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Sample records for polarized density functional

  1. Current density functional theory for optical spectra : A polarization functional

    NARCIS (Netherlands)

    Boeij, P.L. de; Kootstra, F.; Berger, J.A.; Leeuwen, R. van; Snijders, J.G.

    2001-01-01

    In this paper we present a new approach to calculate optical spectra, which for the first time uses a polarization dependent functional within current density functional theory (CDFT), which was proposed by Vignale and Kohn. This polarization dependent functional includes exchange-correlation (xc)

  2. Molecular density functional theory of water including density-polarization coupling.

    Science.gov (United States)

    Jeanmairet, Guillaume; Levy, Nicolas; Levesque, Maximilien; Borgis, Daniel

    2016-06-22

    We present a three-dimensional molecular density functional theory of water derived from first-principles that relies on the particle's density and multipolar polarization density and includes the density-polarization coupling. This brings two main benefits: (i) scalar density and vectorial multipolar polarization density fields are much more tractable and give more physical insight than the full position and orientation densities, and (ii) it includes the full density-polarization coupling of water, that is known to be non-vanishing but has never been taken into account. Furthermore, the theory requires only the partial charge distribution of a water molecule and three measurable bulk properties, namely the structure factor and the Fourier components of the longitudinal and transverse dielectric susceptibilities.

  3. Molecular density functional theory of water including density–polarization coupling

    OpenAIRE

    Jeanmairet, Guillaume; Lévy, Nicolas; Levesque, Maximilien; Borgis, Daniel

    2016-01-01

    International audience; We present a three-dimensional molecular density functional theory of water derived fromfirst-principles that relies on the particle’s density and multipolar polarization density andincludes the density–polarization coupling. This brings two main benefits: (i) scalar densityand vectorial multipolar polarization density fields are much more tractable and give morephysical insight than the full position and orientation densities, and (ii) it includes the fulldensity–pola...

  4. Nuclear reactivity indices in the context of spin polarized density functional theory

    International Nuclear Information System (INIS)

    Cardenas, Carlos; Lamsabhi, Al Mokhtar; Fuentealba, Patricio

    2006-01-01

    In this work, the nuclear reactivity indices of density functional theory have been generalized to the spin polarized case and their relationship to electron spin polarized indices has been established. In particular, the spin polarized version of the nuclear Fukui function has been proposed and a finite difference approximation has been used to evaluate it. Applications to a series of triatomic molecules demonstrate the ability of the new functions to predict the geometrical changes due to a change in the spin multiplicity. The main equations in the different ensembles have also been presented

  5. Generalized nuclear Fukui functions in the framework of spin-polarized density-functional theory

    International Nuclear Information System (INIS)

    Chamorro, E.; Proft, F. de; Geerlings, P.

    2005-01-01

    An extension of Cohen's nuclear Fukui function is presented in the spin-polarized framework of density-functional theory (SP-DFT). The resulting new nuclear Fukui function indices Φ Nα and Φ Sα are intended to be the natural descriptors for the responses of the nuclei to changes involving charge transfer at constant multiplicity and also the spin polarization at constant number of electrons. These generalized quantities allow us to gain new insights within a perturbative scheme based on DFT. Calculations of the electronic and nuclear SP-DFT quantities are presented within a Kohn-Sham framework of chemical reactivity for a sample of molecules, including H 2 O, H 2 CO, and some simple nitrenes (NX) and phosphinidenes (PX), with X=H, Li, F, Cl, OH, SH, NH 2 , and PH 2 . Results have been interpreted in terms of chemical bonding in the context of Berlin's theorem, which provides a separation of the molecular space into binding and antibinding regions

  6. Hardness and softness reactivity kernels within the spin-polarized density-functional theory

    International Nuclear Information System (INIS)

    Chamorro, Eduardo; De Proft, Frank; Geerlings, Paul

    2005-01-01

    Generalized hardness and softness reactivity kernels are defined within a spin-polarized density-functional theory (SP-DFT) conceptual framework. These quantities constitute the basis for the global, local (i.e., r-position dependent), and nonlocal (i.e., r and r ' -position dependents) indices devoted to the treatment of both charge-transfer and spin-polarization processes in such a reactivity framework. The exact relationships between these descriptors within a SP-DFT framework are derived and the implications for chemical reactivity in such context are outlined

  7. Polar-solvation classical density-functional theory for electrolyte aqueous solutions near a wall

    Science.gov (United States)

    Warshavsky, Vadim; Marucho, Marcelo

    2016-01-01

    A precise description of the structural and dielectric properties of liquid water is critical to understanding the physicochemical properties of solutes in electrolyte solutions. In this article, a mixture of ionic and dipolar hard spheres is considered to account for water crowding and polarization effects on ionic electrical double layers near a uniformly charged hard wall. As a unique feature, solvent hard spheres carrying a dipole at their centers were used to model water molecules at experimentally known concentration, molecule size, and dipolar moment. The equilibrium ionic and dipole density profiles of this electrolyte aqueous model were calculated using a polar-solvation classical density-functional theory (PSCDFT). These profiles were used to calculate the charge density distribution, water polarization, dielectric permittivity function, and mean electric potential profiles as well as differential capacitance, excess adsorptions, and wall-fluid surface tension. These results were compared with those corresponding to the pure dipolar model and unpolar primitive solvent model of electrolyte aqueous solutions to understand the role that water crowding and polarization effects play on the structural and thermodynamic properties of these systems. Overall, PSCDFT predictions are in agreement with available experimental data. PMID:27176352

  8. Polarization Dependent Bulk-sensitive Valence Band Photoemission Spectroscopy and Density Functional Theory Calculations: Part I. 3d Transition Metals

    Science.gov (United States)

    Ueda, Shigenori; Hamada, Ikutaro

    2017-12-01

    The X-ray polarization dependent valence band HAXPES spectra of 3d transition metals (TMs) of Ti-Zn were measured to investigate the orbital resolved electronic structures by utilizing that the fact the photoionization cross-section of the atomic orbitals strongly depends on the experimental geometry. We have calculated the HAXPES spectra, which correspond to the cross-section weighted densities of states (CSW-DOSs), where the DOSs were obtained by the density functional theory calculations, and we have determined the relative photoionization cross-sections of the 4s and 4p orbitals to the 3d orbital in the 3d TMs. The experimentally obtained bulk-sensitive 3d and 4s DOSs were good agreement with the calculated DOSs in Ti, V, Cr, and Cu. In contrast, the deviations between the experimental and calculated 3d DOSs for Mn, Fe, Co, Ni were found, suggesting that the electron correlation plays an important role in the electronic structures for these materials.

  9. Ab initio density functional theory study of non-polar (101¯0), (112¯0) and semipolar (202¯1) GaN surfaces

    International Nuclear Information System (INIS)

    Mutombo, P.; Romanyuk, O.

    2014-01-01

    The atomic structures of non-polar GaN(101 ¯ 0), (112 ¯ 0) and semipolar GaN(202 ¯ 1), (202 ¯ 1 ¯ ) surfaces were studied using ab initio calculations within density functional theory. The bulk-like truncated (1 × 1) structure with buckled Ga-N or Ga-Ga dimers was found stable on the non-polar GaN(101 ¯ 0) surface in agreement with previous works. Ga-N heterodimers were found energetically stable on the GaN(112 ¯ 0)-(1 × 1) surface. The formation of vacancies and substitution site defects was found unfavorable for non-polar GaN surfaces. Semipolar GaN(202 ¯ 1)-(1 × 1) surface unit cells consist of non-polar (101 ¯ 0) and semipolar (101 ¯ 1) nano-facets. The (101 ¯ 1) nano-facets consist of two-fold coordinated atoms, which form N-N dimers within a (2 × 1) surface unit cell on a GaN(202 ¯ 1) surface. Dimers are not formed on the GaN(202 ¯ 1 ¯ ) surface. The stability of the surfaces with single (101 ¯ 0) or (101 ¯ 1) nano-facets was analyzed. A single non-polar (101 ¯ 0)-(1 × 1) nano-facet was found stable on the GaN(202 ¯ 1) surface, but unstable on the GaN(202 ¯ 1 ¯ ) surface. A single (101 ¯ 1) nano-facet was found unstable. Semipolar GaN surfaces with (202 ¯ 1) and (202 ¯ 1 ¯ ) polarity can be stabilized with a Ga overlayer at Ga-rich experimental conditions.

  10. Polarization Charge Density in Strained Graphene

    Science.gov (United States)

    Wilson, Noah

    Graphene, the world's first truly two-dimensional material, is unique for having an electronic structure described by an effective Lorentz invariant theory. One important consequence is that the ratio or Coulomb energy to kinetic energy is a constant, depending only on conditions within the lattice rather than on the average charge density as in a typical Galilean invariant material. Given this unusual property, a natural question would be how do phenomena, such as screening of a Coulomb impurity, happen in graphene? Moreover, how does the addition of uniaxial strain enhance or diminish this behavior? Here I discuss our work to calculate the charge density distribution in a lattice of strained graphene under the effect of an external Coulomb impurity. Graphene can have its band structure significantly altered by the application of uniaxial strain. Two cases are here explored: relatively weak strain at some finite chemical potential, and extreme strain with zero chemical potential. In the first system, the strain induces elliptic Dirac cones, engendering some inherent directionality to graphene's electronic properties that did not exist before. This anisotropy manifests itself in the polarization function, and so too in the screening charge density. A finite chemical potential in this case is necessary for any screening to take place in graphene since, without it, there are no electron states near the Fermi level to polarize. Both in the strained and unstrained case, decaying oscillations known as Friedel oscillations are observed. The result of strain is a multifaceted anisotropy of the charge distribution: the amplitude, frequency, and the position of the first peak in the oscillations are each varied depending on the direction one observes. In the second system, extreme strain in graphene leads to a merging of Dirac cones, yielding a transition to a new energy spectrum. This band structure is unusual in that it becomes quadratic along the direction of strain

  11. Tailoring electronic structure of α-AlH3 to enhance spin polarization: Insights from density functional calculations

    Science.gov (United States)

    Lu, Yi-Lin; Dong, Shengjie; Zhou, Baozeng; Sun, Lili; Zhao, Hui; Wu, Ping

    2017-09-01

    The effects of 3d transition metals doping on the structural, electronic, and magnetic properties of aluminum hydride were investigated based on spin-polarized first-principles calculations. The studies indicated that V, Cr, Mn, and Fe doping could produce polarization of high-spin state, while Co and Ni doping would induce polarization of low-spin state. It was found that the magnetic ground state depended on the distance between two substitutions and the long-range ferromagnetic coupling was achieved upon doping V, Mn, and Fe. The present work indicated that the introduced 3d-block dopants could tailor aluminum hydride into either a potential half-metallic or n-type magnetic semiconductor by tuning the valence electrons of the impurities. The main findings of this work pointed out the possibilities of the applications of hydrides in future hydride electronics and spintronics.

  12. New Vistas on the Anionic Polymerization of Styrene in Non-Polar Solvents by Means of Density Functional Theory

    Directory of Open Access Journals (Sweden)

    Hideo Morita

    2016-10-01

    Full Text Available The elementary processes of anionic styrene polymerization in the gas phase and in cyclohexane were studied using M062X (a recently developed density functional theory (DFT method combined with the 6-31+G(d basis sets, in order to clarify the complicated phenomena caused by the association of the active chain-ends and elucidate the details of the polymerization mechanism. Three types of HSt2Li (a model structure of polystyryllithium chain-ends were obtained; the well-known first structure in which Li is coordinated to the side chain, the second structure in which Li is coordinated to the phenyl ring, (both without the penultimate unit coordination, and the third structure in which Li is coordinated to both the chain-end unit and the penultimate styrene unit. Although the third HSt2Li is the most stable as expected, the free energy for the transition state of its reaction with styrene is higher than those for the other two transition states due to its steric hindrance. The free energy for the transition state of the reaction of the second HSt2Li with styrene is the lowest, suggesting that the route through it is the predominant reaction path. The penultimate unit effect, slower addition of styrene to HSt2Li than to HStLi, is attributed to coordination of the penultimate styrene units of the polystyryllithium dimer (one of the starting materials to its Li atoms. The calculated enthalpy for the reaction barrier of the second HSt2Li with styrene in cyclohexane was found to agree with the observed apparent activation energy in benzene.

  13. Cu–Ni core–shell nanoparticles: structure, stability, electronic, and magnetic properties: a spin-polarized density functional study

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Qiang, E-mail: wangqiang@njtech.edu.cn; Wang, Xinyan; Liu, Jianlan; Yang, Yanhui [Nanjing Tech University, School of Chemistry and Molecular Engineering, Institute of Advanced Synthesis (IAS) (China)

    2017-02-15

    Bimetallic core–shell nanoparticles (CSNPs) have attracted great interest not only because of their superior stability, selectivity, and catalytic activity but also due to their tunable properties achieved by changing the morphology, sequence, and sizes of both core and shell. In this study, the structure, stability, charge transfer, electronic, and magnetic properties of 13-atom and 55-atom Cu and Cu–Ni CSNPs were investigated using the density functional theory (DFT) calculations. The results show that Ni@Cu CSNPs with a Cu surface shell are more energetically favorable than Cu@Ni CSNPs with a Ni surface shell. Interestingly, three-shell Ni@Cu{sub 12}@Ni{sub 42} is more stable than two-shell Cu{sub 13}@Ni{sub 42}, while two-shell Ni{sub 13}@Cu{sub 42} is more stable than three-shell Cu@Ni{sub 12}@Cu{sub 42}. Analysis of Bader charge illustrates that the charge transfer increases from Cu core to Ni shell in Cu@Ni NPs, while it decreases from Ni core to Cu shell in Ni@Cu NPs. Furthermore, the charge transfer results that d-band states have larger shift toward the Fermi level for the Ni@Cu CSNPs with Cu surface shell, while the Cu@Ni CSNPs with Ni surface shell have similar d-band state curves and d-band centers with the monometallic Ni NPs. In addition, the Cu–Ni CSNPs possess higher magnetic moment when the Ni atoms aggregated at core region of CSNPs, while having lower magnetic moment when the Ni atoms segregate on surface region. The change of the Cu atom location in CSNPs has a weak effect on the total magnetic moment. Our findings provide useful insights for the design of bimetallic core–shell catalysts.

  14. Laboratory Density Functionals

    OpenAIRE

    Giraud, B. G.

    2007-01-01

    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.

  15. Density Functional Theory

    Indian Academy of Sciences (India)

    (1) The total energy of an electron system in an external potential is a unique functional of the total electron density; and. (2)The density that minimizes the energy is the ground-state density, and this minimum energy is the ground-state energy of the system.

  16. Density functional theory

    International Nuclear Information System (INIS)

    Das, M.P.

    1984-07-01

    The state of the art of the density functional formalism (DFT) is reviewed. The theory is quantum statistical in nature; its simplest version is the well-known Thomas-Fermi theory. The DFT is a powerful formalism in which one can treat the effect of interactions in inhomogeneous systems. After some introductory material, the DFT is outlined from the two basic theorems, and various generalizations of the theorems appropriate to several physical situations are pointed out. Next, various approximations to the density functionals are presented and some practical schemes, discussed; the approximations include an electron gas of almost constant density and an electron gas of slowly varying density. Then applications of DFT in various diverse areas of physics (atomic systems, plasmas, liquids, nuclear matter) are mentioned, and its strengths and weaknesses are pointed out. In conclusion, more recent developments of DFT are indicated

  17. density functional theory (DFT)

    Indian Academy of Sciences (India)

    Abstract. In the present investigation, interaction of ruthenium (Ru) atoms with fluorine (F) atoms was studied using the density functional theory utilizing B3LYP method. It was found that up to seven F atoms can bind to a single Ru atom which results in increase of electron affinities successively, reaching a peak value of ...

  18. Quantal density functional theory

    CERN Document Server

    Sahni, Viraht

    2016-01-01

    This book deals with quantal density functional theory (QDFT) which is a time-dependent local effective potential theory of the electronic structure of matter. The treated time-independent QDFT constitutes a special case. In the 2nd edition, the theory is extended to include the presence of external magnetostatic fields. The theory is a description of matter based on the ‘quantal Newtonian’ first and second laws which is in terms of “classical” fields that pervade all space, and their quantal sources. The fields, which are explicitly defined, are separately representative of electron correlations due to the Pauli exclusion principle, Coulomb repulsion, correlation-kinetic, correlation-current-density, and correlation-magnetic effects. The book further describes Schrödinger theory from the new physical perspective of fields and quantal sources. It also describes traditional Hohenberg-Kohn-Sham DFT, and explains via QDFT the physics underlying the various energy functionals and functional derivatives o...

  19. Vibrational excitation of cyclopropane by electron impact: An experimental test of the discrete-momentum-representation theory with density-functional-theory approximation of polarization and correlation

    Czech Academy of Sciences Publication Activity Database

    Čurík, Roman; Čársky, Petr; Allan, M.

    2012-01-01

    Roč. 86, č. 6 (2012), 062709 ISSN 1050-2947 R&D Projects: GA MŠk(CZ) OC10046; GA ČR GAP208/11/0452 Institutional support: RVO:61388955 Keywords : Angular range * Density functionals * Electron impact Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.042, year: 2012

  20. Correlation between the Flux Density and Polarization for Flat ...

    Indian Academy of Sciences (India)

    In this paper, using the preliminary database of the University of Michigan Radio Astronomy Observatory (UMRAO) at the radio frequencies, we calculated the weighted polarization at 8 GHz and investigated the correlation between the polarization and the flux density for 92 flat spectrum radio quasars (FSRQs). We found ...

  1. Density functional theory

    International Nuclear Information System (INIS)

    Freyss, M.

    2015-01-01

    This chapter gives an introduction to first-principles electronic structure calculations based on the density functional theory (DFT). Electronic structure calculations have a crucial importance in the multi-scale modelling scheme of materials: not only do they enable one to accurately determine physical and chemical properties of materials, they also provide data for the adjustment of parameters (or potentials) in higher-scale methods such as classical molecular dynamics, kinetic Monte Carlo, cluster dynamics, etc. Most of the properties of a solid depend on the behaviour of its electrons, and in order to model or predict them it is necessary to have an accurate method to compute the electronic structure. DFT is based on quantum theory and does not make use of any adjustable or empirical parameter: the only input data are the atomic number of the constituent atoms and some initial structural information. The complicated many-body problem of interacting electrons is replaced by an equivalent single electron problem, in which each electron is moving in an effective potential. DFT has been successfully applied to the determination of structural or dynamical properties (lattice structure, charge density, magnetisation, phonon spectra, etc.) of a wide variety of solids. Its efficiency was acknowledged by the attribution of the Nobel Prize in Chemistry in 1998 to one of its authors, Walter Kohn. A particular attention is given in this chapter to the ability of DFT to model the physical properties of nuclear materials such as actinide compounds. The specificities of the 5f electrons of actinides will be presented, i.e., their more or less high degree of localisation around the nuclei and correlations. The limitations of the DFT to treat the strong 5f correlations are one of the main issues for the DFT modelling of nuclear fuels. Various methods that exist to better treat strongly correlated materials will finally be presented. (author)

  2. Self-consistent embedding of density-matrix renormalization group wavefunctions in a density functional environment.

    Science.gov (United States)

    Dresselhaus, Thomas; Neugebauer, Johannes; Knecht, Stefan; Keller, Sebastian; Ma, Yingjin; Reiher, Markus

    2015-01-28

    We present the first implementation of a density matrix renormalization group algorithm embedded in an environment described by density functional theory. The frozen density embedding scheme is used with a freeze-and-thaw strategy for a self-consistent polarization of the orbital-optimized wavefunction and the environmental densities with respect to each other.

  3. Spin polarization in high density quark matter

    DEFF Research Database (Denmark)

    Bohr, Henrik; Panda, Prafulla K.; Providênci, Constanca

    2013-01-01

    We investigate the occurrence of a ferromagnetic phase transition in high density hadronic matter (e.g., in the interior of a neutron star). This could be induced by a four-fermion interaction analogous to the one which is responsible for chiral symmetry breaking in the Nambu-Jona-Lasinio model...... the so-called 2 flavor super-conducting phase to the ferromagnetic phase arises. The color-flavor-locked phase may be completely hidden by the FP....

  4. Ab initio density functional theory study of non-polar (10-10), (11-20) and semipolar {20-21} GaN surfaces

    Czech Academy of Sciences Publication Activity Database

    Mutombo, Pingo; Romanyuk, Olexandr

    2014-01-01

    Roč. 115, č. 20 (2014), "203508-1"-"203508-5" ISSN 0021-8979 Grant - others:AVČR(CZ) M100101201 Institutional support: RVO:68378271 Keywords : non-polar GaN * semipolar GaN * surface reconstructions * DFT Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 2.183, year: 2014

  5. Correlation between the Flux Density and Polarization for Flat ...

    Indian Academy of Sciences (India)

    blazars, which show high and variable polarization, rapid variable flux density over different time scales (Fan 2005). Blazars consist of flat spectrum radio quasars. (FSRQs) and BL Lacertae objects (BLs). FSRQs are quite similar to BLs except for their emission line feature with FSRQs showing strong emission lines while.

  6. Correlation between the Flux Density and Polarization for Flat ...

    Indian Academy of Sciences (India)

    3Guangzhou Vocational College of Technology & Business, Guangzhou, China. 4Center for Astrophysics ... blazars, which show high and variable polarization, rapid variable flux density over different time scales (Fan ... emission lines while. BLs show very weak emission line feature or have only non-emission lines. The.

  7. SYNTHESIS, CHARACTERIZATION AND DENSITY FUNCTIONAL ...

    African Journals Online (AJOL)

    Preferred Customer

    KEY WORDS: Monoacyl aniline, Synthesis, Density functional theory, Rotation barrier. INTRODUCTION ... on the electron density in the phenyl ring and the respective accelerating and decelerating effects on the rate of ... compounds were determined using Nujol mulls and of liquids either in dichloromethane or chloroform ...

  8. Density dependence of the nuclear energy-density functional

    Science.gov (United States)

    Papakonstantinou, Panagiota; Park, Tae-Sun; Lim, Yeunhwan; Hyun, Chang Ho

    2018-01-01

    Background: The explicit density dependence in the coupling coefficients entering the nonrelativistic nuclear energy-density functional (EDF) is understood to encode effects of three-nucleon forces and dynamical correlations. The necessity for the density-dependent coupling coefficients to assume the form of a preferably small fractional power of the density ρ is empirical and the power is often chosen arbitrarily. Consequently, precision-oriented parametrizations risk overfitting in the regime of saturation and extrapolations in dilute or dense matter may lose predictive power. Purpose: Beginning with the observation that the Fermi momentum kF, i.e., the cubic root of the density, is a key variable in the description of Fermi systems, we first wish to examine if a power hierarchy in a kF expansion can be inferred from the properties of homogeneous matter in a domain of densities, which is relevant for nuclear structure and neutron stars. For subsequent applications we want to determine a functional that is of good quality but not overtrained. Method: For the EDF, we fit systematically polynomial and other functions of ρ1 /3 to existing microscopic, variational calculations of the energy of symmetric and pure neutron matter (pseudodata) and analyze the behavior of the fits. We select a form and a set of parameters, which we found robust, and examine the parameters' naturalness and the quality of resulting extrapolations. Results: A statistical analysis confirms that low-order terms such as ρ1 /3 and ρ2 /3 are the most relevant ones in the nuclear EDF beyond lowest order. It also hints at a different power hierarchy for symmetric vs. pure neutron matter, supporting the need for more than one density-dependent term in nonrelativistic EDFs. The functional we propose easily accommodates known or adopted properties of nuclear matter near saturation. More importantly, upon extrapolation to dilute or asymmetric matter, it reproduces a range of existing microscopic

  9. Theoretical analysis of polarized structure functions

    International Nuclear Information System (INIS)

    Altarelli, G.; ); Ball, R.D.; Forte, S.; Ridolfi, G.

    1998-01-01

    We review the analysis of polarized structure function data using perturbative QCD and NLO We use the most recent experimental data to obtain updated results for polarized parton distributions, first moments and the strong coupling. We also discuss several theoretical issues involving in this analysis and in the interpretation of its results. Finally, we compare our results with other similar analyses in the recent literature. (author)

  10. Theoretical Analysis of Polarized Structure Functions

    CERN Document Server

    Altarelli, Guido; Forte, Stefano; Ridolfi, G

    1998-01-01

    We review the analysis of polarized structure function data using perturbative QCD at next-to-leading order. We use the most recent experimental data to obtain updated results for polarized parton distributions, first moments and the strong coupling. We also discuss several theoretical issues involved in this analysis and in the interpretation of its results. Finally, we compare our results with other similar analyses in the recent literature.

  11. Ionization Energies, Electron Affinities, and Polarization Energies of Organic Molecular Crystals: Quantitative Estimations from a Polarizable Continuum Model (PCM)–Tuned Range-Separated Density Functional Approach

    KAUST Repository

    Sun, Haitao

    2016-05-16

    We propose a new methodology for the first-principles description of the electronic properties relevant for charge transport in organic molecular crystals. This methodology, which is based on the combination of a non-empirical, optimally tuned range-separated hybrid functional with the polarizable continuum model, is applied to a series of eight representative molecular semiconductor crystals. We show that it provides ionization energies, electron affinities, and transport gaps in very good agreement with experimental values as well as with the results of many-body perturbation theory within the GW approximation at a fraction of the computational costs. Hence, this approach represents an easily applicable and computationally efficient tool to estimate the gas-to-crystal-phase shifts of the frontier-orbital quasiparticle energies in organic electronic materials.

  12. Thermospheric density structures over the polar regions observed with CHAMP

    Directory of Open Access Journals (Sweden)

    K. Schlegel

    2005-07-01

    Full Text Available We report on the unexpected detection of considerable structure in high latitude thermospheric densities, as derived from an accelerometer onboard the CHAMP satellite. The width of the structures, which can either be maxima or minima, varies between a few hundred km and 2000 km. The amplitudes of these density extrema can reach 50% of ambient. Maxima cluster around 75° (N and S, while minima are found closer to the poles. In a magnetic latitude-magnetic local time frame the maxima are found mainly around the cusp region. Overall, the observed structures somewhat resemble so-called density cells previously found in model calculations. However the models generate their cells around 140–300 km altitude and show little, if any remnant at 400 km or above. This has to be contrasted with the fact that the CHAMP observations were obtained near 430 km altitude. We have explored Joule heating as a possible mechanism for the generation of the structures, at least in density enhancement regions, using Hall currents measured on CHAMP and simultaneous incoherent scatter measurements with EISCAT. However, the electric fields were usually quite small during the period of observation, making the quest for an explanation for the structures all the more challenging. Keywords. Meteorology and atmospheric dynamics (Thermospheric dynamics – Magnetospheric physics (Polar cap phenomena – Atmospheric composition and structure (Pressure, density, and temperature

  13. Dynamic polarization in paramagnetic solids and microscopic correlation functions

    International Nuclear Information System (INIS)

    Boucher, Jean-Paul

    1972-01-01

    The different effects of Dynamic Nuclear Polarization in paramagnetic solids are described by means of a single thermodynamic formalism. In the case of large exchange interactions, the Overhauser effect correlated with nuclear relaxation time measurements can provide a way of studying correlation functions between electronic spins. This method is used to study the low-frequency behaviour of the microscopic spectral density which should diverge as ω → 0, in the case of a linear exchange chain. (author) [fr

  14. Density functional theory of nuclei

    International Nuclear Information System (INIS)

    Terasaki, Jun

    2008-01-01

    The density functional theory of nuclei has come to draw attention of scientists in the field of nuclear structure because the theory is expected to provide reliable numerical data in wide range on the nuclear chart. This article is organized to present an overview of the theory to the people engaged in the theory of other fields as well as those people in the nuclear physics experiments. At first, the outline of the density functional theory widely used in the electronic systems (condensed matter, atoms, and molecules) was described starting from the Kohn-Sham equation derived on the variational principle. Then the theory used in the field of nuclear physics was presented. Hartree-Fock and Hartree-Fock-Bogolyubov approximation by using Skyrme interaction was explained. Comparison of the results of calculations and experiments of binding energies and ground state mean square charge radii of some magic number nuclei were shown. The similarity and dissimilarity between the two streams were summarized. Finally the activities of the international project of Universal Nuclear Energy Density Functional (UNEDF) which was started recently lead by US scientist was reported. This project is programmed for five years. One of the applications of the project is the calculation of the neutron capture cross section of nuclei on the r-process, which is absolutely necessary for the nucleosynthesis research. (S. Funahashi)

  15. Density functional theory: Foundations reviewed

    Energy Technology Data Exchange (ETDEWEB)

    Kryachko, Eugene S., E-mail: eugene.kryachko@ulg.ac.be [Bogolyubov Institute for Theoretical Physics, Kiev, 03680 (Ukraine); Ludeña, Eduardo V., E-mail: popluabe@yahoo.es [Centro de Química, Instituto Venezolano de Investigaciones Científicas, IVIC, Apartado 21827, Caracas 1020-A (Venezuela, Bolivarian Republic of); Prometheus Program, Senescyt (Ecuador); Grupo Ecuatoriano para el Estudio Experimental y Teórico de Nanosistemas, GETNano, USFQ, N104-E, Quito (Ecuador); Escuela Politécnica Superior del Litoral, ESPOL, Guayaquil (Ecuador)

    2014-11-10

    Guided by the above motto (quotation), we review a broad range of issues lying at the foundations of Density Functional Theory, DFT, a theory which is currently omnipresent in our everyday computational study of atoms and molecules, solids and nano-materials, and which lies at the heart of modern many-body computational technologies. The key goal is to demonstrate that there are definitely the ways to improve DFT. We start by considering DFT in the larger context provided by reduced density matrix theory (RDMT) and natural orbital functional theory (NOFT), and examine the implications that N-representability conditions on the second-order reduced density matrix (2-RDM) have not only on RDMT and NOFT but, also, by extension, on the functionals of DFT. This examination is timely in view of the fact that necessary and sufficient N-representability conditions on the 2-RDM have recently been attained. In the second place, we review some problems appearing in the original formulation of the first Hohenberg–Kohn theorem which is still a subject of some controversy. In this vein we recall Lieb’s comment on this proof and the extension to this proof given by Pino et al. (2009), and in this context examine the conditions that must be met in order that the one-to-one correspondence between ground-state densities and external potentials remains valid for finite subspaces (namely, the subspaces where all Kohn–Sham solutions are obtained in practical applications). We also consider the issue of whether the Kohn–Sham equations can be derived from basic principles or whether they are postulated. We examine this problem in relation to ab initio DFT. The possibility of postulating arbitrary Kohn–Sham-type equations, where the effective potential is by definition some arbitrary mixture of local and non-local terms, is discussed. We also deal with the issue of whether there exists a universal functional, or whether one should advocate instead the construction of problem

  16. Density functional theory: Foundations reviewed

    Science.gov (United States)

    Kryachko, Eugene S.; Ludeña, Eduardo V.

    2014-11-01

    Guided by the above motto (quotation), we review a broad range of issues lying at the foundations of Density Functional Theory, DFT, a theory which is currently omnipresent in our everyday computational study of atoms and molecules, solids and nano-materials, and which lies at the heart of modern many-body computational technologies. The key goal is to demonstrate that there are definitely the ways to improve DFT. We start by considering DFT in the larger context provided by reduced density matrix theory (RDMT) and natural orbital functional theory (NOFT), and examine the implications that N-representability conditions on the second-order reduced density matrix (2-RDM) have not only on RDMT and NOFT but, also, by extension, on the functionals of DFT. This examination is timely in view of the fact that necessary and sufficient N-representability conditions on the 2-RDM have recently been attained. In the second place, we review some problems appearing in the original formulation of the first Hohenberg-Kohn theorem which is still a subject of some controversy. In this vein we recall Lieb's comment on this proof and the extension to this proof given by Pino et al. (2009), and in this context examine the conditions that must be met in order that the one-to-one correspondence between ground-state densities and external potentials remains valid for finite subspaces (namely, the subspaces where all Kohn-Sham solutions are obtained in practical applications). We also consider the issue of whether the Kohn-Sham equations can be derived from basic principles or whether they are postulated. We examine this problem in relation to ab initio DFT. The possibility of postulating arbitrary Kohn-Sham-type equations, where the effective potential is by definition some arbitrary mixture of local and non-local terms, is discussed. We also deal with the issue of whether there exists a universal functional, or whether one should advocate instead the construction of problem

  17. Metallicity at interphase boundaries due to polar catastrophe induced by charge density discontinuity

    KAUST Repository

    Albar, Arwa

    2018-02-09

    The electronic properties of interphase boundaries are of basic importance for most materials, particularly when those properties deviate strongly from the bulk behavior. We introduce a mechanism that can result in metallicity at stoichiometric interphase boundaries between semiconductors based on the idea of polar catastrophe, which is usually considered only in the context of heterostructures. To this end, we perform ab initio calculations within density functional theory to investigate the electronic states at stoichiometric SnO/SnO2 (110) interphase boundaries. In this system, one would not expect polar catastrophe to have a role according to state-of-the-art theory because the interface lacks formal charge discontinuity. However, we observe the formation of a hole gas between the semiconductors SnO and SnO2. To explain these findings, we provide a generalized theory based on the idea that the charge density discontinuity between SnO and SnO2, a consequence of lattice mismatch, drives a polar catastrophe scenario. As a result, SnO/SnO2 (110) interphase boundaries can develop metallicity depending on the grain size. The concept of metallicity due to polar catastrophe induced by charge density discontinuity is of general validity and applies to many interphase boundaries with lattice mismatch.

  18. Polarization-Dependent Multi-Functional Metamaterial as Polarization Filter, Transparent Wall and Circular Polarizer using Ring-Cross Resonator

    Directory of Open Access Journals (Sweden)

    Z. Zhang

    2017-09-01

    Full Text Available We propose a polarization-dependent multi-functional metamaterial using ring-cross resonator. Based on the analysis of surface current distributions induced by different polarized incidence, we demonstrate that the proposed metamaterial serves as a polarization filter, a transparent wall and a circular polarizer under different polarization normal incidence. Additionally, parameter analyses on the control of resonance are discussed to complementally explain the physical origin. Simulated results show that the proposed metamaterial functions as a polarization filter eliminating the x-polarization wave at 10.1 GHz and y-polarization wave at 14.3 GHz, a transparent wall transmitting both x-polarized and y-polarized incident waves at 12.6 GHz, and a broadband circular polarizer converting the +45° polarized (-45° polarized incident wave to the left (right handed circularly polarized wave from 10.8 to 12.8 GHz, respectively. Measured results agree well with the simulation and validate the performance of the proposed multifunctional metamaterial.

  19. Polar Functions for Anisotropic Gaussian Random Fields

    Directory of Open Access Journals (Sweden)

    Zhenlong Chen

    2014-01-01

    Full Text Available Let X be an (N, d-anisotropic Gaussian random field. Under some general conditions on X, we establish a relationship between a class of continuous functions satisfying the Lipschitz condition and a class of polar functions of X. We prove upper and lower bounds for the intersection probability for a nonpolar function and X in terms of Hausdorff measure and capacity, respectively. We also determine the Hausdorff and packing dimensions of the times set for a nonpolar function intersecting X. The class of Gaussian random fields that satisfy our conditions includes not only fractional Brownian motion and the Brownian sheet, but also such anisotropic fields as fractional Brownian sheets, solutions to stochastic heat equation driven by space-time white noise, and the operator-scaling Gaussian random field with stationary increments.

  20. Multiconfiguration Pair-Density Functional Theory.

    Science.gov (United States)

    Li Manni, Giovanni; Carlson, Rebecca K; Luo, Sijie; Ma, Dongxia; Olsen, Jeppe; Truhlar, Donald G; Gagliardi, Laura

    2014-09-09

    We present a new theoretical framework, called Multiconfiguration Pair-Density Functional Theory (MC-PDFT), which combines multiconfigurational wave functions with a generalization of density functional theory (DFT). A multiconfigurational self-consistent-field (MCSCF) wave function with correct spin and space symmetry is used to compute the total electronic density, its gradient, the on-top pair density, and the kinetic and Coulomb contributions to the total electronic energy. We then use a functional of the total density, its gradient, and the on-top pair density to calculate the remaining part of the energy, which we call the on-top-density-functional energy in contrast to the exchange-correlation energy of Kohn-Sham DFT. Because the on-top pair density is an element of the two-particle density matrix, this goes beyond the Hohenberg-Kohn theorem that refers only to the one-particle density. To illustrate the theory, we obtain first approximations to the required new type of density functionals by translating conventional density functionals of the spin densities using a simple prescription, and we perform post-SCF density functional calculations using the total density, density gradient, and on-top pair density from the MCSCF calculations. Double counting of dynamic correlation or exchange does not occur because the MCSCF energy is not used. The theory is illustrated by applications to the bond energies and potential energy curves of H2, N2, F2, CaO, Cr2, and NiCl and the electronic excitation energies of Be, C, N, N(+), O, O(+), Sc(+), Mn, Co, Mo, Ru, N2, HCHO, C4H6, c-C5H6, and pyrazine. The method presented has a computational cost and scaling similar to MCSCF, but a quantitative accuracy, even with the present first approximations to the new types of density functionals, that is comparable to much more expensive multireference perturbation theory methods.

  1. Density functional theory and multiscale materials modeling

    Indian Academy of Sciences (India)

    In the macroscopic length scale, however, matter is usually treated as a continuous medium and a description using local mass density, energy density and other related density functions has been found to be quite appropriate. A unique single unified theoretical framework that emerges through the density concept at these ...

  2. Short time behaviour of density correlation functions

    NARCIS (Netherlands)

    Konijnendijk, H.H.U.

    1977-01-01

    In this thesis the dynamical behaviour of the atoms in a fluid or gas is studied with time dependent correlation functions as the density-density correlation function and the velocity autocorrelation function. Theoretically it is not possible to calculate these correlation functions exactly for the

  3. Generalized density-functional theory: Conquering the ...

    Indian Academy of Sciences (India)

    Home; Journals; Journal of Chemical Sciences; Volume 117; Issue 5. Generalized density-functional theory: Conquering the -representability problem with exact functionals for the electron pair density and the second-order reduced density matrix. Paul W Ayers Mel Levy. Volume 117 Issue 5 September 2005 pp 507-514 ...

  4. Density functional theory and parallel processing

    International Nuclear Information System (INIS)

    Ward, R.C.; Geist, G.A.; Butler, W.H.

    1987-01-01

    The authors demonstrate a method for obtaining the ground state energies and charge densities of a system of atoms described within density functional theory using simulated annealing on a parallel computer

  5. A Density Functional Theory Study

    KAUST Repository

    Lim, XiaoZhi

    2011-12-11

    Complexes with pincer ligand moieties have garnered much attention in the past few decades. They have been shown to be highly active catalysts in several known transition metal-catalyzed organic reactions as well as some unprecedented organic transformations. At the same time, the use of computational organometallic chemistry to aid in the understanding of the mechanisms in organometallic catalysis for the development of improved catalysts is on the rise. While it was common in earlier studies to reduce computational cost by truncating donor group substituents on complexes such as tertbutyl or isopropyl groups to hydrogen or methyl groups, recent advancements in the processing capabilities of computer clusters and codes have streamlined the time required for calculations. As the full modeling of complexes become increasingly popular, a commonly overlooked aspect, especially in the case of complexes bearing isopropyl substituents, is the conformational analysis of complexes. Isopropyl groups generate a different conformer with each 120 ° rotation (rotamer), and it has been found that each rotamer typically resides in its own potential energy well in density functional theory studies. As a result, it can be challenging to select the most appropriate structure for a theoretical study, as the adjustment of isopropyl substituents from a higher-energy rotamer to the lowest-energy rotamer usually does not occur during structure optimization. In this report, the influence of the arrangement of isopropyl substituents in pincer complexes on calculated complex structure energies as well as a case study on the mechanism of the isomerization of an iPrPCP-Fe complex is covered. It was found that as many as 324 rotamers can be generated for a single complex, as in the case of an iPrPCP-Ni formato complex, with the energy difference between the global minimum and the highest local minimum being as large as 16.5 kcalmol-1. In the isomerization of a iPrPCP-Fe complex, it was found

  6. Dimensionality reduction when data are density functions

    OpenAIRE

    Delicado Useros, Pedro Francisco

    2011-01-01

    Functional Data Analysis deals with samples where a whole function is observed for each individual. A relevant case of FDA is when the observed functions are density functions. Among the particular characteristics of density functions, the most of the fact that they are an example of infinite dimensional compositional data (parts of some whole which only carry relative information) is made. Several dimensionality reduction methods for this particular type of data are compared: fun...

  7. Interplay between spin polarization and color superconductivity in high density quark matter

    DEFF Research Database (Denmark)

    Tsue, Yasuhiko; da Providência, João; Providência, Constança

    2013-01-01

    Here, it is suggested that a four-point interaction of the tensor type may lead to spin polarization in quark matter at high density. It is found that the two-flavor superconducting phase and the spin polarized phase correspond to distinct local minima of a certain generalized thermodynamical...... potential. It follows that a transition from one to the other phase occurs, passing through true minima with both a spin polarization and a color superconducting gap. It is shown that the quark spin polarized phase is realized at rather high density, while the two-flavor color superconducting phase...

  8. Energy vs. density on paths toward more exact density functionals.

    Science.gov (United States)

    Kepp, Kasper P

    2018-03-14

    Recently, the progression toward more exact density functional theory has been questioned, implying a need for more formal ways to systematically measure progress, i.e. a "path". Here I use the Hohenberg-Kohn theorems and the definition of normality by Burke et al. to define a path toward exactness and "straying" from the "path" by separating errors in ρ and E[ρ]. A consistent path toward exactness involves minimizing both errors. Second, a suitably diverse test set of trial densities ρ' can be used to estimate the significance of errors in ρ without knowing the exact densities which are often inaccessible. To illustrate this, the systems previously studied by Medvedev et al., the first ionization energies of atoms with Z = 1 to 10, the ionization energy of water, and the bond dissociation energies of five diatomic molecules were investigated using CCSD(T)/aug-cc-pV5Z as benchmark at chemical accuracy. Four functionals of distinct designs was used: B3LYP, PBE, M06, and S-VWN. For atomic cations regardless of charge and compactness up to Z = 10, the energy effects of the different ρ are energy-wise insignificant. An interesting oscillating behavior in the density sensitivity is observed vs. Z, explained by orbital occupation effects. Finally, it is shown that even large "normal" problems such as the Co-C bond energy of cobalamins can use simpler (e.g. PBE) trial densities to drastically speed up computation by loss of a few kJ mol -1 in accuracy. The proposed method of using a test set of trial densities to estimate the sensitivity and significance of density errors of functionals may be useful for testing and designing new balanced functionals with more systematic improvement of densities and energies.

  9. Density functional theory in quantum chemistry

    CERN Document Server

    Tsuneda, Takao

    2014-01-01

    This book examines density functional theory based on the foundation of quantum chemistry. Unconventional in approach, it reviews basic concepts, then describes the physical meanings of state-of-the-art exchange-correlation functionals and their corrections.

  10. RETRIEVAL OF AEROSOL PHASE FUNCTION AND POLARIZED PHASE FUNCTION FROM POLARIZATION OF SKYLIGHT FOR DIFFERENT OBSERVATION GEOMETRIES

    Directory of Open Access Journals (Sweden)

    L. Li

    2018-04-01

    Full Text Available The phase function and polarized phase function are important optical parameters, which describe scattering properties of atmospheric aerosol particles. Polarization of skylight induced by the scattering processes is sensitive to the scattering properties of aerosols. The Stokes parameters I, Q, U and the polarized radiance Lp of skylight measured by the CIMEL dual-polar sun-sky radiometer CE318- DP can be use to retrieve the phase function and polarized phase function, respectively. Two different observation geometries (i.e., the principal plane and almucantar are preformed by the CE318-DP to detect skylight polarization. Polarization of skylight depends on the illumination and observation geometries. For the same solar zenith angle, retrievals of the phase function and the polarized phase function are still affected by the observation geometry. The performance of the retrieval algorithm for the principal plane and almucantar observation geometries was assessed by the numerical experiments at two typical high and low sun’s positions (i.e. solar zenith angles are equal to 45° and 65°. Comparing the results for the principal plane and almucantar geometries, it is recommended to utilize the principal plane observations to retrieve the phase function when the solar zenith angle is small. The Stokes parameter U and the polarized radiance Lp from the almucantar observations are suggested to retrieve the polarized phase function, especially for short wavelength channels (e.g., 440 and 500 nm.

  11. A multiconfigurational hybrid density-functional theory

    DEFF Research Database (Denmark)

    Sharkas, Kamal; Savin, Andreas; Jensen, Hans Jørgen Aagaard

    2012-01-01

    We propose a multiconfigurational hybrid density-functional theory which rigorously combines a multiconfiguration self-consistent-field calculation with a density-functional approximation based on a linear decomposition of the electron-electron interaction. This gives a straightforward extension ...

  12. Magnetic fields and density functional theory

    International Nuclear Information System (INIS)

    Salsbury, Freddie Jr.

    1999-01-01

    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

  13. Penile density and globally used chemicals in Canadian and Greenland polar bears.

    Science.gov (United States)

    Sonne, Christian; Dyck, Markus; Rigét, Frank F; Beck Jensen, Jens-Erik; Hyldstrup, Lars; Letcher, Robert J; Gustavson, Kim; Gilbert, M Thomas P; Dietz, Rune

    2015-02-01

    Industrially produced chemicals have been a major environmental concern across our entire Globe since the onset of rapid industrial development around the early 1900. Many of the substances being used are known to be endocrine disrupting chemicals (EDCs) and are also known to be long-range dispersed and to biomagnify to very high concentrations in the tissues of Arctic apex predators such as polar bears (Ursus maritimus). A major concern relating to EDCs is their effects on vital organ-tissues such as bone and it is possible that EDCs represent a more serious challenge to the species' survival than the more conventionally proposed prey reductions linked to climate change. We therefore analyzed penile bone mineral density (BMD) as a key phenotype for reproductive success in 279 polar bear samples born 1990-2000 representing eight polar bear subpopulations. Since EDC concentrations were not available from the same specimens, we compared BMD with published literature information on EDC concentrations. Latitudinal and longitudinal BMD and EDC gradients were clearly observed, with Western Hudson bears having the highest BMD and lowest EDCs, and North East Greenland polar bears carrying the lowest BMD and highest EDCs. A BMD vs. polychlorinated biphenyls (PCB) regression analysis showed that BMD decreased as a function of the eight subpopulations' PCB concentrations and this relationship was close to being significant (p=0.10, R(2)=0.39). Risk quotient (RQ) estimation demonstrated that PCBs could be in a range that may lead to disruption of normal reproduction and development. It is therefore likely that EDCs directly affect development and bone density in polar bears. Canadian bears had in general the best health and the North East Greenland subpopulation being at the highest risk of having negative health effects. While reductions in BMD is in general unhealthy, reductions in penile BMD could lead to increased risk of species extinction because of mating and subsequent

  14. Polar cap hot patches: Enhanced density structures different from the classical patches in the ionosphere

    Science.gov (United States)

    Zhang, Q.-H.; Ma, Y.-Z.; Jayachandran, P. T.; Moen, J.; Lockwood, M.; Zhang, Y.-L.; Foster, J. C.; Zhang, S.-R.; Wang, Y.; Themens, D. R.; Zhang, B.-C.; Xing, Z. Y.

    2017-08-01

    Based on in situ and ground-based observations, a new type of "polar cap hot patch" has been identified that is different from the classical polar cap enhanced density structure (cold patches). Comparing with the classical polar cap patches, which are transported from the dayside sunlit region with dense and cold plasma, the polar cap hot patches are associated with particle precipitations (therefore field-aligned currents), ion upflows, and flow shears. The hot patches may have the same order of density enhancement as classical patches in the topside ionosphere, suggesting that the hot patches may be produced by transported photoionization plasma into flow channels. Within the flow channels, the hot patches have low-energy particle precipitation and/or ion upflows associated with field-aligned currents and flow shears. Corresponding Global Navigation Satellite System (GNSS) signal scintillation measurements indicate that hot patches may produce slightly stronger radio signal scintillation in the polar cap region than classical patches. A new type of polar cap patches, "polar cap hot patches," is identified to differentiate enhanced density structures from classical patches. Hot patches are associated with particle precipitations, ion upflows, field-aligned currents, and shear flows in the polar cap. Hot patches may lead to slightly stronger ionospheric scintillations of GNSS signals in the polar cap region than classical patches.

  15. On the theory of pyro- and ferroelectrics: Dipole moment density and polarization

    Science.gov (United States)

    Belyavskii, V. I.; Gorbatsevich, A. A.

    2017-04-01

    The physical origin of the ambiguity related to the dependence of the polarization on the choice of the unit cell in a crystal is established in the framework of classical electrodynamics. It is shown that the electric polarization of a crystal is determined not only by the charge distribution in the unit cell (dipole moment density) but also by the microscopic mechanism of symmetry breaking in the polar phase. An approach to the calculation of the polarization invariant with respect to the choice of the unit cell is suggested. It is demonstrated that the dependence of the polarization on the mechanism of formation of the polar phase exists in the "modern topological theory" of polarization too.

  16. Multicomponent density functional theory embedding formulation.

    Science.gov (United States)

    Culpitt, Tanner; Brorsen, Kurt R; Pak, Michael V; Hammes-Schiffer, Sharon

    2016-07-28

    Multicomponent density functional theory (DFT) methods have been developed to treat two types of particles, such as electrons and nuclei, quantum mechanically at the same level. In the nuclear-electronic orbital (NEO) approach, all electrons and select nuclei, typically key protons, are treated quantum mechanically. For multicomponent DFT methods developed within the NEO framework, electron-proton correlation functionals based on explicitly correlated wavefunctions have been designed and used in conjunction with well-established electronic exchange-correlation functionals. Herein a general theory for multicomponent embedded DFT is developed to enable the accurate treatment of larger systems. In the general theory, the total electronic density is separated into two subsystem densities, denoted as regular and special, and different electron-proton correlation functionals are used for these two electronic densities. In the specific implementation, the special electron density is defined in terms of spatially localized Kohn-Sham electronic orbitals, and electron-proton correlation is included only for the special electron density. The electron-proton correlation functional depends on only the special electron density and the proton density, whereas the electronic exchange-correlation functional depends on the total electronic density. This scheme includes the essential electron-proton correlation, which is a relatively local effect, as well as the electronic exchange-correlation for the entire system. This multicomponent DFT-in-DFT embedding theory is applied to the HCN and FHF(-) molecules in conjunction with two different electron-proton correlation functionals and three different electronic exchange-correlation functionals. The results illustrate that this approach provides qualitatively accurate nuclear densities in a computationally tractable manner. The general theory is also easily extended to other types of partitioning schemes for multicomponent systems.

  17. Locality of correlation in density functional theory.

    Science.gov (United States)

    Burke, Kieron; Cancio, Antonio; Gould, Tim; Pittalis, Stefano

    2016-08-07

    The Hohenberg-Kohn density functional was long ago shown to reduce to the Thomas-Fermi (TF) approximation in the non-relativistic semiclassical (or large-Z) limit for all matter, i.e., the kinetic energy becomes local. Exchange also becomes local in this limit. Numerical data on the correlation energy of atoms support the conjecture that this is also true for correlation, but much less relevant to atoms. We illustrate how expansions around a large particle number are equivalent to local density approximations and their strong relevance to density functional approximations. Analyzing highly accurate atomic correlation energies, we show that EC → -AC ZlnZ + BCZ as Z → ∞, where Z is the atomic number, AC is known, and we estimate BC to be about 37 mhartree. The local density approximation yields AC exactly, but a very incorrect value for BC, showing that the local approximation is less relevant for the correlation alone. This limit is a benchmark for the non-empirical construction of density functional approximations. We conjecture that, beyond atoms, the leading correction to the local density approximation in the large-Z limit generally takes this form, but with BC a functional of the TF density for the system. The implications for the construction of approximate density functionals are discussed.

  18. Solvent density mode instability in non-polar solutions

    Indian Academy of Sciences (India)

    1Department of Chemical, Biological and Macromolecular Sciences, S. N. Bose National. Centre for Basic Sciences, ... upon excitation mainly drives the solvent reorganization [12,13]. However, the. Stokes shifts ..... process [17] where a solvent density mode with momentum q is scattered to another density mode of ...

  19. Instabilities in the Nuclear Energy Density Functional

    Energy Technology Data Exchange (ETDEWEB)

    Kortelainen, Erno M [ORNL; Lesinski, Thomas [ORNL

    2010-01-01

    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.

  20. Relativistic density functional for nuclear structure

    CERN Document Server

    2016-01-01

    This book aims to provide a detailed introduction to the state-of-the-art covariant density functional theory, which follows the Lorentz invariance from the very beginning and is able to describe nuclear many-body quantum systems microscopically and self-consistently. Covariant density functional theory was introduced in nuclear physics in the 1970s and has since been developed and used to describe the diversity of nuclear properties and phenomena with great success. In order to provide an advanced and updated textbook of covariant density functional theory for graduate students and nuclear physics researchers, this book summarizes the enormous amount of material that has accumulated in the field of covariant density functional theory over the last few decades as well as the latest developments in this area. Moreover, the book contains enough details for readers to follow the formalism and theoretical results, and provides exhaustive references to explore the research literature.

  1. Gender Differences in Brain Functional Connectivity Density

    OpenAIRE

    Tomasi, Dardo; Volkow, Nora D.

    2011-01-01

    The neural bases of gender differences in emotional, cognitive, and socials behaviors are largely unknown. Here, magnetic resonance imaging data from 336 women and 225 men revealed a gender dimorphism in the functional organization of the brain. Consistently across five research sites, women had 14% higher local functional connectivity density (lFCD) and up to 5% higher gray matter density than men in cortical and subcortical regions. The negative power scaling of the lFCD was steeper for men...

  2. Rational Density Functional Selection Using Game Theory.

    Science.gov (United States)

    McAnanama-Brereton, Suzanne; Waller, Mark P

    2018-01-22

    Theoretical chemistry has a paradox of choice due to the availability of a myriad of density functionals and basis sets. Traditionally, a particular density functional is chosen on the basis of the level of user expertise (i.e., subjective experiences). Herein we circumvent the user-centric selection procedure by describing a novel approach for objectively selecting a particular functional for a given application. We achieve this by employing game theory to identify optimal functional/basis set combinations. A three-player (accuracy, complexity, and similarity) game is devised, through which Nash equilibrium solutions can be obtained. This approach has the advantage that results can be systematically improved by enlarging the underlying knowledge base, and the deterministic selection procedure mathematically justifies the density functional and basis set selections.

  3. Computing the hadronic vacuum polarization function by analytic continuation

    Energy Technology Data Exchange (ETDEWEB)

    Feng, Xu [KEK National High Energy Physics, Tsukuba (Japan); Hashimoto, Shoji [KEK National High Energy Physics, Tsukuba (Japan); The Graduate Univ. for Advanced Studies, Tsukuba (Japan). School of High Energy Accelerator Science; Hotzel, Grit [Humboldt-Universitaet, Berlin (Germany). Inst. fuer Physik; Jansen, Karl [Deutsches Elektronen-Synchrotron (DESY), Zeuthen (Germany). John von Neumann-Inst. fuer Computing NIC; Cyprus Univ., Nicosia (Cyprus). Dept. of Physics; Petschlies, Marcus [The Cyprus Institute, Nicosia (Cyprus); Renner, Dru B. [Thomas Jefferson National Accelerator Facility, Newport News, VA (United States)

    2013-07-15

    We propose a method to compute the hadronic vacuum polarization function on the lattice at continuous values of photon momenta bridging between the space-like and time-like regions. We provide two independent derivations of this method showing that it leads to the desired hadronic vacuum polarization function in Minkowski space-time. We show with the example of the leading- order QCD correction to the muon anomalous magnetic moment that this approach can provide a valuable alternative method for calculations of physical quantities where the hadronic vacuum polarization function enters.

  4. Modeling optical and UV polarization of AGNs. III. From uniform-density to clumpy regions

    Science.gov (United States)

    Marin, F.; Goosmann, R. W.; Gaskell, C. M.

    2015-05-01

    Context. A growing body of evidence suggests that some, if not all, scattering regions of active galactic nuclei (AGNs) are clumpy. The inner AGN components cannot be spatially resolved with current instruments and must be studied by numerical simulations of observed spectroscopy and polarization data. Aims: We run radiative transfer models in the optical/UV for a variety of AGN reprocessing regions with different distributions of clumpy scattering media. We obtain geometry-sensitive polarization spectra and images to improve our previous AGN models and their comparison with the observations. Methods: We use the latest public version 1.2 of the Monte Carlo code stokes presented in the first two papers of this series to model AGN reprocessing regions of increasing morphological complexity. We replace previously uniform-density media with up to thousands of constant-density clumps. We couple a continuum source to fragmented equatorial scattering regions, polar outflows, and toroidal obscuring dust regions and investigate a wide range of geometries. We also consider different levels of fragmentation in each scattering region to evaluate the importance of fragmentation for the net polarization of the AGN. Results: In comparison with uniform-density models, equatorial distributions of gas and dust clouds result in grayer spectra and show a decrease in the net polarization percentage at all lines of sight. The resulting polarization position angle depends on the morphology of the clumpy structure, with extended tori favoring parallel polarization while compact tori produce orthogonal polarization position angles. In the case of polar scattering regions, fragmentation increases the net polarization unless the cloud filling factor is small. A complete AGN model constructed from the individual, fragmented regions can produce low polarization percentages (<2%), with a parallel polarization angle for observer inclinations up to 70° for a torus half opening angle of 60°. For

  5. Density functional theory, methods, techniques, and applications

    International Nuclear Information System (INIS)

    Chretien, S.; Salahub, S.

    2001-01-01

    Important concepts of Density Functional Theory (DFT) and the different types of approximation for the exchange-correlation energy functional are presented. Applications illustrate the advantages of using DFT as a computational tool and point out some limitations as well. (authors)

  6. Solvent density mode instability in non-polar solutions

    Indian Academy of Sciences (India)

    this region produces time scales, one in the range of 1–2 ps and the other in the range of ≥10 ps for f = 4 as reported earlier [17]. Note also that both the values of f (f = 4) and density for which these two time scales are predicted are very close to the solute–solvent systems for which the experiments have reported multiple ...

  7. Nonlocal kinetic-energy-density functionals

    International Nuclear Information System (INIS)

    Garcia-Gonzalez, P.; Alvarellos, J.E.; Chacon, E.

    1996-01-01

    In this paper we present nonlocal kinetic-energy functionals T[n] within the average density approximation (ADA) framework, which do not require any extra input when applied to any electron system and recover the exact kinetic energy and the linear response function of a homogeneous system. In contrast with previous ADA functionals, these present good behavior of the long-range tail of the exact weight function. The averaging procedure for the kinetic functional (averaging the Fermi momentum of the electron gas, instead of averaging the electron density) leads to a functional without numerical difficulties in the calculation of extended systems, and it gives excellent results when applied to atoms and jellium surfaces. copyright 1996 The American Physical Society

  8. Density functional approaches to nuclear dynamics

    OpenAIRE

    Nakatsukasa, T.; Ebata, S.; Avogadro, P.; Guo, L.; Inakura, T.; Yoshida, K.

    2012-01-01

    We present background concepts of the nuclear density functional theory (DFT) and applications of the time-dependent DFT with the Skyrme energy functional for nuclear response functions. Practical methods for numerical applications of the time-dependent Hartree-Fock-Bogoliubov theory (TDHFB) are proposed; finite amplitude method and canonical-basis TDHFB. These approaches are briefly reviewed and some numerical applications are shown to demonstrate their feasibility.

  9. Versatile Density Functionals for Computational Surface Science

    DEFF Research Database (Denmark)

    Wellendorff, Jess

    resampling techniques, thereby systematically avoiding problems with overfitting. The first ever density functional presenting both reliable accuracy and convincing error estimation is generated. The methodology is general enough to be applied to more complex functional forms with higher-dimensional fitting...... and resampling. This is illustrated by searching for meta-GGA type functionals that outperform current meta-GGAs while allowing for error estimation....

  10. Periodic subsystem density-functional theory

    Science.gov (United States)

    Genova, Alessandro; Ceresoli, Davide; Pavanello, Michele

    2014-11-01

    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.

  11. Protein dynamics governed by interfaces of high polarity and low packing density.

    Directory of Open Access Journals (Sweden)

    Vladimir Espinosa Angarica

    Full Text Available The folding pathway, three-dimensional structure and intrinsic dynamics of proteins are governed by their amino acid sequences. Internal protein surfaces with physicochemical properties appropriate to modulate conformational fluctuations could play important roles in folding and dynamics. We show here that proteins contain buried interfaces of high polarity and low packing density, coined as LIPs: Light Interfaces of high Polarity, whose physicochemical properties make them unstable. The structures of well-characterized equilibrium and kinetic folding intermediates indicate that the LIPs of the corresponding native proteins fold late and are involved in local unfolding events. Importantly, LIPs can be identified using very fast and uncomplicated computational analysis of protein three-dimensional structures, which provides an easy way to delineate the protein segments involved in dynamics. Since LIPs can be retained while the sequences of the interacting segments diverge significantly, proteins could in principle evolve new functional features reusing pre-existing encoded dynamics. Large-scale identification of LIPS may contribute to understanding evolutionary constraints of proteins and the way protein intrinsic dynamics are encoded.

  12. Size and density of East Greenland polar bear (Ursus maritimus) skulls

    DEFF Research Database (Denmark)

    Sonne, Christian; Bechshoft, Thea Ø.; Rigét, Frank F.

    2013-01-01

    density (BMD) in 87 East Greenland male polar bears (Ursus maritimus) sampled in the time period of 1892-2010. The purpose of the study was to investigate if these measures are potential candidates as indicators for stress associated with climate change and long-range transported toxic industrial...... polar bear skulls continue in order to further explore how CBL and BMD reflect individual and population response upon exposure to environmental stress. (C) 2013 Elsevier Ltd. All rights reserved....

  13. Effects of polarity, hydrophobicity, and density of ionic liquids on cellulose solubility.

    Science.gov (United States)

    Abe, Mitsuru; Kuroda, Kosuke; Sato, Daiki; Kunimura, Haruhito; Ohno, Hiroyuki

    2015-12-28

    We have synthesised novel ionic liquids (ILs) to show both cellulose dissolution ability and LCST-type phase transition after mixing with water. To realise both polar and hydrophobic properties, tetraalkylphosphonium cations and a series of carboxylate anions were employed to assume hydrophobic and highly polar properties, respectively. Effects of their alkyl chain length on the water compatibility and cellulose solubility of the corresponding ILs were systematically examined. We succeeded in synthesising novel ILs which dissolve cellulose and separable with water at moderate temperature. Through the present study, we have clarified that not only polarity but also density of ILs is an important factor in designing the ILs for cellulose dissolution.

  14. Energy vs. density on paths toward exact density functionals

    DEFF Research Database (Denmark)

    Kepp, Kasper Planeta

    2018-01-01

    Recently, the progression toward more exact density functional theory has been questioned, implying a need for more formal ways to systematically measure progress, i.e. a “path”. Here I use the Hohenberg-Kohn theorems and the definition of normality by Burke et al. to define a path toward exactness...... inaccessible. To illustrate this, the systems previously studied by Medvedev et al., the first ionization energies of atoms with Z = 1 to 10, the ionization energy of water, and the bond dissociation energies of five diatomic molecules were investigated using CCSD(T)/aug-cc-pV5Z as benchmark at chemical...... accuracy. Four functionals of distinct designs was used: B3LYP, PBE, M06, and S-VWN. For atomic cations regardless of charge and compactness up to Z = 10, the energy effects of the different ρ are

  15. Large plasma density enhancements occurring in the northern polar region during the 6 April 2000 superstorm

    Science.gov (United States)

    Horvath, Ildiko; Lovell, Brian C.

    2014-06-01

    We focus on the ionospheric response of northern high-latitude region to the 6 April 2000 superstorm and aim to investigate how the storm-enhanced density (SED) plume plasma became distributed in the regions of auroral zone and polar cap plus to study the resultant ionospheric features and their development. Multi-instrument observational results combined with model-generated, two-cell convection maps permitted identifying the high-density plasma's origin and the underlying plasma transportation processes. Results show the plasma density feature of polar cap enhancement (PCE; 600 × 103 i+/cm3) appearing for 7 h during the main phase and characterized by increases reaching up to 6 times of the quiet time values. Meanwhile, strong westward convections ( 17,500 m/s) created low plasma densities in a wider region of the dusk cell. Oppositely, small ( 750 m/s) but rigorous westward drifts drove the SED plume plasma through the auroral zone, wherein plasma densities doubled. As the SED plume plasma traveled along the convection streamlines and entered the polar cap, a continuous enhancement of the tongue of ionization (TOI) developed under steady convection conditions. However, convection changes caused slow convections and flow stagnations and thus segmented the TOI feature by locally depleting the plasma in the affected regions of the auroral zone and polar cap. From the strong correspondence of polar cap potential drop and subauroral polarization stream (SAPS), we conclude that the SAPS E-field strength remained strong, and under its prolonged influence, the SED plume provided a continuous supply of downward flowing high-density plasma for the development and maintenance of PCEs.

  16. Communication: Embedded fragment stochastic density functional theory

    International Nuclear Information System (INIS)

    Neuhauser, Daniel; Baer, Roi; Rabani, Eran

    2014-01-01

    We develop a method in which the electronic densities of small fragments determined by Kohn-Sham density functional theory (DFT) are embedded using stochastic DFT to form the exact density of the full system. The new method preserves the scaling and the simplicity of the stochastic DFT but cures the slow convergence that occurs when weakly coupled subsystems are treated. It overcomes the spurious charge fluctuations that impair the applications of the original stochastic DFT approach. We demonstrate the new approach on a fullerene dimer and on clusters of water molecules and show that the density of states and the total energy can be accurately described with a relatively small number of stochastic orbitals

  17. Density functional theory studies of etoricoxib

    Science.gov (United States)

    Sachdeva, Ritika; Kaur, Prabhjot; Singh, V. P.; Saini, G. S. S.

    2016-05-01

    Etoricoxib is a COX-2 selective inhibitor drug with molecular formula C18H15ClN2O2S. It is primarily used for the treatment of arthritis(rheumatoid, psoriatic, osteoarthritis), ankylosing spondylitis, gout and chronic low back pain. Theoretical studies of the molecule including geometry optimization and vibrational frequency calculations were carried out with the help of density functional theory calculations using 6-311++ g (d, p) basis set and B3LYP functional.

  18. Chemical hardness and density functional theory

    Indian Academy of Sciences (India)

    Unknown

    (PMH) density functional theory (DFT). 1. The HSAB .... hardness. He and his colleagues had already (1978) published a pioneering paper on the application of DFT to chemical systems. What Parr showed was that for every chemical sys- tem there is a ..... open systems, since the electron affinity requires the adding of one ...

  19. Density Functional Simulation of a Breaking Nanowire

    DEFF Research Database (Denmark)

    Nakamura, A.; Brandbyge, Mads; Hansen, Lars Bruno

    1999-01-01

    We study the deformation and breaking of an atomic-sized sodium wire using density functional simulations. The wire deforms through sudden atomic rearrangements and smoother atomic displacements. The conductance of the wire exhibits plateaus at integer values in units of 2e(2)/h corresponding...

  20. Synthesis, characterization and density functional theory ...

    African Journals Online (AJOL)

    We synthesized a number of aniline derivatives containing acyl groups to compare their barriers of rotation around the N-CO groups. Geometry optimization for all the rotamers have been performed using density functional theory (DFT) at the B3LYP/6-31G** level of theory. For each stationary point we carried out vibrational ...

  1. Chemical hardness and density functional theory

    Indian Academy of Sciences (India)

    Home; Journals; Journal of Chemical Sciences; Volume 117; Issue 5. Chemical hardness and density functional theory. Ralph G Pearson. Volume 117 Issue 5 September 2005 pp 369-377. Fulltext. Click here to view fulltext PDF. Permanent link: http://www.ias.ac.in/article/fulltext/jcsc/117/05/0369-0377. Keywords. Hardness ...

  2. A new family of hybrid density functionals

    Science.gov (United States)

    Swart, Marcel

    2013-08-01

    A new family of (range-separated) hybrid functionals is presented that corrects several of the shortcomings of the recently reported SSB-D functional. The new functionals include Grimme's D3 dispersion energy, contain a reduced number of parameters which have been optimized against a number of different interaction types. When comparing the new functionals with over thirty other density functionals, the new hybrid functional S12h and its range-separated analogue CAM-S12h are found to be the best performing ones for the different interaction types. The performance for spin states is poor for the hybrid functionals, but very well for the GGA counterpart S12g.

  3. Penile density and globally used chemicals in Canadian and Greenland polar bears

    DEFF Research Database (Denmark)

    Sonne, Christian; Dyck, Markus; Rigét, Frank F

    2015-01-01

    -range dispersed and to biomagnify to very high concentrations in the tissues of Arctic apex predators such as polar bears (Ursus maritimus). A major concern relating to EDCs is their effects on vital organ-tissues such as bone and it is possible that EDCs represent a more serious challenge to the species......' survival than the more conventionally proposed prey reductions linked to climate change. We therefore analyzed penile bone mineral density (BMD) as a key phenotype for reproductive success in 279 polar bear samples born 1990-2000 representing eight polar bear subpopulations. Since EDC concentrations were...... not available from the same specimens, we compared BMD with published literature information on EDC concentrations. Latitudinal and longitudinal BMD and EDC gradients were clearly observed, with Western Hudson bears having the highest BMD and lowest EDCs, and North East Greenland polar bears carrying the lowest...

  4. Spin polarization versus color–flavor locking in high-density quark matter

    DEFF Research Database (Denmark)

    Tsue, Yasuhiko; da Providência, João; Providência, Constança

    2015-01-01

    It is shown that spin polarization with respect to each flavor in three-flavor quark matter occurs instead of color–flavor locking at high baryon density by using the Nambu–Jona-Lasinio model with four-point tensor-type interaction. Also, it is indicated that the order of phase transition between...... the color–flavor-locked phase and the spin-polarized phase is the first order by means of second-order perturbation theory.......It is shown that spin polarization with respect to each flavor in three-flavor quark matter occurs instead of color–flavor locking at high baryon density by using the Nambu–Jona-Lasinio model with four-point tensor-type interaction. Also, it is indicated that the order of phase transition between...

  5. Spin density measurement of water-bridged Co-dimer using polarized neutrons

    DEFF Research Database (Denmark)

    Damgaard-Møller, Emil; Overgaard, Jacob; Chilton, Nick

    present an experimentally determined spin density using polarized neutron diffraction in a simple water-bridged cobalt dimer [Co2(H2O)(piv)4(Hpiv)2(py)2] which is known to have a small ferromagnetic coupling between the spin centers. Visualizing the SDD could get us one step further in understanding...

  6. Spin-polarized versus chiral condensate in quark matter at finite temperature and density

    DEFF Research Database (Denmark)

    Matsuoka, Hiroaki; Tsue, Yasuhiko; da Providencia, Joao

    2016-01-01

    It is shown that the spin-polarized condensate appears in quark matter at high baryon density and low temperature due to the tensor-type four-point interaction in the Nambu-Jona-Lasiniotype model as a low-energy effective theory of quantum chromodynamics. It is indicated within this low...

  7. Isospin constraints between three cross sections and two polarization density matrices

    CERN Document Server

    Doncel, M G; Minnaert, P

    1972-01-01

    The authors give the relation which isospin conservation imposes between the three cross sections and two polarization density matrices, for three reactions related by two isospin channels. It is valid for arbitrary spin and for spin correlations. Its application to the most usual cases of spin 1 and /sup 3///sub 2/ is given. (6 refs).

  8. Linear scaling of density functional algorithms

    International Nuclear Information System (INIS)

    Stechel, E.B.; Feibelman, P.J.; Williams, A.R.

    1993-01-01

    An efficient density functional algorithm (DFA) that scales linearly with system size will revolutionize electronic structure calculations. Density functional calculations are reliable and accurate in determining many condensed matter and molecular ground-state properties. However, because current DFA's, including methods related to that of Car and Parrinello, scale with the cube of the system size, density functional studies are not routinely applied to large systems. Linear scaling is achieved by constructing functions that are both localized and fully occupied, thereby eliminating the need to calculate global eigenfunctions. It is, however, widely believed that exponential localization requires the existence of an energy gap between the occupied and unoccupied states. Despite this, the authors demonstrate that linear scaling can still be achieved for metals. Using a linear scaling algorithm, they have explicitly constructed localized, almost fully occupied orbitals for the quintessential metallic system, jellium. The algorithm is readily generalizable to any system geometry and Hamiltonian. They will discuss the conceptual issues involved, convergence properties and scaling for their new algorithm

  9. Evolution of Mars’ Northern Polar Seasonal CO2 deposits: variations in surface brightness and bulk density

    Science.gov (United States)

    Mount, Christopher P.; Titus, Timothy N.

    2015-01-01

    Small scale variations of seasonal ice are explored at different geomorphic units on the Northern Polar Seasonal Cap (NPSC). We use seasonal rock shadow measurements, combined with visible and thermal observations, to calculate density over time. The coupling of volume density and albedo allows us to determine the microphysical state of the seasonal CO2 ice. We find two distinct endmembers across the NPSC: 1) Snow deposits may anneal to form an overlying slab layer that fractures. These low density deposits maintain relatively constant densities over springtime. 2) Porous slab deposits likely anneal rapidly in early spring and fracture in late spring. These high density deposits dramatically increase in density over time. The endmembers appear to be correlated with latitude.

  10. Teaching Density Functional Theory Through Experiential Learning

    Science.gov (United States)

    Narasimhan, Shobhana

    2015-09-01

    Today, quantum mechanical density functional theory is often the method of choice for performing accurate calculations on atomic, molecular and condensed matter systems. Here, I share some of my experiences in teaching the necessary basics of solid state physics, as well as the theory and practice of density functional theory, in a number of workshops held in developing countries over the past two decades. I discuss the advantages of supplementing the usual mathematically formal teaching methods, characteristic of graduate courses, with the use of visual imagery and analogies. I also describe a successful experiment we carried out, which resulted in a joint publication co-authored by 67 lecturers and students participating in a summer school.

  11. Density functional theory a practical introduction

    CERN Document Server

    Sholl, David

    2009-01-01

    Demonstrates how anyone in math, science, and engineering can master DFT calculations Density functional theory (DFT) is one of the most frequently used computational tools for studying and predicting the properties of isolated molecules, bulk solids, and material interfaces, including surfaces. Although the theoretical underpinnings of DFT are quite complicated, this book demonstrates that the basic concepts underlying the calculations are simple enough to be understood by anyone with a background in chemistry, physics, engineering, or mathematics. The authors show how the widespread availability of powerful DFT codes makes it possible for students and researchers to apply this important computational technique to a broad range of fundamental and applied problems. Density Functional Theory: A Practical Introduction offers a concise, easy-to-follow introduction to the key concepts and practical applications of DFT, focusing on plane-wave DFT. The authors have many years of experience introducing DFT to studen...

  12. Teaching Density Functional Theory Through Experiential Learning

    International Nuclear Information System (INIS)

    Narasimhan, Shobhana

    2015-01-01

    Today, quantum mechanical density functional theory is often the method of choice for performing accurate calculations on atomic, molecular and condensed matter systems. Here, I share some of my experiences in teaching the necessary basics of solid state physics, as well as the theory and practice of density functional theory, in a number of workshops held in developing countries over the past two decades. I discuss the advantages of supplementing the usual mathematically formal teaching methods, characteristic of graduate courses, with the use of visual imagery and analogies. I also describe a successful experiment we carried out, which resulted in a joint publication co-authored by 67 lecturers and students participating in a summer school. (paper)

  13. Functionalized liquid crystal polymers generate optical and polarization vortex beams

    Science.gov (United States)

    Sakamoto, Moritsugu; Nakamoto, Yuki; Tien, Tran Minh; Kawai, Kotaro; Noda, Kohei; Sasaki, Tomoyuki; Kawatsuki, Nobuhiro; Ono, Hiroshi

    2017-08-01

    In recent year, optical and polarization vortex (OV and PV) beams, which has phase and polarization singularities, have much-attracted attention in various research fields due to their unique physical properties. In this presentation, we report our attempts for the vortex beam generation based on the photo-alignment technique of functionalized liquid crystal polymers. The OV and PV beam generations are respectively demonstrated by using azo-dye-doped liquid crystal polymers and photocrosslinkable polymer liquid crystal. Our approaches realize highly functionalized vortex beam generators which are expected to evolve the photonics applications of vortex beams.

  14. Extended screened exchange functional derived from transcorrelated density functional theory.

    Science.gov (United States)

    Umezawa, Naoto

    2017-09-14

    We propose a new formulation of the correlation energy functional derived from the transcorrelated method in use in density functional theory (TC-DFT). An effective Hamiltonian, H TC , is introduced by a similarity transformation of a many-body Hamiltonian, H, with respect to a complex function F: H TC =1FHF. It is proved that an expectation value of H TC for a normalized single Slater determinant, D n , corresponds to the total energy: E[n] = ⟨Ψ n |H|Ψ n ⟩/⟨Ψ n |Ψ n ⟩ = ⟨D n |H TC |D n ⟩ under the two assumptions: (1) The electron density nr associated with a trial wave function Ψ n = D n F is v-representable and (2) Ψ n and D n give rise to the same electron density nr. This formulation, therefore, provides an alternative expression of the total energy that is useful for the development of novel correlation energy functionals. By substituting a specific function for F, we successfully derived a model correlation energy functional, which resembles the functional form of the screened exchange method. The proposed functional, named the extended screened exchange (ESX) functional, is described within two-body integrals and is parametrized for a numerically exact correlation energy of the homogeneous electron gas. The ESX functional does not contain any ingredients of (semi-)local functionals and thus is totally free from self-interactions. The computational cost for solving the self-consistent-field equation is comparable to that of the Hartree-Fock method. We apply the ESX functional to electronic structure calculations for a solid silicon, H - ion, and small atoms. The results demonstrate that the TC-DFT formulation is promising for the systematic improvement of the correlation energy functional.

  15. Reduced density matrix functional theory at finite temperature

    Energy Technology Data Exchange (ETDEWEB)

    Baldsiefen, Tim

    2012-10-15

    Density functional theory (DFT) is highly successful in many fields of research. There are, however, areas in which its performance is rather limited. An important example is the description of thermodynamical variables of a quantum system in thermodynamical equilibrium. Although the finite-temperature version of DFT (FT-DFT) rests on a firm theoretical basis and is only one year younger than its brother, groundstate DFT, it has been successfully applied to only a few problems. Because FT-DFT, like DFT, is in principle exact, these shortcomings can be attributed to the difficulties of deriving valuable functionals for FT-DFT. In this thesis, we are going to present an alternative theoretical description of quantum systems in thermal equilibrium. It is based on the 1-reduced density matrix (1RDM) of the system, rather than on its density and will rather cumbersomly be called finite-temperature reduced density matrix functional theory (FT-RDMFT). Its zero-temperature counterpart (RDMFT) proved to be successful in several fields, formerly difficult to address via DFT. These fields include, for example, the calculation of dissociation energies or the calculation of the fundamental gap, also for Mott insulators. This success is mainly due to the fact that the 1RDM carries more directly accessible ''manybody'' information than the density alone, leading for example to an exact description of the kinetic energy functional. This sparks the hope that a description of thermodynamical systems employing the 1RDM via FT-RDMFT can yield an improvement over FT-DFT. Giving a short review of RDMFT and pointing out difficulties when describing spin-polarized systems initiates our work. We then lay the theoretical framework for FT-RDMFT by proving the required Hohenberg-Kohn-like theorems, investigating and determining the domain of FT-RDMFT functionals and by deriving several properties of the exact functional. Subsequently, we present a perturbative method to

  16. Reduced density matrix functional theory at finite temperature

    International Nuclear Information System (INIS)

    Baldsiefen, Tim

    2012-10-01

    Density functional theory (DFT) is highly successful in many fields of research. There are, however, areas in which its performance is rather limited. An important example is the description of thermodynamical variables of a quantum system in thermodynamical equilibrium. Although the finite-temperature version of DFT (FT-DFT) rests on a firm theoretical basis and is only one year younger than its brother, groundstate DFT, it has been successfully applied to only a few problems. Because FT-DFT, like DFT, is in principle exact, these shortcomings can be attributed to the difficulties of deriving valuable functionals for FT-DFT. In this thesis, we are going to present an alternative theoretical description of quantum systems in thermal equilibrium. It is based on the 1-reduced density matrix (1RDM) of the system, rather than on its density and will rather cumbersomly be called finite-temperature reduced density matrix functional theory (FT-RDMFT). Its zero-temperature counterpart (RDMFT) proved to be successful in several fields, formerly difficult to address via DFT. These fields include, for example, the calculation of dissociation energies or the calculation of the fundamental gap, also for Mott insulators. This success is mainly due to the fact that the 1RDM carries more directly accessible ''manybody'' information than the density alone, leading for example to an exact description of the kinetic energy functional. This sparks the hope that a description of thermodynamical systems employing the 1RDM via FT-RDMFT can yield an improvement over FT-DFT. Giving a short review of RDMFT and pointing out difficulties when describing spin-polarized systems initiates our work. We then lay the theoretical framework for FT-RDMFT by proving the required Hohenberg-Kohn-like theorems, investigating and determining the domain of FT-RDMFT functionals and by deriving several properties of the exact functional. Subsequently, we present a perturbative method to iteratively construct

  17. Density Functional Theory An Advanced Course

    CERN Document Server

    Dreizler, Reiner M

    2011-01-01

    Density Functional Theory (DFT) has firmly established itself as the workhorse for the atomic-level simulation of condensed matter phases, pure or composite materials and quantum chemical systems. The present book is a rigorous and detailed introduction to the foundations up to and including such advanced topics as orbital-dependent functionals and both time-dependent and relativistic DFT. Given the many ramifications of contemporary DFT, this text concentrates on the self-contained presentation of the basics of the most widely used DFT variants. This implies a thorough discussion of the corresponding existence theorems and effective single particle equations, as well as of key approximations utilized in implementations. The formal results are complemented by selected quantitative results, which primarily aim at illustrating strengths and weaknesses of a particular approach or functional. DFT for superconducting or nuclear and hadronic systems are not addressed in this work. The structure and material contain...

  18. What can we learn from polarized structure function data?

    CERN Document Server

    Ball, Richard D.; Altarelli, Guido; Forte, Stefano; Ball, Richard D.; Ridolfi, Giovanni; Altarelli, Guido; Forte, Stefano

    1997-04-20

    We summarise the perturbative QCD analysis of the structure function data for g_1 from longitudinally polarized deep inelastic scattering from proton, deuteron and neutron targets, with particular emphasis on testing sum rules, determining helicity fractions, and extracting the strong coupling from both scaling violations and the Bjorken sum rule.

  19. Covariant density functional theory for nuclear matter

    International Nuclear Information System (INIS)

    Badarch, U.

    2007-01-01

    The present thesis is organized as follows. In Chapter 2 we study the Nucleon-Nucleon (NN) interaction in Dirac-Brueckner (DB) approach. We start by considering the NN interaction in free-space in terms of the Bethe-Salpeter (BS) equation to the meson exchange potential model. Then we present the DB approach for nuclear matter by extending the BS equation for the in-medium NN interaction. From the solution of the three-dimensional in-medium BS equation, we derive the DB self-energies and total binding energy which are the main results of the DB approach, which we later incorporate in the field theoretical calculation of the nuclear equation of state. In Chapter 3, we introduce the basic concepts of density functional theory in the context of Quantum Hadrodynamics (QHD-I). We reach the main point of this work in Chapter 4 where we introduce the DDRH approach. In the DDRH theory, the medium dependence of the meson-nucleon vertices is expressed as functionals of the baryon field operators. Because of the complexities of the operator-valued functionals we decide to use the mean-field approximation. In Chapter 5, we contrast microscopic and phenomenological approaches to extracting density dependent meson-baryon vertices. Chapter 6 gives the results of our studies of the EOS of infinite nuclear matter in detail. Using formulas derived in Chapters 4 and 5 we calculate the properties of symmetric and asymmetric nuclear matter and pure neutron matter. (orig.)

  20. Covariant density functional theory for nuclear matter

    Energy Technology Data Exchange (ETDEWEB)

    Badarch, U.

    2007-07-01

    The present thesis is organized as follows. In Chapter 2 we study the Nucleon-Nucleon (NN) interaction in Dirac-Brueckner (DB) approach. We start by considering the NN interaction in free-space in terms of the Bethe-Salpeter (BS) equation to the meson exchange potential model. Then we present the DB approach for nuclear matter by extending the BS equation for the in-medium NN interaction. From the solution of the three-dimensional in-medium BS equation, we derive the DB self-energies and total binding energy which are the main results of the DB approach, which we later incorporate in the field theoretical calculation of the nuclear equation of state. In Chapter 3, we introduce the basic concepts of density functional theory in the context of Quantum Hadrodynamics (QHD-I). We reach the main point of this work in Chapter 4 where we introduce the DDRH approach. In the DDRH theory, the medium dependence of the meson-nucleon vertices is expressed as functionals of the baryon field operators. Because of the complexities of the operator-valued functionals we decide to use the mean-field approximation. In Chapter 5, we contrast microscopic and phenomenological approaches to extracting density dependent meson-baryon vertices. Chapter 6 gives the results of our studies of the EOS of infinite nuclear matter in detail. Using formulas derived in Chapters 4 and 5 we calculate the properties of symmetric and asymmetric nuclear matter and pure neutron matter. (orig.)

  1. Modulation Based on Probability Density Functions

    Science.gov (United States)

    Williams, Glenn L.

    2009-01-01

    A proposed method of modulating a sinusoidal carrier signal to convey digital information involves the use of histograms representing probability density functions (PDFs) that characterize samples of the signal waveform. The method is based partly on the observation that when a waveform is sampled (whether by analog or digital means) over a time interval at least as long as one half cycle of the waveform, the samples can be sorted by frequency of occurrence, thereby constructing a histogram representing a PDF of the waveform during that time interval.

  2. Density functional and neural network analysis

    DEFF Research Database (Denmark)

    Jalkanen, K. J.; Suhai, S.; Bohr, Henrik

    1997-01-01

    Density functional theory (DFT) calculations have been carried out for hydrated L-alanine, L-alanyl-L-alanine and N-acetyl L-alanine N'-methylamide and examined with respect to the effect of water on the structure, the vibrational frequencies, vibrational absorption (VA) and vibrational circular...... dichroism (VCD) intensities. The large changes due to hydration on the structures, relative stability of conformers, and in the VA and VCD spectra observed experimentally are reproduced by the DFT calculations. Furthermore a neural network was constructed for reproducing the inverse scattering data (infer...

  3. A density functional study of backbone structures of polydiacetylene: destabilization of butatriene structure

    International Nuclear Information System (INIS)

    Katagiri, Hideki; Shimoi, Yukihiro; Abe, Shuji

    2004-01-01

    Backbone structures of polydiacetylene are studied with first-principles electronic structure method using plane-waves within generalized gradient approximation (GGA) of density functional theory. In spin-restricted calculations a coarse k-point sampling gives a potential energy curve with two local minima corresponding to acetylene and butatriene structures. However, the potential barrier between the two structures rapidly decreases with increasing number of k-points, which results in destabilization of the butatriene structure. Spin polarization effects also destabilize the butatriene structure, inducing atom-centered spin-density-wave state. These potential energies were compared with those obtained by Hartree-Fock, density functional within local density approximation (LDA) and GGA, and hybrid density functional methods using a gaussian basis set. The comparison shows that the density functional methods within LDA and GGA favor the destabilization of the butatriene structure in contrast to the Hartree-Fock method

  4. Polarization Potential Has No Effect on Maximum Current Density Produced by Halotolerant Bioanodes

    Directory of Open Access Journals (Sweden)

    Muriel González-Muñoz

    2018-03-01

    Full Text Available Halotolerant bioanodes are considered an attractive alternative in microbial electrochemical systems, as they can operate under higher conductive electrolytes, in comparison with traditional wastewater and freshwater bioanodes. The dependency between energetic performance and polarization potential has been addressed in several works; however the vast majority discusses its effect when wastewater or freshwater inocula are employed, and fewer reports focus on inocula from highly-saline environments. Moreover, the effect of the polarization potential on current production is not fully understood. To determine if the polarization potential has a significant effect on current production, eight bioanodes were grown by chronoamperometry at positive and negative potentials relative to the reference electrode (+0.34 V/SHE and −0.16 V/SHE, in a three-electrode set-up employing sediments from a hyperhaline coastal lagoon. The maximum current density obtained was the same, despite the differences in the applied potential. Our findings indicate that even if differences in organic matter removal and coulombic efficiency are obtained, the polarization potential had no statistically significant effect on overall current density production.

  5. Thermal inertia and radar reflectivity of the Martian north polar ERG: Low-density aggregates

    Science.gov (United States)

    Herkenhoff, K. E.

    1993-01-01

    The north polar layered deposits on Mars appear to be the source of the dark material that comprises the north polar erg. The physical properties and chemical composition of the erg material therefore have important implications for the origin and evolution of the Martian layered deposits. Viking bistatic radar and infrared thermal mapping (IRTM) data indicate that the bulk density of the erg material is lower than that of the average Martian surface. These data are consistent with hypotheses involving formation of filamentary sublimation residue (FSR) particles from erosion of the layered deposits. The color and albedo of the erg and of the layered deposits, and the presence of magnetic material on Mars, suggest that the dark material is composed of low-density aggregates of magnetic dust grains, perhaps similar to FSR particles created in laboratory experiments.

  6. Screening in orbital-density-dependent functionals.

    Science.gov (United States)

    Colonna, Nicola; Nguyen, Ngoc Linh; Ferretti, Andrea; Marzari, Nicola

    2018-03-01

    Electronic-structure functionals that include screening effects, such as Hubbard or Koopmans' functionals, require to describe the response of a system to the fractional addition or removal of an electron from an orbital or a manifold. Here, we present a general method to incorporate screening based on linear-response theory, and we apply it to the case of the orbital-by-orbital screening of Koopmans' functionals. We illustrate the importance of such generalization when dealing with challenging systems containing orbitals with very different chemical character, also highlighting the simple dependence of the screening on the localization of the orbitals. We choose a set of 46 transition-metal complexes for which experimental data and accurate many-body perturbation theory calculations are available. When compared to experiment, results for ionization potentials show a very good performance with a mean absolute error of $~0.2$ eV, comparable to the most accurate many-body perturbation theory approaches. These results reiterate the role of Koopmans' compliant functionals as simple and accurate quasiparticle approximations to the exact spectral functional, bypassing diagrammatic expansions and relying only on the physics of the local density or generalized-gradient approximation.

  7. Functional conservation study of polarity protein Crumbs intracellular domain.

    Science.gov (United States)

    Shi, Qi-ping; Cao, Hao-wei; Xu, Rui; Zhang, Dan-dan; Huang, Juan

    2017-01-20

    The transmembrane protein Crumbs (Crb) plays key roles in the establishing and maintaining cell apical-basal polarity in epithelial cells by determining the apical plasma membrane identity. Although its intracellular domain contains only 37 amino acids, it is absolutely essential for its function. In Drosophila, mutations in this intracellular domain result in severe defects in epithelial polarity and abnormal embryonic development. The intracellular domain of Crb shows high homology across species from Drosophila to Mus musculus and Homo sapiens. However, the intracellular domains of the two Crb proteins in C. elegans are rather divergent from those of Drosophila and mammals, raising the question on whether the function of the intracellular domain of the Crb protein is conserved in C. elegans. Using genomic engineering approach, we replaced the intracellular domain of the Drosophila Crb with that of C. elegans Crb2 (CeCrb2), which has extremely low homology with those from the Crb proteins of Drosophila and mammals. Surprisingly, substituting the intracellular domain of Drosophila Crb with that of CeCrb2 did not cause any abnormalities in development of the Drosophila embryo, in terms of expression and localization of Crb and other polarity proteins and apical-basal polarity in embryonic epithelial cells. Our results support the notion that despite their extensive sequence variations, all functionally critical amino acid residues and motifs of the intercellular domain of Crb proteins are fully conserved between Drosophila and C. elegans.

  8. Density functional theory and an experimentally-designed energy functional of electron density.

    Science.gov (United States)

    Miranda, David A; Bueno, Paulo R

    2016-09-21

    We herein demonstrate that capacitance spectroscopy (CS) experimentally allows access to the energy associated with the quantum mechanical ground state of many-electron systems. Priorly, electrochemical capacitance, C [small mu, Greek, macron] [ρ], was previously understood from conceptual and computational density functional theory (DFT) calculations. Thus, we herein propose a quantum mechanical experiment-based variational method for electron charging processes based on an experimentally-designed functional of the ground state electron density. In this methodology, the electron state density, ρ, and an energy functional of the electron density, E [small mu, Greek, macron] [ρ], can be obtained from CS data. CS allows the derivative of the electrochemical potential with respect to the electron density, (δ[small mu, Greek, macron][ρ]/δρ), to be obtained as a unique functional of the energetically minimised system, i.e., β/C [small mu, Greek, macron] [ρ], where β is a constant (associated with the size of the system) and C [small mu, Greek, macron] [ρ] is an experimentally observable quantity. Thus the ground state energy (at a given fixed external potential) can be obtained simply as E [small mu, Greek, macron] [ρ], from the experimental measurement of C [small mu, Greek, macron] [ρ]. An experimental data-set was interpreted to demonstrate the potential of this quantum mechanical experiment-based variational principle.

  9. Time-dependent quantum fluid density functional theory of hydrogen ...

    Indian Academy of Sciences (India)

    dependent density; density functional theory; quantum fluid dynamics. ... (HHG) is also examined. The present approach goes beyond the linear response formalism and, in principle, calculates the TD electron density to all orders of change.

  10. Development of high-polarization Fe/Ge neutron polarizing supermirror: Possibility of fine-tuning of scattering length density in ion beam sputtering

    Science.gov (United States)

    Maruyama, R.; Yamazaki, D.; Akutsu, K.; Hanashima, T.; Miyata, N.; Aoki, H.; Takeda, M.; Soyama, K.

    2018-04-01

    The multilayer structure of Fe/Si and Fe/Ge systems fabricated by ion beam sputtering (IBS) was investigated using X-ray and polarized neutron reflectivity measurements and scanning transmission electron microscopy with energy-dispersive X-ray analysis. The obtained result revealed that the incorporation of sputtering gas particles (Ar) in the Ge layer gives rise to a marked reduction in the neutron scattering length density (SLD) and contributes to the SLD contrast between the Fe and Ge layers almost vanishing for spin-down neutrons. Bundesmann et al. (2015) have shown that the implantation of primary Ar ions backscattered at the target is responsible for the incorporation of Ar particles and that the fraction increases with increasing ion incidence angle and increasing polar emission angle. This leads to a possibility of fine-tuning of the SLD for the IBS, which is required to realize a high polarization efficiency of a neutron polarizing supermirror. Fe/Ge polarizing supermirror with m = 5 fabricated under the same condition showed a spin-up reflectivity of 0.70 at the critical momentum transfer. The polarization was higher than 0.985 for the qz range where the correction for the polarization inefficiencies of the beamline works properly. The result of the polarized neutron reflectivity measurement suggests that the "magnetically-dead" layers formed at both sides of the Fe layer, together with the SLD contrast, play a critical role in determining the polarization performance of a polarizing supermirror.

  11. When combined X-ray and polarized neutron diffraction data challenge high-level calculations: spin-resolved electron density of an organic radical.

    Science.gov (United States)

    Voufack, Ariste Bolivard; Claiser, Nicolas; Lecomte, Claude; Pillet, Sébastien; Pontillon, Yves; Gillon, Béatrice; Yan, Zeyin; Gillet, Jean Michel; Marazzi, Marco; Genoni, Alessandro; Souhassou, Mohamed

    2017-08-01

    Joint refinement of X-ray and polarized neutron diffraction data has been carried out in order to determine charge and spin density distributions simultaneously in the nitronyl nitroxide (NN) free radical Nit(SMe)Ph. For comparison purposes, density functional theory (DFT) and complete active-space self-consistent field (CASSCF) theoretical calculations were also performed. Experimentally derived charge and spin densities show significant differences between the two NO groups of the NN function that are not observed from DFT theoretical calculations. On the contrary, CASSCF calculations exhibit the same fine details as observed in spin-resolved joint refinement and a clear asymmetry between the two NO groups.

  12. Chiroptical Properties of Amino Acids: A Density Functional Theory Study

    Directory of Open Access Journals (Sweden)

    Martine Adrian-Scotto

    2010-04-01

    Full Text Available Amino acids are involved in many scientific theories elucidating possible origins of life on Earth. One of the challenges when discussing the evolutionary origin of biopolymers such as proteins and oligonucleotides in living organisms is the phenomenon that these polymers implement monomers of exclusively one handedness, a feature called biomolecular homochirality. Many attempts have been made to understand this process of racemic symmetry breaking. Assuming an extraterrestrial origin of the molecular building blocks of living organisms, their susceptibility to asymmetric photolysis by the absorption of circularly polarized electromagnetic radiation in interstellar space was proposed. In order to predict whether the interaction of circularly polarized light with various racemic amino acids can induce an enantiomeric excess, we investigated the electronic and chiroptical properties of the amino acids valine and isovaline by a molecular modelling approach based on quantum chemistry (Density Functional Theory. The average spectra of both L-valine and L-isovaline have been produced on the basis of Boltzmann population analysis using computed spectra for the various conformations of each amino acid.

  13. Decay of autoionizing states in time-dependent density functional and reduced density matrix functional theory

    Energy Technology Data Exchange (ETDEWEB)

    Kapoor, Varun; Brics, Martins; Bauer, Dieter [Institut fuer Physik, Universitaet Rostock, 18051 Rostock (Germany)

    2013-07-01

    Autoionizing states are inaccessible to time-dependent density functional theory (TDDFT) using known, adiabatic Kohn-Sham (KS) potentials. We determine the exact KS potential for a numerically exactly solvable model Helium atom interacting with a laser field that is populating an autoionizing state. The exact single-particle density of the population in the autoionizing state corresponds to that of the energetically lowest quasi-stationary state in the exact KS potential. We describe how this exact potential controls the decay by a barrier whose height and width allows for the density to tunnel out and decay with the same rate as in the ab initio time-dependent Schroedinger calculation. However, devising a useful exchange-correlation potential that is capable of governing such a scenario in general and in more complex systems is hopeless. As an improvement over TDDFT, time-dependent reduced density matrix functional theory has been proposed. We are able to obtain for the above described autoionization process the exact time-dependent natural orbitals (i.e., the eigenfunctions of the exact, time-dependent one-body reduced density matrix) and study the potentials that appear in the equations of motion for the natural orbitals and the structure of the two-body density matrix expanded in them.

  14. Chemistry by Way of Density Functional Theory

    Science.gov (United States)

    Bauschlicher, Charles W., Jr.; Ricca, Alessandra; Partridge, Harry; Langohff, Stephen R.; Arnold, James O. (Technical Monitor)

    1996-01-01

    In this work we demonstrate that density functional theory (DFT) methods make an important contribution to understanding chemical systems and are an important additional method for the computational chemist. We report calibration calculations obtained with different functionals for the 55 G2 molecules to justify our selection of the B3LYP functional. We show that accurate geometries and vibrational frequencies obtained at the B3LYP level can be combined with traditional methods to simplify the calculation of accurate heats of formation. We illustrate the application of the B3LYP approach to a variety of chemical problems from the vibrational frequencies of polycyclic aromatic hydrocarbons to transition metal systems. We show that the B3LYP method typically performs better than the MP2 method at a significantly lower computational cost. Thus the B3LYP method allows us to extend our studies to much larger systems while maintaining a high degree of accuracy. We show that for transition metal systems, the B3LYP bond energies are typically of sufficient accuracy that they can be used to explain experimental trends and even differentiate between different experimental values. We show that for boron clusters the B3LYP energetics are not as good as for many of the other systems presented, but even in this case the B3LYP approach is able to help understand the experimental trends.

  15. Microbial diversity and functional capacity in polar soils.

    Science.gov (United States)

    Makhalanyane, Thulani Peter; Van Goethem, Marc Warwick; Cowan, Don Arthur

    2016-04-01

    Global change is disproportionately affecting cold environments (polar and high elevation regions), with potentially negative impacts on microbial diversity and functional processes. In most cold environments the combination of low temperatures, and physical stressors, such as katabatic wind episodes and limited water availability result in biotic systems, which are in trophic terms very simple and primarily driven by microbial communities. Metagenomic approaches have provided key insights on microbial communities in these systems and how they may adapt to stressors and contribute towards mediating crucial biogeochemical cycles. Here we review, the current knowledge regarding edaphic-based microbial diversity and functional processes in Antarctica, and the Artic. Such insights are crucial and help to establish a baseline for understanding the impact of climate change on Polar Regions. Copyright © 2016 Elsevier Ltd. All rights reserved.

  16. Imaging of fast moving electron-density structures in the polar cap

    Directory of Open Access Journals (Sweden)

    C. N. Mitchell

    2007-06-01

    Full Text Available The imaging of fast-moving electron-density structures in the polar cap presents a unique set of challenges that are not encountered in other ionospheric imaging problems. GPS observations of total electron content in the polar cap are sparse compared to other regions in the Northern Hemisphere. Furthermore, the slow relative motion of the satellites across the sky complicates the problem since the velocity of the plasma can be large in comparison and traditional approaches could result in image blurring. This paper presents a Kalman-filter based method that incorporates a forward projection of the solution based on a model plasma drift velocity field. This is the first time that the plasma motion, rather than just integrations of electron density, has been used in an ionospheric imaging algorithm. The motion is derived from the Weimer model of the electric field. It is shown that this novel approach to the implementation of a Kalman filter provides a detailed view of the polar cap ionosphere under severe storm conditions. A case study is given for the October 2003 Halloween storm where verification is provided by incoherent scatter radars.

  17. Occurrence Locations, Dipole Tilt Angle Effects, and Plasma Cloud Drift Paths of Polar Cap Neutral Density Anomalies

    Science.gov (United States)

    Lin, C. S.; Sutton, E. K.; Huang, C. Y.; Cooke, D. L.

    2018-02-01

    Polar cap neutral density anomaly (PCNDA) with large mass density enhancements over the background has been frequently observed in the polar cap during magnetic storms. By tracing field lines to the magnetosphere from the polar ionosphere, we divide the polar cap into two regions, an open field line (OFL) region with field lines connecting to the magnetopause boundary and a distant tail field line (TFL) region threaded with magnetotail lobe field lines. A statistical study of neutral density observed by the Challenging Minisatellite Payload satellite during major magnetic storms with Dst atmospheric disturbance could be generated in the nightside polar cap. From the PCNDA size and speed of sound at 400 km, we derive an initial energy deposition duration for producing traveling atmospheric disturbance in the range from 0.5 to 2.5 hr.

  18. Building a Universal Nuclear Energy Density Functional

    Energy Technology Data Exchange (ETDEWEB)

    Carlson, Joe A. [Michigan State Univ., East Lansing, MI (United States); 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.

  19. Local-scaling density-functional method: Intraorbit and interorbit density optimizations

    International Nuclear Information System (INIS)

    Koga, T.; Yamamoto, Y.; Ludena, E.V.

    1991-01-01

    The recently proposed local-scaling density-functional theory provides us with a practical method for the direct variational determination of the electron density function ρ(r). The structure of ''orbits,'' which ensures the one-to-one correspondence between the electron density ρ(r) and the N-electron wave function Ψ({r k }), is studied in detail. For the realization of the local-scaling density-functional calculations, procedures for intraorbit and interorbit optimizations of the electron density function are proposed. These procedures are numerically illustrated for the helium atom in its ground state at the beyond-Hartree-Fock level

  20. Orbital functionals in density-matrix- and current-density-functional theory

    Energy Technology Data Exchange (ETDEWEB)

    Helbig, N.

    2006-05-15

    Density-Functional Theory (DFT), although widely used and very successful in the calculation of several observables, fails to correctly describe strongly correlated materials. In the first part of this work we, therefore, introduce reduced-densitymatrix- functional theory (RDMFT) which is one possible way to treat electron correlation beyond DFT. Within this theory the one-body reduced density matrix (1- RDM) is used as the basic variable. Our main interest is the calculation of the fundamental gap which proves very problematic within DFT. In order to calculate the fundamental gap we generalize RDMFT to fractional particle numbers M by describing the system as an ensemble of an N and an N+1 particle system (with N{<=}M{<=}N+1). For each fixed particle number, M, the total energy is minimized with respect to the natural orbitals and their occupation numbers. This leads to the total energy as a function of M. The derivative of this function with respect to the particle number has a discontinuity at integer particle number which is identical to the gap. In addition, we investigate the necessary and sufficient conditions for the 1- RDM of a system with fractional particle number to be N-representable. Numerical results are presented for alkali atoms, small molecules, and periodic systems. Another problem within DFT is the description of non-relativistic many-electron systems in the presence of magnetic fields. It requires the paramagnetic current density and the spin magnetization to be used as basic variables besides the electron density. However, electron-gas-based functionals of current-spin-density-functional Theory (CSDFT) exhibit derivative discontinuities as a function of the magnetic field whenever a new Landau level is occupied, which makes them difficult to use in practice. Since the appearance of Landau levels is, intrinsically, an orbital effect it is appealing to use orbital-dependent functionals. We have developed a CSDFT version of the optimized

  1. [Particle Size and Number Density Online Analysis for Particle Suspension with Polarization-Differentiation Elastic Light Scattering Spectroscopy].

    Science.gov (United States)

    Chen, Wei-kang; Fang, Hui

    2016-03-01

    The basic principle of polarization-differentiation elastic light scattering spectroscopy based techniques is that under the linear polarized light incidence, the singlely scattered light from the superficial biological tissue and diffusively scattered light from the deep tissue can be separated according to the difference of polarization characteristics. The novel point of the paper is to apply this method to the detection of particle suspension and, to realize the simultaneous measurement of its particle size and number density in its natural status. We design and build a coaxial cage optical system, and measure the backscatter signal at a specified angle from a polystyrene microsphere suspension. By controlling the polarization direction of incident light with a linear polarizer and adjusting the polarization direction of collected light with another linear polarizer, we obtain the parallel polarized elastic light scattering spectrum and cross polarized elastic light scattering spectrum. The difference between the two is the differential polarized elastic light scattering spectrum which include only the single scattering information of the particles. We thus compare this spectrum to the Mie scattering calculation and extract the particle size. We then also analyze the cross polarized elastic light scattering spectrum by applying the particle size already extracted. The analysis is based on the approximate expressions taking account of light diffusing, from which we are able to obtain the number density of the particle suspension. We compare our experimental outcomes with the manufacturer-provided values and further analyze the influence of the particle diameter standard deviation on the number density extraction, by which we finally verify the experimental method. The potential applications of the method include the on-line particle quality monitoring for particle manufacture as well as the fat and protein density detection of milk products.

  2. Free energy functionals for polarization fluctuations: Pekar factor revisited.

    Science.gov (United States)

    Dinpajooh, Mohammadhasan; Newton, Marshall D; Matyushov, Dmitry V

    2017-02-14

    The separation of slow nuclear and fast electronic polarization in problems related to electron mobility in polarizable media was considered by Pekar 70 years ago. Within dielectric continuum models, this separation leads to the Pekar factor in the free energy of solvation by the nuclear degrees of freedom. The main qualitative prediction of Pekar's perspective is a significant, by about a factor of two, drop of the nuclear solvation free energy compared to the total (electronic plus nuclear) free energy of solvation. The Pekar factor enters the solvent reorganization energy of electron transfer reactions and is a significant mechanistic parameter accounting for the solvent effect on electron transfer. Here, we study the separation of the fast and slow polarization modes in polar molecular liquids (polarizable dipolar liquids and polarizable water force fields) without relying on the continuum approximation. We derive the nonlocal free energy functional and use atomistic numerical simulations to obtain nonlocal, reciprocal space electronic and nuclear susceptibilities. A consistent transition to the continuum limit is introduced by extrapolating the results of finite-size numerical simulation to zero wavevector. The continuum nuclear susceptibility extracted from the simulations is numerically close to the Pekar factor. However, we derive a new functionality involving the static and high-frequency dielectric constants. The main distinction of our approach from the traditional theories is found in the solvation free energy due to the nuclear polarization: the anticipated significant drop of its magnitude with increasing liquid polarizability does not occur. The reorganization energy of electron transfer is either nearly constant with increasing the solvent polarizability and the corresponding high-frequency dielectric constant (polarizable dipolar liquids) or actually noticeably increases (polarizable force fields of water).

  3. Free energy functionals for polarization fluctuations: Pekar factor revisited

    International Nuclear Information System (INIS)

    Dinpajooh, Mohammadhasan; Newton, Marshall D.; Matyushov, Dmitry V.

    2017-01-01

    The separation of slow nuclear and fast electronic polarization in problems related to electron mobility in polarizable media was considered by Pekar 70 years ago. This separation leads to the Pekar factor in the free energy of solvation by the nuclear degrees of freedom, within dielectric continuum models. The main qualitative prediction of Pekar’s perspective is a significant, by about a factor of two, drop of the nuclear solvation free energy compared to the total (electronic plus nuclear) free energy of solvation. The Pekar factor enters the solvent reorganization energy of electron transfer reactions and is a significant mechanistic parameter accounting for the solvent effect on electron transfer. We study the separation of the fast and slow polarization modes in polar molecular liquids (polarizable dipolar liquids and polarizable water force fields) without relying on the continuum approximation. We derive the nonlocal free energy functional and use atomistic numerical simulations to obtain nonlocal, reciprocal space electronic and nuclear susceptibilities. A consistent transition to the continuum limit is introduced by extrapolating the results of finite-size numerical simulation to zero wavevector. The continuum nuclear susceptibility extracted from the simulations is numerically close to the Pekar factor. But, we derive a new functionality involving the static and high-frequency dielectric constants. The main distinction of our approach from the traditional theories is found in the solvation free energy due to the nuclear polarization: the anticipated significant drop of its magnitude with increasing liquid polarizability does not occur. The reorganization energy of electron transfer is either nearly constant with increasing the solvent polarizability and the corresponding high-frequency dielectric constant (polarizable dipolar liquids) or actually noticeably increases (polarizable force fields of water).

  4. The Density of the North Polar Layered Deposit from Gravity and Topography

    Science.gov (United States)

    Ojha, L.; Lewis, K. W.

    2017-12-01

    The North Polar Layered Deposit (NPLD) of Mars is a vast reservoir of water ice with a volume of 1.14 million km3. Radar data indicates that the ice in the NPLD is extremely pure with dust content between 5 % to 10 %, however the radar data has not been able to put a direct constraint on the density of the NPLD. Here, we localize the gravity and topography signature of the NPLD and place a direct constraint on its density. We performed a grid search by generating admittance spectrum at each latitude and longitude between 75° N to 90° N and 0° E to 360° E, using a spherical cap of angular radius () of 7°, and a harmonic-bandwidth of the localization window Lwin of 37°. A region between Gemina Lingula and Planum Boreum was found to possesss an adequate correlation between gravity and topography. The estimated admittance spectra were compared with synthetic admittance spectra to constrain the load-density and the elastic thickness of the lithosphere. We constructed forward models by assuming that the lithosphere is a thin shell that deforms elastically in response to surface loads. We find that the bulk density of the NPLD ranges between 1000 to 1100 kg.m-3. Assuming a grain density of 3000 kg.m-3 for dust, the NPLD region within our localized window can contain dust content between 3 - 8 %, which is in an excellent agreement with the radar data.

  5. Functional polarization of neuroglia: Implications in neuroinflammation and neurological disorders.

    Science.gov (United States)

    Jha, Mithilesh Kumar; Lee, Won-Ha; Suk, Kyoungho

    2016-03-01

    Recent neuroscience research has established the adult brain as a dynamic organ having a unique ability to undergo changes with time. Neuroglia, especially microglia and astrocytes, provide dynamicity to the brain. Activation of these glial cells is a major component of the neuroinflammatory responses underlying brain injury and neurodegeneration. Glial cells execute functional reaction programs in response to diverse microenvironmental signals manifested by neuropathological conditions. Activated microglia exist along a continuum of two functional states of polarization namely M1-type (classical/proinflammatory activation) and M2-type (alternative/anti-inflammatory activation) as in macrophages. The balance between classically and alternatively activated microglial phenotypes influences disease progression in the CNS. The classically activated state of microglia drives the neuroinflammatory response and mediates the detrimental effects on neurons, whereas in their alternative activation state, which is apparently a beneficial activation state, the microglia play a crucial role in tissue maintenance and repair. Likewise, in response to immune or inflammatory microenvironments astrocytes also adopt neurotoxic or neuroprotective phenotypes. Reactive astrocytes exhibit two distinctive functional phenotypes defined by pro- or anti-inflammatory gene expression profile. In this review, we have thoroughly covered recent advances in the understanding of the functional polarization of brain and peripheral glia and its implications in neuroinflammation and neurological disorders. The identifiable phenotypes adopted by neuroglia in response to specific insult or injury can be exploited as promising diagnostic markers of neuroinflammatory diseases. Furthermore, harnessing the beneficial effects of the polarized glia could undoubtedly pave the way for the formulation of novel glia-based therapeutic strategies for diverse neurological disorders. Copyright © 2015 Elsevier Inc

  6. Density functional theory and multiscale materials modeling

    Indian Academy of Sciences (India)

    One of the vital ingredients in the theoretical tools useful in materials modeling at all the length scales of interest is the concept of density. In the microscopic length scale, it is the electron density that has played a major role in providing a deeper understanding of chemical binding in atoms, molecules and solids.

  7. Graphene on metals: A van der Waals density functional study

    DEFF Research Database (Denmark)

    Vanin, Marco; Mortensen, Jens Jørgen; Kelkkanen, Kari André

    2010-01-01

    We use density functional theory (DFT) with a recently developed van der Waals density functional (vdW-DF) to study the adsorption of graphene on Co, Ni, Pd, Ag, Au, Cu, Pt, and Al(111) surfaces. In contrast to the local-density approximation (LDA) which predicts relatively strong binding for Ni...

  8. Magnetized Reverse Shock: Density-fluctuation-induced Field Distortion, Polarization Degree Reduction, and Application to GRBs

    Energy Technology Data Exchange (ETDEWEB)

    Deng Wei; Zhang Bing [Department of Physics and Astronomy, University of Nevada Las Vegas, Las Vegas, NV 89154 (United States); Li Hui [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Stone, James M., E-mail: deng@physics.unlv.edu, E-mail: zhang@physics.unlv.edu, E-mail: hli@lanl.gov, E-mail: jstone@astro.princeton.edu [Department of Astrophysical Sciences, Princeton University, Princeton, NJ 08544-1001 (United States)

    2017-08-10

    The early optical afterglow emission of several gamma-ray bursts (GRBs) shows a high linear polarization degree (PD) of tens of percent, suggesting an ordered magnetic field in the emission region. The light curves are consistent with being of a reverse shock (RS) origin. However, the magnetization parameter, σ , of the outflow is unknown. If σ is too small, an ordered field in the RS may be quickly randomized due to turbulence driven by various perturbations so that the PD may not be as high as observed. Here we use the “Athena++” relativistic MHD code to simulate a relativistic jet with an ordered magnetic field propagating into a clumpy ambient medium, with a focus on how density fluctuations may distort the ordered magnetic field and reduce PD in the RS emission for different σ values. For a given density fluctuation, we discover a clear power-law relationship between the relative PD reduction and the σ value of the outflow. Such a relation may be applied to estimate σ of the GRB outflows using the polarization data of early afterglows.

  9. Fully Parameter-Free Calculation of Optical Spectra for Insulators, Semiconductors, and Metals from a Simple Polarization Functional.

    Science.gov (United States)

    Berger, J A

    2015-09-25

    We present a fully parameter-free density-functional approach for the accurate description of optical absorption spectra of insulators, semiconductors, and metals. We show that this can be achieved within time-dependent current-density-functional theory using a simple dynamical polarization functional. We derive this functional from physical principles that govern optical spectra. Our method is truly predictive because not a single parameter is used. In particular, we do not use an ad hoc material-dependent broadening parameter to compare theory to experiment as is usually done. Our approach is numerically efficient; the cost equals that of a calculation within the random-phase approximation.

  10. Electron polarization function and plasmons in metallic armchair graphene nanoribbons

    DEFF Research Database (Denmark)

    Shylau, A. A.; Badalyan, S. M.; Peeters, F. M.

    2015-01-01

    Plasmon excitations in metallic armchair graphene nanoribbons are investigated using the random phase approximation. An exact analytical expression for the polarization function of Dirac fermions is obtained, valid for arbitrary temperature and doping. We find that at finite temperatures, due...... mode whose energy dispersion is determined by the graphene's fine structure constant. In the case of two Coulomb-coupled nanoribbons, this plasmon splits into in-phase and out-of-phase plasmon modes with splitting energy determined by the inter-ribbon spacing....

  11. Trivial constraints on orbital-free kinetic energy density functionals

    Science.gov (United States)

    Luo, Kai; Trickey, S. B.

    2018-03-01

    Approximate kinetic energy density functionals (KEDFs) are central to orbital-free density functional theory. Limitations on the spatial derivative dependencies of KEDFs have been claimed from differential virial theorems. We identify a central defect in the argument: the relationships are not true for an arbitrary density but hold only for the minimizing density and corresponding chemical potential. Contrary to the claims therefore, the relationships are not constraints and provide no independent information about the spatial derivative dependencies of approximate KEDFs. A simple argument also shows that validity for arbitrary v-representable densities is not restored by appeal to the density-potential bijection.

  12. Orthogonal bases of radial functions for charge density refinements

    International Nuclear Information System (INIS)

    Restori, R.

    1990-01-01

    Charge density determination from X-ray measurements necessitates the evaluation of the Fourier-Bessel transforms of the radial functions used to expand the charge density. Analytical expressions are given here for four sets of orthogonal functions which can substitute for the 'traditional exponential functions' set in least-squares refinements. (orig.)

  13. The Indigo Molecule Revisited Again: Assessment of the Minnesota Family of Density Functionals for the Prediction of Its Maximum Absorption Wavelengths in Various Solvents

    Directory of Open Access Journals (Sweden)

    Francisco Cervantes-Navarro

    2013-01-01

    Full Text Available The Minnesota family of density functionals (M05, M05-2X, M06, M06L, M06-2X, and M06-HF were evaluated for the calculation of the UV-Vis spectra of the indigo molecule in solvents of different polarities using time-dependent density functional theory (TD-DFT and the polarized continuum model (PCM. The maximum absorption wavelengths predicted for each functional were compared with the known experimental results.

  14. Dynamic Nuclear Polarization of High-Density Atomic Hydrogen in Solid Mixtures of Molecular Hydrogen Isotopes

    Science.gov (United States)

    Sheludiakov, S.; Ahokas, J.; Järvinen, J.; Zvezdov, D.; Vainio, O.; Lehtonen, L.; Vasiliev, S.; Mao, S.; Khmelenko, V. V.; Lee, D. M.

    2014-12-01

    We report on magnetic resonance studies of high-density atomic hydrogen and deuterium in solid hydrogen matrices at temperatures below 1 K. Average concentrations of H atoms ≈3 ×1019 cm-3 are obtained in chemical tunneling reactions of isotope exchange with D atoms. The products of these reactions are closely located pairs of H atoms near D2 molecules with strong exchange interactions. We discovered a dynamic nuclear polarization effect on H atoms created by pumping the center of the H electron spin resonance spectrum, similar to the Overhauser effect in metals. Our results indicate that H atoms may be arranged inside molecular matrices at separations equivalent to local concentrations of 2.6 ×1021 cm-3 . This opens up a way to build a metallic state of atomic hydrogen at zero pressure.

  15. A New Method for Simulating Power Flow Density Focused by a Silicon Lens Antenna Irradiated with Linearly Polarized THz Wave

    Directory of Open Access Journals (Sweden)

    Catur Apriono

    2015-08-01

    Full Text Available A terahertz system uses dielectric lens antennas for focusing and collimating beams of terahertz wave radiation. Linearly polarized terahertz wave radiation has been widely applied in the terahertz system. Therefore, an accurate method for analyzing the power flow density in the dielectric lens antenna irradiated with the linearly polarized terahertz wave radiation is important to design the terahertz systems. In optics, ray-tracing method has been used to calculate the power flow density by a number density of rays. In this study, we propose a method of ray-tracing combined with Fresnel’s transmission, including transmittance and polarization of the terahertz wave radiation to calculate power flow density in a Silicon lens antenna. We compare power flow density calculated by the proposed method with the regular ray-tracing method. When the Silicon lens antenna is irradiated with linearly polarized terahertz wave radiation, the proposed method calculates the power flow density more accurately than the regular ray-tracing.

  16. Density Functional Restricted-Unrestricted/Molecular Mechanics Theory for Hyperfine Coupling Constants of Molecules in Solution.

    Science.gov (United States)

    Rinkevicius, Zilvinas; Murugan, N Arul; Kongsted, Jacob; Frecuş, Bogdan; Steindal, Arnfinn Hykkerud; Ågren, Hans

    2011-10-11

    A density functional restricted-unrestricted approach, capable of evaluating hyperfine coupling constants with the inclusion of spin polarization effects in a spin-restricted Kohn-Sham method, has been extended to incorporate environmental effects. This is accomplished by means of a hybrid quantum mechanics/molecular mechanics formalism which allows for a granular representation of the polarization and electrostatic interactions with the classically described medium. By this technique, it is possible to trace the physical origin of hyperfine coupling constants in terms of spin polarization and spin density contributions and disentangle the dependence of these contributions on molecular geometry and solvent environment, something that increases the prospects for optimal design of spin labels for particular applications. A demonstration is given for the nitrogen isotropic hyperfine coupling constant in di-tert-butyl nitroxide solvated in water. The results indicate that the direct spin density contribution is about 5 times smaller than the spin polarization contribution to the nitrogen isotropic hyperfine coupling constant and that the latter contribution is solely responsible for the solvent shift of the constant. The developed approach is found capable of achieving satisfactory accuracy in prediction of the hyperfine coupling constants of solvated di-tert-butyl nitroxide and other similar nitroxides without the inclusion of solvent molecules in the quantum region provided polarizable force fields are used for the description of these molecules.

  17. Bone mineral density and menstrual function in adolescent female ...

    African Journals Online (AJOL)

    Bone mineral density and menstrual function in adolescent female long-distance runners - A prospective comparative study of bone structure and menstrual function in adolescent female endurance athletes from five secondary schools in Pretoria.

  18. On the discretization of probability density functions and the ...

    Indian Academy of Sciences (India)

    function f (x) with respect to a probability density function (PDF) ρ(x) := |ψ (x) |2, where ψ(x) is the wave function in ... fields of science, the calculation of Rényi and Tsallis entropies [1–3] for probability density function ρ(x) ... on the second mean-value theorem (SMVT) for integrals by postulating that: (i) The PDF ρ(x) can be ...

  19. Linking density functional and mode coupling models for supercooled liquids

    OpenAIRE

    Premkumar, Leishangthem; Bidhoodi, Neeta; Das, Shankar P.

    2015-01-01

    We compare predictions from two familiar models of the metastable supercooled liquid respectively constructed with thermodynamic and dynamic approach. In the so called density functional theory (DFT) the free energy $F[\\rho]$ of the liquid is a functional of the inhomogeneous density $\\rho({\\bf r})$. The metastable state is identified as a local minimum of $F[\\rho]$. The sharp density profile characterizing $\\rho({\\bf r})$ is identified as a single particle oscillator, whose frequency is obta...

  20. Introduction to Classical Density Functional Theory by a Computational Experiment

    Science.gov (United States)

    Jeanmairet, Guillaume; Levy, Nicolas; Levesque, Maximilien; Borgis, Daniel

    2014-01-01

    We propose an in silico experiment to introduce the classical density functional theory (cDFT). Density functional theories, whether quantum or classical, rely on abstract concepts that are nonintuitive; however, they are at the heart of powerful tools and active fields of research in both physics and chemistry. They led to the 1998 Nobel Prize in…

  1. Asymptotic Con dence Bands for Density and Regression Functions ...

    African Journals Online (AJOL)

    Abstract. In this paper, we obtain asymptotic confidence bands for both the density and regression functions in the framework of nonparametric estimation. Beforehand, the asymptotic behaviors in probability of the kernel estimator of the density and the Nadaraya-Watson estimator of the regression function are described ...

  2. A Density-Dependent Switch Drives Stochastic Clustering and Polarization of Signaling Molecules

    Science.gov (United States)

    Jilkine, Alexandra; Angenent, Sigurd B.; Wu, Lani F.; Altschuler, Steven J.

    2011-01-01

    Positive feedback plays a key role in the ability of signaling molecules to form highly localized clusters in the membrane or cytosol of cells. Such clustering can occur in the absence of localizing mechanisms such as pre-existing spatial cues, diffusional barriers, or molecular cross-linking. What prevents positive feedback from amplifying inevitable biological noise when an un-clustered “off” state is desired? And, what limits the spread of clusters when an “on” state is desired? Here, we show that a minimal positive feedback circuit provides the general principle for both suppressing and amplifying noise: below a critical density of signaling molecules, clustering switches off; above this threshold, highly localized clusters are recurrently generated. Clustering occurs only in the stochastic regime, suggesting that finite sizes of molecular populations cannot be ignored in signal transduction networks. The emergence of a dominant cluster for finite numbers of molecules is partly a phenomenon of random sampling, analogous to the fixation or loss of neutral mutations in finite populations. We refer to our model as the “neutral drift polarity model.” Regulating the density of signaling molecules provides a simple mechanism for a positive feedback circuit to robustly switch between clustered and un-clustered states. The intrinsic ability of positive feedback both to create and suppress clustering is a general mechanism that could operate within diverse biological networks to create dynamic spatial organization. PMID:22102805

  3. A density-dependent switch drives stochastic clustering and polarization of signaling molecules.

    Directory of Open Access Journals (Sweden)

    Alexandra Jilkine

    2011-11-01

    Full Text Available Positive feedback plays a key role in the ability of signaling molecules to form highly localized clusters in the membrane or cytosol of cells. Such clustering can occur in the absence of localizing mechanisms such as pre-existing spatial cues, diffusional barriers, or molecular cross-linking. What prevents positive feedback from amplifying inevitable biological noise when an un-clustered "off" state is desired? And, what limits the spread of clusters when an "on" state is desired? Here, we show that a minimal positive feedback circuit provides the general principle for both suppressing and amplifying noise: below a critical density of signaling molecules, clustering switches off; above this threshold, highly localized clusters are recurrently generated. Clustering occurs only in the stochastic regime, suggesting that finite sizes of molecular populations cannot be ignored in signal transduction networks. The emergence of a dominant cluster for finite numbers of molecules is partly a phenomenon of random sampling, analogous to the fixation or loss of neutral mutations in finite populations. We refer to our model as the "neutral drift polarity model." Regulating the density of signaling molecules provides a simple mechanism for a positive feedback circuit to robustly switch between clustered and un-clustered states. The intrinsic ability of positive feedback both to create and suppress clustering is a general mechanism that could operate within diverse biological networks to create dynamic spatial organization.

  4. Density-functional theory for internal magnetic fields

    Science.gov (United States)

    Tellgren, Erik I.

    2018-01-01

    A density-functional theory is developed based on the Maxwell-Schrödinger equation with an internal magnetic field in addition to the external electromagnetic potentials. The basic variables of this theory are the electron density and the total magnetic field, which can equivalently be represented as a physical current density. Hence, the theory can be regarded as a physical current density-functional theory and an alternative to the paramagnetic current density-functional theory due to Vignale and Rasolt. The energy functional has strong enough convexity properties to allow a formulation that generalizes Lieb's convex analysis formulation of standard density-functional theory. Several variational principles as well as a Hohenberg-Kohn-like mapping between potentials and ground-state densities follow from the underlying convex structure. Moreover, the energy functional can be regarded as the result of a standard approximation technique (Moreau-Yosida regularization) applied to the conventional Schrödinger ground-state energy, which imposes limits on the maximum curvature of the energy (with respect to the magnetic field) and enables construction of a (Fréchet) differentiable universal density functional.

  5. Analyses of zonal atmospheric excitation functions and their correlation with polar motion excitation functions

    Directory of Open Access Journals (Sweden)

    J. Nastula

    1997-11-01

    Full Text Available The atmospheric influence on the Earth's, rotation can be described by the effective atmospheric angular momentum (EAAM functions. In this study we focus on the analysis of short period variations of the equatorial components of the zonal EAAM excitation functions χ1 and χ2 and their influence on similar variations of polar motion. The global objective analysis data of the Japanese Meteorological Agency for the period 1986–1992 were used to compute the EAAM excitation functions in different latitude belts. Time- and latitude-variable amplitude spectra of variations of these functions with periods shorter than 150 days, containing pressure, pressure with the inverted barometric correction, and wind terms were computed. The spectra show distinct latitude and time variations of the prograde and retrograde oscillations which reach their maxima mainly in mid-latitudes. Prograde and retrograde oscillations with periods of about 40–60 days and about 110–120 days are seen in the spectra of pressure terms of the equatorial components of the zonal EAAM excitation functions. Additionally, correlation coefficients and cross-spectra between variations of the geodetic polar motion and equatorial components of the zonal EAAM excitation functions were computed to identify the latitude belts of the globe over which atmospheric circulation changes are correlated mostly with short period variations of the polar motion excitation functions. The correlation coefficients vary in time and latitude and reach maximum values in the northern latitudes from 50°N to 60°N. In the cross-spectra between the polar motion excitation functions and pressure terms of the zonal EAAM excitation functions there are peaks of common prograde oscillations with the periods around 20, 30, 40–50, 60 and 80–150 days and of common retrograde oscillations around 20, 30, 40 and 50–70 days.

  6. Analyses of zonal atmospheric excitation functions and their correlation with polar motion excitation functions

    Directory of Open Access Journals (Sweden)

    J. Nastula

    Full Text Available The atmospheric influence on the Earth's, rotation can be described by the effective atmospheric angular momentum (EAAM functions. In this study we focus on the analysis of short period variations of the equatorial components of the zonal EAAM excitation functions χ1 and χ2 and their influence on similar variations of polar motion. The global objective analysis data of the Japanese Meteorological Agency for the period 1986–1992 were used to compute the EAAM excitation functions in different latitude belts. Time- and latitude-variable amplitude spectra of variations of these functions with periods shorter than 150 days, containing pressure, pressure with the inverted barometric correction, and wind terms were computed. The spectra show distinct latitude and time variations of the prograde and retrograde oscillations which reach their maxima mainly in mid-latitudes. Prograde and retrograde oscillations with periods of about 40–60 days and about 110–120 days are seen in the spectra of pressure terms of the equatorial components of the zonal EAAM excitation functions. Additionally, correlation coefficients and cross-spectra between variations of the geodetic polar motion and equatorial components of the zonal EAAM excitation functions were computed to identify the latitude belts of the globe over which atmospheric circulation changes are correlated mostly with short period variations of the polar motion excitation functions. The correlation coefficients vary in time and latitude and reach maximum values in the northern latitudes from 50°N to 60°N. In the cross-spectra between the polar motion excitation functions and pressure terms of the zonal EAAM excitation functions there are peaks of common prograde oscillations with the periods around 20, 30, 40–50, 60 and 80–150 days and of common retrograde oscillations around 20, 30, 40 and 50–70 days.

  7. Nonperturbative vacuum polarization effects in two-dimensional supercritical Dirac-Coulomb system I. Vacuum charge density

    Science.gov (United States)

    Davydov, A.; Sveshnikov, K.; Voronina, Yu.

    2018-01-01

    Based on the original combination of analytical methods, computer algebra tools and numerical calculations, proposed recently in Refs. 1-3, the nonperturbative vacuum polarization effects in the 2+1D supercritical Dirac-Coulomb system with Z > Zcr,1 are explored. Both the vacuum charge density ρV P(r→) and vacuum energy ℰV P are considered. The main result of the work is that in the overcritical region ℰV P turns out to be a rapidly decreasing function ˜-ηeffZ3/R with ηeff > 0 and R being the size of the external Coulomb source. Due to a lot of details of calculation the whole work is divided into two parts I and II. In the present part I, we consider the evaluation and behavior of the vacuum density ρV P, which further is used in part II for evaluation of the vacuum energy, with emphasis on the renormalization, convergence of the partial expansion for ρV P and behavior of the integral induced charge QV P in the overcritical region.

  8. Measurement of the Polarized Structure Function $g_1^p$ at HERA

    CERN Document Server

    Ball, R.D.; Forte, S.; Hughes, V.W.; Lichtenstadt, J.; Ridolfi, G.; Ball, Richard D.; Deshpande, Abhay; Forte, Stefano; Hughes, Vernon W.; Lichtenstadt, Jechiel; Ridolfi, Giovanni

    1996-01-01

    We present estimates of possible data on spin-dependent asymmetries in inclusive scattering of high energy polarized electrons by high energy polarized protons at HERA, including statistical errors, and discuss systematic uncertainties. We show that these data would shed light on the small x behaviour of the polarized structure function g_1, and would reduce substantially the uncertainty on the determination of the polarized gluon distribution.

  9. Analytical gradients for subsystem density functional theory within the slater-function-based amsterdam density functional program.

    Science.gov (United States)

    Schlüns, Danny; Franchini, Mirko; Götz, Andreas W; Neugebauer, Johannes; Jacob, Christoph R; Visscher, Lucas

    2017-02-05

    We present a new implementation of analytical gradients for subsystem density-functional theory (sDFT) and frozen-density embedding (FDE) into the Amsterdam Density Functional program (ADF). The underlying theory and necessary expressions for the implementation are derived and discussed in detail for various FDE and sDFT setups. The parallel implementation is numerically verified and geometry optimizations with different functional combinations (LDA/TF and PW91/PW91K) are conducted and compared to reference data. Our results confirm that sDFT-LDA/TF yields good equilibrium distances for the systems studied here (mean absolute deviation: 0.09 Å) compared to reference wave-function theory results. However, sDFT-PW91/PW91k quite consistently yields smaller equilibrium distances (mean absolute deviation: 0.23 Å). The flexibility of our new implementation is demonstrated for an HCN-trimer test system, for which several different setups are applied. © 2016 Wiley Periodicals, Inc. © 2016 Wiley Periodicals, Inc.

  10. Density functional theory and multiscale materials modeling*

    Indian Academy of Sciences (India)

    Unknown

    Here the hardness kernel (Berkowitz et al 1985;. Ghosh 1990), ηµν(r, r′), represents the energy functional derivative . )( )( ],[. ),(. 2......... ′. =′ r r rr ν. µ β α. µν δρ δρ ρρ δ η. F. (27). We now specialize to the case of a set of atoms (say, M in number) located at the fixed positions {Ri} corre- sponding to a ...

  11. Current-induced spin polarization in InGaAs and GaAs epilayers with varying doping densities

    Science.gov (United States)

    Luengo-Kovac, M.; Huang, S.; Del Gaudio, D.; Occena, J.; Goldman, R. S.; Raimondi, R.; Sih, V.

    2017-11-01

    The current-induced spin polarization and momentum-dependent spin-orbit field were measured in InxGa1 -xAs epilayers with varying indium concentrations and silicon doping densities. Samples with higher indium concentrations and carrier concentrations and lower mobilities were found to have larger electrical spin generation efficiencies. Furthermore, current-induced spin polarization was detected in GaAs epilayers despite the absence of measurable spin-orbit fields, indicating that the extrinsic contributions to the spin-polarization mechanism must be considered. Theoretical calculations based on a model that includes extrinsic contributions to the spin dephasing and the spin Hall effect, in addition to the intrinsic Rashba and Dresselhaus spin-orbit coupling, are found to reproduce the experimental finding that the crystal direction with the smaller net spin-orbit field has larger electrical spin generation efficiency and are used to predict how sample parameters affect the magnitude of the current-induced spin polarization.

  12. Machine learning (ML)-guided OPC using basis functions of polar Fourier transform

    Science.gov (United States)

    Choi, Suhyeong; Shim, Seongbo; Shin, Youngsoo

    2016-03-01

    With shrinking feature size, runtime has become a limitation of model-based OPC (MB-OPC). A few machine learning-guided OPC (ML-OPC) have been studied as candidates for next-generation OPC, but they all employ too many parameters (e.g. local densities), which set their own limitations. We propose to use basis functions of polar Fourier transform (PFT) as parameters of ML-OPC. Since PFT functions are orthogonal each other and well reflect light phenomena, the number of parameters can significantly be reduced without loss of OPC accuracy. Experiments demonstrate that our new ML-OPC achieves 80% reduction in OPC time and 35% reduction in the error of predicted mask bias when compared to conventional ML-OPC.

  13. Relationship of Quantum Entanglement to Density Functional Theory

    OpenAIRE

    Rajagopal, A. K.; Rendell, R. W.

    2005-01-01

    The maximum von Neumann entropy principle subject to given constraints of mean values of some physical observables determines the density matrix. Similarly the stationary action principle in the case of time-dependent (dissipative) situations under similar constraints yields the density matrix. The free energy and measures of entanglement are expressed in terms of such a density matrix and thus define respective functionals of the mean values. In the light of several model calculations, it is...

  14. Resolution enhancement in active underwater polarization imaging with modulation transfer function analysis.

    Science.gov (United States)

    Han, Jiefei; Yang, Kecheng; Xia, Min; Sun, Liying; Cheng, Zao; Liu, Hao; Ye, Junwei

    2015-04-10

    Active polarization imaging technology is a convenient and promising method for imaging in a scattering medium such as fog and turbid water. However, few studies have investigated the influence of polarization on the resolution in underwater imaging. This paper reports on the effects of polarization detection on the resolution of underwater imaging by using active polarization imaging technology. An experimental system is designed to determine the influence under various polarization and water conditions. The modulation transfer function is introduced to estimate the resolution variations at different spatial frequencies. Results show that orthogonal detection supplies the best resolution compared with other polarization directions in the turbid water. The performance of the circular polarization method is better than the linear process. However, if the light propagates under low scattering conditions, such as imaging in clean water or at small optical thickness, the resolution enhancement is not sensitive to the polarization angles.

  15. Active Space Dependence in Multiconfiguration Pair-Density Functional Theory.

    Science.gov (United States)

    Sharma, Prachi; Truhlar, Donald G; Gagliardi, Laura

    2018-02-13

    In multiconfiguration pair-density functional theory (MC-PDFT), multiconfiguration self-consistent-field calculations and on-top density functionals are combined to describe both static and dynamic correlation. Here, we investigate how the MC-PDFT total energy and its components depend on the active space choice in the case of the H 2 and N 2 molecules. The active space dependence of the on-top pair density, the total density, the ratio of on-top pair density to half the square of the electron density, and the satisfaction of the virial theorem are also explored. We find that the density and on-top pair density do not change significantly with changes in the active space. However, the on-top ratio does change significantly with respect to active space change, and this affects the on-top energy. This study provides a foundation for designing on-top density functionals and automatizing the active space choice in MC-PDFT.

  16. Bond energy decomposition analysis for subsystem density functional theory

    NARCIS (Netherlands)

    Beyhan, S.M.; Gotz, A.W.; Visscher, L.

    2013-01-01

    We employed an explicit expression for the dispersion (D) energy in conjunction with Kohn-Sham (KS) density functional theory and frozen-density embedding (FDE) to calculate interaction energies between DNA base pairs and a selected set of amino acid pairs in the hydrophobic core of a small protein

  17. Excitation Spectra of Nucleobases with Multiconfigurational Density Functional Theory

    DEFF Research Database (Denmark)

    Hubert, Mickaël; Jensen, Hans Jørgen Aa; Hedegård, Erik D.

    2016-01-01

    Range-separated hybrid methods between wave function theory and density functional theory (DFT) can provide high-accuracy results, while correcting some of the inherent flaws of both the underlying wave function theory and DFT. We here assess the accuracy for excitation energies of the nucleobases...

  18. Density Functional Calculations of Solid State Heats of Formation

    National Research Council Canada - National Science Library

    Politzer, Peter

    1999-01-01

    It is now feasible to compute quite accurate gas phase heats of formation for relatively small molecules by means of ab initio or density functional techniques and one of several possible approaches...

  19. Dynamical density functional theory for dense atomic liquids

    International Nuclear Information System (INIS)

    Archer, A J

    2006-01-01

    Starting from Newton's equations of motion, we derive a dynamical density functional theory (DDFT) applicable to atomic liquids. The theory has the feature that it requires as input the Helmholtz free energy functional from equilibrium density functional theory. This means that, given a reliable equilibrium free energy functional, the correct equilibrium fluid density profile is guaranteed. We show that when the isothermal compressibility is small, the DDFT generates the correct value for the speed of sound in a dense liquid. We also interpret the theory as a dynamical equation for a coarse grained fluid density and show that the theory can be used (making further approximations) to derive the standard mode coupling theory that is used to describe the glass transition. The present theory should provide a useful starting point for describing the dynamics of inhomogeneous atomic fluids

  20. Time-dependent quantum fluid density functional theory of hydrogen ...

    Indian Academy of Sciences (India)

    WINTEC

    GNLSE) of motion was earlier derived in our laboratory by combining density functional theory and quantum fluid dynamics in three- dimensional space. In continuation of the work reported previously, the GNLSE is applied to provide addi-.

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

    International Nuclear Information System (INIS)

    Yang, Weitao

    2014-01-01

    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

  2. Energy decomposition analysis of single bonds within Kohn-Sham density functional theory.

    Science.gov (United States)

    Levine, Daniel S; Head-Gordon, Martin

    2017-11-28

    An energy decomposition analysis (EDA) for single chemical bonds is presented within the framework of Kohn-Sham density functional theory based on spin projection equations that are exact within wave function theory. Chemical bond energies can then be understood in terms of stabilization caused by spin-coupling augmented by dispersion, polarization, and charge transfer in competition with destabilizing Pauli repulsions. The EDA reveals distinguishing features of chemical bonds ranging across nonpolar, polar, ionic, and charge-shift bonds. The effect of electron correlation is assessed by comparison with Hartree-Fock results. Substituent effects are illustrated by comparing the C-C bond in ethane against that in bis(diamantane), and dispersion stabilization in the latter is quantified. Finally, three metal-metal bonds in experimentally characterized compounds are examined: a [Formula: see text]-[Formula: see text] dimer, the [Formula: see text]-[Formula: see text] bond in dizincocene, and the Mn-Mn bond in dimanganese decacarbonyl.

  3. Density functional theory for polymeric systems in 2D.

    Science.gov (United States)

    Słyk, Edyta; Roth, Roland; Bryk, Paweł

    2016-06-22

    We propose density functional theory for polymeric fluids in two dimensions. The approach is based on Wertheim's first order thermodynamic perturbation theory (TPT) and closely follows density functional theory for polymers proposed by Yu and Wu (2002 J. Chem. Phys. 117 2368). As a simple application we evaluate the density profiles of tangent hard-disk polymers at hard walls. The theoretical predictions are compared against the results of the Monte Carlo simulations. We find that for short chain lengths the theoretical density profiles are in an excellent agreement with the Monte Carlo data. The agreement is less satisfactory for longer chains. The performance of the theory can be improved by recasting the approach using the self-consistent field theory formalism. When the self-avoiding chain statistics is used, the theory yields a marked improvement in the low density limit. Further improvements for long chains could be reached by going beyond the first order of TPT.

  4. Tuning the polarization-induced free hole density in nanowires graded from GaN to AlN

    OpenAIRE

    Sarwar, A. T. M. Golam; Carnevale, Santino D.; Kent, Thomas F.; Yang, Fan; McComb, David W.; Myers, Roberto C.

    2014-01-01

    We report a systematic study of p-type polarization induced doping in graded AlGaN nanowire light emitting diodes grown on silicon wafers by plasma-assisted molecular beam epitaxy. The composition gradient in the p-type base is varied in a set of samples from 0.7 %Al/nm to 4.95 %Al/nm corresponding to negative bound polarization charge densities of 2.2x10^18 cm^-3 to 1.6x10^19 cm^-3. Capacitance measurements and energy band modeling reveal that for gradients greater than or equal to 1.30 %Al/...

  5. Uniform magnetic fields in density-functional theory.

    Science.gov (United States)

    Tellgren, Erik I; Laestadius, Andre; Helgaker, Trygve; Kvaal, Simen; Teale, Andrew M

    2018-01-14

    We construct a density-functional formalism adapted to uniform external magnetic fields that is intermediate between conventional density functional theory and Current-Density Functional Theory (CDFT). In the intermediate theory, which we term linear vector potential-DFT (LDFT), the basic variables are the density, the canonical momentum, and the paramagnetic contribution to the magnetic moment. Both a constrained-search formulation and a convex formulation in terms of Legendre-Fenchel transformations are constructed. Many theoretical issues in CDFT find simplified analogs in LDFT. We prove results concerning N-representability, Hohenberg-Kohn-like mappings, existence of minimizers in the constrained-search expression, and a restricted analog to gauge invariance. The issue of additivity of the energy over non-interacting subsystems, which is qualitatively different in LDFT and CDFT, is also discussed.

  6. Storm-enhanced plasma density and polar tongue of ionization development during the 15 May 2005 superstorm

    Science.gov (United States)

    Horvath, Ildiko; Lovell, Brian C.

    2015-06-01

    We investigate the ionosphere's global response to the 15 May 2005 superstorm in terms of storm evolution and ionospheric electrodynamics. Our aim is to study the global distribution of plasma and the resultant large-scale ionospheric features including the equatorial ionization anomaly (EIA), storm-enhanced density (SED), and polar tongue of ionization (TOI). We have combined multi-instrument ionospheric data, solar and terrestrial magnetic data, and polar convection maps. Results reveal the prompt penetration of the interplanetary electric field to the polar region and then to the equator with a dusk-to-dawn polarity during the initial phase and with a dawn-to-dusk polarity during the main phase. This drove during the initial phase a weak eastward equatorial electrojet (EEJ) in the American sector at nighttime and a weak westward EEJ in the Indian-Australian sector at daytime. During the main phase, these EEJs intensified and changed polarities. SED and polar TOI development was observed prior to and during the initial phase at evening-premidnight hours over North America and during the main phase in the south at afternoon-evening hours in the Australian sector. During the main phase and early in the recovery phase, the EIA-SED structure was well formed in the Asian longitude sector. Then, polar TOI development was absent in the north because of the long distance from the magnetic pole but was supported in the south because of the closeness of daytime cusp and magnetic pole. Thus, the EIA-SED-TOI structure developed twice but each time in a different longitude sector and with different characteristics.

  7. All-electron density functional theory and time-dependent density functional theory with high-order finite elements

    OpenAIRE

    Lehtovaara, Lauri; Havu, Ville; Puska, Martti

    2009-01-01

    We present for static density functional theory and time-dependent density functional theory calculations an all-electron method which employs high-order hierarchical finite-element bases. Our mesh generation scheme, in which structured atomic meshes are merged to an unstructured molecular mesh, allows a highly nonuniform discretization of the space. Thus it is possible to represent the core and valence states using the same discretization scheme, i.e., no pseudopotentials or similar treatmen...

  8. Using polarized Raman spectroscopy and the pseudospectral method to characterize molecular structure and function

    Science.gov (United States)

    Weisman, Andrew L.

    number of polarized Raman properties of a sample given common output from electronic structure calculations. In Part II, we apply the pseudospectral method to other areas of scientific importance requiring a deeper understanding of molecular structure and function. First, we use it to accurately determine the frequencies of vibrational tags on biomolecules that can be detected in real-time using stimulated Raman spectroscopy. Next, we evaluate the performance of the pseudospectral method for calculating excited-state energies and energy gradients of large molecules -- another new application of the pseudospectral method -- showing that the calculations run much more quickly than those using the analytic method. Finally, we use the pseudospectral method to simulate the bottleneck process of a solar cell used for water splitting, a promising technology for converting the sun's energy into hydrogen fuel. We apply the speed of the pseudospectral method by modeling the relevant part of the system as a large, explicitly passivated titanium dioxide nanoparticle and simulating it realistically using hybrid density functional theory with an implicit solvent model, yielding insight into the physical nature of the rate-limiting step of water splitting. These results further validate the particularly fast and accurate simulation methodologies used, opening the door to efficient and realistic cluster-based, fully quantum-mechanical simulations of the bottleneck process of a promising technology for clean solar energy conversion. Taken together, we show how both polarized Raman spectroscopy and the pseudospectral method are effective tools for analyzing the structure and function of important molecular systems.

  9. Effect of smoking on the gingival capillary density: assessment of gingival capillary density with orthogonal polarization spectral imaging

    NARCIS (Netherlands)

    Lindeboom, J. A.; Mathura, K. R.; Harkisoen, S.; van den Akker, H. P.; Ince, C.

    2005-01-01

    Microvascular changes because of smoking are frequently presumed in models because of the negative effect of smoking portrayed on the microcirculation. We hypothesized that cigarette smoke might lead to a decrease in gingival capillary density. Capillary density was assessed with orthogonal

  10. Basis convergence of range-separated density-functional theory.

    Science.gov (United States)

    Franck, Odile; Mussard, Bastien; Luppi, Eleonora; Toulouse, Julien

    2015-02-21

    Range-separated density-functional theory (DFT) is an alternative approach to Kohn-Sham density-functional theory. The strategy of range-separated density-functional theory consists in separating the Coulomb electron-electron interaction into long-range and short-range components and treating the long-range part by an explicit many-body wave-function method and the short-range part by a density-functional approximation. Among the advantages of using many-body methods for the long-range part of the electron-electron interaction is that they are much less sensitive to the one-electron atomic basis compared to the case of the standard Coulomb interaction. Here, we provide a detailed study of the basis convergence of range-separated density-functional theory. We study the convergence of the partial-wave expansion of the long-range wave function near the electron-electron coalescence. We show that the rate of convergence is exponential with respect to the maximal angular momentum L for the long-range wave function, whereas it is polynomial for the case of the Coulomb interaction. We also study the convergence of the long-range second-order Møller-Plesset correlation energy of four systems (He, Ne, N2, and H2O) with cardinal number X of the Dunning basis sets cc - p(C)V XZ and find that the error in the correlation energy is best fitted by an exponential in X. This leads us to propose a three-point complete-basis-set extrapolation scheme for range-separated density-functional theory based on an exponential formula.

  11. Bayesian error estimation in density-functional theory

    DEFF Research Database (Denmark)

    Mortensen, Jens Jørgen; Kaasbjerg, Kristen; Frederiksen, Søren Lund

    2005-01-01

    We present a practical scheme for performing error estimates for density-functional theory calculations. The approach, which is based on ideas from Bayesian statistics, involves creating an ensemble of exchange-correlation functionals by comparing with an experimental database of binding energies...

  12. Wigner Function of Density Operator for Negative Binomial Distribution

    International Nuclear Information System (INIS)

    Xu Xinglei; Li Hongqi

    2008-01-01

    By using the technique of integration within an ordered product (IWOP) of operator we derive Wigner function of density operator for negative binomial distribution of radiation field in the mixed state case, then we derive the Wigner function of squeezed number state, which yields negative binomial distribution by virtue of the entangled state representation and the entangled Wigner operator

  13. Density functional studies of molecular structures of N-methyl ...

    Indian Academy of Sciences (India)

    Density functional theory was applied to the calculation of molecular structures of N-methyl formamide (NMF), N,N-dimethyl formamide (DMF), and N,Ndimethyl acetamide (DMA). DFT calculations on NMF, DMF, and DMA were performed using a combination of the local functional of Vosko, Wilk, and Nusair (VWN) with the ...

  14. Performance of density functional theory methods to describe ...

    Indian Academy of Sciences (India)

    Unknown

    Abstract. The performance of three exchange and correlation density functionals, LDA, BLYP and B3LYP, with four basis sets is tested in three intramolecular hydrogen shift reactions. The best reaction and acti- vation energies come from the hybrid functional B3LYP with triple-ζ basis sets, when they are compared.

  15. Density Functional Theory and Materials Modeling at Atomistic Length Scales

    Directory of Open Access Journals (Sweden)

    Swapan K. Ghosh

    2002-04-01

    Full Text Available Abstract: We discuss the basic concepts of density functional theory (DFT as applied to materials modeling in the microscopic, mesoscopic and macroscopic length scales. The picture that emerges is that of a single unified framework for the study of both quantum and classical systems. While for quantum DFT, the central equation is a one-particle Schrodinger-like Kohn-Sham equation, the classical DFT consists of Boltzmann type distributions, both corresponding to a system of noninteracting particles in the field of a density-dependent effective potential, the exact functional form of which is unknown. One therefore approximates the exchange-correlation potential for quantum systems and the excess free energy density functional or the direct correlation functions for classical systems. Illustrative applications of quantum DFT to microscopic modeling of molecular interaction and that of classical DFT to a mesoscopic modeling of soft condensed matter systems are highlighted.

  16. Microbial metabolite butyrate facilitates M2 macrophage polarization and function.

    Science.gov (United States)

    Ji, Jian; Shu, Dingming; Zheng, Mingzhu; Wang, Jie; Luo, Chenglong; Wang, Yan; Guo, Fuyou; Zou, Xian; Lv, Xiaohui; Li, Ying; Liu, Tianfei; Qu, Hao

    2016-04-20

    Metabolites from intestinal microbes modulate the mucosal immune system by regulating the polarization and expansion of T cells. Whether the microbial metabolites influence macrophage polarization, however, is poorly understood. Here, we show that the large bowel microbial fermentation product, butyrate, facilitates M2 macrophage polarization, in vitro and in vivo. The supernatant from butyrate-treated M2 macrophage increased the migration and enhanced the wound closure rate of MLE-12 cells. Butyrate attenuated intestinal inflammation in mice with dextran sulfate sodium (DSS)-induced colitis, with a significant increase in colonic expression of the M2 macrophage-associated protein, Arg1. M2 macrophage treated with butyrate, had increased activation of the H3K9/STAT6 signaling pathway, suggesting a mechanism for butyrate facilitated M2 macrophage polarization. Collectively, our study indicated that commensal microbe-derived butyrate is a novel activator of STAT6-mediated transcription through H3K9 acetylation driving M2 macrophage polarization, and delineated new insights into the immune interplay underlying inflammatory bowel disease.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  18. Spin structure function measurements with polarized protons and electrons at HERA

    International Nuclear Information System (INIS)

    Ball, R.D.; Deshpande, A.; Forte, S.; Hughes, V.W.; Lichtenstadt, J.; Ridolfi, G.

    1995-01-01

    Useful insights into the spin structure functions of the nucleon can be achieved by measurements of spin-dependent asymmetries in inclusive scattering of high energy polarized electrons by high energy polarized protons at HERA. Such an experiment would be a natural extension of the polarized lepton-nucleon scattering experiments presently carried out at CERN and SLAC. We present here estimates of possible data in the extended kinematic range of HERA and associated statistical errors. (orig.)

  19. Inclusion of Dispersion Effects in Density Functional Theory

    DEFF Research Database (Denmark)

    Møgelhøj, Andreas

    In this thesis, applications and development will be presented within the field of van der Waals interactions in density functional theory. The thesis is based on the three projects: i) van der Waals interactions effect on the structure of liquid water at ambient conditions, ii) development...... lower first peak consistent with recent experiments, while the outer structure is completely smeared out. The water structures obtained from the ab initio van der Waals simulations clearly resemble high-density liquid water, whereas the PBE molecular dynamics simulation with equivalent computational...... setup resembles low-density liquid. Mixing the vdW-DF2 and the experimental low-density liquid in a 70/30% ratio gives agreement with experimental results. This is consistent with the bimodal picture of water. Also, in this thesis the BEEF-vdW exchange-correlation functional is presented based...

  20. Impact of Molecular Orientation and Packing Density on Electronic Polarization in the Bulk and at Surfaces of Organic Semiconductors

    KAUST Repository

    Ryno, Sean

    2016-05-16

    The polarizable environment surrounding charge carriers in organic semiconductors impacts the efficiency of the charge transport process. Here, we consider two representative organic semiconductors, tetracene and rubrene, and evaluate their polarization energies in the bulk and at the organic-vacuum interface using a polarizable force field that accounts for induced-dipole and quadrupole interactions. Though both oligoacenes pack in a herringbone motif, the tetraphenyl substituents on the tetracene backbone of rubrene alter greatly the nature of the packing. The resulting change in relative orientations of neighboring molecules is found to reduce the bulk polarization energy of holes in rubrene by some 0.3 eV when compared to tetracene. The consideration of model organic-vacuum interfaces highlights the significant variation in the electrostatic environment for a charge carrier at a surface although the net change in polarization energy is small; interestingly, the environment of a charge even just one layer removed from the surface can be viewed already as representative of the bulk. Overall, it is found that in these herringbone-type layered crystals the polarization energy has a much stronger dependence on the intralayer packing density than interlayer packing density.

  1. Tuning the polarization-induced free hole density in nanowires graded from GaN to AlN

    Energy Technology Data Exchange (ETDEWEB)

    Golam Sarwar, A. T. M.; Carnevale, Santino D. [Department of Electrical and Computer Engineering, The Ohio State University, Columbus, Ohio 43210 (United States); Kent, Thomas F.; Yang, Fan; McComb, David W. [Department of Materials Science and Engineering, The Ohio State University, Columbus, Ohio 43210 (United States); Myers, Roberto C., E-mail: myers.1079@osu.edu [Department of Electrical and Computer Engineering, The Ohio State University, Columbus, Ohio 43210 (United States); Department of Materials Science and Engineering, The Ohio State University, Columbus, Ohio 43210 (United States)

    2015-01-19

    We report a systematic study of p-type polarization-induced doping in graded AlGaN nanowire light emitting diodes grown on silicon wafers by plasma-assisted molecular beam epitaxy. The composition gradient in the p-type base is varied in a set of samples from 0.7%Al/nm to 4.95%Al/nm corresponding to negative bound polarization charge densities of 2.2 × 10{sup 18 }cm{sup −3} to 1.6 × 10{sup 19 }cm{sup −3}. Capacitance measurements and energy band modeling reveal that for gradients greater than or equal to 1.30%Al/nm, the deep donor concentration is negligible and free hole concentrations roughly equal to the bound polarization charge density are achieved up to 1.6 × 10{sup 19 }cm{sup −3} at a gradient of 4.95%Al/nm. Accurate grading lengths in the p- and n-side of the pn-junction are extracted from scanning transmission electron microscopy images and are used to support energy band calculation and capacitance modeling. These results demonstrate the robust nature of p-type polarization doping in nanowires and put an upper bound on the magnitude of deep donor compensation.

  2. Tuning the polarization-induced free hole density in nanowires graded from GaN to AlN

    Science.gov (United States)

    Golam Sarwar, A. T. M.; Carnevale, Santino D.; Kent, Thomas F.; Yang, Fan; McComb, David W.; Myers, Roberto C.

    2015-01-01

    We report a systematic study of p-type polarization-induced doping in graded AlGaN nanowire light emitting diodes grown on silicon wafers by plasma-assisted molecular beam epitaxy. The composition gradient in the p-type base is varied in a set of samples from 0.7%Al/nm to 4.95%Al/nm corresponding to negative bound polarization charge densities of 2.2 × 1018 cm-3 to 1.6 × 1019 cm-3. Capacitance measurements and energy band modeling reveal that for gradients greater than or equal to 1.30%Al/nm, the deep donor concentration is negligible and free hole concentrations roughly equal to the bound polarization charge density are achieved up to 1.6 × 1019 cm-3 at a gradient of 4.95%Al/nm. Accurate grading lengths in the p- and n-side of the pn-junction are extracted from scanning transmission electron microscopy images and are used to support energy band calculation and capacitance modeling. These results demonstrate the robust nature of p-type polarization doping in nanowires and put an upper bound on the magnitude of deep donor compensation.

  3. Spin polarization driven by a charge-density wave in monolayer 1T−TaS2

    KAUST Repository

    Zhang, Qingyun

    2014-08-06

    Using first-principles calculations, we investigate the electronic and vibrational properties of monolayer T-phase TaS2. We demonstrate that a charge-density wave is energetically favorable at low temperature, similar to bulk 1T-TaS2. Electron-phonon coupling is found to be essential for the lattice reconstruction. The charge-density wave results in a strong localization of the electronic states near the Fermi level and consequently in spin polarization, transforming the material into a magnetic semiconductor with enhanced electronic correlations. The combination of inherent spin polarization with a semiconducting nature distinguishes the monolayer fundamentally from the bulk compound as well as from other two-dimensional transition metal dichalcogenides. Monolayer T-phase TaS2 therefore has the potential to enable two-dimensional spintronics. © 2014 American Physical Society.

  4. Relation between Characteristic Function of Density Operator and Tomogram

    International Nuclear Information System (INIS)

    Hong-Yi, Fan; Nian-Quan, Jiang

    2009-01-01

    In terms of the intermediate coordinate-momentum representation (Chin. Phys. Lett. 18 (2001) 850) and using the technique of integration within an ordered product of operators, we put the tomography theory into operator version. We reveal the new relation between the tomogram and the characteristic function of the density operator. The new expansion of the density operator in terms of the intermediate coordinate-momentum representation is also obtained. (general)

  5. Time dependent density functional calculation of plasmon response in clusters

    Science.gov (United States)

    Wang, Feng; Zhang, Feng-Shou; Eric, Suraud

    2003-02-01

    We have introduced a theoretical scheme for the efficient description of the optical response of a cluster based on the time-dependent density functional theory. The practical implementation is done by means of the fully fledged time-dependent local density approximation scheme, which is solved directly in the time domain without any linearization. As an example we consider the simple Na2 cluster and compute its surface plasmon photoabsorption cross section, which is in good agreement with the experiments.

  6. Dihadron fragmentation functions in the quark-jet model: Transversely polarized quarks

    Science.gov (United States)

    Matevosyan, Hrayr H.; Kotzinian, Aram; Thomas, Anthony W.

    2018-01-01

    Within the most recent extension of the quark-jet hadronization framework, we explore the transverse-polarization-dependent dihadron fragmentation functions (DiFFs) H1∢ and H1⊥ of a quark into π+π- pairs. Monte Carlo (MC) simulations are employed to model polarized quark hadronization and calculate the corresponding number densities. These, in turn, are used to extract the Fourier cosine moments of the DiFFs H1∢ and H1⊥. A notable finding is that there are previously unnoticed apparent discrepancies between the definitions of the so-called interference DiFF (IFF) H1∢ , entering the cross sections for two-hadron semi-inclusive electroproduction, and those involved in the production of two pairs of hadrons from back-to-back jets in electron-positron annihilation. This manuscript completes the studies of all four leading-twist DiFFs for unpolarized hadron pairs within the quark-jet framework, following our previous work on the helicity-dependent DiFF G1⊥.

  7. Central depression in nucleonic densities: Trend analysis in the nuclear density functional theory approach

    Science.gov (United States)

    Schuetrumpf, B.; Nazarewicz, W.; Reinhard, P.-G.

    2017-08-01

    Background: The central depression of nucleonic density, i.e., a reduction of density in the nuclear interior, has been attributed to many factors. For instance, bubble structures in superheavy nuclei are believed to be due to the electrostatic repulsion. In light nuclei, the mechanism behind the density reduction in the interior has been discussed in terms of shell effects associated with occupations of s orbits. Purpose: The main objective of this work is to reveal mechanisms behind the formation of central depression in nucleonic densities in light and heavy nuclei. To this end, we introduce several measures of the internal nucleonic density. Through the statistical analysis, we study the information content of these measures with respect to nuclear matter properties. Method: We apply nuclear density functional theory with Skyrme functionals. Using the statistical tools of linear least square regression, we inspect correlations between various measures of central depression and model parameters, including nuclear matter properties. We study bivariate correlations with selected quantities as well as multiple correlations with groups of parameters. Detailed correlation analysis is carried out for 34Si for which a bubble structure has been reported recently, 48Ca, and N =82 , 126, and 184 isotonic chains. Results: We show that the central depression in medium-mass nuclei is very sensitive to shell effects, whereas for superheavy systems it is firmly driven by the electrostatic repulsion. An appreciable semibubble structure in proton density is predicted for 294Og, which is currently the heaviest nucleus known experimentally. Conclusion: Our correlation analysis reveals that the central density indicators in nuclei below 208Pb carry little information on parameters of nuclear matter; they are predominantly driven by shell structure. On the other hand, in the superheavy nuclei there exists a clear relationship between the central nucleonic density and symmetry energy.

  8. Polarization study of non-resonant X-ray magnetic scattering from spin-density-wave modulation in chromium

    International Nuclear Information System (INIS)

    Ohsumi, Hiroyuki; Takata, Masaki

    2007-01-01

    We present a polarization study of non-resonant X-ray magnetic scattering in pure chromium. Satellite reflections are observed at +/-Q and +/-2Q, where Q is the modulation wave vector of an itinerant spin-density-wave. The first and second harmonics are confirmed to have magnetic and charge origin, respectively, by means of polarimetry without using an analyzer crystal. This alternative technique eliminates intolerable intensity loss at an analyzer by utilizing the sample crystal also as an analyzer crystal

  9. Knot Undulator to Generate Linearly Polarized Photons with Low on-Axis Power Density

    International Nuclear Information System (INIS)

    Qiao, S.

    2009-01-01

    Heat load on beamline optics is a serious problem to generate pure linearly polarized photons in the third generation synchrotron radiation facilities. For permanent magnet undulators, this problem can be overcome by a figure-8 operating mode. But there is still no good method to tackle this problem for electromagnetic elliptical undulators. Here, a novel operating mode is suggested, which can generate pure linearly polarized photons with very low on-axis heat load. Also the available minimum photon energy of linearly polarized photons can be extended much by this method.

  10. Density functional approach to the many-body problem : Key concepts and exact functionals

    NARCIS (Netherlands)

    van Leeuwen, Robert

    2003-01-01

    We give an overview of the fundamental concepts of density functional theory. We give a careful discussion of the several density functionals and their differentiability properties. We show that for nondegenerate ground states we can calculate the necessary functional derivatives by means of linear

  11. Raman Optical Activity Spectra from Density Functional Perturbation Theory and Density-Functional-Theory-Based Molecular Dynamics.

    Science.gov (United States)

    Luber, Sandra

    2017-03-14

    We describe the calculation of Raman optical activity (ROA) tensors from density functional perturbation theory, which has been implemented into the CP2K software package. Using the mixed Gaussian and plane waves method, ROA spectra are evaluated in the double-harmonic approximation. Moreover, an approach for the calculation of ROA spectra by means of density functional theory-based molecular dynamics is derived and used to obtain an ROA spectrum via time correlation functions, which paves the way for the calculation of ROA spectra taking into account anharmonicities and dynamic effects at ambient conditions.

  12. Quantum fluid dynamics within a relativistic density-functional framework

    International Nuclear Information System (INIS)

    Ghosh, S.K.; Deb, B.M.; Indian Inst. of Tech., Bombay. Group of Theoretical Studies)

    1984-01-01

    The authors explore certain interconnections between density-functional theory and quantum fluid dynamics of many-electron systems, in the relativistic domain, following the hydrodynamical approach for the one-particle Dirac equation. The spinor formulation is transformed into a tensor formulation, by defining a number of density functions. These lead to six 'classical' fluid dynamical equations, for a complete specification of the system. The various density functions and the hydrodynamical equations are physically interpreted. The relativistic hydrodynamics discussed, correspond to a 'spinning' fluid. The net many-electron fluid consists of components each of which is characterised by fluid dynamical quantities corresponding to each spinor. The net hydrodynamical quantities are obtained by summing over the occupied spinors. Thus, the earlier non-relativistic 'classical' picture of the many-electron fluid as a collection of individual fluid components is also valid in the relativistic domain. (author)

  13. Defect-induced photoconductivity in layered manganese oxides: a density functional theory study.

    Science.gov (United States)

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

    2008-04-11

    Enhanced photoconductivity of layered Mn(IV)O2 containing protonated Mn(IV) vacancy defects has been recently demonstrated, suggesting new technological possibilities for photoelectric conversion based on visible light harvesting. Using spin-polarized density functional theory, we provide the first direct evidence that such defects can indeed facilitate photoconductivity by (i) reducing the band-gap energy and (ii) separating electron and hole states. Our results thus support the proposition that nanosheet MnO2 offers an attractive new material for a variety of photoconductivity applications.

  14. Fracture functions and factorization in semi-inclusive polarized DIS

    International Nuclear Information System (INIS)

    Florian, D. de; Garcia Canal, C. A.; Sassot, R.

    1996-01-01

    We analize the O(αs) one-particle inclusive cross section in polarized deep inelastic lepton-hadron scattering and discuss the factorization of all the collinear singularities related to the process. This is done using dimensional regularization in the usual MS scheme and in another one, called MSp, which factorizes soft contributions and guarantees the axial current (non)conservation properties

  15. Linking density functional and mode coupling models for supercooled liquids.

    Science.gov (United States)

    Premkumar, Leishangthem; Bidhoodi, Neeta; Das, Shankar P

    2016-03-28

    We compare predictions from two familiar models of the metastable supercooled liquid, respectively, constructed with thermodynamic and dynamic approaches. In the so called density functional theory the free energy F[ρ] of the liquid is a functional of the inhomogeneous density ρ(r). The metastable state is identified as a local minimum of F[ρ]. The sharp density profile characterizing ρ(r) is identified as a single particle oscillator, whose frequency is obtained from the parameters of the optimum density function. On the other hand, a dynamic approach to supercooled liquids is taken in the mode coupling theory (MCT) which predict a sharp ergodicity-non-ergodicity transition at a critical density. The single particle dynamics in the non-ergodic state, treated approximately, represents a propagating mode whose characteristic frequency is computed from the corresponding memory function of the MCT. The mass localization parameters in the above two models (treated in their simplest forms) are obtained, respectively, in terms of the corresponding natural frequencies depicted and are shown to have comparable magnitudes.

  16. Linking density functional and mode coupling models for supercooled liquids

    Energy Technology Data Exchange (ETDEWEB)

    Premkumar, Leishangthem; Bidhoodi, Neeta; Das, Shankar P. [School of Physical Sciences, Jawaharlal Nehru University, New Delhi 110067 (India)

    2016-03-28

    We compare predictions from two familiar models of the metastable supercooled liquid, respectively, constructed with thermodynamic and dynamic approaches. In the so called density functional theory the free energy F[ρ] of the liquid is a functional of the inhomogeneous density ρ(r). The metastable state is identified as a local minimum of F[ρ]. The sharp density profile characterizing ρ(r) is identified as a single particle oscillator, whose frequency is obtained from the parameters of the optimum density function. On the other hand, a dynamic approach to supercooled liquids is taken in the mode coupling theory (MCT) which predict a sharp ergodicity-non-ergodicity transition at a critical density. The single particle dynamics in the non-ergodic state, treated approximately, represents a propagating mode whose characteristic frequency is computed from the corresponding memory function of the MCT. The mass localization parameters in the above two models (treated in their simplest forms) are obtained, respectively, in terms of the corresponding natural frequencies depicted and are shown to have comparable magnitudes.

  17. Excitation energies from range-separated time-dependent density and density matrix functional theory.

    Science.gov (United States)

    Pernal, Katarzyna

    2012-05-14

    Time-dependent density functional theory (TD-DFT) in the adiabatic formulation exhibits known failures when applied to predicting excitation energies. One of them is the lack of the doubly excited configurations. On the other hand, the time-dependent theory based on a one-electron reduced density matrix functional (time-dependent density matrix functional theory, TD-DMFT) has proven accurate in determining single and double excitations of H(2) molecule if the exact functional is employed in the adiabatic approximation. We propose a new approach for computing excited state energies that relies on functionals of electron density and one-electron reduced density matrix, where the latter is applied in the long-range region of electron-electron interactions. A similar approach has been recently successfully employed in predicting ground state potential energy curves of diatomic molecules even in the dissociation limit, where static correlation effects are dominating. In the paper, a time-dependent functional theory based on the range-separation of electronic interaction operator is rigorously formulated. To turn the approach into a practical scheme the adiabatic approximation is proposed for the short- and long-range components of the coupling matrix present in the linear response equations. In the end, the problem of finding excitation energies is turned into an eigenproblem for a symmetric matrix. Assignment of obtained excitations is discussed and it is shown how to identify double excitations from the analysis of approximate transition density matrix elements. The proposed method used with the short-range local density approximation (srLDA) and the long-range Buijse-Baerends density matrix functional (lrBB) is applied to H(2) molecule (at equilibrium geometry and in the dissociation limit) and to Be atom. The method accounts for double excitations in the investigated systems but, unfortunately, the accuracy of some of them is poor. The quality of the other

  18. Size-dependent error of the density functional theory ionization potential in vacuum and solution

    Energy Technology Data Exchange (ETDEWEB)

    Sosa Vazquez, Xochitl A.; Isborn, Christine M., E-mail: cisborn@ucmerced.edu [Chemistry and Chemical Biology, School of Natural Sciences, University of California, Merced, 5200 North Lake Road, Merced, California 95343 (United States)

    2015-12-28

    Density functional theory is often the method of choice for modeling the energetics of large molecules and including explicit solvation effects. It is preferable to use a method that treats systems of different sizes and with different amounts of explicit solvent on equal footing. However, recent work suggests that approximate density functional theory has a size-dependent error in the computation of the ionization potential. We here investigate the lack of size-intensivity of the ionization potential computed with approximate density functionals in vacuum and solution. We show that local and semi-local approximations to exchange do not yield a constant ionization potential for an increasing number of identical isolated molecules in vacuum. Instead, as the number of molecules increases, the total energy required to ionize the system decreases. Rather surprisingly, we find that this is still the case in solution, whether using a polarizable continuum model or with explicit solvent that breaks the degeneracy of each solute, and we find that explicit solvent in the calculation can exacerbate the size-dependent delocalization error. We demonstrate that increasing the amount of exact exchange changes the character of the polarization of the solvent molecules; for small amounts of exact exchange the solvent molecules contribute a fraction of their electron density to the ionized electron, but for larger amounts of exact exchange they properly polarize in response to the cationic solute. In vacuum and explicit solvent, the ionization potential can be made size-intensive by optimally tuning a long-range corrected hybrid functional.

  19. On the evolution of the density probability density function in strongly self-gravitating systems

    International Nuclear Information System (INIS)

    Girichidis, Philipp; Konstandin, Lukas; Klessen, Ralf S.; Whitworth, Anthony P.

    2014-01-01

    The time evolution of the probability density function (PDF) of the mass density is formulated and solved for systems in free-fall using a simple approximate function for the collapse of a sphere. We demonstrate that a pressure-free collapse results in a power-law tail on the high-density side of the PDF. The slope quickly asymptotes to the functional form P V (ρ)∝ρ –1.54 for the (volume-weighted) PDF and P M (ρ)∝ρ –0.54 for the corresponding mass-weighted distribution. From the simple approximation of the PDF we derive analytic descriptions for mass accretion, finding that dynamically quiet systems with narrow density PDFs lead to retarded star formation and low star formation rates (SFRs). Conversely, strong turbulent motions that broaden the PDF accelerate the collapse causing a bursting mode of star formation. Finally, we compare our theoretical work with observations. The measured SFRs are consistent with our model during the early phases of the collapse. Comparison of observed column density PDFs with those derived from our model suggests that observed star-forming cores are roughly in free-fall.

  20. Density functional theory in surface science and heterogeneous catalysis

    DEFF Research Database (Denmark)

    Nørskov, Jens Kehlet; Scheffler, M.; Toulhoat, H.

    2006-01-01

    Solid surfaces are used extensively as catalysts throughout the chemical industry, in the energy sector, and in environmental protection. Recently, density functional theory has started providing new insight into the atomic-scale mechanisms of heterogeneous catalysis, helping to interpret the large...... amount of experimental data gathered during the last decades. This article shows how density functional theory can be used to describe the state of the surface during reactions and the rate of catalytic reactions. It will also show how we are beginning to understand the variation in catalytic activity...

  1. On Farmer's line, probability density functions, and overall risk

    International Nuclear Information System (INIS)

    Munera, H.A.; Yadigaroglu, G.

    1986-01-01

    Limit lines used to define quantitative probabilistic safety goals can be categorized according to whether they are based on discrete pairs of event sequences and associated probabilities, on probability density functions (pdf's), or on complementary cumulative density functions (CCDFs). In particular, the concept of the well-known Farmer's line and its subsequent reinterpretations is clarified. It is shown that Farmer's lines are pdf's and, therefore, the overall risk (defined as the expected value of the pdf) that they represent can be easily calculated. It is also shown that the area under Farmer's line is proportional to probability, while the areas under CCDFs are generally proportional to expected value

  2. Benchmark density functional theory calculations for nanoscale conductance

    DEFF Research Database (Denmark)

    Strange, Mikkel; Bækgaard, Iben Sig Buur; Thygesen, Kristian Sommer

    2008-01-01

    We present a set of benchmark calculations for the Kohn-Sham elastic transmission function of five representative single-molecule junctions. The transmission functions are calculated using two different density functional theory methods, namely an ultrasoft pseudopotential plane-wave code...... in combination with maximally localized Wannier functions and the norm-conserving pseudopotential code SIESTA which applies an atomic orbital basis set. All calculations have been converged with respect to the supercell size and the number of k(parallel to) points in the surface plane. For all systems we find...

  3. Bioinorganic Chemistry Modeled with the TPSSh Density Functional

    DEFF Research Database (Denmark)

    Kepp, Kasper Planeta

    2008-01-01

    In this work, the TPSSh density functional has been benchmarked against a test set of experimental structures and bond energies for 80 transition-metal-containing diatomics. It is found that the TPSSh functional gives structures of the same quality as other commonly used hybrid and nonhybrid...... functionals such as B3LYP and BP86. TPSSh gives a slope of 0.99 upon linear fitting to experimental bond energies, whereas B3LYP and BP86, representing 20% and 0% exact exchange, respectively, give linear fits with slopes of 0.91 and 1.07. Thus, TPSSh eliminates the large systematic component of the error...... promising density functional for use and further development within the field of bioinorganic chemistry....

  4. KIDS Nuclear Energy Density Functional: 1st Application in Nuclei

    Science.gov (United States)

    Gil, Hana; Papakonstantinou, Panagiota; Hyun, Chang Ho; Oh, Yongseok

    We apply the KIDS (Korea: IBS-Daegu-Sungkyunkwan) nuclear energy density functional model, which is based on the Fermi momentum expansion, to the study of properties of lj-closed nuclei. The parameters of the model are determined by the nuclear properties at the saturation density and theoretical calculations on pure neutron matter. For applying the model to the study of nuclei, we rely on the Skyrme force model, where the Skyrme force parameters are determined through the KIDS energy density functional. Solving Hartree-Fock equations, we obtain the energies per particle and charge radii of closed magic nuclei, namely, 16O, 28O, 40Ca, 48Ca, 60Ca, 90Zr, 132Sn, and 208Pb. The results are compared with the observed data and further improvement of the model is shortly mentioned.

  5. A simple method of extracting the polarization charge density in the AlGaN/GaN heterostructure from current-voltage and capacitance-voltage characteristics

    International Nuclear Information System (INIS)

    Lü Yuan-Jie; Lin Zhao-Jun; Yu Ying-Xia; Meng Ling-Guo; Cao Zhi-Fang; Luan Chong-Biao; Wang Zhan-Guo

    2012-01-01

    An Ni Schottky contact on the AlGaN/GaN heterostructure is fabricated. The flat-band voltage for the Schottky contact on the AlGaN/GaN heterostructure is obtained from the forward current—voltage characteristics. With the measured capacitance—voltage curve and the flat-band voltage, the polarization charge density in the AlGaN/GaN heterostructure is investigated, and a simple formula for calculating the polarization charge density is obtained and analyzed. With the approach described in this paper, the obtained polarization charge density agrees well with the one calculated by self-consistently solving Schrodinger's and Poisson's equations

  6. A comparative study of the performance of some density functionals ...

    Indian Academy of Sciences (India)

    CH SRIDHAR REDDY

    E-mail: mdpsc@uohyd.ac.in. MS received 30 January 2017; revised 9 April 2017; ... Electronic absorption; finite temperature; vibronic spectra; density functionals; Gaussian wave packet propagation. 1. Introduction. Electronic excitation of a molecule is always accompa- nied by vibrational excitations due to the differences in.

  7. Density functional studies of molecular structures of N-methyl ...

    Indian Academy of Sciences (India)

    Administrator

    studies. Sparse experimental data on the gas-phase geometry of DMF reported in the literature compares well with the DFT results on DMF. DFT emerges as a powerful method to calculate molecular structures. Keywords. Density functional theory; alkyl amides; molecular structure of alkyl amides; transition state search; ...

  8. Performance of density functional theory methods to describe ...

    Indian Academy of Sciences (India)

    ... Lecture Workshops · Refresher Courses · Symposia · Live Streaming. Home; Journals; Journal of Chemical Sciences; Volume 117; Issue 5. Performance of density functional theory methods to describe intramolecular hydrogen shifts. Nelly González-Rivas Andrés Cedillo. Volume 117 Issue 5 September 2005 pp 555-560 ...

  9. Equilibrium time correlation functions in the low density limit

    NARCIS (Netherlands)

    Beijeren, H. van; Lanford, O.E.; Lebowitz, J.L.; Spohn, H.

    1980-01-01

    We consider a system of hard spheres in thermal equilibrium. Using Lanford's result about the convergence of the solutions of the BBGKY hierarchy to the solutions of the Boltzmann hierarchy, we show that in the low-density limit (Boltzmann-Grad limit): (i) the total time correlation function is

  10. Use of density functional theory in drug metabolism studies

    DEFF Research Database (Denmark)

    Rydberg, Patrik; Jørgensen, Flemming Steen; Olsen, Lars

    2014-01-01

    INTRODUCTION: The cytochrome P450 enzymes (CYPs) metabolize many drug compounds. They catalyze a wide variety of reactions, and potentially, a large number of different metabolites can be generated. Density functional theory (DFT) has, over the past decade, been shown to be a powerful tool...

  11. Time-dependent quantum fluid density functional theory of hydrogen ...

    Indian Academy of Sciences (India)

    WINTEC

    derived in our laboratory by combining density functional theory and quantum fluid dynamics in three- dimensional space. In continuation of the .... repulsion, electron-nuclear Coulomb attraction, ex- change and correlation interactions, ..... Eberly J H, Grobe R, Law C K and Su Q 1992 Adv. At. Mol. Opt. Phys. Suppl. 1 301. 8.

  12. Density functional theory for chiral nematic liquid crystals

    NARCIS (Netherlands)

    Belli, S.; Dussi, S.|info:eu-repo/dai/nl/372628885; Dijkstra, Marjolein|info:eu-repo/dai/nl/123538807; van Roij, R.|info:eu-repo/dai/nl/152978984

    2014-01-01

    Even though chiral nematic phases were the first liquid crystals experimentally observed more than a century ago, the origin of the thermodynamic stability of cholesteric states is still unclear. In this Rapid Communication we address the problem by means of a density functional theory for the

  13. Theoretical study on β-aminoacroleine; Density functional theory ...

    Indian Academy of Sciences (India)

    Home; Journals; Journal of Chemical Sciences; Volume 124; Issue 3. Theoretical study on β-aminoacroleine; Density functional theory, atoms in molecules theory and natural bond orbitals studies. Heidar Raissi Mehdi Yoosefian Effat Moshfeghi Farzaneh Farzad. Volume 124 Issue 3 May 2012 pp 731-739 ...

  14. The electron-propagator approach to conceptual density-functional ...

    Indian Academy of Sciences (India)

    Unknown

    Abstract. Both electron propagator theory and density-functional theory provide conceptually useful information about chemical reactivity and, most especially, charge transfer. This paper elucidates the qualitative and quantitative links between the two theories, with emphasis on how the reactivity indica- tors of conceptual ...

  15. A density functional study on the adsorption of hydrogen molecule ...

    Indian Academy of Sciences (India)

    An all-electron scalar relativistic calculation on the adsorption of hydrogen molecule onto small copper clusters has been performed by using density functional theory with the generalized gradient approximation (GGA) at PW91 level. Our results reveal that after adsorption of H2 molecule, the Cu-Cu interaction is ...

  16. Time-dependent density functional theory for periodic systems

    NARCIS (Netherlands)

    Kootstra, Freddie

    2001-01-01

    In this thesis the time-dependent version of density functional theory is described, which has been developed for crystalline non-metallic systems with periodicity in one to three dimensions. The application of this theory to the calculation of the optical reponse properties of a wide range of

  17. Time-dependent quantum fluid density functional theory of hydrogen ...

    Indian Academy of Sciences (India)

    A time-dependent generalized non-linear Schrödinger equation (GNLSE) of motion was earlier derived in our laboratory by combining density functional theory and quantum fluid dynamics in threedimensional space. In continuation of the work reported previously, the GNLSE is applied to provide additional knowledge on ...

  18. Density functional study of : Electronic and optical properties

    Indian Academy of Sciences (India)

    K C Bhamu

    2017-06-20

    Jun 20, 2017 ... the refractive index in zero frequency limits is 2.42. The absorption coefficient predicts the applicability of AgScO2 in solar cells and flat panel liquid crystal display as a transparent top window layer. Keywords. Density functional theory; band structure; optical properties. PACS Nos 71.15.Mb; 71.20.−b; 78.20.

  19. Density functional studies of endosulphan and its interaction with ...

    Indian Academy of Sciences (India)

    action between endosulphan and amino acids employ- ing density functional methods. Two conformers of both α- and β-endosulphan were considered in the present study. Two amino acids, glycine and GABA were chosen, as they are known to be chief neurotrans- mitters in the central nervous system. It has been shown.

  20. Dynamic behavior of chemical reactivity indices in density functional ...

    Indian Academy of Sciences (India)

    Dynamic behaviors of chemical concepts in density functional theory such as frontier orbitals (HOMO/LUMO), chemical potential, hardness, and electrophilicity index have been investigated in this work in the context of Bohn-Oppenheimer quantum molecular dynamics in association with molecular conformation changes.

  1. Quantum chemical calculations of using density functional theory ...

    Indian Academy of Sciences (India)

    K RACKESH JAWAHER

    2018-02-15

    Feb 15, 2018 ... Quantum chemical calculations of Cr2O3/SnO2 using density functional theory method ... Quantum chemical calculations have been employed to study the molecular effects produced by. Cr2O3/SnO2 optimised structure. .... optical memory for emerging technologies in areas such as telecommunications ...

  2. A density functional study on the adsorption of hydrogen molecule

    Indian Academy of Sciences (India)

    An all-electron scalar relativistic calculation on the adsorption of hydrogen molecule onto small copper clusters has been performed by using density functional theory with the generalized gradient approximation (GGA) at PW91 level. Our results reveal that after adsorption of H2 molecule, the Cu-Cu interaction is ...

  3. A density functional study on the adsorption of hydrogen molecule ...

    Indian Academy of Sciences (India)

    Abstract. An all-electron scalar relativistic calculation on the adsorption of hydrogen molecule onto small copper clusters has been performed by using density functional theory with the generalized gradient approxi- mation (GGA) at PW91 level. Our results reveal that after adsorption of H2 molecule, the Cu–Cu interaction.

  4. Density-functional theory of atoms and molecules

    CERN Document Server

    Parr, Robert G

    1995-01-01

    Provides an account of the fundamental principles of the density-functional theory of the electronic structure of matter and its applications to atoms and molecules. This book contains a discussion of the chemical potential and its derivatives. It is intended for physicists, chemists, and advanced students in chemistry.

  5. Density functional study of ferromagnetism in alkali metal thin films

    Indian Academy of Sciences (India)

    model (UJM), and it is argued that within LSDA or GGA, alkali metal thin films cannot be claimed to have an FM ground state. Relevance of these results to the experiments on transition metal-doped alkali metal thin films and bulk hosts are also discussed. Keywords. Alkali metal; thin films; magnetism; density functional ...

  6. The electron-propagator approach to conceptual density-functional ...

    Indian Academy of Sciences (India)

    Both electron propagator theory and density-functional theory provide conceptually useful information about chemical reactivity and, most especially, charge transfer. This paper elucidates thequalitative and quantitative links between the two theories, with emphasis on how the reactivity indicators of conceptual ...

  7. Density functional theory calculations of charge transport properties ...

    Indian Academy of Sciences (India)

    ZIRAN CHEN

    2017-08-04

    Aug 4, 2017 ... Density functional theory calculations of charge transport properties of 'plate-like' coronene topological structures. ZIRAN CHENa, ZHANRONG HEa, YOUHUI XUa and WENHAO YUb,∗. aDepartment of Architecture and Environment Engineering, Sichuan Vocational and Technical College, Suining,.

  8. Reproducibility in density functional theory calculations of solids

    DEFF Research Database (Denmark)

    Lejaeghere, Kurt; Bihlmayer, Gustav; Björkman, Torbjörn

    2016-01-01

    The widespread popularity of density functional theory has given rise to an extensive range of dedicated codes for predicting molecular and crystalline properties. However, each code implements the formalism in a different way, raising questions about the reproducibility of such predictions. We...

  9. Ground-state densities from the Rayleigh-Ritz variation principle and from density-functional theory.

    Science.gov (United States)

    Kvaal, Simen; Helgaker, Trygve

    2015-11-14

    The relationship between the densities of ground-state wave functions (i.e., the minimizers of the Rayleigh-Ritz variation principle) and the ground-state densities in density-functional theory (i.e., the minimizers of the Hohenberg-Kohn variation principle) is studied within the framework of convex conjugation, in a generic setting covering molecular systems, solid-state systems, and more. Having introduced admissible density functionals as functionals that produce the exact ground-state energy for a given external potential by minimizing over densities in the Hohenberg-Kohn variation principle, necessary and sufficient conditions on such functionals are established to ensure that the Rayleigh-Ritz ground-state densities and the Hohenberg-Kohn ground-state densities are identical. We apply the results to molecular systems in the Born-Oppenheimer approximation. For any given potential v ∈ L(3/2)(ℝ(3)) + L(∞)(ℝ(3)), we establish a one-to-one correspondence between the mixed ground-state densities of the Rayleigh-Ritz variation principle and the mixed ground-state densities of the Hohenberg-Kohn variation principle when the Lieb density-matrix constrained-search universal density functional is taken as the admissible functional. A similar one-to-one correspondence is established between the pure ground-state densities of the Rayleigh-Ritz variation principle and the pure ground-state densities obtained using the Hohenberg-Kohn variation principle with the Levy-Lieb pure-state constrained-search functional. In other words, all physical ground-state densities (pure or mixed) are recovered with these functionals and no false densities (i.e., minimizing densities that are not physical) exist. The importance of topology (i.e., choice of Banach space of densities and potentials) is emphasized and illustrated. The relevance of these results for current-density-functional theory is examined.

  10. Ab initio calculations versus polarized neutron diffraction for the spin density of free radicals

    CERN Document Server

    Ressouche, E

    2003-01-01

    The determination of the magnetization distribution using polarized neutron diffraction has played a key role during the last twenty years in the field of molecular magnetism. This distribution can also be obtained by first principle ab initio calculations. Such calculations always rely on approximations and the question that arises is to know whether the obtained results are reliable enough to represent accurately the properties of these molecules. The comparison between polarized neutron experimental results and ab initio calculations has turned to provide stringent tests for these methods. In the resent article a comparison between experimental and theoretical results is made and is illustrated by examples based on magnetic free radicals. (author)

  11. Comparison of exact-exchange calculations for solids in current-spin-density- and spin-density-functional theory

    DEFF Research Database (Denmark)

    Sharma, S.; Pittalis, S.; Kurth, S.

    2007-01-01

    The relative merits of current-spin-density- and spin-density-functional theory are investigated for solids treated within the exact-exchange-only approximation. Spin-orbit splittings and orbital magnetic moments are determined at zero external magnetic field. We find that for magnetic (Fe, Co......, and Ni) and nonmagnetic (Si and Ge) solids, the exact-exchange current-spin-density functional approach does not significantly improve the accuracy of the corresponding spin-density functional results....

  12. Efficient molecular density functional theory using generalized spherical harmonics expansions.

    Science.gov (United States)

    Ding, Lu; Levesque, Maximilien; Borgis, Daniel; Belloni, Luc

    2017-09-07

    We show that generalized spherical harmonics are well suited for representing the space and orientation molecular density in the resolution of the molecular density functional theory. We consider the common system made of a rigid solute of arbitrary complexity immersed in a molecular solvent, both represented by molecules with interacting atomic sites and classical force fields. The molecular solvent density ρ(r,Ω) around the solute is a function of the position r≡(x,y,z) and of the three Euler angles Ω≡(θ,ϕ,ψ) describing the solvent orientation. The standard density functional, equivalent to the hypernetted-chain closure for the solute-solvent correlations in the liquid theory, is minimized with respect to ρ(r,Ω). The up-to-now very expensive angular convolution products are advantageously replaced by simple products between projections onto generalized spherical harmonics. The dramatic gain in speed of resolution enables to explore in a systematic way molecular solutes of up to nanometric sizes in arbitrary solvents and to calculate their solvation free energy and associated microscopic solvent structure in at most a few minutes. We finally illustrate the formalism by tackling the solvation of molecules of various complexities in water.

  13. Functional fixedness and functional reduction as common sense reasonings in chemical equilibrium and in geometry and polarity of molecules

    Science.gov (United States)

    Furió, C.; Calatayud, M. L.; Bárcenas, S. L.; Padilla, O. M.

    2000-09-01

    Many of the learning difficulties in the specific domain of chemistry are found not only in the ideas already possessed by students but in the strategic and procedural knowledge that is characteristic of everyday thinking. These defects in procedural knowledge have been described as functional fixedness and functional reduction. This article assesses the procedural difficulties of students (grade 12 and first and third year of university) based on common sense reasoning in two areas of chemistry: chemical equilibrium and geometry and polarity of molecules. In the first area, the theme of external factors affecting equilibria (temperature and concentration change) was selected because the explanations given by the students could be analyzed easily. The existence of a functional fixedness where Le Chatelier's principle was almost exclusively applied by rote could be observed, with this being the cause of the incorrect responses given to the proposed items. Functional fixedness of the Lewis structure also led to an incorrect prediction of molecular geometry. When molecular geometry was correctly determined by the students, it seemed that other methodological or procedural difficulties appeared when the task was to determine molecular polarity. The students showed a tendency, in many cases, to reduce the factors affecting molecular polarity in two possible ways: (a) assuming that polarity depends only on shape (geometric functional reduction) or (b) assuming that molecular polarity depends only on the polarity of bonds (bonding functional reduction).

  14. Recent advances in density functional methods, pt. 1-2

    CERN Document Server

    Chong, Delano P

    1995-01-01

    Of all the different areas in computational chemistry, density functional theory (DFT) enjoys the most rapid development. Even at the level of the local density approximation (LDA), which is computationally less demanding, DFT can usually provide better answers than Hartree-Fock formalism for large systems such as clusters and solids. For atoms and molecules, the results from DFT often rival those obtained by ab initio quantum chemistry, partly because larger basis sets can be used. Such encouraging results have in turn stimulated workers to further investigate the formal theory as well as the

  15. Thermodynamical transcription of density functional theory with minimum Fisher information

    Science.gov (United States)

    Nagy, Á.

    2018-03-01

    Ghosh, Berkowitz and Parr designed a thermodynamical transcription of the ground-state density functional theory and introduced a local temperature that varies from point to point. The theory, however, is not unique because the kinetic energy density is not uniquely defined. Here we derive the expression of the phase-space Fisher information in the GBP theory taking the inverse temperature as the Fisher parameter. It is proved that this Fisher information takes its minimum for the case of constant temperature. This result is consistent with the recently proven theorem that the phase-space Shannon information entropy attains its maximum at constant temperature.

  16. Relations among several nuclear and electronic density functional reactivity indexes

    Science.gov (United States)

    Torrent-Sucarrat, Miquel; Luis, Josep M.; Duran, Miquel; Toro-Labbé, Alejandro; Solà, Miquel

    2003-11-01

    An expansion of the energy functional in terms of the total number of electrons and the normal coordinates within the canonical ensemble is presented. A comparison of this expansion with the expansion of the energy in terms of the total number of electrons and the external potential leads to new relations among common density functional reactivity descriptors. The formulas obtained provide explicit links between important quantities related to the chemical reactivity of a system. In particular, the relation between the nuclear and the electronic Fukui functions is recovered. The connection between the derivatives of the electronic energy and the nuclear repulsion energy with respect to the external potential offers a proof for the "Quantum Chemical le Chatelier Principle." Finally, the nuclear linear response function is defined and the relation of this function with the electronic linear response function is given.

  17. Polarization observables in the longitudinal basis for pseudo-scalar meson photoproduction using a density matrix approach

    Energy Technology Data Exchange (ETDEWEB)

    Biplab Dey, Michael E. McCracken, David G. Ireland, Curtis A. Meyer

    2011-05-01

    The complete expression for the intensity in pseudo-scalar meson photoproduction with a polarized beam, target, and recoil baryon is derived using a density matrix approach that offers great economy of notation. A Cartesian basis with spins for all particles quantized along a single direction, the longitudinal beam direction, is used for consistency and clarity in interpretation. A single spin-quantization axis for all particles enables the amplitudes to be written in a manifestly covariant fashion with simple relations to those of the well-known CGLN formalism. Possible sign discrepancies between theoretical amplitude-level expressions and experimentally measurable intensity profiles are dealt with carefully. Our motivation is to provide a coherent framework for coupled-channel partial-wave analysis of several meson photoproduction reactions, incorporating recently published and forthcoming polarization data from Jefferson Lab.

  18. Natural Units for Nuclear Energy Density Functional Theory

    Energy Technology Data Exchange (ETDEWEB)

    Kortelainen, Erno M [ORNL; Furnstahl, R. J. [Ohio State University; Nazarewicz, W. [University of Tennessee, Knoxville (UTK) & Oak Ridge National Laboratory (ORNL); Stoitsov, M. V. [University of Tennessee, Knoxville (UTK) & Oak Ridge National Laboratory (ORNL)

    2010-01-01

    Naive dimensional analysis based on chiral effective theory, when adapted to nuclear energy density functionals, prescribes natural units and a hierarchy of contributions that could be used to constrain fits of generalized functionals. By applying these units, a large sample of Skyrme parametrizations is examined for naturalness, which is signaled by dimensionless coupling constants of order one. The bulk of the parameters are found to be natural, with an underlying scale consistent with other determinations. Significant deviations from unity are associated with deficiencies in the corresponding terms of particular functionals or with an incomplete optimization procedure.

  19. Best Probability Density Function for Random Sampled Data.

    Science.gov (United States)

    Jacobs, Donald J

    2009-12-04

    The maximum entropy method is a theoretically sound approach to construct an analytical form for the probability density function (pdf) given a sample of random events. In practice, numerical methods employed to determine the appropriate Lagrange multipliers associated with a set of moments are generally unstable in the presence of noise due to limited sampling. A robust method is presented that always returns the best pdf, where tradeoff in smoothing a highly varying function due to noise can be controlled. An unconventional adaptive simulated annealing technique, called funnel diffusion, determines expansion coefficients for Chebyshev polynomials in the exponential function.

  20. Best Probability Density Function for Random Sampled Data

    Directory of Open Access Journals (Sweden)

    Donald J. Jacobs

    2009-12-01

    Full Text Available The maximum entropy method is a theoretically sound approach to construct an analytical form for the probability density function (pdf given a sample of random events. In practice, numerical methods employed to determine the appropriate Lagrange multipliers associated with a set of moments are generally unstable in the presence of noise due to limited sampling. A robust method is presented that always returns the best pdf, where tradeoff in smoothing a highly varying function due to noise can be controlled. An unconventional adaptive simulated annealing technique, called funnel diffusion, determines expansion coefficients for Chebyshev polynomials in the exponential function.

  1. General framework for fluctuating dynamic density functional theory

    Science.gov (United States)

    Durán-Olivencia, Miguel A.; Yatsyshin, Peter; Goddard, Benjamin D.; Kalliadasis, Serafim

    2017-12-01

    We introduce a versatile bottom-up derivation of a formal theoretical framework to describe (passive) soft-matter systems out of equilibrium subject to fluctuations. We provide a unique connection between the constituent-particle dynamics of real systems and the time evolution equation of their measurable (coarse-grained) quantities, such as local density and velocity. The starting point is the full Hamiltonian description of a system of colloidal particles immersed in a fluid of identical bath particles. Then, we average out the bath via Zwanzig’s projection-operator techniques and obtain the stochastic Langevin equations governing the colloidal-particle dynamics. Introducing the appropriate definition of the local number and momentum density fields yields a generalisation of the Dean-Kawasaki (DK) model, which resembles the stochastic Navier-Stokes description of a fluid. Nevertheless, the DK equation still contains all the microscopic information and, for that reason, does not represent the dynamical law of observable quantities. We address this controversial feature of the DK description by carrying out a nonequilibrium ensemble average. Adopting a natural decomposition into local-equilibrium and nonequilibrium contribution, where the former is related to a generalised version of the canonical distribution, we finally obtain the fluctuating-hydrodynamic equation governing the time-evolution of the mesoscopic density and momentum fields. Along the way, we outline the connection between the ad hoc energy functional introduced in previous DK derivations and the free-energy functional from classical density-functional theory. The resultant equation has the structure of a dynamical density-functional theory (DDFT) with an additional fluctuating force coming from the random interactions with the bath. We show that our fluctuating DDFT formalism corresponds to a particular version of the fluctuating Navier-Stokes equations, originally derived by Landau and Lifshitz

  2. Solvent density inhomogeneities and solvation free energies in supercritical diatomic fluids: a density functional approach.

    Science.gov (United States)

    Husowitz, B; Talanquer, V

    2007-02-07

    Density functional theory is used to explore the solvation properties of a spherical solute immersed in a supercritical diatomic fluid. The solute is modeled as a hard core Yukawa particle surrounded by a diatomic Lennard-Jones fluid represented by two fused tangent spheres using an interaction site approximation. The authors' approach is particularly suitable for thoroughly exploring the effect of different interaction parameters, such as solute-solvent interaction strength and range, solvent-solvent long-range interactions, and particle size, on the local solvent structure and the solvation free energy under supercritical conditions. Their results indicate that the behavior of the local coordination number in homonuclear diatomic fluids follows trends similar to those reported in previous studies for monatomic fluids. The local density augmentation is particularly sensitive to changes in solute size and is affected to a lesser degree by variations in the solute-solvent interaction strength and range. The associated solvation free energies exhibit a nonmonotonous behavior as a function of density for systems with weak solute-solvent interactions. The authors' results suggest that solute-solvent interaction anisotropies have a major influence on the nature and extent of local solvent density inhomogeneities and on the value of the solvation free energies in supercritical solutions of heteronuclear molecules.

  3. LABORATORY FREQUENCY REDISTRIBUTION FUNCTION FOR THE POLARIZED Λ-TYPE THREE-TERM ATOM

    Energy Technology Data Exchange (ETDEWEB)

    Casini, R. [High Altitude Observatory, National Center for Atmospheric Research, P.O. Box 3000, Boulder, CO 80307-3000 (United States); Manso Sainz, R. [Max Planck Institute for Solar System Research, Justus-von-Liebig-Weg 3, D-37077 Göttingen (Germany)

    2016-12-20

    We present the frequency redistribution function for a polarized three-term atom of the Λ-type in the collisionless regime, and we specialize it to the case where both the initial and final terms of the three-state transition are metastable (i.e., with infinitely sharp levels). This redistribution function represents a generalization of the well-known R {sub II} function to the case where the lower terms of the transition can be polarized and carry atomic coherence, and it can be applied to the investigation of polarized line formation in tenuous plasmas, where collisional rates may be low enough that anisotropy-induced atomic polarization survives even in the case of metastable levels.

  4. Steady-State Density Functional Theory for Finite Bias Conductances.

    Science.gov (United States)

    Stefanucci, G; Kurth, S

    2015-12-09

    In the framework of density functional theory, a formalism to describe electronic transport in the steady state is proposed which uses the density on the junction and the steady current as basic variables. We prove that, in a finite window around zero bias, there is a one-to-one map between the basic variables and both local potential on as well as bias across the junction. The resulting Kohn-Sham system features two exchange-correlation (xc) potentials, a local xc potential, and an xc contribution to the bias. For weakly coupled junctions the xc potentials exhibit steps in the density-current plane which are shown to be crucial to describe the Coulomb blockade diamonds. At small currents these steps emerge as the equilibrium xc discontinuity bifurcates. The formalism is applied to a model benzene junction, finding perfect agreement with the orthodox theory of Coulomb blockade.

  5. 3-D time-domain induced polarization tomography: a new approach based on a source current density formulation

    Science.gov (United States)

    Soueid Ahmed, A.; Revil, A.

    2018-04-01

    Induced polarization (IP) of porous rocks can be associated with a secondary source current density, which is proportional to both the intrinsic chargeability and the primary (applied) current density. This gives the possibility of reformulating the time domain induced polarization (TDIP) problem as a time-dependent self-potential-type problem. This new approach implies a change of strategy regarding data acquisition and inversion, allowing major time savings for both. For inverting TDIP data, we first retrieve the electrical resistivity distribution. Then, we use this electrical resistivity distribution to reconstruct the primary current density during the injection/retrieval of the (primary) current between the current electrodes A and B. The time-lapse secondary source current density distribution is determined given the primary source current density and a distribution of chargeability (forward modelling step). The inverse problem is linear between the secondary voltages (measured at all the electrodes) and the computed secondary source current density. A kernel matrix relating the secondary observed voltages data to the source current density model is computed once (using the electrical conductivity distribution), and then used throughout the inversion process. This recovered source current density model is in turn used to estimate the time-dependent chargeability (normalized voltages) in each cell of the domain of interest. Assuming a Cole-Cole model for simplicity, we can reconstruct the 3-D distributions of the relaxation time τ and the Cole-Cole exponent c by fitting the intrinsic chargeability decay curve to a Cole-Cole relaxation model for each cell. Two simple cases are studied in details to explain this new approach. In the first case, we estimate the Cole-Cole parameters as well as the source current density field from a synthetic TDIP data set. Our approach is successfully able to reveal the presence of the anomaly and to invert its Cole

  6. Stability criterion for superfluidity based on the density spectral function

    Science.gov (United States)

    Watabe, Shohei; Kato, Yusuke

    2013-12-01

    We study a stability criterion hypothesis for superfluids expressed in terms of the local density spectral function In(r,ω) that is applicable to both homogeneous and inhomogeneous systems. We evaluate the local density spectral function in the presence of a one-dimensional repulsive or attractive external potential within Bogoliubov theory, using solutions for the tunneling problem. We also evaluate the local density spectral function using an orthogonal basis, and calculate the autocorrelation function Cn(r,t). When superfluids in a d-dimensional system flow below a threshold, In(r,ω)∝ωd holds in the low-energy regime and Cn(r,t)∝1/td+1 holds in the long-time regime. However, when superfluids flow with the critical current, In(r,ω)∝ωβ holds in the low-energy regime and Cn(r,t)∝1/tβ+1 holds in the long-time regime with β

  7. Open-system Kohn-Sham density functional theory.

    Science.gov (United States)

    Zhou, Yongxi; Ernzerhof, Matthias

    2012-03-07

    A simple model for electron transport through molecules is provided by the source-sink potential (SSP) method [F. Goyer, M. Ernzerhof, and M. Zhuang, J. Chem. Phys. 126, 144104 (2007)]. In SSP, the boundary conditions of having an incoming and outgoing electron current are enforced through complex potentials that are added to the Hamiltonian. Depending on the sign of the imaginary part of the potentials, current density is generated or absorbed. In this way, a finite system can be used to model infinite molecular electronic devices. The SSP has originally been developed for the Hückel method and subsequently it has been extended [F. Goyer and M. Ernzerhof, J. Chem. Phys. 134, 174101 (2011)] to the Hubbard model. Here we present a step towards its generalization for first-principles electronic structure theory methods. In particular, drawing on our earlier work, we discuss a new generalized density functional theory for complex non-Hermitian Hamiltonians. This theory enables us to combine SSP and Kohn-Sham theory to obtain a method for the description of open systems that exchange current density with their environment. Similarly, the Hartree-Fock method is extended to the realm of non-Hermitian, SSP containing Hamiltonians. As a proof of principle, we present the first applications of complex-density functional theory (CODFT) as well as non-Hermitian Hartree-Fock theory to electron transport through molecules. © 2012 American Institute of Physics

  8. Extending density functional embedding theory for covalently bonded systems.

    Science.gov (United States)

    Yu, Kuang; Carter, Emily A

    2017-12-19

    Quantum embedding theory aims to provide an efficient solution to obtain accurate electronic energies for systems too large for full-scale, high-level quantum calculations. It adopts a hierarchical approach that divides the total system into a small embedded region and a larger environment, using different levels of theory to describe each part. Previously, we developed a density-based quantum embedding theory called density functional embedding theory (DFET), which achieved considerable success in metals and semiconductors. In this work, we extend DFET into a density-matrix-based nonlocal form, enabling DFET to study the stronger quantum couplings between covalently bonded subsystems. We name this theory density-matrix functional embedding theory (DMFET), and we demonstrate its performance in several test examples that resemble various real applications in both chemistry and biochemistry. DMFET gives excellent results in all cases tested thus far, including predicting isomerization energies, proton transfer energies, and highest occupied molecular orbital-lowest unoccupied molecular orbital gaps for local chromophores. Here, we show that DMFET systematically improves the quality of the results compared with the widely used state-of-the-art methods, such as the simple capped cluster model or the widely used ONIOM method.

  9. One-Photon Absorption Properties from a Hybrid Polarizable Density Embedding/Complex Polarization Propagator Approach for Polarizable Solutions

    DEFF Research Database (Denmark)

    Hršak, Dalibor; Nørby, Morten Steen; Coriani, Sonia

    2018-01-01

    We present a formulation of the polarizable density embedding (PDE) method in combination with the complex polarization propagator (CPP) method for the calculation of absorption spectra of molecules in solutions. The method is particularly useful for the calculation of near-edge X-ray absorption...... fine structure (NEXAFS) spectra. We compare the performance of PDE-CPP with the previously formulated polarizable embedding (PE)-CPP model for the calculation of the NEXAFS spectra of adenine, formamide, glycine, and adenosine triphosphate (ATP) in water at the carbon and nitrogen K-edges, as well...

  10. Off-diagonal helicity density matrix elements for vector mesons produced in polarized e+e- processes

    International Nuclear Information System (INIS)

    Anselmino, M.; Murgia, F.; Quintairos, P.

    1999-04-01

    Final state q q-bar interactions give origin to non zero values of the off-diagonal element ρ 1,-1 of the helicity density matrix of vector mesons produced in e + e - annihilations, as confirmed by recent OPAL data on φ, D * and K * 's. New predictions are given for ρ 1,-1 of several mesons produced at large x E and small p T - i.e. collinear with the parent jet - in the annihilation of polarized 3 + and 3 - , the results depend strongly on the elementary dynamics and allow further non trivial tests of the standard model. (author)

  11. Classical and quantum theories of the polarization bremsstrahlung in the local electron density model

    International Nuclear Information System (INIS)

    Astapenko, V.A.; Bureeva, L.A.; Lisitsa, V.S.

    2000-01-01

    Classical and quantum theories of polarization bremsstrahlung in a statistical (Thomas-Fermi) potential of complex atoms and ions are developed. The basic assumptions of the theories correspond to the approximations employed earlier in classical and quantum calculations of ordinary bremsstrahlung in a static potential. This makes it possible to study on a unified basis the contribution of both channels in the radiation taking account of their interference. The classical model makes it possible to obtain simple universal formulas for the spectral characteristics of the radiation. The theory is applied to electrons with moderate energies, which are characteristic for plasma applications, specifically, radiation from electrons on the argon-like ion KII at frequencies close to its ionization potential. The computational results show the importance of taking account of the polarization channel of the radiation for plasma with heavy ions

  12. Analyzing the financial crisis using the entropy density function

    Science.gov (United States)

    Oh, Gabjin; Kim, Ho-yong; Ahn, Seok-Won; Kwak, Wooseop

    2015-02-01

    The risk that is created by nonlinear interactions among subjects in economic systems is assumed to increase during an abnormal state of a financial market. Nevertheless, investigating the systemic risk in financial markets following the global financial crisis is not sufficient. In this paper, we analyze the entropy density function in the return time series for several financial markets, such as the S&P500, KOSPI, and DAX indices, from October 2002 to December 2011 and analyze the variability in the entropy value over time. We find that the entropy density function of the S&P500 index during the subprime crisis exhibits a significant decrease compared to that in other periods, whereas the other markets, such as those in Germany and Korea, exhibit no significant decrease during the market crisis. These findings demonstrate that the S&P500 index generated a regular pattern in the return time series during the financial crisis.

  13. A J matrix engine for density functional theory calculations

    International Nuclear Information System (INIS)

    White, C.A.; Head-Gordon, M.

    1996-01-01

    We introduce a new method for the formation of the J matrix (Coulomb interaction matrix) within a basis of Cartesian Gaussian functions, as needed in density functional theory and Hartree endash Fock calculations. By summing the density matrix into the underlying Gaussian integral formulas, we have developed a J matrix open-quote open-quote engine close-quote close-quote which forms the exact J matrix without explicitly forming the full set of two electron integral intermediates. Several precomputable quantities have been identified, substantially reducing the number of floating point operations and memory accesses needed in a J matrix calculation. Initial timings indicate a speedup of greater than four times for the (pp parallel pp) class of integrals with speedups increasing to over ten times for (ff parallel ff) integrals. copyright 1996 American Institute of Physics

  14. Covariance analysis for energy density functionals and instabilities

    International Nuclear Information System (INIS)

    Roca-Maza, X; Colò, G; Paar, N

    2015-01-01

    We present the covariance analysis of two successful nuclear energy density functionals (EDFs), (i) a non-relativistic Skyrme functional built from a zero-range effective interaction, and (ii) a relativistic nuclear EDF based on density dependent meson–nucleon couplings. The covariance analysis is a useful tool for understanding the limitations of a model, the correlations between observables and the statistical errors. We show, for our selected test nucleus 208 Pb, that when the constraint on a property A included in the fit is relaxed, correlations with other observables B become larger; on the other hand, when a strong constraint is imposed on A, the correlations with other properties become very small. We also provide a brief review, partly connected with the covariance analysis, of some instabilities displayed by several EDFs currently used in nuclear physics. (paper)

  15. Spin Propensities of Octahedral Complexes From Density Functional Theory

    DEFF Research Database (Denmark)

    Mortensen, Sara R.; Kepp, Kasper Planeta

    2015-01-01

    The fundamental balance between high- and low-spin states of transition metal systems depends on both the metal ion and the ligands surrounding it, as often visualized by the spectrochemical series. Most density functionals do not reproduce this balance, and real spin state propensities depend...... on orbital pairing and vibrational entropies absent in the spectrochemical series. Thus, we systematically computed the tendency toward high or low spin of "text-book" octahedral metal complexes versus ligand and metal type, using eight density functionals. Dispersion effects were generally ... assessment of spin state propensities versus ligand and metal type and reveal, e.g., that CN- is consistently weaker than CO for M(II) but stronger than CO for M(III) and SCN- and NCS- change order in M(II) versus M(III) complexes. Contrary to expectation based on the spectrochemical series, Cl- and Br...

  16. What Density Functional Theory could do for Quantum Information

    Science.gov (United States)

    Mattsson, Ann

    2015-03-01

    The Hohenberg-Kohn theorem of Density Functional Theory (DFT), and extensions thereof, tells us that all properties of a system of electrons can be determined through their density, which uniquely determines the many-body wave-function. Given access to the appropriate, universal, functionals of the density we would, in theory, be able to determine all observables of any electronic system, without explicit reference to the wave-function. On the other hand, the wave-function is at the core of Quantum Information (QI), with the wave-function of a set of qubits being the central computational resource in a quantum computer. While there is seemingly little overlap between DFT and QI, reliance upon observables form a key connection. Though the time-evolution of the wave-function and associated phase information is fundamental to quantum computation, the initial and final states of a quantum computer are characterized by observables of the system. While observables can be extracted directly from a system's wave-function, DFT tells us that we may be able to intuit a method for extracting them from its density. In this talk, I will review the fundamentals of DFT and how these principles connect to the world of QI. This will range from DFT's utility in the engineering of physical qubits, to the possibility of using it to efficiently (but approximately) simulate Hamiltonians at the logical level. The apparent paradox of describing algorithms based on the quantum mechanical many-body wave-function with a DFT-like theory based on observables will remain a focus throughout. The ultimate goal of this talk is to initiate a dialog about what DFT could do for QI, in theory and in practice. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

  17. Polarization dependence of the spin-density-wave excitations in single-domain chromium

    Energy Technology Data Exchange (ETDEWEB)

    Boeni, P. [Paul Scherrer Inst. (PSI), Villigen (Switzerland); Roessli, B. [Institut Max von Laue - Paul Langevin, 75 - Paris (France); Sternlieb, B.J. [Brookhaven (United States); Lorenzo, E. [Centre National de la Recherche Scientifique (CNRS), 38 - Grenoble (France); Werner, S.A. [Missouri (United States)

    1997-09-01

    A polarized neutron scattering experiment has been performed with a single-Q, single domain sample of chromium in a magnetic field of 4 T. It is confirmed that the longitudinal fluctuations are enhanced for small energy transfers and that the spin wave modes with {delta}S parallel to Q and {delta}S perpendicular to Q are similar. (author) 2 figs., 1 tab., 2 refs.

  18. Buckled graphene: A model study based on density functional theory

    KAUST Repository

    Khan, Yasser

    2010-09-01

    We make use of ab initio calculations within density functional theory to investigate the influence of buckling on the electronic structure of single layer graphene. Our systematic study addresses a wide range of bond length and bond angle variations in order to obtain insights into the energy scale associated with the formation of ripples in a graphene sheet. © 2010 Elsevier B.V. All rights reserved.

  19. Green's function based density estimation

    Energy Technology Data Exchange (ETDEWEB)

    Kovesarki, Peter; Brock, Ian C.; Nuncio Quiroz, Adriana Elizabeth [Physikalisches Institut, Universitaet Bonn (Germany)

    2012-07-01

    A method was developed based on Green's function identities to estimate probability densities. This can be used for likelihood estimations and for binary classifications. It offers several advantages over neural networks, boosted decision trees and other, regression based classifiers. For example, it is less prone to overtraining, and it is much easier to combine several samples. Some capabilities are demonstrated using ATLAS data.

  20. Density functional theory calculations of charge transport properties ...

    Indian Academy of Sciences (India)

    In this paper, we used density functional theory (DFT) at the M06-2X/6−31+G(d) level to compute the charge transport rates of nine coronene topological structures. The results show that the energy gap of these nine coronene derivatives is in the range 2.90–3.30 eV, falling into the organic semiconductor category. The size ...

  1. Density functional theory studies of transition metal nanoparticles in catalysis

    DEFF Research Database (Denmark)

    Greeley, Jeffrey Philip; Rankin, Rees; Zeng, Zhenhua

    2013-01-01

    Periodic Density Functional Theory calculations are capable of providing powerful insights into the structural, energetics, and electronic phenomena that underlie heterogeneous catalysis on transition metal nanoparticles. Such calculations are now routinely applied to single crystal metal surfaces...... and electrocatalysis, in which single crystal models are combined with Wulff construction-based ideas to produce descriptions of average nanocatalyst behavior. Then, I will proceed to describe explicitly DFT-based descriptions of catalysis on truly nanosized particles (

  2. Energy-Pressure-Velocity Filtered Mass Density Function

    Science.gov (United States)

    Nik, Mehdi B.; Givi, Peyman; Madnia, Cyrus; Pope, Stephen B.

    2010-11-01

    A new methodology termed "energy-pressure-velocity filtered mass density function" (EPV-FMDF) is developed for large eddy simulation of high speed turbulent flows. This is an extension of the previously developed "velocity filtered density function" (V-FDF) method [1] in low speed flows. To account for the effect of compressibility, the formulation includes two additional thermodynamic variables: the pressure and the internal energy. This is the most general form of the FDF for high speed flow simulations. The EPV-FMDF is obtained by solving its transport equation, in which the effects of convection appear in a closed form. The unclosed terms are modeled in a fashion similar to that in RANS-PDF methods. The modeled EPV-FMDF transport equation is solved by a Lagrangian Monte Carlo method and is employed for LES of a temporally developing mixing layer at several values of the convective Mach number. The predicted results are assessed by comparison with direct numerical simulation (DNS) data.[4pt] [1] Gicquel, L. Y. M., Givi, P., Jaberi, F. A., and Pope, S. B., Velocity Filtered Density Function for Large Eddy Simulation of Turbulent Flows, Phys. Fluids, 14 (3):1196-1213 (2002).

  3. Spin dependent fragmentation functions for heavy flavor baryons and single heavy hyperon polarization

    CERN Document Server

    Goldstein, G R

    2001-01-01

    Spin dependent fragmentation functions for heavy flavor quarks to fragment into heavy baryons are calculated in a quark-diquark model. The production of intermediate spin 1/2 and 3/2 excited states is explicity included. $\\Lambda_b$ , $\\Lambda_c$ and $\\Xi_c$ production rate and polarization at LEP energies are calculated and, where possible, compared with experiment. A different approach, also relying on a heavy quark-diquark model, is proposed for the small momentum transfer inclusive production of polarized heavy flavor hyperons. The predicted $\\Lambda_c$ polarization is roughly in agreement with experiment.

  4. Spin-density functional for exchange anisotropic Heisenberg model

    International Nuclear Information System (INIS)

    Prata, G.N.; Penteado, P.H.; Souza, F.C.; Libero, Valter L.

    2009-01-01

    Ground-state energies for antiferromagnetic Heisenberg models with exchange anisotropy are estimated by means of a local-spin approximation made in the context of the density functional theory. Correlation energy is obtained using the non-linear spin-wave theory for homogeneous systems from which the spin functional is built. Although applicable to chains of any size, the results are shown for small number of sites, to exhibit finite-size effects and allow comparison with exact-numerical data from direct diagonalization of small chains.

  5. Time-dependent density-functional theory concepts and applications

    CERN Document Server

    Ullrich, Carsten A

    2011-01-01

    Time-dependent density-functional theory (TDDFT) describes the quantum dynamics of interacting electronic many-body systems formally exactly and in a practical and efficient manner. TDDFT has become the leading method for calculating excitation energies and optical properties of large molecules, with accuracies that rival traditional wave-function based methods, but at a fraction of the computational cost.This book is the first graduate-level text on the concepts and applications of TDDFT, including many examples and exercises, and extensive coverage of the literature. The book begins with a s

  6. Formation energies of rutile metal dioxides using density functional theory

    DEFF Research Database (Denmark)

    Martinez, Jose Ignacio; Hansen, Heine Anton; Rossmeisl, Jan

    2009-01-01

    We apply standard density functional theory at the generalized gradient approximation (GGA) level to study the stability of rutile metal oxides. It is well known that standard GGA exchange and correlation in some cases is not sufficient to address reduction and oxidation reactions. Especially......, Ge, Ti, Cr, Nb, W, Mo, and V, using the electrochemical series as reference. The mean absolute error of the formation energy is 0.29 eV using the revised Perdew-Burke-Ernzerhof (PBE) GGA functional. We believe that the reason for the success is due to the reference level being H-2 and H2O and not O-2...

  7. Local and linear chemical reactivity response functions at finite temperature in density functional theory

    International Nuclear Information System (INIS)

    Franco-Pérez, Marco; Ayers, Paul W.; Gázquez, José L.; Vela, Alberto

    2015-01-01

    We explore the local and nonlocal response functions of the grand canonical potential density functional at nonzero temperature. In analogy to the zero-temperature treatment, local (e.g., the average electron density and the local softness) and nonlocal (e.g., the softness kernel) intrinsic response functions are defined as partial derivatives of the grand canonical potential with respect to its thermodynamic variables (i.e., the chemical potential of the electron reservoir and the external potential generated by the atomic nuclei). To define the local and nonlocal response functions of the electron density (e.g., the Fukui function, the linear density response function, and the dual descriptor), we differentiate with respect to the average electron number and the external potential. The well-known mathematical relationships between the intrinsic response functions and the electron-density responses are generalized to nonzero temperature, and we prove that in the zero-temperature limit, our results recover well-known identities from the density functional theory of chemical reactivity. Specific working equations and numerical results are provided for the 3-state ensemble model

  8. Functional thermo-dynamics: a generalization of dynamic density functional theory to non-isothermal situations.

    Science.gov (United States)

    Anero, Jesús G; Español, Pep; Tarazona, Pedro

    2013-07-21

    We present a generalization of Density Functional Theory (DFT) to non-equilibrium non-isothermal situations. By using the original approach set forth by Gibbs in his consideration of Macroscopic Thermodynamics (MT), we consider a Functional Thermo-Dynamics (FTD) description based on the density field and the energy density field. A crucial ingredient of the theory is an entropy functional, which is a concave functional. Therefore, there is a one to one connection between the density and energy fields with the conjugate thermodynamic fields. The connection between the three levels of description (MT, DFT, FTD) is clarified through a bridge theorem that relates the entropy of different levels of description and that constitutes a generalization of Mermin's theorem to arbitrary levels of description whose relevant variables are connected linearly. Although the FTD level of description does not provide any new information about averages and correlations at equilibrium, it is a crucial ingredient for the dynamics in non-equilibrium states. We obtain with the technique of projection operators the set of dynamic equations that describe the evolution of the density and energy density fields from an initial non-equilibrium state towards equilibrium. These equations generalize time dependent density functional theory to non-isothermal situations. We also present an explicit model for the entropy functional for hard spheres.

  9. Linear density response function in the projector augmented wave method

    DEFF Research Database (Denmark)

    Yan, Jun; Mortensen, Jens Jørgen; Jacobsen, Karsten Wedel

    2011-01-01

    We present an implementation of the linear density response function within the projector-augmented wave method with applications to the linear optical and dielectric properties of both solids, surfaces, and interfaces. The response function is represented in plane waves while the single...... functions of Si, C, SiC, AlP, and GaAs compare well with previous calculations. While optical properties of semiconductors, in particular excitonic effects, are generally not well described by ALDA, we obtain excellent agreement with experiments for the surface loss function of graphene and the Mg(0001......) surface with plasmon energies deviating by less than 0.2 eV. Finally, the method is applied to study the influence of substrates on the plasmon excitations in graphene....

  10. Density Functional Methods for Shock Physics and High Energy Density Science

    Science.gov (United States)

    Desjarlais, Michael

    2017-06-01

    Molecular dynamics with density functional theory has emerged over the last two decades as a powerful and accurate framework for calculating thermodynamic and transport properties with broad application to dynamic compression, high energy density science, and warm dense matter. These calculations have been extensively validated against shock and ramp wave experiments, are a principal component of high-fidelity equation of state generation, and are having wide-ranging impacts on inertial confinement fusion, planetary science, and shock physics research. In addition to thermodynamic properties, phase boundaries, and the equation of state, one also has access to electrical conductivity, thermal conductivity, and lower energy optical properties. Importantly, all these properties are obtained within the same theoretical framework and are manifestly consistent. In this talk I will give a brief history and overview of molecular dynamics with density functional theory and its use in calculating a wide variety of thermodynamic and transport properties for materials ranging from ambient to extreme conditions and with comparisons to experimental data. I will also discuss some of the limitations and difficulties, as well as active research areas. Sandia is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

  11. Recent developments in LIBXC - A comprehensive library of functionals for density functional theory

    Science.gov (United States)

    Lehtola, Susi; Steigemann, Conrad; Oliveira, Micael J. T.; Marques, Miguel A. L.

    2018-01-01

    LIBXC is a library of exchange-correlation functionals for density-functional theory. We are concerned with semi-local functionals (or the semi-local part of hybrid functionals), namely local-density approximations, generalized-gradient approximations, and meta-generalized-gradient approximations. Currently we include around 400 functionals for the exchange, correlation, and the kinetic energy, spanning more than 50 years of research. Moreover, LIBXC is by now used by more than 20 codes, not only from the atomic, molecular, and solid-state physics, but also from the quantum chemistry communities.

  12. Individual effects of seasonal changes, visitor density, and concurrent bear behavior on stereotypical behaviors in captive polar bears (Ursus maritimus).

    Science.gov (United States)

    Kelly, Krista R; Harrison, Michelle L; Size, Daniele D; MacDonald, Suzanne E

    2015-01-01

    Stereotypical behaviors in captive polar bears (Ursus maritimus) can be detrimental to their welfare. These behaviors can be reduced through enrichment programs but are often not completely eliminated, so identifying potential triggers is important. The present study investigated the influences of seasonal changes, visitor density, and concurrent bear activity on stereotypical behaviors exhibited by 3 captive polar bears at the Toronto Zoo. All bears exhibited these behaviors; however, individual differences were found in duration and form. The male exhibited less stereotypical behavior during spring, and the females exhibited less stereotypical behavior during winter. An increase in visitor density was associated with more stereotypical behavior in 1 female but less stereotypical behavior in the other 2 bears. All bears engaged in more stereotypical behaviors when the other bears were inactive, and 1 female engaged in more stereotypical behaviors when the other bears were out of sight. Further, when conspecifics were active, all bears engaged in less stereotypical behaviors. Given the variability among individual bears, future enrichment programs must be tailored to the needs of individuals to maximize efficacy.

  13. Drifting field-aligned density structures in the night-side polar cap

    Czech Academy of Sciences Publication Activity Database

    Santolík, Ondřej; Persoon, A. M.; Gurnett, D. A.; Décréau, P. M. E.; Pickett, J. S.; Maršálek, O.; Maksimovic, M.; Cornilleau-Wehrlin, N.

    2005-01-01

    Roč. 32, - (2005), L06106-1 ISSN 0094-8276 R&D Projects: GA ČR(CZ) GA202/03/0832; GA MŠk ME 650; GA MŠk 1P05ME811 Grant - others: NASA (US) NAG5-9974; NASA (US) NNG04GB98G; NSF(US) 0307319; ESA PECS(XE) 98025 Institutional research plan: CEZ:AV0Z30420517 Keywords : Magnetospheric Physics * Plasma convection * Plasma waves and instabilities * Polar cap phenomena * Magnetospheric configuration and dynamics Subject RIV: BL - Plasma and Gas Discharge Physics Impact factor: 2.491, year: 2005

  14. The polarized structure function of the nucleons with a non-extensive statistical quark model

    Energy Technology Data Exchange (ETDEWEB)

    Trevisan, Luis A. [Departamento de Matematica e Estatistica, Universidade Estadual de Ponta Grossa, 84010-790, Ponta Grossa, PR (Brazil); Mirez, Carlos [Instituto de Ciencia, Engenharia e Tecnologia - ICET, Universidade Federal dos Vales do Jequitinhonha e Mucuri - UFVJM, Campus do Mucuri, Rua do Cruzeiro 01, Jardim Sao Paulo, 39803-371, Teofilo Otoni, Minas Gerais (Brazil)

    2013-05-06

    We studied an application of nonextensive thermodynamics to describe the polarized structure function of nucleon, in a model where the usual Fermi-Dirac and Bose-Einstein energy distribution, often used in the statistical models, were replaced by the equivalent functions of the q-statistical. The parameters of the model are given by an effective temperature T, the q parameter (from Tsallis statistics), and the chemical potentials given by the corresponding up (u) and down (d) quark normalization in the nucleon and by {Delta}u and {Delta}d of the polarized functions.

  15. A relationship between the weighted density approximation and the local-scaling transformation version of density functional theory

    International Nuclear Information System (INIS)

    Diez, Reinaldo Pis; Karasiev, Valentin V

    2003-01-01

    A relationship between the auxiliary density, ρ(r), defined within the framework of the weighted density approximation and the kinetic energy modulating factor, A N ([ρ(r)]; r), which appears in the local-scaling transformation version of density functional theory is presented. This relationship imposes the condition of positiveness on the kinetic energy modulating factor and this, in turn, leads to an important mathematical condition on any approximate kinetic energy density functional. It is shown that two well-known approximate kinetic energy density functionals do not satisfy the above relationship at distances very close to the nucleus. By forcing a given approximate kinetic energy density functional to obey the above condition, both the kinetic and exchange energies can be obtained within a framework similar to that of the weighted density approximation. Results on some closed-shell atomic systems provide support for those ideas

  16. Density-dependence of functional spiking networks in vitro

    Energy Technology Data Exchange (ETDEWEB)

    Ham, Michael I [Los Alamos National Laboratory; Gintautuas, Vadas [Los Alamos National Laboratory; Rodriguez, Marko A [Los Alamos National Laboratory; Bettencourt, Luis M A [Los Alamos National Laboratory; Bennett, Ryan [UNIV OF NORTH TEXAS; Santa Maria, Cara L [UNIV OF NORTH TEXAS

    2008-01-01

    During development, the mammalian brain differentiates into specialized regions with unique functional abilities. While many factors contribute to this functional specialization, we explore the effect neuronal density can have on neuronal interactions. Two types of networks, dense (50,000 neurons and glia support cells) and sparse (12,000 neurons and glia support cells), are studied. A competitive first response model is applied to construct activation graphs that represent pairwise neuronal interactions. By observing the evolution of these graphs during development in vitro we observe that dense networks form activation connections earlier than sparse networks, and that link-!llltropy analysis of the resulting dense activation graphs reveals that balanced directional connections dominate. Information theoretic measures reveal in addition that early functional information interactions (of order 3) are synergetic in both dense and sparse networks. However, during development in vitro, such interactions become redundant in dense, but not sparse networks. Large values of activation graph link-entropy correlate strongly with redundant ensembles observed in the dense networks. Results demonstrate differences between dense and sparse networks in terms of informational groups, pairwise relationships, and activation graphs. These differences suggest that variations in cell density may result in different functional specialization of nervous system tissue also in vivo.

  17. Small scale density variations of electrons and charged particles in the vicinity of polar mesosphere summer echoes

    Directory of Open Access Journals (Sweden)

    M. Rapp

    2003-01-01

    Full Text Available We present small scale variations of electron number densities and particle charge number densities measured in situ in the presence of polar mesosphere summer echoes. It turns out that the small scale fluctuations of electrons and negatively charged particles show a strong anticorrelation down to the smallest scales observed. Comparing these small scale structures with the simultaneously measured radar signal to noise profile, we find that the radar profile is well described by the power spectral density of both electrons and charged particles at the radar half wavelength (=the Bragg scale. Finally, we consider the shape of the power spectra of the observed plasma fluctuations and find that both charged particles and electrons show spectra that can be explained in terms of either neutral air turbulence acting on the distribution of a low diffusivity tracer or the fossil remnants of a formerly active turbulent region. All these results are consistent with the theoretical ideas by Rapp and Lübken (2003 suggesting that PMSE can be explained by a combination of active and fossil neutral air turbulence acting on the large and heavy charged aerosol particles which are subsequently mirrored in the electron number density distribution that becomes visible to a VHF radar when small scale fluctuations are present.

  18. Benchmarks for electronically excited states: Time-dependent density functional theory and density functional theory based multireference configuration interaction

    DEFF Research Database (Denmark)

    Silva-Junior, Mario R.; Schreiber, Marko; Sauer, Stephan P. A.

    2008-01-01

    Time-dependent density functional theory (TD-DFT) and DFT-based multireference configuration interaction (DFT/MRCI) calculations are reported for a recently proposed benchmark set of 28 medium-sized organic molecules. Vertical excitation energies, oscillator strengths, and excited-state dipole...... moments are computed using the same geometries (MP2/6-31G*) and basis set (TZVP) as in our previous ab initio benchmark study on electronically excited states. The results from TD-DFT (with the functionals BP86, B3LYP, and BHLYP) and from DFT/MRCI are compared against the previous high-level ab initio...

  19. Dynamic density functional theory of solid tumor growth: Preliminary models

    Directory of Open Access Journals (Sweden)

    Arnaud Chauviere

    2012-03-01

    Full Text Available Cancer is a disease that can be seen as a complex system whose dynamics and growth result from nonlinear processes coupled across wide ranges of spatio-temporal scales. The current mathematical modeling literature addresses issues at various scales but the development of theoretical methodologies capable of bridging gaps across scales needs further study. We present a new theoretical framework based on Dynamic Density Functional Theory (DDFT extended, for the first time, to the dynamics of living tissues by accounting for cell density correlations, different cell types, phenotypes and cell birth/death processes, in order to provide a biophysically consistent description of processes across the scales. We present an application of this approach to tumor growth.

  20. Density functional calculations for atoms, molecules and clusters

    International Nuclear Information System (INIS)

    Gunnarsson, O.; Jones, R.O.

    1980-01-01

    The density functional formalism provides a framework for including exchange and correlation effects in the calculation of ground state properties of many-electron systems. The reduction of the problem to the solution of single-particle equations leads to important numerical advantages over other ab initio methods of incorporating correlation effects. The essential features of the scheme are outlined and results obtained for atomic and molecular systems are surveyed. The local spin density (LSD) approximation gives generally good results for systems where the bonding involves s and p electrons, but results are less satisfactory for d-bonded systems. Non-local modifications to the LSD approximation have been tested on atomic systems yielding much improved total energies. (Auth.)

  1. Spin exchange in polarized deuterium

    International Nuclear Information System (INIS)

    Przewoski, B. von; Meyer, H.O.; Balewski, J.; Doskow, J.; Ibald, R.; Pollock, R.E.; Rinckel, T.; Wellinghausen, A.; Whitaker, T.J.; Daehnick, W.W.; Haeberli, W.; Schwartz, B.; Wise, T.; Lorentz, B.; Rathmann, F.; Pancella, P.V.; Saha, Swapan K.; Thoerngren-Engblom, P.

    2003-01-01

    We have measured the vector and tensor polarization of an atomic deuterium target as a function of the target density. The polarized deuterium was produced in an atomic beam source and injected into a storage cell. For this experiment, the atomic beam source was operated without rf transitions, in order to avoid complications from the unknown efficiency of these transitions. In this mode, the atomic beam is vector and tensor polarized and both polarizations can be measured simultaneously. We used a 1.2-cm-diam and 27-cm-long storage cell, which yielded an average target density between 3 and 9x10 11 at/cm 3 . We find that the tensor polarization decreases with increasing target density while the vector polarization remains constant. The data are in quantitative agreement with the calculated effect of spin exchange between deuterium atoms at low field

  2. Density-functional method for nonequilibrium electron transport

    DEFF Research Database (Denmark)

    Brandbyge, Mads; Mozos, J.L.; Ordejon, P.

    2002-01-01

    We describe an ab initio method for calculating the electronic structure, electronic transport, and forces acting on the atoms, for atomic scale systems connected to semi-infinite electrodes and with an applied voltage bias. Our method is based on the density-functional theory (DFT) as implemented...... in the well tested SIESTA approach (which uses nonlocal norm-conserving pseudopotentials to describe the effect of the core electrons, and linear combination of finite-range numerical atomic orbitals to describe the valence states). We fully deal with the atomistic structure of the whole system, treating both...... the contact and the electrodes on the same footing. The effect of the finite bias (including self-consistency and the solution of the electrostatic problem) is taken into account using nonequilibrium Green's functions. We relate the nonequilibrium Green's function expressions to the more transparent scheme...

  3. Multi detector input and function generator for polarized neutron experiments

    International Nuclear Information System (INIS)

    De Blois, J.; Beunes, A.J.H.; Ende, P. v.d.; Osterholt, E.A.; Rekveldt, M.T.; Schipper, M.N.; Velthuis, S.G.E. te

    1998-01-01

    In this paper a VME module is described for static or stroboscopic measurements with a neutron scattering instrument, consisting essentially of a series of up to 64 3 He neutron detectors around a sample environment. Each detector is provided with an amplifier and a discriminator to separate the neutrons from noise. To reduce the wiring, the discriminator outputs are connected to the module by coding boxes. Two 16-inputs to one-output coding boxes generate serial output codes on a fiber optic connection. This basically fast connection reduces the dead time introduced by the coding, and the influence of environmental noise. With stroboscopic measurements a periodic function is used to affect the sample surrounded by a field coil. Each detected neutron is labeled with a data label containing the detector number and the time of detection with respect to a time reference. The data time base can be programmed on a linear or a nonlinear scale. An external source or an attribute of the periodic function may generate the time reference pulse. A 12-bit DAC connected to the output of an 8 K, 16-bits memory, where the pattern of the current has been stored before, generates the function. The function memory is scanned by the programmable function time base. Attributes are set by the four remaining bits of the memory. One separate detector input connects a monitor detector in the neutron beam with a 32-bit counter/timer that provides measuring on a preset count, preset time or preset frame. (orig.)

  4. Graphene oxide and adsorption of chloroform: A density functional study

    Energy Technology Data Exchange (ETDEWEB)

    Kuisma, Elena; Hansson, C. Fredrik; Lindberg, Th. Benjamin; Gillberg, Christoffer A.; Idh, Sebastian; Schröder, Elsebeth, E-mail: schroder@chalmers.se [Quantum Device Physics Laboratory, Microtechnology and Nanoscience (MC2), Chalmers University of Technology, SE-412 96 Göteborg (Sweden)

    2016-05-14

    Chlorinated hydrocarbon compounds are of environmental concerns, since they are toxic to humans and other mammals, and are widespread, and exposure is hard to avoid. Understanding and improving methods to reduce the amount of the substances are important. We present an atomic-scale calculational study of the adsorption of chlorine-based substance chloroform (CHCl{sub 3}) on graphene oxide, as a step in estimating the capacity of graphene oxide for filtering out such substances, e.g., from drinking water. The calculations are based on density functional theory, and the recently developed consistent-exchange functional for the van der Waals density-functional method is employed. We obtain values of the chloroform adsorption energy varying from roughly 0.2 to 0.4 eV per molecule. This is comparable to previously found results for chloroform adsorbed directly on clean graphene, using similar calculations. In a wet environment, like filters for drinking water, the graphene will not stay clean and will likely oxidize, and thus adsorption onto graphene oxide, rather than clean graphene, is a more relevant process to study.

  5. INTERACTIVE VISUALIZATION OF PROBABILITY AND CUMULATIVE DENSITY FUNCTIONS

    KAUST Repository

    Potter, Kristin

    2012-01-01

    The probability density function (PDF), and its corresponding cumulative density function (CDF), provide direct statistical insight into the characterization of a random process or field. Typically displayed as a histogram, one can infer probabilities of the occurrence of particular events. When examining a field over some two-dimensional domain in which at each point a PDF of the function values is available, it is challenging to assess the global (stochastic) features present within the field. In this paper, we present a visualization system that allows the user to examine two-dimensional data sets in which PDF (or CDF) information is available at any position within the domain. The tool provides a contour display showing the normed difference between the PDFs and an ansatz PDF selected by the user and, furthermore, allows the user to interactively examine the PDF at any particular position. Canonical examples of the tool are provided to help guide the reader into the mapping of stochastic information to visual cues along with a description of the use of the tool for examining data generated from an uncertainty quantification exercise accomplished within the field of electrophysiology.

  6. Density-functional computation of 99Ru NMR parameters

    Science.gov (United States)

    Buhl; Gaemers; Elsevier

    2000-09-01

    Gradient-corrected and hybrid variants of density-functional theory are used to compute the geometries and 99Ru chemical shifts of RuO4, [RuCp2], [K4Ru(CN)6], [Ru3(CO)12], [Ru(CO)3X3]- (X=Cl, I), [Ru(CO)2Cl4]2-, [Ru(bipy)3]2+, and [Ru(CO)2(iPr-DAB)(X)(Y)] [XY= Cl2, I2, MeCl, MeI, or (SnMe3)2]. For this set of compounds, substituent effects on delta(99Ru) are somewhat underestimated with the BPW91 pure density functional but are described well by the B3LYP hybrid functional, which can also be used to reproduce empirical trends in electric field gradients (EFGs) at the Ru nucleus qualitatively. In the [Ru(CO)2(iPr-DAB)XY] series, trends in the computed EFGs parallel those in the observed 99Ru NMR linewidths, in accordance with the quadrupolar relaxation mechanism expected for this nucleus. For this series of compounds, the use of X-ray-derived geometries affords a worse correlation between calculated EFGs and experimental linewidths than does the use of optimized geometries.

  7. New Methods of Esterification of Nanodiamonds in Fighting Breast Cancer-A Density Functional Theory Approach.

    Science.gov (United States)

    Landeros-Martinez, Linda-Lucila; Glossman-Mitnik, Daniel; Orrantia-Borunda, Erasmo; Flores-Holguín, Norma

    2017-10-19

    The use of nanodiamonds as anticancer drug delivery vehicles has received much attention in recent years. In this theoretical paper, we propose using different esterification methods for nanodiamonds. The monomers proposed are 2-hydroxypropanal, polyethylene glycol, and polyglicolic acid. Specifically, the hydrogen bonds, infrared (IR) spectra, molecular polar surface area, and reactivity parameters are analyzed. The monomers proposed for use in esterification follow Lipinski's rule of five, meaning permeability is good, they have good permeation, and their bioactivity is high. The results show that the complex formed between tamoxifen and nanodiamond esterified with polyglicolic acid presents the greatest number of hydrogen bonds and a good amount of molecular polar surface area. Calculations concerning the esterified nanodiamond and reactivity parameters were performed using Density Functional Theory with the M06 functional and the basis set 6-31G (d); for the esterified nanodiamond-Tamoxifen complexes, the semi-empirical method PM6 was used. The solvent effect has been taken into account by using implicit modelling and the conductor-like polarizable continuum model.

  8. New Methods of Esterification of Nanodiamonds in Fighting Breast Cancer—A Density Functional Theory Approach

    Directory of Open Access Journals (Sweden)

    Linda-Lucila Landeros-Martinez

    2017-10-01

    Full Text Available The use of nanodiamonds as anticancer drug delivery vehicles has received much attention in recent years. In this theoretical paper, we propose using different esterification methods for nanodiamonds. The monomers proposed are 2-hydroxypropanal, polyethylene glycol, and polyglicolic acid. Specifically, the hydrogen bonds, infrared (IR spectra, molecular polar surface area, and reactivity parameters are analyzed. The monomers proposed for use in esterification follow Lipinski’s rule of five, meaning permeability is good, they have good permeation, and their bioactivity is high. The results show that the complex formed between tamoxifen and nanodiamond esterified with polyglicolic acid presents the greatest number of hydrogen bonds and a good amount of molecular polar surface area. Calculations concerning the esterified nanodiamond and reactivity parameters were performed using Density Functional Theory with the M06 functional and the basis set 6–31G (d; for the esterified nanodiamond–Tamoxifen complexes, the semi-empirical method PM6 was used. The solvent effect has been taken into account by using implicit modelling and the conductor-like polarizable continuum model.

  9. Benchmarking Density Functionals for Chemical Bonds of Gold

    DEFF Research Database (Denmark)

    Kepp, Kasper Planeta

    2017-01-01

    Gold plays a major role in nanochemistry, catalysis, and electrochemistry. Accordingly, hundreds of studies apply density functionals to study chemical bonding with gold, yet there is no systematic attempt to assess the accuracy of these methods applied to gold. This paper reports a benchmark...... considering the diverse bonds to gold and the complication of relativistic effects. Thus, studies that use DFT with effective core potentials for gold chemistry, with no alternative due to computational cost, are on solid ground using TPSS-D3 or PBE-D3....

  10. Visualization techniques for spatial probability density function data

    Directory of Open Access Journals (Sweden)

    Udeepta D Bordoloi

    2006-01-01

    Full Text Available Novel visualization methods are presented for spatial probability density function data. These are spatial datasets, where each pixel is a random variable, and has multiple samples which are the results of experiments on that random variable. We use clustering as a means to reduce the information contained in these datasets; and present two different ways of interpreting and clustering the data. The clustering methods are used on two datasets, and the results are discussed with the help of visualization techniques designed for the spatial probability data.

  11. Application of Density Functional Theory to Systems Containing Metal Atoms

    Science.gov (United States)

    Bauschlicher, Charles W., Jr.

    2006-01-01

    The accuracy of density functional theory (DFT) for problems involving metal atoms is considered. The DFT results are compared with experiment as well as results obtained using the coupled cluster approach. The comparisons include geometries, frequencies, and bond energies. The systems considered include MO2, M(OH)+n, MNO+, and MCO+2. The DFT works well for frequencies and geometries, even in case with symmetry breaking; however, some examples have been found where the symmetry breaking is quite severe and the DFT methods do not work well. The calculation of bond energies is more difficult and examples of successes as well as failures of DFT will be given.

  12. Continuation of probability density functions using a generalized Lyapunov approach

    Energy Technology Data Exchange (ETDEWEB)

    Baars, S., E-mail: s.baars@rug.nl [Johann Bernoulli Institute for Mathematics and Computer Science, University of Groningen, P.O. Box 407, 9700 AK Groningen (Netherlands); Viebahn, J.P., E-mail: viebahn@cwi.nl [Centrum Wiskunde & Informatica (CWI), P.O. Box 94079, 1090 GB, Amsterdam (Netherlands); Mulder, T.E., E-mail: t.e.mulder@uu.nl [Institute for Marine and Atmospheric research Utrecht, Department of Physics and Astronomy, Utrecht University, Princetonplein 5, 3584 CC Utrecht (Netherlands); Kuehn, C., E-mail: ckuehn@ma.tum.de [Technical University of Munich, Faculty of Mathematics, Boltzmannstr. 3, 85748 Garching bei München (Germany); Wubs, F.W., E-mail: f.w.wubs@rug.nl [Johann Bernoulli Institute for Mathematics and Computer Science, University of Groningen, P.O. Box 407, 9700 AK Groningen (Netherlands); Dijkstra, H.A., E-mail: h.a.dijkstra@uu.nl [Institute for Marine and Atmospheric research Utrecht, Department of Physics and Astronomy, Utrecht University, Princetonplein 5, 3584 CC Utrecht (Netherlands); School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, NY (United States)

    2017-05-01

    Techniques from numerical bifurcation theory are very useful to study transitions between steady fluid flow patterns and the instabilities involved. Here, we provide computational methodology to use parameter continuation in determining probability density functions of systems of stochastic partial differential equations near fixed points, under a small noise approximation. Key innovation is the efficient solution of a generalized Lyapunov equation using an iterative method involving low-rank approximations. We apply and illustrate the capabilities of the method using a problem in physical oceanography, i.e. the occurrence of multiple steady states of the Atlantic Ocean circulation.

  13. Density functional theory calculations of Rh-β-diketonato complexes.

    Science.gov (United States)

    Conradie, J

    2015-01-28

    Density functional theory (DFT) results on the geometry, energies and charges of selected Rh-β-diketonato reactants, products and transition states are discussed. Various DFT techniques are used to increase our understanding of the orientation of ligands coordinated to Rh, to identify the lowest energy geometry of possible geometrical isomers and to get a molecular orbital understanding of ground and transition states. Trends and relationships obtained between DFT calculated energies and charges, experimentally measured values and electronic parameters describing the electron donating power of groups and ligands, enable the design of ligands and complexes of specific reactivity.

  14. The density functional theory and the charged fluid molecular dynamics

    International Nuclear Information System (INIS)

    Hansen, J.P.; Zerah, G.

    1993-01-01

    Car and Parrinello had the idea of combining the density functional theory (Hohenberg, Kohn and Sham) to the 'molecular dynamics' numerical modelling method, in order to simulate metallic or co-valent solids and liquids from the first principles. The objective of this paper is to present a simplified version of this method ab initio, applicable to classical and quantal charged systems. The method is illustrated with recent results on charged colloidal suspensions and highly correlated electron-proton plasmas. 1 fig., 21 refs

  15. Nuclear clustering in the energy density functional approach

    Energy Technology Data Exchange (ETDEWEB)

    Ebran, J.-P., E-mail: jean-paul.ebran@cea.fr [CEA,DAM,DIF, F-91297 Arpajon (France); Khan, E. [Institut de Physique Nucléaire, Université Paris-Sud CEA, IN2P3 CNRS, F-91406 Orsay Cedex (France); Nikšić, T.; Vretenar, D. [Physics Department, Faculty of Science, University of Zagreb, 10000 Zagreb (Croatia)

    2015-10-15

    Nuclear Energy Density Functionals (EDFs) are a microscopic tool of choice extensively used over the whole chart to successfully describe the properties of atomic nuclei ensuing from their quantum liquid nature. In the last decade, they also have proved their ability to deal with the cluster phenomenon, shedding a new light on its fundamental understanding by treating on an equal footing both quantum liquid and cluster aspects of nuclei. Such a unified microscopic description based on nucleonic degrees of freedom enables to tackle the question pertaining to the origin of the cluster phenomenon and emphasizes intrinsic mechanisms leading to the emergence of clusters in nuclei.

  16. Combining Density Functional Theory and Green's Function Theory: Range-Separated, Nonlocal, Dynamic, and Orbital-Dependent Hybrid Functional.

    Science.gov (United States)

    Kananenka, Alexei A; Zgid, Dominika

    2017-11-14

    We present a rigorous framework which combines single-particle Green's function theory with density functional theory based on a separation of electron-electron interactions into short- and long-range components. Short-range contribution to the total energy and exchange-correlation potential is provided by a density functional approximation, while the long-range contribution is calculated using an explicit many-body Green's function method. Such a hybrid results in a nonlocal, dynamic, and orbital-dependent exchange-correlation functional of a single-particle Green's function. In particular, we present a range-separated hybrid functional called srSVWN5-lrGF2 which combines the local-density approximation and the second-order Green's function theory. We illustrate that similarly to density functional approximations, the new functional is weakly basis-set dependent. Furthermore, it offers an improved description of the short-range dynamic correlation. The many-body contribution to the functional mitigates the many-electron self-interaction error present in many density functional approximations and provides a better description of molecular properties. Additionally, we illustrate that the new functional can be used to scale down the self-energy and, therefore, introduce an additional sparsity to the self-energy matrix that in the future can be exploited in calculations for large molecules or periodic systems.

  17. Effects of Heme Electronic Structure and Distal Polar Interaction on Functional and Vibrational Properties of Myoglobin.

    Science.gov (United States)

    Kanai, Yuki; Nishimura, Ryu; Nishiyama, Kotaro; Shibata, Tomokazu; Yanagisawa, Sachiko; Ogura, Takashi; Matsuo, Takashi; Hirota, Shun; Neya, Saburo; Suzuki, Akihiro; Yamamoto, Yasuhiko

    2016-02-15

    We analyzed the oxygen (O2) and carbon monoxide (CO) binding properties, autoxidation reaction rate, and FeO2 and FeCO vibrational frequencies of the H64Q mutant of sperm whale myoglobin (Mb) reconstituted with chemically modified heme cofactors possessing a variety of heme Fe electron densities (ρ(Fe)), and the results were compared with those for the previously studied native [Shibata, T. et al. J. Am. Chem. Soc. 2010, 132, 6091-6098], and H64L [Nishimura, R. et al. Inorg. Chem. 2014, 53, 1091-1099], and L29F [Nishimura, R. et al. Inorg. Chem. 2014, 53, 9156-9165] mutants in order to elucidate the effect of changes in the heme electronic structure and distal polar interaction contributing to stabilization of the Fe-bound ligand on the functional and vibrational properties of the protein. The study revealed that, as in the cases of the previously studied native protein [Shibata, T. et al. Inorg. Chem. 2012, 51, 11955-11960], the O2 affinity and autoxidation reaction rate of the H64Q mutant decreased with a decrease in ρ(Fe), as expected from the effect of a change in ρ(Fe) on the resonance between the Fe(2+)-O2 bond and Fe(3+)-O2(-)-like species in the O2 form, while the CO affinity of the protein is independent of a change in ρ(Fe). We also found that the well-known inverse correlation between the frequencies of Fe-bound CO (ν(CO)) and Fe-C (ν(FeC)) stretching [Li, X.-Y.; Spiro, T. G. J. Am. Chem. Soc. 1988, 110, 6024-6033] is affected differently by changes in ρ(Fe) and the distal polar interaction, indicating that the effects of the two electronic perturbations due to the chemical modification of a heme cofactor and the replacement of nearby amino acid residues on the resonance between the two alternative canonical forms of the FeCO fragment in the protein are slightly different from each other. These findings provide a new insight for deeper understanding of the functional regulation of the protein.

  18. Polarization functions for the modified m6-31G basis sets for atoms Ga through Kr.

    Science.gov (United States)

    Mitin, Alexander V

    2013-09-05

    The 2df polarization functions for the modified m6-31G basis sets of the third-row atoms Ga through Kr (Int J Quantum Chem, 2007, 107, 3028; Int J. Quantum Chem, 2009, 109, 1158) are proposed. The performances of the m6-31G, m6-31G(d,p), and m6-31G(2df,p) basis sets were examined in molecular calculations carried out by the density functional theory (DFT) method with B3LYP hybrid functional, Møller-Plesset perturbation theory of the second order (MP2), quadratic configuration interaction method with single and double substitutions and were compared with those for the known 6-31G basis sets as well as with the other similar 641 and 6-311G basis sets with and without polarization functions. Obtained results have shown that the performances of the m6-31G, m6-31G(d,p), and m6-31G(2df,p) basis sets are better in comparison with the performances of the known 6-31G, 6-31G(d,p) and 6-31G(2df,p) basis sets. These improvements are mainly reached due to better approximations of different electrons belonging to the different atomic shells in the modified basis sets. Applicability of the modified basis sets in thermochemical calculations is also discussed. © 2013 Wiley Periodicals, Inc.

  19. Spin polarization in high density quark matter under a strong external magnetic field

    DEFF Research Database (Denmark)

    Tsue, Yasuhiko; Da Providência, João; Providência, Constança

    2016-01-01

    In high density quark matter under a strong external magnetic field, possible phases are investigated by using the two-flavor Nambu-Jona-Lasinio (NJL) model with tensor-type four-point interaction between quarks, as well as the axial-vector-type four-point interaction. In the tensor-type interact......In high density quark matter under a strong external magnetic field, possible phases are investigated by using the two-flavor Nambu-Jona-Lasinio (NJL) model with tensor-type four-point interaction between quarks, as well as the axial-vector-type four-point interaction. In the tensor...... phase appears in the wide range of the quark chemical potential. In both the interactions, the quark mass in zero and small chemical potential regions increases which indicates that the chiral symmetry breaking is enhanced, namely the magnetic catalysis occurs....

  20. Injection-modulated polarity conversion by charge carrier density control via a self-assembled monolayer for all-solution-processed organic field-effect transistors

    Science.gov (United States)

    Roh, Jeongkyun; Lee, Taesoo; Kang, Chan-Mo; Kwak, Jeonghun; Lang, Philippe; Horowitz, Gilles; Kim, Hyeok; Lee, Changhee

    2017-04-01

    We demonstrated modulation of charge carrier densities in all-solution-processed organic field-effect transistors (OFETs) by modifying the injection properties with self-assembled monolayers (SAMs). The all-solution-processed OFETs based on an n-type polymer with inkjet-printed Ag electrodes were fabricated as a test platform, and the injection properties were modified by the SAMs. Two types of SAMs with different dipole direction, thiophenol (TP) and pentafluorobenzene thiol (PFBT) were employed, modifying the work function of the inkjet-printed Ag (4.9 eV) to 4.66 eV and 5.24 eV with TP and PFBT treatments, respectively. The charge carrier densities were controlled by the SAM treatment in both dominant and non-dominant carrier-channel regimes. This work demonstrates that control of the charge carrier densities can be efficiently achieved by modifying the injection property with SAM treatment; thus, this approach can achieve polarity conversion of the OFETs.

  1. Surface regulated arsenenes as Dirac materials: From density functional calculations

    Energy Technology Data Exchange (ETDEWEB)

    Yuan, Junhui; Xie, Qingxing; Yu, Niannian, E-mail: niannianyu@whut.edu.cn; Wang, Jiafu, E-mail: jasper@whut.edu.cn

    2017-02-01

    Highlights: • The presence of Dirac cones in chemically decorated buckled arsenene AsX (X = CN, NC, NCO, NCS, and NCSe) has been revealed. • First-principles calculations show that all these chemically decorated arsenenes are kinetically stable in defending thermal fluctuations in room temperature. - Abstract: Using first principle calculations based on density functional theory (DFT), we have systematically investigated the structure stability and electronic properties of chemically decorated arsenenes, AsX (X = CN, NC, NCO, NCS and NCSe). Phonon dispersion and formation energy analysis reveal that all the five chemically decorated buckled arsenenes are energetically favorable and could be synthesized. Our study shows that wide-bandgap arsenene would turn into Dirac materials when functionalized by -X (X = CN, NC, NCO, NCS and NCSe) groups, rendering new promises in next generation high-performance electronic devices.

  2. Building a universal nuclear energy density functional (UNEDF)

    Energy Technology Data Exchange (ETDEWEB)

    Nazarewicz, Witold [Univ. of Tennessee, Knoxville, TN (United States)

    2012-07-01

    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.

  3. Electronic properties of graphene nanoribbons: A density functional investigation

    International Nuclear Information System (INIS)

    Kumar, Sandeep; Sharma, Hitesh

    2015-01-01

    Density functional theory calculations have been performed on graphene nano ribbons (GNRs) to investigate the electronic properties as a function of chirality, size and hydrogenation on the edges. The calculations were performed on GNRs with armchair and zigzag configurations with 28, 34, 36, 40, 50, 56, 62, 66 carbon atoms. The structural stability of AGNR and ZGNR increases with the size of nanoribbon where as hydrogenation of GNR tends to lowers their structural stability. All GNRs considered have shown semiconducting behavior with HOMO-LUMO gap decreasing with the increase in the GNR size. The hydrogenation of GNR decreases its HOMO-LUMO gap significantly. The results are in agreement with the available experimental and theoretical results

  4. Beyond Kohn-Sham Approximation: Hybrid Multistate Wave Function and Density Functional Theory.

    Science.gov (United States)

    Gao, Jiali; Grofe, Adam; Ren, Haisheng; Bao, Peng

    2016-12-15

    A multistate density functional theory (MSDFT) is presented in which the energies and densities for the ground and excited states are treated on the same footing using multiconfigurational approaches. The method can be applied to systems with strong correlation and to correctly describe the dimensionality of the conical intersections between strongly coupled dissociative potential energy surfaces. A dynamic-then-static framework for treating electron correlation is developed to first incorporate dynamic correlation into contracted state functions through block-localized Kohn-Sham density functional theory (KSDFT), followed by diagonalization of the effective Hamiltonian to include static correlation. MSDFT can be regarded as a hybrid of wave function and density functional theory. The method is built on and makes use of the current approximate density functional developed in KSDFT, yet it retains its computational efficiency to treat strongly correlated systems that are problematic for KSDFT but too large for accurate WFT. The results presented in this work show that MSDFT can be applied to photochemical processes involving conical intersections.

  5. Time-dependent density-functional calculation of nuclear response functions

    OpenAIRE

    Nakatsukasa, Takashi

    2017-01-01

    Basic issues of the time-dependent density-functional theory are discussed, especially on the real-time calculation of the linear response functions. Some remarks on the derivation of the time-dependent Kohn-Sham equations and on the numerical methods are given.

  6. Elucidating Cellular Population Dynamics by Molecular Density Function Perturbations

    Directory of Open Access Journals (Sweden)

    Thanneer Malai Perumal

    2018-01-01

    Full Text Available Studies performed at single-cell resolution have demonstrated the physiological significance of cell-to-cell variability. Various types of mathematical models and systems analyses of biological networks have further been used to gain a better understanding of the sources and regulatory mechanisms of such variability. In this work, we present a novel sensitivity analysis method, called molecular density function perturbation (MDFP, for the dynamical analysis of cellular heterogeneity. The proposed analysis is based on introducing perturbations to the density or distribution function of the cellular state variables at specific time points, and quantifying how such perturbations affect the state distribution at later time points. We applied the MDFP analysis to a model of a signal transduction pathway involving TRAIL (tumor necrosis factor-related apoptosis-inducing ligand-induced apoptosis in HeLa cells. The MDFP analysis shows that caspase-8 activation regulates the timing of the switch-like increase of cPARP (cleaved poly(ADP-ribose polymerase, an indicator of apoptosis. Meanwhile, the cell-to-cell variability in the commitment to apoptosis depends on mitochondrial outer membrane permeabilization (MOMP and events following MOMP, including the release of Smac (second mitochondria-derived activator of caspases and cytochrome c from mitochondria, the inhibition of XIAP (X-linked inhibitor of apoptosis by Smac, and the formation of the apoptosome.

  7. Density functional study on the derivatives of purine.

    Science.gov (United States)

    Wei-Jie, Chi; Lu-Lin, Li; Bu-Tong, Li; Hai-Shun, Wu

    2012-08-01

    The derivatives of purine are designed through substituting the hydrogen atoms on it for nitro and amino functional groups. Geometries and frequency are analyzed at the B3LYP/6-31 G** level of density functional theory(DFT). Heats of formation (HOF), bond dissociation energy(BDE) and detonation parameters (detonation velocity and detonation pressure) are obtained in detail at the same level. It is found that the BDE values of all derivatives are over 120KJ·mol(-1), and have high positive heats of formation. These derivatives possess excellent detonation properties, for B1, B2, and C, the detonation velocity are 9.58, 9.57,and 9.90 km·s(-1), and the detonation pressure are 43.40,46.05, and 46.37 Gpa, respectively, the detonation performances are better than cyclotrimethylenetrinitramine (RDX)and cyclotetramethylenetetranitramine (HMX). Hence, the derivations of purine may be promising well-behaved high energy density materials.

  8. Nuclear charge radii: density functional theory meets Bayesian neural networks

    Science.gov (United States)

    Utama, R.; Chen, Wei-Chia; Piekarewicz, J.

    2016-11-01

    The distribution of electric charge in atomic nuclei is fundamental to our understanding of the complex nuclear dynamics and a quintessential observable to validate nuclear structure models. The aim of this study is to explore a novel approach that combines sophisticated models of nuclear structure with Bayesian neural networks (BNN) to generate predictions for the charge radii of thousands of nuclei throughout the nuclear chart. A class of relativistic energy density functionals is used to provide robust predictions for nuclear charge radii. In turn, these predictions are refined through Bayesian learning for a neural network that is trained using residuals between theoretical predictions and the experimental data. Although predictions obtained with density functional theory provide a fairly good description of experiment, our results show significant improvement (better than 40%) after BNN refinement. Moreover, these improved results for nuclear charge radii are supplemented with theoretical error bars. We have successfully demonstrated the ability of the BNN approach to significantly increase the accuracy of nuclear models in the predictions of nuclear charge radii. However, as many before us, we failed to uncover the underlying physics behind the intriguing behavior of charge radii along the calcium isotopic chain.

  9. JDFTx: Software for joint density-functional theory

    Directory of Open Access Journals (Sweden)

    Ravishankar Sundararaman

    2017-01-01

    Full Text Available Density-functional theory (DFT has revolutionized computational prediction of atomic-scale properties from first principles in physics, chemistry and materials science. Continuing development of new methods is necessary for accurate predictions of new classes of materials and properties, and for connecting to nano- and mesoscale properties using coarse-grained theories. JDFTx is a fully-featured open-source electronic DFT software designed specifically to facilitate rapid development of new theories, models and algorithms. Using an algebraic formulation as an abstraction layer, compact C++11 code automatically performs well on diverse hardware including GPUs (Graphics Processing Units. This code hosts the development of joint density-functional theory (JDFT that combines electronic DFT with classical DFT and continuum models of liquids for first-principles calculations of solvated and electrochemical systems. In addition, the modular nature of the code makes it easy to extend and interface with, facilitating the development of multi-scale toolkits that connect to ab initio calculations, e.g. photo-excited carrier dynamics combining electron and phonon calculations with electromagnetic simulations.

  10. Functional renormalization group and Kohn-Sham scheme in density functional theory

    Science.gov (United States)

    Liang, Haozhao; Niu, Yifei; Hatsuda, Tetsuo

    2018-04-01

    Deriving accurate energy density functional is one of the central problems in condensed matter physics, nuclear physics, and quantum chemistry. We propose a novel method to deduce the energy density functional by combining the idea of the functional renormalization group and the Kohn-Sham scheme in density functional theory. The key idea is to solve the renormalization group flow for the effective action decomposed into the mean-field part and the correlation part. Also, we propose a simple practical method to quantify the uncertainty associated with the truncation of the correlation part. By taking the φ4 theory in zero dimension as a benchmark, we demonstrate that our method shows extremely fast convergence to the exact result even for the highly strong coupling regime.

  11. Migrational polarization in high-current density molten salt electrochemical devices

    Energy Technology Data Exchange (ETDEWEB)

    Braunstein, J.; Vallet, C.E.

    1977-01-01

    Electrochemical flux equations based on the thermodynamics of irreversible processes have been derived in terms of experimental transport coefficients for binary molten salt mixtures analogous to those proposed for high temperature batteries and fuel cells. The equations and some numerical solutions indicate steady state composition gradients of significant magnitude. The effects of migrational separation must be considered along with other melt properties in the characterization of electrode behavior, melt composition, operating temperatures and differences of phase stability, wettability and other physicochemical properties at positive and negative electrodes of high current density devices with mixed electrolytes.

  12. Enhanced photocatalytic properties of titania-graphene nanocomposites: a density functional theory study.

    Science.gov (United States)

    Geng, Wei; Liu, Huanxiang; Yao, Xiaojun

    2013-04-28

    In this work, we systematically studied the mechanism for the enhanced photocatalytic activities of TiO2-graphene composites by using density functional theory (DFT) calculations. The studied composites include: TiO2-pristine graphene, TiO2-graphene with defect, as well as TiO2-graphene oxide. The results from geometry optimization can reveal information about the interface structure and anchoring orientation of the composites. The calculated electronic properties including total and difference charge density, as well as charge population, demonstrate the polarization and electron redistribution for the composites. Projected density of states and energy bands can provide some useful information about the photocatalytic mechanism involving the electrons excitation from the O-2p orbital on the valence band to the C-2p on the conduction band maximum for the composites. The results of our study can provide some useful information for understanding the detailed molecular mechanism of the better performance of composites compared to the individual components.

  13. Olive oil phenolic compounds and high-density lipoprotein function.

    Science.gov (United States)

    Hernáez, Alvaro; Farràs, Marta; Fitó, Montserrat

    2016-02-01

    The functional capacities of high-density lipoproteins (HDLs) reflect the physiological role of the particle better than the quantity of HDL cholesterol. Owing to its phenolic compounds, the consumption of virgin olive oil has emerged as a promising therapy to promote these capacities. This review highlights the human studies that explain these benefits and explores some possible mechanisms. The consumption of olive oil phenolic compounds increased the ability of HDLs to pick up cholesterol excess in peripheral cells (the cholesterol efflux capacity). Olive oil phenolic compounds have also been shown to improve HDL antioxidant capacities and some anti-inflammatory traits. These changes respond to an improvement of HDL oxidative status and composition. Novel strategies to increase HDL functional capacities are in demand from clinicians. The attainment of a fully-functional HDL through dietary or lifestyle changes is a priority in cardiovascular research. Within this context, the consumption of virgin olive oil, because of its phenolic compounds, may be a relevant protective approach. Further studies in large-scale, randomized controlled trials are, however, required to confirm these effects in HDL functionality.

  14. Ferroelectric critical size and vortex domain structures of PbTiO3 nanodots: A density functional theory study

    Science.gov (United States)

    Wang, Xiaoyuan; Yan, Yabin; Shimada, Takahiro; Wang, Jie; Kitamura, Takayuki

    2018-03-01

    The ferroelectric critical size and microscopic domain structure of PbTiO3 nanodots with unit cells of N × N × N (N = 1-3) have been investigated by ab initio (first-principles) density functional theory calculations. Nanodots with PbO and TiO surface terminations are investigated, and the ground state of TiO-terminated nanodots is found to be paraelectric regardless of the size. However, for PbO-terminated nanodots, the ferroelectric state is energetically favorable even in the smallest nanodot, indicating the absence of an intrinsic critical size for ferroelectricity in the nanodot structure. Moreover, the distributions of polarizations in nanodots with different sizes are analyzed. The vortex polarizations rotating around both the central [001] axis and diagonal [1 1 ¯ 1 ] directions of nanodots can stably exist. The vortex polarization arises from the opposite rotation between the cations and anions around the [001] and the [1 1 ¯ 1 ] directions of nanodots, respectively. On the other hand, the toroidal moments of vortex polarizations both around the [001] and [1 1 ¯ 1 ] directions increase with the increment of nanodot size, and these vortex polarizations are energetically favorable in small and large nanodots, respectively.

  15. Density functional theory of the electrical double layer: the RFD functional

    International Nuclear Information System (INIS)

    Gillespie, Dirk; Valisko, Monika; Boda, Dezso

    2005-01-01

    Density functional theory (DFT) of electrolytes is applied to the electrical double layer under a wide range of conditions. The ions are charged, hard spheres of different size and valence, and the wall creating the double layer is uncharged, weakly charged, and strongly charged. Under all conditions, the density and electrostatic potential profiles calculated using the recently proposed RFD electrostatic functional (Gillespie et al 2002 J. Phys.: Condens. Matter 14 12129; 2003 Phys. Rev. E 68 031503) compare well to Monte Carlo simulations. When the wall is strongly charged, the RFD functional results agree with the results of a simpler perturbative electrostatic DFT, but the two functionals' results qualitatively disagree when the wall is uncharged or weakly charged. The RFD functional reproduces these phenomena of weakly charged double layers. It also reproduces bulk thermodynamic quantities calculated from pair correlation functions

  16. Near-surface bulk densities of asteroids derived from dual-polarization radar observations

    Science.gov (United States)

    Virkki, A.; Taylor, P. A.; Zambrano-Marin, L. F.; Howell, E. S.; Nolan, M. C.; Lejoly, C.; Rivera-Valentin, E. G.; Aponte, B. A.

    2017-09-01

    We present a new method to constrain the near-surface bulk density and surface roughness of regolith on asteroid surfaces using planetary radar measurements. The number of radar observations has increased rapidly during the last five years, allowing us to compare and contrast the radar scattering properties of different small-body populations and compositional types. This provides us with new opportunities to investigate their near-surface physical properties such as the chemical composition, bulk density, porosity, or the structural roughness in the scale of centimeters to meters. Because the radar signal can penetrate into a planetary surface up to a few decimeters, radar can reveal information that is hidden from other ground-based methods, such as optical and infrared measurements. The near-surface structure of asteroids and comets in centimeter-to-meter scale is essential information for robotic and human space missions, impact threat mitigation, and understanding the history of these bodies as well as the formation of the whole Solar System.

  17. Anatomical Reconstruction and Functional Imaging Reveal an Ordered Array of Skylight Polarization Detectors in Drosophila.

    Science.gov (United States)

    Weir, Peter T; Henze, Miriam J; Bleul, Christiane; Baumann-Klausener, Franziska; Labhart, Thomas; Dickinson, Michael H

    2016-05-11

    Many insects exploit skylight polarization as a compass cue for orientation and navigation. In the fruit fly, Drosophila melanogaster, photoreceptors R7 and R8 in the dorsal rim area (DRA) of the compound eye are specialized to detect the electric vector (e-vector) of linearly polarized light. These photoreceptors are arranged in stacked pairs with identical fields of view and spectral sensitivities, but mutually orthogonal microvillar orientations. As in larger flies, we found that the microvillar orientation of the distal photoreceptor R7 changes in a fan-like fashion along the DRA. This anatomical arrangement suggests that the DRA constitutes a detector for skylight polarization, in which different e-vectors maximally excite different positions in the array. To test our hypothesis, we measured responses to polarized light of varying e-vector angles in the terminals of R7/8 cells using genetically encoded calcium indicators. Our data confirm a progression of preferred e-vector angles from anterior to posterior in the DRA, and a strict orthogonality between the e-vector preferences of paired R7/8 cells. We observed decreased activity in photoreceptors in response to flashes of light polarized orthogonally to their preferred e-vector angle, suggesting reciprocal inhibition between photoreceptors in the same medullar column, which may serve to increase polarization contrast. Together, our results indicate that the polarization-vision system relies on a spatial map of preferred e-vector angles at the earliest stage of sensory processing. The fly's visual system is an influential model system for studying neural computation, and much is known about its anatomy, physiology, and development. The circuits underlying motion processing have received the most attention, but researchers are increasingly investigating other functions, such as color perception and object recognition. In this work, we investigate the early neural processing of a somewhat exotic sense, called

  18. The probability density function (PDF) of Lagrangian Turbulence

    Science.gov (United States)

    Birnir, B.

    2012-12-01

    The statistical theory of Lagrangian turbulence is derived from the stochastic Navier-Stokes equation. Assuming that the noise in fully-developed turbulence is a generic noise determined by the general theorems in probability, the central limit theorem and the large deviation principle, we are able to formulate and solve the Kolmogorov-Hopf equation for the invariant measure of the stochastic Navier-Stokes equations. The intermittency corrections to the scaling exponents of the structure functions require a multiplicative (multipling the fluid velocity) noise in the stochastic Navier-Stokes equation. We let this multiplicative noise, in the equation, consists of a simple (Poisson) jump process and then show how the Feynmann-Kac formula produces the log-Poissonian processes, found by She and Leveque, Waymire and Dubrulle. These log-Poissonian processes give the intermittency corrections that agree with modern direct Navier-Stokes simulations (DNS) and experiments. The probability density function (PDF) plays a key role when direct Navier-Stokes simulations or experimental results are compared to theory. The statistical theory of turbulence is determined, including the scaling of the structure functions of turbulence, by the invariant measure of the Navier-Stokes equation and the PDFs for the various statistics (one-point, two-point, N-point) can be obtained by taking the trace of the corresponding invariant measures. Hopf derived in 1952 a functional equation for the characteristic function (Fourier transform) of the invariant measure. In distinction to the nonlinear Navier-Stokes equation, this is a linear functional differential equation. The PDFs obtained from the invariant measures for the velocity differences (two-point statistics) are shown to be the four parameter generalized hyperbolic distributions, found by Barndorff-Nilsen. These PDF have heavy tails and a convex peak at the origin. A suitable projection of the Kolmogorov-Hopf equations is the

  19. Existence of time-dependent density-functional theory for open electronic systems: time-dependent holographic electron density theorem.

    Science.gov (United States)

    Zheng, Xiao; Yam, ChiYung; Wang, Fan; Chen, GuanHua

    2011-08-28

    We present the time-dependent holographic electron density theorem (TD-HEDT), which lays the foundation of time-dependent density-functional theory (TDDFT) for open electronic systems. For any finite electronic system, the TD-HEDT formally establishes a one-to-one correspondence between the electron density inside any finite subsystem and the time-dependent external potential. As a result, any electronic property of an open system in principle can be determined uniquely by the electron density function inside the open region. Implications of the TD-HEDT on the practicality of TDDFT are also discussed.

  20. Accurate and systematically improvable density functional theory embedding for correlated wavefunctions

    International Nuclear Information System (INIS)

    Goodpaster, Jason D.; Barnes, Taylor A.; Miller, Thomas F.; Manby, Frederick R.

    2014-01-01

    We analyze the sources of error in quantum embedding calculations in which an active subsystem is treated using wavefunction methods, and the remainder using density functional theory. We show that the embedding potential felt by the electrons in the active subsystem makes only a small contribution to the error of the method, whereas the error in the nonadditive exchange-correlation energy dominates. We test an MP2 correction for this term and demonstrate that the corrected embedding scheme accurately reproduces wavefunction calculations for a series of chemical reactions. Our projector-based embedding method uses localized occupied orbitals to partition the system; as with other local correlation methods, abrupt changes in the character of the localized orbitals along a reaction coordinate can lead to discontinuities in the embedded energy, but we show that these discontinuities are small and can be systematically reduced by increasing the size of the active region. Convergence of reaction energies with respect to the size of the active subsystem is shown to be rapid for all cases where the density functional treatment is able to capture the polarization of the environment, even in conjugated systems, and even when the partition cuts across a double bond

  1. Density functional theory and phytochemical study of 8-hydroxyisodiospyrin

    Science.gov (United States)

    Ullah, Zakir; Ata-ur-Rahman; Fazl-i-Sattar; Rauf, Abdur; Yaseen, Muhammad; Hassan, Waseem; Tariq, Muhammad; Ayub, Khurshid; Tahir, Asif Ali; Ullah, Habib

    2015-09-01

    Comprehensive theoretical and experimental studies of a natural product, 8-hydroxyisodiospyrin (HDO) have been carried out. Based on the correlation of experimental and theoretical data, an appropriate computational model was developed for obtaining the electronic, spectroscopic, and thermodynamic parameters of HDO. First of all, the exact structure of HDO is confirmed from the nice correlation of theory and experiment, prior to determination of its electroactive nature. Hybrid density functional theory (DFT) is employed for all theoretical simulations. The experimental and predicted IR and UV-vis spectra [B3LYP/6-31+G(d,p) level of theory] have excellent correlation. Inter-molecular non-covalent interaction of HDO with different gases such as NH3, CO2, CO, H2O is investigated through geometrical counterpoise (gCP) i.e., B3LYP-gCP-D3/6-31G∗ method. Furthermore, the inter-molecular interaction is also supported by geometrical parameters, electronic properties, thermodynamic parameters and charge analysis. All these characterizations have corroborated each other and confirmed the electroactive nature (non-covalent interaction ability) of HDO for the studied gases. Electronic properties such as Ionization Potential (IP), Electron Affinities (EA), electrostatic potential (ESP), density of states (DOS), HOMO, LUMO, and band gap of HDO have been estimated for the first time theoretically.

  2. Hydrodynamic tensor density functional theory with correct susceptibility

    Science.gov (United States)

    Ovchinnikov, Igor V.; Bartell, Lizette A.; Neuhauser, Daniel

    2007-04-01

    In a previous work the authors developed a family of orbital-free tensor equations for the density functional theory [J. Chem. Phys. 124, 024105 (2006)]. The theory is a combination of the coupled hydrodynamic moment equation hierarchy with a cumulant truncation of the one-body electron density matrix. A basic ingredient in the theory is how to truncate the series of equation of motion for the moments. In the original work the authors assumed that the cumulants vanish above a certain order (N). Here the authors show how to modify this assumption to obtain the correct susceptibilities. This is done for N =3, a level above the previous study. At the desired truncation level a few relevant terms are added, which, with the right combination of coefficients, lead to excellent agreement with the Kohn-Sham Lindhard susceptibilities for an uninteracting system. The approach is also powerful away from linear response, as demonstrated in a nonperturbative study of a jellium with a repulsive core, where excellent matching with Kohn-Sham simulations is obtained, while the Thomas-Fermi and von Weiszacker methods show significant deviations. In addition, time-dependent linear response studies at the new N =3 level demonstrate the author's previous assertion that as the order of the theory is increased new additional transverse sound modes appear mimicking the random phase approximation transverse dispersion region.

  3. Interactive design of probability density functions for shape grammars

    KAUST Repository

    Dang, Minh

    2015-11-02

    A shape grammar defines a procedural shape space containing a variety of models of the same class, e.g. buildings, trees, furniture, airplanes, bikes, etc. We present a framework that enables a user to interactively design a probability density function (pdf) over such a shape space and to sample models according to the designed pdf. First, we propose a user interface that enables a user to quickly provide preference scores for selected shapes and suggest sampling strategies to decide which models to present to the user to evaluate. Second, we propose a novel kernel function to encode the similarity between two procedural models. Third, we propose a framework to interpolate user preference scores by combining multiple techniques: function factorization, Gaussian process regression, autorelevance detection, and l1 regularization. Fourth, we modify the original grammars to generate models with a pdf proportional to the user preference scores. Finally, we provide evaluations of our user interface and framework parameters and a comparison to other exploratory modeling techniques using modeling tasks in five example shape spaces: furniture, low-rise buildings, skyscrapers, airplanes, and vegetation.

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

    Energy Technology Data Exchange (ETDEWEB)

    Carlson, Joe [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Furnstahl, Dick [The Ohio State Univ., Columbus, OH (United States); Horoi, Mihai [Central Michigan Univ., Mount Pleasant, MI (United States); Lusk, Rusty [Argonne National Lab. (ANL), Argonne, IL (United States); Nazarewicz, Witek [Univ. of Tennessee, Knoxville, TN (United States); Ng, Esmond [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Thompson, Ian [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Vary, James [Iowa State Univ., Ames, IA (United States)

    2012-09-30

    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. 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.

  5. Statistics of polarization speckle: theory versus experiment

    DEFF Research Database (Denmark)

    Wang, Wei; Hanson, Steen Grüner; Takeda, Mitsuo

    2010-01-01

    In this paper, we reviewed our recent work on the statistical properties of polarization speckle, described by stochastic Stokes parameters fluctuating in space. Based on the Gaussian assumption for the random electric field components and polar-interferometer, we investigated theoretically...... and experimentally the statistics of Stokes parameters of polarization speckle, including probability density function of Stokes parameters with the spatial degree of polarization, autocorrelation of Stokes vector and statistics of spatial derivatives for Stokes parameters....

  6. The "JK-only" approximation in density matrix functional and wave function theory.

    Science.gov (United States)

    Kollmar, Christian

    2004-12-15

    Various energy functionals applying the "JK-only" approximation which leads to two-index two-electron integrals instead of four-index two-electron integrals in the electron-electron interaction term of the electronic energy are presented. Numerical results of multiconfiguration self-consistent field calculations for the best possible "JK-only" wave function are compared to those obtained from the pair excitation multiconfiguration self-consistent (PEMCSCF) method and two versions of density matrix functional theory. One of these is derived making explicit use of some necessary conditions for N representability of the second-order density matrix. It is shown that this method models the energy functional based on the best possible "JK-only" wave function with good accuracy. The calculations also indicate that only a minor fraction of the total correlation energy is incorporated by "JK-only" approaches for larger molecules. (c) 2004 American Institute of Physics

  7. Gutzwiller density functional theory for solid hydrogen calculations

    Science.gov (United States)

    Liu, Jun; Yao, Yongxin; Liu, Chen; Lu, Wencai; Wang, Cai-Zhuang; Ho, Kai-Ming

    2014-03-01

    We have recently proposed a Gutzwiller density functional theory (G-DFT) by innovatively replacing the noninteracting trial wavefunction in Kohn-Sham DFT with the Gutzwiller projected trial wavefunction to explicitly account for correlation effects, which renders a renormalized correlation matrix in the calculation as the key ingredient in our theory. Our approach does not require adjustable Coulomb interaction parameters, nor need of double counting terms present in LDA +U and LDA +DMFT. Our method has been demonstrated to work well in hydrogen and nitrogen molecule systems. In the presentation we will show its performance on the Hydrogen solid by specifically work out the total energy curves for different phases discussed in the literature, and compare them against the benchmark Quantum Monte Carlo (QMC) calculations.

  8. Electrocatalytic Activity and Selectivity - a Density Functional Theory Study

    DEFF Research Database (Denmark)

    Karamad, Mohammadreza

    The focus of the current PhD thesis is to design new electro-catalysts, by changing the morphology and composition of the catalysts, to tune the electro-catalytic performance. We use Density Functional Theory (DFT) calculations, to examine activity, selectivity and stability of the designed electro...... by the location of Cu atoms into different layers of Pt(111). While the presence of Cu into the surface layer strengthens the interaction between surface and adsorbates, the presence of Cu atoms into the subsurface layer has the opposite effect. These findings can be used to design new electro...... reduction of CO2 at the cathode side: 1) high overpotential that hinders this reaction from being an energy efficient process, and 2) low selectivity towards desired reaction products. We have taken two approaches to improve the selectivity and activity in the reduction of CO2. Firstly, we create...

  9. Study of spontaneous fission lifetimes using nuclear density functional theory

    Directory of Open Access Journals (Sweden)

    Sadhukhan Jhilam

    2013-12-01

    Full Text Available The spontaneous fission lifetimes have been studied microscopically by minimizing the collective action integral in a two-dimensional collective space of quadrupole moments (Q20, Q22 representing elongation and triaxiality. The microscopic collective potential and inertia tensor are obtained by solving the self-consistent Hartree-Fock-Bogoliubov (HFB equations with the Skyrme energy density functional and mixed pairing interaction. The mass tensor is computed within the perturbative Adiabatic Time-Dependent HFB (ATDHFB approach in the cranking approximation. The dynamic fission trajectories have been obtained by minimizing the collective action using two different numerical techniques. The values of spontaneous fission lifetimes obtained in this way are compared with the static results.

  10. Density Functional Studies of Methanol Decomposition on Subnanometer Pd Clusters

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-12-31

    A density functional theory study of the decomposition of methanol on subnanometer palladium clusters (primarily Pd4) is presented. Methanol dehydrogenation through C-H bond breaking to form hydroxymethyl (CH2OH) as the initial step, followed by steps involving formation of hydroxymethylene (CHOH), formyl (CHO), and carbon monoxide (CO), is found to be the most favorable reaction pathway. A competing dehydrogenation pathway with O-H bond breaking as the first step, followed by formation of methoxy (CH3O) and formaldehyde (CH2O), is slightly less favorable. In contrast, pathways involving C-O bond cleavage are much less energetically favorable, and no feasible pathways involving C-O bond formation to yield dimethyl ether (CH3OCH3) are found. Comparisons of the results are made with methanol decomposition products adsorbed on more extended Pd surfaces; all reaction intermediates are found to bind slightly more strongly to the clusters than to the surfaces.

  11. Descriptions of carbon isotopes within the energy density functional theory

    Energy Technology Data Exchange (ETDEWEB)

    Ismail, Atef [Fundamental and Applied Sciences Department, Universiti Teknologi PETRONAS, Bandar Seri Iskandar, 31750 Tronoh, Perak, Malaysia and Department of Physics, Al-Azhar University, 71524 Assiut (Egypt); Cheong, Lee Yen; Yahya, Noorhana [Fundamental and Applied Sciences Department, Universiti Teknologi PETRONAS, Bandar Seri Iskandar, 31750 Tronoh, Perak (Malaysia); Tammam, M. [Department of Physics, Al-Azhar University, 71524 Assiut (Egypt)

    2014-10-24

    Within the energy density functional (EDF) theory, the structure properties of Carbon isotopes are systematically studied. The shell model calculations are done for both even-A and odd-A nuclei, to study the structure of rich-neutron Carbon isotopes. The EDF theory indicates the single-neutron halo structures in {sup 15}C, {sup 17}C and {sup 19}C, and the two-neutron halo structures in {sup 16}C and {sup 22}C nuclei. It is also found that close to the neutron drip-line, there exist amazing increase in the neutron radii and decrease on the binding energies BE, which are tightly related with the blocking effect and correspondingly the blocking effect plays a significant role in the shell model configurations.

  12. Density functional theory studies of transition metal nanoparticles in catalysis

    DEFF Research Database (Denmark)

    Greeley, Jeffrey Philip; Rankin, Rees; Zeng, Zhenhua

    2013-01-01

    Periodic Density Functional Theory calculations are capable of providing powerful insights into the structural, energetics, and electronic phenomena that underlie heterogeneous catalysis on transition metal nanoparticles. Such calculations are now routinely applied to single crystal metal surfaces...... and to subnanometer metal clusters. Descriptions of catalysis on truly nanosized structures, however, are generally not as well developed. In this talk, I will illustrate different approaches to analyzing nanocatalytic phenomena with DFT calculations. I will describe case studies from heterogeneous catalysis...... and electrocatalysis, in which single crystal models are combined with Wulff construction-based ideas to produce descriptions of average nanocatalyst behavior. Then, I will proceed to describe explicitly DFT-based descriptions of catalysis on truly nanosized particles (

  13. Density functional theory study of Al-doped hematite

    International Nuclear Information System (INIS)

    Rivera, Richard; Stashans, Arvids; Piedra, Lorena; Pinto, Henry P

    2012-01-01

    Using first-principles density functional theory calculations within the generalized gradient approximation (GGA) as well as the GGA+U approach, we study Al-doped α-Fe 2 O 3 crystals. Structural, electronic, magnetic and optical properties due to impurity incorporation have been investigated and discussed in detail. Atomic displacements and Bader charges on atoms have been computed, showing that Al dopant converts the chemical bonding in its neighbourhood into a more ionic one. This work enhances our knowledge about how a crystalline lattice reacts in the presence of an Al impurity. It was found that Al incorporation produces some local changes in the band structure of the material without the creation of local energy levels within the band gap. The results provide evidence for changes in the magnetic moments in the vicinity of a defect, which means that α-Fe 2 O 3 doped with aluminum might not act as an antiferromagnetic substance.

  14. Nuclear level density and gamma strength function in 64Fe

    Science.gov (United States)

    Smith, M. K.; Spyrou, A.; Ahn, T.; Dombos, A. C.; Liddick, S. N.; Montes, F.; Naqvi, F.; Richman, D.; Schatz, H.; Brown, J.; Childers, K.; Crider, B. P.; Prokop, C. J.; Deleeuw, E.; Deyoung, P. A.; Langer, C.; Lewis, R.; Meisel, Z.; Pereira, J.; Quinn, S. J.; Schmidt, K.; Larsen, A. C.; Guttormsen, M.

    2017-09-01

    The Fe-Cd mass region exhibits enhanced collectivity and an unexpected increased in gamma-decay probability at low energies. These effects could be significant for r-process nucleosynthesis, where masses, beta-decay probabilities, and neutron capture cross sections are among the most important inputs. Neutron capture is notoriously difficult to measure; so the recent development of an indirect technique to constrain neutron-captures far from stability is especially valuable. This is the beta-Oslo method, which allows the extraction of the nuclear level density and gamma-ray strength function to compute neutron-capture cross sections. This work reports on 64Fe, populated via beta-decay of 64Mn at the National Superconducting Cyclotron Laboratory and measured with the 4pi Summing NaI (SuN) total gamma-ray spectrometer.

  15. Probability density functions for CP-violating rephasing invariants

    Science.gov (United States)

    Fortin, Jean-François; Giasson, Nicolas; Marleau, Luc

    2018-05-01

    The implications of the anarchy principle on CP violation in the lepton sector are investigated. A systematic method is introduced to compute the probability density functions for the CP-violating rephasing invariants of the PMNS matrix from the Haar measure relevant to the anarchy principle. Contrary to the CKM matrix which is hierarchical, it is shown that the Haar measure, and hence the anarchy principle, are very likely to lead to the observed PMNS matrix. Predictions on the CP-violating Dirac rephasing invariant |jD | and Majorana rephasing invariant |j1 | are also obtained. They correspond to 〈 |jD | 〉 Haar = π / 105 ≈ 0.030 and 〈 |j1 | 〉 Haar = 1 / (6 π) ≈ 0.053 respectively, in agreement with the experimental hint from T2K of |jDexp | ≈ 0.032 ± 0.005 (or ≈ 0.033 ± 0.003) for the normal (or inverted) hierarchy.

  16. Defects in AlSb: a density functional study

    International Nuclear Information System (INIS)

    Du, Mao-Hua

    2009-01-01

    We carry out density functional calculations to study both intrinsic and extrinsic defects in AlSb. We focus on the carrier compensation and trapping properties of these defects, which are important to the radiation detection applications. We show that the Sb antisite is a low-energy defect, baring much similarity to the As antisite in GaAs. The SbAl is effective in compensating holes induced by the residual carbon, but is also a deep electron trap that reduces the carrier drifting length. We discuss the possibility of using hydrogenated isovalent N impurity in AlSb and GaAs to pin the Fermi level without causing efficient carrier trapping.

  17. Periodic Density Functional Theory Solver using Multiresolution Analysis with MADNESS

    Science.gov (United States)

    Harrison, Robert; Thornton, William

    2011-03-01

    We describe the first implementation of the all-electron Kohn-Sham density functional periodic solver (DFT) using multi-wavelets and fast integral equations using MADNESS (multiresolution adaptive numerical environment for scientific simulation; http://code.google.com/p/m-a-d-n-e-s-s). The multiresolution nature of a multi-wavelet basis allows for fast computation with guaranteed precision. By reformulating the Kohn-Sham eigenvalue equation into the Lippmann-Schwinger equation, we can avoid using the derivative operator which allows better control of overall precision for the all-electron problem. Other highlights include the development of periodic integral operators with low-rank separation, an adaptable model potential for nuclear potential, and an implementation for Hartree Fock exchange. This work was supported by NSF project OCI-0904972 and made use of resources at the Center for Computational Sciences at Oak Ridge National Laboratory under contract DE-AC05-00OR22725.

  18. Density Functional Theory using Multiresolution Analysis with MADNESS

    Science.gov (United States)

    Thornton, Scott; Harrison, Robert

    2012-02-01

    We describe the first implementation of the all-electron Kohn-Sham density functional periodic solver (DFT) using multi-wavelets and fast integral equations using MADNESS (multiresolution adaptive numerical environment for scientific simulation; http://code.google.com/p/m-a-d-n-e-s-s). The multiresolution nature of a multi-wavelet basis allows for fast computation with guaranteed precision. By reformulating the Kohn-Sham eigenvalue equation into the Lippmann-Schwinger equation, we can avoid using the derivative operator which allows better control of overall precision for the all-electron problem. Other highlights include the development of periodic integral operators with low-rank separation, an adaptable model potential for the nuclear potential, and an implementation for Hartree-Fock exchange.

  19. Comment on "Density functional theory is straying from the path toward the exact functional"

    DEFF Research Database (Denmark)

    Kepp, Kasper Planeta

    2017-01-01

    Medvedev et al (Reports, 6 January 2017, p. 49) argue that recent density functionals stray from the path toward exactness. This conclusion rests on very compact 1s2 and 1s22s2 systems favored by the Hartree-Fock picture. Comparison to actual energies for the same systems indicates that the "stra......Medvedev et al (Reports, 6 January 2017, p. 49) argue that recent density functionals stray from the path toward exactness. This conclusion rests on very compact 1s2 and 1s22s2 systems favored by the Hartree-Fock picture. Comparison to actual energies for the same systems indicates...

  20. Comparison of the surface ion density of silica gel evaluated via spectral induced polarization versus acid-base titration

    Science.gov (United States)

    Hao, Na; Moysey, Stephen M. J.; Powell, Brian A.; Ntarlagiannis, Dimitrios

    2016-12-01

    Surface complexation models are widely used with batch adsorption experiments to characterize and predict surface geochemical processes in porous media. In contrast, the spectral induced polarization (SIP) method has recently been used to non-invasively monitor in situ subsurface chemical reactions in porous media, such as ion adsorption processes on mineral surfaces. Here we compare these tools for investigating surface site density changes during pH-dependent sodium adsorption on a silica gel. Continuous SIP measurements were conducted using a lab scale column packed with silica gel. A constant inflow of 0.05 M NaCl solution was introduced to the column while the influent pH was changed from 7.0 to 10.0 over the course of the experiment. The SIP measurements indicate that the pH change caused a 38.49 ± 0.30 μS cm- 1 increase in the imaginary conductivity of the silica gel. This increase is thought to result from deprotonation of silanol groups on the silica gel surface caused by the rise in pH, followed by sorption of Na+ cations. Fitting the SIP data using the mechanistic model of Leroy et al. (Leroyet al., 2008), which is based on the triple layer model of a mineral surface, we estimated an increase in the silica gel surface site density of 26.9 × 1016 sites m- 2. We independently used a potentiometric acid-base titration data for the silica gel to calibrate the triple layer model using the software FITEQL and observed a total increase in the surface site density for sodium sorption of 11.2 × 1016 sites m- 2, which is approximately 2.4 times smaller than the value estimated using the SIP model. By simulating the SIP response based on the calibrated surface complexation model, we found a moderate association between the measured and estimated imaginary conductivity (R2 = 0.65). These results suggest that the surface complexation model used here does not capture all mechanisms contributing to polarization of the silica gel captured by the SIP data.

  1. Evolution and development of hair cell polarity and efferent function in the inner ear.

    Science.gov (United States)

    Sienknecht, Ulrike J; Köppl, Christine; Fritzsch, Bernd

    2014-01-01

    The function of the inner ear critically depends on mechanoelectrically transducing hair cells and their afferent and efferent innervation. The first part of this review presents data on the evolution and development of polarized vertebrate hair cells that generate a sensitive axis for mechanical stimulation, an essential part of the function of hair cells. Beyond the cellular level, a coordinated alignment of polarized hair cells across a sensory epithelium, a phenomenon called planar cell polarity (PCP), is essential for the organ's function. The coordinated alignment of hair cells leads to hair cell orientation patterns that are characteristic of the different sensory epithelia of the vertebrate inner ear. Here, we review the developmental mechanisms that potentially generate molecular and morphological asymmetries necessary for the control of PCP. In the second part, this review concentrates on the evolution, development and function of the enigmatic efferent neurons terminating on hair cells. We present evidence suggestive of efferents being derived from motoneurons and synapsing predominantly onto a unique but ancient cholinergic receptor. A review of functional data shows that the plesiomorphic role of the efferent system likely was to globally shut down and protect the peripheral sensors, be they vestibular, lateral line or auditory hair cells, from desensitization and damage during situations of self-induced sensory overload. The addition of a dedicated auditory papilla in land vertebrates appears to have favored the separation of vestibular and auditory efferents and specializations for more sophisticated and more diverse functions. © 2014 S. Karger AG, Basel.

  2. Reduced density-matrix functional theory: Correlation and spectroscopy.

    Science.gov (United States)

    Di Sabatino, S; Berger, J A; Reining, L; Romaniello, P

    2015-07-14

    In this work, we explore the performance of approximations to electron correlation in reduced density-matrix functional theory (RDMFT) and of approximations to the observables calculated within this theory. Our analysis focuses on the calculation of total energies, occupation numbers, removal/addition energies, and spectral functions. We use the exactly solvable Hubbard dimer at 1/4 and 1/2 fillings as test systems. This allows us to analyze the underlying physics and to elucidate the origin of the observed trends. For comparison, we also report the results of the GW approximation, where the self-energy functional is approximated, but no further hypothesis is made concerning the approximations of the observables. In particular, we focus on the atomic limit, where the two sites of the dimer are pulled apart and electrons localize on either site with equal probability, unless a small perturbation is present: this is the regime of strong electron correlation. In this limit, using the Hubbard dimer at 1/2 filling with or without a spin-symmetry-broken ground state allows us to explore how degeneracies and spin-symmetry breaking are treated in RDMFT. We find that, within the used approximations, neither in RDMFT nor in GW, the signature of strong correlation is present, when looking at the removal/addition energies and spectral function from the spin-singlet ground state, whereas both give the exact result for the spin-symmetry broken case. Moreover, we show how the spectroscopic properties change from one spin structure to the other.

  3. Reduced density-matrix functional theory: Correlation and spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Di Sabatino, S.; Romaniello, P. [Laboratoire de Physique Théorique, CNRS, IRSAMC, Université Toulouse III–Paul Sabatier, 118 Route de Narbonne, 31062 Toulouse Cedex, France and ETSF (France); Berger, J. A. [Laboratoire de Chimie et Physique Quantiques, IRSAMC, Université Toulouse III–Paul Sabatier, CNRS, 118 Route de Narbonne, 31062 Toulouse Cedex, France and ETSF (France); Reining, L. [Laboratoire des Solides Irradiés, École Polytechnique, CNRS, CEA-DSM, 91128 Palaiseau, France and ETSF (France)

    2015-07-14

    In this work, we explore the performance of approximations to electron correlation in reduced density-matrix functional theory (RDMFT) and of approximations to the observables calculated within this theory. Our analysis focuses on the calculation of total energies, occupation numbers, removal/addition energies, and spectral functions. We use the exactly solvable Hubbard dimer at 1/4 and 1/2 fillings as test systems. This allows us to analyze the underlying physics and to elucidate the origin of the observed trends. For comparison, we also report the results of the GW approximation, where the self-energy functional is approximated, but no further hypothesis is made concerning the approximations of the observables. In particular, we focus on the atomic limit, where the two sites of the dimer are pulled apart and electrons localize on either site with equal probability, unless a small perturbation is present: this is the regime of strong electron correlation. In this limit, using the Hubbard dimer at 1/2 filling with or without a spin-symmetry-broken ground state allows us to explore how degeneracies and spin-symmetry breaking are treated in RDMFT. We find that, within the used approximations, neither in RDMFT nor in GW, the signature of strong correlation is present, when looking at the removal/addition energies and spectral function from the spin-singlet ground state, whereas both give the exact result for the spin-symmetry broken case. Moreover, we show how the spectroscopic properties change from one spin structure to the other.

  4. Multiconfiguration Pair-Density Functional Theory Spectral Calculations Are Stable to Adding Diffuse Basis Functions.

    Science.gov (United States)

    Hoyer, Chad E; Gagliardi, Laura; Truhlar, Donald G

    2015-11-05

    Time-dependent Kohn-Sham density functional theory (TD-KS-DFT) is useful for calculating electronic excitation spectra of large systems, but the low-energy spectra are often complicated by artificially lowered higher-energy states. This affects even the lowest energy excited states. Here, by calculating the lowest energy spin-conserving excited state for atoms from H to K and for formaldehyde, we show that this problem does not occur in multiconfiguration pair-density functional theory (MC-PDFT). We use the tPBE on-top density functional, which is a translation of the PBE exchange-correlation functional. We compare to a robust multireference method, namely, complete active space second-order perturbation theory (CASPT2), and to TD-KS-DFT with two popular exchange-correlation functionals, PBE and PBE0. We find for atoms that the mean unsigned error (MUE) of MC-PDFT with the tPBE functional improves from 0.42 to 0.40 eV with a double set of diffuse functions, whereas the MUEs for PBE and PBE0 drastically increase from 0.74 to 2.49 eV and from 0.45 to 1.47 eV, respectively.

  5. The QTP family of consistent functionals and potentials in Kohn-Sham density functional theory

    Science.gov (United States)

    Jin, Yifan; Bartlett, Rodney J.

    2016-07-01

    This manuscript presents the second, consistent density functional in the QTP (Quantum Theory Project) family, that is, the CAM-QTP(01). It is a new range-separated exchange-correlation functional in which the non-local exchange contribution is 100% at large separation. It follows the same basic principles of this family that the Kohn-Sham eigenvalues of the occupied orbitals approximately equal the vertical ionization energies, which is not fulfilled by most of the traditional density functional methods. This new CAM-QTP(01) functional significantly improves the accuracy of the vertical excitation energies especially for the Rydberg states in the test set. It also reproduces many other properties such as geometries, reaction barrier heights, and atomization energies.

  6. Antisites in III-V semiconductors: Density functional theory calculations

    Energy Technology Data Exchange (ETDEWEB)

    Chroneos, A., E-mail: alex.chroneos@open.ac.uk [Engineering and Innovation, The Open University, Milton Keynes MK7 6AA (United Kingdom); Tahini, H. A. [Department of Materials, Imperial College London, London SW7 2AZ (United Kingdom); PSE Division, KAUST, Thuwal 23955-6900 (Saudi Arabia); Schwingenschlögl, U., E-mail: udo.schwingenschlogl@kaust.edu.sa [PSE Division, KAUST, Thuwal 23955-6900 (Saudi Arabia); Grimes, R. W., E-mail: r.grimes@imperial.ac.uk [Department of Materials, Imperial College London, London SW7 2AZ (United Kingdom)

    2014-07-14

    Density functional based simulation, corrected for finite size effects, is used to investigate systematically the formation of antisite defects in III-V semiconductors (III = Al, Ga, and In and V = P, As, and Sb). Different charge states are modelled as a function of the Fermi level and under different growth conditions. The formation energies of group III antisites (III{sub V}{sup q}) decrease with increasing covalent radius of the group V atom though not group III radius, whereas group V antisites (V{sub III}{sup q}) show a consistent decrease in formation energies with increase in group III and group V covalent radii. In general, III{sub V}{sup q} defects dominate under III-rich conditions and V{sub III}{sup q} under V-rich conditions. Comparison with equivalent vacancy formation energy simulations shows that while antisite concentrations are always dominant under stoichiometric conditions, modest variation in growth or doping conditions can lead to a significantly higher concentration of vacancies.

  7. Self-interaction corrections in density functional theory

    International Nuclear Information System (INIS)

    Tsuneda, Takao; Hirao, Kimihiko

    2014-01-01

    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

  8. Hardness of FeB4: Density functional theory investigation

    Science.gov (United States)

    Zhang, Miao; Lu, Mingchun; Du, Yonghui; Gao, Lili; Lu, Cheng; Liu, Hanyu

    2014-05-01

    A recent experimental study reported the successful synthesis of an orthorhombic FeB4 with a high hardness of 62(5) GPa [H. Gou et al., Phys. Rev. Lett. 111, 157002 (2013)], which has reignited extensive interests on whether transition-metal borides compounds will become superhard materials. However, it is contradicted with some theoretical studies suggesting transition-metal boron compounds are unlikely to become superhard materials. Here, we examined structural and electronic properties of FeB4 using density functional theory. The electronic calculations show the good metallicity and covalent Fe-B bonding. Meanwhile, we extensively investigated stress-strain relations of FeB4 under various tensile and shear loading directions. The calculated weakest tensile and shear stresses are 40 GPa and 25 GPa, respectively. Further simulations (e.g., electron localization function and bond length along the weakest loading direction) on FeB4 show the weak Fe-B bonding is responsible for this low hardness. Moreover, these results are consistent with the value of Vickers hardness (11.7-32.3 GPa) by employing different empirical hardness models and below the superhardness threshold of 40 GPa. Our current results suggest FeB4 is a hard material and unlikely to become superhard (>40 GPa).

  9. Acrolein impairs the cholesterol transport functions of high density lipoproteins.

    Science.gov (United States)

    Chadwick, Alexandra C; Holme, Rebecca L; Chen, Yiliang; Thomas, Michael J; Sorci-Thomas, Mary G; Silverstein, Roy L; Pritchard, Kirkwood A; Sahoo, Daisy

    2015-01-01

    High density lipoproteins (HDL) are considered athero-protective, primarily due to their role in reverse cholesterol transport, where they transport cholesterol from peripheral tissues to the liver for excretion. The current study was designed to determine the impact of HDL modification by acrolein, a highly reactive aldehyde found in high abundance in cigarette smoke, on the cholesterol transport functions of HDL. HDL was chemically-modified with acrolein and immunoblot and mass spectrometry analyses confirmed apolipoprotein crosslinking, as well as acrolein adducts on apolipoproteins A-I and A-II. The ability of acrolein-modified HDL (acro-HDL) to serve as an acceptor of free cholesterol (FC) from COS-7 cells transiently expressing SR-BI was significantly decreased. Further, in contrast to native HDL, acro-HDL promotes higher neutral lipid accumulation in murine macrophages as judged by Oil Red O staining. The ability of acro-HDL to mediate efficient selective uptake of HDL-cholesteryl esters (CE) into SR-BI-expressing cells was reduced compared to native HDL. Together, the findings from our studies suggest that acrolein modification of HDL produces a dysfunctional particle that may ultimately promote atherogenesis by impairing functions that are critical in the reverse cholesterol transport pathway.

  10. Polymer density functional approach to efficient evaluation of path integrals

    DEFF Research Database (Denmark)

    Brukhno, Andrey; Vorontsov-Velyaminov, Pavel N.; Bohr, Henrik

    2005-01-01

    A polymer density functional theory (P-DFT) has been extended to the case of quantum statistics within the framework of Feynman path integrals. We start with the exact P-DFT formalism for an ideal open chain and adapt its efficient numerical solution to the case of a ring. We show that, similarly......, the path integral problem can, in principle, be solved exactly by making use of the two-particle pair correlation function (2p-PCF) for the ends of an open polymer, half of the original. This way the exact data for one-dimensional quantum harmonic oscillator are reproduced in a wide range of temperatures....... The exact solution is not, though, reachable in three dimensions (3D) because of a vast amount of storage required for 2p-PCF. In order to treat closed paths in 3D, we introduce a so-called "open ring" approximation which proves to be rather accurate in the limit of long chains. We also employ a simple self...

  11. Antisites in III-V semiconductors: Density functional theory calculations

    KAUST Repository

    Chroneos, A.

    2014-07-14

    Density functional based simulation, corrected for finite size effects, is used to investigate systematically the formation of antisite defects in III-V semiconductors (III=Al, Ga, and In and V=P, As, and Sb). Different charge states are modelled as a function of the Fermi level and under different growth conditions. The formation energies of group III antisites (III V q) decrease with increasing covalent radius of the group V atom though not group III radius, whereas group V antisites (V I I I q) show a consistent decrease in formation energies with increase in group III and group V covalent radii. In general, III V q defects dominate under III-rich conditions and V I I I q under V-rich conditions. Comparison with equivalent vacancy formation energy simulations shows that while antisite concentrations are always dominant under stoichiometric conditions, modest variation in growth or doping conditions can lead to a significantly higher concentration of vacancies. © 2014 AIP Publishing LLC.

  12. Some late-term thoughts of a density-functional theorist

    Indian Academy of Sciences (India)

    Unknown

    Fourteen problems are stated within the density-functional theory of molecular electronic structure. Their alleviation will bring the subject closer to maturity. Keywords. Density-functional theory; molecular electronic structure; quantum chemistry; molecular behavior. 1. Preface. Density-functional theory (DFT) of the electronic.

  13. Transport through correlated systems with density functional theory.

    Science.gov (United States)

    Kurth, S; Stefanucci, G

    2017-10-18

    We present recent advances in density functional theory (DFT) for applications in the field of quantum transport, with particular emphasis on transport through strongly correlated systems. We review the foundations of the popular Landauer-Büttiker(LB)  +  DFT approach. This formalism, when using approximations to the exchange-correlation (xc) potential with steps at integer occupation, correctly captures the Kondo plateau in the zero bias conductance at zero temperature but completely fails to capture the transition to the Coulomb blockade (CB) regime as the temperature increases. To overcome the limitations of LB  +  DFT, the quantum transport problem is treated from a time-dependent (TD) perspective using TDDFT, an exact framework to deal with nonequilibrium situations. The steady-state limit of TDDFT shows that in addition to an xc potential in the junction, there also exists an xc correction to the applied bias. Open shell molecules in the CB regime provide the most striking examples of the importance of the xc bias correction. Using the Anderson model as guidance we estimate these corrections in the limit of zero bias. For the general case we put forward a steady-state DFT which is based on one-to-one correspondence between the pair of basic variables, steady density on and steady current across the junction and the pair local potential on and bias across the junction. Like TDDFT, this framework also leads to both an xc potential in the junction and an xc correction to the bias. Unlike TDDFT, these potentials are independent of history. We highlight the universal features of both xc potential and xc bias corrections for junctions in the CB regime and provide an accurate parametrization for the Anderson model at arbitrary temperatures and interaction strengths, thus providing a unified DFT description for both Kondo and CB regimes and the transition between them.

  14. Nanodrop on a nanorough solid surface: Density functional theory considerations

    Science.gov (United States)

    Berim, Gersh O.; Ruckenstein, Eli

    2008-07-01

    The density distributions and contact angles of liquid nanodrops on nanorough solid surfaces are determined on the basis of a nonlocal density functional theory. Two kinds of roughness, chemical and physical, are examined. The former considers the substrate as a sequence of two kinds of semi-infinite vertical plates of equal thicknesses but of different natures with different strengths for the liquid-solid interactions. The physical roughness involves an ordered set of pillars on a flat homogeneous surface. Both hydrophobic and hydrophilic surfaces were considered. For the chemical roughness, the contact angle which the drop makes with the flat surface increases when the strength of the liquid-solid interaction for one kind of plates decreases with respect to the fixed value of the other kind of plates. Such a behavior is in agreement with the Cassie-Baxter expression derived from macroscopic considerations. For the physical roughness on a hydrophobic surface, the contact angle which a drop makes with the plane containing the tops of the pillars increases with increasing roughness. Such a behavior is consistent with the Wenzel formula developed for macroscopic drops. For hydrophilic surfaces, as the roughness increases the contact angle first increases, in contradiction with the Wenzel formula, which predicts for hydrophilic surfaces a decrease of the contact angle with increasing roughness. However, a further increase in roughness changes nonmonotonously the contact angle, and at some roughness, the drop disappears and only a liquid film is present on the surface. It was also found that the contact angle has a periodic dependence on the volume of the drop.

  15. Transport through correlated systems with density functional theory

    Science.gov (United States)

    Kurth, S.; Stefanucci, G.

    2017-10-01

    We present recent advances in density functional theory (DFT) for applications in the field of quantum transport, with particular emphasis on transport through strongly correlated systems. We review the foundations of the popular Landauer–Büttiker(LB)  +  DFT approach. This formalism, when using approximations to the exchange-correlation (xc) potential with steps at integer occupation, correctly captures the Kondo plateau in the zero bias conductance at zero temperature but completely fails to capture the transition to the Coulomb blockade (CB) regime as the temperature increases. To overcome the limitations of LB  +  DFT, the quantum transport problem is treated from a time-dependent (TD) perspective using TDDFT, an exact framework to deal with nonequilibrium situations. The steady-state limit of TDDFT shows that in addition to an xc potential in the junction, there also exists an xc correction to the applied bias. Open shell molecules in the CB regime provide the most striking examples of the importance of the xc bias correction. Using the Anderson model as guidance we estimate these corrections in the limit of zero bias. For the general case we put forward a steady-state DFT which is based on one-to-one correspondence between the pair of basic variables, steady density on and steady current across the junction and the pair local potential on and bias across the junction. Like TDDFT, this framework also leads to both an xc potential in the junction and an xc correction to the bias. Unlike TDDFT, these potentials are independent of history. We highlight the universal features of both xc potential and xc bias corrections for junctions in the CB regime and provide an accurate parametrization for the Anderson model at arbitrary temperatures and interaction strengths, thus providing a unified DFT description for both Kondo and CB regimes and the transition between them.

  16. Acetylene chain reaction on hydrogenated boron nitride monolayers: a density functional theory study.

    Science.gov (United States)

    Ponce-Pérez, R; Cocoletzi, Gregorio H; Takeuchi, Noboru

    2017-11-28

    Spin-polarized first-principles total-energy calculations have been performed to investigate the possible chain reaction of acetylene molecules mediated by hydrogen abstraction on hydrogenated hexagonal boron nitride monolayers. Calculations have been done within the periodic density functional theory (DFT), employing the PBE exchange correlation potential, with van der Waals corrections (vdW-DF). Reactions at two different sites have been considered: hydrogen vacancies on top of boron and on top of nitrogen atoms. As previously calculated, at the intermediate state of the reaction, when the acetylene molecule is attached to the surface, the adsorption energy is of the order of -0.82 eV and -0.20 eV (measured with respect to the energy of the non interacting molecule-substrate system) for adsorption on top of boron and nitrogen atoms, respectively. After the hydrogen abstraction takes place, the system gains additional energy, resulting in adsorption energies of -1.52 eV and -1.30 eV, respectively. These results suggest that the chain reaction is energetically favorable. The calculated minimum energy path (MEP) for hydrogen abstraction shows very small energy barriers of the order of 5 meV and 22 meV for the reaction on top of boron and nitrogen atoms, respectively. Finally, the density of states (DOS) evolution study helps to understand the chain reaction mechanism. Graphical abstract Acetylene chain reaction on hydrogenated boron nitride monolayers.

  17. Green's function based unparameterised multi-dimensional kernel density and likelihood ratio estimator

    International Nuclear Information System (INIS)

    Kövesárki, P; Brock, I C; Quiroz, A E Nuncio

    2012-01-01

    This paper introduces a probability density estimator based on Green's function identities. A density model is constructed under the sole assumption that the probability density is differentiable. The method is implemented as a binary likelihood estimator for classification purposes, so issues such as mis-modeling and overtraining are also discussed. The identity behind the density estimator can be interpreted as a real-valued, non-scalar kernel method which is able to reconstruct differentiable density functions.

  18. Persistent organic pollutants and penile bone mineral density in East Greenland and Canadian polar bears (Ursus maritimus) during 1996-2015

    DEFF Research Database (Denmark)

    Daugaard-Petersen, Tobias; Langebæk, Rikke; Rigét, Frank F

    2018-01-01

    Persistent organic pollutants (POPs) are long-range transported to the Arctic via atmospheric and oceanic currents, where they biomagnify to high concentrations in the tissues of apex predators such as polar bears (Ursus maritimus). A major concern of POP exposure is their physiological effects...... on vital organ-tissues posing a threat to the health and survival of polar bears. Here we examined the relationship between selected POPs and baculum bone mineral density (BMD) in the East Greenland and seven Canadian subpopulations of polar bears. BMD was examined in 471 bacula collected between years...... 1996-2015 while POP concentrations in adipose tissue were determined in 67-192 of these individuals collected from 1999 to -2015. A geographical comparison showed that baculum BMD was significantly lowest in polar bears from East Greenland (EG) when compared to Gulf of Boothia (GB), Southern Hudson (SH...

  19. A transmembrane polar interaction is involved in the functional regulation of integrin alpha L beta 2.

    Science.gov (United States)

    Vararattanavech, Ardcharaporn; Chng, Choon-Peng; Parthasarathy, Krupakar; Tang, Xiao-Yan; Torres, Jaume; Tan, Suet-Mien

    2010-05-14

    Integrins are heterodimeric transmembrane (TM) receptors formed by noncovalent associations of alpha and beta subunits. Each subunit contains a single alpha-helical TM domain. Inside-out activation of an integrin involves the separation of its cytoplasmic tails, leading to disruption of alphabeta TM packing. The leukocyte integrin alpha L beta 2 is required for leukocyte adhesion, migration, proliferation, cytotoxic function, and antigen presentation. In this study, we show by mutagenesis experiments that the packing of alpha L beta 2 TMs is consistent with that of the integrin alpha IIb beta 3 TMs. However, molecular dynamics simulations of alpha L beta 2 TMs in lipids predicted a polar interaction involving the side chains of alpha L Ser1071 and beta2 Thr686 in the outer-membrane association clasp (OMC). This is supported by carbonyl vibrational shifts observed in isotope-labeled alpha L beta 2 TM peptides that were incorporated into lipid bilayers. Molecular dynamics studies simulating the separation of alpha L beta 2 tails showed the presence of polar interaction during the initial perturbation of the inner-membrane association clasp. When the TMs underwent further separation, the polar interaction was disrupted. OMC polar interaction is important in regulating the functions of beta2 integrins because mutations that disrupt the OMC polar interaction generated constitutively activated alpha L beta 2, alpha M beta 2, and alpha X beta 2 in 293T transfectants. We also show that the expression of mutant beta2 Thr686Gly in beta2-deficient T cells rescued cell adhesion to intercellular adhesion molecule 1, but the cells showed overt elongated morphologies in response to chemokine stromal-cell-derived factor 1 alpha treatment as compared to wild-type beta2-expressing cells. These two TM polar residues are totally conserved in other members of the beta2 integrins in humans and across different species. Our results provide an example of the stabilizing effect of polar

  20. A Precision Measurement of the Neutron Spin Structure Functions Using a Polarized HE-3 Target

    Energy Technology Data Exchange (ETDEWEB)

    Smith, T

    2003-11-05

    This thesis describes a precision measurement of the neutron spin dependent structure function, g{sub 1}{sup n}(x). The measurement was made by the E154 collaboration at SLAC using a longitudinally polarized, 48.3 GeV electron beam, and a {sup 3}He target polarized by spin exchange with optically pumped rubidium. A target polarization as high as 50% was achieved. The elements of the experiment which pertain to the polarized {sup 3}He target will be described in detail in this thesis. To achieve a precision measurement, it has been necessary to minimize the systematic error from the uncertainty in the target parameters. All of the parameters of the target have been carefully measured, and the most important parameters of the target have been measured using multiple techniques. The polarization of the target was measured using nuclear magnetic resonance techniques, and has been calibrated using both proton NMR and by measuring the shift of the Rb Zeeman resonance frequency due to the {sup 3}He polarization. The fraction of events which originated in the {sup 3}He, as measured by the spectrometers, has been determined using a physical model of the target and the spectrometers. It was also measured during the experiment using a variable pressure {sup 3}He reference cell in place of the polarized {sup 3}He target. The spin dependent structure function g{sub 1}{sup n}(z) was measured in the Bjorken x range of 0.014 < x < 0.7 with an average Q{sup 2} of 5 (GeV/c){sup 2}. One of the primary motivations for this experiment was to test the Bjorken sum rule. Because the experiment had smaller statistical errors and a broader kinematic coverage than previous experiments, the behavior of the spin structure function g{sub 1}{sup n}(x) could be studied in detail at low values of the Bjorken scaling variable x. It was found that g{sub 1}{sup n}(x) has a strongly divergent behavior at low values of x, calling into question the methods commonly used to extrapolate the value of g

  1. Reliable energy level alignment at physisorbed molecule-metal interfaces from density functional theory.

    Science.gov (United States)

    Egger, David A; Liu, Zhen-Fei; Neaton, Jeffrey B; Kronik, Leeor

    2015-04-08

    A key quantity for molecule-metal interfaces is the energy level alignment of molecular electronic states with the metallic Fermi level. We develop and apply an efficient theoretical method, based on density functional theory (DFT) that can yield quantitatively accurate energy level alignment information for physisorbed metal-molecule interfaces. The method builds on the "DFT+Σ" approach, grounded in many-body perturbation theory, which introduces an approximate electron self-energy that corrects the level alignment obtained from conventional DFT for missing exchange and correlation effects associated with the gas-phase molecule and substrate polarization. Here, we extend the DFT+Σ approach in two important ways: first, we employ optimally tuned range-separated hybrid functionals to compute the gas-phase term, rather than rely on GW or total energy differences as in prior work; second, we use a nonclassical DFT-determined image-charge plane of the metallic surface to compute the substrate polarization term, rather than the classical DFT-derived image plane used previously. We validate this new approach by a detailed comparison with experimental and theoretical reference data for several prototypical molecule-metal interfaces, where excellent agreement with experiment is achieved: benzene on graphite (0001), and 1,4-benzenediamine, Cu-phthalocyanine, and 3,4,9,10-perylene-tetracarboxylic-dianhydride on Au(111). In particular, we show that the method correctly captures level alignment trends across chemical systems and that it retains its accuracy even for molecules for which conventional DFT suffers from severe self-interaction errors.

  2. Non-empirical energy density functional for the nuclear structure

    International Nuclear Information System (INIS)

    Rot ival, V.

    2008-09-01

    The energy density functional (EDF) formalism is the tool of choice for large-scale low-energy nuclear structure calculations both for stable experimentally known nuclei whose properties are accurately reproduced and systems that are only theoretically predicted. We highlight in the present dissertation the capability of EDF methods to tackle exotic phenomena appearing at the very limits of stability, that is the formation of nuclear halos. We devise a new quantitative and model-independent method that characterizes the existence and properties of halos in medium- to heavy-mass nuclei, and quantifies the impact of pairing correlations and the choice of the energy functional on the formation of such systems. These results are found to be limited by the predictive power of currently-used EDFs that rely on fitting to known experimental data. In the second part of this dissertation, we initiate the construction of non-empirical EDFs that make use of the new paradigm for vacuum nucleon-nucleon interactions set by so-called low-momentum interactions generated through the application of renormalization group techniques. These soft-core vacuum potentials are used as a step-stone of a long-term strategy which connects modern many-body techniques and EDF methods. We provide guidelines for designing several non-empirical models that include in-medium many-body effects at various levels of approximation, and can be handled in state-of-the art nuclear structure codes. In the present work, the first step is initiated through the adjustment of an operator representation of low-momentum vacuum interactions using a custom-designed parallel evolutionary algorithm. The first results highlight the possibility to grasp most of the relevant physics for low-energy nuclear structure using this numerically convenient Gaussian vertex. (author)

  3. Accurate prediction of defect properties in density functional supercell calculations

    International Nuclear Information System (INIS)

    Lany, Stephan; Zunger, Alex

    2009-01-01

    The theoretical description of defects and impurities in semiconductors is largely based on density functional theory (DFT) employing supercell models. The literature discussion of uncertainties that limit the predictivity of this approach has focused mostly on two issues: (1) finite-size effects, in particular for charged defects; (2) the band-gap problem in local or semi-local DFT approximations. We here describe how finite-size effects (1) in the formation energy of charged defects can be accurately corrected in a simple way, i.e. by potential alignment in conjunction with a scaling of the Madelung-like screened first order correction term. The factor involved with this scaling depends only on the dielectric constant and the shape of the supercell, and quite accurately accounts for the full third order correction according to Makov and Payne. We further discuss in some detail the background and justification for this correction method, and also address the effect of the ionic screening on the magnitude of the image charge energy. In regard to (2) the band-gap problem, we discuss the merits of non-local external potentials that are added to the DFT Hamiltonian and allow for an empirical band-gap correction without significantly increasing the computational demand over that of standard DFT calculations. In combination with LDA + U, these potentials are further instrumental for the prediction of polaronic defects with localized holes in anion-p orbitals, such as the metal-site acceptors in wide-gap oxide semiconductors

  4. Study of iridium silicide monolayers using density functional theory

    Science.gov (United States)

    Popis, Minh D.; Popis, Sylvester V.; Oncel, Nuri; Hoffmann, Mark R.; ćakır, Deniz

    2018-02-01

    In this study, we investigated physical and electronic properties of possible two-dimensional structures formed by Si (silicon) and Ir (iridium). To this end, different plausible structures were modeled by using density functional theory and the cohesive energies calculated for the geometry of optimized structures, with the lowest equilibrium lattice constants. Among several candidate structures, we identified three mechanically (via elastic constants and Young's modulus), dynamically (via phonon calculations), and thermodynamically stable iridium silicide monolayer structures. The lowest energy structure has a chemical formula of Ir2Si4 (called r-IrSi2), with a rectangular lattice (Pmmn space group). Its cohesive energy was calculated to be -0.248 eV (per IrSi2 unit) with respect to bulk Ir and bulk Si. The band structure indicates that the Ir2Si4 monolayer exhibits metallic properties. Other stable structures have hexagonal (P-3m1) and tetragonal (P4/nmm) cell structures with 0.12 and 0.20 eV/f.u. higher cohesive energies, respectively. Our calculations showed that Ir-Si monolayers are reactive. Although O2 molecules exothermically dissociate on the surface of the free-standing iridium silicide monolayers with large binding energies, H2O molecules bind to the monolayers with a rather weak interaction.

  5. Density Functional Studies of Molecular Polarizabilities. 10. Fulvenes and Fulvalenes

    Directory of Open Access Journals (Sweden)

    Humberto J. Soscún Machado

    2000-09-01

    Full Text Available We report accurate Ab Initio Hartree Fock (HF and Density Functional Theory (DFT studies of the static dipole polarizabilities and first hyperpolarizabilities of the [n] fulvene and the [n,m] fulvalene series of molecules (with n, m = 3,5,7. Calculations are also reported for the parent cycloalkenes: cyclopropene, cyclopentadiene and cycloheptatriene (1-3 respectively. Geometries were optimized at the HF/6-311G(3d,2p level of theory. All the fulvenes (4-6 and the smaller fulvalenes (7, 9 and 10 are found to be planar. Pentaheptafulvalene (11 is slightly non-planar whilst heptafulvalene (12 has a folded C2h structure. Calculated C-C bond lengths are consistently smaller than the experimental values. Dipole polarizabilities and non-zero hyperpolarizabilities were calculated at the HF/6-311++G(3d,2p and BLYP/6-311++G(3d,2p levels of theory, using HF/6-311G(3d,2p geometries. Dipole polarizabilities correlate well with those given on the basis of atom additivity. Molecules (8, (9 and (11 show very large dipole hyperpolarizabilities.

  6. Embedding germanium in graphene: A density functional theory study

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Zhuo; Li, Yangping, E-mail: liyp@nwpu.edu.cn; Tan, Tingting; Liu, Zhengtang

    2017-03-31

    Highlights: • Substitutional Ge in graphene is more stable in double vacancy site than in single vacancy site. • Metallic and semiconductor behaviors are obtained for Ge-substituted graphene depending on different substitution sites, concentrations, and vacancy types. • Tunable electronic and magnetic behaviors are observed in graphene sheet with Ge-chain impurity. - Abstract: Based on the density functional theory, we investigate the structural, electronic, and magnetic properties of graphene sheet with substitutional Ge atoms in both single and double vacancies, and graphene sheet with Ge-chain impurity. We find the substitutional Ge is chemically bonded to graphene, and is more stable in the double vacancy site. The electronic properties indicate that metallic and semiconductor states with a range of band gaps from 0 to 0.87 eV could be obtained depending on different substitution sites, concentrations, and vacancy types. Magnetic moment is observed in graphene with single vacancy. Tunable electronic behaviors are also observed in graphene sheet with Ge-chain impurity, and a magnetic moment of 2.9 μB is observed in single Ge-chain incorporated 4 × 4 graphene supercell. From these investigations, we conclude that by doping of Ge in vacancy-contained graphene, it could provide great advantages for its application in future nanoscale devices.

  7. Density functional theory study of finite carbon chains.

    Science.gov (United States)

    Fan, XiaoFeng; Liu, Lei; Lin, JianYi; Shen, ZeXiang; Kuo, Jer-Lai

    2009-11-24

    The structural, electronic, and vibrational properties of the free finite carbon chains and those encapsulated inside carbon nanotubes (CNTs) are studied by density functional theory calculations. The end effect and chain symmetry are found to play key roles in deciding the structural characteristics of the free finite carbon chains based on the parity of the carbon numbers. Due to the potential interaction between the carbon chains and CNTs, the electrons of the chain-CNT systems will redistribute, and some charges may transfer to the inner carbon chains from CNTs. We suggest that the attractive potential of chain atoms inside CNTs could be the driving force for formation of the linear carbon inside CNTs. Unexpectedly, we find that inside CNTs the carbon chains with even-numbered carbons present almost constant bond length alternation, which is independent of the chain length. This trend of the even-numbered carbon chains in CNTs helps to explain the universal experimental observation that the Raman peaks from chains in CNTs are within 1820-1860 cm(-1).

  8. Fission barriers from multidimensionally-constrained covariant density functional theories

    Directory of Open Access Journals (Sweden)

    Lu Bing-Nan

    2017-01-01

    Full Text Available In recent years, we have developed the multidimensionally-constrained covariant density functional theories (MDC-CDFTs in which both axial and spatial reflection symmetries are broken and all shape degrees of freedom described by βλμ with even μ, such as β20, β22, β30, β32, β40, etc., are included self-consistently. The MDC-CDFTs have been applied to the investigation of potential energy surfaces and fission barriers of actinide nuclei, third minima in potential energy surfaces of light actinides, shapes and potential energy surfaces of superheavy nuclei, octupole correlations between multiple chiral doublet bands in 78Br, octupole correlations in Ba isotopes, the Y32 correlations in N = 150 isotones and Zr isotopes, the spontaneous fission of Fm isotopes, and shapes of hypernuclei. In this contribution we present the formalism of MDC-CDFTs and the application of these theories to the study of fission barriers and potential energy surfaces of actinide nuclei.

  9. Analytical gradients for density functional calculations with approximate spin projection.

    Science.gov (United States)

    Saito, Toru; Thiel, Walter

    2012-11-08

    We have derived and implemented analytical gradients for broken-symmetry unrestricted density functional calculations (BS-UDFT) with removal of spin contamination by Yamaguchi's approximate spin projection method. Geometry optimizations with these analytical gradients (AGAP-opt) yield results consistent with those obtained with the previously available numerical gradients (NAP-opt). The AGAP-opt approach is found to be more precise, efficient, and robust than NAP-opt. It allows full geometry optimizations for large open-shell systems. We report results for three types of organic diradicals and for a binuclear vanadium(II) complex to demonstrate the merits of removing the spin contamination effects during geometry optimization (AGAP-opt vs BS-UDFT) and to illustrate the superior performance of the analytical gradients (AGAP-opt vs NAP-opt). The results for the vanadium(II) complex indicate that the AGAP-opt method is capable of handling pronounced spin contamination effects in large binuclear transition metal complexes with two magnetic centers.

  10. Density Functional Theory for Phase-Ordering Transitions

    Energy Technology Data Exchange (ETDEWEB)

    Wu, Jianzhong [Univ. of California, Riverside, CA (United States)

    2016-03-30

    Colloids display astonishing structural and dynamic properties that can be dramatically altered by modest changes in the solution condition or an external field. This complex behavior stems from a subtle balance of colloidal forces and intriguing mesoscopic and macroscopic phase transitions that are sensitive to the processing conditions and the dispersing environment. Whereas the knowledge on the microscopic structure and phase behavior of colloidal systems at equilibrium is now well-advanced, quantitative predictions of the dynamic properties and the kinetics of phase-ordering transitions in colloids are not always realized. Many important mesoscopic and off-equilibrium colloidal states remain poorly understood. The proposed research aims to develop a new, unifying approach to describe colloidal dynamics and the kinetics of phase-ordering transitions based on accomplishments from previous work for the equilibrium properties of both uniform and inhomogeneous systems and on novel concepts from the state-of-the-art dynamic density functional theory. In addition to theoretical developments, computational research is designed to address a number of fundamental questions on phase-ordering transitions in colloids, in particular those pertinent to a competition of the dynamic pathways leading to various mesoscopic structures, off-equilibrium states, and crystalline phases. By providing a generic theoretical framework to describe equilibrium, metastable as well as non-ergodic phase transitions concurrent with the colloidal self-assembly processes, accomplishments from this work will have major impacts on both fundamental research and technological applications.

  11. Efficiency issues related to probability density function comparison

    Energy Technology Data Exchange (ETDEWEB)

    Kelly, P.M.; Cannon, M.; Barros, J.E.

    1996-03-01

    The CANDID project (Comparison Algorithm for Navigating Digital Image Databases) employs probability density functions (PDFs) of localized feature information to represent the content of an image for search and retrieval purposes. A similarity measure between PDFs is used to identify database images that are similar to a user-provided query image. Unfortunately, signature comparison involving PDFs is a very time-consuming operation. In this paper, we look into some efficiency considerations when working with PDFS. Since PDFs can take on many forms, we look into tradeoffs between accurate representation and efficiency of manipulation for several data sets. In particular, we typically represent each PDF as a Gaussian mixture (e.g. as a weighted sum of Gaussian kernels) in the feature space. We find that by constraining all Gaussian kernels to have principal axes that are aligned to the natural axes of the feature space, computations involving these PDFs are simplified. We can also constrain the Gaussian kernels to be hyperspherical rather than hyperellipsoidal, simplifying computations even further, and yielding an order of magnitude speedup in signature comparison. This paper illustrates the tradeoffs encountered when using these constraints.

  12. Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties

    Science.gov (United States)

    Fortunato, Leandro F.; Zubieta, Carolina E.; Fuente, Silvia A.; Belelli, Patricia G.; Ferullo, Ricardo M.

    2016-11-01

    We report a density functional theory (DFT) investigation on the interaction of tiny Aun (n = 1-5) clusters with the bare and hydroxylated (110) surfaces of goethite (α-FeOOH). Both adsorption and atom-by-atom nucleation processes were modeled. The adsorption is shown to be strong on the bare surface and takes place preferentially through the interaction of Au atoms with unsaturated surface oxygen anions, accompanied with an electronic charge transfer from the metal to the support. Au3, Au4 and Au5 planar structures resulted to be particularly stable due to polarization effects; indeed, Coulombic repulsion between basal Au atoms and surface oxygen anions promotes the displacement of the electronic density toward terminal Au atoms producing a Au+δ(basal)/Au-δ(terminal) polarization. On the hydroxylated surface, Au clusters adsorb more weakly with respect to the bare surface, mainly through monocoordinated surface hydroxyl groups and tricoordinated oxygen ions. Concerning the nucleation mechanism, while on the hydroxylated surface the nucleation energy is governed by the spin of the interacting systems, on the bare surface polarization effects seems to play a predominant role.

  13. Synthesis and Biological Evaluation of Polar Functionalities Containing Nitrodihydroimidazooxazoles as Anti-TB Agents.

    Science.gov (United States)

    Yempalla, Kushalava Reddy; Munagala, Gurunadham; Singh, Samsher; Kour, Gurleen; Sharma, Shweta; Chib, Reena; Kumar, Sunil; Wazir, Priya; Singh, G D; Raina, Sushil; Bharate, Sonali S; Khan, Inshad Ali; Vishwakarma, Ram A; Singh, Parvinder Pal

    2015-10-08

    Novel polar functionalities containing 6-nitro-2,3-dihydroimidazooxazole (NHIO) analogues were synthesized to produce a compound with enhanced solubility. Polar functionalities including sulfonyl, uridyl, and thiouridyl-bearing NHIO analogues were synthesized and evaluated against Mycobacterium tuberculosis (MTB) H37Rv. The aqueous solubility of compounds with MIC values ≤0.5 μg/mL were tested, and six compounds showed enhanced aqueous solubility. The best six compounds were further tested against resistant (Rif(R) and MDR) and dormant strains of MTB and tested for cytotoxicity in HepG2 cell line. Based on its overall in vitro characteristics and solubility profile, compound 6d was further shown to possess high microsomal stability, solubility under all tested biological conditions (PBS, SGF and SIF), and favorable oral in vivo pharmacokinetics and in vivo efficacy.

  14. Salidroside attenuates neuroinflammation and improves functional recovery after spinal cord injury through microglia polarization regulation.

    Science.gov (United States)

    Wang, Chenggui; Wang, Qingqing; Lou, Yiting; Xu, Jianxiang; Feng, Zhenhua; Chen, Yu; Tang, Qian; Zheng, Gang; Zhang, Zengjie; Wu, Yaosen; Tian, Naifeng; Zhou, Yifei; Xu, Huazi; Zhang, Xiaolei

    2018-02-01

    Spinal cord injury (SCI) is a severe neurological disease; however, few drugs have been proved to treat SCI effectively. Neuroinflammation is the major pathogenesis of SCI secondary injury and considered to be the therapeutic target of SCI. Salidroside (Sal) has been reported to exert anti-inflammatory effects in airway, adipose and myocardial tissue; however, the role of Sal in SCI therapeutics has not been clarified. In this study, we showed that Sal could improve the functional recovery of spinal cord in rats as revealed by increased BBB locomotor rating scale, angle of incline, and decreased cavity of spinal cord injury and apoptosis of neurons in vivo. Immunofluorescence double staining of microglia marker and M1/M2 marker demonstrated that Sal could suppress M1 microglia polarization and activate M2 microglia polarization in vivo. To verify how Sal exerts its effects on microglia polarization and neuron protection, we performed the mechanism study in vitro in microglia cell line BV-2 and neuron cell line PC12. The results showed that Sal prevents apoptosis of PC12 cells in coculture with LPS-induced M1 BV-2 microglia, also the inflammatory secretion phenotype of M1 BV-2 microglia was suppressed by Sal, and further studies demonstrated that autophagic flux regulation through AMPK/mTOR pathway was involved in Sal regulated microglia polarization after SCI. Overall, our study illustrated that Sal could promote spinal cord injury functional recovery in rats, and the mechanism may relate to its microglia polarization modulation through AMPK-/mTOR-mediated autophagic flux stimulation. © 2017 The Authors. Journal of Cellular and Molecular Medicine published by John Wiley & Sons Ltd and Foundation for Cellular and Molecular Medicine.

  15. Adsorption of nitrogen oxides on graphene and graphene oxides: insights from density functional calculations.

    Science.gov (United States)

    Tang, Shaobin; Cao, Zexing

    2011-01-28

    The interactions of nitrogen oxides NO(x) (x = 1,2,3) and N(2)O(4) with graphene and graphene oxides (GOs) were studied by the density functional theory. Optimized geometries, binding energies, and electronic structures of the gas molecule-adsorbed graphene and GO were determined on the basis of first-principles calculations. The adsorption of nitrogen oxides on GO is generally stronger than that on graphene due to the presence of the active defect sites, such as the hydroxyl and carbonyl functional groups and the carbon atom near these groups. These active defect sites increase the binding energies and enhance charge transfers from nitrogen oxides to GO, eventually leading to the chemisorption of gas molecules and the doping character transition from acceptor to donor for NO(2) and NO. The interaction of nitrogen oxides with GO with various functional groups can result in the formation of hydrogen bonds OH⋅⋅⋅O (N) between -OH and nitrogen oxides and new weak covalent bonds C⋅⋅⋅N and C⋅⋅⋅O, as well as the H abstraction to form nitrous acid- and nitric acidlike moieties. The spin-polarized density of states reveals a strong hybridization of frontier orbitals of NO(2) and NO(3) with the electronic states around the Fermi level of GO, and gives rise to the strong acceptor doping by these molecules and remarkable charge transfers from molecules to GO, compared to NO and N(2)O(4) adsorptions on GO. The calculated results show good agreement with experimental observations.

  16. Tensor-polarized structure function b1 in the standard convolution description of the deuteron

    Science.gov (United States)

    Cosyn, W.; Dong, Yu-Bing; Kumano, S.; Sargsian, M.

    2017-04-01

    Tensor-polarized structure functions of a spin-1 hadron are additional observables, which do not exist for the spin-1 /2 nucleon. They could probe novel aspects of the internal hadron structure. Twist-2 tensor-polarized structure functions are b1 and b2, and they are related by the Callan-Gross-like relation in the Bjorken scaling limit. In this work, we theoretically calculate b1 in the standard convolution description for the deuteron. Two different theoretical models, a basic convolution description and a virtual nucleon approximation, are used for calculating b1, and their results are compared with the HERMES measurement. We found large differences between our theoretical results and the data. Although there is still room to improve by considering higher-twist effects and in the experimental extraction of b1 from the spin asymmetry Az z, there is a possibility that the large differences require physics beyond the standard deuteron model for their interpretation. Future b1 studies could shed light on a new field of hadron physics. In particular, detailed experimental studies of b1 will start soon at the Thomas Jefferson National Accelerator Facility. In addition, there are possibilities to investigate tensor-polarized parton distribution functions and b1 at Fermi National Accelerator Laboratory and a future electron-ion collider. Therefore, further theoretical studies are needed for understanding the tensor structure of the spin-1 deuteron, including a new mechanism to explain the large differences between the current data and our theoretical results.

  17. Solvent Dependence of (14)N Nuclear Magnetic Resonance Chemical Shielding Constants as a Test of the Accuracy of the Computed Polarization of Solute Electron Densities by the Solvent.

    Science.gov (United States)

    Ribeiro, Raphael F; Marenich, Aleksandr V; Cramer, Christopher J; Truhlar, Donald G

    2009-09-08

    Although continuum solvation models have now been shown to provide good quantitative accuracy for calculating free energies of solvation, questions remain about the accuracy of the perturbed solute electron densities and properties computed from them. Here we examine those questions by applying the SM8, SM8AD, SMD, and IEF-PCM continuum solvation models in combination with the M06-L density functional to compute the (14)N magnetic resonance nuclear shieldings of CH3CN, CH3NO2, CH3NCS, and CH3ONO2 in multiple solvents, and we analyze the dependence of the chemical shifts on solvent dielectric constant. We examine the dependence of the computed chemical shifts on the definition of the molecular cavity (both united-atom models and models based on superposed individual atomic spheres) and three kinds of treatments of the electrostatics, namely the generalized Born approximation with the Coulomb field approximation, the generalized Born model with asymmetric descreening, and models based on approximate numerical solution schemes for the nonhomogeneous Poisson equation. Our most systematic analyses are based on the computation of relative (14)N chemical shifts in a series of solvents, and we compare calculated shielding constants relative to those in CCl4 for various solvation models and density functionals. While differences in the overall results are found to be reasonably small for different solvation models and functionals, the SMx models SM8, and SM8AD, using the same cavity definitions (which for these models means the same atomic radii) as those employed for the calculation of free energies of solvation, exhibit the best agreement with experiment for every functional tested. This suggests that in addition to predicting accurate free energies of solvation, the SM8 and SM8AD generalized Born models also describe the solute polarization in a manner reasonably consistent with experimental (14)N nuclear magnetic resonance spectroscopy. Models based on the

  18. Local Approximation of the Correlation Energy Functional in the Density Matrix Functional Theory

    Science.gov (United States)

    Yasuda, Koji

    2002-02-01

    A local approximation formula of the correlation energy functional Ec in terms of the first-order reduced density matrix (1-RDM) is presented. With the contracted Schrödinger equation the principal dependence of Ec on the natural occupation numbers ni is identified. Using the effective mass theory, Ec is expressed as a functional of the local density and the local variable, J = Σi(ni(1-ni)) \\|ϕi\\|2, where ϕi are the natural spin orbitals. This local approximation satisfies the homogeneous coordinate scaling relation, gives the exact result for a one-electron system, and is almost free from the exchange energy error. It reproduced about 90% of the correlation energies of atoms and molecules.

  19. Density Functional Theory Calculations of Activation Energies for Carrier Capture by Defects in Semiconductors

    Science.gov (United States)

    Modine, N. A.; Wright, A. F.; Lee, S. R.

    The rate of defect-induced carrier recombination is determined by both defect levels and carrier capture cross-sections. Density functional theory (DFT) has been widely and successfully used to predict defect levels, but only recently has work begun to focus on using DFT to determine carrier capture cross-sections. Lang and Henry developed the theory of carrier-capture by multiphonon emission in the 1970s and showed that carrier-capture cross-sections differ between defects primarily due to differences in their carrier capture activation energies. We present an approach to using DFT to calculate carrier capture activation energies that does not depend on an assumed configuration coordinate and that fully accounts for anharmonic effects, which can substantially modify carrier activation energies. We demonstrate our approach for intrinisic defects in GaAs and GaN and discuss how our results depend on the choice of exchange-correlation functional and the treatment of spin polarization. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under Contract DE-AC04-94AL85000.

  20. Polarizable embedding with a multiconfiguration short-range density functional theory linear response method

    International Nuclear Information System (INIS)

    Hedegård, Erik Donovan; Olsen, Jógvan Magnus Haugaard; Knecht, Stefan; Kongsted, Jacob; Jensen, Hans Jørgen Aagaard

    2015-01-01

    We present here the coupling of a polarizable embedding (PE) model to the recently developed multiconfiguration short-range density functional theory method (MC-srDFT), which can treat multiconfigurational systems with a simultaneous account for dynamical and static correlation effects. PE-MC-srDFT is designed to combine efficient treatment of complicated electronic structures with inclusion of effects from the surrounding environment. The environmental effects encompass classical electrostatic interactions as well as polarization of both the quantum region and the environment. Using response theory, molecular properties such as excitation energies and oscillator strengths can be obtained. The PE-MC-srDFT method and the additional terms required for linear response have been implemented in a development version of DALTON. To benchmark the PE-MC-srDFT approach against the literature data, we have investigated the low-lying electronic excitations of acetone and uracil, both immersed in water solution. The PE-MC-srDFT results are consistent and accurate, both in terms of the calculated solvent shift and, unlike regular PE-MCSCF, also with respect to the individual absolute excitation energies. To demonstrate the capabilities of PE-MC-srDFT, we also investigated the retinylidene Schiff base chromophore embedded in the channelrhodopsin protein. While using a much more compact reference wave function in terms of active space, our PE-MC-srDFT approach yields excitation energies comparable in quality to CASSCF/CASPT2 benchmarks

  1. Polarizable embedding with a multiconfiguration short-range density functional theory linear response method

    Science.gov (United States)

    Hedegârd, Erik Donovan; Olsen, Jógvan Magnus Haugaard; Knecht, Stefan; Kongsted, Jacob; Jensen, Hans Jørgen Aagaard

    2015-03-01

    We present here the coupling of a polarizable embedding (PE) model to the recently developed multiconfiguration short-range density functional theory method (MC-srDFT), which can treat multiconfigurational systems with a simultaneous account for dynamical and static correlation effects. PE-MC-srDFT is designed to combine efficient treatment of complicated electronic structures with inclusion of effects from the surrounding environment. The environmental effects encompass classical electrostatic interactions as well as polarization of both the quantum region and the environment. Using response theory, molecular properties such as excitation energies and oscillator strengths can be obtained. The PE-MC-srDFT method and the additional terms required for linear response have been implemented in a development version of Dalton. To benchmark the PE-MC-srDFT approach against the literature data, we have investigated the low-lying electronic excitations of acetone and uracil, both immersed in water solution. The PE-MC-srDFT results are consistent and accurate, both in terms of the calculated solvent shift and, unlike regular PE-MCSCF, also with respect to the individual absolute excitation energies. To demonstrate the capabilities of PE-MC-srDFT, we also investigated the retinylidene Schiff base chromophore embedded in the channelrhodopsin protein. While using a much more compact reference wave function in terms of active space, our PE-MC-srDFT approach yields excitation energies comparable in quality to CASSCF/CASPT2 benchmarks.

  2. Accuracy of density functional theory in the prediction of carbon dioxide adsorbent materials.

    Science.gov (United States)

    Cazorla, Claudio; Shevlin, Stephen A

    2013-04-07

    Density functional theory (DFT) has become the computational method of choice for modeling and characterization of carbon dioxide adsorbents, a broad family of materials which at present are urgently sought after for environmental applications. The description of polar carbon dioxide (CO(2)) molecules in low-coordinated environments like surfaces and porous materials, however, may be challenging for local and semi-local DFT approximations. Here, we present a thorough computational study in which the accuracy of DFT methods in describing the interactions of CO(2) with model alkali-earth-metal (AEM, Ca and Li) decorated carbon structures, namely anthracene (C(14)H(10)) molecules, is assessed. We find that gas-adsorption energies and equilibrium structures obtained with standard (i.e. LDA and GGA), hybrid (i.e. PBE0 and B3LYP) and van der Waals exchange-correlation functionals of DFT dramatically differ from the results obtained with second-order Møller-Plesset perturbation theory (MP2), an accurate computational quantum chemistry method. The major disagreements found can be mostly rationalized in terms of electron correlation errors that lead to wrong charge-transfer and electrostatic Coulomb interactions between CO(2) and AEM-decorated anthracene molecules. Nevertheless, we show that when the concentration of AEM atoms in anthracene is tuned to resemble as closely as possible the electronic structure of AEM-decorated graphene (i.e. an extended two-dimensional material), hybrid exchange-correlation DFT and MP2 methods quantitatively provide similar results.

  3. Antioxidant Properties of Kynurenines: Density Functional Theory Calculations

    Science.gov (United States)

    2016-01-01

    Kynurenines, the main products of tryptophan catabolism, possess both prooxidant and anioxidant effects. Having multiple neuroactive properties, kynurenines are implicated in the development of neurological and cognitive disorders, such as Alzheimer's, Parkinson's, and Huntington's diseases. Autoxidation of 3-hydroxykynurenine (3HOK) and its derivatives, 3-hydroxyanthranilic acid (3HAA) and xanthommatin (XAN), leads to the hyperproduction of reactive oxygen species (ROS) which damage cell structures. At the same time, 3HOK and 3HAA have been shown to be powerful ROS scavengers. Their ability to quench free radicals is believed to result from the presence of the aromatic hydroxyl group which is able to easily abstract an electron and H-atom. In this study, the redox properties for kynurenines and several natural and synthetic antioxidants have been calculated at different levels of density functional theory in the gas phase and water solution. Hydroxyl bond dissociation enthalpy (BDE) and ionization potential (IP) for 3HOK and 3HAA appear to be lower than for xanthurenic acid (XAA), several phenolic antioxidants, and ascorbic acid. BDE and IP for the compounds with aromatic hydroxyl group are lower than for their precursors without hydroxyl group. The reaction rate for H donation to *O-atom of phenoxyl radical (Ph-O*) and methyl peroxy radical (Met-OO*) decreases in the following rankings: 3HOK ~ 3HAA > XAAOXO > XAAENOL. The enthalpy absolute value for Met-OO* addition to the aromatic ring of the antioxidant radical increases in the following rankings: 3HAA* < 3HOK* < XAAOXO* < XAAENOL*. Thus, the high free radical scavenging activity of 3HAA and 3HOK can be explained by the easiness of H-atom abstraction and transfer to O-atom of the free radical, rather than by Met-OO* addition to the kynurenine radical. PMID:27861556

  4. Antioxidant Properties of Kynurenines: Density Functional Theory Calculations.

    Directory of Open Access Journals (Sweden)

    Aleksandr V Zhuravlev

    2016-11-01

    Full Text Available Kynurenines, the main products of tryptophan catabolism, possess both prooxidant and anioxidant effects. Having multiple neuroactive properties, kynurenines are implicated in the development of neurological and cognitive disorders, such as Alzheimer's, Parkinson's, and Huntington's diseases. Autoxidation of 3-hydroxykynurenine (3HOK and its derivatives, 3-hydroxyanthranilic acid (3HAA and xanthommatin (XAN, leads to the hyperproduction of reactive oxygen species (ROS which damage cell structures. At the same time, 3HOK and 3HAA have been shown to be powerful ROS scavengers. Their ability to quench free radicals is believed to result from the presence of the aromatic hydroxyl group which is able to easily abstract an electron and H-atom. In this study, the redox properties for kynurenines and several natural and synthetic antioxidants have been calculated at different levels of density functional theory in the gas phase and water solution. Hydroxyl bond dissociation enthalpy (BDE and ionization potential (IP for 3HOK and 3HAA appear to be lower than for xanthurenic acid (XAA, several phenolic antioxidants, and ascorbic acid. BDE and IP for the compounds with aromatic hydroxyl group are lower than for their precursors without hydroxyl group. The reaction rate for H donation to *O-atom of phenoxyl radical (Ph-O* and methyl peroxy radical (Met-OO* decreases in the following rankings: 3HOK ~ 3HAA > XAAOXO > XAAENOL. The enthalpy absolute value for Met-OO* addition to the aromatic ring of the antioxidant radical increases in the following rankings: 3HAA* < 3HOK* < XAAOXO* < XAAENOL*. Thus, the high free radical scavenging activity of 3HAA and 3HOK can be explained by the easiness of H-atom abstraction and transfer to O-atom of the free radical, rather than by Met-OO* addition to the kynurenine radical.

  5. Density functional study of condensation in capped capillaries

    Science.gov (United States)

    Yatsyshin, P.; Savva, N.; Kalliadasis, S.

    2015-07-01

    We study liquid adsorption in narrow rectangular capped capillaries formed by capping two parallel planar walls (a slit pore) with a third wall orthogonal to the two planar walls. The most important transition in confined fluids is arguably condensation, where the pore becomes filled with the liquid phase which is metastable in the bulk. Depending on the temperature T, the condensation in capped capillaries can be first-order (at T≤slant {{T}\\text{cw}} ) or continuous (at T\\gt {{T}\\text{cw}} ), where {{T}\\text{cw}} is the capillary wetting temperature. At T \\gt {{T}\\text{cw}} , the capping wall can adsorb mesoscopic amounts of metastable under-condensed liquid. The onset of condensation is then manifested by the continuous unbinding of the interface between the liquid adsorbed on the capping wall and the gas filling the rest of the capillary volume. In wide capped capillaries there may be a remnant of wedge filling transition, which is manifested by the adsorption of liquid drops in the corners. Our classical statistical mechanical treatment predicts a possibility of three-phase coexistence between gas, corner drops and liquid slabs adsorbed on the capping wall. In sufficiently wide capillaries we find that thick prewetting films of finite length may be nucleated at the capping wall below the boundary of the prewetting transition. Prewetting then proceeds in a continuous manner manifested by the unbinding interface between the thick and thin films adsorbed on the side walls. Our analysis is based on a detailed numerical investigation of the density functional theory for the fluid equilibria for a number of illustrative case studies.

  6. Subspace accelerated inexact Newton method for large scale wave functions calculations in Density Functional Theory

    Energy Technology Data Exchange (ETDEWEB)

    Fattebert, J

    2008-07-29

    We describe an iterative algorithm to solve electronic structure problems in Density Functional Theory. The approach is presented as a Subspace Accelerated Inexact Newton (SAIN) solver for the non-linear Kohn-Sham equations. It is related to a class of iterative algorithms known as RMM-DIIS in the electronic structure community. The method is illustrated with examples of real applications using a finite difference discretization and multigrid preconditioning.

  7. Microscopically-Based Energy Density Functionals for Nuclei Using the Density Matrix Expansion. I: Implementation and Pre-Optimization

    Energy Technology Data Exchange (ETDEWEB)

    Stoitsov, M. V. [University of Tennessee, Knoxville (UTK) & Oak Ridge National Laboratory (ORNL); Kortelainen, Erno M [ORNL; Bogner, S. K. [Michigan State University, East Lansing; Duguet, T. [CEA, Saclay, France; Furnstahl, R. J. [Ohio State University; Gebremariam, B. [Michigan State University, East Lansing; Schunck, N. [University of Tennessee, Knoxville (UTK) & Oak Ridge National Laboratory (ORNL)

    2010-01-01

    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 in {chi}^{2} compared to standard Skyrme functionals, thus justifying its suitability for future global optimizations and large-scale calculations.

  8. Tuning electronic properties in graphene quantum dots by chemical functionalization: Density functional theory calculations

    Science.gov (United States)

    Abdelsalam, Hazem; Elhaes, Hanan; Ibrahim, Medhat A.

    2018-03-01

    The energy gap and dipole moment of chemically functionalized graphene quantum dots are investigated by density functional theory. The energy gap can be tuned through edge passivation by different elements or groups. Edge passivation by oxygen considerably decreases the energy gap in hexagonal nanodots. Edge states in triangular quantum dots can also be manipulated by passivation with fluorine. The dipole moment depends on: (a) shape and edge termination of the quantum dot, (b) attached group, and (c) position to which the groups are attached. Depending on the position of attached groups, the total dipole can be increased, decreased, or eliminated.

  9. Robust functional statistics applied to Probability Density Function shape screening of sEMG data.

    Science.gov (United States)

    Boudaoud, S; Rix, H; Al Harrach, M; Marin, F

    2014-01-01

    Recent studies pointed out possible shape modifications of the Probability Density Function (PDF) of surface electromyographical (sEMG) data according to several contexts like fatigue and muscle force increase. Following this idea, criteria have been proposed to monitor these shape modifications mainly using High Order Statistics (HOS) parameters like skewness and kurtosis. In experimental conditions, these parameters are confronted with small sample size in the estimation process. This small sample size induces errors in the estimated HOS parameters restraining real-time and precise sEMG PDF shape monitoring. Recently, a functional formalism, the Core Shape Model (CSM), has been used to analyse shape modifications of PDF curves. In this work, taking inspiration from CSM method, robust functional statistics are proposed to emulate both skewness and kurtosis behaviors. These functional statistics combine both kernel density estimation and PDF shape distances to evaluate shape modifications even in presence of small sample size. Then, the proposed statistics are tested, using Monte Carlo simulations, on both normal and Log-normal PDFs that mimic observed sEMG PDF shape behavior during muscle contraction. According to the obtained results, the functional statistics seem to be more robust than HOS parameters to small sample size effect and more accurate in sEMG PDF shape screening applications.

  10. Neural-network-based depth-resolved multiscale structural optimization using density functional theory and electron diffraction data

    Science.gov (United States)

    Pennington, Robert S.; Coll, Catalina; Estradé, Sònia; Peiró, Francesca; Koch, Christoph T.

    2018-01-01

    Iterative neural-network-based three-dimensional structural optimization of atomic positions over tens of nanometers is performed using transmission electron microscope (TEM) diffraction data simulated from density functional theory (DFT) all-electron densities, thus retrieving parameter variations along the beam direction. We first use experimental data to show that the GPAW DFT code's all-electron densities are considerably more accurate for electron diffraction calculations compared to conventional isolated-atom scattering factors, and they also compare well to Wien2K DFT simulations. This DFT-TEM combination is then integrated into an iterative neural-network-optimization-based algorithm (PRIMES, parameter retrieval and inversion from multiple electron scattering) to retrieve nanometer-scale ferroelectric polarization domains and strain in theoretical bulklike specimens from TEM data. DFT and isolated-atom methods produce substantially different diffraction patterns and retrieved polarization domain parameters, and DFT is sufficient to retrieve strain properties from a silicon specimen simulated using experimentally derived structure factors. Thus, we show that the improved accuracy, fast computation, and intuitive integration make the GPAW DFT code well suited for three-dimensional materials characterization and demonstrate this using an iterative neural-network algorithm that is verifiable on the mesoscale and, with DFT integration, self-consistent on the nanoscale.

  11. One-electron properties of several small molecules calculated using the local density approximation within density functional theory

    Science.gov (United States)

    Duffy, Patrick; Chong, Delano P.; Dupuis, Michel

    1995-02-01

    Density functional theory (DFT) is a field enjoying a tremendous recent surge in popularity among theoretical and practical chemists alike because of its ability to more easily handle larger molecular systems than conventional ab initio methods. Until recently, however, assessment of the quality of the properties predicted (and therefore the charge density) from DFT had been limited mainly to dipole moments and their nuclear coordinate and electric field derivatives. This paper presents the calculated results for some of the one-electron properties of the eight small molecules (NH3, PH3, H2O, H2S, HF, HCl, CO, and N2). The properties chosen weight different regions of the charge density, from either very close in or at the nucleus (e.g., δ, the electron density at the nucleus) to regions farther out from the nucleus (e.g., the diamagnetic susceptibility ). It is found that properties which depend on an accurate knowledge of the electron density near to the nucleus are predicted poorly by the local density approximation (LDA), while others more dependent on the charge density farther out from the nucleus are predicted much more accurately, possibly due to cancellation of errors. Use of the LDA is therefore not recommended for ``tight'' properties; use of a functional employing gradient corrections would be more suitable for this purpose.

  12. Point-spread functions of a polarizing microscope equipped with high-numerical-aperture lenses.

    Science.gov (United States)

    Oldenbourg, R; Török, P

    2000-12-01

    In an effort to establish the imaging properties of a new type of polarized-light microscope, we recorded images of small, uniaxial, birefringent crystals. We show that the sequence of in-focus and out-of-focus images, the so-called point-spread function, of a submicroscopic crystal can be used to measure the orientation of its optic axis in three-dimensional space. By analogy to conoscopic images out-of-focus images reveal the changes in relative phase shift between the extraordinary and the ordinary rays that propagate at different directions through the crystal. We also present simulated images of a pointlike anisotropic scattering particle and compare these with our experimental findings. The theoretical model is based on a complete vectorial theory for partial coherent imaging by use of polarized light and high-numerical-aperture lenses.

  13. Multiconfiguration Pair-Density Functional Theory Outperforms Kohn-Sham Density Functional Theory and Multireference Perturbation Theory for Ground-State and Excited-State Charge Transfer.

    Science.gov (United States)

    Ghosh, Soumen; Sonnenberger, Andrew L; Hoyer, Chad E; Truhlar, Donald G; Gagliardi, Laura

    2015-08-11

    The correct description of charge transfer in ground and excited states is very important for molecular interactions, photochemistry, electrochemistry, and charge transport, but it is very challenging for Kohn-Sham (KS) density functional theory (DFT). KS-DFT exchange-correlation functionals without nonlocal exchange fail to describe both ground- and excited-state charge transfer properly. We have recently proposed a theory called multiconfiguration pair-density functional theory (MC-PDFT), which is based on a combination of multiconfiguration wave function theory with a new type of density functional called an on-top density functional. Here we have used MC-PDFT to study challenging ground- and excited-state charge-transfer processes by using on-top density functionals obtained by translating KS exchange-correlation functionals. For ground-state charge transfer, MC-PDFT performs better than either the PBE exchange-correlation functional or CASPT2 wave function theory. For excited-state charge transfer, MC-PDFT (unlike KS-DFT) shows qualitatively correct behavior at long-range with great improvement in predicted excitation energies.

  14. Theoretical study on β-aminoacroleine; Density functional theory ...

    Indian Academy of Sciences (India)

    The local potential energy density V(rCP) can be obtained from the virial equation25: 2G (rCP) + V (rCP) = (1/4)∇2ρ (rCP). All values in the realations mentioned above are expressed in atomic units. EHB energies calculated from the potential energy densities of O...H contacts are included in table 1. It is worthy to mention ...

  15. Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties

    Energy Technology Data Exchange (ETDEWEB)

    Fortunato, Leandro F.; Zubieta, Carolina E. [INQUISUR (UNS-CONICET) and Departamento de Química, Universidad Nacional del Sur, Av. Alem 1253, Bahía Blanca (Argentina); Fuente, Silvia A.; Belelli, Patricia G. [IFISUR (UNS-CONICET) and Departamento de Física, Universidad Nacional del Sur, Av. Alem 1253, Bahía Blanca (Argentina); Ferullo, Ricardo M., E-mail: caferull@criba.edu.ar [INQUISUR (UNS-CONICET) and Departamento de Química, Universidad Nacional del Sur, Av. Alem 1253, Bahía Blanca (Argentina)

    2016-11-30

    Highlights: • On the hydroxylated surface, the adsorption of Au clusters is relatively weak. • Au-oxide interaction induces a polarization of the Au particles on the bare surface. • A predominance of planar (111) arrangements was obtained on both surfaces. • Comparing both surfaces, atom-by-atom nucleation energies show opposite behaviors. - Abstract: We report a density functional theory (DFT) investigation on the interaction of tiny Au{sub n} (n = 1–5) clusters with the bare and hydroxylated (110) surfaces of goethite (α-FeOOH). Both adsorption and atom-by-atom nucleation processes were modeled. The adsorption is shown to be strong on the bare surface and takes place preferentially through the interaction of Au atoms with unsaturated surface oxygen anions, accompanied with an electronic charge transfer from the metal to the support. Au{sub 3}, Au{sub 4} and Au{sub 5} planar structures resulted to be particularly stable due to polarization effects; indeed, Coulombic repulsion between basal Au atoms and surface oxygen anions promotes the displacement of the electronic density toward terminal Au atoms producing a Au{sup +δ}(basal)/Au{sup −δ}(terminal) polarization. On the hydroxylated surface, Au clusters adsorb more weakly with respect to the bare surface, mainly through monocoordinated surface hydroxyl groups and tricoordinated oxygen ions. Concerning the nucleation mechanism, while on the hydroxylated surface the nucleation energy is governed by the spin of the interacting systems, on the bare surface polarization effects seems to play a predominant role.

  16. A unified approach to the density-potential mapping in a family of time-dependent density functional theories

    Science.gov (United States)

    Tokatly, I. V.

    2011-11-01

    It is shown that the density-potential mapping and the V-representability problems in the time-dependent current density functional theory (TDCDFT) are reduced to the solution of a certain many-body nonlinear Schrödinger equation (NLSE). The derived NLSE for TDCDFT links the earlier NLSE-based formulations of the time-dependent deformation functional theory (TDDefFT) and the time-dependent density functional theory (TDDFT). We establish a close relation between the nonlinear many-body problems which control the existence of TDCDFT, TDDFT, and TDDefFT, and thus develop a unified point of view on the whole family of the TDDFT-type theories.

  17. Probability density functions for use when calculating standardised drought indices

    Science.gov (United States)

    Svensson, Cecilia; Prosdocimi, Ilaria; Hannaford, Jamie

    2015-04-01

    Time series of drought indices like the standardised precipitation index (SPI) and standardised flow index (SFI) require a statistical probability density function to be fitted to the observed (generally monthly) precipitation and river flow data. Once fitted, the quantiles are transformed to a Normal distribution with mean = 0 and standard deviation = 1. These transformed data are the SPI/SFI, which are widely used in drought studies, including for drought monitoring and early warning applications. Different distributions were fitted to rainfall and river flow data accumulated over 1, 3, 6 and 12 months for 121 catchments in the United Kingdom. These catchments represent a range of catchment characteristics in a mid-latitude climate. Both rainfall and river flow data have a lower bound at 0, as rains and flows cannot be negative. Their empirical distributions also tend to have positive skewness, and therefore the Gamma distribution has often been a natural and suitable choice for describing the data statistically. However, after transformation of the data to Normal distributions to obtain the SPIs and SFIs for the 121 catchments, the distributions are rejected in 11% and 19% of cases, respectively, by the Shapiro-Wilk test. Three-parameter distributions traditionally used in hydrological applications, such as the Pearson type 3 for rainfall and the Generalised Logistic and Generalised Extreme Value distributions for river flow, tend to make the transformed data fit better, with rejection rates of 5% or less. However, none of these three-parameter distributions have a lower bound at zero. This means that the lower tail of the fitted distribution may potentially go below zero, which would result in a lower limit to the calculated SPI and SFI values (as observations can never reach into this lower tail of the theoretical distribution). The Tweedie distribution can overcome the problems found when using either the Gamma or the above three-parameter distributions. The

  18. Density functional study of hydrogen in amorphous silicon

    Science.gov (United States)

    Tuttle, Blair R.

    Hydrogenated amorphous silicon is a relatively new material with device applications including photovoltaics. Intrinsic and light-induced electronic defects reduce the efficiency of a-Si:H solar cells. Although hydrogen is implicated in these defects, microscopic understanding of the structure and energetics of hydrogen in a-Si:H has been limited. The current limits are in part due to the lack of reliable theoretical calculations. Here we apply density functional methods to study H in a-Si:H. First, we develop a new atomistic model for a-Si:H. Then, using molecular dynamics simulations, we compare several currently available atomistic models. Finally, we calculate the properties of hydrogen in these models, including the geometric environments, the energetics, the electronic structure and the vibrational properties. Our most important conclusions are presented below. Our calculations are consistent with the following microscopic picture for long range diffusion of H in a-Si:H. Clustered Si-H bonds constitute the dominant trapping species. Upon the dissociation of 2 H atoms, a Si-Si bond forms leaving a nominally 4-fold coordinated weak bond complex. The 2 H atoms move away separately along Si-Si bond center sites until trapped at another weak bond complex. The calculated activation energy is found in agreement with established experimental results. Also, our calculations are successfully applied to observations of H evolution, hydrogen-deuterium exchange and long range diffusion in p-type amorphous silicon. Our calculations clarify the role of H during electronic defect formation. We calculate the energetics for H to move from a variety of Si-H bonds to the bulk chemical potential. For isolated Si-H bonds (i.e. in micro-cavities without any bond reconstruction) the energetics are not consistent with observations. However, if the remaining Si reconstructs with a nearby silicon creating a 5-fold coordinated defect then the energetics are in agreement with

  19. Lymphatic vessel density and function in experimental bladder cancer

    International Nuclear Information System (INIS)

    Saban, Marcia R; Wu, Xue-Ru; Saban, Ricardo; Towner, Rheal; Smith, Nataliya; Abbott, Andrew; Neeman, Michal; Davis, Carole A; Simpson, Cindy; Maier, Julie; Mémet, Sylvie

    2007-01-01

    The lymphatics form a second circulatory system that drains the extracellular fluid and proteins from the tumor microenvironment, and provides an exclusive environment in which immune cells interact and respond to foreign antigen. Both cancer and inflammation are known to induce lymphangiogenesis. However, little is known about bladder lymphatic vessels and their involvement in cancer formation and progression. A double transgenic mouse model was generated by crossing a bladder cancer-induced transgenic, in which SV40 large T antigen was under the control of uroplakin II promoter, with another transgenic mouse harboring a lacZ reporter gene under the control of an NF-κB-responsive promoter (κB-lacZ) exhibiting constitutive activity of β-galactosidase in lymphatic endothelial cells. In this new mouse model (SV40-lacZ), we examined the lymphatic vessel density (LVD) and function (LVF) during bladder cancer progression. LVD was performed in bladder whole mounts and cross-sections by fluorescent immunohistochemistry (IHC) using LYVE-1 antibody. LVF was assessed by real-time in vivo imaging techniques using a contrast agent (biotin-BSA-Gd-DTPA-Cy5.5; Gd-Cy5.5) suitable for both magnetic resonance imaging (MRI) and near infrared fluorescence (NIRF). In addition, IHC of Cy5.5 was used for time-course analysis of co-localization of Gd-Cy5.5 with LYVE-1-positive lymphatics and CD31-positive blood vessels. SV40-lacZ mice develop bladder cancer and permitted visualization of lymphatics. A significant increase in LVD was found concomitantly with bladder cancer progression. Double labeling of the bladder cross-sections with LYVE-1 and Ki-67 antibodies indicated cancer-induced lymphangiogenesis. MRI detected mouse bladder cancer, as early as 4 months, and permitted to follow tumor sizes during cancer progression. Using Gd-Cy5.5 as a contrast agent for MRI-guided lymphangiography, we determined a possible reduction of lymphatic flow within the tumoral area. In addition, NIRF

  20. Native defects in oxide semiconductors: a density functional approach.

    Science.gov (United States)

    Oba, Fumiyasu; Choi, Minseok; Togo, Atsushi; Seko, Atsuto; Tanaka, Isao

    2010-09-29

    We report a semilocal and hybrid Hartree-Fock density functional study of native defects in three oxide semiconductors: ZnO, SrTiO(3), and SnO. The defect that is responsible for the n-type conductivity of ZnO has been debated, in which the O vacancy, Zn interstitial, their complexes, and residual H impurity are considered candidates. Our results indicate that the O vacancy induces a deep and localized in-gap state, whereas the Zn interstitial is a shallow donor and hence can be a source of the carriers. In view of the formation energies, the O vacancy is likely to form with a substantial concentration under O-poor conditions, but the Zn interstitial is unlikely. We thus propose that the O vacancy is relevant to the nonstoichiometry of ZnO and that a source other than the native defects, such as the H impurity, needs to be considered for the n-type conductivity. For SrTiO(3), the O vacancy and its complexes have been regarded as the origins of some of the remarkable electrical and optical properties. We suggest significant roles of the Ti antisite for a new insight into the defect-induced properties. Two types of Ti antisite, both of which are off-centered from the Sr site but toward different directions, exhibit low formation energies under Ti-rich conditions as does the O vacancy. They can explain optical properties such as visible-light emission, deep-level absorption, and the ferroelectricity observed in reduced SrTiO(3). As an example of p-type conductors, SnO has been investigated with a focus on the acceptor-like native defects. Under O-rich conditions, the Sn vacancy and O interstitial are found to be energetically favorable. The Sn vacancy induces shallow acceptor levels and can therefore be a source of carriers. The O interstitial shows no in-gap levels and hence it is inactive in terms of the carrier generation and compensation. However, this defect is a key to the understanding of the structures of intermediate compounds between SnO and SnO(2).

  1. Density Functional Theory Modeling of Ferrihydrite Nanoparticle Adsorption Behavior

    Science.gov (United States)

    Kubicki, J.

    2016-12-01

    Ferrihydrite is a critical substrate for adsorption of oxyanion species in the environment1. The nanoparticulate nature of ferrihydrite is inherent to its formation, and hence it has been called a "nano-mineral"2. The nano-scale size and unusual composition of ferrihydrite has made structural determination of this phase problematic. Michel et al.3 have proposed an atomic structure for ferrihydrite, but this model has been controversial4,5. Recent work has shown that the Michel et al.3 model structure may be reasonably accurate despite some deficiencies6-8. An alternative model has been proposed by Manceau9. This work utilizes density functional theory (DFT) calculations to model both the structure of ferrihydrite nanoparticles based on the Michel et al. 3 model as refined in Hiemstra8 and the modified akdalaite model of Manceau9. Adsorption energies of carbonate, phosphate, sulfate, chromate, arsenite and arsenate are calculated. Periodic projector-augmented planewave calculations were performed with the Vienna Ab-initio Simulation Package (VASP10) on an approximately 1.7 nm diameter Michel nanoparticle (Fe38O112H110) and on a 2 nm Manceau nanoparticle (Fe38O95H76). After energy minimization of the surface H and O atoms. The model will be used to assess the possible configurations of adsorbed oxyanions on the model nanoparticles. Brown G.E. Jr. and Calas G. (2012) Geochemical Perspectives, 1, 483-742. Hochella M.F. and Madden A.S. (2005) Elements, 1, 199-203. Michel, F.M., Ehm, L., Antao, S.M., Lee, P.L., Chupas, P.J., Liu, G., Strongin, D.R., Schoonen, M.A.A., Phillips, B.L., and Parise, J.B., 2007, Science, 316, 1726-1729. Rancourt, D.G., and Meunier, J.F., 2008, American Mineralogist, 93, 1412-1417. Manceau, A., 2011, American Mineralogist, 96, 521-533. Maillot, F., Morin, G., Wang, Y., Bonnin, D., Ildefonse, P., Chaneac, C., Calas, G., 2011, Geochimica et Cosmochimica Acta, 75, 2708-2720. Pinney, N., Kubicki, J.D., Middlemiss, D.S., Grey, C.P., and Morgan, D

  2. Exact density functional and wave function embedding schemes based on orbital localization

    International Nuclear Information System (INIS)

    Hégely, Bence; Nagy, Péter R.; Kállay, Mihály; Ferenczy, György G.

    2016-01-01

    Exact schemes for the embedding of density functional theory (DFT) and wave function theory (WFT) methods into lower-level DFT or WFT approaches are introduced utilizing orbital localization. First, a simple modification of the projector-based embedding scheme of Manby and co-workers [J. Chem. Phys. 140, 18A507 (2014)] is proposed. We also use localized orbitals to partition the system, but instead of augmenting the Fock operator with a somewhat arbitrary level-shift projector we solve the Huzinaga-equation, which strictly enforces the Pauli exclusion principle. Second, the embedding of WFT methods in local correlation approaches is studied. Since the latter methods split up the system into local domains, very simple embedding theories can be defined if the domains of the active subsystem and the environment are treated at a different level. The considered embedding schemes are benchmarked for reaction energies and compared to quantum mechanics (QM)/molecular mechanics (MM) and vacuum embedding. We conclude that for DFT-in-DFT embedding, the Huzinaga-equation-based scheme is more efficient than the other approaches, but QM/MM or even simple vacuum embedding is still competitive in particular cases. Concerning the embedding of wave function methods, the clear winner is the embedding of WFT into low-level local correlation approaches, and WFT-in-DFT embedding can only be more advantageous if a non-hybrid density functional is employed.

  3. Angle-dependent strong-field molecular ionization rates with tuned range-separated time-dependent density functional theory.

    Science.gov (United States)

    Sissay, Adonay; Abanador, Paul; Mauger, François; Gaarde, Mette; Schafer, Kenneth J; Lopata, Kenneth

    2016-09-07

    Strong-field ionization and the resulting electronic dynamics are important for a range of processes such as high harmonic generation, photodamage, charge resonance enhanced ionization, and ionization-triggered charge migration. Modeling ionization dynamics in molecular systems from first-principles can be challenging due to the large spatial extent of the wavefunction which stresses the accuracy of basis sets, and the intense fields which require non-perturbative time-dependent electronic structure methods. In this paper, we develop a time-dependent density functional theory approach which uses a Gaussian-type orbital (GTO) basis set to capture strong-field ionization rates and dynamics in atoms and small molecules. This involves propagating the electronic density matrix in time with a time-dependent laser potential and a spatial non-Hermitian complex absorbing potential which is projected onto an atom-centered basis set to remove ionized charge from the simulation. For the density functional theory (DFT) functional we use a tuned range-separated functional LC-PBE*, which has the correct asymptotic 1/r form of the potential and a reduced delocalization error compared to traditional DFT functionals. Ionization rates are computed for hydrogen, molecular nitrogen, and iodoacetylene under various field frequencies, intensities, and polarizations (angle-dependent ionization), and the results are shown to quantitatively agree with time-dependent Schrödinger equation and strong-field approximation calculations. This tuned DFT with GTO method opens the door to predictive all-electron time-dependent density functional theory simulations of ionization and ionization-triggered dynamics in molecular systems using tuned range-separated hybrid functionals.

  4. Kohn-Sham density-functional theory and renormalization of many-body perturbation expansions

    Science.gov (United States)

    Valiev, Marat

    1998-03-01

    Numerous practical applications provide strong evidence that despite its simplicity and crude approximations, density-functional theory leads to a rather accurate description of ground state properties of various condensed matter systems. Although well documented numerically, to our knowledge a theoretical explanation of the accuracy of density-functional theory has not been given. This issue is clarified in marat/>this work by demonstrating that density-functional theory represents a particular renormalization procedure of a many-body perturbation expansion. In other words, it is shown that density-functional theory is a many-body perturbation theory whose convergence properties have been optimized. The realization of this fact brings new meaning into density-functional theory and explains the success of density-functional based calculations. For more information go to marat/>http://alchemy.ucsd.edu/marat/ .

  5. Persistent organic pollutants, skull size and bone density of polar bears (Ursus maritimus) from East Greenland 1892-2015 and Svalbard 1964-2004

    DEFF Research Database (Denmark)

    Daugaard-Petersen, Tobias; Langebæk, Rikke; Rigét, Frank F

    2018-01-01

    We investigated skull size (condylobasal length; CBL) and bone mineral density (BMD) in polar bears (Ursus maritimus) from East Greenland (n = 307) and Svalbard (n = 173) sampled during the period 1892–2015 in East Greenland and 1964–2004 at Svalbard. Adult males from East Greenland showed...... that the skull size of adult East Greenland females was negatively correlated with collection year 1892–2015 (linear regression: p = 0.06). No temporal change was found for BMD or skull size in Svalbard polar bears (ANOVA: all p > 0.05) nor was there any significant difference in BMD between Svalbard and East...... Greenland subpopulations. Skull size was larger in polar bears from Svalbard than from East Greenland (two-way ANOVA: p = 0.003). T-scores reflecting risk of osteoporosis showed that adult males from both East Greenland and Svalbard are at risk of developing osteopenia. Finally, when correcting for age...

  6. The probability density function of completed length of service (CLS ...

    African Journals Online (AJOL)

    ... functions this paper estimates the functions for some secondary schools in Enugu State. Wastage probabilities are calculated, survivor functions estimated. The accompanying standard errors are also obtained. Key words: Manpower Planning, Length of Service, Modelling, Survivor Functions. [Global Jnl Mathematical Sci ...

  7. Connections between variation principles at the interface of wave-function and density-functional theories.

    Science.gov (United States)

    Irons, Tom J P; Furness, James W; Ryley, Matthew S; Zemen, Jan; Helgaker, Trygve; Teale, Andrew M

    2017-10-07

    A recently proposed variation principle [N. I. Gidopoulos, Phys. Rev. A 83, 040502(R) (2011)] for the determination of Kohn-Sham effective potentials is examined and extended to arbitrary electron-interaction strengths and to mixed states. Comparisons are drawn with Lieb's convex-conjugate functional, which allows for the determination of a potential associated with a given electron density by maximization, yielding the Kohn-Sham potential for a non-interacting system. The mathematical structure of the two functionals is shown to be intrinsically related; the variation principle put forward by Gidopoulos may be expressed in terms of the Lieb functional. The equivalence between the information obtained from the two approaches is illustrated numerically by their implementation in a common framework.

  8. Time-dependent density-functional and reduced density-matrix methods for few electrons: Exact versus adiabatic approximations

    International Nuclear Information System (INIS)

    Helbig, N.; Fuks, J.I.; Tokatly, I.V.; Appel, H.; Gross, E.K.U.; Rubio, A.

    2011-01-01

    Graphical abstract: We solve a 1D N-electron system, with N small, by mapping it onto an N-dimensional one-electron problem. We compare the exact solutions to the results from adiabatic density and density matrix functionals for different physical situations. Highlights: ► Static and dynamical correlations. ► Memory dependence of exchange-correlation functionals in TDDFT. ► Linear and non-linear response. ► Laser-induced population control. - Abstract: To address the impact of electron correlations in the linear and non-linear response regimes of interacting many-electron systems exposed to time-dependent external fields, we study one-dimensional (1D) systems where the interacting problem is solved exactly by exploiting the mapping of the 1D N-electron problem onto an N-dimensional single electron problem. We analyze the performance of the recently derived 1D local density approximation as well as the exact-exchange orbital functional for those systems. We show that the interaction with an external resonant laser field shows Rabi oscillations which are detuned due to the lack of memory in adiabatic approximations. To investigate situations where static correlations play a role, we consider the time-evolution of the natural occupation numbers associated to the reduced one-body density matrix. Those studies shed light on the non-locality and time-dependence of the exchange and correlation functionals in time-dependent density and density-matrix functional theories.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  10. Blind polarization demultiplexing by constructing a cost function for coherent optical PDM-OFDM.

    Science.gov (United States)

    Yu, Zhenming; Chen, Minghua; Chen, Hongwei; Yi, Xingwen; Yang, Sigang; Xie, Shizhong

    2015-07-13

    We propose a training symbols-free polarization demultiplexing method by constructing a cost function (CCF-PDM) for coherent optical PDM-OFDM. This method is applicable for high-speed, wide-bandwidth OFDM signals, different subcarrier modulation formats and long-haul transmission. It shows comparable performance with that of conventional method but without overhead and converges fast. Since the neighboring subcarriers experience similar polarization effects, we set the initial matrix parameters by the neighboring subcarrier to reduce the number of iteration for the gradient algorithm and prevent swapping the data of the two orthogonal polarizations. We verify this method in experiment by transmitting 66.6-Gb/s PDM-OFDM signal with 4QAM subcarrier modulation over 5440 km SSMF and 133.3-Gb/s PDM-OFDM signal with 16QAM subcarrier modulation over 960 km SSMF respectively. We compare its performance with that of training symbols. We also analyze the convergence speed of this method.

  11. Ratiometric fluorescence polarization as a cytometric functional parameter: theory and practice

    Energy Technology Data Exchange (ETDEWEB)

    Yishai, Yitzhak; Fixler, Dror; Cohen-Kashi, Meir; Zurgil, Naomi; Deutsch, Mordechai [The Biophysical Interdisciplinary Jerome Schottenstein Center for the Research and the Technology of the Cellome, Department of Physics, Bar-Ilan University, Ramat-Gan 52900 (Israel)

    2003-08-07

    The use of ratiometric fluorescence polarization (RFP) as a functional parameter in monitoring cellular activation is suggested, based on the physical phenomenon of fluorescence polarization dependency on emission wavelengths in multiple (at least binary) solutions. The theoretical basis of this dependency is thoroughly discussed and examined via simulation. For simulation, aimed to imitate a fluorophore-stained cell, real values of the fluorescence spectrum and polarization of different single fluorophore solutions were used. The simulation as well as the experimentally obtained values of RFP indicated the high sensitivity of this measure. Finally, the RFP parameter was utilized as a cytometric measure in three exemplary cellular bioassays. In the first, the apoptotic effect of oxLDL in a human Jurkat FDA-stained T cell line was monitored by RFP. In the second, the interaction between cell surface membrane receptors of human T lymphocyte cells was monitored by RFP measurements as a complementary means to the fluorescence resonance energy transfer (FRET) technique. In the third bioassay, cellular thiol level of FDA- and CMFDA-labelled Jurkat T cells was monitored via RFP.

  12. Sound velocity variation as function of polarization state in Lead Zirconate Titanate (PZT) Ceramics

    International Nuclear Information System (INIS)

    Essolaani, W; Farhat, N

    2012-01-01

    There are several ultrasonic techniques to measure the sound velocity, for example, the pulse-echo method. In such method, the size of transducer used to measure the sound velocity must be in the same order of the sample size. If not, the incompatibility of sizes becomes an error source of the sound velocity measurement. In this work, the Laser Induced Pressure Pulse (LIPP) method is used as ultrasonic method. This method has been very useful for studying the spatial distribution of charges and polarization in dielectrics. We take advantage of the fact that the method allows the sound velocity measurement, to study its variation as function of polarization state in (PZT) ceramics. In a sample with a known thickness e, the sound velocity ν is deduced from the measurement of the transit time T. The sound velocity depends on the elastic constants which in turn they depend on poling conditions. Thus, the variation of the sound velocity is related to the direction and the amplitude of the polarization.

  13. Synthesis, characterization and density functional theory study of low cost hydrazone sensitizers

    KAUST Repository

    G. Al-Sehemi, A.

    2015-01-18

    © 2015 Chemical Society of Ethiopia The 2-{4-[2-benzylidenehydrazino]phenyl}ethylene-1,1,2-tricarbonitrile (System 1), 2-{4-[2-(1- naphthylmethylene)hydrazino]phenyl}ethylene-1,1,2-tricarbonitrile (System 2) and 2-{4-[2-(9-anthrylmethylene)- hydrazino]phenyl}ethylene-1,1,2-tricarbonitrile (System 3) were synthesized by direct tricyanovinylation of hydrazones. The bathochromic shift in absorption spectra has been observed by increasing the solvent polarity. The FTIR spectra of these new dyes exhibited three important absorption bands. The first band centered near 3260 cm-1 in System 1 while 3208 cm-1 and 3211 cm-1 in System 2 and System 3 for the vNH absorption, respectively. The second band is a sharp absorption band in the region of 2212-2209 cm-1, which was attributed to the cyano group absorption. The third is an absorption band in the region of 1611-1603 cm-1 ascribed for the C=N. Density functional theory (DFT) calculation of relative energies, relative enthalpies and free energies shows that E isomers are the most stable except System 3 in which the most stable is Z isomers. The conformational energy profile shows two maxima near (-90 and 90°) while three local minima observed at (-180, 0 and 180) for N1-N2-C1-C2 torsional angle. The highest occupied molecular orbitals (HOMOs) are localized on the whole molecules while lowest unoccupied molecular orbitals (LUMOs) are distributed on the tricarbonitrile.

  14. Density functional theory study of magnetic coupling in the Gd12O18 cluster.

    Science.gov (United States)

    Ning, Lixin; Zhang, Yongfan; Cui, Zhifeng; Trioni, Mario Italo; Brivio, Gian Paolo

    2008-12-25

    The magnetic properties of the Gd(12)O(18) cluster cut from the bulk Gd(2)O(3) crystal are investigated using the spin-polarized density functional theory within the broken-symmetry approach. Our work reveals that in the ground state of the cluster the antiferromagnetic coupling between adjacent Gd (4f(7)) spins is preferred energetically. This result is in contrast to a recent prediction made by Pedersen and Ojamae (Pedersen, H.; Ojamae, L. Nano Lett. 2006, 6, 2004) but is consistent with recent experimental observations. The optimized structures of the cluster in the lowest-energy broken-symmetry state and the highest-spin ferromagnetic state are almost identical. The latter state is 71.5 cm(-1) higher in energy than the former one, giving a value of about -0.24 cm(-1) for the magnetic coupling constant, which is comparable to that estimated from experiments on the bulk crystal. The relative energies of various 4f(7) spin patterns of the cluster are calculated, and certain characteristics of the cluster in the lowest-energy broken-symmetry state are discussed.

  15. Particle number and probability density functional theory and A-representability.

    Science.gov (United States)

    Pan, Xiao-Yin; Sahni, Viraht

    2010-04-28

    In Hohenberg-Kohn density functional theory, the energy E is expressed as a unique functional of the ground state density rho(r): E = E[rho] with the internal energy component F(HK)[rho] being universal. Knowledge of the functional F(HK)[rho] by itself, however, is insufficient to obtain the energy: the particle number N is primary. By emphasizing this primacy, the energy E is written as a nonuniversal functional of N and probability density p(r): E = E[N,p]. The set of functions p(r) satisfies the constraints of normalization to unity and non-negativity, exists for each N; N = 1, ..., infinity, and defines the probability density or p-space. A particle number N and probability density p(r) functional theory is constructed. Two examples for which the exact energy functionals E[N,p] are known are provided. The concept of A-representability is introduced, by which it is meant the set of functions Psi(p) that leads to probability densities p(r) obtained as the quantum-mechanical expectation of the probability density operator, and which satisfies the above constraints. We show that the set of functions p(r) of p-space is equivalent to the A-representable probability density set. We also show via the Harriman and Gilbert constructions that the A-representable and N-representable probability density p(r) sets are equivalent.

  16. Persistent organic pollutants, skull size and bone density of polar bears (Ursus maritimus) from East Greenland 1892-2015 and Svalbard 1964-2004.

    Science.gov (United States)

    Daugaard-Petersen, Tobias; Langebæk, Rikke; Rigét, Frank F; Letcher, Robert J; Hyldstrup, Lars; Jensen, Jens-Erik Bech; Bechshoft, Thea; Wiig, Øystein; Jenssen, Bjørn Munro; Pertoldi, Cino; Lorenzen, Eline D; Dietz, Rune; Sonne, Christian

    2018-04-01

    We investigated skull size (condylobasal length; CBL) and bone mineral density (BMD) in polar bears (Ursus maritimus) from East Greenland (n = 307) and Svalbard (n = 173) sampled during the period 1892-2015 in East Greenland and 1964-2004 at Svalbard. Adult males from East Greenland showed a continuous decrease in BMD from 1892 to 2015 (linear regression: p 0.05) nor was there any significant difference in BMD between Svalbard and East Greenland subpopulations. Skull size was larger in polar bears from Svalbard than from East Greenland (two-way ANOVA: p = 0.003). T-scores reflecting risk of osteoporosis showed that adult males from both East Greenland and Svalbard are at risk of developing osteopenia. Finally, when correcting for age and sex, BMD in East Greenland polar bears increased with increasing concentrations of persistent organic pollutants (POPs) i.e. ΣPCB (polychlorinated biphenyls), ΣHCH (hexachlorohexane), HCB (hexachlorobenzene) and ΣPBDE (polybrominated diphenyl ethers) while skull size increased with ΣHCH concentrations all in the period 1999-2014 (multiple linear regression: all p < 0.05, n = 175). The results suggest that environmental changes over time, including exposure to POPs, may affect bone density and size of polar bears. Copyright © 2017 Elsevier Inc. All rights reserved.

  17. Lee-Yang-inspired functional with a density-dependent neutron-neutron scattering length

    Science.gov (United States)

    Grasso, M.; Lacroix, D.; Yang, C. J.

    2017-05-01

    Inspired by the low-density Lee-Yang expansion for the energy of a dilute Fermi gas of density ρ and momentum kF, we introduce here a Skyrme-type functional that contains only s -wave terms and provides, at the mean-field level, (i) a satisfactory equation of state for neutron matter from extremely low densities up to densities close to the equilibrium point, and (ii) a good-quality equation of state for symmetric matter at density scales around the saturation point. This is achieved by using a density-dependent neutron-neutron scattering length a (ρ ) which satisfies the low-density limit (for Fermi momenta going to zero) and has a density dependence tuned in such a way that the low-density constraint |a (ρ ) kF|≤1 is satisfied at all density scales.

  18. Density functional study of ferromagnetism in alkali metal thin films

    Indian Academy of Sciences (India)

    Home; Journals; Pramana – Journal of Physics; Volume 74; Issue 4. Density ... Prasenjit Sen. Research Articles Volume 74 Issue 4 April 2010 pp 653-659 ... Only a six-layer Cs film is found to have a ferromagnetic (FM) state which is degenerate with a paramagnetic (PM) state within the accuracy of these calculations.

  19. A density functional theory-based chemical potential equalisation ...

    Indian Academy of Sciences (India)

    The electron density changes in molecular systems in the presence of external electric fields are modeled for simplicity in terms of the induced charges and dipole moments at the individual atomic sites. A chemical potential equalisation scheme is proposed for the calculation of these quantities and hence the dipole ...

  20. Two-dimensional carbon structures study within density functional theory

    Science.gov (United States)

    Sharin, Egor P.; Tihonov, Roman S.

    2017-11-01

    In this paper by means of ab initio, from the first principles, modeling, electronic properties of a monolayer and bilayer of graphene are studied. Calculations of electron density and band structure of these substances are carried out. For verification of obtained results, calculated values are compared with known experimental results from angle-resolved photoemission spectroscopy (ARPES).

  1. The functional response to prey density in an acarine system

    NARCIS (Netherlands)

    Fransz, H.G.

    1974-01-01

    Predacious mites are considered to be important natural enemies of phytophagous mites. Their efficiency in the natural control of prey populations depends on the relationships of the number of prey killed per predator per time unit and the oviposition rate on the one hand and prey density on the

  2. The QED vacuum polarization function at four loops and the anomalous magnetic moment at five loops

    International Nuclear Information System (INIS)

    Baikov, P.

    2013-07-01

    The anomalous moment of the muon is one of the most fundamental observables. It has been measured experimentally with a very high precision and on theory side the contributions from perturbative QED have been calculated up to five-loop level by numerical methods. Contributions to the muon anomalous magnetic moment from certain diagram classes are also accessible by alternative methods. In this paper we present the evaluation of contributions to the QCD corrections due to insertions of the vacuum polarization function at five-loop level.

  3. Density functional studies of functionalized graphitic materials with late transition metals for oxygen reduction reactions

    DEFF Research Database (Denmark)

    Vallejo, Federico Calle; Martinez, Jose Ignacio; Rossmeisl, Jan

    2011-01-01

    Reaction (OER). Spin analyses suggest that the oxidation state of those elements in the active sites should in general be +2. Moreover, our results verify that the adsorption behavior of transition metals is not intrinsic, since it can be severely altered by changes in the local geometry of the active site......) at the cathode. In this contribution, on the basis of Density Functional Theory (DFT) calculations, we show that graphitic materials with active sites composed of 4 nitrogen atoms and transition metal atoms belonging to groups 7 to 9 in the periodic table are active towards ORR, and also towards Oxygen Evolution...

  4. Performance of density functional theory methods to describe ...

    Indian Academy of Sciences (India)

    Fukui function shows a small dependence with both the exchange and correlation functional and the basis set. Evolution of the Fukui function along the reaction path describes important changes in the basic sites of the corresponding molecules. These results are in agreement with the chemical behavior of those species.

  5. Spin-Multiplet Components and Energy Splittings by Multistate Density Functional Theory.

    Science.gov (United States)

    Grofe, Adam; Chen, Xin; Liu, Wenjian; Gao, Jiali

    2017-10-05

    Kohn-Sham density functional theory has been tremendously successful in chemistry and physics. Yet, it is unable to describe the energy degeneracy of spin-multiplet components with any approximate functional. This work features two contributions. (1) We present a multistate density functional theory (MSDFT) to represent spin-multiplet components and to determine multiplet energies. MSDFT is a hybrid approach, taking advantage of both wave function theory and density functional theory. Thus, the wave functions, electron densities and energy density-functionals for ground and excited states and for different components are treated on the same footing. The method is illustrated on valence excitations of atoms and molecules. (2) Importantly, a key result is that for cases in which the high-spin components can be determined separately by Kohn-Sham density functional theory, the transition density functional in MSDFT (which describes electronic coupling) can be defined rigorously. The numerical results may be explored to design and optimize transition density functionals for configuration coupling in multiconfigurational DFT.

  6. HI column density distribution function at z=0 : Connection to damped Ly alpha statistics

    NARCIS (Netherlands)

    Zwaan, Martin; Verheijen, MAW; Briggs, FH

    We present a measurement of the HI column density distribution function f(N-HI) at the present epoch for column densities > 10(20) cm(-2). These high column densities compare to those measured in damped Ly alpha lines seen in absorption against background quasars. Although observationally rare, it

  7. Real photon spectral weight functions, imaginary part of vacuum polarization and electromagnetic vertices

    International Nuclear Information System (INIS)

    Chahine, C.; College de France, 75 - Paris. Lab. de Physique Corpusculaire)

    1978-02-01

    The concept of a real photon spectral weight function for any cross-section involving charged particles is introduced as a simple approximation taking into account the soft part of photon emission to all orders in perturbation theory. The spectral weight function replaces the energy-momentum conservation delta function in the elastic cross-section. The spectral weight function is computed in closed form in space-time and in the peaking approximation in momentum space. The spectral weight function description is applied to the imaginary part of vacuum polarization ImPI and to electron-proton scattering. A spectral representation for ImPI is derived and its content compared with the known fourth order result, showing in particular the identity of the soft and peaking approximations in lowest order. The virtual photon radiative corrections are discussed in part, with emphasis on the threshold behavior of the vertex functions. A relativistic generalization of the electric non-relativistic vertex function is given, whose asymptotic behavior is approppriate to use in conjuction with the spectral weight function

  8. PREFACE: Classical density functional theory methods in soft and hard matter Classical density functional theory methods in soft and hard matter

    Science.gov (United States)

    Haataja, Mikko; Gránásy, László; Löwen, Hartmut

    2010-08-01

    materials parameters such as crystal symmetry, lattice spacing, elastic constants, surface energies and stresses, dislocation core energy, and dislocation mobility, without sacrificing numerical efficiency. The issue of constructing PFC free energies, which give rise to a given crystal symmetry, has been addressed very recently; see, e.g., [17-19]. Going beyond the question of crystal symmetry, an appealing possibility is to further develop the so-called amplitude equation approach [75-77]., in which the density field is essentially expressed in terms of slowly-varying envelope functions (i.e., amplitudes), modulated by the fundamental spatial periodicity of the density. In fact, it has been demonstrated recently that such an approach provides a truly multi-scale approach to studying phase transformations in solid-liquid systems [78]. The goal is to construct amplitude equations, which accurately incorporate, e.g., surface tension anisotropies for simulations of solid-solid, solid-liquid, and solid-vapor systems. Alternatively, one can work directly with the PFC density field and introduce additional model parameters which can be fitted so that a required set of physical properties is recovered, such as the properties of the solid-liquid interface in pure iron [79]. (k) How to simulate electronic materials with PFC? Ferroelectrics comprise an interesting class of materials, which undergo a structural phase transformation (typically cubic-to-tetragonal) below a Curie temperature and acquire a non-zero electric polarization. It has been suggested that the manipulation of these polarization domains by means of an external field can be exploited in novel non-volatile memory devices [80, 81]. The PFC approach would present an appealing means to study ferroelectrics exhibiting one or more (ferroic) order parameters, provided that the crystal lattice can be coupled to the local order parameter(s) in a physically-based manner. 4. Concluding remarks The workshop 'Classical density

  9. The density functional study of electronic structure, electronic charge density, linear and nonlinear optical properties of single crystal alpha-LiAlTe{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Reshak, A.H. [New Technologies-Research Center, University of West Bohemia, Univerzitni 8, 306 14 Pilsen (Czech Republic); Center of Excellence Geopolymer and Green Technology, School of Material Engineering, University Malaysia Perlis, 01007 Kangar, Perlis (Malaysia); Khan, Wilayat, E-mail: walayat76@gmail.com [New Technologies-Research Center, University of West Bohemia, Univerzitni 8, 306 14 Pilsen (Czech Republic)

    2014-04-01

    Highlights: • FP-LAPW technique is used for calculating the electronic structure. • The band structure shows that the calculated compound is semiconductor. • The complex dielectric function has been calculated. • Nonlinear optical properties has also been calculated. • This compound can be used for molecular engineering of the crystals. - Abstract: Self-consistent calculations is performed using the full potential linear augmented plane wave (FP-LAPW) technique based on density functional theory (DFT) to investigate the electronic band structure, density of states, electronic charge density, linear and non-linear optical properties of α-LiAlTe{sub 2} compound having tetragonal symmetry with space group I4{sup ¯}2d. The electronic structure are calculated using the Ceperley Alder local density approach (CA-LDA), Perdew Burke and Ernzerhof generalize gradient approach (PBE-GGA), Engel–Vosko generalize gradient approach (EVGGA) and modified Becke Johnson approach (mBJ). Band structure calculations of (α-LiAlTe{sub 2}) depict semiconducting nature with direct band gap of 2.35 eV (LDA), 2.48 eV (GGA), 3.05 eV (EVGGA) and 3.13 eV (mBJ), which is comparable to experimental value. The calculated electronic charge density show ionic interaction between Te and Li atoms and polar covalent interaction between Al and Te atoms. Some optical susceptibilities like dielectric constants, refractive index, extension co-efficient, reflectivity and energy loss function have been calculated and analyzed on the basis of electronic structure. The compound α-LiAlTe{sub 2} provides a considerable negative value of birefringence of −0.01. Any anisotropy observed in the linear optical properties which are in favor to enhance the nonlinear optical properties. The symbol χ{sub abc}{sup (2)}(ω) represents the second order nonlinear optical susceptibilities, possess six non-zero components in this symmetry (tetragonal), called: 1 2 3, 2 1 3, 2 3 1, 1 3 2, 3 1 2 and 3 2 1

  10. Correlation Between Computed Tomography Density and Functional Status of the Thyroid Gland.

    Science.gov (United States)

    Pandey, Vivek; Reis, Martin; Zhou, Yihua

    2016-01-01

    This study aimed to determine the correlation between thyroid computed tomography (CT) density and thyroid functional status. Thyroid CT densities were determined in patients who had a noncontrast CT of the cervical spine and a recent thyroid-stimulating hormone (TSH) measurement in a cohort of 157 patients. Thyroid CT densities of patients with abnormally low TSH and high TSH were compared to those with normal TSH. A correlation analysis was performed to determine the correlation between TSH levels and CT densities. Both low and high TSH groups demonstrated significantly decreased thyroid CT densities (P thyroid CT densities and TSH levels (r = 0.40; P thyroid CT density and serum TSH levels. A low thyroid CT density indicates abnormal thyroid function.

  11. Local thermodynamic mapping for effective liquid density-functional theory

    Science.gov (United States)

    Kyrlidis, Agathagelos; Brown, Robert A.

    1992-01-01

    The structural-mapping approximation introduced by Lutsko and Baus (1990) in the generalized effective-liquid approximation is extended to include a local thermodynamic mapping based on a spatially dependent effective density for approximating the solid phase in terms of the uniform liquid. This latter approximation, called the local generalized effective-liquid approximation (LGELA) yields excellent predictions for the free energy of hard-sphere solids and for the conditions of coexistence of a hard-sphere fcc solid with a liquid. Moreover, the predicted free energy remains single valued for calculations with more loosely packed crystalline structures, such as the diamond lattice. The spatial dependence of the weighted density makes the LGELA useful in the study of inhomogeneous solids.

  12. A Density Functional Theory Study of New Boron Nanotubes

    Science.gov (United States)

    Chen, Zhao-Hua; Xie, Zun

    2017-11-01

    Using first-principles calculations, a series of new boron nanotubes (BNTs), which show various electronic properties, were theoretically predicted. Stable nanotubes with various chiral vectors and diameters can be formed by rolling up the boron sheet with relative stability [H. Tang and S. I. Beigi, Phys. Rev. B 82, 115412 (2010).]. By increasing the diameter for BNT, the stability is enhanced. The calculated density of states and band structures demonstrate that all the predicted BNTs are metallic, regardless of their diameter and chirality. The multicentre chemical bonds of the relatively stable boron sheet and BNTs are analysed using the deformation electron density. Within our study, the BNTs all have metallic conductive characteristics, in addition to having a low effective quality and high carrier concentration, which are very good nanoconductive material properties and could be combined to form high-power electrodes for lithium-ion batteries such as those used in many modern electronics.

  13. Accurate van der Waals coefficients from density functional theory

    Science.gov (United States)

    Tao, Jianmin; Perdew, John P.; Ruzsinszky, Adrienn

    2012-01-01

    The van der Waals interaction is a weak, long-range correlation, arising from quantum electronic charge fluctuations. This interaction affects many properties of materials. A simple and yet accurate estimate of this effect will facilitate computer simulation of complex molecular materials and drug design. Here we develop a fast approach for accurate evaluation of dynamic multipole polarizabilities and van der Waals (vdW) coefficients of all orders from the electron density and static multipole polarizabilities of each atom or other spherical object, without empirical fitting. Our dynamic polarizabilities (dipole, quadrupole, octupole, etc.) are exact in the zero- and high-frequency limits, and exact at all frequencies for a metallic sphere of uniform density. Our theory predicts dynamic multipole polarizabilities in excellent agreement with more expensive many-body methods, and yields therefrom vdW coefficients C6, C8, C10 for atom pairs with a mean absolute relative error of only 3%. PMID:22205765

  14. Many-Body Spectral Functions from Steady State Density Functional Theory.

    Science.gov (United States)

    Jacob, David; Kurth, Stefan

    2018-03-14

    We propose a scheme to extract the many-body spectral function of an interacting many-electron system from an equilibrium density functional theory (DFT) calculation. To this end we devise an ideal scanning tunneling microscope (STM) setup and employ the recently proposed steady-state DFT formalism (i-DFT) which allows one to calculate the steady current through a nanoscopic region coupled to two biased electrodes. In our setup, one of the electrodes serves as a probe ("STM tip"), which is weakly coupled to the system we want to measure. In the ideal STM limit of vanishing coupling to the tip, the system is restored to quasi-equilibrium and the normalized differential conductance yields the exact equilibrium many-body spectral function. Calculating this quantity from i-DFT, we derive an exact relation expressing the interacting spectral function in terms of the Kohn-Sham one. As illustrative examples, we apply our scheme to calculate the spectral functions of two nontrivial model systems, namely the single Anderson impurity model and the Constant Interaction Model.

  15. Density functional theory calculations on azobenzene derivatives: a comparative study of functional group effect.

    Science.gov (United States)

    Piyanzina, Irina; Minisini, Benoit; Tayurskii, Dmitrii; Bardeau, Jean-François

    2015-02-01

    Density functional theory (DFT) calculations have been used to investigate the structural properties, dipole moments, polarizabilities, Gibbs energies, hardness, electronegativity, HOMO/LUMO energies, and chemical potentials of trans and cis configurations of eight para-substituted azobenzene derivatives. All properties have been obtained using the B3LYP functional and 6-31++G(d,p) basis set. The planar structures have been obtained for all optimized trans configurations. The energy difference between trans and cis configurations for considered derivatives was found to be between 64.2-73.1 kJ/mole. It has been obtained that the p-aminodiazo-benzene (ADAB) has the difference in the dipole moments between trans and cis forms higher than for trans and cis azobenzene.

  16. Shifts of community composition and population density substantially affect ecosystem function despite invariant richness

    NARCIS (Netherlands)

    Spaak, Jurg W.; Baert, Jan M.; Baird, Donald J.; Eisenhauer, Nico; Maltby, Lorraine; Pomati, Francesco; Radchuk, Viktoriia; Rohr, Jason R.; Brink, van den Paul J.; Laender, De Frederik

    2017-01-01

    There has been considerable focus on the impacts of environmental change on ecosystem function arising from changes in species richness. However, environmental change may affect ecosystem function without affecting richness, most notably by affecting population densities and community

  17. Density functional theory for molecular and periodic systems using density fitting and continuous fast multipole method: Analytical gradients.

    Science.gov (United States)

    Łazarski, Roman; Burow, Asbjörn Manfred; Grajciar, Lukáš; Sierka, Marek

    2016-10-30

    A full implementation of analytical energy gradients for molecular and periodic systems is reported in the TURBOMOLE program package within the framework of Kohn-Sham density functional theory using Gaussian-type orbitals as basis functions. Its key component is a combination of density fitting (DF) approximation and continuous fast multipole method (CFMM) that allows for an efficient calculation of the Coulomb energy gradient. For exchange-correlation part the hierarchical numerical integration scheme (Burow and Sierka, Journal of Chemical Theory and Computation 2011, 7, 3097) is extended to energy gradients. Computational efficiency and asymptotic O(N) scaling behavior of the implementation is demonstrated for various molecular and periodic model systems, with the largest unit cell of hematite containing 640 atoms and 19,072 basis functions. The overall computational effort of energy gradient is comparable to that of the Kohn-Sham matrix formation. © 2016 Wiley Periodicals, Inc. © 2016 Wiley Periodicals, Inc.

  18. Chemical functionalization of graphene by carbene cycloaddition: A density functional theory study

    International Nuclear Information System (INIS)

    Zan, Wenyan

    2014-01-01

    Graphical abstract: - Highlights: • The reaction process of graphene functionalization with CCl 2 group in atomic scales was studied. • The potential candidate carbenes CR 2 (R = H, F, CN, NO 2 0 , NO 2 90 , CH 3 , OCH 3 , CCH, C 6 H 5 ) were separately combined with graphene. • The functionalization of graphene nanoribbon with dichlorocarbene group was investigated. • The electronic properties of graphene functionalized by carbene groups were discussed. - Abstract: In this work, we have systematically studied the structural, energetic and electronic properties of graphene functionalized with carbene groups by using density functional theory. Introducing a low concentration of CCl 2 group in graphene was studied in detail by DFT, and closed cyclopropane-like three-membered ring structure was formed, meanwhile, the potential candidate carbene groups CR 2 (R = H, F, CH 3 , CN, NO 2 , OCH 3 , CCH, C 6 H 5 ) were added to graphene sheet, and CR 2 (R = H, NO 2 , CH 3 ) groups were expected to be good reactive species to covalently modify graphene. The graphene functionalization with carbene groups above can open graphene's band gap. More CCl 2 molecules were added to graphene, and different concentrations of CCl 2 group can tune graphene's band gap. In addition, the addition of CCl 2 group to graphene edges was investigated, and the stronger binding energy was found. Multiple CCl 2 molecules preferred to be bound with the same edge of graphene nanoribbon. This work provides an insight into the detailed molecular mechanism of graphene functionalization with carbene groups

  19. The Precision Measurement of the Neutron Spin Structure Function Using Polarized HE-3 Target

    Energy Technology Data Exchange (ETDEWEB)

    Wang, X

    2004-01-05

    Using a 48.6 GeV polarized electron beam scattering off a polarized {sup 3}He target at Stanford Linear Accelerator Centre (SLAC), they measured the neutron spin structure function g{sub 1}{sup n} over kinematic(x) ranging 0.014 < x <0.7 and 1 < Q{sup 2} < 17GeV{sup 2}. The measurement gave the integral result over the neutron spin structure function {integral}{sub 0.014}{sup 0.7} g{sub 1}{sup n}(x)dx = -0.036 {+-} 0.004(stat) {+-} 0.005(syst) at an average Q{sup 2} = 5GeV{sup 2}. Along with the proton results from SLAC E143 experiment (0.03 < x) and SMC experiment (0.014 < x < 0.03), they find the Bjorken sum rule appears to be largely saturated by the data integrated down to x of 0.014. However, they observe relatively large values for g{sub 1}{sup n} at low x. The result calls into question the usual methods (Regge theory) for extrapolating to x = 0 to find the full neutron integral {integral}{sub 0}{sup t} g{sub 1}{sup n}(x) dx, needed for testing the Quark-Parton Model (QMP).

  20. Determination of the Bjorken Sum and Strong Coupling from Polarized Structure Functions

    CERN Document Server

    Altarelli, Guido; Forte, Stefano; Ridolfi, G; Altarelli, Guido; Ball, Richard D.; Forte, Stefano; Ridolfi, Giovanni

    1997-01-01

    We present a NLO perturbative analysis of all available data on the polarized structure function g_1(x,Q^2) with the aim of making a quantitative test of the validity of the Bjorken sum rule, of measuring \\alpha_s, and of deriving helicity fractions. We take particular care over the small x extrapolation, since it is now known that Regge behaviour is unreliable at perturbative scales. For fixed \\alpha_s we find that if all the most recent data are included g_A=1.18\\pm0.09, confirming the Bjorken sum rule at the 8% level. We further show that the value of \\alpha_s is now reasonably well constrained by scaling violations in the structure function data, despite the fact that it cannot yet be reliably fixed by the value of the Bjorken sum: our final result is \\alpha_s(m_Z) = 0.120+0.010-0.008. We also confirm earlier indications of a sizeable positive gluon polarization in the nucleon.

  1. Evolutionarily conserved sites in yeast tropomyosin function in cell polarity, transport and contractile ring formation

    Directory of Open Access Journals (Sweden)

    Susanne Cranz-Mileva

    2015-08-01

    Full Text Available Tropomyosin is a coiled-coil protein that binds and regulates actin filaments. The tropomyosin gene in Schizosaccharomyces pombe, cdc8, is required for formation of actin cables, contractile rings, and polar localization of actin patches. The roles of conserved residues were investigated in gene replacement mutants. The work validates an evolution-based approach to identify tropomyosin functions in living cells and sites of potential interactions with other proteins. A cdc8 mutant with near-normal actin affinity affects patch polarization and vacuole fusion, possibly by affecting Myo52p, a class V myosin, function. The presence of labile residual cell attachments suggests a delay in completion of cell division and redistribution of cell patches following cytokinesis. Another mutant with a mild phenotype is synthetic negative with GFP-fimbrin, inferring involvement of the mutated tropomyosin sites in interaction between the two proteins. Proteins that assemble in the contractile ring region before actin do so in a mutant cdc8 strain that cannot assemble condensed actin rings, yet some cells can divide. Of general significance, LifeAct-GFP negatively affects the actin cytoskeleton, indicating caution in its use as a biomarker for actin filaments.

  2. Energy expressions in density-functional theory using line integrals.

    NARCIS (Netherlands)

    van Leeuwen, R.; Baerends, E.J.

    1995-01-01

    In this paper we will address the question of how to obtain energies from functionals when only the functional derivative is given. It is shown that one can obtain explicit expressions for the exchange-correlation energy from approximate exchange-correlation potentials using line integrals along

  3. GPU Acceleration for Density Functional Theory with Slater-Type Orbitals

    NARCIS (Netherlands)

    van Schoot, H.; Visscher, L.; Walker, R.C.; Gotz, A.W.

    2016-01-01

    This chapter describes the graphics processing unit (GPU) acceleration of density functional theory (DFT) calculations with Slater-type orbital (STOs) as developed for the Amsterdam Density Functional (ADF) program. This implementation is focused on accelerating the numerical integration step in

  4. Gas physisorption studied with density functional theory: hysteresis and the Kelvin equation

    NARCIS (Netherlands)

    Gijzeman, O.L.J.; Roij, R. van

    2005-01-01

    We study nitrogen adsorption on oxidic surfaces within the framework of density functional theory. On the basis of a simple free energy functional, with which we calculate nitrogen density profiles and adsorption isotherms, we argue that some experimental hysteresis effects can directly be

  5. Element orbitals for Kohn-Sham density functional theory

    Energy Technology Data Exchange (ETDEWEB)

    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.

  6. Polarized atomic beams for targets

    International Nuclear Information System (INIS)

    Grueebler, W.

    1984-01-01

    The basic principle of the production of polarized atomic hydrogen and deuterium beams are reviewed. The status of the present available polarization, density and intensity are presented. The improvement of atomic beam density by cooling the hydrogen atoms to low velocity is discussed. The possible use of polarized atomic beams as targets in storage rings is shown. It is proposed that polarized atomic beams can be used to produce polarized gas targets with high polarization and greatly improved density

  7. Work function mediated by deposition of ultrathin polar FeO on Pt(111)

    Energy Technology Data Exchange (ETDEWEB)

    Lu, Shuangzan; Qin, Zhihui; Guo, Qinmin; Cao, Gengyu, E-mail: gycao@wipm.ac.cn

    2017-01-15

    Highlights: • Growth of FeO layers on Pt(111) is found to consecutively reduce the work function of the system. • The electrostatic compression effect and the structural relaxation make major contributions to the reductions. • Significant rectifying effect observed in the FeO layer is induced by band alignment shift as work function changing. - Abstract: Significant work function changes from bare Pt(111) surface to 1 monolayer and 2 monolayers of ultrathin iron oxide (FeO) films on it are investigated by means of scanning tunneling microscopy/spectroscopy (STM/STS). With FeO layer-by-layer growth, a continuous reduction of the work function along with the surface vacuum level (VL) shifting is observed. We found that the compression of the electron spill-out at the metal-oxide interface and the substantial reconstruction of 2 ML FeO film, respectively, make major contributions to the first and the second reductions of the work function. The rectifying effect in FeO films is also observed, which is attributed to the downward shift of band alignment imposed by the total change in surface dipole. Our work shows that the polar oxide films play an important role to adjust surface electronic structures for enhancing device functionality.

  8. Persistent organic pollutants and penile bone mineral density in East Greenland and Canadian polar bears (Ursus maritimus) during 1996-2015.

    Science.gov (United States)

    Daugaard-Petersen, Tobias; Langebæk, Rikke; Rigét, Frank F; Dyck, Markus; Letcher, Robert J; Hyldstrup, Lars; Jensen, Jens-Erik Bech; Dietz, Rune; Sonne, Christian

    2018-03-06

    Persistent organic pollutants (POPs) are long-range transported to the Arctic via atmospheric and oceanic currents, where they biomagnify to high concentrations in the tissues of apex predators such as polar bears (Ursus maritimus). A major concern of POP exposure is their physiological effects on vital organ-tissues posing a threat to the health and survival of polar bears. Here we examined the relationship between selected POPs and baculum bone mineral density (BMD) in the East Greenland and seven Canadian subpopulations of polar bears. BMD was examined in 471 bacula collected between years 1996-2015 while POP concentrations in adipose tissue were determined in 67-192 of these individuals collected from 1999 to -2015. A geographical comparison showed that baculum BMD was significantly lowest in polar bears from East Greenland (EG) when compared to Gulf of Boothia (GB), Southern Hudson (SH) and Western Hudson (WH) Bay subpopulations (all p bears as a reference group gave a T-score of -1.44 which indicate risk of osteopenia. Concentrations of ΣPCB 74 (polychlorinated biphenyls), ΣDDT 3 (dichlorodiphenyltrichloroethanes), p,p'-DDE (dichlorodiphenyldichloroethylene), ΣHCH 3 (hexachlorohexane) and α-HCH was significantly highest in EG bears while ΣPBDE (polybrominated diphenyl ethers), BDE-47 and BDE-153 was significantly highest in SH bears (all p polar bears despite the positive statistical correlations of BMD vs. POPs. Other important factors such as nutritional status, body mass and body condition was not available for the statistical modelling. Since on-going environmental changes are known to affect these, future studies need to incorporate nutritional, endocrine and genetic parameters to further understand how POP exposure may disrupt bone homeostasis and affect baculum BMD across polar bear subpopulations. Copyright © 2018 Elsevier Ltd. All rights reserved.

  9. On the accuracy of density functional theory and wave function methods for calculating vertical ionization energies

    Energy Technology Data Exchange (ETDEWEB)

    McKechnie, Scott [Cavendish Laboratory, Department of Physics, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE (United Kingdom); Booth, George H. [Theory and Simulation of Condensed Matter, King’s College London, The Strand, London WC2R 2LS (United Kingdom); Cohen, Aron J. [Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW (United Kingdom); Cole, Jacqueline M., E-mail: jmc61@cam.ac.uk [Cavendish Laboratory, Department of Physics, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE (United Kingdom); Argonne National Laboratory, 9700 S Cass Avenue, Argonne, Illinois 60439 (United States)

    2015-05-21

    The best practice in computational methods for determining vertical ionization energies (VIEs) is assessed, via reference to experimentally determined VIEs that are corroborated by highly accurate coupled-cluster calculations. These reference values are used to benchmark the performance of density functional theory (DFT) and wave function methods: Hartree-Fock theory, second-order Møller-Plesset perturbation theory, and Electron Propagator Theory (EPT). The core test set consists of 147 small molecules. An extended set of six larger molecules, from benzene to hexacene, is also considered to investigate the dependence of the results on molecule size. The closest agreement with experiment is found for ionization energies obtained from total energy difference calculations. In particular, DFT calculations using exchange-correlation functionals with either a large amount of exact exchange or long-range correction perform best. The results from these functionals are also the least sensitive to an increase in molecule size. In general, ionization energies calculated directly from the orbital energies of the neutral species are less accurate and more sensitive to an increase in molecule size. For the single-calculation approach, the EPT calculations are in closest agreement for both sets of molecules. For the orbital energies from DFT functionals, only those with long-range correction give quantitative agreement with dramatic failing for all other functionals considered. The results offer a practical hierarchy of approximations for the calculation of vertical ionization energies. In addition, the experimental and computational reference values can be used as a standardized set of benchmarks, against which other approximate methods can be compared.

  10. On the accuracy of density functional theory and wave function methods for calculating vertical ionization energies

    International Nuclear Information System (INIS)

    McKechnie, Scott; Booth, George H.; Cohen, Aron J.; Cole, Jacqueline M.

    2015-01-01

    The best practice in computational methods for determining vertical ionization energies (VIEs) is assessed, via reference to experimentally determined VIEs that are corroborated by highly accurate coupled-cluster calculations. These reference values are used to benchmark the performance of density functional theory (DFT) and wave function methods: Hartree-Fock theory, second-order Møller-Plesset perturbation theory, and Electron Propagator Theory (EPT). The core test set consists of 147 small molecules. An extended set of six larger molecules, from benzene to hexacene, is also considered to investigate the dependence of the results on molecule size. The closest agreement with experiment is found for ionization energies obtained from total energy difference calculations. In particular, DFT calculations using exchange-correlation functionals with either a large amount of exact exchange or long-range correction perform best. The results from these functionals are also the least sensitive to an increase in molecule size. In general, ionization energies calculated directly from the orbital energies of the neutral species are less accurate and more sensitive to an increase in molecule size. For the single-calculation approach, the EPT calculations are in closest agreement for both sets of molecules. For the orbital energies from DFT functionals, only those with long-range correction give quantitative agreement with dramatic failing for all other functionals considered. The results offer a practical hierarchy of approximations for the calculation of vertical ionization energies. In addition, the experimental and computational reference values can be used as a standardized set of benchmarks, against which other approximate methods can be compared

  11. Multiconfiguration pair-density functional theory: barrier heights and main group and transition metal energetics.

    Science.gov (United States)

    Carlson, Rebecca K; Li Manni, Giovanni; Sonnenberger, Andrew L; Truhlar, Donald G; Gagliardi, Laura

    2015-01-13

    Kohn-Sham density functional theory, resting on the representation of the electronic density and kinetic energy by a single Slater determinant, has revolutionized chemistry, but for open-shell systems, the Kohn-Sham Slater determinant has the wrong symmetry properties as compared to an accurate wave function. We have recently proposed a theory, called multiconfiguration pair-density functional theory (MC-PDFT), in which the electronic kinetic energy and classical Coulomb energy are calculated from a multiconfiguration wave function with the correct symmetry properties, and the rest of the energy is calculated from a density functional, called the on-top density functional, that depends on the density and the on-top pair density calculated from this wave function. We also proposed a simple way to approximate the on-top density functional by translation of Kohn-Sham exchange-correlation functionals. The method is much less expensive than other post-SCF methods for calculating the dynamical correlation energy starting with a multiconfiguration self-consistent-field wave function as the reference wave function, and initial tests of the theory were quite encouraging. Here, we provide a broader test of the theory by applying it to bond energies of main-group molecules and transition metal complexes, barrier heights and reaction energies for diverse chemical reactions, proton affinities, and the water dimerization energy. Averaged over 56 data points, the mean unsigned error is 3.2 kcal/mol for MC-PDFT, as compared to 6.9 kcal/mol for Kohn-Sham theory with a comparable density functional. MC-PDFT is more accurate on average than complete active space second-order perturbation theory (CASPT2) for main-group small-molecule bond energies, alkyl bond dissociation energies, transition-metal-ligand bond energies, proton affinities, and the water dimerization energy.

  12. Structural analysis of the antimalarial drug halofantrine by means of Raman spectroscopy and density functional theory calculations.

    Science.gov (United States)

    Frosch, Torsten; Popp, Jürgen

    2010-01-01

    The structure of the antimalarial drug halofantrine is analyzed by means of density functional theory (DFT) calculations, IR, and Raman spectroscopy. Strong, selective enhancements of the Raman bands of halofantrine at 1621 and 1590 cm(-1) are discovered by means of UV resonance Raman spectroscopy with excitation wavelength lambda(exc)=244 nm. These signal enhancements can be exploited for a localization of small concentrations of halofantrine in a biological environment. The Raman spectrum of halofantrine is calculated by means of DFT calculations [B3LYP/6-311+G(d,p)]. The calculation is very useful for a thorough mode assignment of the Raman bands of halofantrine. The strong bands at 1621 and 1590 cm(-1) in the UV Raman spectrum are assigned to combined C[Double Bond]C stretching vibrations in the phenanthrene ring of halofantrine. These bands are considered as putative marker bands for pipi interactions with the biological target molecules. The calculation of the electron density demonstrates a strong distribution across the phenanthrene ring of halofantrine, besides the electron withdrawing effect of the Cl and CF(3) substituents. This strong and even electron density distribution supports the hypothesis of pipi stacking as a possible mode of action of halofantrine. Complementary IR spectroscopy is performed for an investigation of vibrations of polar functional groups of the halofantrine molecule.

  13. Density-functional theory in one dimension for contact-interacting fermions

    International Nuclear Information System (INIS)

    Magyar, R.J.; Burke, K.

    2004-01-01

    A density-functional theory is developed for fermions in one dimension, interacting via a δ function. Such systems provide a natural testing ground for questions of principle, as the local-density approximation should be highly accurate since for this interaction type the exchange contribution to the local-density approximation is intrinsically self-interaction-free. The exact-exchange contribution to the total energy is a local functional of the density. A local-density approximation for correlation is obtained using perturbation theory and Bethe ansatz results for the one-dimensional contact-interacting uniform Fermi gas. The ground-state energies are calculated for two finite systems, the analogs of helium and of Hooke's atom. The local-density approximation is shown to be excellent as expected

  14. Avoiding self-repulsion in density functional description of biased molecular junctions

    International Nuclear Information System (INIS)

    Baer, Roi; Livshits, Ester; Neuhauser, Daniel

    2006-01-01

    We examine the effects of self-repulsion on the predictions of charge distribution in biased molecular junctions by the local density functional theory methods. This is done using a functional with explicit long-range exchange term effects [R. Baer, D. Neuhauser, Phys. Rev. Lett. 94 (2005) 043002]. We discuss in detail the new density functional, pointing out some of the remaining difficulties in the theory. We find that in weakly coupled junctions (the typical molecular electronics case) local-density functionals fail to describe correctly the charge distribution in the intermediate bias regime

  15. Osmosensation in vasopressin neurons: changing actin density to optimize function.

    Science.gov (United States)

    Prager-Khoutorsky, Masha; Bourque, Charles W

    2010-02-01

    The proportional relation between circulating vasopressin concentration and plasma osmolality is fundamental for body fluid homeostasis. Although changes in the sensitivity of this relation are associated with pathophysiological conditions, central mechanisms modulating osmoregulatory gain are unknown. Here, we review recent data that sheds important light on this process. The cell autonomous osmosensitivity of vasopressin neurons depends on cation channels comprising a variant of the transient receptor potential vanilloid 1 (TRPV1) channel. Hyperosmotic activation is mediated by a mechanical process where sensitivity increases in proportion with actin filament density. Moreover, angiotensin II amplifies osmotic activation by a rapid stimulation of actin polymerization, suggesting that neurotransmitter-induced changes in cytoskeletal organization in osmosensory neurons can mediate central changes in osmoregulatory gain. (c) 2009 Elsevier Ltd. All rights reserved.

  16. Obtaining Hartree-Fock and density functional theory doubly excited states with Car-Parrinello density matrix search

    Science.gov (United States)

    Liang, Wenkel; Isborn, Christine M.; Li, Xiaosong

    2009-11-01

    The calculation of doubly excited states is one of the major problems plaguing the modern day excited state workhorse methodology of linear response time dependent Hartree-Fock (TDHF) and density function theory (TDDFT). We have previously shown that the use of a resonantly tuned field within real-time TDHF and TDDFT is able to simultaneously excite both the α and β electrons to achieve the two-electron excited states of minimal basis H2 and HeH+ [C. M. Isborn and X. Li, J. Chem. Phys. 129, 204107 (2008)]. We now extend this method to many electron systems with the use of our Car-Parrinello density matrix search (CP-DMS) with a first-principles fictitious mass method for wave function optimization [X. Li, C. L. Moss, W. Liang, and Y. Feng, J. Chem. Phys. 130, 234115 (2009)]. Real-time TDHF/TDDFT is used during the application of the laser field perturbation, driving the electron density toward the doubly excited state. The CP-DMS method then converges the density to the nearest stationary state. We present these stationary state doubly excited state energies and properties at the HF and DFT levels for H2, HeH+, lithium hydride, ethylene, and butadiene.

  17. Quest for a universal density functional: the accuracy of density functionals across a broad spectrum of databases in chemistry and physics.

    Science.gov (United States)

    Peverati, Roberto; Truhlar, Donald G

    2014-03-13

    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 towards that goal and to measure our progress, we have developed-building on earlier work of 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 this 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 two 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.

  18. Density functional approximation for spin dependent quantum transport in magnetic nano structures

    International Nuclear Information System (INIS)

    Nyunt, Khine

    2009-01-01

    In quasi-classical theoretical framework, the transport of electrons and holes in semiconductor devices is treated with the Boltzmann transport equation or quantum-mechanical energy band theory - viz., the effective mass approximation and the random phase approximation. On the other hand, in the mesoscopic, nano electronic devices, for three- and lower- dimensional structures with nanometer scaling, the wave properties, spin, charge and the interactions between spin and charge of electrons are fully utilized, such as in artificial mini-Brillouin zones, quantum size effects, Coulomb blockade of single-electron tunneling and spin-polarized giant magnetoresistance tunneling. The complexity associated with the classical quantum-mechanical formalism in the study of transport in magnetic nano structures can be avoided by applying the so-called, Hohenberg-Kohns density functional theory. In particular, the N-electron problem is formulated as N one-electron equations where each electron interacts with all other electrons via an effective exchange-correlation potential. These interactions are augmented using the electron charge density. Plane wave sets and total energy pseudo-potential methods can be used self-consistently, to solve the Kohn-Sham one-electron equations. Because of the limitations of quasi-classical theory, it is more appropriate to treat the magneto-transport problem in nano structures by using quantum many-body theory. The starting point of the quantum transport theory is to take an external field as a perturbation for the many-particle system in equilibrium. This leads to a linear response and gives corresponding transport coefficients. One useful application of the Greens function techniques in quantum magneto-transport is to convert a homogeneous differential equation into an integral equation, viz., as in the time-dependent Schrodinger equation. We have applied to scattering of nano structural defects (impurities) in the electron gas (metal) as many

  19. Magnetic-Field Density-Functional Theory (BDFT): Lessons from the Adiabatic Connection.

    Science.gov (United States)

    Reimann, Sarah; Borgoo, Alex; Tellgren, Erik I; Teale, Andrew M; Helgaker, Trygve

    2017-09-12

    We study the effects of magnetic fields in the context of magnetic field density-functional theory (BDFT), where the energy is a functional of the electron density ρ and the magnetic field B. We show that this approach is a worthwhile alternative to current-density functional theory (CDFT) and may provide a viable route to the study of many magnetic phenomena using density-functional theory (DFT). The relationship between BDFT and CDFT is developed and clarified within the framework of the four-way correspondence of saddle functions and their convex and concave parents in convex analysis. By decomposing the energy into its Kohn-Sham components, we demonstrate that the magnetizability is mainly determined by those energy components that are related to the density. For existing density functional approximations, this implies that, for the magnetizability, improvements of the density will be more beneficial than introducing a magnetic-field dependence in the correlation functional. However, once a good charge density is achieved, we show that high accuracy is likely only obtainable by including magnetic-field dependence. We demonstrate that adiabatic-connection (AC) curves at different field strengths resemble one another closely provided each curve is calculated at the equilibrium geometry of that field strength. In contrast, if all AC curves are calculated at the equilibrium geometry of the field-free system, then the curves change strongly with increasing field strength due to the increasing importance of static correlation. This holds also for density functional approximations, for which we demonstrate that the main error encountered in the presence of a field is already present at zero field strength, indicating that density-functional approximations may be applied to systems in strong fields, without the need to treat additional static correlation.

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

    Directory of Open Access Journals (Sweden)

    L.B. Bhuiyan

    2012-06-01

    Full Text Available A recently proposed, local second contact value theorem [Henderson D., Boda D., J. Electroanal. Chem., 2005, Vol. 582, 16] for the charge profile of an electric double layer is used in conjunction with 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.

  1. Reconstructing Regional Ionospheric Electron Density: A Combined Spherical Slepian Function and Empirical Orthogonal Function Approach

    Science.gov (United States)

    Farzaneh, Saeed; Forootan, Ehsan

    2018-03-01

    The computerized ionospheric tomography is a method for imaging the Earth's ionosphere using a sounding technique and computing the slant total electron content (STEC) values from data of the global positioning system (GPS). The most common approach for ionospheric tomography is the voxel-based model, in which (1) the ionosphere is divided into voxels, (2) the STEC is then measured along (many) satellite signal paths, and finally (3) an inversion procedure is applied to reconstruct the electron density distribution of the ionosphere. In this study, a computationally efficient approach is introduced, which improves the inversion procedure of step 3. Our proposed method combines the empirical orthogonal function and the spherical Slepian base functions to describe the vertical and horizontal distribution of electron density, respectively. Thus, it can be applied on regional and global case studies. Numerical application is demonstrated using the ground-based GPS data over South America. Our results are validated against ionospheric tomography obtained from the constellation observing system for meteorology, ionosphere, and climate (COSMIC) observations and the global ionosphere map estimated by international centers, as well as by comparison with STEC derived from independent GPS stations. Using the proposed approach, we find that while using 30 GPS measurements in South America, one can achieve comparable accuracy with those from COSMIC data within the reported accuracy (1 × 1011 el/cm3) of the product. Comparisons with real observations of two GPS stations indicate an absolute difference is less than 2 TECU (where 1 total electron content unit, TECU, is 1016 electrons/m2).

  2. The adaptation of polar fishes to climatic changes: Structure, function and phylogeny of haemoglobin.

    Science.gov (United States)

    Verde, Cinzia; Giordano, Daniela; di Prisco, Guido

    2008-01-01

    In the Antarctic, fishes of dominant suborder Notothenioidei have evolved in a unique thermal scenario. Phylogenetically related taxa of the suborder live in a wide range of latitudes, in Antarctic, sub-Antarctic and temperate oceans. Consequently, they offer a remarkable opportunity to study the physiological and biochemical characters gained and, conversely, lost during their evolutionary history. The evolutionary perspective has also been pursued by comparative studies of some features of the heme protein devoted to O(2) transport in fish living in the other polar region, the Arctic. The two polar regions differ by age and isolation. Fish living in each habitat have undergone regional constraints and fit into different evolutionary histories. The aim of this contribution is to survey the current knowledge of molecular structure, functional features, phylogeny and adaptations of the haemoglobins of fish thriving in the Antarctic, sub-Antarctic and Arctic regions (with some excursions in the temperate latitudes), in search of insights into the convergent processes evolved in response to cooling. Current climate change may disturb adaptation, calling for strategies aimed at neutralising threats to biodiversity.

  3. The electron-propagator approach to conceptual density-functional ...

    Indian Academy of Sciences (India)

    Unknown

    (4), the external potential is fixed by identity of the molecular system and is thus treated as a parameter and not a variable. Equation (4) is an exact expres- sion for the ...... the virtual spin-orbitals, and {χp} is a set of ortho- normal basis functions. The expression for the third- order correction is more complicated. Because the.

  4. Abstract: Synthesis, structure and density functional theory (DFT ...

    Indian Academy of Sciences (India)

    Ruthenium Complexes of Chelating Amido-functionalized N-heterocyclic Carbene Ligands: Synthesis, Structure and DFT Studies. Sachin Kumar,† Anantha Narayanan,† Mitta Nageswar Rao,† Mobin M. Shaikh§ and Prasenjit Ghosh*,†. †Department of Chemistry and. §National Single Crystal X-ray Diffraction Facility,.

  5. Comparing lightning polarity and cloud microphysical properties over regions of high ground flash density in South Africa

    CSIR Research Space (South Africa)

    Simpson, LA

    2011-09-01

    Full Text Available This study aims to find a correlation between lightning polarity and microphysical properties of a storm cloud, for events where large amounts of lightning damage have occured and/or there has been a reported lightning-related fatality....

  6. Magnetic Exchange Couplings with Range-Separated Hybrid Density Functionals.

    Science.gov (United States)

    Peralta, Juan E; Melo, Juan I

    2010-06-08

    We investigate the effect of Hartree-Fock range-separation on the calculation of magnetic exchange couplings in a set of nine bimetallic transition-metal complexes containing 3d elements (V, Cr, Mn, and Cu). To this end, we have compared magnetic exchange couplings calculated as self-consistent energy differences using two global hybrid functionals, B3LYP (Becke 3-parameter exchange and Lee-Yang-Parr correlation) and PBEh (hybrid Perdew-Burke-Ernzerhof) with the short-range separated HSE (Heyd-Scuseria-Ernzerhof) and the long-range corrected LC-ωPBE. Our results show that, although there is no clear superiority of any of these functionals when compared with experimental data, the LC-ωPBE provides a better description of the magnetization on the metallic centers, yielding self-consistent solutions that mimic more closely a Heisenberg-like behavior.

  7. Density functional study of the electronic structure of dye-functionalized fullerenes and their model donor-acceptor complexes containing P3HT

    Energy Technology Data Exchange (ETDEWEB)

    Baruah, Tunna; Garnica, Amanda; Paggen, Marina; Basurto, Luis; Zope, Rajendra R. [Department of Physics, The University of Texas at El Paso, El Paso, Texas 79958 (United States)

    2016-04-14

    We study the electronic structure of C{sub 60} fullerenes functionalized with a thiophene-diketo-pyrrolopyrrole-thiophene based chromophore using density functional theory combined with large polarized basis sets. As the attached chromophore has electron donor character, the functionalization of the fullerene leads to a donor-acceptor (DA) system. We examine in detail the effect of the linker and the addition site on the electronic structure of the functionalized fullerenes. We further study the electronic structure of these DA complexes with a focus on the charge transfer excitations. Finally, we examine the interface of the functionalized fullerenes with the widely used poly(3-hexylthiophene-2,5-diyl) (P3HT) donor. Our results show that all functionalized fullerenes with an exception of the C{sub 60}-pyrrolidine [6,6], where the pyrrolidine is attached at a [6,6] site, have larger electron affinities relative to the pristine C{sub 60} fullerene. We also estimate the quasi-particle gap, lowest charge transfer excitation energy, and the exciton binding energies of the functionalized fullerene-P3MT model systems. Results show that the exciton binding energies in these model complexes are slightly smaller compared to a similarly prepared phenyl-C{sub 61}-butyric acid methyl ester (PCBM)-P3MT complex.

  8. Avoiding the 4-index transformation in one-body reduced density matrix functional calculations for separable functionals

    NARCIS (Netherlands)

    Giesbertz, K.J.H.

    2016-01-01

    One of the major computational bottlenecks in one-body reduced density matrix (1RDM) functional theory is the evaluation of approximate 1RDM functionals and their derivatives. The reason is that more advanced approximate functionals are almost exclusively defined in the natural orbital basis, so a

  9. Synthesis, characterization and density functional theory study of low cost hydrazone sensitizers

    Directory of Open Access Journals (Sweden)

    A. G. Al-Sehemi

    2015-01-01

    Full Text Available The 2-{4-[2-benzylidenehydrazino]phenyl}ethylene-1,1,2-tricarbonitrile (System 1, 2-{4-[2-(1-naphthylmethylenehydrazino]phenyl}ethylene-1,1,2-tricarbonitrile (System 2 and 2-{4-[2-(9-anthrylmethylene- hydrazino]phenyl}ethylene-1,1,2-tricarbonitrile (System 3 were synthesized by direct tricyanovinylation of hydrazones. The bathochromic shift in absorption spectra has been observed by increasing the solvent polarity. The FTIR spectra of these new dyes exhibited three important absorption bands. The first band centered near 3260 cm-1 in System 1 while 3208 cm-1 and 3211 cm-1 in System 2 and System 3 for the nNH absorption, respectively. The second band is a sharp absorption band in the region of 2212-2209 cm-1, which was attributed to the cyano group absorption. The third is an absorption band in the region of 1611-1603 cm-1 ascribed for the C=N. Density functional theory (DFT calculation of relative energies, relative enthalpies and free energies shows that E isomers are the most stable except System 3 in which the most stable is Z isomers. The conformational energy profile shows two maxima near (-90 and 90o while three local minima observed at (-180, 0 and 180 for N1-N2-C1-C2 torsional angle. The highest occupied molecular orbitals (HOMOs are localized on the whole molecules while lowest unoccupied molecular orbitals (LUMOs are distributed on the tricarbonitrile. DOI: http://dx.doi.org/10.4314/bcse.v29i1.13

  10. Multiconfiguration Pair-Density Functional Theory Is as Accurate as CASPT2 for Electronic Excitation.

    Science.gov (United States)

    Hoyer, Chad E; Ghosh, Soumen; Truhlar, Donald G; Gagliardi, Laura

    2016-02-04

    A correct description of electronically excited states is critical to the interpretation of visible-ultraviolet spectra, photochemical reactions, and excited-state charge-transfer processes in chemical systems. We have recently proposed a theory called multiconfiguration pair-density functional theory (MC-PDFT), which is based on a combination of multiconfiguration wave function theory and a new kind of density functional called an on-top density functional. Here, we show that MC-PDFT with a first-generation on-top density functional performs as well as CASPT2 for an organic chemistry database including valence, Rydberg, and charge-transfer excitations. The results are very encouraging for practical applications.

  11. Optimization of effective atom centered potentials for london dispersion forces in density functional theory.

    Science.gov (United States)

    von Lilienfeld, O Anatole; Tavernelli, Ivano; Rothlisberger, Ursula; Sebastiani, Daniel

    2004-10-08

    We add an effective atom-centered nonlocal term to the exchange-correlation potential in order to cure the lack of London dispersion forces in standard density functional theory. Calibration of this long-range correction is performed using density functional perturbation theory and an arbitrary reference. Without any prior assignment of types and structures of molecular fragments, our corrected generalized gradient approximation density functional theory calculations yield correct equilibrium geometries and dissociation energies of argon-argon, benzene-benzene, graphite-graphite, and argon-benzene complexes.

  12. U(1 )×SU (2 ) gauge invariance made simple for density functional approximations

    Science.gov (United States)

    Pittalis, S.; Vignale, G.; Eich, F. G.

    2017-07-01

    A semirelativistic density-functional theory that includes spin-orbit couplings and Zeeman fields on equal footing with the electromagnetic potentials, is an appealing framework to develop a unified first-principles computational approach for noncollinear magnetism, spintronics, orbitronics, and topological states. The basic variables of this theory include the paramagnetic current and the spin-current density, besides the particle and the spin density, and the corresponding exchange-correlation (xc) energy functional is invariant under local U (1 )×SU (2 ) gauge transformations. The xc-energy functional must be approximated to enable practical applications, but, contrary to the case of the standard density functional theory, finding simple approximations suited to deal with realistic atomistic inhomogeneities has been a long-standing challenge. Here we propose a way out of this impasse by showing that approximate gauge-invariant functionals can be easily generated from existing approximate functionals of ordinary density-functional theory by applying a simple minimal substitution on the kinetic energy density, which controls the short-range behavior of the exchange hole. Our proposal opens the way to the construction of approximate, yet nonempirical functionals, which do not assume weak inhomogeneity and therefore may have a wide range of applicability in atomic, molecular, and condensed matter physics.

  13. Optimizing conical intersections of solvated molecules: The combined spin-flip density functional theory/effective fragment potential method

    Science.gov (United States)

    Minezawa, Noriyuki; Gordon, Mark S.

    2012-07-01

    Solvent effects on a potential energy surface crossing are investigated by optimizing a conical intersection (CI) in solution. To this end, the analytic energy gradient has been derived and implemented for the collinear spin-flip density functional theory (SFDFT) combined with the effective fragment potential (EFP) solvent model. The new method is applied to the azomethane-water cluster and the chromophore of green fluorescent protein in aqueous solution. These applications illustrate not only dramatic changes in the CI geometries but also strong stabilization of the CI in a polar solvent. Furthermore, the CI geometries obtained by the hybrid SFDFT/EFP scheme reproduce those by the full SFDFT, indicating that the SFDFT/EFP method is an efficient and promising approach for understanding nonadiabatic processes in solution.

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

    Directory of Open Access Journals (Sweden)

    M. Schmidt

    2012-12-01

    Full Text Available 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 functional is laid out. Recent extensions, based on the Kierlik-Rosinberg scalar weight functions, to binary and ternary non-additive hard sphere mixtures are described.

  15. A classical density functional theory for the asymmetric restricted primitive model of ionic liquids

    Science.gov (United States)

    Lu, Hongduo; Nordholm, Sture; Woodward, Clifford E.; Forsman, Jan

    2018-05-01

    A new three-parameter (valency, ion size, and charge asymmetry) model, the asymmetric restricted primitive model (ARPM) of ionic liquids, has recently been proposed. Given that ionic liquids generally are composed of monovalent species, the ARPM effectively reduces to a two-parameter model. Monte Carlo (MC) simulations have demonstrated that the ARPM is able to reproduce key properties of room temperature ionic liquids (RTILs) in bulk and at charged surfaces. The relatively modest complexity of the model raises the possibility, which is explored here, that a classical density functional theory (DFT) could resolve its properties. This is relevant because it might generate great improvements in terms of both numerical efficiency and understanding in the continued research of RTILs and their applications. In this report, a DFT for rod-like molecules is proposed as an approximate theoretical tool for an ARPM fluid. Borrowing data on the ion pair fraction from a single bulk simulation, the ARPM is modelled as a mixture of dissociated ions and connected ion pairs. We have specifically studied an ARPM where the hard-sphere diameter is 5 Å, with the charge located 1 Å from the hard-sphere centre. We focus on fluid structure and electrochemical behaviour of this ARPM fluid, into which a model electrode is immersed. The latter is modelled as a perfect conductor, and surface polarization is handled by the method of image charges. Approximate methods, which were developed in an earlier study, to take image interactions into account, are also incorporated in the DFT. We make direct numerical comparisons between DFT predictions and corresponding simulation data. The DFT theory is implemented both in the normal mean field form with respect to the electrostatic interactions and in a correlated form based on hole formation by both steric repulsions and ion-ion Coulomb interactions. The results clearly show that ion-ion correlations play a very important role in the screening of

  16. A comparison model between density functional and wave function theories by means of the Löwdin partitioning technique.

    Science.gov (United States)

    Caballero, Marc; Moreira, Ibério de P R; Bofill, Josep Maria

    2013-05-07

    A comparison model is proposed based on the Löwdin partitioning technique to analyze the differences in the treatment of electron correlation by the wave function and density functional models. This comparison model provides a tool to understand the inherent structure of both theories and its discrepancies in terms of the subjacent mathematical structure and the necessary conditions for variationality required for the energy functional. Some numerical results on simple molecules are also reported revealing the known phenomenon of "overcorrelation" of density functional theory methods.

  17. Path integrals for electronic densities, reactivity indices, and localization functions in quantum systems.

    Science.gov (United States)

    Putz, Mihai V

    2009-11-10

    The density matrix theory, the ancestor of density functional theory, provides the immediate framework for Path Integral (PI) development, allowing the canonical density be extended for the many-electronic systems through the density functional closure relationship. Yet, the use of path integral formalism for electronic density prescription presents several advantages: assures the inner quantum mechanical description of the system by parameterized paths; averages the quantum fluctuations; behaves as the propagator for time-space evolution of quantum information; resembles Schrödinger equation; allows quantum statistical description of the system through partition function computing. In this framework, four levels of path integral formalism were presented: the Feynman quantum mechanical, the semiclassical, the Feynman-Kleinert effective classical, and the Fokker-Planck non-equilibrium ones. In each case the density matrix or/and the canonical density were rigorously defined and presented. The practical specializations for quantum free and harmonic motions, for statistical high and low temperature limits, the smearing justification for the Bohr's quantum stability postulate with the paradigmatic Hydrogen atomic excursion, along the quantum chemical calculation of semiclassical electronegativity and hardness, of chemical action and Mulliken electronegativity, as well as by the Markovian generalizations of Becke-Edgecombe electronic focalization functions - all advocate for the reliability of assuming PI formalism of quantum mechanics as a versatile one, suited for analytically and/or computationally modeling of a variety of fundamental physical and chemical reactivity concepts characterizing the (density driving) many-electronic systems.

  18. Density functional theory studies of screw dislocation core structures in bcc metals

    DEFF Research Database (Denmark)

    Frederiksen, Søren Lund; Jacobsen, Karsten Wedel

    2003-01-01

    The core structures of (I 11) screw dislocations in bee metals are studied using density functional theory in the local-density approximation. For Mo and Fe, direct calculations of the core structures show the cores to be symmetric with respect to 180degrees rotations around an axis perpendicular...

  19. Path Integrals for Electronic Densities, Reactivity Indices, and Localization Functions in Quantum Systems

    Directory of Open Access Journals (Sweden)

    Mihai V. Putz

    2009-11-01

    Full Text Available The density matrix theory, the ancestor of density functional theory, provides the immediate framework for Path Integral (PI development, allowing the canonical density be extended for the many-electronic systems through the density functional closure relationship. Yet, the use of path integral formalism for electronic density prescription presents several advantages: assures the inner quantum mechanical description of the system by parameterized paths; averages the quantum fluctuations; behaves as the propagator for time-space evolution of quantum information; resembles Schrödinger equation; allows quantum statistical description of the system through partition function computing. In this framework, four levels of path integral formalism were presented: the Feynman quantum mechanical, the semiclassical, the Feynman-Kleinert effective classical, and the Fokker-Planck non-equilibrium ones. In each case the density matrix or/and the canonical density were rigorously defined and presented. The practical specializations for quantum free and harmonic motions, for statistical high and low temperature limits, the smearing justification for the Bohr’s quantum stability postulate with the paradigmatic Hydrogen atomic excursion, along the quantum chemical calculation of semiclassical electronegativity and hardness, of chemical action and Mulliken electronegativity, as well as by the Markovian generalizations of Becke-Edgecombe electronic focalization functions – all advocate for the reliability of assuming PI formalism of quantum mechanics as a versatile one, suited for analytically and/or computationally modeling of a variety of fundamental physical and chemical reactivity concepts characterizing the (density driving many-electronic systems.

  20. Quantum master equation method based on the broken-symmetry time-dependent density functional theory: application to dynamic polarizability of open-shell molecular systems.

    Science.gov (United States)

    Kishi, Ryohei; Nakano, Masayoshi

    2011-04-21

    A novel method for the calculation of the dynamic polarizability (α) of open-shell molecular systems is developed based on the quantum master equation combined with the broken-symmetry (BS) time-dependent density functional theory within the Tamm-Dancoff approximation, referred to as the BS-DFTQME method. We investigate the dynamic α density distribution obtained from BS-DFTQME calculations in order to analyze the spatial contributions of electrons to the field-induced polarization and clarify the contributions of the frontier orbital pair to α and its density. To demonstrate the performance of this method, we examine the real part of dynamic α of singlet 1,3-dipole systems having a variety of diradical characters (y). The frequency dispersion of α, in particular in the resonant region, is shown to strongly depend on the exchange-correlation functional as well as on the diradical character. Under sufficiently off-resonant condition, the dynamic α is found to decrease with increasing y and/or the fraction of Hartree-Fock exchange in the exchange-correlation functional, which enhances the spin polarization, due to the decrease in the delocalization effects of π-diradical electrons in the frontier orbital pair. The BS-DFTQME method with the BHandHLYP exchange-correlation functional also turns out to semiquantitatively reproduce the α spectra calculated by a strongly correlated ab initio molecular orbital method, i.e., the spin-unrestricted coupled-cluster singles and doubles.

  1. Introduction to Density Functional Theory: Calculations by Hand on the Helium Atom

    Science.gov (United States)

    Baseden, Kyle A.; Tye, Jesse W.

    2014-01-01

    Density functional theory (DFT) is a type of electronic structure calculation that has rapidly gained popularity. In this article, we provide a step-by-step demonstration of a DFT calculation by hand on the helium atom using Slater's X-Alpha exchange functional on a single Gaussian-type orbital to represent the atomic wave function. This DFT…

  2. Density-functional calculation of van der Waals forces for free-electron-like surfaces

    DEFF Research Database (Denmark)

    Hult, E.; Hyldgaard, P.; Rossmeisl, Jan

    2001-01-01

    A recently proposed general density functional for asymptotic van der Waals forces is used to calculate van der Waals coefficients and reference-plane positions for realistic low-indexed Al surfaces. Results are given for a number of atoms and molecules outside the surfaces, as well as for the in......A recently proposed general density functional for asymptotic van der Waals forces is used to calculate van der Waals coefficients and reference-plane positions for realistic low-indexed Al surfaces. Results are given for a number of atoms and molecules outside the surfaces, as well...... as for the interaction between the surfaces themselves. The densities and static image-plane positions that are needed as input in the van der Waals functional are calculated self-consistently within density-functional theory using the generalized-gradient approximation, pseudopotentials, and plane waves. This study...

  3. Time-dependent density functional theory for multi-component systems

    International Nuclear Information System (INIS)

    Tiecheng Li; Peiqing Tong

    1985-10-01

    The Runge-Gross version of Hohenberg-Kohn-Sham's density functional theory is generalized to multi-component systems, both for arbitrary time-dependent pure states and for arbitrary time-dependent ensembles. (author)

  4. Density Functional Theory Applied to Pt and Pt Alloy Clusters and Adsorbate

    National Research Council Canada - National Science Library

    Smotkin, Eugine

    2001-01-01

    ...). Using this advanced and powerful multiprocessor SGI server, we were able to dramatically speed and further advance our computational Density Functional calculations on CO absorbed on Pt and alloy clusters...

  5. Ionization Potentials of Chemical Warfare Agents and Related Compounds Determined with Density Functional Theory

    National Research Council Canada - National Science Library

    Wright, J

    2000-01-01

    ...) agents at contaminated sites. Reported herein are theoretical ionization potentials for CW agents and their related compounds calculated using density functional theory at the B3LYP/6-311+G(2d,p) level of theory...

  6. New AB Initio Based Density Functional Methods for Molecules, Polymers, and Crystals

    National Research Council Canada - National Science Library

    Bartlett, Rodney

    2000-01-01

    My efforts in the Density Functional Theory (DFT) project of Dr. Bartlett's research group have been limited to the implementation of analytical energy gradients with respect to nuclear displacement in ACES2...

  7. Object performance as a function of pileup density for CMS PhaseII

    CERN Document Server

    CMS Collaboration

    2017-01-01

    This document collects the performance of physics objects (electrons, muons, taus, jets, MET) reconstructed with the CMS Phase-2 upgraded detector as a function of the pileup density for the High Luminosity LHC environment of 200 PU.

  8. QSAR and density functional approaches to evaluate trichothecene toxicity and detection

    Science.gov (United States)

    Occasionally, agricultural commodities are contaminated with molds capable of producing structurally related trichothecene metabolites at levels associated with food safety risks. A comprehensive study on 34 trichothecene mycotoxins and biosynthetic precursors was conducted using density functional ...

  9. Pressure and surface tension of soild-liquid interface using Tarazona density functional theory

    Directory of Open Access Journals (Sweden)

    M. M.

    2000-12-01

    Full Text Available   The weighted density functional theory proposed by Tarazona is applied to study the solid-liquid interface. In the last two decades the weighted density functional became a useful tool to consider the properties of inhomogeneous liquids. In this theory, the role of the size of molecules or the particles of which the matter is composed, was found to be important. In this resarch we study a hard sphere fluid beside a hard wall. For this study the liquid is an inhomogeneous system. We use the definition of the direct correlation function as a second derivative of free energy with respect to the density. We use this definition and the definition of the weighting function, then we minimize the grand potential with respect to the density to get the Euler Lagrange equation and we obtain an integral equation to find the inhomogeneous density profile. The obtained density profile as a function of the distance from the wall, for different bulk density is plotted in three dimensions. We also calculate the pressure and compare it with the Carnahan-starling results, and finally we obtained the surface tension at liquid-solid interface and compared it with the results of Monte Carlo simulation.

  10. Structures, vibrational absorption and vibrational circular dichroism spectra of L-alanine in aqueous solution: a density functional theory and RHF study

    DEFF Research Database (Denmark)

    Frimand, Kenneth; Bohr, Henrik; Jalkanen, Karl J.

    2000-01-01

    A detailed comparative study of structures, vibrational absorption (VA) and vibrational circular dichroism (VCD) spectra has been carried out for the zwitterionic structure of the amino acid L-alanine. Theoretically determined structures necessary for deriving VA and VCD spectra were calculated...... at the density functional theory level using the B3LYP functional with the 6-31G* basis set. The Hessians and atomic polar tensors and atomic axial tensors were all calculated at the B3LYP/6-31G* level of theory. An important result is the method of treating solvent effects by both adding explicit water...

  11. Population alignment collisional radiative model for helium-like carbon. Polarization of emission lines and anisotropy of the electron velocity distribution function in plasmas

    International Nuclear Information System (INIS)

    Iwamae, Atsushi; Fujimoto, Takashi; Zhang, Honglin; Kilcrease, David P.; Csanak, George; Berrington, Keith A.

    2003-08-01

    The polarization of emission lines from a plasma carries information about the anisotropic velocity distribution of electrons in the plasma, and thus polarization spectroscopy can give information that is inaccessible by other methods. We have developed a comprehensive population-alignment collisional-radiative (PACR) model code for helium-like carbon CV ions. This code is intended to correlate quantitatively the observed polarization of emission lines from the ions in a plasma with the anisotropy of the electron velocity distribution function. Specifically, the longitudinal alignment of CV triplet emission lines for the 1s2s 3 S 1 - 1s2p 3 P 1,2 ) transitions are studied by this PACR model. The predominant process which produces alignment in the 1s2p 3 P 1,2 levels is the alignment production from the ground state, 1s 21 S 1 and from the metastable level, 1s2s 3 S 1 . The alignment-production fluxes from these levels are in the opposite directions in the temperature range of practical interest, depending on the electron density n e . When n e > 10 16 m -3 , the alignment-production flux from the metastable level is larger than that from the ground state. An anisotropic electron velocity distribution function that has higher values in the axial (toroidal) direction than in the radial (poloidal) direction produces negative longitudinal alignment of the emission lines, i.e., higher intensity of the linear polarized component in the radial direction than that in the axial direction. (author)

  12. Accurate Semilocal Density Functional for Condensed-Matter Physics and Quantum Chemistry.

    Science.gov (United States)

    Tao, Jianmin; Mo, Yuxiang

    2016-08-12

    Most density functionals have been developed by imposing the known exact constraints on the exchange-correlation energy, or by a fit to a set of properties of selected systems, or by both. However, accurate modeling of the conventional exchange hole presents a great challenge, due to the delocalization of the hole. Making use of the property that the hole can be made localized under a general coordinate transformation, here we derive an exchange hole from the density matrix expansion, while the correlation part is obtained by imposing the low-density limit constraint. From the hole, a semilocal exchange-correlation functional is calculated. Our comprehensive test shows that this functional can achieve remarkable accuracy for diverse properties of molecules, solids, and solid surfaces, substantially improving upon the nonempirical functionals proposed in recent years. Accurate semilocal functionals based on their associated holes are physically appealing and practically useful for developing nonlocal functionals.

  13. Assessment of density-functional approximations: Long-range correlations and self-interaction effects

    International Nuclear Information System (INIS)

    Jung, J.; Alvarellos, J.E.; Garcia-Gonzalez, P.; Godby, R.W.

    2004-01-01

    The complex nature of electron-electron correlations is made manifest in the very simple but nontrivial problem of two electrons confined within a sphere. The description of highly nonlocal correlation and self-interaction effects by widely used local and semilocal exchange-correlation energy density functionals is shown to be unsatisfactory in most cases. Even the best such functionals exhibit significant errors in the Kohn-Sham potentials and density profiles

  14. DNA-functionalized gold nanoparticle-based fluorescence polarization for the sensitive detection of silver ions.

    Science.gov (United States)

    Wang, Gongke; Wang, Shuangli; Yan, Changling; Bai, Guangyue; Liu, Yufang

    2018-04-05

    Despite their practical applications, Ag + ions are environmental pollutants and affect human health. So the effective detection methods of Ag + ions are imperative. Herein, we developed a simple, sensitive, selective, and cost-effective fluorescence polarization sensor for Ag + detection in aqueous solution using thiol-DNA-functionalized gold nanoparticles (AuNPs). In this sensing strategy, Ag + ions can specifically interact with a cytosine-cytosine (CC) mismatch in DNA duplexes and form stable metal-mediated cytosine-Ag + -cytosine (C-Ag + -C) base pairs. The formation of the C-Ag + -C complex results in evident changes in the molecular volume and fluorescence polarization signal. To achieve our aims, we prepared two complementary DNA strands containing C-base mismatches (probe A: 5'-SH-A 10 -TACCACTCCTCAC-3' and probe B: 5'-TCCTCACCAGTCCTA-FAM-3'). The stable hybridization between probe A and probe B occurs with the formation of the C-Ag + -C complex in the presence of Ag + ions, leading to obvious fluorescence quenching in comparison to the system without AuNP enhancement. The assay can be used to identify nanomolar levels of Ag + within 6 min at room temperature, and has extremely high specificity for Ag + , even in the presence of higher concentrations of interfering metal ions. Furthermore, the sensor was successfully applied to the detection of Ag + ions in environmental water samples and showed excellent selectivity and high sensitivity, implying its promising application in the future. Copyright © 2018 Elsevier B.V. All rights reserved.

  15. Electron mobility in supercritical pentanes as a function of density and temperature

    International Nuclear Information System (INIS)

    Itoh, Kengo; Nakagawa, Kazumichi; Nishikawa, Masaru

    1988-01-01

    The excess electron mobility in supercritical n-, iso- and neopentane was measured isothermally as a function of density. The density-normalized mobility μN in all three isomers goes through a minimum at a density below the respective critical densities, and the mobility is quite temperature-dependent in this region, then goes through a minimum. The μN behavior around the minimum in n-pentane is well accounted for by the Cohen-Lekner model with the structure factor S(K) estimated from the speed of sound, while that in iso- and neopentane is not. (author)

  16. Extending pairing energy density functional using pairing rotational moments of inertia

    Science.gov (United States)

    Hinohara, Nobuo

    2018-02-01

    The pairing energy density functionals (EDFs) that include the spatial derivative and kinetic terms of the pair densities are discussed. The coupling constants of the pairing EDF are adjusted to reproduce the experimental pairing rotational moment of inertia, and the pair-density derivative terms are shown to systematically improve the values of the pairing rotational moments of inertia in Sn and Pb isotopes. It is pointed out that the conventional average pairing gaps overestimate the experimental odd–even mass staggering in the presence of the pair-density derivative terms.

  17. Theoretical investigations into spectral and non-linear optical properties of brucine and strychnine using density functional theory

    Science.gov (United States)

    Islam, Nasarul; Niaz, Saba; Manzoor, Taniya; Pandith, Altaf Hussain

    2014-10-01

    The density functional theoretical (DFT) computations were performed at the B3LYP/6-311G++(d, p) level to calculate the equilibrium geometry, vibrational wave numbers, intensities, and various other molecular properties of brucine and strychnine, which were found in satisfactory agreement with the experimental data. The out-of-phase stretching modes of aromatic rings and carbonyl stretching modes in combination with CH stretching modes at stereogenic centers generate VCD signals, which are remarkably efficient configuration markers for these chiral molecular systems. NBOs analysis reveals that the large values of second order perturbation energy (47.24 kcal/mol for brucine and 46.93 kcal/mol for strychnine) confirms strong hyperconjugative interaction between the orbital containing the lone pair of electron of nitrogen and the neighboring Cdbnd O antibonding orbital. The molecular electrostatic potential map of strychnine molecule, with no polar groups other than the lone keto group, shows less polarization, which accounts for its lower susceptibility towards electrophilic attack as compared to brucine.

  18. Interpolative Separable Density Fitting Decomposition for Accelerating Hybrid Density Functional Calculations with Applications to Defects in Silicon.

    Science.gov (United States)

    Hu, Wei; Lin, Lin; Yang, Chao

    2017-11-14

    We present a new efficient way to perform hybrid density functional theory (DFT)-based electronic structure calculations. The new method uses an interpolative separable density fitting (ISDF) procedure to construct a set of numerical auxiliary basis vectors and a compact approximation of the matrix consisting of products of occupied orbitals represented in a large basis set such as the planewave basis. Such an approximation allows us to reduce the number of Poisson solves from [Formula: see text] to [Formula: see text] when we apply the exchange operator to occupied orbitals in an iterative method for solving the Kohn-Sham equations, where N e is the number of electrons in the system to be studied. We show that the ISDF procedure can be carried out in [Formula: see text] operations, with a much smaller preconstant compared to methods used in existing approaches. When combined with the recently developed adaptively compressed exchange (ACE) operator formalism, which reduces the number of times the exchange operator needs to be updated, the resulting ACE-ISDF method significantly reduces the computational cost associated with the exchange operator by nearly 2 orders of magnitude compared to existing approaches for a large silicon system with 1000 atoms. We demonstrate that the ACE-ISDF method can produce accurate energies and forces for insulating and metallic systems and that it is possible to obtain converged hybrid functional calculation results for a 1000-atom bulk silicon within 10 min on 2000 computational cores. We also show that ACE-ISDF can scale to 8192 computational cores for a 4096-atom bulk silicon system. We use the ACE-ISDF method to geometrically optimize a 1000-atom silicon system with a vacancy defect using the HSE06 functional and computes its electronic structure. We find that that the computed energy gap from the HSE06 functional is much closer to the experimental value compared to that produced by semilocal functionals in the DFT calculations.

  19. Ground-state properties of third-row elements with nonlocal density functionals

    International Nuclear Information System (INIS)

    Bagno, P.; Jepsen, O.; Gunnarsson, O.

    1989-01-01

    The cohesive energy, the lattice parameter, and the bulk modulus of third-row elements are calculated using the Langreth-Mehl-Hu (LMH), the Perdew-Wang (PW), and the gradient expansion functionals. The PW functional is found to give somewhat better results than the LMH functional and both are found to typically remove half the errors in the local-spin-density (LSD) approximation, while the gradient expansion gives worse results than the local-density approximation. For Fe both the LMH and PW functionals correctly predict a ferromagnetic bcc ground state, while the LSD approximation and the gradient expansion predict a nonmagnetic fcc ground state

  20. Thermodynamics of technetium: reconciling theory and experiment using density functional perturbation analysis.

    Science.gov (United States)

    Weck, Philippe F; Kim, Eunja

    2015-07-28

    The structure, lattice dynamics and thermodynamic properties of bulk technetium were investigated within the framework of density functional theory. The phonon density of states spectrum computed with density functional perturbation theory closely matches inelastic coherent neutron scattering measurements. The thermal properties of technetium were derived from phonon frequencies calculated within the quasi-harmonic approximation (QHA), which introduces a volume dependence of phonon frequencies as a part of the anharmonic effect. The predicted thermal expansion and isobaric heat capacity of technetium are in excellent agreement with available experimental data for temperatures up to ∼1600 K.