; Genoud, G.; Wojda, F.; Burza, M.; Persson, A.; Lundh, O.; Wahlström, C.-G. [Department of Physics, Lund University, P.O. Box 118, S-22100 Lund (Sweden)] [Department of Physics, Lund University, P.O. Box 118, S-22100 Lund (Sweden); Ferrari, H. [Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET) and CNEA-CAB (Argentina)] [Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET) and CNEA-CAB (Argentina)
2013-08-15T23:59:59.000Z
Laser wakefield electron acceleration in the blow-out regime and the associated betatron X-ray radiation were investigated experimentally as a function of the plasma density in a configuration where the laser is guided. Dielectric capillary tubes were employed to assist the laser keeping self-focused over a long distance by collecting the laser energy around its central focal spot. With a 40 fs, 16 TW pulsed laser, electron bunches with tens of pC charge were measured to be accelerated to an energy up to 300 MeV, accompanied by X-ray emission with a peak brightness of the order of 10{sup 21} ph/s/mm{sup 2}/mrad{sup 2}/0.1%BW. Electron trapping and acceleration were studied using the emitted X-ray beam distribution to map the acceleration process; the number of betatron oscillations performed by the electrons was inferred from the correlation between measured X-ray fluence and beam charge. A study of the stability of electron and X-ray generation suggests that the fluctuation of X-ray emission can be reduced by stabilizing the beam charge. The experimental results are in good agreement with 3D particle-in-cell (PIC) simulation.
Masao Iwamatsu
2009-04-04T23:59:59.000Z
The generic square-gradient density-functional model with triple-parabolic free energy is used to study the stability of a cavity introduced into the stretched liquid. The various properties of the critical cavity, which is the largest stable cavity within the liquid, are compared with those of the critical bubble of the homogeneous bubble nucleation. It is found that the size of the critical cavity is always smaller than that of the critical bubble, while the work of formation of the former is always higher than the latter in accordance with the conjectures made by Punnathanam and Corti [J. Chem. Phys. {\\bf 119}, 10224 (2003)] deduced from the Lennard-Jones fluids. Therefore their conjectures about the critical cavity size and the work of formation would be more general and valid even for other types of liquid such as metallic liquid or amorphous. However, the scaling relations they found for the critical cavity in the Lennard-Jones fluid are marginally satisfied only near the spinodal.
Density matrix of black hole radiation
Lasma Alberte; Ram Brustein; Andrei Khmelnitsky; A. J. M. Medved
2015-02-09T23:59:59.000Z
Hawking's model of black hole evaporation is not unitary and leads to a mixed density matrix for the emitted radiation, while the Page model describes a unitary evaporation process in which the density matrix evolves from an almost thermal state to a pure state. We compare a recently proposed model of semiclassical black hole evaporation to the two established models. In particular, we study the density matrix of the outgoing radiation and determine how the magnitude of the off-diagonal corrections differs for the three frameworks. For Hawking's model, we find power-law corrections to the two-point functions that induce exponentially suppressed corrections to the off-diagonal elements of the full density matrix. This verifies that the Hawking result is correct to all orders in perturbation theory and also allows one to express the full density matrix in terms of the single-particle density matrix. We then consider the semiclassical theory for which the corrections, being non-perturbative from an effective field-theory perspective, are much less suppressed and grow monotonically in time. In this case, the R\\'enyi entropy for the outgoing radiation is shown to grow linearly at early times; but this growth slows down and the entropy eventually starts to decrease at the Page time. In addition to comparing models, we emphasize the distinction between the state of the radiation emitted from a black hole, which is highly quantum, and that of the radiation emitted from a typical classical black body at the same temperature.
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.
Modelling charge transfer reactions with the frozen density embedding formalism
Pavanello, Michele [Gorlaeus Laboratories, Leiden Institute of Chemistry, Leiden University, P.O. Box 9502, 2300 RA Leiden (Netherlands); Neugebauer, Johannes [Institute for Physical and Theoretical Chemistry, Technische Universitaet Braunschweig, Hans-Sommer-Strasse 10, 38106 Braunschweig (Germany)
2011-12-21T23:59:59.000Z
The frozen density embedding (FDE) subsystem formulation of density-functional theory is a useful tool for studying charge transfer reactions. In this work charge-localized, diabatic states are generated directly with FDE and used to calculate electronic couplings of hole transfer reactions in two {pi}-stacked nucleobase dimers of B-DNA: 5{sup '}-GG-3{sup '} and 5{sup '}-GT-3{sup '}. The calculations rely on two assumptions: the two-state model, and a small differential overlap between donor and acceptor subsystem densities. The resulting electronic couplings agree well with benchmark values for those exchange-correlation functionals that contain a high percentage of exact exchange. Instead, when semilocal GGA functionals are used the electronic couplings are grossly overestimated.
Boyer, Edmond
of water content and bulk density K. Saffih-Hdadi1 , P. Défossez2 , G. Richard3 , Y-J. Cui4 , A-M. Tang4 physical properties. Because the soil compaction depends on its water content, bulk density and texture between soil mechanical properties and easily measurable soil properties as well as water content and bulk
W. Z. Jiang; Z. Z. Ren; Z. Q. Sheng; Z. Y. Zhu
2010-04-11T23:59:59.000Z
The relationship between deexcitation energies of superdeformed secondary minima relative to ground states and the density dependence of the symmetry energy is investigated for heavy nuclei using the relativistic mean field (RMF) model. It is shown that the deexcitation energies of superdeformed secondary minima are sensitive to differences in the symmetry energy that are mimicked by the isoscalar-isovector coupling included in the model. With deliberate investigations on a few Hg isotopes that have data of deexcitation energies, we find that the description for the deexcitation energies can be improved due to the softening of the symmetry energy. Further, we have investigated deexcitation energies of odd-odd heavy nuclei that are nearly independent of pairing correlations, and have discussed the possible extraction of the constraint on the density dependence of the symmetry energy with the measurement of deexcitation energies of these nuclei.