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Sample records for md density functional

  1. RADIATION PRESSURE DETECTION AND DENSITY ESTIMATE FOR 2011 MD

    SciTech Connect (OSTI)

    Micheli, Marco; Tholen, David J.; Elliott, Garrett T. E-mail: tholen@ifa.hawaii.edu

    2014-06-10

    We present our astrometric observations of the small near-Earth object 2011 MD (H ? 28.0), obtained after its very close fly-by to Earth in 2011 June. Our set of observations extends the observational arc to 73 days, and, together with the published astrometry obtained around the Earth fly-by, allows a direct detection of the effect of radiation pressure on the object, with a confidence of 5?. The detection can be used to put constraints on the density of the object, pointing to either an unexpectedly low value of ?=(640±330)kg m{sup ?3} (68% confidence interval) if we assume a typical probability distribution for the unknown albedo, or to an unusually high reflectivity of its surface. This result may have important implications both in terms of impact hazard from small objects and in light of a possible retrieval of this target.

  2. Laboratory Density Functionals

    E-Print Network [OSTI]

    B. G. Giraud

    2007-07-26

    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.

  3. Density-dependent covariant energy density functionals

    SciTech Connect (OSTI)

    Lalazissis, G. A.

    2012-10-20

    Relativistic nuclear energy density functionals are applied to the description of a variety of nuclear structure phenomena at and away fromstability line. Isoscalar monopole, isovector dipole and isoscalar quadrupole giant resonances are calculated using fully self-consistent relativistic quasiparticle randomphase approximation, based on the relativistic Hartree-Bogoliubovmodel. The impact of pairing correlations on the fission barriers in heavy and superheavy nuclei is examined. The role of pion in constructing desnity functionals is also investigated.

  4. Bivariate lognormal density function 

    E-Print Network [OSTI]

    Schreyer, Glenn William

    1972-01-01

    . 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...

  5. Phenomenological Relativistic Energy Density Functionals

    SciTech Connect (OSTI)

    Lalazissis, G. A.; Kartzikos, S.; Niksic, T.; Paar, N.; Vretenar, D.; Ring, P.

    2009-08-26

    The framework of relativistic nuclear energy density functionals is applied to the description of a variety of nuclear structure phenomena, not only in spherical and deformed nuclei along the valley of beta-stability, but also in exotic systems with extreme isospin values and close to the particle drip-lines. Dynamical aspects of exotic nuclear structure is explored using the fully consistent quasiparticle random-phase approximation based on the relativistic Hartree-Bogoliubov model. Recent applications of energy density functionals with explicit density dependence of the meson-nucleon couplings are presented.

  6. Jacek Dobaczewski Density functional theory and energy

    E-Print Network [OSTI]

    Dobaczewski, Jacek

    Jacek Dobaczewski Density functional theory and energy density functionals in nuclear physics Jacek UNEDFCollaboration,http://unedf.org/ Universal Nuclear Energy Density FunctionalUniversal Nuclear Energy Density in Poland per voivodship Energy density functional 245 647 Price voivodship functional 654 763 295 580

  7. Time Dependent Density Functional Theory An introduction

    E-Print Network [OSTI]

    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

  8. About density functional theory interpretation

    E-Print Network [OSTI]

    Kirill Koshelev

    2015-05-28

    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.

  9. Gedanken densities and exact constraints in density functional theory

    SciTech Connect (OSTI)

    Perdew, John P.; Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122 ; Ruzsinszky, Adrienn; Sun, Jianwei; Burke, Kieron

    2014-05-14

    Approximations to the exact density functional for the exchange-correlation energy of a many-electron ground state can be constructed by satisfying constraints that are universal, i.e., valid for all electron densities. Gedanken densities are designed for the purpose of this construction, but need not be realistic. The uniform electron gas is an old gedanken density. Here, we propose a spherical two-electron gedanken density in which the dimensionless density gradient can be an arbitrary positive constant wherever the density is non-zero. The Lieb-Oxford lower bound on the exchange energy can be satisfied within a generalized gradient approximation (GGA) by bounding its enhancement factor or simplest GGA exchange-energy density. This enhancement-factor bound is well known to be sufficient, but our gedanken density shows that it is also necessary. The conventional exact exchange-energy density satisfies no such local bound, but energy densities are not unique, and the simplest GGA exchange-energy density is not an approximation to it. We further derive a strongly and optimally tightened bound on the exchange enhancement factor of a two-electron density, which is satisfied by the local density approximation but is violated by all published GGA's or meta-GGA’s. Finally, some consequences of the non-uniform density-scaling behavior for the asymptotics of the exchange enhancement factor of a GGA or meta-GGA are given.

  10. Density Functional Theory (DFT) Rob Parrish

    E-Print Network [OSTI]

    Sherrill, David

    · References 2 #12;Wavefunction Approach 3 Hydrogen 421 Wavefunction at Density Isosurface. Really hard to find Easy to do this Why? Because of Hermitian Operators: Kinetic Energy Density: #12;Density Functional Approach 4 Hydrogen 421 Density (Why is it grayscale?) A bit less obvious Probably easier to find

  11. Uncertainty Quantification for Nuclear Density Functional Theory...

    Office of Scientific and Technical Information (OSTI)

    Uncertainty Quantification for Nuclear Density Functional Theory and Information Content of New Measurements Citation Details In-Document Search Title: Uncertainty Quantification...

  12. Uncertainty Quantification for Nuclear Density Functional Theory...

    Office of Scientific and Technical Information (OSTI)

    Uncertainty Quantification for Nuclear Density Functional Theory and Information Content of New Measurements Citation Details In-Document Search This content will become publicly...

  13. Building a Universal Nuclear Energy Density Functional

    SciTech Connect (OSTI)

    Bertulani, Carlos A.

    2014-09-10

    This grant had two components: Density functional theory and pairing and Nuclear reactions. This final report summarizes the activities for this SciDAC-2 project.

  14. Time Dependent Density Functional Theory An Introduction

    E-Print Network [OSTI]

    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

  15. Magnetic fields and density functional theory

    SciTech Connect (OSTI)

    Salsbury Jr., Freddie

    1999-02-01

    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.

  16. Density functional theory for carbon dioxide crystal

    SciTech Connect (OSTI)

    Chang, Yiwen; Mi, Jianguo Zhong, Chongli

    2014-05-28

    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.

  17. Scaling Dynamical Correlation Energy from Density Functional Theory Correlation Functionals

    E-Print Network [OSTI]

    Ramachandran, Bala (Ramu)

    Scaling Dynamical Correlation Energy from Density Functional Theory Correlation Functionals B for molecules by scaling the electron correlation energy calculated by density functional theory (DFT)1 ReceiVed: February 2, 2005; In Final Form: April 18, 2005 The scaling of dynamical correlation energy

  18. Instabilities in the Nuclear Energy Density Functional

    E-Print Network [OSTI]

    M. Kortelainen; T. Lesinski

    2010-02-05

    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.

  19. Periodic subsystem density-functional theory

    SciTech Connect (OSTI)

    Genova, Alessandro; Pavanello, Michele; Ceresoli, Davide

    2014-11-07

    By partitioning the electron density into subsystem contributions, the Frozen Density Embedding (FDE) formulation of subsystem Density Functional Theory (DFT) has recently emerged as a powerful tool for reducing the computational scaling of Kohn–Sham DFT. To date, however, FDE has been employed to molecular systems only. Periodic systems, such as metals, semiconductors, and other crystalline solids have been outside the applicability of FDE, mostly because of the lack of a periodic FDE implementation. To fill this gap, in this work we aim at extending FDE to treat subsystems of molecular and periodic character. This goal is achieved by a dual approach. On one side, the development of a theoretical framework for periodic subsystem DFT. On the other, the realization of the method into a parallel computer code. We find that periodic FDE is capable of reproducing total electron densities and (to a lesser extent) also interaction energies of molecular systems weakly interacting with metallic surfaces. In the pilot calculations considered, we find that FDE fails in those cases where there is appreciable density overlap between the subsystems. Conversely, we find FDE to be in semiquantitative agreement with Kohn–Sham DFT when the inter-subsystem density overlap is low. We also conclude that to make FDE a suitable method for describing molecular adsorption at surfaces, kinetic energy density functionals that go beyond the GGA level must be employed.

  20. Density functional theory study of (OCS)2^-

    E-Print Network [OSTI]

    Bilalbegovic, G

    2007-01-01

    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.

  1. Density Functional Theory Models for Radiation Damage

    E-Print Network [OSTI]

    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

  2. Error Analysis in Nuclear Density Functional Theory (Journal...

    Office of Scientific and Technical Information (OSTI)

    Error Analysis in Nuclear Density Functional Theory Citation Details In-Document Search Title: Error Analysis in Nuclear Density Functional Theory Authors: Schunck, N ; McDonnell,...

  3. Error Analysis in Nuclear Density Functional Theory (Journal...

    Office of Scientific and Technical Information (OSTI)

    Error Analysis in Nuclear Density Functional Theory Citation Details In-Document Search Title: Error Analysis in Nuclear Density Functional Theory You are accessing a document...

  4. Configuration Interactions Constrained by Energy Density Functionals

    E-Print Network [OSTI]

    B. Alex Brown; Angelo Signoracci; Morten Hjorth-Jensen

    2010-09-24

    A new method for constructing a Hamiltonian for configuration interaction calculations with constraints to energies of spherical configurations obtained with energy-density-functional (EDF) methods is presented. This results in a unified model that reproduced the EDF binding-energy in the limit of single-Slater determinants, but can also be used for obtaining energy spectra and correlation energies with renormalized nucleon-nucleon interactions. The three-body and/or density-dependent terms that are necessary for good nuclear saturation properties are contained in the EDF. Applications to binding energies and spectra of nuclei in the region above 208Pb are given.

  5. The problem of the universal density functional and the density matrix functional theory

    SciTech Connect (OSTI)

    Bobrov, V. B. Trigger, S. A.

    2013-04-15

    The analysis in this paper shows that the Hohenberg-Kohn theorem is the constellation of two statements: (i) the mathematically rigorous Hohenberg-Kohn lemma, which demonstrates that the same ground-state density cannot correspond to two different potentials of an external field, and (ii) the hypothesis of the existence of the universal density functional. Based on the obtained explicit expression for the nonrel-ativistic particle energy in a local external field, we prove that the energy of the system of more than two non-interacting electrons cannot be a functional of the inhomogeneous density. This result is generalized to the system of interacting electrons. It means that the Hohenberg-Kohn lemma cannot provide justification of the universal density functional for fermions. At the same time, statements of the density functional theory remain valid when considering any number of noninteracting ground-state bosons due to the Bose condensation effect. In the framework of the density matrix functional theory, the hypothesis of the existence of the universal density matrix functional corresponds to the cases of noninteracting particles and to interaction in the Hartree-Fock approximation.

  6. Nuclear fission in covariant density functional theory

    E-Print Network [OSTI]

    A. V. Afanasjev; H. Abusara; P. Ring

    2013-09-12

    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.

  7. Orbital-optimized density cumulant functional theory

    SciTech Connect (OSTI)

    Sokolov, Alexander Yu. Schaefer, Henry F.

    2013-11-28

    In density cumulant functional theory (DCFT) the electronic energy is evaluated from the one-particle density matrix and two-particle density cumulant, circumventing the computation of the wavefunction. To achieve this, the one-particle density matrix is decomposed exactly into the mean-field (idempotent) and correlation components. While the latter can be entirely derived from the density cumulant, the former must be obtained by choosing a specific set of orbitals. In the original DCFT formulation [W. Kutzelnigg, J. Chem. Phys. 125, 171101 (2006)] the orbitals were determined by diagonalizing the effective Fock operator, which introduces partial orbital relaxation. Here we present a new orbital-optimized formulation of DCFT where the energy is variationally minimized with respect to orbital rotations. This introduces important energy contributions and significantly improves the description of the dynamic correlation. In addition, it greatly simplifies the computation of analytic gradients, for which expressions are also presented. We offer a perturbative analysis of the new orbital stationarity conditions and benchmark their performance for a variety of chemical systems.

  8. Symmetry energy in nuclear density functional theory

    E-Print Network [OSTI]

    W. Nazarewicz; P. -G. Reinhard; W. Satula; D. Vretenar

    2013-07-22

    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.

  9. Building a Universal Nuclear Energy Density Functional

    SciTech Connect (OSTI)

    Carlson, Joe A.; Furnstahl, Dick; Horoi, Mihai; Lust, Rusty; Nazaewicc, Witek; Ng, Esmond; Thompson, Ian; Vary, James

    2012-12-30

    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.

  10. Density functional theory of freezing: Analysis of crystal density

    E-Print Network [OSTI]

    Laird, Brian Bostian; McCoy, John D.; Haymet, A. D. J.

    1987-09-01

    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...

  11. Ions in solution: Density corrected density functional theory (DC-DFT)

    SciTech Connect (OSTI)

    Kim, Min-Cheol; Sim, Eunji; Burke, Kieron

    2014-05-14

    Standard density functional approximations often give questionable results for odd-electron radical complexes, with the error typically attributed to self-interaction. In density corrected density functional theory (DC-DFT), certain classes of density functional theory calculations are significantly improved by using densities more accurate than the self-consistent densities. We discuss how to identify such cases, and how DC-DFT applies more generally. To illustrate, we calculate potential energy surfaces of HO·Cl{sup ?} and HO·H{sub 2}O complexes using various common approximate functionals, with and without this density correction. Commonly used approximations yield wrongly shaped surfaces and/or incorrect minima when calculated self consistently, while yielding almost identical shapes and minima when density corrected. This improvement is retained even in the presence of implicit solvent.

  12. Density functional theory and optimal transportation with Coulomb cost

    E-Print Network [OSTI]

    Codina Cotar; Gero Friesecke; Claudia Klüppelberg

    2011-04-04

    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.

  13. Nuclear Energy Density Functionals Constrained by Low-Energy QCD

    E-Print Network [OSTI]

    Dario Vretenar

    2008-02-06

    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.

  14. Improved association in a classical density functional theory for water

    E-Print Network [OSTI]

    Eric J. Krebs; Jeff B. Schulte; David Roundy

    2013-09-07

    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.

  15. Density functional theory for self-bound systems

    E-Print Network [OSTI]

    Nir Barnea

    2007-11-06

    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.

  16. Density and spin response functions in ultracold fermionic atom gases

    E-Print Network [OSTI]

    Bogdan Mihaila; Sergio Gaudio; Krastan B. Blagoev; Alexander V. Balatsky; Peter B. Littlewood; Darryl L. Smith

    2005-02-03

    We propose a new method of detecting the onset of superfluidity in a two-component ultracold fermionic gas of atoms governed by an attractive short-range interaction. By studying the two-body correlation functions we find that a measurement of the momentum distribution of the density and spin response functions allows one to access separately the normal and anomalous densities. The change in sign at low momentum transfer of the density response function signals the transition between a BEC and a BCS regimes, characterized by small and large pairs, respectively. This change in sign of the density response function represents an unambiguous signature of the BEC to BCS crossover. Also, we predict spin rotational symmetry-breaking in this system.

  17. Preface: Special Topic on Advances in Density Functional Theory

    SciTech Connect (OSTI)

    Yang, Weitao

    2014-05-14

    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.

  18. Density Functional Theory with Dissipation: Transport through Single Molecules

    SciTech Connect (OSTI)

    Kieron Burke

    2012-04-30

    A huge amount of fundamental research was performed on this grant. Most of it focussed on fundamental issues of electronic structure calculations of transport through single molecules, using density functional theory. Achievements were: (1) First density functional theory with dissipation; (2) Pseudopotential plane wave calculations with master equation; (3) Weak bias limit; (4) Long-chain conductance; and (5) Self-interaction effects in tunneling.

  19. Neutron Drops and Skyrme Energy-Density Functionals

    E-Print Network [OSTI]

    B. S. Pudliner; A. Smerzi; J. Carlson; V. R. Pandharipande; Steven C. Pieper; D. G. Ravenhall

    1995-10-12

    The J$^{\\pi}$=0$^+$ ground state of a drop of 8 neutrons and the lowest 1/2$^-$ and 3/2$^-$ states of 7-neutron drops, all in an external well, are computed accurately with variational and Green's function Monte Carlo methods for a Hamiltonian containing the Argonne $v_{18}$ two-nucleon and Urbana IX three-nucleon potentials. These states are also calculated using Skyrme-type energy-density functionals. Commonly used functionals overestimate the central density of these drops and the spin-orbit splitting of 7-neutron drops. Improvements in the functionals are suggested.

  20. Self-interaction errors in nuclear energy density functionals

    E-Print Network [OSTI]

    N. Chamel

    2010-12-21

    When applied to a single nucleon, nuclear energy density functionals may yield a non-vanishing internal energy thus implying that the nucleon is interacting with itself. It is shown how to avoid this unphysical feature for semi-local phenomenological functionals containing all possible bilinear combinations of local densities and currents up to second order in the derivatives. The method outlined in this Rapid Communication could be easily extended to functionals containing higher order terms, and could serve as a guide for constraining the time-odd part of the functional.

  1. Linear response of homogeneous nuclear matter with energy density functionals

    E-Print Network [OSTI]

    A. Pastore; D. Davesne; J. Navarro

    2014-12-07

    Response functions of infinite nuclear matter with arbitrary isospin asymmetry are studied in the framework of the random phase approximation. The residual interaction is derived from a general nuclear Skyrme energy density functional. Besides the usual central, spin-orbit and tensor terms it could also include other components as new density-dependent terms or three-body terms. Algebraic expressions for the response functions are obtained from the Bethe-Salpeter equation for the particle-hole propagator. Applications to symmetric nuclear matter, pure neutron matter and asymmetric nuclear matter are presented and discussed. Spin-isospin strength functions are analyzed for varying conditions of density, momentum transfer, isospin asymmetry, and temperature for some representative Skyrme functionals. Particular attention is paid to the discussion of instabilities, either real or unphysical, which could manifest in finite nuclei.

  2. Monte Carlo tests of Orbital-Free Density Functional Theory

    E-Print Network [OSTI]

    D. I. Palade

    2014-12-12

    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.

  3. Neutron skin uncertainties of Skyrme energy density functionals

    E-Print Network [OSTI]

    M. Kortelainen; J. Erler; W. Nazarewicz; N. Birge; Y. Gao; E. Olsen

    2013-07-16

    Background: Neutron-skin thickness is an excellent indicator of isovector properties of atomic nuclei. As such, it correlates strongly with observables in finite nuclei that depend on neutron-to-proton imbalance and the nuclear symmetry energy that characterizes the equation of state of neutron-rich matter. A rich worldwide experimental program involving studies with rare isotopes, parity violating electron scattering, and astronomical observations is devoted to pinning down the isovector sector of nuclear models. Purpose: We assess the theoretical systematic and statistical uncertainties of neutron-skin thickness and relate them to the equation of state of nuclear matter, and in particular to nuclear symmetry energy parameters. Methods: We use the nuclear superfluid Density Functional Theory with several Skyrme energy density functionals and density dependent pairing. To evaluate statistical errors and their budget, we employ the statistical covariance technique. Results: We find that the errors on neutron skin increase with neutron excess. Statistical errors due to uncertain coupling constants of the density functional are found to be larger than systematic errors, the latter not exceeding 0.06 fm in most neutron-rich nuclei across the nuclear landscape. The single major source of uncertainty is the poorly determined slope L of the symmetry energy that parametrizes its density dependence. Conclusions: To provide essential constraints on the symmetry energy of the nuclear energy density functional, next-generation measurements of neutron skins are required to deliver precision better than 0.06 fm.

  4. Nuclear Energy Density Functionals: What do we really know?

    E-Print Network [OSTI]

    Bulgac, Aurel; Jin, Shi

    2015-01-01

    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...

  5. Probability distribution functions in the finite density lattice QCD

    E-Print Network [OSTI]

    S. Ejiri; Y. Nakagawa; S. Aoki; K. Kanaya; H. Saito; T. Hatsuda; H. Ohno; T. Umeda

    2012-12-04

    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.

  6. Addressing spectroscopic quality of covariant density functional theory

    E-Print Network [OSTI]

    A. V. Afanasjev

    2014-09-17

    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.

  7. Relativistic Nuclear Energy Density Functionals: adjusting parameters to binding energies

    E-Print Network [OSTI]

    T. Niksic; D. Vretenar; P. Ring

    2008-09-08

    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.

  8. A Classical Density-Functional Theory for Describing Water Interfaces

    E-Print Network [OSTI]

    Jessica Hughes; Eric Krebs; David Roundy

    2012-08-31

    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.

  9. Binding Energies in Benzene Dimers: Nonlocal Density Functional Calculations

    E-Print Network [OSTI]

    Aaron Puzder; Maxime Dion; David C. Langreth

    2005-09-15

    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.

  10. Relativistic density functional theory for finite nuclei and neutron stars

    E-Print Network [OSTI]

    J. Piekarewicz

    2015-02-05

    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.

  11. Probability Density Function Estimation Using Orthogonal Forward Regression

    E-Print Network [OSTI]

    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

  12. Finding Density Functionals with Machine Learning John C. Snyder,1

    E-Print Network [OSTI]

    Burke, Kieron

    ) energy as a functional of the electronic spin densities. The quality of the results cru- cially depends) of Kohn and Sham [2] is uniquely defined by the properties of the uniform gas and has been argued attraction to the nuclei. ML is a natural tool

  13. Understanding Kernel Ridge Regression: Common behaviors from simple functions to density functionals

    E-Print Network [OSTI]

    Vu, Kevin; Li, Li; Rupp, Matthias; Chen, Brandon F; Khelif, Tarek; Müller, Klaus-Robert; Burke, Kieron

    2015-01-01

    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.

  14. Ab Initio Derivation of Model Energy Density Functionals

    E-Print Network [OSTI]

    Dobaczewski, J

    2015-01-01

    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.

  15. Ab Initio Derivation of Model Energy Density Functionals

    E-Print Network [OSTI]

    J. Dobaczewski

    2015-07-07

    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.

  16. Spin projection with double hybrid density functional theory

    SciTech Connect (OSTI)

    Thompson, Lee M.; Hratchian, Hrant P.

    2014-07-21

    A spin projected double-hybrid density functional theory is presented that accounts for different scaling of opposite and same spin terms in the second order correction. This method is applied to three dissociation reactions which in the unprojected formalism exhibit significant spin contamination with higher spin states. This gives rise to a distorted potential surface and can lead to poor geometries and energies. The projected method presented is shown to improve the description of the potential over unprojected double hybrid density functional theory. Comparison is made with the reference states of the two double hybrid functionals considered here (B2PLYP and mPW2PLYP) in which the projected potential surface is degraded by an imbalance in the description of dynamic and static correlation.

  17. Surface Symmetry Energy of Nuclear Energy Density Functionals

    E-Print Network [OSTI]

    N. Nikolov; N. Schunck; W. Nazarewicz; M. Bender; J. Pei

    2010-12-28

    We study the bulk deformation properties of the Skyrme nuclear energy density functionals. Following simple arguments based on the leptodermous expansion and liquid drop model, we apply the nuclear density functional theory to assess the role of the surface symmetry energy in nuclei. To this end, we validate the commonly used functional parametrizations against the data on excitation energies of superdeformed band-heads in Hg and Pb isotopes, and fission isomers in actinide nuclei. After subtracting shell effects, the results of our self-consistent calculations are consistent with macroscopic arguments and indicate that experimental data on strongly deformed configurations in neutron-rich nuclei are essential for optimizing future nuclear energy density functionals. The resulting survey provides a useful benchmark for further theoretical improvements. Unlike in nuclei close to the stability valley, whose macroscopic deformability hangs on the balance of surface and Coulomb terms, the deformability of neutron-rich nuclei strongly depends on the surface-symmetry energy; hence, its proper determination is crucial for the stability of deformed phases of the neutron- rich matter and description of fission rates for r-process nucleosynthesis.

  18. Differentiable but exact formulation of density-functional theory

    SciTech Connect (OSTI)

    Kvaal, Simen Ekström, Ulf; Helgaker, Trygve; Teale, Andrew M.; School of Chemistry, University of Nottingham, University Park, Nottingham NG7 2RD

    2014-05-14

    The universal density functional F of density-functional theory is a complicated and ill-behaved function of the density—in particular, F is not differentiable, making many formal manipulations more complicated. While F has been well characterized in terms of convex analysis as forming a conjugate pair (E, F) with the ground-state energy E via the Hohenberg–Kohn and Lieb variation principles, F is nondifferentiable and subdifferentiable only on a small (but dense) subset of its domain. In this article, we apply a tool from convex analysis, Moreau–Yosida regularization, to construct, for any ? > 0, pairs of conjugate functionals ({sup ?}E, {sup ?}F) that converge to (E, F) pointwise everywhere as ? ? 0{sup +}, and such that {sup ?}F is (Fréchet) differentiable. For technical reasons, we limit our attention to molecular electronic systems in a finite but large box. It is noteworthy that no information is lost in the Moreau–Yosida regularization: the physical ground-state energy E(v) is exactly recoverable from the regularized ground-state energy {sup ?}E(v) in a simple way. All concepts and results pertaining to the original (E, F) pair have direct counterparts in results for ({sup ?}E, {sup ?}F). The Moreau–Yosida regularization therefore allows for an exact, differentiable formulation of density-functional theory. In particular, taking advantage of the differentiability of {sup ?}F, a rigorous formulation of Kohn–Sham theory is presented that does not suffer from the noninteracting representability problem in standard Kohn–Sham theory.

  19. Measuring the Density Fluctuation From the Cluster Gas Mass Function

    E-Print Network [OSTI]

    Kazuhiro Shimasaku

    1997-01-27

    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.

  20. Finite-size instabilities in nuclear energy density functionals

    SciTech Connect (OSTI)

    Hellemans, V.; Heenen, P.-H.; Bender, M.

    2012-10-20

    The systematic lack of convergence of self-consistent mean-field calculations with certain parameterizations of the Skyrme energy density functional has been attributed to the appearance of finite-size instabilities. In this contribution, we investigate what happens at the instability associated with the C{sub 0}{sup {Delta}s}s{sub 0} Dot-Operator {Delta}s{sub 0} term in a high-spin state of the superdeformed band in {sup 194}Hg.

  1. Progress at the interface of wave-function and density-functional theories

    SciTech Connect (OSTI)

    Gidopoulos, Nikitas I.

    2011-04-15

    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.

  2. [1] Digital library of mathematical functions. DLMF; electronic version, NIST, Gaithersburg, MD, 2001, http://dlmf.nist.gov/.

    E-Print Network [OSTI]

    Stein, William

    References [1] Digital library of mathematical functions. DLMF; electronic version, NIST] , Sage Publication List, 2009, http://sagemath.org/library-publications.html. 1 #12; of mathematical functions with formulas, graphs, and mathematical tables, National Bureau of Standards Applied

  3. Vibrational Lifetimes and Spectral Shifts in Supercritical Fluids as a Function of Density: Experiments and Theory

    E-Print Network [OSTI]

    Fayer, Michael D.

    (CO2) as a function of density from low density (well below the critical density) to high densityVibrational Lifetimes and Spectral Shifts in Supercritical Fluids as a Function of Density Vibrational lifetime and spectral shift data for the asymmetric CO stretching mode of W(CO)6 in supercritical

  4. Time-dependent density-functional studies on strength functions in neutron-rich nuclei

    E-Print Network [OSTI]

    Shuichiro Ebata; Tsunenori Inakura; Takashi Nakatsukasa

    2013-02-08

    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.

  5. Quantification of Uncertainties in Nuclear Density Functional theory

    E-Print Network [OSTI]

    N. Schunck; J. D. McDonnell; D. Higdon; J. Sarich; S. Wild

    2014-09-17

    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.

  6. Hole Localization in Molecular Crystals from Hybrid Density Functional Theory

    SciTech Connect (OSTI)

    Sai, Na; Barbara, Paul F.; Leung, Kevin

    2011-06-02

    We use first-principles computational methods to examine hole trapping in organic molecular crystals. We present a computational scheme based on the tuning of the fraction of exact exchange in hybrid density functional theory to eliminate the many-electron self-interaction error. With small organic molecules, we show that this scheme gives accurate descriptions of ionization and dimer dissociation. We demonstrate that the excess hole in perfect molecular crystals forms self-trapped molecular polarons. The predicted absolute ionization potentials of both localized and delocalized holes are consistent with experimental values.

  7. Towards the island of stability with relativistic energy density functionals

    SciTech Connect (OSTI)

    Prassa, V.; Niksic, T.; Lalazissis, G. A.; Vretenar, D.

    2012-10-20

    Relativistic energy density functionals (REDF) provide a complete and accurate, global description of nuclear structure phenomena. Modern semi-empirical functionals, adjusted to the nuclear matter equation of state and to empirical masses of deformed nuclei, are applied to studies of shapes of superheavy nuclei. The theoretical framework is tested in a comparison to empirical masses, quadrupole deformations, and energy barriers of actinide nuclei. The model is used in a self-consistent mean-field calculation of spherical, axial and triaxial shapes of superheavy nuclei, alpha-decay energies and lifetimes. The effect of explicit treatment of collective correlations is analyzed in calculations that consistently use a collective Hamiltonian model based on REDFs.

  8. Practical Attacks on Digital Signatures Using MD5 Message Digest

    E-Print Network [OSTI]

    Practical Attacks on Digital Signatures Using MD5 Message Digest Ondrej Mikle Department schemes based on MD5 message digest on an example using GPG. Keywords: collision, hash function, MD5 1 used for file integrity checking and as a message digest in digital signature schemes. During CRYPTO

  9. Daubechies wavelets for linear scaling density functional theory

    SciTech Connect (OSTI)

    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)

    2014-05-28

    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.

  10. Density functional theory based generalized effective fragment potential method

    SciTech Connect (OSTI)

    Nguyen, Kiet A. E-mail: ruth.pachter@wpafb.af.mil; Pachter, Ruth E-mail: ruth.pachter@wpafb.af.mil; Day, Paul N.

    2014-06-28

    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.

  11. Particle-vibration coupling within covariant density functional theory

    E-Print Network [OSTI]

    E. Litvinova; P. Ring; V. Tselyaev

    2007-05-08

    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.

  12. Building A Universal Nuclear Energy Density Functional (UNEDF)

    SciTech Connect (OSTI)

    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

    2012-09-30

    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.

  13. Semiclassical Origins of Density Functionals Peter Elliott, Donghyung Lee, Attila Cangi, and Kieron Burke

    E-Print Network [OSTI]

    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

  14. Predicting Stability Constants for Uranyl Complexes Using Density Functional Theory

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

    Vukovic, Sinisa; Hay, Benjamin P.; Bryantsev, Vyacheslav S.

    2015-04-02

    The ability to predict the equilibrium constants for the formation of 1:1 uranyl:ligand complexes (log K1 values) provides the essential foundation for the rational design of ligands with enhanced uranyl affinity and selectivity. We also use density functional theory (B3LYP) and the IEFPCM continuum solvation model to compute aqueous stability constants for UO22+ complexes with 18 donor ligands. Theoretical calculations permit reasonably good estimates of relative binding strengths, while the absolute log K1 values are significantly overestimated. Accurate predictions of the absolute log K1 values (root mean square deviation from experiment 1 values ranging from 0more »to 16.8) can be obtained by fitting the experimental data for two groups of mono and divalent negative oxygen donor ligands. The utility of correlations is demonstrated for amidoxime and imide dioxime ligands, providing a useful means of screening for new ligands with strong chelate capability to uranyl.« less

  15. Dipole polarizability of 120Sn and nuclear energy density functionals

    E-Print Network [OSTI]

    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

    2015-03-28

    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.

  16. Deviations from piecewise linearity in the solid-state limit with approximate density functionals

    E-Print Network [OSTI]

    Baer, Roi

    Deviations from piecewise linearity in the solid-state limit with approximate density functionals (2015) Deviations from piecewise linearity in the solid-state limit with approximate density functionals functional methods J. Chem. Phys. 141, 124123 (2014); 10.1063/1.4896455 Thermally-assisted-occupation density

  17. Spin-Multiplet Energies from Time-Dependent Density-Functional Theory

    E-Print Network [OSTI]

    Gross, E.K.U.

    Spin-Multiplet Energies from Time-Dependent Density-Functional Theory M. Petersilka and E excitation energies, we develop a density-functional method for the calculation of excitation energies energies which is based on time-dependent density- functional theory (TDDFT) [26]. In the linear response

  18. Self-interaction corrections in density functional theory

    SciTech Connect (OSTI)

    Tsuneda, Takao; Hirao, Kimihiko

    2014-05-14

    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.

  19. 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.

    2015-01-06

    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 forcingmore »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.« less

  20. 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.

    2015-01-06

    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

  1. Hybrid Dynamic Density Functional Theory for Polymer Melts and Blends

    E-Print Network [OSTI]

    Takashi Honda; Toshihiro Kawakatsu

    2006-09-05

    We propose a high-speed and accurate hybrid dynamic density functional theory for the computer simulations of the phase separation processes of polymer melts and blends. The proposed theory is a combination of the dynamic self-consistent field (SCF) theory and a time-dependent Ginzburg-Landau type theory with the random phase approximation (GRPA). The SCF theory is known to be accurate in evaluating the free energy of the polymer systems in both weak and strong segregation regions although it has a disadvantage of the requirement of a considerable amount of computational cost. On the other hand, the GRPA theory has an advantage of much smaller amount of required computational cost than the SCF theory while its applicability is limited to the weak segregation region. To make the accuracy of the SCF theory and the high-performance of the GRPA theory compatible, we adjust the chemical potential of the GRPA theory by using the SCF theory every constant time steps in the dynamic simulations. The performance of the GRPA and the hybrid theories is tested by using several systems composed of an A/B homopolymer, an AB diblock copolymer, or an ABC triblock copolymer. Using the hybrid theory, we succeeded in reproducing the metastable complex phase-separated domain structures of an ABC triblock copolymer observed by experiments.

  2. Parameterizing deep convection using the assumed probability density function method

    SciTech Connect (OSTI)

    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)

    2015-01-01

    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.

  3. Tests of second-generation and third-generation density functionals for thermochemical kineticsy

    E-Print Network [OSTI]

    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

  4. Communication: Embedded fragment stochastic density functional theory Daniel Neuhauser, Roi Baer, and Eran Rabani

    E-Print Network [OSTI]

    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) Roi­18 Recently, we formulated KS-DFT as a statistical theory in which the electron density is determined from

  5. Nuclear Physics A 770 (2006) 131 Relativistic nuclear energy density functional

    E-Print Network [OSTI]

    Weise, Wolfram

    2006-01-01

    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

  6. NT@UW-15-05 Nuclear Energy Density Functionals: What do we really know?

    E-Print Network [OSTI]

    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

  7. Microscopically-based energy density functionals for nuclei using the density matrix expansion: Implementation and pre-optimization

    E-Print Network [OSTI]

    M. Stoitsov; M. Kortelainen; S. K. Bogner; T. Duguet; R. J. Furnstahl; B. Gebremariam; N. Schunck

    2010-09-17

    In a recent series of papers, Gebremariam, Bogner, and Duguet derived a microscopically based nuclear energy density functional by applying the Density Matrix Expansion (DME) to the Hartree-Fock energy obtained from chiral effective field theory (EFT) two- and three-nucleon interactions. Due to the structure of the chiral interactions, each coupling in the DME functional is given as the sum of a coupling constant arising from zero-range contact interactions and a coupling function of the density arising from the finite-range pion exchanges. Since the contact contributions have essentially the same structure as those entering empirical Skyrme functionals, a microscopically guided Skyrme phenomenology has been suggested in which the contact terms in the DME functional are released for optimization to finite-density observables to capture short-range correlation energy contributions from beyond Hartree-Fock. The present paper is the first attempt to assess the ability of the newly suggested DME functional, which has a much richer set of density dependencies than traditional Skyrme functionals, to generate sensible and stable results for nuclear applications. The results of the first proof-of-principle calculations are given, and numerous practical issues related to the implementation of the new functional in existing Skyrme codes are discussed. Using a restricted singular value decomposition (SVD) optimization procedure, it is found that the new DME functional gives numerically stable results and exhibits a small but systematic reduction of our test $\\chi^2$ function compared to standard Skyrme functionals, thus justifying its suitability for future global optimizations and large-scale calculations.

  8. Simple Methods To Reduce Charge-Transfer Contamination in Time-Dependent Density-Functional

    E-Print Network [OSTI]

    Herbert, John

    Simple Methods To Reduce Charge-Transfer Contamination in Time-Dependent Density) contamination in condensed-phase, time- dependent density-functional theory. These calculations are plagued spectra can still be obtained, upon configurational averaging, despite pervasive CT contamination

  9. Symmetry Energy as a Function of Density and Mass

    E-Print Network [OSTI]

    Pawel Danielewicz; Jenny Lee

    2007-08-21

    Energy in nuclear matter is, in practice, completely characterized at different densities and asymmetries, when the density dependencies of symmetry energy and of energy of symmetric matter are specified. The density dependence of the symmetry energy at subnormal densities produces mass dependence of nuclear symmetry coefficient and, thus, can be constrained by that latter dependence. We deduce values of the mass dependent symmetry coefficients, by using excitation energies to isobaric analog states. The coefficient systematic, for intermediate and high masses, is well described in terms of the symmetry coefficient values of a_a^V=(31.5-33.5) MeV for the volume coefficient and a_a^S=(9-12) MeV for the surface coefficient. These two further correspond to the parameter values describing density dependence of symmetry energy, of L~95 MeV and K_{sym}~25 MeV.

  10. Linear response time-dependent density functional theory for van der Waals coefficients

    E-Print Network [OSTI]

    Chu, Xi

    Linear response time-dependent density functional theory for van der Waals coefficients X. Chu Received 9 January 2004; accepted 15 June 2004 A linear response time-dependent density functional theory description of the linear response function and of the induced self- consistent field, which adequately

  11. Stretched hydrogen molecule from a constrained-search density-functional perspective

    SciTech Connect (OSTI)

    Valone, Steven M [Los Alamos National Laboratory; Levy, Mel [DIKE UNIV.

    2009-01-01

    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.

  12. On the breaking and restoration of symmetries within the nuclear energy density functional formalism

    E-Print Network [OSTI]

    T. Duguet; J. Sadoudi

    2010-10-19

    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.

  13. Zinc surface complexes on birnessite: A density functional theory study

    SciTech Connect (OSTI)

    Kwon, Kideok D.; Refson, Keith; Sposito, Garrison

    2009-01-05

    Biogeochemical cycling of zinc is strongly influenced by sorption on birnessite minerals (layer-type MnO2), which are found in diverse terrestrial and aquatic environments. Zinc has been observed to form both tetrahedral (Zn{sup IV}) and octahedral (Zn{sup VI}) triple-corner-sharing surface complexes (TCS) at Mn(IV) vacancy sites in hexagonal birnessite. The octahedral complex is expected to be similar to that of Zn in the Mn oxide mineral, chalcophanite (ZnMn{sub 3}O{sub 7} {center_dot} 3H{sub 2}O), but the reason for the occurrence of the four-coordinate Zn surface species remains unclear. We address this issue computationally using spin-polarized Density Functional Theory (DFT) to examine the Zn{sub IV}-TCS and Zn{sup VI}-TCS species. Structural parameters obtained by DFT geometry optimization were in excellent agreement with available experimental data on Zn-birnessites. Total energy, magnetic moments, and electron-overlap populations obtained by DFT for isolated Zn{sup IV}-TCS revealed that this species is stable in birnessite without a need for Mn(III) substitution in the octahedral sheet and that it is more effective in reducing undersaturation of surface O at a Mn vacancy than is Zn{sub VI}-TCS. Comparison between geometry-optimized ZnMn{sub 3}O{sub 7} {center_dot} 3H{sub 2}O (chalcophanite) and the hypothetical monohydrate mineral, ZnMn{sub 3}O{sub 7} {center_dot} H{sub 2}O, which contains only tetrahedral Zn, showed that the hydration state of Zn significantly affects birnessite structural stability. Finally, our study also revealed that, relative to their positions in an ideal vacancy-free MnO{sub 2}, Mn nearest to Zn in a TCS surface complex move toward the vacancy by 0.08-0.11 {angstrom}, while surface O bordering the vacancy move away from it by 0.16-0.21 {angstrom}, in agreement with recent X-ray absorption spectroscopic analyses.

  14. Density Functional Theory Calculations of Mass Transport in UO2

    SciTech Connect (OSTI)

    Andersson, Anders D.; Dorado, Boris; Uberuaga, Blas P.; Stanek, Christopher R.

    2012-06-26

    In this talk we present results of density functional theory (DFT) calculations of U, O and fission gas diffusion in UO{sub 2}. These processes all impact nuclear fuel performance. For example, the formation and retention of fission gas bubbles induce fuel swelling, which leads to mechanical interaction with the clad thereby increasing the probability for clad breach. Alternatively, fission gas can be released from the fuel to the plenum, which increases the pressure on the clad walls and decreases the gap thermal conductivity. The evolution of fuel microstructure features is strongly coupled to diffusion of U vacancies. Since both U and fission gas transport rates vary strongly with the O stoichiometry, it is also important to understand O diffusion. In order to better understand bulk Xe behavior in UO{sub 2{+-}x} we first calculate the relevant activation energies using DFT techniques. By analyzing a combination of Xe solution thermodynamics, migration barriers and the interaction of dissolved Xe atoms with U, we demonstrate that Xe diffusion predominantly occurs via a vacancy-mediated mechanism. Since Xe transport is closely related to diffusion of U vacancies, we have also studied the activation energy for this process. In order to explain the low value of 2.4 eV found for U migration from independent damage experiments (not thermal equilibrium) the presence of vacancy clusters must be included in the analysis. Next we investigate species transport on the (111) UO{sub 2} surface, which is motivated by the formation of small voids partially filled with fission gas atoms (bubbles) in UO{sub 2} under irradiation. Surface diffusion could be the rate-limiting step for diffusion of such bubbles, which is an alternative mechanism for mass transport in these materials. As expected, the activation energy for surface diffusion is significantly lower than for bulk transport. These results are further discussed in terms of engineering-scale fission gas release models. Finally, oxidation of UO{sub 2} and the importance of cluster formation for understanding thermodynamic and kinetic properties of UO{sub 2+x} are investigated.

  15. Complex-energy approach to sum rules within nuclear density functional...

    Office of Scientific and Technical Information (OSTI)

    Complex-energy approach to sum rules within nuclear density functional theory Citation Details In-Document Search This content will become publicly available on April 27, 2016...

  16. Supplementary data for "Relativistic density functional theory modeling of plutonium and

    E-Print Network [OSTI]

    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

  17. Complex-energy approach to sum rules within nuclear density functional...

    Office of Scientific and Technical Information (OSTI)

    Journal Article: Complex-energy approach to sum rules within nuclear density functional theory Citation Details In-Document Search This content will become publicly available on...

  18. DENSITY FUNCTIONAL THEORY OF NORMAL AND SUPERCONDUCTING ELECTRON LIQUIDS: EXPLICIT

    E-Print Network [OSTI]

    Gross, E.K.U.

    22 5.1 Green's functions for the non-interacting system . . . . . . . . . . . . . . . 22 5 the Green's functions . . . . . . . . . . . . 28 5.5 Poles of the zero-order Green's functions theory is to describe a many-electron system exclusively and completely in terms of its ground

  19. Density-matrix functionals for pairing in mesoscopic superconductors

    E-Print Network [OSTI]

    Denis Lacroix; Guillaume Hupin

    2010-09-03

    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.

  20. Pressure Correction in Classical Density Functional Theory: Hyper Netted Chain and Hard Sphere Bridge Functionals

    E-Print Network [OSTI]

    Volodymyr Sergiievskyi; Guillaume Jeanmairet; Maximilien Levesque; Daniel Borgis

    2015-09-04

    Low accuracy of the Solvation Free Energy (SFE) calculation is a known problem of the numerical methods of the Integral Equation Theory of Liquids and the Classical Density Functional Theory (Classical DFT). Although functionals with empirical corrections can essentially improve the predictability of the methods, their universality is still a question. In our recent paper we connected the SFE calculation errors with the incorrect pressure in the Classical DFT and proposed the a posteriory correction to improve the results (J. Phys. Chem. Lett., 5, 1925-1942 ). This paper raised a discussion in the community. In particular, recently appeared a critical reply where pointed some thermodynamical inconsistencies of the derivations in our paper (J. Chem. Theory Comput., 11, 378-380). In the present work we re-derive the pressure correction in a more simple way and show that despite the inaccuracies during the derivation, the final form of the previously derived correction is correct. We also test the applicability of the proposed correction to the functionals which include a three- and many- body terms from the fundamental measure theory (FMT) for hard sphere fluid. We test all the functionals on a set of model systems and discuss the obtained results.

  1. PUBLISHED VERSION Constrained density functional for noncollinear magnetism

    E-Print Network [OSTI]

    © 2015 UNITED KINGDOM ATOMIC ENERGY AUTHORITY This article may be downloaded for personal use only. Any­19]. Although ab initio calculations often assume collinear mag- netic configurations, spin-polarized density] and are widely adopted in ab initio programs [29­31]. Magnetic DFT calculations are often performed in the atomic

  2. Density-Functional Theory and Quantum Chemistry Studies on "dry" and "wet"

    E-Print Network [OSTI]

    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

  3. Band structures Optical absorption Summary Key concepts in Density Functional Theory (II)

    E-Print Network [OSTI]

    Botti, Silvana

    Band structures Optical absorption Summary Key concepts in Density Functional Theory (II) Kohn-Sham scheme, band structure and optical spectra Silvana Botti European Theoretical Spectroscopy Facility (ETSF, Belfast Key concepts in Density Functional Theory (II) Silvana Botti #12;Band structures Optical

  4. Covariant energy density functionals: the assessment of global performance across the nuclear landscape

    E-Print Network [OSTI]

    Afanasjev, A V

    2015-01-01

    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.

  5. Electronvibration coupling in time-dependent density-functional theory: Application to benzene

    E-Print Network [OSTI]

    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

  6. Irradiation-Induced Magnetism in Graphite: A Density Functional Study P. O. Lehtinen,1

    E-Print Network [OSTI]

    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

  7. Probability-density function for energy perturbations of isolated optical pulses

    E-Print Network [OSTI]

    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

  8. Covariant energy density functionals: the assessment of global performance across the nuclear landscape

    E-Print Network [OSTI]

    A. V. Afanasjev

    2015-08-22

    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.

  9. Supplementary material to "Curvature and frontier orbital energies in density functional theory", by Stein et al.

    E-Print Network [OSTI]

    Baer, Roi

    Supplementary material to "Curvature and frontier orbital energies in density functional theory: [{ }] [{ }] #12;Supplementary material to "Curvature and frontier orbital energies in density functional theory the average curvature. This relation is Eq. (8) in the paper. #12;Supplementary material to "Curvature

  10. LES/probability density function approach for the simulation of an ethanol spray flame

    E-Print Network [OSTI]

    Raman, Venkat

    LES/probability density function approach for the simulation of an ethanol spray flame Colin Heye a an experimental pilot-stabilized ethanol spray flame. In this particular flame, droplet evaporation occurs away: Large-eddy simulation; Probability density function; Flamelet/progress variable approach; Ethanol

  11. Calculations of free energies in liquid and solid phases: Fundamental measure density-functional approach

    E-Print Network [OSTI]

    Song, Xueyu

    Calculations of free energies in liquid and solid phases: Fundamental measure density energies of liquid and solid phases using a fundamental measure density-functional theory. Namely, we can, a theoretical description of the free energies and correlation functions of hard-sphere (HS) liquid and solid

  12. Density Functional Theory for Protein Transfer Free Energy Eric A. Mills and Steven S. Plotkin*

    E-Print Network [OSTI]

    Plotkin, Steven S.

    Density Functional Theory for Protein Transfer Free Energy Eric A. Mills and Steven S. Plotkin ABSTRACT: We cast the problem of protein transfer free energy within the formalism of density functional excluded volume, solvent-accessible surface area, and temperature dependence of the transfer free energy

  13. Applications of Skyrme energy-density functional to fusion reactions spanning the fusion barriers

    E-Print Network [OSTI]

    Min Liu; Ning Wang; Zhuxia Li; Xizhen Wu; Enguang Zhao

    2006-01-25

    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.

  14. Element orbitals for Kohn-Sham density functional theory

    SciTech Connect (OSTI)

    Lin, Lin; Ying, Lexing

    2012-05-08

    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.

  15. The quest for a universal density functional: The accuracy of density functionals across a broad spectrum of databases in chemistry and physics

    E-Print Network [OSTI]

    Roberto Peverati; Donald G. Truhlar

    2013-09-06

    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.

  16. Free energies, vacancy concentrations and density distribution anisotropies in hard--sphere crystals: A combined density functional and simulation study

    E-Print Network [OSTI]

    M. Oettel; S. Goerig; A. Haertel; H. Loewen; M. Radu; T. Schilling

    2010-09-03

    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.

  17. TELEPSYCHIATRY Peter Yellowlees MBBS MD

    E-Print Network [OSTI]

    Leistikow, Bruce N.

    TELEPSYCHIATRY Peter Yellowlees MBBS MD Professor of Psychiatry UC Davis, California #12; Providing #12;UC Davis Prima Care Network Woodland Dignity Health Clinic CURRENT CLINICAL TRIAL OF ATP VS. STP-Maria Iosif PhD · Paul Leigh PhD · Bill Brady MD and Auburn Clinic staff ­ UCD PCN · Jeff Yee MD and Woodland

  18. Spin densities from subsystem density-functional theory: Assessment and application to a photosynthetic reaction center complex model

    SciTech Connect (OSTI)

    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)

    2012-05-21

    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.

  19. Nuclear energy density functional from chiral pion-nucleon dynamics revisited

    E-Print Network [OSTI]

    N. Kaiser; W. Weise

    2009-12-16

    We use a recently improved density-matrix expansion to calculate the nuclear energy density functional in the framework of in-medium chiral perturbation theory. Our calculation treats systematically the effects from $1\\pi$-exchange, iterated $1\\pi$-exchange, and irreducible $2\\pi$-exchange with intermediate $\\Delta$-isobar excitations, including Pauli-blocking corrections up to three-loop order. We find that the effective nucleon mass $M^*(\\rho)$ entering the energy density functional is identical to the one of Fermi-liquid theory when employing the improved density-matrix expansion. The strength $F_\

  20. Communication: Self-interaction correction with unitary invariance in density functional theory

    SciTech Connect (OSTI)

    Pederson, Mark R.; Ruzsinszky, Adrienn; Perdew, John P.; Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122

    2014-03-28

    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.

  1. arXiv:1107.5966v1[nucl-th]29Jul2011 Nuclear energy density functional from

    E-Print Network [OSTI]

    Weise, Wolfram

    arXiv:1107.5966v1[nucl-th]29Jul2011 Nuclear energy density functional from chiral two- and three. With this input the nuclear energy density functional is derived to first order in the two- and three.15.Ew Keywords: Nuclear energy density functional; Density-matrix expansion; Chiral two- and three

  2. Recent developments in classical density functional theory: Internal energy functional and diagrammatic structure of fundamental measure theory

    E-Print Network [OSTI]

    M. Schmidt; M. Burgis; W. S. B. Dwandaru; G. Leithall; P. Hopkins

    2012-12-27

    An overview of several recent developments in density functional theory for classical inhomogeneous liquids is given. We show how Levy's constrained search method can be used to derive the variational principle that underlies density functional theory. An advantage of the method is that the Helmholtz free energy as a functional of a trial one-body density is given as an explicit expression, without reference to an external potential as is the case in the standard Mermin-Evans proof by reductio ad absurdum. We show how to generalize the approach in order to express the internal energy as a functional of the one-body density distribution and of the local entropy distribution. Here the local chemical potential and the bulk temperature play the role of Lagrange multipliers in the Euler-Lagrange equations for minimiziation of the functional. As an explicit approximation for the free-energy functional for hard sphere mixtures, the diagrammatic structure of Rosenfeld's fundamental measure density unctional is laid out. Recent extensions, based on the Kierlik-Rosinberg scalar weight functions, to binary and ternary non-additive hard sphere mixtures are described.

  3. On the contact values of the density profiles in an electric double layer using density functional theory

    E-Print Network [OSTI]

    L. B. Bhuiyan; D. Henderson; S. Soko?owski

    2012-07-13

    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.

  4. Ensemble density variational methods with self- and ghost-interaction-corrected functionals

    SciTech Connect (OSTI)

    Pastorczak, Ewa; Pernal, Katarzyna

    2014-05-14

    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.

  5. Fluid - solid transition in simple systems using density functional theory

    E-Print Network [OSTI]

    Atul S. Bharadwaj; Yashwant Singh

    2014-11-24

    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.

  6. Bethe ansatz density-functional theory of ultracold repulsive fermions in one-dimensional optical lattices

    SciTech Connect (OSTI)

    Xianlong, Gao; Polini, Marco; Tosi, M. P.; Campo, Vivaldo L. Jr.; Capelle, Klaus; Rigol, Marcos

    2006-04-15

    We present an extensive numerical study of the ground-state properties of confined repulsively interacting fermions in one-dimensional optical lattices. Detailed predictions for the atom-density profiles are obtained from parallel Kohn-Sham density-functional calculations and quantum Monte Carlo simulations. The density-functional calculations employ a Bethe ansatz based local-density approximation for the correlation energy that accounts for Luttinger-liquid and Mott-insulator physics. Semianalytical and fully numerical formulations of this approximation are compared with each other and with a cruder Thomas-Fermi-type local-density approximation for the total energy. Precise quantum Monte Carlo simulations are used to assess the reliability of the various local-density approximations, and in conjunction with these provide a detailed microscopic picture of the consequences of the interplay between particle-particle interactions and confinement in one-dimensional systems of strongly correlated fermions.

  7. Double-Pole Approximation in Time-Dependent Density Functional Theory

    E-Print Network [OSTI]

    Gross, E.K.U.

    Double-Pole Approximation in Time-Dependent Density Functional Theory H. Appel and E.K.U. Gross-dependent density func- tional theory (TDDFT) is given. This extends the single-pole approximation (SPA) to two strongly- coupled poles. The analysis provides both an illustration of how TDDFT works when strong exchange

  8. The Materials genome : rapid materials screening for renewable energy using high-throughput density functional theory

    E-Print Network [OSTI]

    Jain, Anubhav, Ph.D. Massachusetts Institute of Technology

    2011-01-01

    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, ...

  9. Extra-galactic high-energy transients: event rate densities and luminosity functions

    E-Print Network [OSTI]

    Sun, Hui; Li, Zhuo

    2015-01-01

    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...

  10. Degenerate ground states and nonunique potentials: Breakdown and restoration of density functionals

    SciTech Connect (OSTI)

    Capelle, K.; Ullrich, C. A.; Vignale, G.

    2007-07-15

    The Hohenberg-Kohn (HK) theorem is one of the most fundamental theorems of quantum mechanics, and constitutes the basis for the very successful density-functional approach to inhomogeneous interacting many-particle systems. Here we show that in formulations of density-functional theory (DFT) that employ more than one density variable, applied to systems with a degenerate ground state, there is a subtle loophole in the HK theorem, as all mappings between densities, wave functions, and potentials can break down. Two weaker theorems which we prove here, the joint-degeneracy theorem and the internal-energy theorem, restore the internal, total, and exchange-correlation energy functionals to the extent needed in applications of DFT to atoms, molecules, and solids. The joint-degeneracy theorem constrains the nature of possible degeneracies in general many-body systems.

  11. Charge transport, configuration interaction and Rydberg states under density functional theory

    E-Print Network [OSTI]

    Cheng, Chiao-Lun

    2008-01-01

    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 ...

  12. Double-hybrid density-functional theory with meta-generalized-gradient approximations

    SciTech Connect (OSTI)

    Souvi, Sidi M. O. Sharkas, Kamal; Toulouse, Julien; CNRS, UMR 7616, Laboratoire de Chimie Théorique, F-75005 Paris

    2014-02-28

    We extend the previously proposed one-parameter double-hybrid density-functional theory [K. Sharkas, J. Toulouse, and A. Savin, J. Chem. Phys. 134, 064113 (2011)] to meta-generalized-gradient-approximation (meta-GGA) exchange-correlation density functionals. We construct several variants of one-parameter double-hybrid approximations using the Tao-Perdew-Staroverov-Scuseria (TPSS) meta-GGA functional and test them on test sets of atomization energies and reaction barrier heights. The most accurate variant uses the uniform coordinate scaling of the density and of the kinetic energy density in the correlation functional, and improves over both standard Kohn-Sham TPSS and second-order Møller-Plesset calculations.

  13. Low density expansion and isospin dependence of nuclear energy functional: comparison between relativistic and Skyrme models

    E-Print Network [OSTI]

    C. Providencia; D. P. Menezes; L. Brito; Ph. Chomaz

    2007-04-26

    In the present work we take the non relativistic limit of relativistic models and compare the obtained functionals with the usual Skyrme parametrization. Relativistic models with both constant couplings and with density dependent couplings are considered. While some models present very good results already at the lowest order in the density, models with non-linear terms only reproduce the energy functional if higher order terms are taken into account in the expansion.

  14. The Hubbard Dimer: A density functional case study of a many-body problem

    E-Print Network [OSTI]

    Carrascal, Diego; Smith, Justin C; Burke, Kieron

    2015-01-01

    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...

  15. Exact relations of the quasienergy functional and the exchange-correlation potential from the Floquet formulation of time-dependent density functional theory

    E-Print Network [OSTI]

    Telnov, Dmitry A.; Chu, Shih-I

    2000-12-13

    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 ...

  16. Electronic density-of-states of amorphous vanadium pentoxide films: Electrochemical data and density functional theory calculations

    SciTech Connect (OSTI)

    Lykissa, Iliana; Li, Shu-Yi; Granqvist, Claes G.; Niklasson, Gunnar A.; Ramzan, Muhammad; Chakraborty, Sudip; Ahuja, Rajeev

    2014-05-14

    Thin films of V{sub 2}O{sub 5} were prepared by sputter deposition onto transparent and electrically conducting substrates and were found to be X-ray amorphous. Their electrochemical density of states was determined by chronopotentiometry and displayed a pronounced low-energy peak followed by an almost featureless contribution at higher energies. These results were compared with density functional theory calculations for amorphous V{sub 2}O{sub 5}. Significant similarities were found between measured data and computations; specifically, the experimental low-energy peak corresponds to a split-off part of the conduction band apparent in the computations. Furthermore, the calculations approximately reproduce the experimental band gap observed in optical measurements.

  17. Level density of $^{56}$Fe and low-energy enhancement of $?$-strength function

    E-Print Network [OSTI]

    A. V. Voinov; S. M. Grimes; U. Agvaanluvsan; E. Algin; T. Belgya; C. R. Brune; M. Guttormsen; M. J. Hornish; T. Massey; G. E. Mitchell; J. Rekstad; A. Schiller; S. Siem

    2006-04-06

    The $^{55}$Mn$(d,n)^{56}$Fe differential cross section is measured at $E_d=7$ MeV\\@. The $^{56}$Fe level density obtained from neutron evaporation spectra is compared to the level density extracted from the $^{57}$Fe$(^3$He,$\\alpha\\gamma)^{56}$Fe reaction by the Oslo-type technique. Good agreement is found between the level densities determined by the two methods. With the level density function obtained from the neutron evaporation spectra, the $^{56}$Fe $\\gamma$-strength function is also determined from the first-generation $\\gamma$ matrix of the Oslo experiment. The good agreement between the past and present results for the $\\gamma$-strength function supports the validity of both methods and is consistent with the low-energy enhancement of the $\\gamma$ strength below $\\sim 4$ MeV first discovered by the Oslo method in iron and molybdenum isotopes.

  18. Erratum: "Density-functional and electron correlated study of five linear birefringences--Kerr, CottonMouton, Buckingham, Jones and

    E-Print Network [OSTI]

    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

  19. New parameterization of Skyrme's interaction for regularized multi-reference energy density functional calculations

    E-Print Network [OSTI]

    K. Washiyama; K. Bennaceur; B. Avez; M. Bender; P. -H. Heenen; V. Hellemans

    2012-09-24

    [Background] Symmetry restoration and configuration mixing in the spirit of the generator coordinate method based on energy density functionals have become widely used techniques in low-energy nuclear structure physics. Recently, it has been pointed out that these techniques are ill-defined for standard Skyrme functionals, and a regularization procedure has been proposed to remove the resulting spuriosities from such calculations. This procedure imposes an integer power of the density for the density dependent terms of the functional. At present, only dated parameterizations of the Skyrme interaction fulfill this condition. [Purpose] To construct a set of parameterizations of the Skyrme energy density functional for multi-reference energy density functional calculations with regularization using the state-of-the-art fitting protocols. [Method] The parameterizations were adjusted to reproduce ground state properties of a selected set of doubly magic nuclei and properties of nuclear matter. Subsequently, these parameter sets were validated against properties of spherical and deformed nuclei. [Results] Our parameter sets successfully reproduce the experimental binding energies and charge radii for a wide range of singly-magic nuclei. Compared to the widely used SLy5 and to the SIII parameterization that has integer powers of the density, a significant improvement of the reproduction of the data is observed. Similarly, a good description of the deformation properties at $A\\sim 80$ was obtained. [Conclusions] We have constructed new Skyrme parameterizations with integer powers of the density and validated them against a broad set of experimental data for spherical and deformed nuclei. These parameterizations are tailor-made for regularized multi-reference energy density functional calculations and can be used to study correlations beyond the mean-field in atomic nuclei.

  20. Continuity equation and local gauge invariance for the N3LO nuclear Energy Density Functionals

    E-Print Network [OSTI]

    F. Raimondi; B. G. Carlsson; J. Dobaczewski; J. Toivanen

    2011-10-13

    Background: The next-to-next-to-next-to-leading order (N3LO) nuclear energy density functional extends the standard Skyrme functional with new terms depending on higher-order derivatives of densities, introduced to gain better precision in the nuclear many-body calculations. A thorough study of the transformation properties of the functional with respect to different symmetries is required, as a step preliminary to the adjustment of the coupling constants. Purpose: Determine to which extent the presence of higher-order derivatives in the functional can be compatible with the continuity equation. In particular, to study the relations between the validity of the continuity equation and invariance of the functional under gauge transformations. Methods: Derive conditions for the validity of the continuity equation in the framework of time-dependent density functional theory. The conditions apply separately to the four spin-isospin channels of the one-body density matrix. Results: We obtained four sets of constraints on the coupling constants of the N3LO energy density functional that guarantee the validity of the continuity equation in all spin-isospin channels. In particular, for the scalar-isoscalar channel, the constraints are the same as those resulting from imposing the standard U(1) local-gauge-invariance conditions. Conclusions: Validity of the continuity equation in the four spin-isospin channels is equivalent to the local-gauge invariance of the energy density functional. For vector and isovector channels, such validity requires the invariance of the functional under local rotations in the spin and isospin spaces.

  1. Phonons and related crystal properties from density-functional perturbation theory

    E-Print Network [OSTI]

    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

  2. Valence excitation energies of alkenes, carbonyl compounds, and azabenzenes by time-dependent density functional theory: Linear response

    E-Print Network [OSTI]

    Truhlar, Donald G

    -dependent density functional theory: Linear response of the ground state compared to collinear and noncollinear spin, carbonyl compounds, and azabenzenes by time-dependent density functional theory: Linear response; accepted 13 March 2013; published online 3 April 2013) Time-dependent density functional theory (TDDFT

  3. Time-dependent localized Hartree-Fock density-functional linear response approach for photoionization of atomic excited states

    E-Print Network [OSTI]

    Chu, Shih-I

    Time-dependent localized Hartree-Fock density-functional linear response approach-dependent localized Hartree-Fock density-functional linear response approach for the treatment of photoionization, density-functional theory DFT com- bined with linear response approximation LRA 1,2 has been successfully

  4. arXiv:1003.1143v1[nucl-th]4Mar2010 Nuclear energy density functional from chiral

    E-Print Network [OSTI]

    Weise, Wolfram

    arXiv:1003.1143v1[nucl-th]4Mar2010 Nuclear energy density functional from chiral pion energy density functional approach is the many-body method of choice in order to calculate the properties nuclear energy density functional [10, 11, 12] focusses less on the fitting of experimental data

  5. arXiv:0912.3207v1[nucl-th]16Dec2009 Nuclear energy density functional from

    E-Print Network [OSTI]

    Weise, Wolfram

    arXiv:0912.3207v1[nucl-th]16Dec2009 Nuclear energy density functional from chiral pion to calculate the nuclear energy density functional in the framework of in-medium chiral perturbation theory-loop order. We find that the effective nucleon mass M() entering the energy density functional is identical

  6. Density functional with full exact exchange, balanced nonlocality of correlations, and constraint satisfaction

    SciTech Connect (OSTI)

    Tao, Jianmin; Perdew, John P; Staroverov, Viktor N; Scuseria, Gustavo E

    2008-01-01

    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'.

  7. Molecular Density Functional Theory for water with liquid-gas coexistence and correct pressure

    E-Print Network [OSTI]

    Jeanmairet, Guillaume; Sergiievskyi, Volodymyr; Borgis, Daniel

    2015-01-01

    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...

  8. Meng Law, MD Amit M. Saindane, MD

    E-Print Network [OSTI]

    Laidlaw, David

    , flow dynamics, 17.12144 Magnetic resonance (MR), perfusion study, 18.12144 Sclerosis, multiple, 18 function CBF cerebral blood flow CBV cerebral blood volume MS multiple sclerosis MTT mean transit time NAWM in Relapsing-Remitting Multiple Sclerosis: Perfusion MR Imaging Findings in Normal-appearing White Matter1

  9. Isospin coupling-channel decomposition of nuclear symmetry energy in covariant density functional theory

    E-Print Network [OSTI]

    Qian Zhao; Bao Yuan Sun; Wen Hui Long

    2014-11-23

    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.

  10. Constraints on the inner edge of neutron star crusts from relativistic nuclear energy density functionals

    SciTech Connect (OSTI)

    Moustakidis, Ch. C.; Lalazissis, G. A.; Niksic, T.; Vretenar, D.; Ring, P.

    2010-06-15

    The transition density n{sub t} and pressure P{sub t} at the inner edge between the liquid core and the solid crust of a neutron star are analyzed using the thermodynamical method and the framework of relativistic nuclear energy density functionals. Starting from a functional that has been carefully adjusted to experimental binding energies of finite nuclei, and varying the density dependence of the corresponding symmetry energy within the limits determined by isovector properties of finite nuclei, we estimate the constraints on the core-crust transition density and pressure of neutron stars: 0.086 fm{sup -3}<=n{sub t}<0.090 fm{sup -3} and 0.3 MeV fm{sup -3}

  11. Density functional theory of freezing for soft interactions in two dimensions

    E-Print Network [OSTI]

    Sven van Teeffelen; Christos N. Likos; Norman Hoffmann; Hartmut Löwen

    2006-04-18

    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.

  12. Interaction energies of monosubstituted benzene dimers via nonlocal density functional theory

    E-Print Network [OSTI]

    T. Thonhauser; Aaron Puzder; David C. Langreth

    2005-09-15

    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.

  13. Isovector part of nuclear energy density functional from chiral two- and three-nucleon forces

    E-Print Network [OSTI]

    N. Kaiser

    2012-03-28

    A recent calculation of the nuclear energy density functional from chiral two- and three-nucleon forces is extended to the isovector terms pertaining to different proton and neutron densities. An improved density-matrix expansion is adapted to the situation of small isospin-asymmetries and used to calculate in the Hartree-Fock approximation the density-dependent strength functions associated with the isovector terms. The two-body interaction comprises of long-range multi-pion exchange contributions and a set of contact terms contributing up to fourth power in momenta. In addition, the leading order chiral three-nucleon interaction is employed with its parameters fixed in computations of nuclear few-body systems. With this input one finds for the asymmetry energy of nuclear matter the value $A(\\rho_0) \\simeq 26.5\\,$MeV, compatible with existing semi-empirical determinations. The strength functions of the isovector surface and spin-orbit coupling terms come out much smaller than those of the analogous isoscalar coupling terms and in the relevant density range one finds agreement with phenomenological Skyrme forces. The specific isospin- and density-dependences arising from the chiral two- and three-nucleon interactions can be explored and tested in neutron-rich systems.

  14. A density functional theory study of electric potential saturation: planar geometry

    E-Print Network [OSTI]

    Gabriel Tellez; Emmanuel Trizac

    2003-08-01

    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.

  15. The Kinetic Energy of Hydrocarbons as a Function of Electron Density and Convolutional Neural Networks

    E-Print Network [OSTI]

    Yao, Kun

    2015-01-01

    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.

  16. Theory of melting at high pressures: Amending density functional theory with quantum Monte Carlo

    SciTech Connect (OSTI)

    Shulenburger, L.; Desjarlais, M. P.; Mattsson, T. R.

    2014-10-01

    We present an improved first-principles description of melting under pressure based on thermodynamic integration comparing Density Functional Theory (DFT) and quantum Monte Carlo (QMC) treatments of the system. The method is applied to address the longstanding discrepancy between density functional theory (DFT) calculations and diamond anvil cell (DAC) experiments on the melting curve of xenon, a noble gas solid where van der Waals binding is challenging for traditional DFT methods. The calculations show excellent agreement with data below 20 GPa and that the high-pressure melt curve is well described by a Lindemann behavior up to at least 80 GPa, a finding in stark contrast to DAC data.

  17. Ultra-nonlocality in density functional theory for photo-emission spectroscopy

    SciTech Connect (OSTI)

    Uimonen, A.-M.; Stefanucci, G.; INFN, Laboratori Nazionali di Frascati, Via E. Fermi 40, 00044 Frascati; European Theoretical Spectroscopy Facility , Louvain-la Neuve ; Leeuwen, R. van; European Theoretical Spectroscopy Facility , Louvain-la Neuve

    2014-05-14

    We derive an exact expression for the photocurrent of photo-emission spectroscopy using time-dependent current density functional theory (TDCDFT). This expression is given as an integral over the Kohn-Sham spectral function renormalized by effective potentials that depend on the exchange-correlation kernel of current density functional theory. We analyze in detail the physical content of this expression by making a connection between the density-functional expression and the diagrammatic expansion of the photocurrent within many-body perturbation theory. We further demonstrate that the density functional expression does not provide us with information on the kinetic energy distribution of the photo-electrons. Such information can, in principle, be obtained from TDCDFT by exactly modeling the experiment in which the photocurrent is split into energy contributions by means of an external electromagnetic field outside the sample, as is done in standard detectors. We find, however, that this procedure produces very nonlocal correlations between the exchange-correlation fields in the sample and the detector.

  18. On the accuracy of density-functional theory exchange-correlation functionals for H bonds in small water clusters. II. The water hexamer

    E-Print Network [OSTI]

    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

  19. A new local density functional for main-group thermochemistry, transition metal bonding, thermochemical kinetics, and noncovalent interactions

    E-Print Network [OSTI]

    Truhlar, Donald G

    A new local density functional for main-group thermochemistry, transition metal bonding online 15 November 2006 We present a new local density functional, called M06-L, for main is designed to capture the main dependence of the exchange-correlation energy on local spin density, spin

  20. Analytic Representations of Bath Correlation Functions for Ohmic and Superohmic Spectral Densities Using Simple Poles

    E-Print Network [OSTI]

    Gerhard Ritschel; Alexander Eisfeld

    2014-08-19

    We present a scheme to express a bath correlation function (BCF) corresponding to a given spectral density (SD) as a sum of damped harmonic oscillations. Such a representation is needed, for example, in many open quantum system approaches. To this end we introduce a class of fit functions that enables us to model ohmic as well as superohmic behavior. We show that these functions allow for an analytic calculation of the BCF using pole expansions of the temperature dependent hyperbolic cotangent. We demonstrate how to use these functions to fit spectral densities exemplarily for cases encountered in the description of photosynthetic light harvesting complexes. Finally, we compare absorption spectra obtained for different fits with exact spectra and show that it is crucial to take properly into account the behavior at small frequencies when fitting a given SD.

  1. The quest for a universal density functional: The accuracy of density functionals across a broad spectrum of databases in chemistry and physics

    E-Print Network [OSTI]

    Peverati, Roberto

    2012-01-01

    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 ...

  2. Orbital-free density functional theory of out-of-plane charge screening in graphene

    E-Print Network [OSTI]

    Jianfeng Lu; Vitaly Moroz; Cyrill B. Muratov

    2015-06-30

    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.

  3. Extended Lagrangian Density Functional Tight-Binding Molecular Dynamics for Molecules and Solids

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

    Aradi, Bálint; Niklasson, Anders M. N.; Frauenheim, Thomas

    2015-06-26

    A computationally fast quantum mechanical molecular dynamics scheme using an extended Lagrangian density functional tight-binding formulation has been developed and implemented in the DFTB+ electronic structure program package for simulations of solids and molecular systems. The scheme combines the computational speed of self-consistent density functional tight-binding theory with the efficiency and long-term accuracy of extended Lagrangian Born–Oppenheimer molecular dynamics. Furthermore, for systems without self-consistent charge instabilities, only a single diagonalization or construction of the single-particle density matrix is required in each time step. The molecular dynamics simulation scheme can also be applied to a broad range of problems in materialsmore »science, chemistry, and biology.« less

  4. PHYSICAL REVIEW C 74, 034301 (2006) Effective quadrupole-quadrupole interaction from density functional theory

    E-Print Network [OSTI]

    Bertsch George F.

    2006-01-01

    called density functional theory,1 and the other is the configuration-interaction shell-model (CISM energies, and the treatment of excitations requires extensions of the theory. In contrast, the CISM gives] proposed to use the SCMF to determine the single-particle Hamiltonian of the CISM so as to gain

  5. Density Functional Theory investigations of titanium gamma-surfaces and stacking faults

    E-Print Network [OSTI]

    Benoit, Magali; Morillo, Joseph

    2015-01-01

    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.

  6. A quadrature-based LES/transported probability density function approach for

    E-Print Network [OSTI]

    Raman, Venkat

    and a cavity-stabilized supersonic combustor. Comparisons with experimental data demon- strate the predictiveA quadrature-based LES/transported probability density function approach for modeling supersonic the direct quadrature method of moments (DQMOM) is developed for evolving the PDF-based supersonic combustion

  7. Density functional study of molecular crystals: Polyethylene and a crystalline analog of bisphenol-A polycarbonate

    E-Print Network [OSTI]

    Density functional study of molecular crystals: Polyethylene and a crystalline analog of bisphenol polyethylene comprising covalently bonded parallel chains with weak interchain interactions, and b reaction barriers.8 In a recent study of the interchain interactions in crystalline polyethylene PE ,9 we

  8. A Framework to Determine the Probability Density Function for the Output Power of Wind Farms

    E-Print Network [OSTI]

    Dominguez-Garcia, Alejandro

    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

  9. Freezing of 4 He and its liquid-solid interface from density functional theory

    E-Print Network [OSTI]

    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

  10. A Density Functional Theory Study of Hydrogen Adsorption in MOF-5 Tim Mueller and Gerbrand Ceder*

    E-Print Network [OSTI]

    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

  11. van der Waals density functional study of CO2 binding in zeolitic imidazolate frameworks

    E-Print Network [OSTI]

    Ray, Keith G.; Olmsted, David; He, Ning; Houndonougbo, Yao; Laird, Brian Bostian; Asta, Mark

    2012-02-06

    The van der Waals density functional (vdW-DF) formalism is employed in a study of the binding energetics for CO2 in a set of five zeolitic imidazolate framework (ZIF) compounds. The ZIF structures investigated share the same RHO-type zeolite...

  12. Density functional study of chemical reaction equilibrium for dimerization reactions in slit and cylindrical nanopores

    E-Print Network [OSTI]

    Lisal, Martin

    Density functional study of chemical reaction equilibrium for dimerization reactions in slit a theoretical study of the effects of confinement on chemical reaction equilibrium in slit and cylindrical equilibrium, for which much less is known. The behavior of chemical reactions in confinement spans a wide

  13. Relativistic density functional theory modeling of plutonium and americium higher oxide molecules

    E-Print Network [OSTI]

    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

  14. Carbon species confined inside carbon nanotubes: A density functional study Yi Liu and R. O. Jones*

    E-Print Network [OSTI]

    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

  15. LARGE EDDY SIMULATION/EULERIAN PROBABILITY DENSITY FUNCTION APPROACH FOR SIMULATING HYDROGEN-ENRICHED GAS TURBINE

    E-Print Network [OSTI]

    Raman, Venkat

    LARGE EDDY SIMULATION/EULERIAN PROBABILITY DENSITY FUNCTION APPROACH FOR SIMULATING HYDROGEN 78712 Email: v.raman@mail.utexas.edu Scott Martin Siemens Energy Corp. Orlando, Florida Email:scott.m.martin@siemens.com ABSTRACT To describe partially-premixed combustion inside hydrogen- rich combustors, a novel quadrature

  16. Two-scale convergence of elliptic spectral problems with indefinite density function in perforated domains

    E-Print Network [OSTI]

    Douanla, Hermann Yonta

    2011-01-01

    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.

  17. Two-scale convergence of elliptic spectral problems with indefinite density function in perforated domains

    E-Print Network [OSTI]

    Hermann Yonta Douanla

    2012-08-21

    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.

  18. Multiresolution quantum chemistry in multiwavelet bases: Analytic derivatives for HartreeFock and density functional theory

    E-Print Network [OSTI]

    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

  19. Energy density functional analysis of shape coexistence in {sup 44}S

    SciTech Connect (OSTI)

    Li, Z. P.; Yao, J. M.; Vretenar, D.; Niksic, T.; Meng, J.

    2012-10-20

    The structure of low-energy collective states in the neutron-rich nucleus {sup 44}S is analyzed using a microscopic collective Hamiltonian model based on energy density functionals (EDFs). The calculated triaxial energy map, low-energy spectrum and corresponding probability distributions indicate a coexistence of prolate and oblate shapes in this nucleus.

  20. Electronvibration coupling in time-dependent density-functional theory: Application to benzene

    E-Print Network [OSTI]

    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

  1. The 2dF Galaxy Redshift Survey: luminosity functions by density environment and galaxy type

    E-Print Network [OSTI]

    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

    2005-02-08

    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.

  2. A density functional theory study of hydroxyl and the intermediate in the water formation reaction on Pt

    E-Print Network [OSTI]

    Alavi, Ali

    A density functional theory study of hydroxyl and the intermediate in the water formation reaction: Wed, 28 Jan 2015 16:19:40 #12;A density functional theory study of hydroxyl and the intermediate functional theory has been used to study the adsorption of hydroxyl at low and high coverages and also

  3. Assessment of Density Functional Methods for Exciton Binding Energies and Related Optoelectronic Properties

    E-Print Network [OSTI]

    Lee, Jui-Che; Lin, Shiang-Tai

    2015-01-01

    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...

  4. Assessment of Density Functional Methods for Exciton Binding Energies and Related Optoelectronic Properties

    E-Print Network [OSTI]

    Jui-Che Lee; Jeng-Da Chai; Shiang-Tai Lin

    2015-08-29

    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 investigated.

  5. Fundamental gaps with approximate density functionals: The derivative discontinuity revealed from ensemble considerations

    SciTech Connect (OSTI)

    Kraisler, Eli; Kronik, Leeor

    2014-05-14

    The fundamental gap is a central quantity in the electronic structure of matter. Unfortunately, the fundamental gap is not generally equal to the Kohn-Sham gap of density functional theory (DFT), even in principle. The two gaps differ precisely by the derivative discontinuity, namely, an abrupt change in slope of the exchange-correlation energy as a function of electron number, expected across an integer-electron point. Popular approximate functionals are thought to be devoid of a derivative discontinuity, strongly compromising their performance for prediction of spectroscopic properties. Here we show that, in fact, all exchange-correlation functionals possess a derivative discontinuity, which arises naturally from the application of ensemble considerations within DFT, without any empiricism. This derivative discontinuity can be expressed in closed form using only quantities obtained in the course of a standard DFT calculation of the neutral system. For small, finite systems, addition of this derivative discontinuity indeed results in a greatly improved prediction for the fundamental gap, even when based on the most simple approximate exchange-correlation density functional – the local density approximation (LDA). For solids, the same scheme is exact in principle, but when applied to LDA it results in a vanishing derivative discontinuity correction. This failure is shown to be directly related to the failure of LDA in predicting fundamental gaps from total energy differences in extended systems.

  6. Time-dependent density functional theory quantum transport simulation in non-orthogonal basis

    SciTech Connect (OSTI)

    Kwok, Yan Ho; Xie, Hang; Yam, Chi Yung; Chen, Guan Hua; Zheng, Xiao

    2013-12-14

    Basing on the earlier works on the hierarchical equations of motion for quantum transport, we present in this paper a first principles scheme for time-dependent quantum transport by combining time-dependent density functional theory (TDDFT) and Keldysh's non-equilibrium Green's function formalism. This scheme is beyond the wide band limit approximation and is directly applicable to the case of non-orthogonal basis without the need of basis transformation. The overlap between the basis in the lead and the device region is treated properly by including it in the self-energy and it can be shown that this approach is equivalent to a lead-device orthogonalization. This scheme has been implemented at both TDDFT and density functional tight-binding level. Simulation results are presented to demonstrate our method and comparison with wide band limit approximation is made. Finally, the sparsity of the matrices and computational complexity of this method are analyzed.

  7. Local pressure of confined fluids inside nanoslit pores -- A density functional theory prediction

    E-Print Network [OSTI]

    F. Heidari; G. A. Mansoori; E. Keshavarzi

    2013-07-18

    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.

  8. Role of exchange in density-functional theory for weakly interacting systems: Quantum Monte Carlo analysis of electron density and interaction energy

    E-Print Network [OSTI]

    Grossman, Jeffrey C.

    We analyze the density-functional theory (DFT) description of weak interactions by employing diffusion and reptation quantum Monte Carlo (QMC) calculations, for a set of benzene-molecule complexes. While the binding energies ...

  9. Matrix Methods for Estimating the Coherence Functions from Estimates of the Cross-Spectral Density Matrix

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

    Smallwood, D.O.

    1996-01-01

    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.

  10. Dynamical density functional theory for the diffusion of injected Brownian particles

    E-Print Network [OSTI]

    H. Löwen; M. Heinen

    2014-09-08

    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.

  11. Rume nach Gebude Gebude MD Hirnbckhalle

    E-Print Network [OSTI]

    Arnold, Anton

    EG 01 Lager 4.1 Lagerräume 222 100 200 28,30 MD EG 02 Wasserbaulabor 3.1 Werkhallen 222 100 200 182,90 MD EG 07 Werkstätte 3.1 Werkhallen 222 100 200 200,36 MD EG 18 Wasserbaulabor 3.1 Werkhallen 222 100 200 1.128,10 MD EG 25 Sozialraum 1.2 Gemeinschaftsräume 222 100 200 17,95 MD EG 25A Dusche, Vorraum 7

  12. Electronic and structural properties of ultrathin tungsten nanowires and nanotubes by density functional theory calculation

    SciTech Connect (OSTI)

    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)

    2014-10-07

    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.

  13. Theory of melting at high pressures: Amending density functional theory with quantum Monte Carlo

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

    Shulenburger, L.; Desjarlais, M. P.; Mattsson, T. R.

    2014-10-01

    We present an improved first-principles description of melting under pressure based on thermodynamic integration comparing Density Functional Theory (DFT) and quantum Monte Carlo (QMC) treatments of the system. The method is applied to address the longstanding discrepancy between density functional theory (DFT) calculations and diamond anvil cell (DAC) experiments on the melting curve of xenon, a noble gas solid where van der Waals binding is challenging for traditional DFT methods. The calculations show excellent agreement with data below 20 GPa and that the high-pressure melt curve is well described by a Lindemann behavior up to at least 80 GPa, amore »finding in stark contrast to DAC data.« less

  14. The Van der Waals interaction of the hydrogen molecule - an exact local energy density functional

    E-Print Network [OSTI]

    T. C. Choy

    1999-11-26

    We verify that the van der Waals interaction and hence all dispersion interactions for the hydrogen molecule given by: W"= -{A/R^6}-{B/R^8}-{C/R^10}- ..., in which R is the internuclear separation, are exactly soluble. The constants A=6.4990267..., B=124.3990835 ... and C=1135.2140398... (in Hartree units) first obtained approximately by Pauling and Beach (PB) [1] using a linear variational method, can be shown to be obtainable to any desired accuracy via our exact solution. In addition we shall show that a local energy density functional can be obtained, whose variational solution rederives the exact solution for this problem. This demonstrates explicitly that a static local density functional theory exists for this system. We conclude with remarks about generalising the method to other hydrogenic systems and also to helium.

  15. Quark-Antiquark Energy Density Function applied to Di-Gauge Boson Production at the LHC

    E-Print Network [OSTI]

    Gideon Alexander; Erez Reinherz-Aronis

    2008-09-03

    In view of the start up of the 14 TeV pp Large Hadron Collider the quark anti-quark reactions leading to the final states W^+W^-, W^+-Z^0 and Z^0Z^0 are studied, in the frame workn of the Standard Model (SM), using helicity amplitudes. The differential and total cross sections are first evaluated in the parton-parton center of mass system. They are then transformed to their expected behavior in pp collisions through the parton-parton Energy Density Functions which are here derived from the known Parton Density Functions of the proton. In particular the single and joint longitudinal polarizations of the final state di-bosons are calculated. The effect on these reactions from the presence of s-channel heavy vector bosons, like the W' and Z', are evaluated to explore the possibility to utilize the gauge boson pair production as a probe for these 'Beyond the SM' phenomena.

  16. Acoustic Kappa-Density Fluctuation Waves in Suprathermal Kappa Function Fluids

    E-Print Network [OSTI]

    Michael R. Collier; Aaron Roberts; Adolfo Vinas

    2007-10-20

    We describe a new wave mode similar to the acoustic wave in which both density and velocity fluctuate. Unlike the acoustic wave in which the underlying distribution is Maxwellian, this new wave mode occurs when the underlying distribution is a suprathermal kappa function and involves fluctuations in the power law index, kappa. This wave mode always propagates faster than the acoustic wave with an equivalent effective temperature and becomes the acoustic wave in the Maxwellian limit as kappa goes to infinity.

  17. Linear-response calculation in the time-dependent density functional theory

    E-Print Network [OSTI]

    Takashi Nakatsukasa; Tsunenori Inakura; Paolo Avogadro; Shuichiro Ebata; Koichi Sato; Kazuhiro Yabana

    2012-09-22

    Linear response calculations based on the time-dependent density-functional theory are presented. Especially, we report results of the finite amplitude method which we have recently proposed as an alternative and feasible approach to the (quasiparticle-)random-phase approximation. Calculated properties of the giant resonances and low-energy E1 modes are discussed. We found a universal linear correlation between the low-energy E1 strength and the neutron skin thickness.

  18. Generalized second law at linear order for actions that are functions of Lovelock densities

    E-Print Network [OSTI]

    Sudipta Sarkar; Aron C. Wall

    2015-05-19

    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.

  19. Nuclear charge-exchange excitations in localized covariant density functional theory

    E-Print Network [OSTI]

    H. Z. Liang; J. Meng; T. Nakatsukasa; Z. M. Niu; P. Ring; X. Roca-Maza; N. Van Giai; P. W. Zhao

    2013-10-15

    The recent progress in the studies of nuclear charge-exchange excitations with localized covariant density functional theory is briefly presented, by taking the fine structure of spin-dipole excitations in 16O as an example. It is shown that the constraints introduced by the Fock terms of the relativistic Hartree-Fock scheme into the particle-hole residual interactions are straightforward and robust.

  20. Steam Reforming on Transition-metal Carbides from Density-functional Theory

    SciTech Connect (OSTI)

    Vojvodic, Aleksandra

    2012-05-11

    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.

  1. Nuclear energy density functionals: What we can learn about/from their global performance?

    SciTech Connect (OSTI)

    Afanasjev, A. V.; Agbemava, S. E.; Ray, D.; Ring, P.

    2014-10-15

    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.

  2. Application of nuclear density functionals to lepton number violating weak processes

    SciTech Connect (OSTI)

    Rodriguez, Tomas R.; Martinez-Pinedo, Gabriel

    2012-10-20

    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.

  3. Covariant density functional theory with two-phonon coupling in nuclei

    SciTech Connect (OSTI)

    Ring, P.; Litvinova, E.; Tselyaev, V.

    2012-10-20

    A full description of excited states within the framework of density functional theory requires energy dependent self energies. We present a new class of many-body models. It allows a parameter free description of the fragmentation of nuclear states induced by mode coupling of two-quasiparticle and two-phonon configurations. The method is applied for an investigation of low-lying dipole excitations in Sn isotopes with large neutron excess.

  4. Freezing of soft spheres: A critical test for weighted-density-functional theories

    E-Print Network [OSTI]

    Laird, Brian Bostian; Kroll, D. M.

    1990-10-15

    ~ d e ry, r2, & p r2 —p, 0 4814 BRIAN B. LAIRD AND D. M. KROLL 42 Since C is, for the most part, unknown, we approxi- mate it by an as yet unspecified homogeneous two-point function g: C(ri, r2; [p]) = g(~ ri —rz ~; p) . (25) This approximation is due..., NUMBER 8 15 OCTOBER 1990 Freezing of soft spheres: A critical test for weighted-density-functional theories Brian B. Laird and D.M. Kroll Institut fur Festkorperforschung, Forschungszentrurn Julich G rn .b H. .., Postfach I9IS, D SI7-0 Jiilich I, Federal...

  5. A density functional theory study of the correlation between analyte basicity, ZnPc adsorption strength, and sensor response

    E-Print Network [OSTI]

    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

  6. Thermally-assisted-occupation density functional theory with generalized-gradient approximations

    SciTech Connect (OSTI)

    Chai, Jeng-Da

    2014-05-14

    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.

  7. Correlated density-dependent chiral forces for infinite matter calculations within the Green's function approach

    E-Print Network [OSTI]

    Arianna Carbone; Arnau Rios; Artur Polls

    2014-11-19

    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.

  8. Interactions in 1-ethyl-3-methyl imidazolium tetracyanoborate ion pair: Spectroscopic and density functional study

    SciTech Connect (OSTI)

    Mao, James X.; Lee, Anita S.; Kitchin, John R.; Nulwala, Hunaid B; Luebke, David R.; Damodaran, Krishnan

    2013-04-24

    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.

  9. Density Functional Study of the Structure, Stability and Oxygen Reduction Activity of Ultrathin Platinum Nanowires

    SciTech Connect (OSTI)

    Matanovic, Ivana; Kent, Paul; Garzon, Fernando; Henson, Neil J.

    2013-03-14

    We used density functional theory to study the difference in the structure, stability and catalytic reactivity between ultrathin, 0.5–1.0 nm diameter, platinum nanotubes and nanowires. Model nanowires were formed by inserting an inner chain of platinum atoms in small diameter nanotubes. In this way more stable, non-hollow structures were formed. The difference in the electronic structure of platinum nanotubes and nanowires was examined by inspecting the density of surface states and band structure. Furthermore, reactivity toward the oxygen reduction reaction of platinum nanowires was assessed by studying the change in the chemisorption energies of oxygen, hydroxyl, and hydroperoxyl groups, induced by converting the nanotube models to nanowires. Both ultrathin platinum nanotubes and nanowires show distinct properties compared to bulk platinum. Single-wall nanotubes and platinum nanowires with diameters larger than 1 nm show promise for use as oxygen reduction catalysts.

  10. Ground state properties and high pressure behavior of plutonium dioxide: Systematic density functional calculations

    E-Print Network [OSTI]

    Zhang, Ping; Zhao, Xian-Geng

    2010-01-01

    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...

  11. Quantitative assessment of electrostatic embedding in Density Functional Theory calculations of biomolecular systems

    SciTech Connect (OSTI)

    Fattebert, J; Law, R J; Bennion, B; Lau, E Y; Schwegler, E; Lightstone, F C

    2009-04-24

    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.

  12. Alternative separation of exchange and correlation energies in range-separated density-functional perturbation theory

    E-Print Network [OSTI]

    Cornaton, Yann; Jensen, Hans Jørgen Aa; Fromager, Emmanuel

    2013-01-01

    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...

  13. Optical absorption in B{sub 13} cluster: A time-dependent density functional approach

    SciTech Connect (OSTI)

    Shinde, Ravindra; Tayade, Meenakshi

    2013-02-05

    The linear optical absorption spectra of three isomers of planar boron cluster B{sub 13} are calculated using time-dependent spin-polarized density functional approach. The geometries of these cluster are optimized at the B3LYP/6-311+G* level of theory. Even though the isomers are almost degenerate, the calculated spectra are quite different, indicating a strong structure-property relationship. Therefore, these computed spectra can be used in the photo-absorption experiments to distinguish between different isomers of a cluster.

  14. Growth mechanism of atomic layer deposition of zinc oxide: A density functional theory approach

    SciTech Connect (OSTI)

    Afshar, Amir; Cadien, Kenneth C., E-mail: kcadien@ualberta.ca [Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta T6G 2V4 (Canada)

    2013-12-16

    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.

  15. Tuning Range-Separated Density Functional Theory for Photocatalytic Water Splitting Systems

    E-Print Network [OSTI]

    Bokareva, Olga S; Bokarev, Sergey I; Kühn, Oliver

    2015-01-01

    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.

  16. Ferromagnetism in Mn Substituted Zirconia: A Density-functional Theory Study

    E-Print Network [OSTI]

    Xingtao Jia; Wei Yang; Minghui Qin; Xinglai Zhang; Mingai Sun; Jianping Li

    2008-09-05

    We study the electronic structure and magnetism of 25% Mn substituted cubic Zirconia (ZrO2) with several homogeneous and heterogeneous doping profiles using density-functional theory calculations. We find that all doping profiles show half-metallic ferromagnetism (HMF), and delta-doping is most energy favorable while homogeneous doping has largest ferromagnetic stabilization energy. Using crystal field theory, we discuss the formation scheme of HMF. Finally, we speculate the potential spintronics applications for Mn doped ZrO2, especially as spin direction controllment.

  17. Homogenization of Steklov spectral problems with indefinite density function in perforated domains

    E-Print Network [OSTI]

    Douanla, Hermann Yonta

    2011-01-01

    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.

  18. Homogenization of Steklov spectral problems with indefinite density function in perforated domains

    E-Print Network [OSTI]

    Hermann Yonta Douanla

    2012-08-21

    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.

  19. Interacting boson model from energy density functionals: {gamma}-softness and the related topics

    SciTech Connect (OSTI)

    Nomura, K.

    2012-10-20

    A comprehensive way of deriving the Hamiltonian of the interacting boson model (IBM) is described. Based on the fact that the multi-nucleon induced surface deformation in finite nucleus is simulated by effective boson degrees of freedom, the potential energy surface calculated with self-consistent mean-field method employing a given energy density functional (EDF) is mapped onto the IBM analog, and thereby the excitation spectra and transition rates with good symmetry quantum numbers are calculated. Recent applications of the proposed approach are reported: (i) an alternative robust interpretation of the {gamma}-soft nuclei and (ii) shape coexistence in lead isotopes.

  20. 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

    2014-12-22

    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

  1. Free Energy Calculations of Crystalline Hard Sphere Complexes Using Density Functional Theory

    SciTech Connect (OSTI)

    Gunawardana, K. G.S.H.; Song, Xueyu

    2014-12-22

    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, 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.

  2. Energy Density Functional Study of Nuclear Matrix Elements for Neutrinoless {beta}{beta} Decay

    SciTech Connect (OSTI)

    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)

    2010-12-17

    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.

  3. Quasi-particle energy spectra in local reduced density matrix functional theory

    SciTech Connect (OSTI)

    Lathiotakis, Nektarios N.; Helbig, Nicole; Rubio, Angel

    2014-10-28

    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.

  4. Density-functional theory of freezing of quantum liquids at zero temperature using exact liquid-state linear response

    E-Print Network [OSTI]

    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

  5. Steve Nelson, MD Backes, PhD

    E-Print Network [OSTI]

    Dean Steve Nelson, MD Associate Dean for Research Wayne Backes, PhD Associate Dean for Fiscal Gregory, PhD Assistant Dean of VA Affairs Paul Rosenfeld, MD Basic Science Department Heads (6) Clinical, MD Director of Basic Sciences Curriculum Michael Levitzky, PhD Assistant Dean at Children's Hospital

  6. Flow of colloidal solids and fluids through constrictions: dynamical density functional theory versus simulation

    E-Print Network [OSTI]

    Urs Zimmermann; Frank Smallenburg; Hartmut Löwen

    2015-12-02

    Using both dynamical density functional theory and particle-resolved Brownian dynamics simulations, we explore the flow of two-dimensional colloidal solids and fluids driven through a linear channel with a geometric constriction. The flow is generated by a constant external force acting on all colloids. The initial configuration is equilibrated in the absence of flow and then the external force is switched on instantaneously. Upon starting the flow, we observe four different scenarios: a complete blockade, a monotonic decay to a constant particle flux (typical for a fluid), a damped oscillatory behaviour in the particle flux, and a long-lived stop-and-go behaviour in the flow (typical for a solid). The dynamical density functional theory describes all four situations but predicts infinitely long undamped oscillations in the flow which are always damped in the simulations. We attribute the mechanisms of the underlying stop-and-go flow to symmetry conditions on the flowing solid. Our predictions are verifiable in real-space experiments on magnetic colloidal monolayers which are driven through structured microchannels and can be exploited to steer the flow throughput in microfluidics.

  7. Uncertainty Quantification for Nuclear Density Functional Theory and Information Content of New Measurements

    E-Print Network [OSTI]

    J. D. McDonnell; N. Schunck; D. Higdon; J. Sarich; S. M. Wild; W. Nazarewicz

    2015-01-15

    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.

  8. Quadrupole collective dynamics from energy density functionals: Collective Hamiltonian and the interacting boson model

    SciTech Connect (OSTI)

    Nomura, K.; Vretenar, D.; Niksic, T.; Otsuka, T.; Shimizu, N.

    2011-07-15

    Microscopic energy density functionals 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 paper, we compare two approaches to five-dimensional quadrupole dynamics: the collective Hamiltonian for quadrupole vibrations and rotations and the interacting boson model (IBM). The two models are compared in a study of the evolution of nonaxial shapes in Pt isotopes. Starting from the binding energy surfaces of {sup 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 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.

  9. Self-interaction-free density-functional theoretical study of the electronic structure of spherical and vertical quantum dots

    E-Print Network [OSTI]

    Jiang, T. F.; Tong, Xiao-Min; Chu, Shih-I

    2001-01-09

    We study the electronic structure and shell-filling effects of both spherical and vertical quantum dots by means of the density functional theory (DFT) with optimized effective potential (OEP) and self-interaction-correction (SIC) recently developed...

  10. Enantioselectivity of (321) chiral noble metal surfaces: A density functional theory study of lactate adsorption

    SciTech Connect (OSTI)

    Franke, J.-H.; Kosov, D. S.

    2013-12-14

    The adsorption of the chiral molecule lactate on the intrinsically chiral noble metal surfaces Pt(321), Au(321), and Ag(321) is studied by density functional theory calculations. We use the oPBE-vdW functional which includes van der Waals forces on an ab initio level. It is shown that the molecule binds via its carboxyl and the hydroxyl oxygen atoms to the surface. The binding energy is larger on Pt(321) and Ag(321) than on Au(321). An analysis of the contributions to the binding energy of the different molecular functional groups reveals that the deprotonated carboxyl group contributes most to the binding energy, with a much smaller contribution of the hydroxyl group. The Pt(321) surface shows considerable enantioselectivity of 0.06 eV. On Au(321) and Ag(321) it is much smaller if not vanishing. The chiral selectivity of the Pt(321) surface can be explained by two factors. First, it derives from the difference in van der Waals attraction of L- and D-lactate to the surface that we trace to differences in the binding energy of the methyl group. Second, the multi-point binding pattern for lactate on the Pt(321) surface is sterically more sensitive to surface chirality and also leads to large binding energy contributions of the hydroxyl group. We also calculate the charge transfer to the molecule and the work function to gauge changes in electronic structure of the adsorbed molecule. The work function is lowered by 0.8 eV on Pt(321) with much smaller changes on Au(321) and Ag(321)

  11. Microscopically-constrained Fock energy density functionals from chiral effective field theory. I. Two-nucleon interactions

    E-Print Network [OSTI]

    B. Gebremariam; S. K. Bogner; T. Duguet

    2010-03-26

    The density matrix expansion (DME) of Negele and Vautherin is a convenient tool to map finite-range physics associated with vacuum two- and three-nucleon interactions into the form of a Skyme-like energy density functional (EDF) with density-dependent couplings. In this work, we apply the improved formulation of the DME proposed recently in arXiv:0910.4979 by Gebremariam {\\it et al.} to the non-local Fock energy obtained from chiral effective field theory (EFT) two-nucleon (NN) interactions at next-to-next-to-leading-order (N$^2$LO). The structure of the chiral interactions is such that each coupling in the DME Fock functional can be decomposed into a cutoff-dependent coupling {\\it constant} arising from zero-range contact interactions and a cutoff-independent coupling {\\it function} of the density arising from the universal long-range pion exchanges. This motivates a new microscopically-guided Skyrme phenomenology where the density-dependent couplings associated with the underlying pion-exchange interactions are added to standard empirical Skyrme functionals, and the density-independent Skyrme parameters subsequently refit to data. A Mathematica notebook containing the novel density-dependent couplings is provided.

  12. Mixing of equations of state for xenon-deuterium using density functional theory

    SciTech Connect (OSTI)

    Magyar, Rudolph J.; Mattsson, Thomas R. [Sandia National Laboratories, Albuquerque, New Mexico 87185 (United States)

    2013-03-15

    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.

  13. Thermodynamics of baryonic matter with strangeness within non-relativistic energy density functional model

    E-Print Network [OSTI]

    Ad. R. Raduta; F. Gulminelli; M. Oertel

    2014-09-15

    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.

  14. Radical Coupling Reactions in Lignin Synthesis: A Density Functional Theory Study

    SciTech Connect (OSTI)

    Sangha, A. K.; Parks, J. M.; Standaert, R. F.; Ziebell, A.; Davis, M.; Smith, J. C.

    2012-04-26

    Lignin is a complex, heterogeneous polymer in plant cell walls that provides mechanical strength to the plant stem and confers resistance to degrading microbes, enzymes, and chemicals. Lignin synthesis initiates through oxidative radical-radical coupling of monolignols, the most common of which are p-coumaryl, coniferyl, and sinapyl alcohols. Here, we use density functional theory to characterize radical-radical coupling reactions involved in monolignol dimerization. We compute reaction enthalpies for the initial self- and cross-coupling reactions of these monolignol radicals to form dimeric intermediates via six major linkages observed in natural lignin. The 8-O-4, 8-8, and 8-5 coupling are computed to be the most favorable, whereas the 5-O-4, 5-5, and 8-1 linkages are less favorable. Overall, p-coumaryl self- and cross-coupling reactions are calculated to be the most favorable. For cross-coupling reactions, in which each radical can couple via either of the two sites involved in dimer formation, the more reactive of the two radicals is found to undergo coupling at its site with the highest spin density.

  15. Shape coexistence in Lead isotopes in the interacting boson model with Gogny energy density functional

    E-Print Network [OSTI]

    K. Nomura; R. Rodriguez-Guzman; L. M. Robledo; N. Shimizu

    2012-08-23

    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.

  16. Time-odd mean fields in covariant density functional theory I. Non-rotating systems

    E-Print Network [OSTI]

    A. V. Afanasjev; H. Abusara

    2010-10-09

    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.

  17. Density functional study of H-induced defects as nucleation sites in hybrid carbon nanomaterials.

    SciTech Connect (OSTI)

    Barnard, A.; Terranova, M. L.; Rossi, M.; Dip. Scienze e Tecnologie Chimiche; Dip di Energetica; INFM

    2005-01-01

    Recently we have reported on the growth of an exciting new class of hybrid nanostructured carbon materials, coupling nanosized diamond with single-walled carbon nanotubes. The inner structures were shown to be single-walled C nanotubes or bundles of single-walled nanotubes up to 15 {micro}m long, and the outer deposit consisted of faceted diamond crystallites with diameters in the range of 20-100 nm. To aid in understanding the mechanisms responsible for the formation of such materials, the present study uses density functional theory to examine the role of atomic hydrogen in creating localized sp{sup 3} hybridized defects on the outer wall of carbon nanotubes. The results illustrate that certain absorption configurations may produce defects containing dangling carbon bonds, and thus promote the formation of suitable sites for nanodiamond nucleation.

  18. Analytic cubic and quartic force fields using density-functional theory

    SciTech Connect (OSTI)

    Ringholm, Magnus; Gao, Bin; Thorvaldsen, Andreas J.; Ruud, Kenneth; Jonsson, Dan; High Performance Computing Group, University of Tromsø—The Arctic University of Norway, 9037 Tromsø ; Bast, Radovan; Ekström, Ulf; Helgaker, Trygve

    2014-01-21

    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.

  19. Time-dependent density functional studies of nuclear quantum dynamics in large amplitudes

    E-Print Network [OSTI]

    Wen, Kai; Fang, Ni; Nakatsukasa, Takashi

    2015-01-01

    The time-dependent density functional theory (TDDFT) provides a unified description of the structure and reaction. The linear approximation leads to the random-phase approximation (RPA) which is capable of describing a variety of collective motion in a harmonic regime. Beyond the linear regime, we present applications of the TDDFT to nuclear fusion and fission reaction. In particular, the extraction of the internuclear potential and the inertial mass parameter is performed using two different methods. A fusion hindrance mechanism for heavy systems is investigated from the microscopic point of view. The canonical collective variables are determined by the adiabatic self-consistent collective coordinate method. Preliminary results of the spontaneous fission path, the potential, and the collective mass parameter are shown for 8Be --> alpha+alpha.

  20. Wide range equation of state for fluid hydrogen from density functional theory

    SciTech Connect (OSTI)

    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)

    2013-09-15

    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.

  1. Nuclear matrix elements in neutrinoless double beta decay: beyond mean-field covariant density functional theory

    E-Print Network [OSTI]

    Yao, J M; Hagino, K; Ring, P; Meng, J

    2014-01-01

    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.

  2. The importance of nonlinear fluid response in joint density-functional theory studies of battery systems

    E-Print Network [OSTI]

    Gunceler, Deniz; Sundararaman, Ravishankar; Schwarz, Kathleen A; Arias, T A

    2013-01-01

    Delivering the full benefits of first principles calculations to battery materials demands the development of accurate and computationally-efficient electronic structure methods that incorporate the effects of the electrolyte environment and electrode potential. Realistic electrochemical interfaces containing polar surfaces are beyond the regime of validity of existing continuum solvation theories developed for molecules, due to the presence of significantly stronger electric fields. We present an ab initio theory of the nonlinear dielectric and ionic response of solvent environments within the framework of joint density-functional theory, with precisely the same optimizable parameters as conventional polarizable continuum models. We demonstrate that the resulting nonlinear theory agrees with the standard linear models for organic molecules and metallic surfaces under typical operating conditions. However, we find that the saturation effects in the rotational response of polar solvent molecules, inherent to o...

  3. Combinatorial density functional theory-based screening of surface alloys for the oxygen reduction reaction.

    SciTech Connect (OSTI)

    Greeley, J.; Norskov, J.; Center for Nanoscale Materials; Technical Univ. of Denmark

    2009-03-26

    A density functional theory (DFT) -based, combinatorial search for improved oxygen reduction reaction (ORR) catalysts is presented. A descriptor-based approach to estimate the ORR activity of binary surface alloys, wherein alloying occurs only in the surface layer, is described, and rigorous, potential-dependent computational tests of the stability of these alloys in aqueous, acidic environments are presented. These activity and stability criteria are applied to a database of DFT calculations on nearly 750 binary transition metal surface alloys; of these, many are predicted to be active for the ORR but, with few exceptions, they are found to be thermodynamically unstable in the acidic environments typical of low-temperature fuel cells. The results suggest that, absent other thermodynamic or kinetic mechanisms to stabilize the alloys, surface alloys are unlikely to serve as useful ORR catalysts over extended periods of operation.

  4. Density functional and theoretical study of the temperature and pressure dependency of the plasmon energy of solids

    SciTech Connect (OSTI)

    Attarian Shandiz, M. Gauvin, R.

    2014-10-28

    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.

  5. Applications of Skyrme energy-density functional to fusion reactions for synthesis of superheavy nuclei

    E-Print Network [OSTI]

    Ning Wang; Xizhen Wu; Zhuxia Li; Min Liu; Werner Scheid

    2006-09-18

    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.

  6. Coupled cluster benchmarks of water monomers and dimers extracted from density-functional theory liquid water: The importance of monomer

    E-Print Network [OSTI]

    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

  7. Spin Contamination in Hartree-Fock and Density Functional Theory Wavefunctions in Modeling of Adsorption on Graphite

    E-Print Network [OSTI]

    Truong, Thanh N.

    Spin Contamination in Hartree-Fock and Density Functional Theory Wavefunctions in Modeling: April 27, 2000 We have examined the effect of spin contamination in single determinant wave function) method, we found that UHF has a large spin contamination. Consequently, this yields large errors

  8. Tests of the RPBE, revPBE, -HCTHhyb, B97X-D, and MOHLYP density functional approximations and 29 others against representative

    E-Print Network [OSTI]

    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

  9. Validating density-functional theory simulations at high energy-density conditions with liquid krypton shock experiments to 850 GPa on Sandia's Z machine

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

    Mattsson, Thomas R.; Root, Seth; Mattsson, Ann E.; Shulenburger, Luke; Magyar, Rudolph J.; Flicker, Dawn G.

    2014-11-11

    We use Sandia's Z machine and magnetically accelerated flyer plates to shock compress liquid krypton to 850 GPa and compare with results from density-functional theory (DFT) based simulations using the AM05 functional. We also employ quantum Monte Carlo calculations to motivate the choice of AM05. We conclude that the DFT results are sensitive to the quality of the pseudopotential in terms of scattering properties at high energy/temperature. A new Kr projector augmented wave potential was constructed with improved scattering properties which resulted in excellent agreement with the experimental results to 850 GPa and temperatures above 10 eV (110 kK). Inmore »conclusion, we present comparisons of our data from the Z experiments and DFT calculations to current equation of state models of krypton to determine the best model for high energy-density applications.« less

  10. Validating density-functional theory simulations at high energy-density conditions with liquid krypton shock experiments to 850 GPa on Sandia's Z machine

    SciTech Connect (OSTI)

    Mattsson, Thomas R.; Root, Seth; Mattsson, Ann E.; Shulenburger, Luke; Magyar, Rudolph J.; Flicker, Dawn G.

    2014-11-11

    We use Sandia's Z machine and magnetically accelerated flyer plates to shock compress liquid krypton to 850 GPa and compare with results from density-functional theory (DFT) based simulations using the AM05 functional. We also employ quantum Monte Carlo calculations to motivate the choice of AM05. We conclude that the DFT results are sensitive to the quality of the pseudopotential in terms of scattering properties at high energy/temperature. A new Kr projector augmented wave potential was constructed with improved scattering properties which resulted in excellent agreement with the experimental results to 850 GPa and temperatures above 10 eV (110 kK). In conclusion, we present comparisons of our data from the Z experiments and DFT calculations to current equation of state models of krypton to determine the best model for high energy-density applications.

  11. Complex-energy approach to sum rules within nuclear density functional theory

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

    Hinohara, Nobuo; Kortelainen, Markus; Nazarewicz, Witold; Olsen, Erik

    2015-04-27

    The linear response of the nucleus to an external field contains unique information about the effective interaction, correlations governing the behavior of the many-body system, 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 nuclear energy density functional (EDF). But the additional information comes at a price: compared to the ground state, computation of excited states is more demanding. To establish anmore »efficient framework to compute energy-weighted 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 finite-amplitude method (FAM) based on the quasiparticle random- phase approximation. 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. As a result, the FAM formulation is especially useful when standard theorems based on commutation relations involving the nuclear Hamiltonian and external field cannot be used.« less

  12. ATLAS: A Real-Space Finite-Difference Implementation of Orbital-Free Density Functional Theory

    E-Print Network [OSTI]

    Wenhui Mi; Xuecheng Shao; Chuanxun Su; Yuanyuan Zhou; Shoutao Zhang; Quan Li; Hui Wang; Lijun Zhang; Maosheng Miao; Yanchao Wang; Yanming Ma

    2015-07-28

    Orbital-free density functional theory (OF-DFT) is a promising method for large-scale quantum mechanics simulation as it provides a good balance of accuracy and computational cost. Its applicability to large-scale simulations has been aided by progress in constructing kinetic energy functionals and local pseudopotentials. However, the widespread adoption of OF-DFT requires further improvement in its efficiency and robustly implemented software. Here we develop a real-space finite-difference method for the numerical solution of OF-DFT in periodic systems. Instead of the traditional self-consistent method, a powerful scheme for energy minimization is introduced to solve the Euler--Lagrange equation. Our approach engages both the real-space finite-difference method and a direct energy-minimization scheme for the OF-DFT calculations. The method is coded into the ATLAS software package and benchmarked using periodic systems of solid Mg, Al, and Al$_{3}$Mg. The test results show that our implementation can achieve high accuracy, efficiency, and numerical stability for large-scale simulations.

  13. ATLAS: A Real-Space Finite-Difference Implementation of Orbital-Free Density Functional Theory

    E-Print Network [OSTI]

    Mi, Wenhui; Sua, Chuanxun; Zhoua, Yuanyuan; Zhanga, Shoutao; Lia, Quan; Wanga, Hui; Zhang, Lijun; Miao, Maosheng; Wanga, Yanchao; Ma, Yanming

    2015-01-01

    Orbital-free density functional theory (OF-DFT) is a promising method for large-scale quantum mechanics simulation as it provides a good balance of accuracy and computational cost. Its applicability to large-scale simulations has been aided by progress in constructing kinetic energy functionals and local pseudopotentials. However, the widespread adoption of OF-DFT requires further improvement in its efficiency and robustly implemented software. Here we develop a real-space finite-difference method for the numerical solution of OF-DFT in periodic systems. Instead of the traditional self-consistent method, a powerful scheme for energy minimization is introduced to solve the Euler--Lagrange equation. Our approach engages both the real-space finite-difference method and a direct energy-minimization scheme for the OF-DFT calculations. The method is coded into the ATLAS software package and benchmarked using periodic systems of solid Mg, Al, and Al$_{3}$Mg. The test results show that our implementation can achieve ...

  14. Building a Universal Nuclear Energy Density Functional (UNEDF): SciDAC-2 Project

    SciTech Connect (OSTI)

    Carlson, Joe; Furnstahl, Dick; Lusk, Rusty; Nazarewicz, Witek; Ng, Esmond; Thompson, Ian; Vary, James

    2012-06-30

    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.

  15. Microscopic description of fission in neutron-rich Radium isotopes with the Gogny energy density functional

    E-Print Network [OSTI]

    Rodriguez-Guzman, R R

    2015-01-01

    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 ...

  16. Interatomic potentials for ionic systems with density functional accuracy based on charge densities obtained by a neural network

    E-Print Network [OSTI]

    Ghasemi, S Alireza; Saha, Santanu; Goedecker, Stefan

    2015-01-01

    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...

  17. Complex-energy approach to sum rules within nuclear density functional theory

    E-Print Network [OSTI]

    Nobuo Hinohara; Markus Kortelainen; Witold Nazarewicz; Erik Olsen

    2015-01-28

    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.

  18. Computing the partition function, ensemble averages, and density of states for lattice spin systems by sampling the mean

    SciTech Connect (OSTI)

    Gillespie, Dirk

    2013-10-01

    An algorithm to approximately calculate the partition function (and subsequently ensemble averages) and density of states of lattice spin systems through non-Monte-Carlo random sampling is developed. This algorithm (called the sampling-the-mean algorithm) can be applied to models where the up or down spins at lattice nodes interact to change the spin states of other lattice nodes, especially non-Ising-like models with long-range interactions such as the biological model considered here. Because it is based on the Central Limit Theorem of probability, the sampling-the-mean algorithm also gives estimates of the error in the partition function, ensemble averages, and density of states. Easily implemented parallelization strategies and error minimizing sampling strategies are discussed. The sampling-the-mean method works especially well for relatively small systems, systems with a density of energy states that contains sharp spikes or oscillations, or systems with little a priori knowledge of the density of states.

  19. The magnetic and electronic structure of vanadyl pyrophosphate from density functional theory

    SciTech Connect (OSTI)

    Cheng, Mu-Jeng; Nielsen, Robert J.; Tahir-Kheli, Jamil; Goddard III, William A.

    2011-01-01

    We have studied the magnetic structure of the high symmetry vanadyl pyrophosphate ((VO)?P?O?, VOPO), focusing on the spin exchange couplings, using density functional theory (B3LYP) with the full three-dimensional periodicity. VOPO involves four distinct spin couplings: two larger couplings exist along the chain direction (a-axis), which we predict to be antiferromagnetic, JOPO = ?156.8 K and JO = ?68.6 K, and two weaker couplings appear along the c (between two layers) and b directions (between two chains in the same layer), which we calculate to be ferromagnetic, Jlayer = 19.2 K and Jchain = 2.8 K. Based on the local density of states and the response of spin couplings to varying the cell parameter a, we found that JOPO originates from a super-exchange interaction through the bridging –O–P–O– unit. In contrast, JO results from a direct overlap of 3dx²?y² orbitals on two vanadium atoms in the same V2O8 motif, making it very sensitive to structural fluctuations. Based on the variations in V–O bond length as a function of strain along a, we found that the V–O bonds of V–(OPO)2–V are covalent and rigid, whereas the bonds of V–(O)2–V are fragile and dative. These distinctions suggest that compression along the a-axis would have a dramatic impact on JO, changing the magnetic structure and spin gap of VOPO. This result also suggests that assuming JO to be a constant over the range of 2–300 K whilst fitting couplings to the experimental magnetic susceptibility is an invalid method. Regarding its role as a catalyst, the bonding pattern suggests that O2 can penetrate beyond the top layers of the VOPO surface, converting multiple V atoms from the +4 to +5 oxidation state, which seems crucial to explain the deep oxidation of n-butane to maleic anhydride.

  20. Functional renormalization group study of Nambu--Jona-Lasinio model at finite temperature and density in external magnetic field

    E-Print Network [OSTI]

    Ken-Ichi Aoki; Hidenari Uoi; Masatoshi Yamada

    2015-07-09

    We study the Nambu--Jona-Lasinio (NJL) model at finite temperature and finite density in an external magnetic field using the Functional Renormalization Group (FRG). The dependence of the position of UltraViolet Fixed Point (UVFP) of the four-fermi coupling constant on temperature, density and external magnetic field is investigated and we obtain the chiral phase structure. The UVFP at low temperature and finite chemical potential oscillates in small external magnetic field, which can be interpreted as the de-Haas--van-Alfen effect. We also find that the external magnetic field moves the chiral phase boundary towards the symmetric side at low temperature and high density region.

  1. Functional renormalization group study of Nambu--Jona-Lasinio model at finite temperature and density in external magnetic field

    E-Print Network [OSTI]

    Aoki, Ken-Ichi; Yamada, Masatoshi

    2015-01-01

    We study the Nambu--Jona-Lasinio (NJL) model at finite temperature and finite density in an external magnetic field using the Functional Renormalization Group (FRG). The dependence of the position of UltraViolet Fixed Point (UVFP) of the four-fermi coupling constant on temperature, density and external magnetic field is investigated and we obtain the chiral phase structure. The UVFP at low temperature and finite chemical potential oscillates in small external magnetic field, which can be interpreted as the de-Haas--van-Alfen effect. We also find that the external magnetic field moves the chiral phase boundary towards the symmetric side at low temperature and high density region.

  2. Real-time linear response for time-dependent density-functional theory Department of Physical Chemistry and the Lise Meitner Minerva-Center for Quantum Chemistry,

    E-Print Network [OSTI]

    Baer, Roi

    Real-time linear response for time-dependent density-functional theory Roi Baer Department a linear-response approach for time-dependent density-functional theories using time-adiabatic functionals describing the evolution is not strictly linear in the wave function representation. Only after going

  3. Combining linear interpolation with extrapolation methods in range-separated ensemble density-functional theory

    E-Print Network [OSTI]

    Senjean, Bruno; Alam, Md Mehboob; Knecht, Stefan; Fromager, Emmanuel

    2015-01-01

    The combination of a recently proposed linear interpolation method (LIM) [Senjean et al., Phys. Rev. A 92, 012518 (2015)], which enables the calculation of weight-independent excitation energies in range-separated ensemble density-functional approximations, with the extrapolation scheme of Savin [J. Chem. Phys. 140, 18A509 (2014)] is presented in this work. It is shown that LIM excitation energies vary quadratically with the inverse of the range-separation parameter mu when the latter is large. As a result, the extrapolation scheme, which is usually applied to long-range interacting energies, can be adapted straightforwardly to LIM. This extrapolated LIM (ELIM) has been tested on a small test set consisting of He, Be, H2 and HeH+. Relatively accurate results have been obtained for the first singlet excitation energies with the typical mu=0.4 value. The improvement of LIM after extrapolation is remarkable, in particular for the doubly-excited 2^1Sigma+g state in the stretched H2 molecule. Three-state ensemble ...

  4. 2007 Time_Dependent Density-Functional Therory (July 15-20, 2007 Colby College, Maine)

    SciTech Connect (OSTI)

    Ullrich Carsten Nancy Ryan Gray

    2008-09-19

    Time-dependent density-functional theory (TDDFT) provides an efficient, elegant, and formally exact way of describing the dynamics of interacting many-body quantum systems, circumventing the need for solving the full time-dependent Schroedinger equation. In the 20 years since it was first rigorously established in 1984, the field of TDDFT has made rapid and significant advances both formally as well as in terms of successful applications in chemistry, physics and materials science. Today, TDDFT has become the method of choice for calculating excitation energies of complex molecules, and is becoming increasingly popular for describing optical and spectroscopic properties of a variety of materials such as bulk solids, clusters and nanostructures. Other growing areas of applications of TDDFT are nonlinear dynamics of strongly excited electronic systems and molecular electronics. The purpose and scope of this Gordon Research Conference is to provide a platform for discussing the current state of the art of the rapidly progressing, highly interdisciplinary field of TDDFT, to identify and debate open questions, and to point out new promising research directions. The conference will bring together experts with a diverse background in chemistry, physics, and materials science.

  5. 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

    2015-08-01

    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

  6. Density functional study of CaN mono and bilayer on Cu(001)

    SciTech Connect (OSTI)

    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)

    2014-01-15

    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.

  7. Trends in Formic Acid Decomposition on Model Transition Metal Surfaces: A Density Functional Theory Study

    SciTech Connect (OSTI)

    Herron, Jeffrey A.; Scaranto, Jessica; Ferrin, Peter A.; Li, Sha; Mavrikakis, Manos

    2014-12-05

    We present a first-principles, self-consistent periodic density functional theory (PW91-GGA) study of formic acid (HCOOH) decomposition on model (111) and (100) facets of eight fcc metals (Au, Ag, Cu, Pt, Pd, Ni, Ir, and Rh) and (0001) facets of four hcp (Co, Os, Ru, and Re) metals. The calculated binding energies of key formic acid decomposition intermediates including formate (HCOO), carboxyl (COOH), carbon monoxide (CO), water (H2O), carbon dioxide (CO2), hydroxyl (OH), carbon (C), oxygen (O), and hydrogen (H; H2) are presented. Using these energetics, we develop thermochemical potential energy diagrams for both the carboxyl-mediated and the formate-mediated dehydrogenation mechanisms on each surface. We evaluate the relative stability of COOH, HCOO, and other isomeric intermediates (i.e., CO + OH, CO2 + H, CO + O + H) on these surfaces. These results provide insights into formic acid decomposition selectivity (dehydrogenation versus dehydration), and in conjunction with calculated vibrational frequency modes, the results can assist with the experimental search for the elusive carboxyl (COOH) surface intermediate. Results are compared against experimental reports in the literature.

  8. Density functional theory calculations of stability and diffusion mechanisms of impurity atoms in Ge crystals

    SciTech Connect (OSTI)

    Maeta, Takahiro; Sueoka, Koji

    2014-08-21

    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.

  9. Comparative Density Functional Study of Methanol Decomposition on Cu4 and Co4 Clusters

    SciTech Connect (OSTI)

    Mehmood, Faisal; Greeley, Jeffrey P.; Zapol, Peter; Curtiss, Larry A.

    2010-11-18

    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.

  10. 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

    2015-01-01

    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

  11. The role of presumed probability density function in the simulation of non premixed turbulent combustion

    E-Print Network [OSTI]

    Coclite, Alessandro; De Palma, Pietro; Cutrone, Luigi

    2013-01-01

    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...

  12. Uranium (VI)Bis(imido) chalcogenate complexes:synthesis and density functional theory analysis

    SciTech Connect (OSTI)

    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

    2009-01-01

    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.

  13. Singlet and triplet excitons and charge polarons in cycloparaphenylenes. A density functional theory study

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

    Liu, Jin; Adamska, Lyudmyla; Doorn, Stephen K.; Tretiak, Sergei

    2015-05-14

    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

  14. Introducing constricted variational density functional theory in its relaxed self-consistent formulation (RSCF-CV-DFT) as an alternative to adiabatic time dependent density functional theory for studies of charge transfer transitions

    SciTech Connect (OSTI)

    Krykunov, Mykhaylo; Seth, Mike; Ziegler, Tom

    2014-05-14

    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.

  15. Density functional theory investigation of 3d, 4d, and 5d 13-atom metal clusters

    SciTech Connect (OSTI)

    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)

    2010-04-15

    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.

  16. arXiv:1203.6284v1[nucl-th]28Mar2012 Isovector part of nuclear energy density functional

    E-Print Network [OSTI]

    Weise, Wolfram

    arXiv:1203.6284v1[nucl-th]28Mar2012 Isovector part of nuclear energy density functional from chiral The nuclear energy density functional approach is the many-body method of choice in order to calculate the contributions to the energy are written in terms of density-matrices convoluted with the finite

  17. Accurate description of torsion potentials in conjugated polymers using density functionals with reduced self-interaction error

    SciTech Connect (OSTI)

    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)

    2014-02-07

    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.

  18. van der Waals density functionals built upon the electron-gas tradition: Facing the challenge of competing interactions

    SciTech Connect (OSTI)

    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)

    2014-05-14

    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.

  19. van der Waals density functionals built upon the electron-gas tradition: Facing the challenge of competing interactions

    SciTech Connect (OSTI)

    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

    2014-01-01

    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.

  20. Higher-order adaptive finite-element methods for Kohn–Sham density functional theory

    SciTech Connect (OSTI)

    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)

    2013-11-15

    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.

  1. Magnetism in undoped ZnS studied from density functional theory

    SciTech Connect (OSTI)

    Xiao, Wen-Zhi E-mail: llwang@hun.edu.cn; Rong, Qing-Yan; Xiao, Gang; Wang, Ling-ling E-mail: llwang@hun.edu.cn; Meng, Bo

    2014-06-07

    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.

  2. Calculation of semiconductor band gaps with the M06-L density functional Yan Zhao and Donald G. Truhlara

    E-Print Network [OSTI]

    Truhlar, Donald G

    .3,6,7 However, the computational cost for HF exchange in solid-state physics calculations is very indirect.24 In this paper we calculate the lowest excitation energy whether direct or in- direct by Eq. 1Calculation of semiconductor band gaps with the M06-L density functional Yan Zhao and Donald G

  3. Catalytic Role of Gold in Gold-Based Catalysts: A Density Functional Theory Study on the CO Oxidation on Gold

    E-Print Network [OSTI]

    Alavi, Ali

    Catalytic Role of Gold in Gold-Based Catalysts: A Density Functional Theory Study on the CO Oxidation on Gold Zhi-Pan Liu and P. Hu* Contribution from the School of Chemistry, The Queen's Uni years, being regarded as a new generation of catalysts due to their unusually high catalytic performance

  4. How Does Ammonium Interact with Aromatic Groups? A Density Functional Theory (DFT/B3LYP) Investigation

    E-Print Network [OSTI]

    Sussman, Joel L.

    %) of the total binding energy, while the NH4 + -aromatic hydrogen bond interaction has the largest electrostaticHow Does Ammonium Interact with Aromatic Groups? A Density Functional Theory (DFT/B3LYP heterocyclic-NH3 hydrogen bond complexes, and heterocyclic-NH4 + hydrogen bond complexes. For NH4 + - complexes

  5. The density matrix functional approach to electron correlation: Dynamic and nondynamic correlation along the full dissociation coordinate

    SciTech Connect (OSTI)

    Mentel, ?. M.; Meer, R. van; Gritsenko, O. V.; Baerends, E. J.

    2014-06-07

    For chemistry an accurate description of bond weakening and breaking is vital. The great advantage of density matrix functionals, as opposed to density functionals, is their ability to describe such processes since they naturally cover both nondynamical and dynamical correlation. This is obvious in the Löwdin-Shull functional, the exact natural orbital functional for two-electron systems. We present in this paper extensions of this functional for the breaking of a single electron pair bond in N-electron molecules, using LiH, BeH{sup +}, and Li{sub 2} molecules as prototypes. Attention is given to the proper formulation of the functional in terms of not just J and K integrals but also the two-electron L integrals (K integrals with a different distribution of the complex conjugation of the orbitals), which is crucial for the calculation of response functions. Accurate energy curves are obtained with extended Löwdin-Shull functionals along the complete dissociation coordinate using full CI calculations as benchmark.

  6. Exploring the limit of accuracy for density functionals based on the generalized gradient approximation: Local, global hybrid, and range-separated hybrid functionals with and without dispersion corrections

    SciTech Connect (OSTI)

    Mardirossian, Narbe; Head-Gordon, Martin

    2014-05-14

    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.

  7. Error Estimation and Parameter Dependence of the Calculation of the Fast Ion Distribution Function, Temperature and Density using Data from the KF1 High Energy NPA on JET

    E-Print Network [OSTI]

    Error Estimation and Parameter Dependence of the Calculation of the Fast Ion Distribution Function, Temperature and Density using Data from the KF1 High Energy NPA on JET

  8. The scaling functions of the free energy density and its derivatives for the 3d O(4) model

    E-Print Network [OSTI]

    Engels, Juergen

    2011-01-01

    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.

  9. Structure of cylindrical electric double layers: Comparison of density functional and modified Poisson-Boltzmann theories with Monte Carlo simulations

    E-Print Network [OSTI]

    V. Dorvilien; C. N. Patra; L. B. Bhuiyan; C. W. Outhwaite

    2013-12-17

    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.

  10. Searching for 4$?$ linear-chain structure in excited states of $^{16}$O with a covariant density functional theory

    E-Print Network [OSTI]

    J. M. Yao; N. Itagaki; J. Meng

    2014-09-19

    A study of 4$\\alpha$ linear-chain structure in high-lying collective excitation states of $^{16}$O with a covariant density functional theory is presented. The low-spin states are obtained by configuration mixing of particle-number and angular-momentum projected quadrupole deformed mean-field states with generator coordinate method. The high-spin states are determined by cranking calculations. These two calculations are based on the same energy density functional PC-PK1. We have found a rotational band at low-spin with the dominated intrinsic configuration considered to be the one that 4$\\alpha$ clusters stay along a common axis. The strongly deformed rod shape also appears in the high-spin region with the angular momentum $13-18\\hbar$; however whether the state is pure $4\\alpha$ linear chain or not is less obvious than that in the low-spin states.

  11. Potential energy surfaces of actinide and transfermium nuclei from multi-dimensional constraint covariant density functional theories

    E-Print Network [OSTI]

    Bing-Nan Lu; Jie Zhao; En-Guang Zhao; Shan-Gui Zhou

    2013-03-04

    Multi-dimensional constrained covariant density functional theories were developed recently. In these theories, all shape degrees of freedom \\beta_{\\lambda\\mu} deformations with even \\mu are allowed, e.g., \\beta_{20}, \\beta_{22}, \\beta_{30}, \\beta_{32}, \\beta_{40}, \\beta_{42}, \\beta_{44}, and so on and the CDFT functional can be one of the following four forms: the meson exchange or point-coupling nucleon interactions combined with the non-linear or density-dependent couplings. In this contribution, some applications of these theories are presented. The potential energy surfaces of actinide nuclei in the (\\beta_{20}, \\beta_{22}, \\beta_{30}) deformation space are investigated. It is found that besides the octupole deformation, the triaxiality also plays an important role upon the second fission barriers. The non-axial reflection-asymmetric \\beta_{32} shape in some transfermium nuclei with N = 150, namely 246Cm, 248Cf, 250Fm, and 252No are studied.

  12. Ab initio molecular dynamics with nuclear quantum effects at classical cost: ring polymer contraction for density functional theory

    E-Print Network [OSTI]

    Marsalek, Ondrej

    2015-01-01

    Path integral molecular dynamics simulations, combined with an ab initio evaluation of interactions using electronic structure theory, incorporate the quantum mechanical nature of both the electrons and nuclei, which are essential to accurately describe systems containing light nuclei. However, path integral simulations have traditionally required a computational cost around two orders of magnitude greater than treating the nuclei classically, making them prohibitively costly for most applications. Here we show that the cost of path integral simulations can be dramatically reduced by extending our ring polymer contraction approach to ab initio molecular dynamics simulations. By using density functional tight binding as a reference system, we show that our ab initio ring polymer contraction (AI-RPC) scheme gives rapid and systematic convergence to the full path integral density functional theory result. We demonstrate the efficiency of this approach in ab initio simulations of liquid water and the reactive pro...

  13. Relativistic energy density functionals: Low-energy collective states of {sup 240}Pu and {sup 166}Er

    SciTech Connect (OSTI)

    Li, Z. P.; Niksic, T.; Vretenar, D.; Ring, P.; Meng, J.

    2010-06-15

    The empirical relativistic density-dependent, point-coupling energy density functional, adjusted exclusively to experimental binding energies of a large set of deformed nuclei with Aapprox =150-180 and Aapprox =230-250, is tested with spectroscopic data for {sup 166}Er and {sup 240}Pu. Starting from constrained self-consistent triaxial relativistic Hartree-Bogoliubov calculations of binding energy maps as functions of the quadrupole deformation in the beta-gamma plane, excitation spectra and E2 transition probabilities are calculated as solutions of the corresponding microscopic collective Hamiltonian in five dimensions for quadrupole vibrational and rotational degrees of freedom and compared with available data on low-energy collective states.

  14. The structure of mixed {sup 3}He-{sup 4}He droplets doped with OCS: A density functional approach

    SciTech Connect (OSTI)

    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)

    2013-11-07

    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.

  15. Properties of nuclei in the nobelium region studied within the covariant, Skyrme, and Gogny energy density functionals

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

    Dobaczewski, J.; Afanasjev, A. V.; Bender, M.; Robledo, L. M.; Shi, Yue

    2015-07-29

    In this study, we calculate properties of the ground and excited states of nuclei in the nobelium region for proton and neutron numbers of 92 ? Z ? 104 and 144 ? N ? 156, respectively. We use three different energy-density-functional (EDF) approaches, based on covariant, Skyrme, and Gogny functionals, each with two different parameter sets. A comparative analysis of the results obtained for quasiparticle spectra, odd–even and two-particle mass staggering, and moments of inertia allows us to identify single-particle and shell effects that are characteristic to these different models and to illustrate possible systematic uncertainties related to using themore »EDF modelling.« less

  16. Coherent control and time-dependent density functional theory: Towards creation of wave packets by ultrashort laser pulses

    SciTech Connect (OSTI)

    Raghunathan, Shampa; Nest, Mathias [Theoretische Chemie, TU Muenchen, Lichtenbergstr. 4, 85747 Garching (Germany)

    2012-02-14

    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.

  17. Testing Skyrme energy-density functionals with the QRPA in low-lying vibrational states of rare-earth nuclei

    E-Print Network [OSTI]

    J. Terasaki; J. Engel

    2011-05-19

    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.

  18. Potassium permeation through the KcsA channel: a density functional study

    E-Print Network [OSTI]

    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

  19. Analysis of Multiple Scalar Large-Eddy Simulation/Probability Density Function Formulation

    E-Print Network [OSTI]

    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

  20. A Combined Density Functional and Monte Carlo Study of Polycarbonate R. O. Jones and P. Ballone[*

    E-Print Network [OSTI]

    [*] Institut f¨ur Festk¨orperforschung, Forschungszentrum J¨ulich, D-52425 J¨ulich, Germany ABSTRACT Density range of applications. Although production and processing of polycar- bonates have been carried out with pre- dictive capability for calculating total energies, ground state structures and low energy

  1. Energy density functionals from the strong-coupling limit applied to the anions of the He isoelectronic series

    SciTech Connect (OSTI)

    Mirtschink, André; Gori-Giorgi, Paola; Umrigar, C. J.; Morgan, John D.

    2014-05-14

    Anions and radicals are important for many applications including environmental chemistry, semiconductors, and charge transfer, but are poorly described by the available approximate energy density functionals. Here we test an approximate exchange-correlation functional based on the exact strong-coupling limit of the Hohenberg-Kohn functional on the prototypical case of the He isoelectronic series with varying nuclear charge Z < 2, which includes weakly bound negative ions and a quantum phase transition at a critical value of Z, representing a big challenge for density functional theory. We use accurate wavefunction calculations to validate our results, comparing energies and Kohn-Sham potentials, thus also providing useful reference data close to and at the quantum phase transition. We show that our functional is able to bind H{sup ?} and to capture in general the physics of loosely bound anions, with a tendency to strongly overbind that can be proven mathematically. We also include corrections based on the uniform electron gas which improve the results.

  2. Density Functional Theory for Protein Transfer Free Energy Eric A. Mills and Steven S. Plotkin*

    E-Print Network [OSTI]

    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

  3. Functional convergence and optimality of plug-in estimators for stationary densities of moving average processes

    E-Print Network [OSTI]

    Wefelmeyer, Wolfgang

    average processes By Anton Schick1 and Wolfgang Wefelmeyer Binghamton University and University of CologneSupported in part by NSF Grant DMS 0072174 1 #12;2 ANTON SCHICK AND WOLFGANG WEFELMEYER first-order moving of functions ui(X1) + · · · + um(Xm) at a point. Schick and Wefelmeyer (2004b) obtain functional central limit

  4. Time-dependent density-functional theory for strong-field multiphoton processes: Application to the study of the role of dynamical electron correlation

    E-Print Network [OSTI]

    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

  5. Spin-dependent localized Hartree-Fock density-functional calculation of singly, doubly, and triply excited and Rydberg states of He- and Li-like ions

    E-Print Network [OSTI]

    Chu, Shih-I; Zhou, Zhongyuan

    2005-02-28

    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...

  6. Applicability of Density Functional Theory in Reproducing Accurate Vibrational Spectra of Surface Bound Species

    SciTech Connect (OSTI)

    Matanovic, Ivana; Atanassov, Plamen; Kiefer, Boris; Garzon, Fernando; Henson, Neil J.

    2014-10-05

    The structural equilibrium parameters, the adsorption energies, and the vibrational frequencies of the nitrogen molecule and the hydrogen atom adsorbed on the (111) surface of rhodium have been investigated using different generalized-gradient approximation (GGA), nonlocal correlation, meta-GGA, and hybrid functionals, namely, Perdew, Burke, and Ernzerhof (PBE), Revised-RPBE, vdW-DF, Tao, Perdew, Staroverov, and Scuseria functional (TPSS), and Heyd, Scuseria, and Ernzerhof (HSE06) functional in the plane wave formalism. Among the five tested functionals, nonlocal vdW-DF and meta-GGA TPSS functionals are most successful in describing energetics of dinitrogen physisorption to the Rh(111) surface, while the PBE functional provides the correct chemisorption energy for the hydrogen atom. It was also found that TPSS functional produces the best vibrational spectra of the nitrogen molecule and the hydrogen atom on rhodium within the harmonic formalism with the error of 22.62 and 21.1% for the NAN stretching and RhAH stretching frequency. Thus, TPSS functional was proposed as a method of choice for obtaining vibrational spectra of low weight adsorbates on metallic surfaces within the harmonic approximation. At the anharmonic level, by decoupling the RhAH and NAN stretching modes from the bulk phonons and by solving one- and two-dimensional Schr€odinger equation associated with the RhAH, RhAN, and NAN potential energy we calculated the anharmonic correction for NAN and RhAH stretching modes as 231 cm21 and 277 cm21 at PBE level. Anharmonic vibrational frequencies calculated with the use of the hybrid HSE06 function are in best agreement with available experiments.

  7. The effects of gaps between bridge foils and PETN as a function of PETN density and specific surface area

    SciTech Connect (OSTI)

    Phillips, D; Roeske, F; Burnham, A

    2007-06-26

    X-ray computer tomography scans of artificially aged PETN seem to indicate shrinkage of material and, by extension, an increased high explosive density, resulting in potential separation of the HE from the header/bridge foil. We have investigated these phenomena by mimicking this shrinkage of material (load density). Thus, we have evaluated various induced gaps between the exploding bridge foil and the PETN in our custom detonators by changing both specific surface area - recognizing crystal morphology changes - and load density. Analyses for these data include absolute function time relative to bridge burst and careful evaluation of the detonation wave breakout curvature, using an electronic streak camera for wave capture, in cases where the bridge foil (exploding bridge wire - EBW style) initiation successfully traverses the gap (a 'go' condition). In addition, a fireset with subnanosecond trigger jitter was used for these tests allowing easy comparison of relative 'go' function times. Using the same test matrix and fine-tuning the induced gap, a second, smaller subset of these experiments were performed to provide additional insight as to what conditions we might expect detonator anomalies/failure.

  8. Lipkin translational-symmetry restoration in the mean-field and energy-density-functional methods

    E-Print Network [OSTI]

    Jacek Dobaczewski

    2009-06-25

    Based on the 1960 idea of Lipkin, the minimization of energy of a symmetry-restored mean-field state is equivalent to the minimization of a corrected energy of a symmetry-broken state with the Peierls-Yoccoz mass. It is interesting to note that the "unphysical" Peierls-Yoccoz mass, and not the true mass, appears in the Lipkin projected energy. The Peierls-Yoccoz mass can be easily calculated from the energy and overlap kernels, which allows for a systematic, albeit approximate, restoration of translational symmetry within the energy-density formalism. Analogous methods can also be implemented for all other broken symmetries.

  9. Freezing of a two dimensional fluid in to a crystalline phase : Density functional approach

    E-Print Network [OSTI]

    Anubha Jaiswal; Swarn L. Singh; Yashwant Singh

    2012-10-02

    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.

  10. Van der Waals density functional study of the structural and electronic properties of La-doped phenanthrene

    SciTech Connect (OSTI)

    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)

    2013-11-28

    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.

  11. Electrons as probes of dynamics in molecules and clusters : a contribution from Time Dependent Density Functional Theory

    E-Print Network [OSTI]

    Wopperer, P; Reinhard, P -G; Suraud, E

    2014-01-01

    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...

  12. Generalized coherent-state derivation of time-dependent density-functional theory equations for superconductors

    E-Print Network [OSTI]

    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

  13. Charged-Particle Thermonuclear Reaction Rates: II. Tables and Graphs of Reaction Rates and Probability Density Functions

    E-Print Network [OSTI]

    Christian Iliadis; Richard Longland; Art Champagne; Alain Coc; Ryan Fitzgerald

    2010-04-23

    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.

  14. Nonlinear electronic excitations in crystalline solids using meta-generalized gradient approximation and hybrid functional in time-dependent density functional theory

    E-Print Network [OSTI]

    Sato, Shunsuke A; Shinohara, Yasushi; Yabana, Kazuhiro

    2015-01-01

    We develop numerical methods to calculate electron dynamics in crystalline solids in real-time time-dependent density functional theory employing exchange-correlation potentials which reproduce band gap energies of dielectrics; a meta generalized gradient approximation (meta-GGA) proposed by Tran and Blaha [Phys. Rev. Lett. 102, 226401 (2009)] (TBm-BJ) and a hybrid functional proposed by Heyd, Scuseria, and Ernzerhof [J. Chem. Phys. 118, 8207 (2003)] (HSE). In time evolution calculations employing the TB-mBJ potential, we have found it necessary to adopt a predictor-corrector step for stable time-evolution. Since energy functional is not known for the TB-mBJ potential, we propose a method to evaluate electronic excitation energy without referring to the energy functional. Calculations using the HSE hybrid functional is computationally expensive due to the nonlocal Fock-like term. We develop a computational method for the operation of the Fock-like term in Fourier space, for which we employ massively parallel ...

  15. Probability density functions for the variable solar wind near the solar cycle minimum

    E-Print Network [OSTI]

    Vörös,; Leitner, M; Narita, Y; Consolini, G; Kovács, P; Tóth, A; Lichtenberger, J

    2015-01-01

    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...

  16. Redox Potentials and Acidity Constants from Density Functional Theory Based Molecular Dynamics

    E-Print Network [OSTI]

    Cheng, Jun; Liu, Xiandong; VandeVondele, Joost; Sulpizi, Marialore; Sprik, Michiel

    2014-11-03

    . Critical error anal- ysis will be carried out to demonstrate how the delocalization error in GGAs affects redox potentials. The improvement by hybrid functionals reinforces this claim. We will end this Account with some conclusions and an outlook. Method... and theoretical (photo-)electrochemistry and catalysis. Xiandong Liu is an associate professor at Nanjing University. He joined the Sprik group at Cambridge in 2012 to work on computational geochemistry of mineral interfaces and transition metal complexes. Joost...

  17. QCD at nonzero density and canonical partition functions with Wilson fermions

    SciTech Connect (OSTI)

    Alexandru, Andrei; Wenger, Urs

    2011-02-01

    We present a reduction method for Wilson-Dirac fermions with nonzero chemical potential which generates a dimensionally reduced fermion matrix. The size of the reduced fermion matrix is independent of the temporal lattice extent and the dependence on the chemical potential is factored out. As a consequence the reduced matrix allows a simple evaluation of the Wilson fermion determinant for any value of the chemical potential and hence the exact projection to the canonical partition functions.

  18. Solution of self-consistent equations for the N3LO nuclear energy density functional in spherical symmetry. The program HOSPHE (v1.00)

    E-Print Network [OSTI]

    B. G. Carlsson; J. Dobaczewski; J. Toivanen; P. Vesely

    2009-12-16

    We present solution of self-consistent equations for the N3LO nuclear energy density functional. We derive general expressions for the mean fields expressed as differential operators depending on densities and for the densities expressed in terms of derivatives of wave functions. These expressions are then specified to the case of spherical symmetry. We also present the computer program HOSPHE (v1.00), which solves the self-consistent equations by using the expansion of single-particle wave functions on the spherical harmonic oscillator basis.

  19. Time-dependent localized Hartree-Fock density-functional linear response approach for photoionization of atomic excited states

    E-Print Network [OSTI]

    Zhongyuan Zhou; Shih-I Chu

    2009-02-09

    We present a time-dependent localized Hartree-Fock density-functional linear response approach for the treatment of photoionization of atomic systems. This approach employs a spin-dependent localized Hartree-Fock (SLHF) exchange potential to calculate electron orbitals and kernel functions, and thus can be used to study the photoionization from atomic excited states. We have applied the approach to the calculation of photoionization cross sections of Ne ground state. The results are in agreement with available experimental data and have comparable accuracies with other ab initio theoretical results. We have also extended the approach to explore the photoionization from Ne excited states and obtained some new results for the photoionization from outer-shell and inner-shell excited states.

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

    E-Print Network [OSTI]

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

    2014-06-11

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

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

    E-Print Network [OSTI]

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

    2015-01-01

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

  2. Towards time-dependent current-density-functional theory in the non-linear regime

    E-Print Network [OSTI]

    Escartín, J. M.; Vincendon, M.; Romaniello, P.; Dinh, P. M.; Reinhard, P.-G.; Suraud, E.

    2015-02-27

    ? ? 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...

  3. Microscopic description of fission in neutron-rich plutonium isotopes with the Gogny-D1M energy density functional

    E-Print Network [OSTI]

    Rodriguez-Guzman, R

    2014-01-01

    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...

  4. Microscopic description of fission in neutron-rich plutonium isotopes with the Gogny-D1M energy density functional

    E-Print Network [OSTI]

    R. Rodriguez-Guzman; L. M. Robledo

    2014-05-27

    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.

  5. On the Accuracy of van der Waals Inclusive Density-Functional Theory Exchange-Correlation Functionals for Ice at Ambient and High Pressures

    E-Print Network [OSTI]

    Biswajit Santra; Ji?í Klimeš; Alexandre Tkatchenko; Dario Alfè; Ben Slater; Angelos Michaelides; Roberto Car; Matthias Scheffler

    2014-08-14

    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.

  6. On the Accuracy of van der Waals Inclusive Density-Functional Theory Exchange-Correlation Functionals for Ice at Ambient and High Pressures

    E-Print Network [OSTI]

    Santra, Biswajit; Tkatchenko, Alexandre; Alfè, Dario; Slater, Ben; Michaelides, Angelos; Car, Roberto; Scheffler, Matthias

    2013-01-01

    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...

  7. Birgit Arb, MD Cape Fear Cancer

    E-Print Network [OSTI]

    Olszewski Jr., Edward A.

    Birgit Arb, MD Cape Fear Cancer Specialists Women of Hope is a charitable organization dedicated to enhancing the quality of life for the female cancer patient, their families, and friends. They provide through any type of cancer from diagnosis through survivorship. Women of Hope 1642 South 41st Street

  8. Strategic Plan Update Lydia Pleotis Howell MD

    E-Print Network [OSTI]

    Leistikow, Bruce N.

    and Laboratory Medicine #12;Present Findings from: Planning Interviews Stakeholder Survey Environmental diagnostic testing that is tailored to the prevention and management of disease. 4. Develop a culture organization Howell, CAOs #12;Increase our diversity efforts Recommendations from David Acosta MD, UCDHS' new

  9. Generator coordinate method for hypernuclear spectroscopy with a covariant density functional

    E-Print Network [OSTI]

    H. Mei; K. Hagino; J. M. Yao

    2015-11-10

    We apply the generator coordinate method (GCM) to single-$\\Lambda$ hypernuclei in order to discuss the spectra of hypernuclear low-lying states. To this end, we use the same relativistic point-coupling energy functional both for the mean-field and the beyond-mean-field calculations. This relativistic GCM approach provides a unified description of low-lying states in ordinary nuclei and in hypernuclei, and is thus suitable for studying the $\\Lambda$ impurity effect. We carry out an illustrative calculation for the low-lying spectrum of $^{21}_\\Lambda$Ne, in which the interplay between the hypernuclear collective excitations and the single-particle excitations of the unpaired $\\Lambda$ hyperon is taken into account in a full microscopic manner.

  10. Generator coordinate method for hypernuclear spectroscopy with a covariant density functional

    E-Print Network [OSTI]

    Mei, H; Yao, J M

    2015-01-01

    We apply the generator coordinate method (GCM) to single-$\\Lambda$ hypernuclei in order to discuss the spectra of hypernuclear low-lying states. To this end, we use the same relativistic point-coupling energy functional both for the mean-field and the beyond-mean-field calculations. This relativistic GCM approach provides a unified description of low-lying states in ordinary nuclei and in hypernuclei, and is thus suitable for studying the $\\Lambda$ impurity effect. We carry out an illustrative calculation for the low-lying spectrum of $^{21}_\\Lambda$Ne, in which the interplay between the hypernuclear collective excitations and the single-particle excitations of the unpaired $\\Lambda$ hyperon is taken into account in a full microscopic manner.

  11. Towards a specific reaction parameter density functional for reactive scattering of H{sub 2} from Pd(111)

    SciTech Connect (OSTI)

    Boereboom, J. M.; Wijzenbroek, M.; Somers, M. F.; Kroes, G. J.

    2013-12-28

    Recently, an implementation of the specific reaction parameter (SRP) approach to density functional theory (DFT) was used to study several reactive scattering experiments of H{sub 2} on Cu(111). It was possible to obtain chemical accuracy (1 kcal/mol ? 4.2 kJ/mol), and therefore, accurately model this paradigmatic example of activated H{sub 2} dissociation on a metal surface. In this work, the SRP-DFT methodology is applied to the dissociation of hydrogen on a Pd(111) surface, in order to test whether the SRP-DFT approach is also applicable to non-activated H{sub 2}-metal systems. In the calculations, the Born–Oppenheimer static surface approximations are used. A comparison to molecular beam sticking experiments, performed at incidence energies ?125 meV, on H{sub 2} + Pd(111) suggested the PBE-vdW [where the Perdew, Burke, and Ernzerhof (PBE) correlation is replaced by van der Waals correlation] functional as a candidate SRP density functional describing the reactive scattering of H{sub 2} on Pd(111). Unfortunately, quantum dynamics calculations are not able to reproduce the molecular beam sticking results for incidence energies <125 meV. From a comparison to initial state-resolved (degeneracy averaged) sticking probabilities it seems clear that for H{sub 2} + Pd(111) dynamic trapping and steering effects are important, and that these effects are not yet well modeled with the potential energy surfaces considered here. Applying the SRP-DFT method to systems where H{sub 2} dissociation is non-activated remains difficult. It is suggested that a density functional that yields a broader barrier distribution and has more non-activated pathways than PBE-vdW (i.e., non-activated dissociation at some sites but similarly high barriers at the high energy end of the spectrum) should allow a more accurate description of the available experiments. Finally, it is suggested that new and better characterized molecular beam sticking experiments be done on H{sub 2} + Pd(111), to facilitate the development of a more accurate theoretical description of this system.

  12. Testing time-dependent density functional theory with depopulated molecular orbitals for predicting electronic excitation energies of valence, Rydberg, and charge-transfer

    E-Print Network [OSTI]

    Truhlar, Donald G

    transition energies J. Chem. Phys. 137, 244104 (2012); 10.1063/1.4769078 A long-range-corrected densityTesting time-dependent density functional theory with depopulated molecular orbitals for predicting electronic excitation energies of valence, Rydberg, and charge-transfer states and potential energies near

  13. Theoretical study of the ammonia nitridation rate on an Fe (100) surface: A combined density functional theory and kinetic Monte Carlo study

    E-Print Network [OSTI]

    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 ...

  14. Accuracy of density functional theory in predicting formation energies of ternary oxides from binary oxides and its implication on phase stability

    E-Print Network [OSTI]

    Hautier, Geoffroy

    The evaluation of reaction energies between solids using density functional theory (DFT) is of practical importance in many technological fields and paramount in the study of the phase stability of known and predicted ...

  15. Intrinsic point-defect equilibria in tetragonal ZrO[subscript 2]: Density functional theory analysis with finite-temperature effects

    E-Print Network [OSTI]

    Youssef, Mostafa Youssef Mahm

    We present a density functional theory (DFT) framework taking into account the finite temperature effects to quantitatively understand and predict charged defect equilibria in a metal oxide. Demonstration of this approach ...

  16. Integrating Experiment and Theory in Electrochemical Surface Science: Studies on the Molecular Adsorption on Noble-Metal Electrode Surfaces by Density Functional Theory, Electron Spectroscopy, and Electrochemistry 

    E-Print Network [OSTI]

    Javier, Alnald Caintic

    2013-08-05

    Computational techniques based on density functional theory (DFT) and experimental methods based on electrochemistry (EC), electrochemical scanning tunneling microscopy (EC-STM), and high-resolution electron energy loss spectroscopy (HREELS) were...

  17. Complex-energy approach to sum rules within nuclear density functional theory

    E-Print Network [OSTI]

    Hinohara, Nobuo; Nazarewicz, Witold; Olsen, Erik

    2015-01-01

    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...

  18. An extended SMLD approach for presumed probability density function in flamelet combustion model

    E-Print Network [OSTI]

    Coclite, Alessandro; De Palma, Pietro; Cutrone, Luigi

    2013-01-01

    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 ...

  19. FINAL PROJECT REPORT DOE Early Career Principal Investigator Program Project Title: Developing New Mathematical Models for Multiphase Flows Based on a Fundamental Probability Density Function Approach

    SciTech Connect (OSTI)

    Shankar Subramaniam

    2009-04-01

    This final project report summarizes progress made towards the objectives described in the proposal entitled “Developing New Mathematical Models for Multiphase Flows Based on a Fundamental Probability Density Function Approach”. Substantial progress has been made in theory, modeling and numerical simulation of turbulent multiphase flows. The consistent mathematical framework based on probability density functions is described. New models are proposed for turbulent particle-laden flows and sprays.

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

    E-Print Network [OSTI]

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

    2015-03-25

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

  1. Poster Presentations Marcella Alsan, MD, MPH, PhD

    E-Print Network [OSTI]

    Kay, Mark A.

    15 Poster Presentations Marcella Alsan, MD, MPH, PhD The direct and indirect effects of mass vaccination: Evidence from the 1985 Turkish campaign Michele Barry, MD; Stephen Luby, MD; Nancy Federspiel, PhD Global Health Fellows and Scholars Consortium Cynthia M. Castro, PhD; Abby C. King, PhD; Marcia Stefanick

  2. Quantifying the importance of orbital over spin correlations in delta-Pu within density-functional theory

    SciTech Connect (OSTI)

    Soderlind, P; Wolfer, W

    2007-07-27

    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.

  3. Dynamics of observables and exactly solvable quantum problems: Using time-dependent density functional theory to control quantum systems

    E-Print Network [OSTI]

    Mehdi Farzanehpour; I. V. Tokatly

    2015-06-29

    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.

  4. Density Functional Theory Calculations and Analysis of Reaction Pathways for Reduction of Nitric Oxide by Hydrogen on Pt(111)

    SciTech Connect (OSTI)

    Farberow, Carrie A.; Dumesic, James A.; Mavrikakis, Manos

    2014-10-03

    Reaction pathways are explored for low temperature (e.g., 400 K) reduction of nitric oxide by hydrogen on Pt(111). First-principles electronic structure calculations based on periodic, self-consistent density functional theory(DFT-GGA, PW91) are employed to obtain thermodynamic and kinetic parameters for proposed reaction schemes on Pt(111). The surface of Pt(111) during NO reduction by H? at low temperatures is predicted to operate at a high NO coverage, and this environment is explicitly taken into account in the DFT calculations. Maximum rate analyses are performed to assess the most likely reaction mechanisms leading to formation of N?O, the major product observed experimentally at low temperatures. The results of these analyses suggest that the reaction most likely proceeds via the addition of at least two H atoms to adsorbed NO, followed by cleavage of the N-O bond.

  5. Semi-microscopic modeling of heavy-ion fusion reactions with multi-reference covariant density functional theory

    E-Print Network [OSTI]

    K. Hagino; J. M. Yao

    2015-04-15

    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.

  6. Simulation of Charged Systems in Heterogeneous Dielectric Media via a True Energy Functional

    E-Print Network [OSTI]

    Vikram Jadhao; Francisco J. Solis; Monica Olvera de la Cruz

    2013-09-26

    For charged systems in heterogeneous dielectric media, a key obstacle for molecular dynamics (MD) simulations is the need to solve the Poisson equation in the media. This obstacle can be bypassed using MD methods that treat the local polarization charge density as a dynamic variable, but such approaches require access to a true free energy functional; one that evaluates to the equilibrium electrostatic energy at its minimum. In this letter, we derive the needed functional. As an application, we develop a Car-Parrinello MD method for the simulation of free charges present near a spherical emulsion droplet separating two immiscible liquids with different dielectric constants. Our results show the presence of non-monotonic ionic profiles in the dielectric with lower dielectric constant.

  7. Electron dynamics in complex environments with real-time time dependent density functional theory in a QM-MM framework

    SciTech Connect (OSTI)

    Morzan, Uriel N.; Ramírez, Francisco F.; Scherlis, Damián A. E-mail: mcgl@qb.ffyb.uba.ar; Lebrero, Mariano C. González E-mail: mcgl@qb.ffyb.uba.ar

    2014-04-28

    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.

  8. Noise and Signal for Spectra of Intermittent Noiselike Emission C. R. Gwinn, M.D. Johnson

    E-Print Network [OSTI]

    Gwinn, Carl

    Noise and Signal for Spectra of Intermittent Noiselike Emission C. R. Gwinn, M.D. Johnson, affects the distribution of noise in the observed correlation function. Intermittency also affects correlation of noise among channels of the spectrum, but leaves the average spectrum, average correlation

  9. Limbic System Page 1 of 10 Srdjan D. Antic, M.D. Limbic system Emotional Experience

    E-Print Network [OSTI]

    Oliver, Douglas L.

    function. NMDA-dependent long-term potentiation is a cellular mechanism responsible for fear conditioning.M. is the most studied patient with Urbach-Wiethe disease. After a battery of tests, which included spiders Srdjan D. Antic, M.D. 3 as well as an appetitive (positive) conditioning. Individuals with larger

  10. Free Energy Calculation in MD Simulation

    E-Print Network [OSTI]

    Nielsen, Steven O.

    Free Energy Calculation in MD Simulation #12;Basic Thermodynamics Helmoholtz free energy A = U ­ TS + i Ni dA = wrev (reversible, const N V T) eq (22.9) McQuarrie & Simon Gibbs free energy G = U;Implication of Free Energy A B Keq = [A]/[B] Keq = exp (-G0 /RT) G0 = -RT ln Keq G = G0 + RT ln Q G > 0

  11. "Kohn-Shamification" of the classical density-functional theory of inhomogeneous polar molecular liquids with application to liquid hydrogen chloride

    E-Print Network [OSTI]

    Johannes Lischner; T. A. Arias

    2008-06-27

    The Gordian knot of density-functional theories for classical molecular liquids remains finding an accurate free-energy functional in terms of the densities of the atomic sites of the molecules. Following Kohn and Sham, we show how to solve this problem by considering noninteracting molecules in a set of effective potentials. This shift in perspective leads to an accurate and computationally tractable description in terms of simple three-dimensional functions. We also treat both the linear- and saturation- dielectric responses of polar systems, presenting liquid hydrogen chloride as a case study.

  12. Assessing the density functional theory-based multireference configuration interaction (DFT/MRCI) method for transition metal complexes

    SciTech Connect (OSTI)

    Escudero, Daniel E-mail: thiel@kofo.mpg.de; Thiel, Walter E-mail: thiel@kofo.mpg.de

    2014-05-21

    We report an assessment of the performance of density functional theory-based multireference configuration interaction (DFT/MRCI) calculations for a set of 3d- and 4d-transition metal (TM) complexes. The DFT/MRCI results are compared to published reference data from reliable high-level multi-configurational ab initio studies. The assessment covers the relative energies of different ground-state minima of the highly correlated CrF{sub 6} complex, the singlet and triplet electronically excited states of seven typical TM complexes (MnO{sub 4}{sup ?}, Cr(CO){sub 6}, [Fe(CN){sub 6}]{sup 4?}, four larger Fe and Ru complexes), and the corresponding electronic spectra (vertical excitation energies and oscillator strengths). It includes comparisons with results from different flavors of time-dependent DFT (TD-DFT) calculations using pure, hybrid, and long-range corrected functionals. The DFT/MRCI method is found to be superior to the tested TD-DFT approaches and is thus recommended for exploring the excited-state properties of TM complexes.

  13. Density functional theory study of chemical sensing on surfaces of single-layer MoS{sub 2} and graphene

    SciTech Connect (OSTI)

    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)

    2014-04-28

    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.

  14. Density functional theory study of transition metal porphine adsorption on gold surface and electric field induced conformation changes.

    SciTech Connect (OSTI)

    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.

    2005-06-01

    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.

  15. Structure of AgI-doped Ge-In-S glasses: Experiment, reverse Monte Carlo modelling, and density functional calculations

    SciTech Connect (OSTI)

    Chrissanthopoulos, A.; Jovari, P.; Kaban, I.; Gruner, S.; Kavetskyy, T.; Borc, J.; Wang, W.; Ren, J.; Chen, G.; Yannopoulos, S.N.

    2012-08-15

    We report an investigation of the structure and vibrational modes of Ge-In-S-AgI bulk glasses using X-ray diffraction, EXAFS spectroscopy, Reverse Monte-Carlo (RMC) modelling, Raman spectroscopy, and density functional theoretical (DFT) calculations. The combination of these techniques made it possible to elucidate the short- and medium-range structural order of these glasses. Data interpretation revealed that the AgI-free glass structure is composed of a network where GeS{sub 4/2} tetrahedra are linked with trigonal InS{sub 3/2} units; S{sub 3/2}Ge-GeS{sub 3/2} ethane-like species linked with InS{sub 4/2}{sup -} tetrahedra form sub-structures which are dispersed in the network structure. The addition of AgI into the Ge-In-S glassy matrix causes appreciable structural changes, enriching the Indium species with Iodine terminal atoms. The existence of trigonal species InS{sub 2/2}I and tetrahedral units InS{sub 3/2}I{sup -} and InS{sub 2/2}I{sub 2}{sup -} is compatible with the EXAFS and RMC analysis. Their vibrational properties (harmonic frequencies and Raman activities) calculated by DFT are in very good agreement with the experimental values determined by Raman spectroscopy. - Graphical abstract: Experiment (XRD, EXAFS, RMC, Raman scattering) and density functional calculations are employed to study the structure of AgI-doped Ge-In-S glasses. The role of mixed structural units as illustrated in the figure is elucidated. Highlights: Black-Right-Pointing-Pointer Doping Ge-In-S glasses with AgI causes significant changes in glass structure. Black-Right-Pointing-Pointer Experiment and DFT are combined to elucidate short- and medium-range structural order. Black-Right-Pointing-Pointer Indium atoms form both (InS{sub 4/2}){sup -} tetrahedra and InS{sub 3/2} planar triangles. Black-Right-Pointing-Pointer (InS{sub 4/2}){sup -} tetrahedra bond to (S{sub 3/2}Ge-GeS{sub 3/2}){sup 2+} ethane-like units forming neutral sub-structures. Black-Right-Pointing-Pointer Mixed chalcohalide species (InS{sub 3/2}I){sup -} offer vulnerable sites for the uptake of Ag{sup +}.

  16. Bubble Density Dependent Functionals to Describe Deformation and Stress Equilibrium Evolution for In-Reactor Nuclear Fuel Materials

    SciTech Connect (OSTI)

    Stout, Ray B.

    2008-07-01

    Future designs of nuclear fuels require an increased understanding of fission gas bubble density evolution. Derivations will be provided for a generic Boltzmann bubble density evolution equation, a bubble density deformation field equation, and a Cauchy stress/bubble-pressure equilibrium equation. (author)

  17. Density functional theory calculations of the turbostratically disordered compound [(SnSe)1+y]m(VSe2)n

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

    Rudin, Sven P.; Johnson, David C.

    2015-04-30

    Among composite materials that layer constituent substances of nanoscale thicknesses, [(SnSe)1+y ]m(VSe2)n emerges as an example where the constituents retain incommensurate lattice structures. Perpendicular to the stacking direction, the system exhibits random translations and random rotations on average, i.e., turbostratic disorder, with local regions showing twelvefold diffraction patterns. Earlier theoretical work on these structures showed that combining density functional theory with an empirical treatment of the van der Waals interaction gave structural parameters in good agreement with experiment, but no attempt was made to examine the relative orientations. Here we approximate the extended system with one extended constituent and onemore »finite constituent, which allows the treatment of all relative orientations on equal footing. Furthermore, the calculations show how the twelvefold periodicity follows from how the ions of the SnSe layer lock in with favored positions relative to the VSe2 layer, and the associated energy scale supports arguments for the overall turbostratic disorder.« less

  18. Density Functional Studies of Stoichiometric Surfaces of Orthorhombic Hybrid Perovskite CH3NH3PbI3

    SciTech Connect (OSTI)

    Wang, Yun; Huang, Jingsong; Sumpter, Bobby G; Zhang, Haimin; Liu, Porun; Yang, Huagui; Zhao, Huijun

    2015-01-01

    Organic/inorganic hybrid perovskite materials are highly attractive for dye-sensitized solar cells as demonstrated by their rapid advances in energy conversion efficiency. In this work, the structures, energetics, and electronic properties for a range of stoichiometric surfaces of the orthorhombic perovskite CH3NH3PbI3 are theoretically studied using density functional theory. Various possible spatially and constitutionally isomeric surfaces are considered by diversifying the spatial orientations and connectivities of surface Pb-I bonds. The comparison of the surface energies for the most stable configurations identified for various surfaces shows that the stabilities of stoichiometric surfaces are mainly dictated by the coordination numbers of surface atoms, which are directly correlated with the numbers of broken bonds. Additionally, Coulombic interactions between I anions and organic countercations on the surface also contribute to the stabilization. Electronic properties are compared between the most stable (100) surface and the bulk phase, showing generally similar features except for the lifted band degeneracy and the enhanced bandgap energy for the surface. These studies on the stoichiometric surfaces serve as the first step toward gaining a fundamental understanding of the interfacial properties in the current structural design of perovskite based solar cells, in order to achieve further breakthroughs in solar conversion efficiencies.

  19. Estimation of maximum permissible errors in the total gamma-spectra intensities at determination from them of level density and radiative strength functions

    E-Print Network [OSTI]

    A. M. Sukhovoj; V. A. Khitrov

    2010-09-24

    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.

  20. Reactive MD Simulations of Electrochemical Oxide Interfaces at...

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

    National Laboratory Reactive MD Simulations of Electrochemical Oxide Interfaces at Mesoscale PI Name: Subramanian Sankaranarayanan PI Email: skrssank@anl.gov Institution:...

  1. Evaluation of Powertrain Options and Component Sizing for MD...

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

    Sizing for MD and HD Applications on Real World Drive Cycles 2011 DOE Hydrogen and Fuel Cells Program, and Vehicle Technologies Program Annual Merit Review and Peer...

  2. Density-functional approaches to non-bonding interactions: a comparison of dispersion corrections (DFT-D), exchange-hole dipole moment (XDM) theory, and specialized functionals

    SciTech Connect (OSTI)

    Burns, Lori A [ORNL; Sherrill, David [Georgia Institute of Technology; Vazquez-Mayagoitia, Alvaro [ORNL; Sumpter, Bobby G [ORNL

    2011-01-01

    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.

  3. A comparative density functional study of methanol decomposition on Cu{sub 4} and Co{sub 4} clusters.

    SciTech Connect (OSTI)

    Mehmood, F.; Greeley, J.; Zapol, P.; Curtiss, L. A.

    2010-08-12

    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.

  4. Rotational properties of nuclei around $^{254}$No investigated using a spectroscopic-quality Skyrme energy density functional

    E-Print Network [OSTI]

    Yue Shi; J. Dobaczewski; P. T. Greenlees

    2014-03-08

    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.

  5. A density functional theory study of the oxidation of methanol to formaldehyde over vanadia supported on silica, titania, and zirconia

    SciTech Connect (OSTI)

    Khaliullin, Rustam Z.; Bell, Alexis T.

    2002-09-05

    Density functional theory was used to investigate the mechanism and kinetics of methanol oxidation to formaldehyde over vanadia supported on silica, titania, and zirconia. The catalytically active site was modeled as an isolated VO{sub 4} unit attached to the support. The calculated geometry and vibrational frequencies of the active site are in good agreement with experimental measurements both for model compounds and oxide-supported vanadia. Methanol adsorption is found to occur preferentially with the rupture of a V-O-M bond (M = Si, Ti, Zr) and with preferential attachment of a methoxy group to V. The vibrational frequencies of the methoxy group are in good agreement with those observed experimentally as are the calculated isobars. The formation of formaldehyde is assumed to occur via the transfer of an H atom of a methoxy group to the O atom of the V=O group. The activation energy for this process is found to be in the range of 199-214 kJ/mol and apparent activation energies for the overall oxidation of methanol to formaldehyde are predicted to lie in the range of 112-123 kJ/mol, which is significantly higher than that found experimentally. Moreover, the predicted turnover frequency (TOF) for methanol oxidation is found to be essentially independent of support composition, whereas experiments show that the TOF is 10{sup 3} greater for titania- and zirconia-supported vanadia than for silica-supported vanadia. Based on these findings, it is proposed that the formation of formaldehyde from methoxy groups may require pairs of adjacent VO{sub 4} groups or V{sub 2}O{sub 7} dimer structures.

  6. Density functional investigation of intermolecular effects on {sup 13}C NMR chemical-shielding tensors modeled with molecular clusters

    SciTech Connect (OSTI)

    Holmes, Sean T.; Dybowski, Cecil; Iuliucci, Robbie J.; Mueller, Karl T.

    2014-10-28

    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.

  7. L-asparagine crystals with wide gap semiconductor features: Optical absorption measurements and density functional theory computations

    SciTech Connect (OSTI)

    Zanatta, G.; Gottfried, C.; Silva, A. M.; Caetano, E. W. S.; Sales, F. A. M.; Freire, V. N.

    2014-03-28

    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.

  8. Density functional theory study of first-layer adsorption of ZrO2 and HfO2 on Ge(100)

    E-Print Network [OSTI]

    Kummel, Andrew C.

    in this manuscript), usually grown by atomic layer deposition (ALD). These oxides, under normal Ge process- ingDensity functional theory study of first-layer adsorption of ZrO2 and HfO2 on Ge(100) T.J. Grassman

  9. PdnCO (n ) 1,2): Accurate Ab Initio Bond Energies, Geometries, and Dipole Moments and the Applicability of Density Functional Theory for Fuel Cell Modeling

    E-Print Network [OSTI]

    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

  10. Scalar relativistic computations of nuclear magnetic shielding and g-shifts with the zeroth-order regular approximation and range-separated hybrid density functionals

    SciTech Connect (OSTI)

    Aquino, Fredy W.; Govind, Niranjan; Autschbach, Jochen

    2011-10-01

    Density functional theory (DFT) calculations of NMR chemical shifts and molecular g-tensors with Gaussian-type orbitals are implemented via second-order energy derivatives within the scalar relativistic zeroth order regular approximation (ZORA) framework. Nonhybrid functionals, standard (global) hybrids, and range-separated (Coulomb-attenuated, long-range corrected) hybrid functionals are tested. Origin invariance of the results is ensured by use of gauge-including atomic orbital (GIAO) basis functions. The new implementation in the NWChem quantum chemistry package is verified by calculations of nuclear shielding constants for the heavy atoms in HX (X=F, Cl, Br, I, At) and H2X (X = O, S, Se, Te, Po), and Te chemical shifts in a number of tellurium compounds. The basis set and functional dependence of g-shifts is investigated for 14 radicals with light and heavy atoms. The problem of accurately predicting F NMR shielding in UF6-nCln, n = 1 to 6, is revisited. The results are sensitive to approximations in the density functionals, indicating a delicate balance of DFT self-interaction vs. correlation. For the uranium halides, the results with the range-separated functionals are mixed.

  11. Scaling of the known exact explicit forms of the non-interacting kinetic-energy density functional

    E-Print Network [OSTI]

    Lázaro Calderín

    2014-10-15

    It has been previously proven that the Kohn-Sham kinetic energy functional scales homogeneusly under generalized coordinate scaling, in a way that is obeyed by the von Weiz\\"acker functional, but seems to be in contradiction with the scaling of the Thomas-Fermi functional. A very puzzling situation, taking in to account that the von Weiz\\"acker and Thomas-Fermi functionals are exact cases of the Kohn-Sham kinetic energy functional for two electron systems, and the non-interacting electron gas, respectively. The apparent contradiction is resolved in this paper.

  12. PHYSICAL REVIEW A 87, 053406 (2013) Exterior complex scaling method in time-dependent density-functional theory

    E-Print Network [OSTI]

    Chu, Shih-I

    2013-01-01

    -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

  13. RECOMMENDATION FORM UMBC Office of Financial Aid & Scholarships, 1000 Hilltop Circle, Baltimore, MD 21250

    E-Print Network [OSTI]

    Biswas, Animikh

    RECOMMENDATION FORM UMBC Office of Financial Aid & Scholarships, 1000 Hilltop Circle, Baltimore, MD of Financial Aid & Scholarships 1000 Hilltop Circle Baltimore, MD 21250 Name

  14. Why are MD simulated protein folding times wrong? Dmitry Nerukh

    E-Print Network [OSTI]

    Nerukh, Dmitry

    Why are MD simulated protein folding times wrong? Dmitry Nerukh Unilever Centre for Molecular.ac.uk The question of significant deviations of protein folding times simulated using molecular dynamics from

  15. Single-block collision attack on MD5 Marc Stevens

    E-Print Network [OSTI]

    International Association for Cryptologic Research (IACR)

    Single-block collision attack on MD5 Marc Stevens Cryptology Group, CWI P.O. Box 94079, NL-1090 GB Amsterdam, The Netherlands marc@marc-stevens.nl January 29, 2012 Abstract In 2010, Tao Xie and Dengguo Feng

  16. Molly Carnes, MD, MS Professor, Depts of Medicine,

    E-Print Network [OSTI]

    Sheridan, Jennifer

    Molly Carnes, MD, MS Professor, Depts of Medicine, Psychiatry, and Industrial & Systems Engineering University of Wisconsin-Madison Careers in Academic Medicine:Careers in Academic Medicine: Evaluation at

  17. The 2dF Galaxy Redshift Survey correlation functions, peculiar velocities and the matter density of the Universe

    E-Print Network [OSTI]

    Hawkins, E; Cole, S; Madgwick, D; Norberg, P; Peacock, J; Baldry, I K; Baugh, C; Bland-Hawthorn, J; Bridges, T J; Cannon, R; Colless, M; Collins, C; Couch, W; Dalton, G B; De Propris, R; Driver, S; Efstathiou, G P; Ellis, R; Frenk, C; Glazebrook, K; Jackson, C; Jones, B; Lahav, O; Lewis, I; Lumsden, S; Percival, W; Peterson, B; Sutherland, W; Taylor, K; Hawkins, Ed; Maddox, Steve; Cole, Shaun; Madgwick, Darren; Norberg, Peder; Peacock, John; Baldry, Ivan; Baugh, Carlton; Bland-Hawthorn, Joss; Bridges, Terry; Cannon, Russell; Colless, Matthew; Collins, Chris; Couch, Warrick; Dalton, Gavin; Propris, Roberto De; Driver, Simon; Efstathiou, George; Ellis, Richard; Frenk, Carlos; Glazebrook, Karl; Jackson, Carole; Jones, Bryn; Lahav, Ofer; Lewis, Ian; Lumsden, Stuart; Percival, Will; Peterson, Bruce; Sutherland, Will; Taylor, Keith

    2003-01-01

    We present a detailed analysis of the two-point correlation function, from the 2dF Galaxy Redshift Survey (2dFGRS). The large size of the catalogue, which contains ~220000 redshifts, allows us to make high precision measurements of various properties of the galaxy clustering pattern. We estimate the redshift-space correlation function, xi(s), from which we measure the redshift-space clustering length, s0 = 6.82 +/- 0.28 Mpc/h. We also estimate the projected correlation function, and the real-space correlation function, xi(r), which can be fit by a power-law, with r0 = 5.05 +/- 0.26 Mpc/h and slope gamma = 1.67 +/- 0.03. For r > 20 Mpc/h, xi drops below a power-law as, for instance, is expected in the popular LCDM model. The ratio of amplitudes of the real and redshift-space correlation functions on scales of 8 - 30 Mpc/h gives an estimate of the redshift-space distortion parameter beta. The quadrupole moment of xi on scales 30 - 40 Mpc/h provides another estimate of beta. We also estimate the distribution fun...

  18. Revisiting Dedicated and Block Cipher based Hash Functions Anupam Pattanayak

    E-Print Network [OSTI]

    International Association for Cryptologic Research (IACR)

    Revisiting Dedicated and Block Cipher based Hash Functions Anupam Pattanayak Computer Science the compression function from different angles. Two major categories of hash functions are: dedicated hash in this paper. Two dedicated has functions from MD4 family - MD4, and SHA-256 constructions have been detailed

  19. Dynamics of a globular protein and its hydration water studied by neutron scattering and MD simulations

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

    Chen, Sow-Hsin; Lagi, Marco; Chu, Xiang-qiang; Zhang, Yang; Kim, Chansoo; Faraone, Antonio; Fratini, Emiliano; Baglioni, Piero

    2010-01-01

    This review article describes our neutron scattering experiments made in the past four years for the understanding of the single-particle (hydrogen atom) dynamics of a protein and its hydration water and the strong coupling between them. We found that the key to this strong coupling is the existence of a fragile-to-strong dynamic crossover (FSC) phenomenon occurring at aroundTL= 225±5 K in the hydration water. On lowering of the temperature toward FSC, the structure of hydration water makes a transition from predominantly the high density form (HDL), a more fluid state, to predominantly the low density form (LDL), a less fluidmore »state, derived from the existence of a liquid–liquid critical point at an elevated pressure. We show experimentally that this sudden switch in the mobility of hydration water on Lysozyme, B-DNA and RNA triggers the dynamic transition, at a temperatureTD= 220 K, for these biopolymers. In the glassy state, belowTD, the biopolymers lose their vital conformational flexibility resulting in a substantial diminishing of their biological functions. We also performed molecular dynamics (MD) simulations on a realistic model of hydrated lysozyme powder, which confirms the existence of the FSC and the hydration level dependence of the FSC temperature. Furthermore, we show a striking feature in the short time relaxation (?-relaxation) of protein dynamics, which is the logarithmic decay spanning 3 decades (from ps to ns). The long time?-relaxation shows instead a diffusive behavior, which supports the liquid-like motions of protein constituents. We then discuss our recent high-resolution X-ray inelastic scattering studies of globular proteins, Lysozyme and Bovine Serum Albumin. We were able to measure the dispersion relations of collective, intra-protein phonon-like excitations in these proteins for the first time. We found that the phonon energies show a marked softening and at the same time their population increases substantially in a certain wave vector range when temperature crosses over theTD. Thus the increase of biological activities aboveTDhas positive correlation with activation of slower and large amplitude collective motions of a protein.« less

  20. Including screening in van der Waals corrected density functional theory calculations: The case of atoms and small molecules physisorbed on graphene

    SciTech Connect (OSTI)

    Silvestrelli, Pier Luigi; Ambrosetti, Alberto

    2014-03-28

    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.

  1. Ab initio density functional theory investigation of the structural, electronic and optical properties of Ca{sub 3}Sb{sub 2} in hexagonal and cubic phases

    SciTech Connect (OSTI)

    Arghavani Nia, Borhan; Sedighi, Matin; Shahrokhi, Masoud; Moradian, Rostam

    2013-11-15

    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.

  2. Scaling properties of critical bubble of homogeneous nucleation in stretched fluid of square-gradient density-functional model with triple-parabolic free energy

    E-Print Network [OSTI]

    Masao Iwamatsu

    2008-08-07

    The square-gradient density-functional model with triple-parabolic free energy is used to study homogeneous bubble nucleation in a stretched liquid to check the scaling rule for the work of formation of the critical bubble as a function of scaled undersaturation $\\Delta\\mu/\\Delta\\mu_{\\rm spin}$, the difference in chemical potential $\\Delta\\mu$ between the bulk undersaturated and saturated liquid divided by $\\Delta\\mu_{\\rm spin}$ between the liquid spinodal and saturated liquid. In contrast to our study, a similar density-functional study for a Lennard-Jones liquid by Shen and Debenedetti [J. Chem. Phys. {\\bf 114}, 4149 (2001)] found that not only the work of formation but other various quantities related to the critical bubble show the scaling rule, however, we found virtually no scaling relationships in our model near the coexistence. Although some quantities show almost perfect scaling relations near the spinodal, the work of formation divided by the value deduced from the classical nucleation theory shows no scaling in this model even though it correctly vanishes at the spinodal. Furthermore, the critical bubble does not show any anomaly near the spinodal as predicted many years ago. In particular, our model does not show diverging interfacial width at the spinodal, which is due to the fact that compressibility remains finite until the spinodal is reached in our parabolic models.

  3. A time-dependent momentum-space density functional theoretical approach for electron transport dynamics in molecular devices

    E-Print Network [OSTI]

    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

  4. Catalytic Reactions of Living Polymers: Density Functional Study of Reactivity of Phenol and Phenoxides with the Cyclic Tetramer of Polycarbonate

    E-Print Network [OSTI]

    (NaOPh) with the cyclic tetramer of bisphenol A polycarbonate (BPA-PC) has been investigated using of industrial applications of polycarbonates has led to many studies, and bisphenol A polycarbonate (BPA- PC of functionalized bisphenols using a variety of catalysts showed that the carbonate group provided the site for ring

  5. Systematic approach for simultaneously correcting the band-gap andp-dseparation errors of common cation III-V or II-VI binaries in density functional theory calculations within a local density approximation

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

    Wang, Jianwei; Zhang, Yong; Wang, Lin-Wang

    2015-07-31

    We propose a systematic approach that can empirically correct three major errors typically found in a density functional theory (DFT) calculation within the local density approximation (LDA) simultaneously for a set of common cation binary semiconductors, such as III-V compounds, (Ga or In)X with X = N,P,As,Sb, and II-VI compounds, (Zn or Cd)X, with X = O,S,Se,Te. By correcting (1) the binary band gaps at high-symmetry points , L, X, (2) the separation of p-and d-orbital-derived valence bands, and (3) conduction band effective masses to experimental values and doing so simultaneously for common cation binaries, the resulting DFT-LDA-based quasi-first-principles methodmore »can be used to predict the electronic structure of complex materials involving multiple binaries with comparable accuracy but much less computational cost than a GW level theory. This approach provides an efficient way to evaluate the electronic structures and other material properties of complex systems, much needed for material discovery and design.« less

  6. Linear combination of Gaussian-type orbitals--local-density-functional cluster studies of D-D interactions in titanium and palladium

    SciTech Connect (OSTI)

    Dunlap, B.I.; Brenner, D.W.; Mowrey, R.C.; Mintmire, J.W.; White, C.T. )

    1990-05-15

    Linear combination of Gaussian-type orbitals (LCGTO) --local-density-functional (LDF) cluster calculations give the interaction energy of two deuterium atoms in the interstices of titanium and palladium. Octahedral and tetrahedral interstices of the face-centered-cubic (fcc) lattice are modeled by six and four metal atoms, respectively. No short equilibrium separations, compared to the gas-phase equilibrium separation, are found even when expansion of the lattice and loading with additional deuterium and metal atoms are considered. The deuteron affinities of these clusters are in accord with the experimental site preference.

  7. Electronically Excited States of Vitamin B12: Benchmark Calculations Including Time-Dependent Density Functional Theory and Correlated Ab Initio Methods

    E-Print Network [OSTI]

    Kornobis, Karina; Wong, Bryan M; Lodowski, Piotr; Jaworska, Maria; Andruniów, Tadeusz; Rudd, Kenneth; Kozlowski, Pawel M; 10.1021/jp110914y

    2011-01-01

    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 ...

  8. A density functional theory study of magneto-electric Jones birefringence of noble gases, furan homologues, and mono-substituted benzenes

    SciTech Connect (OSTI)

    Fahleson, Tobias; Norman, Patrick; Coriani, Sonia; Rizzo, Antonio; Rikken, Geert L. J. A.

    2013-11-21

    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.

  9. Spin and orbital magnetism of coinage metal trimers (Cu{sub 3}, Ag{sub 3}, Au{sub 3}): A relativistic density functional theory study

    SciTech Connect (OSTI)

    Afshar, Mahdi; Sargolzaei, Mohsen

    2013-11-15

    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.

  10. MD Simulation Study of the Influence of Branch Content on Relaxation and Crystallization of Branched Polyethylene Chains with Uniform Branch Distribution

    E-Print Network [OSTI]

    Hussein, Ibnelwaleed A.

    of Branched Polyethylene Chains with Uniform Branch Distribution I. A. HUSSEIN, B. F. ABU-SHARKH* Department-density polyethylene (LLDPE) chains with different levels of branch content (BC), ranging from 10 to 80 branches/1000 C words: MD simulation, Polyethylene, branch content, chain conformation, radius of gyration

  11. Electronic states of thiophene/phenylene co-oligomers: Extreme-ultra violet excited photoelectron spectroscopy observations and density functional theory calculations

    SciTech Connect (OSTI)

    Kawaguchi, Yoshizo; Sasaki, Fumio; Mochizuki, Hiroyuki; Ishitsuka, Tomoaki; Tomie, Toshihisa; Ootsuka, Teruhisa; Watanabe, Shuji; Shimoi, Yukihiro; Yamao, Takeshi; Hotta, Shu

    2013-02-28

    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.

  12. Symmetry-adapted perturbation theory with Kohn-Sham orbitals using non-empirically tuned, long-range-corrected density functionals

    SciTech Connect (OSTI)

    Lao, Ka Un; Herbert, John M.

    2014-01-28

    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.

  13. A van der Waals density functional study of adenine on graphene: Single molecular adsorption and overlayer binding

    SciTech Connect (OSTI)

    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

    2011-01-01

    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.

  14. Density functional theory study on the interstitial chemical shifts of main-group-element centered hexazirconium halide clusters; synthetic control of speciation in [(Zr6ZCl12)] (Z = B, C)-based mixed ligand complexes 

    E-Print Network [OSTI]

    Shen, Jingyi

    2005-08-29

    The correlation between NMR chemical shifts of interstitial atoms and electronic structures of boron- and carbon-centered hexazirconium halide clusters was investigated by density functional theory (DFT) calculation. The ...

  15. Self-interaction-free time-dependent density-functional theory for molecular processes in strong fields:? High-order harmonic generation of H2 in intense laser fields

    E-Print Network [OSTI]

    Chu, Shih-I; Chu, Xi

    2001-01-17

    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 ...

  16. Time-dependent density-functional theory for strong-field multiphoton processes: Application to the study of the role of dynamical electron correlation in multiple high-order harmonic generation

    E-Print Network [OSTI]

    Tong, Xiao-Min; Chu, Shih-I

    1998-01-01

    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 ...

  17. Time-dependent density-functional theory for molecular processes in strong fields: Study of multiphoton processes and dynamical response of individual valence electrons of N2 in intense laser fields

    E-Print Network [OSTI]

    Chu, Xi; Chu, Shih-I

    2001-11-14

    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. ...

  18. Benchmarking the performance of density functional theory and point charge force fields in their description of sI methane hydrate against diffusion Monte Carlo

    SciTech Connect (OSTI)

    Cox, Stephen J.; Michaelides, Angelos; Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ ; Towler, Michael D.; Theory of Condensed Matter Group, Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, Cambridge CB3 0HE ; Alfè, Dario; Department of Earth Sciences, University College London Gower Street, London WC1E 6BT

    2014-05-07

    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.

  19. An analysis of van der Waals density functional components: Binding and corrugation of benzene and C60 on boron nitride and graphene

    E-Print Network [OSTI]

    Berland, Kristian

    2013-01-01

    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 ...

  20. Numerical Solution of 3D Poisson-Nernst-Planck Equations Coupled with Classical Density Functional Theory for Modeling Ion and Electron Transport in a Confined Environment

    SciTech Connect (OSTI)

    Meng, Da; Zheng, Bin; Lin, Guang; Sushko, Maria L.

    2014-08-29

    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.

  1. Structural, elastic, electronic and phonon properties of SnX{sub 2}O{sub 4} (X=Mg, Zn, Cd) spinel from density functional theory

    SciTech Connect (OSTI)

    U?ur, Gökay; Candan, Abdullah

    2014-10-06

    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.

  2. Ab initio-driven nuclear energy density functional method. A proposal for safe/correlated/improvable parametrizations of the off-diagonal EDF kernels

    E-Print Network [OSTI]

    Duguet, T; Ebran, J -P; Lesinski, T; Somà, V

    2015-01-01

    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.

  3. Ab initio-driven nuclear energy density functional method. A proposal for safe/correlated/improvable parametrizations of the off-diagonal EDF kernels

    E-Print Network [OSTI]

    T. Duguet; M. Bender; J. -P. Ebran; T. Lesinski; V. Somà

    2015-02-12

    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.

  4. Liquid drops on a surface: using density functional theory to calculate the binding potential and drop profiles and comparing with results from mesoscopic modelling

    E-Print Network [OSTI]

    Adam P. Hughes; Uwe Thiele; Andrew J. Archer

    2015-01-28

    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.

  5. Systematic study of nuclear matrix elements in neutrinoless double-beta decay with a beyond mean-field covariant density functional theory

    E-Print Network [OSTI]

    J. M. Yao; L. S. Song; K. Hagino; P. Ring; J. Meng

    2015-01-29

    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.

  6. Subsystem Density-Functional Theory as an Effective Tool for Modeling Ground and Excited States, their Dynamics, and Many-Body Interactions

    E-Print Network [OSTI]

    Krishtal, Alisa; Genova, Alessandro; Pavanello, Michele

    2015-01-01

    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.

  7. Stability of critical bubble in stretched fluid of square-gradient density-functional model with triple-parabolic free energy

    E-Print Network [OSTI]

    Masao Iwamatsu; Yutaka Okabe

    2010-06-11

    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.

  8. Density functional theory studies on theelectronic, structural, phonon dynamicaland thermo-stability properties of bicarbonates MHCO3, M D Li, Na, K

    SciTech Connect (OSTI)

    Duan, Yuhua; Zhang, Bo; Sorescu, Dan C.; Johnson, Karl; Majzoub, Eric H; Luebke, David R.

    2012-07-01

    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.

  9. Corey Casper, MD Head, Program in Global Oncology

    E-Print Network [OSTI]

    Brent, Roger

    Corey Casper, MD Head, Program in Global Oncology Member, Vaccine and Infectious Disease and Public of Washington Dr. Casper focuses on infection-related cancers and cancer in low-resource settings. He is the Head of the Program in Global Oncology at the Fred Hutchinson Cancer Research Center, where he is also

  10. Eric G. Neilson, MD DEAN OF FEINBERG SCHOOL OF

    E-Print Network [OSTI]

    Goldman, Robert D.

    Eric G. Neilson, MD DEAN OF FEINBERG SCHOOL OF MEDICINE AND VICE PRESIDENT FOR MEDICAL AFFAIRS of Robert R. McCormick School of Engineering and Applied Science Dwight A. McBride, Dean of the Graduate and Vice Dean for Development and Alumni Relations for Feinberg School of Medicine Jaci A. Thiede

  11. Cancer Research in Botswana Surbhi Grover, MD MPH

    E-Print Network [OSTI]

    Bushman, Frederic

    Cancer Research in Botswana Surbhi Grover, MD MPH Assistant Professor, Radiation Oncology, UPENN and are developing cancers and other NCDs #12;3 HIV and Cancer wHIV infection increases the risk of cancer wIn the later stages of HIV infection, chronic immunosuppression (& other co-factors) leads to cancer formation

  12. One Physics Ellipse College Park, MD 20740-3844

    E-Print Network [OSTI]

    Nahar, Sultana Nurun

    of physics. When we get closer to the April Meeting, APS will provide easy instructions on how to upload yourAmerican Physical Society One Physics Ellipse College Park, MD 20740-3844 Tel: (301) 209-3269 Fax: (301) 209-0867 www.aps.org President Robert L. Byer Stanford University President-Elect Michael S

  13. Proportional Contact Representations of Planar Graphs Md. J. Alam1

    E-Print Network [OSTI]

    Kobourov, Stephen G.

    Proportional Contact Representations of Planar Graphs Md. J. Alam1 , T. Biedl2 , S. Felsner3 , M-contact between the corresponding polygons. Specifically, we consider proportional contact representations, where, the cartographic error, and the unused area. We describe construc- tive algorithms for proportional contact

  14. Molly Carnes, MD, MS Professor, Depts of Medicine,

    E-Print Network [OSTI]

    Sheridan, Jennifer

    Molly Carnes, MD, MS Professor, Depts of Medicine, Psychiatry, and Industrial & Systems Engineering University of Wisconsin-Madison Careers in Academic Medicine: Evaluation at Gatekeeping Junctures #12;AAMC (N=0) 0 Dept Medicine Chairs at top 25: #12;What about geriatrics? Year med school graduation 1980

  15. md Science Service Featuro By Dr. Charles F. Brooks

    E-Print Network [OSTI]

    No. 745 Sept. 30 md Science Service Featuro By Dr. Charles F. Brooks of Clark University. RAIN SKADOWS Mountains cast rain shadoms; often there is the greatest difference in rain- is fall between in me trade wind, laden with water vapor, blows persistently from one direction. is forced to rise

  16. TSUNAMI INUNDATION MAPPING FOR OCEAN CITY, MD NGDC DEM

    E-Print Network [OSTI]

    Kirby, James T.

    TSUNAMI INUNDATION MAPPING FOR OCEAN CITY, MD NGDC DEM BY BABAK TEHRANIRAD, SAEIDEH BANIHASHEMI BY THE NATIONAL TSUNAMI HAZARD MITIGATION PROGRAM NATIONAL WEATHER SERVICE GRANT NA10NWS4670010 CENTER FOR APPLIED COASTAL RESEARCH Ocean Engineering Laboratory University of Delaware Newark, Delaware 19716 #12;Tsunami

  17. 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

    E-Print Network [OSTI]

    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

  18. End-to-End Rate-Distortion Optimized MD Mode Selection for Multiple Description Video Coding

    E-Print Network [OSTI]

    Apostolopoulos, John G.

    Multiple description (MD) video coding can be used to reduce the detrimental effects caused by transmission over lossy packet networks. A number of approaches have been proposed for MD coding, where each provides a different ...

  19. Density functional theory and DFT+U study of transition metal porphines adsorbed on Au(111) surfaces and effects of applied electric fields

    E-Print Network [OSTI]

    Kevin Leung; Susan B. Rempe; Peter A. Schultz; Eduardo M. Sproviero; Victor S. Batista; Michael E. Chandross; Craig J. Medforth

    2006-10-26

    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.

  20. Simulating Ru L3-Edge X-ray Absorption Spectroscopy with Time-Dependent Density Functional Theory: Model Complexes and Electron Localization in Mixed-Valence Metal Dimers

    SciTech Connect (OSTI)

    Kuiken, Benjamin E. Van; Valiev, Marat; Daifuku, Stephanie L.; Bannan, Caitlin; Strader, Matthew L.; Cho, Hana; Huse, Nils; Schoenlein, Robert W.; Govind, Niranjan; Khalil, Munira

    2013-04-26

    Ruthenium L3-edge X-ray absorption (XA) spectroscopy probes unoccupied 4d orbitals of the metal atom and is increasingly being used to investigate the local electronic structure in ground and excited electronic states of Ru complexes. The simultaneous development of computational tools for simulating Ru L3-edge spectra is crucial for interpreting the spectral features at a molecular level. This study demonstrates that time-dependent density functional theory (TDDFT) is a viable and predictive tool for simulating ruthenium L3-edge XA spectroscopy. We systematically investigate the effects of exchange correlation functional and implicit and explicit solvent interactions on a series of RuII and RuIII complexes in their ground and electronic excited states. The TDDFT simulations reproduce all of the experimentally observed features in Ru L3-edge XA spectra within the experimental resolution (0.4 eV). Our simulations identify ligand-specific charge transfer features in complicated Ru L3-edge spectra of [Ru(CN)6]4- and RuII polypyridyl complexes illustrating the advantage of using TDDFT in complex systems. We conclude that the B3LYP functional most accurately predicts the transition energies of charge transfer features in these systems. We use our TDDFT approach to simulate experimental Ru L3-edge XA spectra of transition metal mixed-valence dimers of the form [(NC)5MII-CN-RuIII(NH3)5] (where M = Fe or Ru) dissolved in water. Our study determines the spectral signatures of electron delocalization in Ru L3-edge XA spectra. We find that the inclusion of explicit solvent molecules is necessary for reproducing the spectral features and the experimentally determined valencies in these mixed-valence complexes. This study validates the use of TDDFT for simulating Ru 2p excitations using popular quantum chemistry codes and providing a powerful interpretive tool for equilibrium and ultrafast Ru L3-edge XA spectroscopy.

  1. Dispersion-correcting potentials can significantly improve the bond dissociation enthalpies and noncovalent binding energies predicted by density-functional theory

    SciTech Connect (OSTI)

    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)

    2014-05-14

    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.

  2. COPD, INFLAMMATION, AND LUNG CANCER Jerome S Brody, M.D., Professor of Medicine

    E-Print Network [OSTI]

    1 COPD, INFLAMMATION, AND LUNG CANCER Jerome S Brody, M.D., Professor of Medicine and Avrum Spira, M.D., Assistant Professor of Medicine Pulmonary Center and Department of Medicine Boston University School of Medicine Corresponding Author; Jerome S Brody, MD Pulmonary Center Boston University School

  3. Electronic and optical properties of pure and modified diamondoids studied by many-body perturbation theory and time-dependent density functional theory

    SciTech Connect (OSTI)

    Demján, Tamás; Vörös, Márton; Palummo, Maurizia; Gali, Adam

    2014-08-14

    Diamondoids are small diamond nanoparticles (NPs) that are built up from diamond cages. Unlike usual semiconductor NPs, their atomic structure is exactly known, thus they are ideal test-beds for benchmarking quantum chemical calculations. Their usage in spintronics and bioimaging applications requires a detailed knowledge of their electronic structure and optical properties. In this paper, we apply density functional theory (DFT) based methods to understand the electronic and optical properties of a few selected pure and modified diamondoids for which accurate experimental data exist. In particular, we use many-body perturbation theory methods, in the G{sub 0}W{sub 0} and G{sub 0}W{sub 0}+BSE approximations, and time-dependent DFT in the adiabatic local density approximation. We find large quasiparticle gap corrections that can exceed thrice the DFT gap. The electron-hole binding energy can be as large as 4 eV but it is considerably smaller than the GW corrections and thus G{sub 0}W{sub 0}+BSE optical gaps are about 50% larger than the Kohn-Sham (KS) DFT gaps. We find significant differences between KS time-dependent DFT and GW+BSE optical spectra on the selected diamondoids. The calculated G{sub 0}W{sub 0} quasiparticle levels agree well with the corresponding experimental vertical ionization energies. We show that nuclei dynamics in the ionization process can be significant and its contribution may reach about 0.5 eV in the adiabatic ionization energies.

  4. Potassium-induced effect on structure and chemical activity of CuxO/Cu(111) (x?2) surface: A combined scanning tunneling microscopy and density functional theory study

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

    Liu, Ping; An, Wei; Stacchiola, Dario; Xu, Fang

    2015-10-16

    Potassium (K) plays an essential role in promoting catalytic reaction in many established industrial catalytic processes. Here, we report a combined study using scanning tunneling microscopy (STM) and density functional theory (DFT) in understanding the effect of depositing K on the atomic and electronic structures as well as chemical activities of CuxO/Cu(111) (x?2). The DFT calculations observe a pseudomorphic growth of K on CuxO/Cu(111) up to 0.19 monolayer (ML) of coverage, where K binds the surface via strong ionic interaction with chemisorbed oxygen and the relatively weak electrostatic interactions with copper ions, lower and upper oxygen on the CuxO rings.more »The simulated STM pattern based on the DFT results agrees well with the experimental observations. The deposited K displays great impact on the surface electronic structure of CuxO/Cu(111), which induces significant reduction in work function and leads to a strong electron polarization on the surface. The promotion of K on the surface binding properties is selective. It varies depending on the nature of adsorbates. According to our results, K has little effect on surface acidity, while it enhances the surface basicity significantly. As a consequence, the presence of K does not help for CO adsorption on CuxO/Cu(111), but being able to accelerate the activation of CO2. Thus, such promotion strongly depends on the combinations from both geometric and electronic effects. Our results highlight the origin of promoting effect of alkalis in the design of catalysts for the complex reactions.« less

  5. Study of electron acceleration and x-ray radiation as a function of plasma density in capillary-guided laser wakefield accelerators

    SciTech Connect (OSTI)

    Ju, J.; Döpp, A.; Cros, B.; Svensson, K.; Genoud, G.; Wojda, F.; Burza, M.; Persson, A.; Lundh, O.; Wahlström, C.-G.; Ferrari, H.

    2013-08-15

    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.

  6. Reaction dynamics of OH{sup +}({sup 3}{sigma}{sup -})+C{sub 2}H{sub 2} studied with crossed beams and density functional theory calculations

    SciTech Connect (OSTI)

    Liu Li; Martin, Courtney; Farrar, James M. [Department of Chemistry, University of Rochester, Rochester, New York 14627 (United States)

    2006-10-07

    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.

  7. Electronic structure of the heavy-fermion caged compound Ce?Pd??X? (X = Si, Ge) studied by density functional theory and photoelectron spectroscopy

    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

    2015-03-30

    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

  8. Electronic structure of the heavy-fermion caged compound Ce3Pd20X6(X=Si,Ge) studied by density functional theory and photoelectron spectroscopy

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

    Yamaoka, Hitoshi; Schwier, Eike F.; Arita, Masashi; Shimada, Kenya; Tsujii, Naohito; Jarrige, Ignace; Jiang, Jian; Hayashi, Hirokazu; Iwasawa, Hideaki; Namatame, Hirofumi; et al

    2015-03-30

    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

  9. Dissociative adsorption of CH{sub 3}X (X = Br and Cl) on a silicon(100) surface revisited by density functional theory

    SciTech Connect (OSTI)

    Wang, Chen-Guang; Huang, Kai E-mail: wji@ruc.edu.cn; Ji, Wei E-mail: wji@ruc.edu.cn

    2014-11-07

    During the dissociative adsorption on a solid surface, the substrate usually participates in a passive manner to accommodate fragments produced upon the cleavage of the internal bond(s) of a (transient) molecular adsorbate. This simple picture, however, neglects the flexibility of surface atoms. Here, we report a Density Functional Theory study to revisit our early studies of the dissociative adsorption of CH{sub 3}X (X = Br and Cl) on Si(100). We have identified a new reaction pathway, which involves a flip of a silicon dimer; this new pathway agrees better with experiments. For our main exemplar of CH{sub 3}Br, insights have been gained using a simple model that involves a three-atom reactive center, Br-C-Si. When the silicon dimer flips, the interaction between C and Si in the Br-C-Si center is enhanced, evident in the increased energy-split of the frontier orbitals. We also examine how the dissociation dynamics of CH{sub 3}Br is altered on a heterodimer (Si-Al, Si-P, and Si-Ge) in a Si(100) surface. In each case, we conclude, on the basis of computed reaction pathways, that no heterodimer flipping is involved before the system transverses the transition state to dissociative adsorption.

  10. Microscopic study of low-lying spectra of $\\Lambda$ hypernuclei based on a beyond-mean-field approach with covariant energy density functional

    E-Print Network [OSTI]

    Mei, H; Yao, J M; Motoba, T

    2015-01-01

    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 hypernucle...

  11. In situ infrared spectroscopic and density-functional studies of the cross-linked structure of one-dimensional C{sub 60} polymer

    SciTech Connect (OSTI)

    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)

    2010-08-15

    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.

  12. Spin-orbit relativistic long-range corrected time-dependent density functional theory for investigating spin-forbidden transitions in photochemical reactions

    SciTech Connect (OSTI)

    Nakata, Ayako; Tsuneda, Takao; Hirao, Kimihiko [Advanced Science Institute, RIKEN, Wako 351-0198 (Japan); CREST, Japan Science and Technology Agency, Kawaguchi 332-0012 (Japan)

    2011-12-14

    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.

  13. Probability density function treatment of turbulence/chemistry interactions during the ignition of a temperature-stratified mixture for application to HCCI engine modeling

    SciTech Connect (OSTI)

    Bisetti, Fabrizio; Chen, J.-Y.; Hawkes, Evatt R.; Chen, Jacqueline H.

    2008-12-15

    Homogeneous charge compression ignition (HCCI) engine technology promises to reduce NO{sub x} and soot emissions while achieving high thermal efficiency. Temperature and mixture stratification are regarded as effective means of controlling the start of combustion and reducing the abrupt pressure rise at high loads. Probability density function methods are currently being pursued as a viable approach to modeling the effects of turbulent mixing and mixture stratification on HCCI ignition. In this paper we present an assessment of the merits of three widely used mixing models in reproducing the moments of reactive scalars during the ignition of a lean hydrogen/air mixture ({phi}=0.1, p=41atm, and T=1070 K) under increasing temperature stratification and subject to decaying turbulence. The results from the solution of the evolution equation for a spatially homogeneous joint PDF of the reactive scalars are compared with available direct numerical simulation (DNS) data [E.R. Hawkes, R. Sankaran, P.P. Pebay, J.H. Chen, Combust. Flame 145 (1-2) (2006) 145-159]. The mixing models are found able to quantitatively reproduce the time history of the heat release rate, first and second moments of temperature, and hydroxyl radical mass fraction from the DNS results. Most importantly, the dependence of the heat release rate on the extent of the initial temperature stratification in the charge is also well captured. (author)

  14. Optimizing minimum free-energy crossing points in solution: Linear-response free energy/spin-flip density functional theory approach

    SciTech Connect (OSTI)

    Minezawa, Noriyuki

    2014-10-28

    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.

  15. Critical cavity in the stretched fluid studied using square-gradient density-functional model with triple-parabolic free energy

    E-Print Network [OSTI]

    Masao Iwamatsu

    2009-04-04

    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.

  16. Brain-Computer Interfaces in Medicine Jerry J. Shih, MD; Dean J. Krusienski, PhD; and Jonathan R. Wolpaw, MD

    E-Print Network [OSTI]

    Nehorai, Arye

    Brain-Computer Interfaces in Medicine Jerry J. Shih, MD; Dean J. Krusienski, PhD; and Jonathan R. Wolpaw, MD Abstract Brain-computer interfaces (BCIs) acquire brain signals, analyze them, and translate, electrocorticographic, and other brain signals for increasingly complex control of cursors, robotic arms, prostheses

  17. UC Davis-LLNL Scientific Advisory Committee Timothy Albertson, MD, PhD, Vice Chair, Internal Medicine

    E-Print Network [OSTI]

    Carmichael, Owen

    UC Davis-LLNL Scientific Advisory Committee Timothy Albertson, MD, PhD, Vice Chair, Internal Berglund, MD, PhD, CTSC Program Director Stuart Cohen, MD, Head of Infection Control, UCDMC Jeffrey Elias, PhD, Manager, Grant Coordination **Captain** Hernando Garzon, MD, Emergency Medicine, Kaiser Jeffrey

  18. Reaction dynamics study of O{sup -}+C{sub 2}H{sub 2} with crossed beams and density-functional theory calculations

    SciTech Connect (OSTI)

    Liu Li; Li Yue; Farrar, James M. [Department of Chemistry, University of Rochester, Rochester, New York 14627 (United States)

    2005-09-01

    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.

  19. Structure, stability, and electronic property of carbon-doped gold clusters Au{sub n}C{sup ?} (n = 1–10): A density functional theory study

    SciTech Connect (OSTI)

    Yan, Li-Li; Liu, Yi-Rong; Huang, Teng; Jiang, Shuai; Wen, Hui; Gai, Yan-Bo; Zhang, Wei-Jun E-mail: wjzhang@aiofm.ac.cn; Huang, Wei E-mail: wjzhang@aiofm.ac.cn; School of Environmental Science and Optoelectronic Technology, University of Science and Technology of China, Hefei, Anhui 230026

    2013-12-28

    The equilibrium geometric structures, relative stabilities, and electronic properties of Au{sub n}C{sup ?} and Au{sub n+1}{sup ?} (n = 1–10) clusters are systematically investigated using density functional theory with hyper-generalized gradient approximation. The optimized geometries show that one Au atom capped on Au{sub n?1}C{sup ?} clusters is a dominant growth pattern for Au{sub n}C{sup ?} clusters. In contrast to Au{sub n+1}{sup ?} clusters, Au{sub n}C{sup ?} clusters are most stable in a quasi-planar or three-dimensional structure because C doping induces the local non-planarity while the rest of the structure continues to grow in a planar mode, resulting in an overall non-2D configuration. The relative stability calculations show that the impurity C atom can significantly enhance the thermodynamic stability of pure gold clusters. Moreover, the effect of C atom on the Au{sub n}{sup ?} host decreases with the increase of cluster size. The HOMO-LUMO gap curves show that the interaction of the C atom with Au{sub n}{sup ?} clusters improves the chemical stability of pure gold clusters, except for Au{sub 3}{sup ?} and Au{sub 4}{sup ?} clusters. In addition, a natural population analysis shows that the charges in corresponding Au{sub n}C{sup ?} clusters transfer from the Au{sub n}{sup ?} host to the C atom. Meanwhile, a natural electronic configuration analysis also shows that the charges mainly transfer between the 2s and 2p orbitals within the C atom.

  20. Microscopic study of low-lying spectra of $?$ hypernuclei based on a beyond-mean-field approach with covariant energy density functional

    E-Print Network [OSTI]

    H. Mei; K. Hagino; J. M. Yao; T. Motoba

    2015-04-20

    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.

  1. Ni(NiO)/single-walled carbon nanotubes composite: Synthesis of electro-deposition, gas sensing property for NO gas and density functional theory calculation

    SciTech Connect (OSTI)

    Li, Li; Zhang, Guo; Chen, Lei; Bi, Hong-Mei; Shi, Ke-Ying

    2013-02-15

    Graphical abstract: The Ni(NiO)/semiconducting single-walled carbon nanotubes composite collected from the cathode after electro-deposition shows a high sensitivity to low-concentration NO gas at room temperature (18 °C). Display Omitted Highlights: ? Ni(NiO) nanoparticles were deposited on semiconducting SWCNTs by electro-deposition. ? Ni(NiO)/semiconducting SWCNTs film shows a high sensitivity to NO gas at 18 °C. ?Theoretical calculation reveals electron transfer from SWCNTs to NO via Ni. -- Abstract: Single-walled carbon nanotubes which contains metallic SWCNTs (m-SWCNTs) and semiconducting SWCNTs (s-SWCNTs) have been obtained under electric arc discharge. Their separation can be effectively achieved by the electro-deposition method. The Ni(NiO)/s-SWCNTs composite was found on cathode where Ni was partially oxidized to NiO at ambient condition with Ni(NiO) nanoparticles deposited uniformly on the bundles of SWCNTs. These results were confirmed by Raman spectra, transmission electron microscopy (TEM), scanning electron microscopy (SEM), UV–vis–NIR and TG characterizations. Furthermore, investigation of the gas sensing property of Ni(NiO)/s-SWCNTs composite film to NO gas at 18 °C demonstrated the sensitivity was approximately 5% at the concentration of 97 ppb. Moreover, density functional theory (DFT) calculations were performed to explore the sensing mechanism which suggested the adsorption of NO molecules onto the composite through N–Ni interaction as well as the proposition of electron transfer mechanisms from SWCNTs to NO via the Ni medium.

  2. C h d Heterogeneity of A d h h Deficiency Lucia Morandi, MD,* Rita Barresi, PhD,* Claudia Di Blasi, PhD,* Daniel Jung, PhD,?

    E-Print Network [OSTI]

    Campbell, Kevin P.

    ,* Renato Mantegazza, MD,* Carlo Antozzi, MD,* Laura Jarre, MD,$ Antonella Pini, MD,S Giuseppe Gobbi, MD, Mantegazza R, Antozzi C, Jarre L, Pini A, Gobbi G, Bianchi C, Cornelio F, Campbell KP, Mora M. Clinical

  3. Microscopic dynamical description of proton-induced fission with the Constrained Molecular Dynamics (CoMD) Model

    E-Print Network [OSTI]

    N. Vonta; G. A. Souliotis; M. Veselsky; A. Bonasera

    2015-06-16

    The microscopic description of nuclear fission still remains a topic of intense basic research. Un- derstanding nuclear fission, apart from a theoretical point of view, is of practical importance for energy production and the transmutation of nuclear waste. In nuclear astrophysics, fission sets the upper limit to the nucleosynthesis of heavy elements via the r-process. In this work we initiated a systematic study of intermediate energy proton-induced fission using the Constrained Molecu- lar Dynamics (CoMD) code. The CoMD code implements an effective interaction with a nuclear matter compressibility of K=200 (soft EOS) with several forms of the density dependence of the nucleon-nucleon symmetry potential. Moreover, a constraint is imposed in the phase-space occu- pation for each nucleon restoring the Pauli principle at each time step of the collision. A proper choice of the surface parameter of the effective interaction has been made to describe fission. In this work, we present results of fission calculations for proton-induced reactions on : a) 232 Th at 27 and 63 MeV, b) 235 U at 10, 30, 60 and 100 MeV, and c) 238 U at 100 and 660 MeV. The calculated observables include fission-fragment mass distributions, total fission energies, neutron multiplicities and fission times. These observables are compared to available experimental data. We show that the microscopic CoMD code is able to describe the complicated many-body dynamics of the fission process at intermediate and high energy and give a reasonable estimate of the fission time scale. Sensitivity of the results to the density dependence of the nucleon symmetry potential (and, thus, the nuclear symmetry energy) is found. Further improvements of the code are necessary to achieve a satisfactory description of low energy fission in which shell effects play a dominant role.

  4. Charge density wave in hydrogen at high pressure

    E-Print Network [OSTI]

    Magdau, Ioan B

    2015-01-01

    We present extensive molecular dynamics (MD) simulations investigating numerous candidate crystal structures for hydrogen in conditions around the present experimental frontier (400GPa). Spontaneous phase transitions in the simulations reveal a new structure candidate comprising twofold coordinated chains of hydrogen atoms. We explain the electronic structure of this phase in terms of a charge density wave and calculate its experimental signature. In detailed tests of the accuracy of our calculation, we find that k-point sampling is far more important in MD than in static calculations, because of the freedom it give the atoms to rearrange themselves optimally for the given sampling.

  5. A method to predict the soil susceptibility to compaction of surface layers as a function of water content and bulk density

    E-Print Network [OSTI]

    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

  6. Covalency Trends in Group IV Metallocene Dichlorides. Chlorine K-Edge X-Ray Absorption Spectroscopy And Time Dependent-Density Functional Theory

    SciTech Connect (OSTI)

    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.

    2009-05-20

    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.

  7. VOLUME 79, NUMBER 20 P H Y S I C A L R E V I E W L E T T E R S 17 NOVEMBER 1997 Sparsity of the Density Matrix in Kohn-Sham Density Functional Theory

    E-Print Network [OSTI]

    Baer, Roi

    energy and Car-Parrinello approaches [1,2]. These methods are, however, capable of dealing with a limited functional theory (DFT) of the many-electron ground state energy has served as a basis for numerous large to contribute to these efforts by introducing a new analytical method to derive estimates for the range

  8. Microscopic dynamical description of proton-induced fission with the Constrained Molecular Dynamics (CoMD) Model

    E-Print Network [OSTI]

    Vonta, N; Veselsky, M; Bonasera, A

    2015-01-01

    The microscopic description of nuclear fission still remains a topic of intense basic research. Un- derstanding nuclear fission, apart from a theoretical point of view, is of practical importance for energy production and the transmutation of nuclear waste. In nuclear astrophysics, fission sets the upper limit to the nucleosynthesis of heavy elements via the r-process. In this work we initiated a systematic study of intermediate energy proton-induced fission using the Constrained Molecu- lar Dynamics (CoMD) code. The CoMD code implements an effective interaction with a nuclear matter compressibility of K=200 (soft EOS) with several forms of the density dependence of the nucleon-nucleon symmetry potential. Moreover, a constraint is imposed in the phase-space occu- pation for each nucleon restoring the Pauli principle at each time step of the collision. A proper choice of the surface parameter of the effective interaction has been made to describe fission. In this work, we present results of fission calculation...

  9. Local density functional calculations of the electronic structures of the intermetallic systems U{sub 2}Fe{sub 2}Sn and UFe{sub 2}Ge{sub 2}

    SciTech Connect (OSTI)

    Matar, S.F.; Chevalier, B.; Etourneau, J.; Eyert, V.

    1997-02-05

    The electronic structures of U{sub 2}Fe{sub 2}Sn and UFe{sub 2}Ge{sub 2} are self-consistently calculated within the local density functional theory using the augmented spherical wave (ASW) method. Calculations are scalar relativistic. The experimentally observed Pauli paramagnetic behavior of the two systems is accounted for and the influence of hybridization between the different l-states on the chemical bonding is discussed from the site-projected densities of states (DOS) as well as from the modulation of the DOS by the sign and magnitude of the overlap integral, i.e., with the so-called COOP. From this, we propose a mechanism for the evolution of bonding within the series to which the two compounds belong. 12 refs., 3 figs.

  10. Convergent sum of gradient expansion of the kinetic-energy density functional up to the sixth order term using Pade approximant

    E-Print Network [OSTI]

    A. Sergeev; R. Jovanovic; S. Kais; F. H. Alharbi

    2015-08-27

    The gradient expansion of the kinetic energy functional, when applied for atoms or finite systems, usually grossly overestimates the energy in the fourth order and generally diverges in the sixth order. We avoid the divergence of the integral by replacing the asymptotic series including the sixth order term in the integrand by a rational function. Pade approximants show moderate improvements in accuracy in comparison with partial sums of the series. The results are discussed for atoms and Hooke law model for two electron atoms.

  11. Mineral density volume gradients in normal and diseased human tissues

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

    Djomehri, Sabra I.; Candell, Susan; Case, Thomas; Browning, Alyssa; Marshall, Grayson W.; Yun, Wenbing; Lau, S. H.; Webb, Samuel; Ho, Sunita P.; Aikawa, Elena

    2015-04-09

    Clinical computed tomography provides a single mineral density (MD) value for heterogeneous calcified tissues containing early and late stage pathologic formations. The novel aspect of this study is that, it extends current quantitative methods of mapping mineral density gradients to three dimensions, discretizes early and late mineralized stages, identifies elemental distribution in discretized volumes, and correlates measured MD with respective calcium (Ca) to phosphorus (P) and Ca to zinc (Zn) elemental ratios. To accomplish this, MD variations identified using polychromatic radiation from a high resolution micro-computed tomography (micro-CT) benchtop unit were correlated with elemental mapping obtained from a microprobe X-raymore »fluorescence (XRF) using synchrotron monochromatic radiation. Digital segmentation of tomograms from normal and diseased tissues (N=5 per group; 40-60 year old males) contained significant mineral density variations (enamel: 2820-3095mg/cc, bone: 570-1415mg/cc, cementum: 1240-1340mg/cc, dentin: 1480-1590mg/cc, cementum affected by periodontitis: 1100-1220mg/cc, hypomineralized carious dentin: 345-1450mg/cc, hypermineralized carious dentin: 1815-2740mg/cc, and dental calculus: 1290-1770mg/cc). A plausible linear correlation between segmented MD volumes and elemental ratios within these volumes was established, and Ca/P ratios for dentin (1.49), hypomineralized dentin (0.32-0.46), cementum (1.51), and bone (1.68) were observed. Furthermore, varying Ca/Zn ratios were distinguished in adapted compared to normal tissues, such as in bone (855-2765) and in cementum (595-990), highlighting Zn as an influential element in prompting observed adaptive properties. Hence, results provide insights on mineral density gradients with elemental concentrations and elemental footprints that in turn could aid in elucidating mechanistic processes for pathologic formations.« less

  12. An Assessment of Density Functional Methods for Potential Energy Curves of Nonbonded Interactions: The XYG3 and B97-D Approximations

    SciTech Connect (OSTI)

    Vazquez-Mayagoitia, Alvaro; Sherrill, David; Apra, Edoardo; Sumpter, Bobby G

    2010-01-01

    A recently proposed double-hybrid functional called XYG3 and a semilocal GGA functional (B97-D) with a semiempirical correction for van der Waals interactions have been applied to study the potential energy curves along the dissociation coordinates of weakly bound pairs of molecules governed by London dispersion and induced dipole forces. Molecules treated in this work were the parallel sandwich, T-shaped, and parallel-displaced benzene dimer, (C6H6)2; hydrogen sulfide and benzene, H2S C6H6; methane and benzene, CH4 C6H6; the methane dimer, (CH4)2; and the pyridine dimer, (C5H5N)2. We compared the potential energy curves of these functionals with previously published benchmarks at the coupled cluster singles, doubles, and perturbative triplets [CCSD(T)] complete-basis-set limit. Both functionals, XYG3 and B97-D, exhibited very good performance, reproducing accurate energies for equilibrium distances and a smooth behavior along the dissociation coordinate. Overall, we found an agreement within a few tenths of one kcal mol-1 with the CCSD(T) results across the potential energy curves.

  13. LDRD Final Report (08-ERD-037): Important Modes to Drive Protein MD Simulations to the Next Conformational Level

    SciTech Connect (OSTI)

    Sadigh, B

    2011-04-07

    Every action in biology is performed by dynamic proteins that convert between multiple states in order to engage their functions. Often binding to various ligands is essential for the rates of desired transitions to be enhanced. The goal of computational biology is to study these transitions and discover the different states to fully understand the protein's normal and diseased function, design drugs to target/bias specific states, and understand all of the interactions in between. We have developed a new methodology that is capable of calculating the absolute free energy of proteins while taking into account all the interactions with the solvent molecules. The efficiency of the new scheme is an order of magnitude greater than any existing technique. This method is now implemented in the massively parallel popular MD program package NAMD. This now makes it possible to calculate the relative stability of different conformational states of biological macromolecules as well as their binding free energies to various ligands.

  14. Vehicle Technologies Office Merit Review 2014: Cummins MD & HD Accessory Hybridization CRADA

    Broader source: Energy.gov [DOE]

    Presentation given by Oak Ridge National Laboratory at 2014 DOE Hydrogen and Fuel Cells Program and Vehicle Technologies Office Annual Merit Review and Peer Evaluation Meeting about Cummins MD &...

  15. Vehicle Technologies Office Merit Review 2015: Cummins MD & HD Accessory Hybridization CRADA

    Office of Energy Efficiency and Renewable Energy (EERE)

    Presentation given by Oak Ridge National Laboratory at 2015 DOE Hydrogen and Fuel Cells Program and Vehicle Technologies Office Annual Merit Review and Peer Evaluation Meeting about Cummins MD &...

  16. Catharine Whiteside, MD PhD Vice Provost, Relations with Health Care Institutions

    E-Print Network [OSTI]

    Zandstra, Peter W.

    Catharine Whiteside, MD PhD Dean Vice Provost, Relations with Health Care Institutions Office. Professor Andrews received her PhD from the University of Toronto and completed further training

  17. Julie Gralow, MD Director Breast Medical Oncology, Seattle Cancer Care Alliance

    E-Print Network [OSTI]

    Brent, Roger

    Julie Gralow, MD Director Breast Medical Oncology, Seattle Cancer Care Alliance Founder Care Alliance, as well as a Member of the Clinical Research Division of the Fred Hutchinson Cancer

  18. Automatic Search of Differential Path in MD4 Pierre-Alain Fouque, Gatan Leurent, Phong Nguyen

    E-Print Network [OSTI]

    International Association for Cryptologic Research (IACR)

    Automatic Search of Differential Path in MD4 Pierre-Alain Fouque, Gaëtan Leurent, Phong Nguyen paths were found "by hand". In this paper, we present an algorithm which automatically finds suitable

  19. A career in bioengineering Christopher Chen, MD '99, PhD (MEMP '97) is the Skirkanich

    E-Print Network [OSTI]

    Gabrieli, John

    A career in bioengineering Christopher Chen, MD '99, PhD (MEMP '97) is the Skirkanich Professor of Innovation in Bioengineering at the University of Pennsylvania, where he directs the Tissue Microfabrication

  20. Density hysteresis of heavy water confined in a nanoporous silica matrix

    E-Print Network [OSTI]

    Chen, Sow-Hsin

    of Technology, Cambridge, MA 02139; b Neutron Scattering Science Division and Joint Institute for Neutron (received for review January 5, 2011) A neutron scattering technique was developed to measure the density and Technology Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, MD

  1. Maximum-likelihood density modification

    SciTech Connect (OSTI)

    Terwilliger, Thomas C., E-mail: terwilliger@lanl.gov [Structural Biology Group, Mail Stop M888, Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)

    2000-08-01

    A likelihood-based density modification approach is developed that can incorporate expected electron-density information from a wide variety of sources. A likelihood-based approach to density modification is developed that can be applied to a wide variety of cases where some information about the electron density at various points in the unit cell is available. The key to the approach consists of developing likelihood functions that represent the probability that a particular value of electron density is consistent with prior expectations for the electron density at that point in the unit cell. These likelihood functions are then combined with likelihood functions based on experimental observations and with others containing any prior knowledge about structure factors to form a combined likelihood function for each structure factor. A simple and general approach to maximizing the combined likelihood function is developed. It is found that this likelihood-based approach yields greater phase improvement in model and real test cases than either conventional solvent flattening and histogram matching or a recent reciprocal-space solvent-flattening procedure [Terwilliger (1999 ?), Acta Cryst. D55, 1863–1871].

  2. ESTIMATION OF DENSITIES AND FUNCTIONALS OF DENSITIES WITH

    E-Print Network [OSTI]

    Klemelä, Jussi

    ¨akel¨ainen for introducing me to the statis- tics of directional data. The Rolf Nevanlinna Institute and the Department of Statis- tics of the University of Helsinki have provided me with excellent working conditions

  3. Form: REG113 2007 University of Maryland, Baltimore County 1000 Hilltop Circle, Baltimore, MD 21250 410-455-2500 Questions? Email: records@umbc.edu

    E-Print Network [OSTI]

    Suri, Manil

    __________________________________________________________________________________________________________________________________ © 2007 University of Maryland, Baltimore County · 1000 Hilltop Circle, Baltimore, MD 21250 · 410

  4. Form: REG112 2007 University of Maryland, Baltimore County 1000 Hilltop Circle, Baltimore, MD 21250 410-455-2500 Questions? Email: records@umbc.edu

    E-Print Network [OSTI]

    Suri, Manil

    __________________________________________________________________________________________________________________________________ © 2007 University of Maryland, Baltimore County · 1000 Hilltop Circle, Baltimore, MD 21250 · 410

  5. Form: REG102 2007 University of Maryland, Baltimore County 1000 Hilltop Circle, Baltimore, MD 21250 410-455-2500 Questions? Email: records@umbc.edu

    E-Print Network [OSTI]

    Suri, Manil

    __________________________________________________________________________________________________________________________________ © 2007 University of Maryland, Baltimore County · 1000 Hilltop Circle, Baltimore, MD 21250 · 410

  6. 2007 University of Maryland, Baltimore County 1000 Hilltop Circle, Baltimore, MD 21250 410-455-2500 Questions? Email: records@umbc.edu OFFICE OF THE REGISTRAR

    E-Print Network [OSTI]

    Suri, Manil

    University of Maryland, Baltimore County 1000 Hilltop Circle, Baltimore, MD 21250 410-455-2500 Questions

  7. The galaxy UV luminosity function at z ~ 2 - 4; new results on faint-end slope and the evolution of luminosity density

    E-Print Network [OSTI]

    Parsa, Shaghayegh; McLure, Ross J; Mortlock, Alice

    2015-01-01

    We present a new, robust measurement of the evolving rest-frame UV galaxy luminosity function (LF) over the key redshift range z = 2 - 4. Our results are based on the high dynamic range provided by combining the HUDF, CANDELS/GOODS-South, and UltraVISTA/COSMOS surveys. We utilise the unparalleled multi-frequency photometry available in this survey `wedding cake' to compile complete galaxy samples at z ~ 2,3,4 via photometric redshifts (calibrated against the latest spectroscopy) rather than colour-colour selection, and to determine accurate rest-frame UV absolute magnitudes from SED fitting. Our new determinations of the UV LF extend from M_{1500} ~ -22 down to M_{1500} = -14.5, -15.5 and -16 at z ~ 2, 3 and 4 respectively (thus reaching ~ 3 - 4 magnitudes fainter than previous blank-field studies at z ~ 2 - 3). At z ~ 2 - 3 we find a much shallower faint-end slope (alpha = -1.32 +- 0.03) than the steeper values (alpha ~ -1.7) reported by Reddy & Steidel (2009) or by Alavi et al. (2014), and show that thi...

  8. Electronic and thermoelectric properties of Ce{sub 3}Te{sub 4} and La{sub 3}Te{sub 4} computed with density functional theory with on-site Coulomb interaction correction

    SciTech Connect (OSTI)

    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)

    2014-10-07

    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.

  9. Restoring the Differential Resistance of MD6 Ethan Heilman

    E-Print Network [OSTI]

    International Association for Cryptologic Research (IACR)

    the greatest performance cost, find a trade-off that greatly reduces this performance cost for those elements-trivial patterns represent a such significant performance cost. We reduce the perfor- mance cost of non. The feedback function starts at index i = 89 (The words A[0] through A[88] contain the message which is being

  10. Building a Universal Nuclear Energy Density Functional

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity ofkandz-cm11 Outreach Home Room News PublicationsAudits &Bradbury Science Museum -BrooklinSecurityBetter BatteryBuilding a

  11. HIV-1 Tat membrane interactions probed using X-ray and neutron scattering, CD spectroscopy and MD simulations

    E-Print Network [OSTI]

    Nagle, John F.

    HIV-1 Tat membrane interactions probed using X-ray and neutron scattering, CD spectroscopy and MD translocation, were provided by wide-angle X-ray scattering (WAXS) and neutron scattering. CD spectroscopy for Neutron Research, 100 Bureau Drive, Stop 6102, Gaithersburg, MD 20899, United States d CHESS, Cornell

  12. iPad: Semantic Annotation and Markup of Radiological Images Daniel L. Rubin, MS, MD,*1,2

    E-Print Network [OSTI]

    Rubin, Daniel L.

    image content in a standard machine-interpretable format. A tool permitting researchers to describe Rodriguez, MD,1 Priyanka Shah,3 and Chris Beaulieu, MD, PhD2 1 Center for Biomedical Informatics Research, 2 trials. Thus, much critical radiological image information is not directly accessible to machines, unlike

  13. Enhancing the MD-Strengthening and Designing Scalable Families of One-Way Hash Algorithms

    E-Print Network [OSTI]

    International Association for Cryptologic Research (IACR)

    Enhancing the MD-Strengthening and Designing Scalable Families of One-Way Hash Algorithms Neil Kauer Tony Suarez Yuliang Zheng November 1, 2005 Abstract One-way hash algorithms are an indispensable tool in data security. Over the last decade or so a number of one-way hash algorithms have been

  14. Ira Helfand, MD International Physicians for the Prevention of Nuclear War

    E-Print Network [OSTI]

    Robock, Alan

    the urgent need to move with all possible speed to the negotiation of a nuclear weapons conventionIra Helfand, MD International Physicians for the Prevention of Nuclear War Physicians for Social Responsibility NUCLEAR FAMINE: A BILLION PEOPLE AT RISK Global Impacts of Limited Nuclear War on Agriculture

  15. Adaptive Regression Testing Strategy: An Empirical Study Md. Junaid Arafeen and Hyunsook Do

    E-Print Network [OSTI]

    Do, Hyunsook

    Adaptive Regression Testing Strategy: An Empirical Study Md. Junaid Arafeen and Hyunsook Do in different versions. These factors can affect the costs and benefits of regression testing techniques in different ways, and thus, there may be no single regression testing technique that is the most cost

  16. CityBizList US Green Building Council -MD Celebrating Move to

    E-Print Network [OSTI]

    design movement. Schilling Green, a 106,208-square-foot, three-story, Class A office building, obtainedCityBizList US Green Building Council - MD Celebrating Move to Hunt Valley Share Email this Article Baltimore County Executive Jim Smith will join the U.S. Green Building Council Maryland to celebrate

  17. February 16, 2008 Connecting renewal age processes and M/D/1

    E-Print Network [OSTI]

    a connection between each of these models through the first hitting time of the renewal age process. FurtherFebruary 16, 2008 Connecting renewal age processes and M/D/1 processor sharing queues through stick breaking J.S.H. van Leeuwaarden1 A.H. L¨opker2 A.J.E.M. Janssen3 Abstract: The renewal age process

  18. Hot Water DJ: Saving Energy by Pre-mixing Hot Water Md Anindya Prodhan

    E-Print Network [OSTI]

    Whitehouse, Kamin

    Hot Water DJ: Saving Energy by Pre-mixing Hot Water Md Anindya Prodhan Department of Computer University of Virginia whitehouse@virginia.edu Abstract After space heating and cooling, water heating consumption. Current water heating systems waste up to 20% of their energy due to poor insulation in pipes

  19. Water adsorption on stepped ZnO surfaces from MD simulation David Raymand a

    E-Print Network [OSTI]

    Goddard III, William A.

    Water adsorption on stepped ZnO surfaces from MD simulation David Raymand a , Adri C.T. van Duin b Keywords: Zinc oxide Water Solid­gas interfaces Construction and use of effective interatomic interactions force-field for use in molecular dynamics simulations of the ZnO­ water system. The force

  20. A survey on vehicular cloud computing Md Whaiduzzaman a,n

    E-Print Network [OSTI]

    Buyya, Rajkumar

    A survey on vehicular cloud computing Md Whaiduzzaman a,n , Mehdi Sookhak a , Abdullah Gani a , Rajkumar Buyya b a Mobile Cloud Computing Research Lab, Faculty of Computer Science & Information control Intelligent transportation systems Cloud computing Vehicular cloud computing a b s t r a c

  1. July 7-10, 2015 National Institute of Standards and Technology Gaithersburg, MD

    E-Print Network [OSTI]

    requirements, which cover cloud security, cloud services, technical language for SLAs, cloud metrics breaches, or to proactively support security and forensics cloud-based applications. In June, 2014 NISTJuly 7-10, 2015 National Institute of Standards and Technology Gaithersburg, MD NIST Cloud

  2. A Word from the Director Frank S. Pidcock, MD, Vice President of Rehabilitation at Kennedy Krieger

    E-Print Network [OSTI]

    Pevsner, Jonathan

    A Word from the Director Frank S. Pidcock, MD, Vice President of Rehabilitation at Kennedy Krieger Institute, Director of the Pediatric Rehabilitation Division in the Department of Physical Medicine & Rehabilitation, Johns Hopkins Hospital In this issue of Neurorehabilitation Updates, we explore disorders

  3. A Word from the Director Frank S. Pidcock, MD, Vice President of Rehabilitation at Kennedy Krieger

    E-Print Network [OSTI]

    Pevsner, Jonathan

    A Word from the Director Frank S. Pidcock, MD, Vice President of Rehabilitation at Kennedy Krieger Institute, Director of the Pediatric Rehabilitation Division in the Department of Physical Medicine & Rehabilitation, Johns Hopkins Hospital Kennedy Krieger Institute provides a wide range of services for patients

  4. Membrane association of the PTEN tumor suppressor: Neutron scattering and MD simulations reveal the structure

    E-Print Network [OSTI]

    Loesche, Mathias

    Membrane association of the PTEN tumor suppressor: Neutron scattering and MD simulations reveal Engineering, Carnegie Mellon University, Pittsburgh, PA 15213, USA c NIST Center for Neutron Research Phosphatidylserine Neutron reflection Tethered bilayer lipid membranes Molecular dynamics simulations a b s t r a c

  5. Cost Analysis of NEMO Protocol Entities Md. Shohrab Hossain, Mohammed Atiquzzaman, William Ivancic

    E-Print Network [OSTI]

    Atiquzzaman, Mohammed

    Cost Analysis of NEMO Protocol Entities Md. Shohrab Hossain, Mohammed Atiquzzaman, William Ivancic to ensure connectivity of the mobile nodes with the Internet. However, there has been no comprehensive cost analysis of mobility protocol entities that considers all possible costs. In this paper, we have developed

  6. Cost Analysis of Mobility Management Entities of Md. Shohrab Hossain, Mohammed Atiquzzaman

    E-Print Network [OSTI]

    Atiquzzaman, Mohammed

    Cost Analysis of Mobility Management Entities of SINEMO Md. Shohrab Hossain, Mohammed Atiquzzaman results in higher level of signalling cost on the mobility agents in a mobility protocol. Previous cost analysis on mobility protocols have not considered all possible costs for mobility management, resulting

  7. On Tackling Virtual Data Center Embedding Md Golam Rabbani, Rafael Pereira Esteves, Maxim Podlesny, Gwendal Simon

    E-Print Network [OSTI]

    Boutaba, Raouf

    On Tackling Virtual Data Center Embedding Problem Md Golam Rabbani, Rafael Pereira Esteves, Maxim (POSTECH), Pohang 790-784, Korea Abstract--Virtualizing data center networks has been con- sidered center (VDC) resources to their physical counterparts, also known as virtual data center embedding, can

  8. On Tackling Virtual Data Center Embedding Md Golam Rabbani, Rafael Esteves, Maxim Podlesny, Gwendal Simon

    E-Print Network [OSTI]

    Paris-Sud XI, Université de

    On Tackling Virtual Data Center Embedding Problem Md Golam Rabbani, Rafael Esteves, Maxim Podlesny Telecom Bretagne, Institut Mines Telecom, France Abstract--Virtualizing data center networks has been con of virtual data center (VDC) resources to their physical counterparts, also known as virtual data center

  9. Intraoperative Electrochemotherapy of Colorectal Liver Metastases IBRAHIM EDHEMOVIC, MD, MSc,1

    E-Print Network [OSTI]

    Ljubljana, University of

    MALI, PhD,3 TOMAZ JARM, PhD,3 BOR KOS, PhD,3 DENIS PAVLIHA, PhD,3 BILJANA GRCAR KUZMANOV, MD, PhD,1 Ljubljana, Ljubljana, Slovenia 3 Department of Biomedical Engineering, Faculty of Electrical Engineering

  10. Advanced age remains an Achilles heel for liver resections. Laurent Sulpice, MD1,3

    E-Print Network [OSTI]

    Paris-Sud XI, Université de

    and Karim Boudjema, MD, PhD1,3 1- Service de Chirurgie Hépatobiliaire et Digestive. Centre Hospitalier, Centre Hospitalier Universitaire, Université de Rennes 1, Rennes, France Email : laurent in surgical techniques, perioperative management and postoperative care, LR has become increasingly common

  11. Body Pose based Pedestrian Tracking in a Particle Filtering Framework Md. Junaedur Rahman1

    E-Print Network [OSTI]

    Nebel, Jean-Christophe

    Body Pose based Pedestrian Tracking in a Particle Filtering Framework Md. Junaedur Rahman1 , Jesus.makris}@kingston.ac.uk ] Abstract A novel body pose based human tracking model is proposed for pedestrian tracking. This work investigates the challenges of reliable pedestrian tracking and pro- poses an improved model under challenging

  12. Faculty of Medicine, Primary Care and Population Sciences PhD/MD students Name Title Email

    E-Print Network [OSTI]

    Molinari, Marc

    Faculty of Medicine, Primary Care and Population Sciences ­ PhD/MD students Name Title Email Primary Supervisor in Faculty of Medicine, PCPS Professor Paul Roderick Sara Afshar Multimorbidities: its14@soton.ac.uk Primary Supervisor in Faculty of Medicine, PCPS Dr Julie Parkes Emma Richards

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

    E-Print Network [OSTI]

    Truong, Thanh N.

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

  14. Mar. Drugs 2015, 13, 3154-3181; doi:10.3390/md13053154 marine drugs

    E-Print Network [OSTI]

    Paré, Paul W.

    Mar. Drugs 2015, 13, 3154-3181; doi:10.3390/md13053154 marine drugs ISSN 1660-3397 www.mdpi.com/journal/marinedrugs Review Molecular Architecture and Biomedical Leads of Terpenes from Red Sea Marine Invertebrates Mohamed Costantino Received: 9 April 2015 / Accepted: 7 May 2015 / Published: 20 May 2015 Abstract: Marine

  15. Mar. Drugs 2013, 11, 4370-4389; doi:10.3390/md11114370 marine drugs

    E-Print Network [OSTI]

    Eirin Lopez, Jose Maria

    Mar. Drugs 2013, 11, 4370-4389; doi:10.3390/md11114370 marine drugs ISSN 1660-3397 www.mdpi.com/journal/marinedrugs Review Bivalve Omics: State of the Art and Potential Applications for the Biomonitoring of Harmful Marine of the marine ecosystem, constitute very valuable commercial resources in aquaculture, and have been widely used

  16. Updated February 2015 UMBC 1000 Hilltop Circle, Baltimore, MD 21250 410-455-2729 Questions? Email: arc@umbc.edu Student Information (Please print)

    E-Print Network [OSTI]

    Suri, Manil

    Updated February 2015 UMBC · 1000 Hilltop Circle, Baltimore, MD 21250 · 410-455-2729 Questions IN EXCESS CREDITS #12;Updated February 2015 UMBC · 1000 Hilltop Circle, Baltimore, MD 21250 · 410

  17. To be presented in the 2005 American Society for Photogrammetry & Remote Sensing, (ASPRS) Annual Conference March 7-11, 2005, Baltimore, MD

    E-Print Network [OSTI]

    Plaza, Antonio J.

    Conference March 7-11, 2005, Baltimore, MD 1 DESIGN OF FAST ALGORITHMS FOR PIXEL PURITY INDEX FOR ENDMEMBER Engineering University of Maryland, Baltimore County, Baltimore, MD 21250 2 Computer Science Department

  18. Dynamics study of the reaction OH{sup -}+C{sub 2}H{sub 2}{yields}C{sub 2}H{sup -}+H{sub 2}O with crossed beams and density-functional theory calculations

    SciTech Connect (OSTI)

    Liu Li; Li Yue; Farrar, James M. [Department of Chemistry, University of Rochester, Rochester, New York 14627 (United States)

    2006-03-28

    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.

  19. The bonding, charge distribution, spin ordering, optical, and elastic properties of four MAX phases Cr{sub 2}AX (A?=?Al or Ge, X?=?C or N): From density functional theory study

    SciTech Connect (OSTI)

    Li, Neng; Mo, Yuxiang; Ching, Wai-Yim

    2013-11-14

    In this work, we assess a full spectrum of properties (chemical bonding, charge distribution, spin ordering, optical, and elastic properties) of Cr{sub 2}AC (A?=?Al, Ge) and their hypothetical nitride counterparts Cr{sub 2}AN (A?=?Al, Ge) based on density functional theory calculations. The calculated total energy values indicate that a variety of spin ordering of these four compounds depending on interlayer-interactions between M-A and M-X within the sublattice, which is supported by bonding analysis. MAX phase materials are discovered to possess exotic magnetic properties which indicates that these materials could serve as promising candidates for novel layered magnetic materials for various electronic and spintronic applications. Further analysis of optical properties for two polarization vectors of Cr{sub 2}AX shows that the reflectivity is high in the visible-ultraviolet region up to ?15?eV suggesting Cr{sub 2}AX as a promising candidate for use as a coating material. The elastic coefficients (C{sub ij}) and bulk mechanical properties [bulk modulus (K), shear modulus (G), Young's modulus (E), Poisson's ratio (?), and Pugh ratio (G/K)] of these four Cr{sub 2}AX compounds are also calculated and analyzed, which pave the way to predict or design new MAX phases that are less brittle or tougher by having a lower G/K value or higher ?.

  20. A density functional tight binding/force field approach to the interaction of molecules with rare gas clusters: Application to (C{sub 6}H{sub 6}){sup +/0}Ar{sub n} clusters

    SciTech Connect (OSTI)

    Iftner, Christophe; Simon, Aude; Korchagina, Kseniia; Rapacioli, Mathias; Spiegelman, Fernand

    2014-01-21

    We propose in the present paper a SCC-DFTB/FF (Self-Consistent-Charge Density Functional based Tight Binding/Force-Field) scheme adapted to the investigation of molecules trapped in rare gas environments. With respect to usual FF descriptions, the model involves the interaction of quantum electrons in a molecule with rare gas atoms in an anisotropic scheme. It includes polarization and dispersion contributions and can be used for both neutral and charged species. Parameters for this model are determined for hydrocarbon-argon complexes and the model is validated for small hydrocarbons. With the future aim of studying polycyclic aromatic hydrocarbons in Ar matrices, extensive benchmark calculations are performed on (C{sub 6}H{sub 6}){sup +/0}Ar{sub n} clusters against DFT and CCSD(T) calculations for the smaller sizes, and more generally against other experimental and theoretical data. Results on the structures and energetics (isomer ordering and energy separation, cohesion energy per Ar atom) are presented in detail for n = 1–8, 13, 20, 27, and 30, for both neutrals and cations. We confirm that the clustering of Ar atoms leads to a monotonous decrease of the ionization potential of benzene for n ? 20, in line with previous experimental and FF data.