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Sample records for hartree-fock interaction parametrisation

  1. A study of self-consistent Hartree-Fock plus Bardeen-Cooper-Schrieffer calculations with finite-range interactions

    Science.gov (United States)

    Anguiano, M.; Lallena, A. M.; Co', G.; De Donno, V.

    2014-02-01

    In this work we test the validity of a Hartree-Fock plus Bardeen-Cooper-Schrieffer model in which a finite-range interaction is used in the two steps of the calculation by comparing the results obtained to those found in fully self-consistent Hartree-Fock-Bogoliubov calculations using the same interaction. Specifically, we consider the Gogny-type D1S and D1M forces. We study a wide range of spherical nuclei, far from the stability line, in various regions of the nuclear chart, from oxygen to tin isotopes. We calculate various quantities related to the ground state properties of these nuclei, such as binding energies, radii, charge and density distributions, and elastic electron scattering cross sections. The pairing effects are studied by direct comparison with the Hartree-Fock results. Despite its relative simplicity, in most cases, our model provides results very close to those of the Hartree-Fock-Bogoliubov calculations, and it reproduces the empirical evidence of pairing effects rather well in the nuclei investigated.

  2. Decomposition of the configuration-interaction coefficients in the multiconfiguration time-dependent Hartree-Fock method

    Energy Technology Data Exchange (ETDEWEB)

    Lötstedt, Erik, E-mail: lotstedt@chem.s.u-tokyo.ac.jp; Kato, Tsuyoshi; Yamanouchi, Kaoru [Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033 (Japan)

    2016-04-21

    An approximate implementation of the multiconfiguration time-dependent Hartree-Fock method is proposed, in which the matrix of configuration-interaction coefficients is decomposed into a product of matrices of smaller dimension. The applicability of this method in which all the configurations are kept in the expansion of the wave function, while the configuration-interaction coefficients are approximately calculated, is discussed by showing the results on three model systems: a one-dimensional model of a beryllium atom, a one-dimensional model of a carbon atom, and a one-dimensional model of a chain of four hydrogen atoms. The time-dependent electronic dynamics induced by a few-cycle, long-wavelength laser pulse is found to be well described at a lower computational cost compared to the standard multiconfiguration time-dependent Hartree-Fock treatment. Drawbacks of the method are also discussed.

  3. Brueckner-Hartree-Fock study of circular quantum dots

    Science.gov (United States)

    Emperador, A.; Lipparini, E.; Serra, Ll.

    2006-06-01

    We calculate ground state energies in the Brueckner-Hartree-Fock theory for N electrons (with N⩽20 ) confined to a circular quantum dot and in presence of a static magnetic field. Comparison with the predictions of Hartree-Fock, local-spin-density and exact configuration-interaction theories is made. We find that the correlations taken into account in Brueckner-Hartree-Fock calculations give an important contribution to the ground state energies, especially in strongly confined dots. In this high-density range, corresponding in practice to self-assembled quantum dots, the results of Brueckner-Hartree-Fock calculations are close to the exact values and better than those obtained in the local-spin-density approximation.

  4. An analysis of angular-momentum-projected Hartree-Fock-Bogoliubov wave functions in terms of interacting bosons

    Science.gov (United States)

    Pannert, W.; Ring, P.; Gambhir, Y. K.

    1985-09-01

    Angular-momentum- and number-projected Hartree-Fock-Bogoliubov (HFB) wave functions of translational and deformed rare earth nuclei are analyzed in terms of fermion pairs coupled to angular momenta L = 0 (S), 2 (D), 4 (G),/3. The fermion space is truncated to contain only S-D or S-D-G pairs. The variation is carried out before and after angular momentum projection and also with different truncations. The influence of the truncation on physical quantities such as moments of inertia, quadrupole moments or pair transfer matrix elements is discussed.

  5. A Fortran 90 program to solve the Hartree-Fock equations for interacting spin- 1/2 > fermions confined in harmonic potentials

    Science.gov (United States)

    Pal, Hridis Kumar; Shukla, Alok

    2008-08-01

    A set of weakly interacting spin- 1/2 > Fermions, confined by a harmonic oscillator potential, and interacting with each other via a contact potential, is a model system which closely represents the physics of a dilute gas of two-component fermionic atoms confined in a magneto-optic trap. In the present work, our aim is to present a Fortran 90 computer program which, using a basis set expansion technique, solves the Hartree-Fock (HF) equations for spin- 1/2 > Fermions confined by a three-dimensional harmonic oscillator potential, and interacting with each other via pair-wise delta-function potentials. Additionally, the program can also account for those anharmonic potentials which can be expressed as a polynomial in the position operators x, y, and z. Both the restricted-HF (RHF), and the unrestricted-HF (UHF) equations can be solved for a given number of Fermions, with either repulsive or attractive interactions among them. The option of UHF solutions for such systems also allows us to study possible magnetic properties of the physics of two-component confined atomic Fermi gases, with imbalanced populations. Using our code we also demonstrate that such a system exhibits shell structure, and follows Hund's rule. Program summaryProgram title: trap.x Catalogue identifier: AEBB_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEBB_v1_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.html No. of lines in distributed program, including test data, etc.: 17 750 No. of bytes in distributed program, including test data, etc.: 205 138 Distribution format: tar.gz Programming language: mostly Fortran 90 Computer: PCs—SUN, HP Alpha, IBM Operating system: Linux, Solaris, Tru64, AIX Classification: 7.7 Nature of problem: The simplest description of a spin 1/2 >; trapped system at the mean field level is given by the Hartree-Fock method. This

  6. Analysis of the half-projected Hartree--Fock function: density matrix, natural orbitals, and configuration interaction equivalence

    Energy Technology Data Exchange (ETDEWEB)

    Smeyers, Y.G.; Delgado-Barrio, G.

    1976-05-01

    The half-projected Hartree--Fock function for singlet states (HPHF) is analyzed in terms of natural electronic configurations. For this purpose the HPHF spinless density matrix and its natural orbitals are first deduced. It is found that the HPHF function does not contain any contribution from odd-times excited configurations. It is seen in addition, in the case of the singlet ground states, this function is approximately equivalent to two closed-shell configurations, although the nature of the excited one depends on the nuclear geometry. An example is given in the case of the LiH ground state. Finally, the application of this model for studying systems of more than two atoms is criticized.

  7. Combining density functional and incremental post-Hartree-Fock approaches for van der Waals dominated adsorbate-surface interactions: Ag{sub 2}/graphene

    Energy Technology Data Exchange (ETDEWEB)

    Lara-Castells, María Pilar de, E-mail: Pilar.deLara.Castells@csic.es [Instituto de Física Fundamental (C.S.I.C.), Serrano 123, E-28006 Madrid (Spain); Mitrushchenkov, Alexander O. [Université Paris-Est, Laboratoire Modélisation et Simulation Multi Echelle, MSME UMR 8208 CNRS, 5 bd Descartes, 77454 Marne-la-Vallée (France); Stoll, Hermann [Institut für Theoretische Chemie, Universität Stuttgart, D-70550 Stuttgart (Germany)

    2015-09-14

    A combined density functional (DFT) and incremental post-Hartree-Fock (post-HF) approach, proven earlier to calculate He-surface potential energy surfaces [de Lara-Castells et al., J. Chem. Phys. 141, 151102 (2014)], is applied to describe the van der Waals dominated Ag{sub 2}/graphene interaction. It extends the dispersionless density functional theory developed by Pernal et al. [Phys. Rev. Lett. 103, 263201 (2009)] by including periodic boundary conditions while the dispersion is parametrized via the method of increments [H. Stoll, J. Chem. Phys. 97, 8449 (1992)]. Starting with the elementary cluster unit of the target surface (benzene), continuing through the realistic cluster model (coronene), and ending with the periodic model of the extended system, modern ab initio methodologies for intermolecular interactions as well as state-of-the-art van der Waals-corrected density functional-based approaches are put together both to assess the accuracy of the composite scheme and to better characterize the Ag{sub 2}/graphene interaction. The present work illustrates how the combination of DFT and post-HF perspectives may be efficient to design simple and reliable ab initio-based schemes in extended systems for surface science applications.

  8. The Calculation of Single-Nucleon Energies of Nuclei by Considering Two-Body Effective Interaction, n(k,ρ, and a Hartree-Fock Inspired Scheme

    Directory of Open Access Journals (Sweden)

    H. Mariji

    2016-01-01

    Full Text Available The nucleon single-particle energies (SPEs of the selected nuclei, that is, O16, Ca40, and Ni56, are obtained by using the diagonal matrix elements of two-body effective interaction, which generated through the lowest-order constrained variational (LOCV calculations for the symmetric nuclear matter with the Aυ18 phenomenological nucleon-nucleon potential. The SPEs at the major levels of nuclei are calculated by employing a Hartree-Fock inspired scheme in the spherical harmonic oscillator basis. In the scheme, the correlation influences are taken into account by imposing the nucleon effective mass factor on the radial wave functions of the major levels. Replacing the density-dependent one-body momentum distribution functions of nucleons, n(k,ρ, with the Heaviside functions, the role of n(k,ρ in the nucleon SPEs at the major levels of the selected closed shell nuclei is investigated. The best fit of spin-orbit splitting is taken into account when correcting the major levels of the nuclei by using the parameterized Wood-Saxon potential and the Aυ18 density-dependent mean field potential which is constructed by the LOCV method. Considering the point-like protons in the spherical Coulomb potential well, the single-proton energies are corrected. The results show the importance of including n(k,ρ, instead of the Heaviside functions, in the calculation of nucleon SPEs at the different levels, particularly the valence levels, of the closed shell nuclei.

  9. Prospects for Brueckner-Hartree-Fock calculations in the Density Matrix Expansion approach

    Science.gov (United States)

    Zhang, Yinu; Dyhdalo, Alex; Bogner, Scott; Furnstahl, Richard

    2017-09-01

    Recently, a microscopically based nuclear energy density functional was derived by applying the Density Matrix Expansion (DME) to the Hartree-Fock energy obtained from chiral effective field theory (χEFT) two- and three-nucleon interactions. The Hartree-Fock approach cannot contain the full many-body correlations. Brueckner-Hartree-Fock (BHF) theory gives an improved definition of the one-body potential U by replacing the interaction by a reaction matrix G. The central result of modern renormalization theory is that a general RG decoupling generates an infinite series of counterterms consistent with the input interaction. Then we can apply the DME at Hartree-Fock level with long-range χEFT interactions and zero-range contact interactions to model BHF correlations. This work was supported in part by the National Science Foundation under Grant No. PHY-1614460 and the NUCLEI SciDAC Collaboration under Department of Energy Grant DE-SC0008533.

  10. Hartree-Fock description of spin systems

    Energy Technology Data Exchange (ETDEWEB)

    Hirsch, J.G.; Castanos, O.; Lopez P, R.; Jimenez F, O. [Instituto de Ciencias Nucleares, Universidad Nacional Autonoma de Mexico, Apartado Postal 70-543 Mexico 04510 D.F. (Mexico); Lopez M, E. [Departamento de Fisica, Facultad de Ciencias, Universidad Nacional Autonoma de Mexico, Apartado Postal 70-542 Mexico 04510 D.F. (Mexico)]. e-mail: hirsch@nucleares.unam.mx

    2007-12-15

    A mean-field treatment of a general spin Hamiltonian containing linear and quadratic terms is presented. The equivalence between atomic coherent states and Hartree-Fock states is explicitly demonstrated. The relevance of symmetry restoration is exhibited. Entanglement properties at the different phases are briefly discussed. (Author)

  11. Hartree-Fock theory for the equilibrium shape of light nuclei; Theorie Hartree-Fock de la forme d'equilibre des noyaux legers

    Energy Technology Data Exchange (ETDEWEB)

    Ripka, G. [Commissariat a l' Energie Atomique, 91 - Saclay (France). Centre d' Etudes Nucleaires

    1968-09-01

    Most of the content of this thesis is published in english in Advances In Nuclear Physics, Vol. 1 (Editors: Baranger and Vogt - Plenum Press). The Hartree- Fock equations are derived. The expansions of the orbits and the possible symmetries of the Hartree-Fock field are discussed. Wavefunctions of even-even N = Z nuclei are given for 12 {<=} A {<=} 40. The role of the monopole, quadrupole and exchange components of the force are discussed. The multiplicity of the solutions and the effect of the spin-orbit interaction are discussed. Exact angular momentum projection is used to generate rotational bands. The validity of the adiabatic rotational model in light nuclei is discussed. Hartree-Fock calculations are extended to include major-shell mixing in order to obtain quadrupole deformations without the use of effective charge. The incompressibility, of nuclei is discussed and the compatibility between the Hartree-Fock solutions, the Mottelson model of quadrupole deformations and the SU3 states of J.P. Elliott and M. Moshinsky is established. (author) [French] La theorie de Hartree-Fock est appliquee au calcul des fonctions d'onde des noyaux legers deformes. Les equations de Hartree-Fock, les symetries permises et le choix du developpement des orbites sont discutes. Les fonctions d'onde des noyaux pair-pairs N = Z (12 {<=} A {<=} 40) sont tabulees. Les contributions des composantes monopolaires et quadrupolaires ainsi que des termes d'echange de la force nucleon-nucleon sont discutees. La methode de projection de moment cinetique est utilisee pour engendrer les bandes de rotation. La validite du modele rotationnel adiabatique est discutee. Les calculs de Hartree-Fock qui tiennent compte du melange de plusieurs couches majeures dans chaque orbite sont appliques au calcul des deformations quadrupolaires sans l'utilisation de charge effective. L'incompressibilite des noyaux et la compatibilite des fonctions d'onde de Hartree- Fock avec les

  12. Molecular symmetry. IV. The coupled perturbed Hartree-Fock method

    Energy Technology Data Exchange (ETDEWEB)

    Takada, T.; Dupuis, M.; King, H.F.

    1983-01-01

    Symmetry methods employed in the ab initio polyatomic program HONDO are extended to the coupled perturbed Hartree-Fock (CPHF) formalism, a key step in the analytical computation of energy first derivatives for configuration interaction (CI) wave functions, and energy second derivatives for Hartree-Fock (HF) wave functions. One possible computational strategy is to construct Fock-Like matrices for each nuclear coordinate in which the one- and two-electron integrals of the usual Fock matrix are replaced by the integral first derivatives. Skeleton matrices are constructed from the unique blocks of electron-repulsion integral derivatives. The correct matrices are generated by applying a symmetrization operator. The analysis is valid for many wave functions, including closed- or open-shell spin-restricted and spin-unrestricted HF wave functions. To illustrate the method, the computer time required for setting up the coupled perturbed HF equations for eclipsed ethane using D/sub 3h/ symmetry point group and various subgroups of D/sub 3h/ are compared. Computational times are roughly inversely proportional to the order of the point group. 10 references, 1 table.

  13. Existence of minimizers in restricted Hartree-Fock theory

    Directory of Open Access Journals (Sweden)

    Fabian Hantsch

    2014-02-01

    Full Text Available In this note we establish the existence of ground states for atoms within several restricted Hartree-Fock theories. It is shown, for example, that there exists a ground state for closed shell atoms with N electrons and nuclear charge $Z \\geq N-1$. This has to be compared with the general Hartree-Fock theory where the existence of a minimizer is known for $Z >N-1$ only.

  14. Using finite element method to tackle the hartree-fock equations

    Energy Technology Data Exchange (ETDEWEB)

    Fau, Amelie; Aubry, Denis [MSSMat Laboratory, Ecole Centrale Paris (France)

    2011-07-01

    It is well know that the Schroedinger equation cannot be solved exactly, except maybe for very simple cases, as it represents a many-body interaction problem. However, it is possible to derive approximations of the Schroedinger equation from variational principles. The Hartree-Fock equations are then generally solved thanks to a set of basis functions, e.g. Gaussians, Slater-type orbitals or plane waves. To avoid to impose a general form to the approximate wave function, we use localized trial functions. We consider here the Finite Element Method as a new approach to solve these Hartree-Fock equations. We shall present the main properties of our computations with the different advantages and drawbacks involved by this strategy. We present numerical results about different electronic systems: such as atoms or molecules (LiH, BeH{sub 2}).

  15. Effect of Coulomb interactions and Hartree-Fock exchange on structural, elastic, optoelectronic and magnetic properties of Co{sub 2}MnSi Heusler: A comparative study

    Energy Technology Data Exchange (ETDEWEB)

    Lantri, T. [Laboratory of Technology and Solid’s Properties, Faculty of Sciences and Technology, Abdelhamid Ibn Badis University, BP 227, Mostaganem 27000 (Algeria); Bentata, S., E-mail: sam_bentata@yahoo.com [Laboratory of Technology and Solid’s Properties, Faculty of Sciences and Technology, Abdelhamid Ibn Badis University, BP 227, Mostaganem 27000 (Algeria); Bouadjemi, B.; Benstaali, W. [Laboratory of Technology and Solid’s Properties, Faculty of Sciences and Technology, Abdelhamid Ibn Badis University, BP 227, Mostaganem 27000 (Algeria); Bouhafs, B. [Modelling and Simulation in Materials Science Laboratory, Djillali Liabès University of Sidi Bel-Abbès, 22000 Sidi Bel-Abbes (Algeria); Abbad, A. [Laboratory of Technology and Solid’s Properties, Faculty of Sciences and Technology, Abdelhamid Ibn Badis University, BP 227, Mostaganem 27000 (Algeria); Modelling and Simulation in Materials Science Laboratory, Djillali Liabès University of Sidi Bel-Abbès, 22000 Sidi Bel-Abbes (Algeria); Zitouni, A. [Laboratory of Technology and Solid’s Properties, Faculty of Sciences and Technology, Abdelhamid Ibn Badis University, BP 227, Mostaganem 27000 (Algeria)

    2016-12-01

    Using the first-principle calculations, we have investigated the structural, elastic, optoelectronic and magnetic properties of Co{sub 2}MnSi Heusler alloy. Based on the density functional theory (DFT) and hiring the full-potential linearized augmented plane wave (FP-LAPW) method, we have used five approaches: the Hybrid on-site exact exchange, the Local Spin Density Approximation (LSDA), the LSDA+U, the Generalized Gradient Approximation GGA and GGA+U; where the Hubbard on-site Coulomb interaction correction U is calculated by constraint local density approximation for Co and Mn atoms. Our results show that the highly-ordered Co{sub 2}MnSi alloy is a ductile, stiff and anisotropic material. It has a half-metallic ferromagnetic character with an integer magnetic moment of 5 µB which is in good agreement with the Slater-Pauling rule. - Highlights: • Each approach gives a half magnetic compound. • EECE gives the largest gap. • Elastic properties show a stiff, ductile and anisotropic material. • Electronic properties are similar for the five approaches. • Total magnetic moment is the same for the five approaches (5 µB).

  16. Scaled hydrogenic approximation wavefunctions. [Hartree-Fock approximation

    Energy Technology Data Exchange (ETDEWEB)

    Shore, B.W.

    1979-09-01

    Although widespread use of computer codes for the solution of Schrodinger equations makes available numerical Hartree-Fock model radial wave functions, there remains persistant interest in simple analytic expressions for atomic wave functions. One such frequency favored approach employs hydrogenic functions, suitably scaled, as approximate wave functions. The following note displays typical inaccuracies to be expected from such approximations. 13 references.

  17. Unrestricted Hartree-Fock theory of Wigner crystals

    OpenAIRE

    Trail, J. R.; Towler, M. D.; Needs, R. J.

    2009-01-01

    We demonstrate that unrestricted Hartree-Fock theory applied to electrons in a uniform potential has stable Wigner crystal solutions for $r_s \\geq 1.44$ in two dimensions and $r_s \\geq 4.5$ in three dimensions. The correlation energies of the Wigner crystal phases are considerably smaller than those of the fluid phases at the same density.

  18. Improved coupled perturbed Hartree Fock and Kohn Sham convergence acceleration

    Science.gov (United States)

    Weber, Valéry; Daul, Claude

    2003-03-01

    A derivative version of the well-known direct inversion in the iterative subspace (DIIS) algorithm is presented. The method is used to solve the coupled perturbed Hartree-Fock (CPHF) equation to obtain the first and second derivatives of the density matrix with respect to an external electric field which, in this case, leads to the electric molecular polarizability and hyperpolarizability. Some comparisons are presented and the method shows good convergences in almost all cases.

  19. Core polarization effects in the Hartree--Fock--random phase approximation schemes

    Energy Technology Data Exchange (ETDEWEB)

    Lipparini, E.; Stringari, S.

    1987-02-01

    Core polarization effects in odd nuclei are investigated in the framework of the Hartree--Fock and random phase approximation schemes. The results of the particle vibration coupling model are recovered by linearizing the equations of motion in the interaction Hamiltonian between the external and the core particles. The formalism is used to study the renormalization of diagonal and off-diagonal M1 matrix elements. It is found that M1 polarization effects exhibit a very strong dependence on the range of the force. Copyright 1987 Academic Press, Inc.

  20. Further explorations of Skyrme-Hartree-Fock-Bogoliubov mass formulas. V. Extension to fission barriers

    Science.gov (United States)

    Samyn, M.; Goriely, S.; Pearson, J. M.

    2005-10-01

    Large-scale fission barrier calculations have been performed in the framework of the Skyrme-Hartree-Fock model. Our Hartree-Fock-Bogoliubov calculations restore broken symmetries such as translational invariance, particle-number conservation, parity, and, in a more approximate way, rotational invariance. Axial symmetry is imposed, but reflection asymmetry is allowed. The energy surface properties are analyzed with the flooding method. A large set of Skyrme interactions, which were fitted to all known masses under different specific constraints, is used to study the main effects influencing the energy surface and the barrier heights. The principal interaction used in the comparison with experimental barriers is BSk8, the force on which the HFB-8 mass table is based. We found that for nuclei with 92≤Z≤98 the agreement of our calculations with experimental data is excellent; the rms deviation on the primary barriers is 0.722 MeV. For lighter nuclei, however, the calculated primary barriers are always too high because of the existence of a third barrier at very high deformations. However, our calculated superheavy barriers appear to be too low, although they are consistent with previous calculations.

  1. Solution of the Skyrme-Hartree-Fock equations in the Cartesian deformed harmonic oscillator basis. (I) the method

    Energy Technology Data Exchange (ETDEWEB)

    Dobaczewski, J.; Dudek, J. [Strasbourg-1 Univ., 67 (France). Centre de Recherches Nucleaires; Dobaczewski, J. [Warsaw Univ. (Poland)

    1996-12-31

    We describe a method of solving the nuclear Skyrme-Hartree-Fock problem by using a deformed Cartesian harmonic oscillator basis. The complete list of expressions required to calculate local densities, total energy, and self-consistent fields is presented, and an implementation of the self-consistent symmetries is discussed. Formulas to calculate matrix elements in the Cartesian harmonic oscillator basis are derived for the nuclear and Coulomb interactions. (authors). 39 refs.

  2. Self-coherent Hartree-Fock theory and the microscopic symmetries of the nucleus; Theorie autocoherente de Hartree-Fock et les symetries microscopiques du noyau

    Energy Technology Data Exchange (ETDEWEB)

    Bouguettoucha, A.

    1996-06-14

    A possible effects of the C{sub 4}-symmetry in the superdeformed nuclei of the A {approx}150 mass range has been studied microscopically using cranking Strutinsky method with the deformed Woods-Saxon potential and the Hartree-Fock approach with the Skyrme interaction. If the existence of such a symmetry is judged by the moments Q{sub 44}, the results of the calculation indicate a very weak effect of this kind. Four new superdeformed bands in the {sup 148}Gd nucleus have been studied in reaction to the recent experimental observations (Eurogam Phase 2): a backbending has been tentatively observed at very high rotational frequency in the third excited band. One of the other bands exhibits a J{sup (2)} moment very similar to that of the yrast band in {sup 152}Dy, and this is the first example of identical bands which differ by four mass units. Calculations with the methods mentioned above have been used to analyse the band structure in terms of the nucleonic configurations. Calculation have been performed for some nuclear configurations predicted to involve the exotic octupole deformations (Y{sub 30-}`pear shapes`; Y{sub 31-}`banana mode`; Y{sub 32-}`T{sub d}-symmetry` and Y{sub 33-}`C{sub 3}-symmetry`). While the previous calculations based on the Strutinsky method could not treat the coupling between those modes, the Hartree-Fock approach allows to see for the first time in which propositions the various modes couple. (author). 116 refs.

  3. Computational Nuclear Physics and Post Hartree-Fock Methods

    Energy Technology Data Exchange (ETDEWEB)

    Lietz, Justin [Michigan State University; Sam, Novario [Michigan State University; Hjorth-Jensen, M. [University of Oslo, Norway; Hagen, Gaute [ORNL; Jansen, Gustav R. [ORNL

    2017-05-01

    We present a computational approach to infinite nuclear matter employing Hartree-Fock theory, many-body perturbation theory and coupled cluster theory. These lectures are closely linked with those of chapters 9, 10 and 11 and serve as input for the correlation functions employed in Monte Carlo calculations in chapter 9, the in-medium similarity renormalization group theory of dense fermionic systems of chapter 10 and the Green's function approach in chapter 11. We provide extensive code examples and benchmark calculations, allowing thereby an eventual reader to start writing her/his own codes. We start with an object-oriented serial code and end with discussions on strategies for porting the code to present and planned high-performance computing facilities.

  4. The Gogny-Hartree-Fock-Bogoliubov nuclear-mass model

    Energy Technology Data Exchange (ETDEWEB)

    Goriely, S. [Universite Libre de Bruxelles, Institut d' Astronomie et d' Astrophysique, CP-226, Brussels (Belgium); Hilaire, S.; Girod, M.; Peru, S. [CEA, DAM, DIF, Arpajon (France)

    2016-07-15

    We present the Gogny-Hartree-Fock-Bogoliubov model which reproduces nuclear masses with an accuracy comparable with the best mass formulas. In contrast to the Skyrme-HFB nuclear-mass models, an explicit and self-consistent account of all the quadrupole correlation energies is included within the 5D collective Hamiltonian approach. The final rms deviation with respect to the 2353 measured masses is 789 keV in the 2012 atomic mass evaluation. In addition, the D1M Gogny force is shown to predict nuclear and neutron matter properties in agreement with microscopic calculations based on realistic two- and three-body forces. The D1M properties and its predictions of various observables are compared with those of D1S and D1N. (orig.)

  5. Spin-projected generalized Hartree-Fock method as a polynomial of particle-hole excitations

    Science.gov (United States)

    Henderson, Thomas M.; Scuseria, Gustavo E.

    2017-08-01

    The past several years have seen renewed interest in the use of symmetry-projected Hartree-Fock for the description of strong correlations. Unfortunately, these symmetry-projected mean-field methods do not adequately account for dynamic correlation. Presumably, this shortcoming could be addressed if one could combine symmetry-projected Hartree-Fock with a many-body method such as coupled-cluster theory, but this is by no means straightforward because the two techniques are formulated in very different ways. However, we have recently shown that the singlet S2-projected unrestricted Hartree-Fock wave function can in fact be written in a coupled-cluster-like wave function. That is, the spin-projected unrestricted Hartree-Fock wave function can be written as a polynomial of a double-excitation operator acting on some closed-shell reference determinant. Here, we extend this result and show that the spin-projected generalized Hartree-Fock wave function (which has both S2 and Sz projection) is likewise a polynomial of low-order excitation operators acting on a closed-shell determinant and provide a closed-form expression for the resulting polynomial coefficients. The spin projection of the generalized Hartree-Fock wave function introduces connected triple and quadruple excitations which are absent when spin-projecting an unrestricted Hartree-Fock determinant. We include a few preliminary applications of the combination of this spin-projected Hartree-Fock and coupled-cluster theory to the Hubbard Hamiltonian and comment on generalizations of the methodology. Results here are not for production level, but a similarity-transformed theory that combines the two offers the promise of being accurate for both weak and strong correlation, and may offer significant improvements in the intermediate correlation regime where neither projected Hartree-Fock nor coupled cluster is particularly accurate.

  6. Dispersion correction derived from first principles for density functional theory and Hartree-Fock theory.

    Science.gov (United States)

    Guidez, Emilie B; Gordon, Mark S

    2015-03-12

    The modeling of dispersion interactions in density functional theory (DFT) is commonly performed using an energy correction that involves empirically fitted parameters for all atom pairs of the system investigated. In this study, the first-principles-derived dispersion energy from the effective fragment potential (EFP) method is implemented for the density functional theory (DFT-D(EFP)) and Hartree-Fock (HF-D(EFP)) energies. Overall, DFT-D(EFP) performs similarly to the semiempirical DFT-D corrections for the test cases investigated in this work. HF-D(EFP) tends to underestimate binding energies and overestimate intermolecular equilibrium distances, relative to coupled cluster theory, most likely due to incomplete accounting for electron correlation. Overall, this first-principles dispersion correction yields results that are in good agreement with coupled-cluster calculations at a low computational cost.

  7. Excited electronic states from a variational approach based on symmetry-projected Hartree--Fock configurations

    CERN Document Server

    Jiménez-Hoyos, Carlos A; Scuseria, Gustavo E

    2013-01-01

    Recent work from our research group has demonstrated that symmetry-projected Hartree--Fock (HF) methods provide a compact representation of molecular ground state wavefunctions based on a superposition of non-orthogonal Slater determinants. The symmetry-projected ansatz can account for static correlations in a computationally efficient way. Here we present a variational extension of this methodology applicable to excited states of the same symmetry as the ground state. Benchmark calculations on the C$_2$ dimer with a modest basis set, which allows comparison with full configuration interaction results, indicate that this extension provides a high quality description of the low-lying spectrum for the entire dissociation profile. We apply the same methodology to obtain the full low-lying vertical excitation spectrum of formaldehyde, in good agreement with available theoretical and experimental data, as well as to a challenging model $C_{2v}$ insertion pathway for BeH$_2$. The variational excited state methodolo...

  8. Nonrelativistic nucleon effective masses in nuclear matter: Brueckner-Hartree-Fock model versus relativistic Hartree-Fock model

    Science.gov (United States)

    Li, A.; Hu, J. N.; Shang, X. L.; Zuo, W.

    2016-01-01

    The density and isospin dependencies of nonrelativistic nucleon effective mass (mN*) are studied, which is a measure of the nonlocality of the single particle (s.p.) potential. It can be decoupled as the so-called k mass (mk*, i.e., the nonlocality in space) and E mass (mE*, i.e., the nonlocality in time). Both k mass and E mass are determined and compared by using the latest versions of the nonrelativistic Brueckner-Hartree-Fock (BHF) model and the relativistic Hartree-Fock (RHF) model. The latter is achieved based on the corresponding Schrödinger equivalent s.p. potential in a relativistic framework. We demonstrate the origins of different effective masses and discuss also their neutron-proton splitting in the asymmetric matter in different models. We find that the neutron-proton splittings of both the k mass and the E mass have the same asymmetry dependencies at the densities considered; namely, mk,n *>mk,p * and mE,p *>mE,n * . However, the resulting splittings of nucleon effective masses could have different asymmetry dependencies in these two models because they could be dominated either by the k mass (then we have mn*>mp* in the BHF model), or by the E mass (then we have mp*>mn* in the RHF model). The isospin splitting in the BHF model is more consistent with the recent analysis from the nucleon-nucleus-scattering data, while the small E mass mE* in the RHF case as a result of the missing ladder summation finally leads to an opposite splitting behavior.

  9. Superconducting nanowires: quantum confinement and spatially dependent Hartree-Fock potential.

    Science.gov (United States)

    Chen, Yajiang; Croitoru, M D; Shanenko, A A; Peeters, F M

    2009-10-28

    It is well known that, in bulk, the solution of the Bogoliubov-de Gennes equations is the same whether or not the Hartree-Fock term is included. Here the Hartree-Fock potential is position independent and so gives the same contribution to both the single-electron energies and the Fermi level (the chemical potential). Thus, the single-electron energies measured from the Fermi level (they control the solution) stay the same. This is not the case for nanostructured superconductors, where quantum confinement breaks the translational symmetry and results in a position-dependent Hartree-Fock potential. In this case its contribution to the single-electron energies depends on the relevant quantum numbers. We numerically solved the Bogoliubov-de Gennes equations with the Hartree-Fock term for a clean superconducting nanocylinder and found a shift of the curve representing the thickness-dependent oscillations of the critical superconducting temperature to larger diameters.

  10. Superconducting nanowires: quantum confinement and spatially dependent Hartree-Fock potential

    Science.gov (United States)

    Chen, Yajiang; Croitoru, M. D.; Shanenko, A. A.; Peeters, F. M.

    2009-10-01

    It is well known that, in bulk, the solution of the Bogoliubov-de Gennes equations is the same whether or not the Hartree-Fock term is included. Here the Hartree-Fock potential is position independent and so gives the same contribution to both the single-electron energies and the Fermi level (the chemical potential). Thus, the single-electron energies measured from the Fermi level (they control the solution) stay the same. This is not the case for nanostructured superconductors, where quantum confinement breaks the translational symmetry and results in a position-dependent Hartree-Fock potential. In this case its contribution to the single-electron energies depends on the relevant quantum numbers. We numerically solved the Bogoliubov-de Gennes equations with the Hartree-Fock term for a clean superconducting nanocylinder and found a shift of the curve representing the thickness-dependent oscillations of the critical superconducting temperature to larger diameters.

  11. Hartree-Fock symmetry breaking around conical intersections.

    Science.gov (United States)

    Jake, Lena C; Henderson, Thomas M; Scuseria, Gustavo E

    2018-01-14

    We study the behavior of Hartree-Fock (HF) solutions in the vicinity of conical intersections. These are here understood as regions of a molecular potential energy surface characterized by degenerate or nearly degenerate eigenfunctions with identical quantum numbers (point group, spin, and electron numbers). Accidental degeneracies between states with different quantum numbers are known to induce symmetry breaking in HF. The most common closed-shell restricted HF instability is related to singlet-triplet spin degeneracies that lead to collinear unrestricted HF solutions. Adding geometric frustration to the mix usually results in noncollinear generalized HF (GHF) solutions, identified by orbitals that are linear combinations of up and down spins. Near conical intersections, we observe the appearance of coplanar GHF solutions that break all symmetries, including complex conjugation and time-reversal, which do not carry good quantum numbers. We discuss several prototypical examples taken from the conical intersection literature. Additionally, we utilize a recently introduced magnetization diagnostic to characterize these solutions, as well as a solution of a Jahn-Teller active geometry of H8+2.

  12. On the problem of representability and the Bogolyubov-Hartree-Fock theory

    Energy Technology Data Exchange (ETDEWEB)

    Knoerr, Hans Konrad

    2013-11-22

    The general topic of this thesis is an approximation of the ground state energy for many-particle quantum systems. In particular the Bogolyubov-Hartree-Fock theory and the representability of one- and two-particle density matrices are studied. After an introductory chapter we specify some basic notation of many-body quantum mechanics in Chapter 2. In Chapter 3 we consider boson, as well as fermion systems. We first tackle the question of representability for bosons, i.e., the question which conditions a one- and a two-particle operator must satisfy to ensure that they are the one- and the two-particle density matrix of a state. For a particle number-conserving system, the representability conditions up to second order for bosons are well-known and called admissibility, P-, and G-conditions. Since, however, most physical systems consisting of bosons are not particle number-conserving, we give an alternative for such systems: Generalizing the two-particle density matrix, we observe that the representability conditions up to second order hold if and only if this generalized two-particle density matrix is positive semi-definite and the one- and the two-particle density matrices fulfill trace class and symmetry conditions. Moreover, we study the Bogolyubov-Hartree-Fock energy of boson and fermion systems. We generalize Lieb's variational principle which in its original formulation holds for purely repulsive particle interactions for fermions only. Our second main result is the following: for bosons, as well as for fermions the infimum of the energy for a variation over pure quasifree states coincides with the one for a variation over all quasifree states under the assumption that the Hamiltonian is bounded below. In the last section of Chapter 3 we specify the relation between centered quasifree states and their corresponding generalized one-particle density matrix, which finds an application in the variational process in the Bogolyubov-Hartree-Fock theory. It is

  13. A New Approach to the Modeling of Local Defects in Crystals: The Reduced Hartree-Fock Case

    Science.gov (United States)

    Cancès, Éric; Deleurence, Amélie; Lewin, Mathieu

    2008-07-01

    This article is concerned with the derivation and the mathematical study of a new mean-field model for the description of interacting electrons in crystals with local defects. We work with a reduced Hartree-Fock model, obtained from the usual Hartree-Fock model by neglecting the exchange term. First, we recall the definition of the self-consistent Fermi sea of the perfect crystal, which is obtained as a minimizer of some periodic problem, as was shown by Catto, Le Bris and Lions. We also prove some of its properties which were not mentioned before. Then, we define and study in detail a nonlinear model for the electrons of the crystal in the presence of a defect. We use formal analogies between the Fermi sea of a perturbed crystal and the Dirac sea in Quantum Electrodynamics in the presence of an external electrostatic field. The latter was recently studied by Hainzl, Lewin, Séré and Solovej, based on ideas from Chaix and Iracane. This enables us to define the ground state of the self-consistent Fermi sea in the presence of a defect. We end the paper by proving that our model is in fact the thermodynamic limit of the so-called supercell model, widely used in numerical simulations.

  14. Excess Charge for Pseudo-relativistic Atoms in Hartree-Fock Theory

    DEFF Research Database (Denmark)

    Dall'Acqua, Anna; Solovej, Jan Philip

    2010-01-01

    We prove within the Hartree-Fock theory of pseudo-relativistic atoms that the maximal negative ionization charge and the ionization energy of an atom remain bounded independently of the nuclear charge $Z$ and the fine structure constant $\\alpha$ as long as $Z\\alpha$ is bounded.......We prove within the Hartree-Fock theory of pseudo-relativistic atoms that the maximal negative ionization charge and the ionization energy of an atom remain bounded independently of the nuclear charge $Z$ and the fine structure constant $\\alpha$ as long as $Z\\alpha$ is bounded....

  15. Parallelization of analytical Hartree-Fock and density functional theory Hessian calculations. Part I: parallelization of coupled-perturbed Hartree-Fock equations

    Science.gov (United States)

    Korambath, Prakashan P.; Kong, Jing; Furlani, Thomas R.; Head-Gordon, Martin

    Solving the coupled-perturbed Hartree-Fock (CPHF) equations is the most time consuming part in the analytical computation of second derivatives of the molecular energy with respect to the nuclei. This paper describes a unique parallelization approach for solving the CPHF equations. The computational load is divided by the nuclear perturbations and distributed evenly among the computing nodes. The parallel algorithm is scalable with respect to the size of the molecule, i.e. the larger the molecule, the greater the parallel speedup. The memory storage requirements are also distributed among the processors, with little communication among the processors. The method is implemented in the Q-Chem software package and its performance is discussed. This work represents the first step in a research project to parallelize analytical frequency calculations at Hartree-Fock and density functional theory levels.

  16. Nuclear Tensor Force and Effective Pions in the Relativistic Hartree-Fock Formalism

    Directory of Open Access Journals (Sweden)

    Marcos S.

    2014-03-01

    Full Text Available In the framework of nonlinear nuclear models based on the relativistic Hartree-Fock approximation, we have isolated the contribution of the tensor force of pions in the effective NN interaction, by means of two different approximate methods, recently developed by us, in order to dilucidate its role in a variety of nuclear properties. Results show that a reduction of the contribution of this tensor force considerably influences the spin-orbit splittings and magic gaps in the spin-unsaturated midweight 56Ni nucleus as well as the behaviour of the total binding energies with A in heavy nuclei. Both methods give similar results. We also study the evolution of the splitting of the proton 1d spin-orbit doublet in the chain Z=14, from N=20 to N=28, and the neutron 2p − 1f shell in the chain N=28, from the 48Ca nucleus to the 42Si nucleus. Whereas, in the first case, the pion tensor force (PTF plays an important role and its reduction is needed to reproduce the corresponding experimental results; in the second case, the quenching of the neutron 2p3/2 − 1f7/2 gap in the mentioned isotonic chain N=28 is hardly affected by the PTF.

  17. Proof of the extended Bloch-Messiah theorem in the thermal Hartree-Fock-Bogoliubov theory

    Science.gov (United States)

    Tanabe, K.; Sugawara-Tanabe, K.

    1990-09-01

    It is shown that an application of the thermo field dynamics (TFD) to the thermal Hartree-Fock-Bogoliubov (THFB) theory leads to the extended form of the Bloch-Messiah theorem for the finite temperature formalism. The generalized density matrix defined on the enlarged operator space including tilded into account the thermal fluctuation of fermion number for the system under consideration.

  18. Assessing the accuracy of Hartree-Fock-Bogoliubov calculations by use of mass relations

    DEFF Research Database (Denmark)

    Hove, D.; Fedorov, D. V.; Jensen, A. S.

    2014-01-01

    The accuracy of three different sets of Hartree-Fock-Bogoliubov calculations of nuclear binding energies is systematically evaluated. To emphasize minor fluctuations, a second order, four-point mass relation, which almost completely eliminates smooth aspects of the binding energy, is introduced...

  19. On the behaviour of the Hartree-Fock energy at short internuclear distances

    DEFF Research Database (Denmark)

    Gilka, Natalie; Solovej, Jan Philip; Taylor, Peter R.

    2011-01-01

    There are well-established mathematical relationships for the energy of a diatomic molecule (the exact energy, but also both the Hartree-Fock and Thomas-Fermi energies) in the limit of large nuclear charge of the atoms and small internuclear distances. We present calculated energies for a number...

  20. Restricted Closed Shell Hartree Fock Roothaan Matrix Method Applied to Helium Atom Using Mathematica

    Science.gov (United States)

    Acosta, César R.; Tapia, J. Alejandro; Cab, César

    2014-01-01

    Slater type orbitals were used to construct the overlap and the Hamiltonian core matrices; we also found the values of the bi-electron repulsion integrals. The Hartree Fock Roothaan approximation process starts with setting an initial guess value for the elements of the density matrix; with these matrices we constructed the initial Fock matrix.…

  1. Spin {ital M}1 excitations in deformed nuclei from self-consistent Hartree-Fock plus random-phase approximation

    Energy Technology Data Exchange (ETDEWEB)

    Sarriguren, P.; Moya de Guerra, E.; Nojarov, R. [Instituto de Estructura de la Materia, Consejo Superior de Investigaciones Cientificas, Serrano 119, E-28006 Madrid (Spain)

    1996-08-01

    We present a method to study spin magnetic dipole excitations in deformed nuclei within the quasiparticle random phase approximation based on self-consistent Hartree-Fock mean fields and residual interactions derived from the same effective two-body force. We perform a comprehensive study covering different Skyrme forces and various mass regions, and discussing the role of the mean field and of the residual interaction. An overall agreement with experimental data is obtained with the SG2 force. We study the systematics and the deformation dependence of the spin {ital M}1 strength distributions of {ital K}{sup {pi}}=1{sup +} excitations. It is found for the first time that the summed spin {ital M}1 strength obeys a quadratic dependence on deformation in the two isotope chains studied, {sup 142,146,148,150}Nd and {sup 144,148,150,152,154}Sm. {copyright} {ital 1996 The American Physical Society.}

  2. Toward a muon-specific electronic structure theory: effective electronic Hartree-Fock equations for muonic molecules.

    Science.gov (United States)

    Rayka, Milad; Goli, Mohammad; Shahbazian, Shant

    2018-02-07

    An effective set of Hartree-Fock (HF) equations are derived for electrons of muonic systems, i.e., molecules containing a positively charged muon, conceiving the muon as a quantum oscillator, which are completely equivalent to the usual two-component HF equations used to derive stationary states of the muonic molecules. In these effective equations, a non-Coulombic potential is added to the orthodox coulomb and exchange potential energy terms, which describes the interaction of the muon and the electrons effectively and is optimized during the self-consistent field cycles. While in the two-component HF equations a muon is treated as a quantum particle, in the effective HF equations it is absorbed into the effective potential and practically transformed into an effective potential field experienced by electrons. The explicit form of the effective potential depends on the nature of muon's vibrations and is derivable from the basis set used to expand the muonic spatial orbital. The resulting effective Hartree-Fock equations are implemented computationally and used successfully, as a proof of concept, in a series of muonic molecules containing all atoms from the second and third rows of the Periodic Table. To solve the algebraic version of the equations muon-specific Gaussian basis sets are designed for both muon and surrounding electrons and it is demonstrated that the optimized exponents are quite distinct from those derived for the hydrogen isotopes. The developed effective HF theory is quite general and in principle can be used for any muonic system while it is the starting point for a general effective electronic structure theory that incorporates various types of quantum correlations into the muonic systems beyond the HF equations.

  3. Multiconfiguration hartree-fock theory for pseudorelativistic systems: The time-dependent case

    KAUST Repository

    Hajaiej, Hichem

    2014-03-01

    In [Setting and analysis of the multi-configuration time-dependent Hartree-Fock equations, Arch. Ration. Mech. Anal. 198 (2010) 273-330] the third author has studied in collaboration with Bardos, Catto and Mauser the nonrelativistic multiconfiguration time-dependent Hartree-Fock system of equations arising in the modeling of molecular dynamics. In this paper, we extend the previous work to the case of pseudorelativistic atoms. We show the existence and the uniqueness of global-in-time solution to the underlying system under technical assumptions on the energy of the initial data and the charge of the nucleus. Moreover, we prove that the result can be extended to the case of neutron stars when the number of electrons is less than a critical number N cr. © 2014 World Scientific Publishing Company.

  4. Accurate alkynyl radical structures from density functional calculations without Hartree-Fock exchange

    Science.gov (United States)

    Janesko, Benjamin G.; Proynov, Emil

    2017-02-01

    Density functional approximations (DFAs) often suffer from self-repulsion and delocalization errors which are reduced by exact (Hartree-Fock-like) exchange admixture. Oyeyemi and co-workers recently showed that several DFAs with little exact exchange incorrectly predict bent alkynyl radical geometries, giving errors in ab initio composite methods using density functional theory geometries [V. B. Oyeyemi et al., J. Phys. Chem. Lett. 3, 289 (2012)]. We show that the simple Hartree-Fock-Slater and Xα DFAs, which have substantial delocalization error, predict linear alkynyl radical geometries without incorporating exact exchange. Our Rung 3.5 DFAs, and rescaled generalized gradient approximations, can give either linear σ, bent σ -π , or nearly linear π radicals, all without incorporating exact exchange. This highlights the complexity of delocalization error, the utility of accurate empirical DFA geometries for ab initio composite methods, and the insights to be gained from Rung 3.5 DFAs.

  5. On the solution of the Hartree-Fock-Bogoliubov equations by the conjugate gradient method

    Energy Technology Data Exchange (ETDEWEB)

    Egido, J.L. [Universidad Autonoma de Madrid (Spain). Dept. de Fisica Teorica; Lessing, J. [Universidad Autonoma de Madrid (Spain). Dept. de Fisica Teorica; Martin, V. [Analisis Numerico, Facultad de Informatica, Universidad Politecnica de Madrid, E-28660 Boadilla del Monte, Madrid (Spain); Robledo, L.M. [Universidad Autonoma de Madrid (Spain). Dept. de Fisica Teorica

    1995-11-06

    The conjugate gradient method is formulated in the Hilbert space for density and non-density dependent Hamiltonians. We apply it to the solution of the Hartree-Fock-Bogoliubov equations with constraints. As a numerical application we show calculations with the finite range density dependent Gogny force. The number of iterations required to reach convergence is reduced by a factor of three to four as compared with the standard gradient method. (orig.).

  6. Convergence rates of supercell calculations in the reduced Hartree-Fock model

    OpenAIRE

    Gontier, David; Lahbabi, Salma

    2015-01-01

    This article is concerned with the numerical simulations of perfect crystals. We study the rate of convergence of the reduced Hartree-Fock (rHF) model in a supercell towards the periodic rHF model in the whole space. We prove that, whenever the crystal is an insulator or a semi-conductor, the supercell energy per unit cell converges exponentially fast towards the periodic rHF energy per unit cell, with respect to the size of the supercell.

  7. Dirac-Hartree-Fock studies of X-ray transitions in meitnerium

    Energy Technology Data Exchange (ETDEWEB)

    Thierfelder, C.; Schwerdtfeger, P. [Massey University (Auckland Campus), Centre of Theoretical Chemistry and Physics, The New Zealand Institute for Advanced Study, North Shore City, Auckland (New Zealand); Hessberger, F.P. [Gesellschaft fuer Schwerionenforschung (GSI), Darmstadt (Germany); Hofmann, S. [Gesellschaft fuer Schwerionenforschung (GSI), Darmstadt (Germany); Johann Wolfgang Goethe-Universitaet, Institut fuer Kernphysik, Frankfurt (Germany)

    2008-05-15

    The K -shell and L -shell ionizations potentials for {sup 268} {sub 109}Mt were calculated at the Dirac-Hartree-Fock level taking into account quantum electrodynamic and finite nuclear-size effects. The K{sub {alpha}}{sub 1} transition energies for different ionization states are accurately predicted and compared with recent experiments in the {alpha} -decay of {sup 272} {sub 111}Rg. (orig.)

  8. Transfer probabilities for the reactions O,2014+20O in terms of multiple time-dependent Hartree-Fock-Bogoliubov trajectories

    Science.gov (United States)

    Scamps, Guillaume; Hashimoto, Yukio

    2017-09-01

    The transfer reaction between two nuclei in the superfluid phase is studied with the time-dependent Hartree-Fock-Bogoliubov (TDHFB) theory. To restore the symmetry of the relative gauge angle, a set of independent TDHFB trajectories is taken into account. Then, the transfer probability is computed using a triple projection method. This method is first tested to determine the transfer probabilities on a toy model and compared to the exact solution. It is then applied to the reactions 20O+20O and 14O+20O in a realistic framework with a Gogny interaction.

  9. Global solutions of restricted open-shell Hartree-Fock theory from semidefinite programming with applications to strongly correlated quantum systems.

    Science.gov (United States)

    Veeraraghavan, Srikant; Mazziotti, David A

    2014-03-28

    We present a density matrix approach for computing global solutions of restricted open-shell Hartree-Fock theory, based on semidefinite programming (SDP), that gives upper and lower bounds on the Hartree-Fock energy of quantum systems. While wave function approaches to Hartree-Fock theory yield an upper bound to the Hartree-Fock energy, we derive a semidefinite relaxation of Hartree-Fock theory that yields a rigorous lower bound on the Hartree-Fock energy. We also develop an upper-bound algorithm in which Hartree-Fock theory is cast as a SDP with a nonconvex constraint on the rank of the matrix variable. Equality of the upper- and lower-bound energies guarantees that the computed solution is the globally optimal solution of Hartree-Fock theory. The work extends a previously presented method for closed-shell systems [S. Veeraraghavan and D. A. Mazziotti, Phys. Rev. A 89, 010502-R (2014)]. For strongly correlated systems the SDP approach provides an alternative to the locally optimized Hartree-Fock energies and densities with a certificate of global optimality. Applications are made to the potential energy curves of C2, CN, Cr2, and NO2.

  10. Tensor numerical methods in quantum chemistry: from Hartree-Fock to excitation energies.

    Science.gov (United States)

    Khoromskaia, Venera; Khoromskij, Boris N

    2015-12-21

    We resume the recent successes of the grid-based tensor numerical methods and discuss their prospects in real-space electronic structure calculations. These methods, based on the low-rank representation of the multidimensional functions and integral operators, first appeared as an accurate tensor calculus for the 3D Hartree potential using 1D complexity operations, and have evolved to entirely grid-based tensor-structured 3D Hartree-Fock eigenvalue solver. It benefits from tensor calculation of the core Hamiltonian and two-electron integrals (TEI) in O(n log n) complexity using the rank-structured approximation of basis functions, electron densities and convolution integral operators all represented on 3D n × n × n Cartesian grids. The algorithm for calculating TEI tensor in a form of the Cholesky decomposition is based on multiple factorizations using algebraic 1D "density fitting" scheme, which yield an almost irreducible number of product basis functions involved in the 3D convolution integrals, depending on a threshold ε > 0. The basis functions are not restricted to separable Gaussians, since the analytical integration is substituted by high-precision tensor-structured numerical quadratures. The tensor approaches to post-Hartree-Fock calculations for the MP2 energy correction and for the Bethe-Salpeter excitation energies, based on using low-rank factorizations and the reduced basis method, were recently introduced. Another direction is towards the tensor-based Hartree-Fock numerical scheme for finite lattices, where one of the numerical challenges is the summation of electrostatic potentials of a large number of nuclei. The 3D grid-based tensor method for calculation of a potential sum on a L × L × L lattice manifests the linear in L computational work, O(L), instead of the usual O(L(3) log L) scaling by the Ewald-type approaches.

  11. Time-dependent Hartree-Fock studies of the dynamical fusion threshold

    Directory of Open Access Journals (Sweden)

    Nakatsukasa Takashi

    2012-12-01

    Full Text Available A microscopic description of dynamical fusion threshold in heavy ion collisions is performed in the framework of time-dependent Hartree-Fock (TDHF theory using Skyrme energy density functional (EDF. TDHF fusion threshold is in a better agreement with experimental fusion barrier. We find that the onset of extra push lies at the effective fissility 33, which is consistent with the prediction of Swiatecki’s macroscopic model. The extra push energy in our TDHF simulation is systematically smaller than the prediction in macroscopic model. The important dynamical effects and the way to fit the parameter might be responsible for the different results.

  12. New Multithreaded Hybrid CPU/GPU Approach to Hartree-Fock.

    Science.gov (United States)

    Asadchev, Andrey; Gordon, Mark S

    2012-11-13

    In this article, a new multithreaded Hartree-Fock CPU/GPU method is presented which utilizes automatically generated code and modern C++ techniques to achieve a significant improvement in memory usage and computer time. In particular, the newly implemented Rys Quadrature and Fock Matrix algorithms, implemented as a stand-alone C++ library, with C and Fortran bindings, provides up to 40% improvement over the traditional Fortran Rys Quadrature. The C++ GPU HF code provides approximately a factor of 17.5 improvement over the corresponding C++ CPU code.

  13. Holomorphic Hartree-Fock Theory: The Nature of Two-Electron Problems

    OpenAIRE

    Burton, Hugh G. A.; Gross, Mark; Thom, Alex J. W.

    2018-01-01

    We explore the existence and behaviour of holomorphic restricted Hartree-Fock (h-RHF) solutions for two-electron problems. Through algebraic geometry, the exact number of solutions with $n$ basis functions is rigorously identified as $\\frac{1}{2}(3^n - 1)$, proving that states must exist for all molecular geometries. A detailed study on the h-RHF states of HZ (STO-3G) then demonstrates both the conservation of holomorphic solutions as geometry or atomic charges are varied and the emergence of...

  14. A new relativistic Hartree-Fock calculation scheme and its application to the evaluation of fine-structure intervals for nd (n = 3-40) series of sodium

    Science.gov (United States)

    He, Liming; Zhu, Yunxia; Zhang, Meng; Tu, Yaoquan

    2011-11-01

    We present a new second-order representation of the relativistic Hartree-Fock equation, which can be solved by the standard Hartree-Fock technique. An alternative reduction for the magnetic part of the Breit interaction is presented in an explicit expression. A corresponding program has been developed, which improves significantly the scaled linear mesh introduced by Herman and Skillman. The structures for a number of atoms and ions are calculated and the agreement of our results with those published is excellent. We evaluate the fine-structure intervals of nd(n = 3-40) Rydberg series for sodium. The inverted fine-structure splitting values are obtained directly as the differences of eigenvalues obtained from a self-consistent field procedure. Taking into account the Gaunt effect enables the accuracy of the calculation to be substantially improved. The complete treatments reproduce very well the inverted fine structures along the Rydberg series and the relative difference between the present results and the experiments does not exceed 4.4%.

  15. Integral processing in beyond-Hartree-Fock calculations

    Science.gov (United States)

    Taylor, P. R.

    1986-01-01

    The increasing rate at which improvements in processing capacity outstrip improvements in input/output performance of large computers has led to recent attempts to bypass generation of a disk-based integral file. The direct self-consistent field (SCF) method of Almlof and co-workers represents a very successful implementation of this approach. This paper is concerned with the extension of this general approach to configuration interaction (CI) and multiconfiguration-self-consistent field (MCSCF) calculations. After a discussion of the particular types of molecular orbital (MO) integrals for which -- at least for most current generation machines -- disk-based storage seems unavoidable, it is shown how all the necessary integrals can be obtained as matrix elements of Coulomb and exchange operators that can be calculated using a direct approach. Computational implementations of such a scheme are discussed.

  16. Spin- and charge-density waves in the Hartree-Fock ground state of the two-dimensional Hubbard model.

    Science.gov (United States)

    Xu, Jie; Chang, Chia-Chen; Walter, Eric J; Zhang, Shiwei

    2011-12-21

    The ground states of the two-dimensional repulsive Hubbard model are studied within the unrestricted Hartree-Fock (UHF) theory. Magnetic and charge properties are determined by systematic, large-scale, exact numerical calculations, and quantified as a function of electron doping, h. In the solution of the self-consistent UHF equations, multiple initial configurations and simulated annealing are used to facilitate convergence to the global minimum. New approaches are employed to minimize finite-size effects in order to reach the thermodynamic limit. At low to moderate interacting strengths and low doping, the UHF ground state is a linear spin-density wave (l-SDW), with antiferromagnetic order and a modulating wave. The wavelength of the modulating wave is 2/h. Corresponding charge order exists but is substantially weaker than the spin order, hence holes are mobile. As the interaction is increased, the l-SDW states evolve into several different phases, with the holes eventually becoming localized. A simple pairing model is presented with analytic calculations for low interaction strength and small doping, to help understand the numerical results and provide a physical picture for the properties of the SDW ground state. By comparison with recent many-body calculations, it is shown that, for intermediate interactions, the UHF solution provides a good description of the magnetic correlations in the true ground state of the Hubbard model. © 2011 IOP Publishing Ltd Printed in the UK & the USA

  17. Finding symmetry breaking Hartree-Fock solutions: The case of triplet instability

    Science.gov (United States)

    Tóth, Zsuzsanna; Pulay, Peter

    2016-10-01

    Determining the lowest unrestricted Hartree-Fock (UHF) solution is often difficult in even-electron systems. We have developed a deterministic method for locating approximately the UHF minimum using the restricted Hartree-Fock triplet instability matrix. The current method is truncated to fourth order. The minimum energy solution for this model can be determined by solving a small linear system of equations. This solution gives a suitable starting point to determine the exact UHF solution. This should be useful for the black-box determination of active spaces spanned by the fractionally occupied charge natural orbitals of the ground-state UHF wavefunction. The results can be generalized to higher (6th and 8th) degree expansions (odd expansion orders vanish by symmetry), and to other types of instability, including complex instability. The results are illustrated by calculations on ozone, benzene, nitrobenzene, butadiene, hexatriene, octatetraene, dichromium, and nickel porphine. Further examples are given in the supplementary material (ftp://ftp.aip.org/epaps/journ_chem_phys/E-JCPSA6-145-011640).

  18. Spectroscopic investigations of 2,5-Difluoronitrobenzene using Hartree-Fock (HF) and density functional theory (DFT) calculations

    Science.gov (United States)

    Saravanan, S. P.; Sankar, A.; Parimala, K.

    2017-01-01

    The complete structural and vibrational analysis of the 2,5-Difluoronitrobenzene (DNB) was carried out by Hartree-Fock (HF) and density functional theory (DFT) method (B3LYP) with 6-311++G (d,p) basis set. The fundamental vibrations are assigned on the basis of the potential energy distribution (PED) of the vibrational modes calculated with scaled quantum mechanics (SQM) method. Using the time-dependent density functional theory (TD-DFT) method, electronic absorption spectra of the title compound have been predicted and a good agreement with the experimental ones is determined. 13C and 1H NMR spectra were recorded and chemical shifts of the molecule were calculated using the gauge independent atomic orbital (GIAO) method. The hyperconjugative interaction energy (E(2)) and electron densities of donor (i) and acceptor (j) bonds were calculated using natural bond orbital (NBO) analysis. In addition, molecular electrostatic potential (MEP) and atomic charges were calculated using B3LYP/6-311++G (d,p) level of theory. Moreover, thermodynamic properties (heat capacities, entropy, enthalpy and Gibb's free energy) of the title compound at different temperatures were calculated.

  19. A theoretical study of molecular conduction. III. A nonequilibrium-Green's-function-based Hartree-Fock approach

    Science.gov (United States)

    Shimazaki, Tomomi; Xue, Yongqiang; Ratner, Mark A.; Yamashita, Koichi

    2006-03-01

    Many recent experimental and theoretical studies have paid attention to the conductivity of single molecule transport junctions, both because it is fundamentally important and because of its significance in the development of molecular-based electronics. In this paper, we discuss a nonequilibrium Green's function (NEGF)-based Hartree-Fock (HF) approach; the NEGF method can appropriately accommodate charge distributions in molecules connected to electrodes. In addition, we show that a NEGF-based density matrix can reduce to an ordinary HF density matrix for an isolated molecule if the molecule does not interact with electrodes. This feature of the NEGF-based density matrix also means that NEGF-based Mulliken charges can be reduced to ordinary Mulliken charges in those cases. Therefore, the NEGF-based HF approach can directly compare molecules that are connected to electrodes with isolated ones, and is useful in investigating complicated features of molecular conduction. We also calculated the transmission probability and conduction for benzenedithiol under finite electrode biases. The coupling between the electrodes and molecule causes electron transfer from the molecule to the electrodes, and the applied bias modifies this electron transfer. In addition, we found that the molecule responds capacitively to the applied bias, by shifting the molecular orbital energies.

  20. Study on formalism of Griffin-Wheeler-Hartree-Fock equations and a propose for its variational discretization; Estudo sobre o formalismo das equacoes Griffin-Wheeler-Hartree-Fock e uma proposta para sua discretizacao variacional

    Energy Technology Data Exchange (ETDEWEB)

    Barbosa, Rugles Cesar

    2002-07-01

    The present thesis is divided into two parts. The first part describes the many kind of the formalisms of the Generator Coordinate Hartree-Fock method (GCHFM) and second part describes the computational aspect applied to the GCHFM formalism in its discreet form. The major aim of this work is the development of an alternative method to non-linear parameters optimization (basis set) and later uses these optimized parameters to adjust the weight function into GCHFM method. The study of the weight function when N {yields} {infinity} (or for large N), where N represents the number of mesh, is important since the GCHFM theory in its continuous form depend on understanding of such behavior. In this thesis, a detailed study is carried out about the methodologies of the self-consistent solution of the GCHFM and some methodology aspects of non-linear parameters optimization. This work shows that the Generator Coordinate Hartree-Fock method is general and it has as particular case the Hartree-Fock Roothaan method. Some possible variations or combinations around of the characteristics of the GCHFM and a comparison with conventional SCF procedure are reported in this thesis. The piecewise weight function method developed in this work shows to be very good for collective parameter optimizations of the Generator Coordinate (GC). The GCHFM calculations are necessary restrict (GCM-RHF), especially when the calculated value energies approach of its numerical values or Hartree-Fock limit. In the optimization methods of state functions for atomic electronic systems is very common the application of the gradient method and its efficacy is not contested. However, the method describes above allow us to obtain results as good as the gradient method. The basis set generated using the piecewise weight function method for Gaussian type function were used in the Restrict Hartree-Fock (RHF) calculations to obtain the total energies for some atomic electronic systems, such as neutron atoms and

  1. Spiral magnetic phases on the Kondo Lattice Model: A Hartree-Fock approach

    Science.gov (United States)

    Costa, N. C.; Lima, J. P.; dos Santos, Raimundo R.

    2017-02-01

    We study the Kondo Lattice Model (KLM) on a square lattice through a Hartree-Fock approximation in which the local spins are treated semi-classically, in the sense that their average values are modulated by a magnetic wavevector Q while they couple with the conduction electrons through fermion operators. In this way, we obtain a ground state phase diagram in which spiral magnetic phases (in which the wavevector depends on the coupling constants and on the density) interpolate between the low-density ferromagnetic phase and the antiferromagnetic phase at half filling; within small regions of the phase diagram commensurate magnetic phases can coexist with Kondo screening. We have also obtained 'Doniach-like' diagrams, showing the effect of temperature on the ground state phases, and established that for some ranges of the model parameters (the exchange coupling and conduction electron density) the magnetic wavevector changes with temperature, either continuously or abruptly (e.g., from spiral to ferromagnetic).

  2. Existence of Infinitely Many Distinct Solutions to the Quasirelativistic Hartree-Fock Equations

    Directory of Open Access Journals (Sweden)

    M. Enstedt

    2009-01-01

    Full Text Available We establish existence of infinitely many distinct solutions to the semilinear elliptic Hartree-Fock equations for N-electron Coulomb systems with quasirelativistic kinetic energy −α−2Δxn+α−4−α−2 for the nth electron. Moreover, we prove existence of a ground state. The results are valid under the hypotheses that the total charge Ztot of K nuclei is greater than N−1 and that Ztot is smaller than a critical charge Zc. The proofs are based on a new application of the Fang-Ghoussoub critical point approach to multiple solutions on a noncompact Riemannian manifold, in combination with density operator techniques.

  3. Ab-initio Hartree-Fock study of tritium desorption from Li{sub 2}O

    Energy Technology Data Exchange (ETDEWEB)

    Taniguchi, Masaki; Tanaka, Satoru [Tokyo Univ. (Japan). Faculty of Engineering

    1998-03-01

    Dissociative adsorption of hydrogen on Li{sub 2}O (110) surface has been investigated with ab-initio Hartree-Fock quantum chemical calculation technique. Heat of adsorption and potential energy surface for H{sub 2} dissociative adsorption was evaluated by calculating the total energy of the system. Calculation results on adsorption heat indicated that H{sub 2} adsorption is endothermic. However, when oxygen vacancy exists adjacent to the adsorption sites, heat of adsorption energy became less endothermic and the activation energy required to dissociate the H-H bonding was smaller than that for the terrace site. This is considered to be caused by the excess charge localized near the defect. (author)

  4. Hartree-Fock calculation of the differential photoionization cross sections of small Li clusters.

    Science.gov (United States)

    Galitskiy, S A; Artemyev, A N; Jänkälä, K; Lagutin, B M; Demekhin, Ph V

    2015-01-21

    Cross sections and angular distribution parameters for the single-photon ionization of all electron orbitals of Li2-8 are systematically computed in a broad interval of the photoelectron kinetic energies for the energetically most stable geometry of each cluster. Calculations of the partial photoelectron continuum waves in clusters are carried out by the single center method within the Hartree-Fock approximation. We study photoionization cross sections per one electron and analyze in some details general trends in the photoionization of inner and outer shells with respect to the size and geometry of a cluster. The present differential cross sections computed for Li2 are in a good agreement with the available theoretical data, whereas those computed for Li3-8 clusters can be considered as theoretical predictions.

  5. New parameterizations of the Gogny effective nuclear interaction; Nouvelles parametrisations de l'interaction nucleaire effective de Gogny

    Energy Technology Data Exchange (ETDEWEB)

    Chappert, F

    2007-06-15

    The effective interaction between nucleons is the basic input to microscopic calculations in nuclear structure. One of the forms used since the 1970's is the phenomenological effective force proposed by D. Gogny. This force gives excellent results in nuclei at the mean-field approximation. The presence of contact terms does not allow, however, to use it for the description of beyond mean-field correlations present in nuclei. In this work, we investigate some extensions of the Gogny force, and especially a generalization in which the zero range density dependent term has been replaced by a finite range term. The parameters occurring in the analytical form of the force have been adjusted on symmetric infinite nuclear matter and neutron matter properties, and on some selected observables for stable nuclei, especially those related to pairing correlations. We present the method to include this kind of force in Hartree-Fock-Bogoliubov calculations and we analyze the results obtained for various nuclei. The new versions of the Gogny force allow us to reproduce nuclear structure properties with improved accuracy as compared to the former version. (author)

  6. Adaptive multi-resolution 3D Hartree-Fock-Bogoliubov solver for nuclear structure

    Science.gov (United States)

    Pei, J. C.; Fann, G. I.; Harrison, R. J.; Nazarewicz, W.; Shi, Yue; Thornton, S.

    2014-08-01

    Background: Complex many-body systems, such as triaxial and reflection-asymmetric nuclei, weakly bound halo states, cluster configurations, nuclear fragments produced in heavy-ion fusion reactions, cold Fermi gases, and pasta phases in neutron star crust, are all characterized by large sizes and complex topologies in which many geometrical symmetries characteristic of ground-state configurations are broken. A tool of choice to study such complex forms of matter is an adaptive multi-resolution wavelet analysis. This method has generated much excitement since it provides a common framework linking many diversified methodologies across different fields, including signal processing, data compression, harmonic analysis and operator theory, fractals, and quantum field theory. Purpose: To describe complex superfluid many-fermion systems, we introduce an adaptive pseudospectral method for solving self-consistent equations of nuclear density functional theory in three dimensions, without symmetry restrictions. Methods: The numerical method is based on the multi-resolution and computational harmonic analysis techniques with a multi-wavelet basis. The application of state-of-the-art parallel programming techniques include sophisticated object-oriented templates which parse the high-level code into distributed parallel tasks with a multi-thread task queue scheduler for each multi-core node. The internode communications are asynchronous. The algorithm is variational and is capable of solving coupled complex-geometric systems of equations adaptively, with functional and boundary constraints, in a finite spatial domain of very large size, limited by existing parallel computer memory. For smooth functions, user-defined finite precision is guaranteed. Results: The new adaptive multi-resolution Hartree-Fock-Bogoliubov (HFB) solver madness-hfb is benchmarked against a two-dimensional coordinate-space solver hfb-ax that is based on the B-spline technique and a three-dimensional solver

  7. The coupled cluster approach with a hybrid treatment of connected triple excitations based on the restricted Hartree-Fock reference.

    Science.gov (United States)

    Shen, Jun; Kou, Zhuangfei; Xu, Enhua; Li, Shuhua

    2011-01-28

    A generalization of the coupled cluster (CC) singles, doubles, and a hybrid treatment of connected triples [denoted as CCSD(T)-h] [Shen et al., J. Chem. Phys. 132, 114115 (2010)] to the restricted Hartree-Fock (RHF) reference is presented. In this approach, active (or pseudoactive) RHF orbitals are constructed automatically by performing unitary transformations of canonical RHF orbitals so that they spatially mimic the natural orbitals of the unrestricted Hartree-Fock reference. The present RHF-based CCSD(T)-h approach has been applied to study the potential energy surfaces in several typical bond breaking processes and the singlet-triplet gaps in a diradical (HFH)(-1). For all systems under study, the overall performance of CCSD(T)-h is very close to that of the corresponding CCSD(T) (CC singles, doubles, and triples), and much better than that of CCSD(T) (CC singles, doubles, and perturbative triples).

  8. Description of the ground state of axially deformed nuclei within the Relativistic Hartree-Fock-Bogoliubov model

    Energy Technology Data Exchange (ETDEWEB)

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

    2011-09-16

    The Relativistic Hartree-Fock-Bogoliubov model for axially deformed nuclei (RHFBz) is presented. The model involves a phenomenological Lagrangian with density-dependent meson-nucleon couplings in the particle-hole channel and the central part of the Gogny force in the particle-particle channel. The RHFBz equations are solved by expansion in the basis of a deformed harmonic oscillator. Illustrative RHFBz calculations are performed for Neon isotopes.

  9. Systematic study of even-even nuclei with Hartree-Fock+BCS method using Skyrme SIII force

    Energy Technology Data Exchange (ETDEWEB)

    Tajima, Naoki; Takahara, Satoshi; Onishi, Naoki [Tokyo Univ. (Japan). Coll. of Arts and Sciences

    1997-03-01

    We have applied the Hartree-Fock+BCS method with Skyrme SIII force formulated in a three-dimensional Cartesian-mesh representation to even-even nuclei with 2 {<=} Z {<=} 114. We discuss the results concerning the atomic masses, the quadrupole (m=0, 2) and hexadecapole (m=0, 2, 4) deformations, the skin thicknesses, and the halo radii. We also discuss the energy difference between oblate and prolate solutions and the shape difference between protons and neutrons. (author)

  10. Quantum supercharger library: hyper-parallelism of the Hartree-Fock method.

    Science.gov (United States)

    Fernandes, Kyle D; Renison, C Alicia; Naidoo, Kevin J

    2015-07-05

    We present here a set of algorithms that completely rewrites the Hartree-Fock (HF) computations common to many legacy electronic structure packages (such as GAMESS-US, GAMESS-UK, and NWChem) into a massively parallel compute scheme that takes advantage of hardware accelerators such as Graphical Processing Units (GPUs). The HF compute algorithm is core to a library of routines that we name the Quantum Supercharger Library (QSL). We briefly evaluate the QSL's performance and report that it accelerates a HF 6-31G Self-Consistent Field (SCF) computation by up to 20 times for medium sized molecules (such as a buckyball) when compared with mature Central Processing Unit algorithms available in the legacy codes in regular use by researchers. It achieves this acceleration by massive parallelization of the one- and two-electron integrals and optimization of the SCF and Direct Inversion in the Iterative Subspace routines through the use of GPU linear algebra libraries. © 2015 Wiley Periodicals, Inc. © 2015 Wiley Periodicals, Inc.

  11. Exploration of (super-)heavy elements using the Skyrme-Hartree-Fock model

    Energy Technology Data Exchange (ETDEWEB)

    Erler, Jochen

    2011-01-31

    Motivated by the steadily increasing number of known nuclei and nuclear properties, theories of nuclear structure are presently a field of intense research. This work concentrates on the self-consistent description of nuclei in terms of the Skyrme-Hartree-Fock (SHF) approach. The extrapolation of nuclear shell structure to the region of super-heavy elements (SHE) using the SHF model, the dependence on different parameterization and the influence of collective correlation will be studied. The general scope of this work are large scale calculation for a global survey of properties of SHE like binding energies, separation energies and decay characteristics and lifetimes. These calculations were done in a collaboration with the theory group of the GSI in Darmstadt and have the aim to develop a database of lifetimes and reaction rates for {alpha}, {beta}-decay and spontaneous fission in a very wide range with proton numbers 86 {<=} Z {<=} 120 and neutron numbers up to N {approx} 260 relevant for the astrophysical r-process. The results of this study for example predictions of a possible islands of very stable nuclei and information of favored decay mode for each nuclei are also applicable in the recent experimental synthesis of exotic SHE. For these calculation a framework to calculate {beta}-decay half-lives within the SHF model has been developed and the existing axial SHF code has been extended to compute {beta}-transition matrix elements and so to provide an estimation of half-lives. (orig.)

  12. Structure factors for tunneling ionization rates of molecules: General Hartree-Fock-based integral representation

    Science.gov (United States)

    Madsen, Lars Bojer; Jensen, Frank; Dnestryan, Andrey I.; Tolstikhin, Oleg I.

    2017-07-01

    In the leading-order approximation of the weak-field asymptotic theory (WFAT), the dependence of the tunneling ionization rate of a molecule in an electric field on its orientation with respect to the field is determined by the structure factor of the ionizing molecular orbital. The WFAT yields an expression for the structure factor in terms of a local property of the orbital in the asymptotic region. However, in general quantum chemistry approaches molecular orbitals are expanded in a Gaussian basis which does not reproduce their asymptotic behavior correctly. This hinders the application of the WFAT to polyatomic molecules, which are attracting increasing interest in strong-field physics. Recently, an integral-equation approach to the WFAT for tunneling ionization of one electron from an arbitrary potential has been developed. The structure factor is expressed in an integral form as a matrix element involving the ionizing orbital. The integral is not sensitive to the asymptotic behavior of the orbital, which resolves the difficulty mentioned above. Here, we extend the integral representation for the structure factor to many-electron systems treated within the Hartree-Fock method and show how it can be implemented on the basis of standard quantum chemistry software packages. We validate the methodology by considering noble-gas atoms and the CO molecule, for which accurate structure factors exist in the literature. We also present benchmark results for CO2 and for NH3 in the pyramidal and planar geometries.

  13. Holomorphic Hartree-Fock Theory: The Nature of Two-Electron Problems.

    Science.gov (United States)

    Burton, Hugh G A; Gross, Mark; Thom, Alex J W

    2018-01-29

    We explore the existence and behavior of holomorphic restricted Hartree-Fock (h-RHF) solutions for two-electron problems. Through algebraic geometry, the exact number of solutions with n basis functions is rigorously identified as 1/2(3n - 1), proving that states must exist for all molecular geometries. A detailed study on the h-RHF states of HZ (STO-3G) then demonstrates both the conservation of holomorphic solutions as geometry or atomic charges are varied and the emergence of complex h-RHF solutions at coalescence points. Using catastrophe theory, the nature of these coalescence points is described, highlighting the influence of molecular symmetry. The h-RHF states of HHeH2+ and HHeH (STO-3G) are then compared, illustrating the isomorphism between systems with two electrons and two electron holes. Finally, we explore the h-RHF states of ethene (STO-3G) by considering the π electrons as a two-electron problem and employ NOCI to identify a crossing of the lowest energy singlet and triplet states at the perpendicular geometry.

  14. Coupled perturbed Hartree-Fock for periodic systems: The role of symmetry and related computational aspects

    Science.gov (United States)

    Ferrero, Mauro; Rérat, Michel; Orlando, Roberto; Dovesi, Roberto

    2008-01-01

    A general and efficient implementation of the coupled perturbed Hartree-Fock (CPHF) scheme in the CRYSTAL06 code that applies to systems periodic in one dimension (polymers), two dimensions (slabs), three dimensions (crystals) and, as a limiting case, zero dimension (molecules) is presented. The dielectric tensor of large unit cell systems such as boehmite (γ-AlOOH, 8 atoms/cell), calcite (CaCO3, 10 atoms/cell), and pyrope (Mg3Al2Si3O12, 80 atoms/cell) has been computed. Results are well converged with respect to the computational parameters, in particular, to the number of k points in the reciprocal space and tolerances used in the truncation of the Coulomb and exchange series, showing that the same standard computational conditions used for the self-consistent-field (SCF) step can also be used safely in a CPHF calculation. Point symmetry, being so important in determining crystal properties, also reduces dramatically the computational cost both of the preliminary SCF step and the CPHF calculation, so that the dielectric tensor for large unit cell systems such as pyrope can be computed within 2 CPU hours on a single processor PC.

  15. All-electron molecular Dirac-Hartree-Fock calculations - Properties of the XH4 and XH2 molecules and the reaction energy XH4 yields XH2 + H2, X = Si, Ge, Sn, Pb

    Science.gov (United States)

    Dyall, Kenneth G.

    1992-01-01

    Relativistic corrections to a number of properties of the Group IV hydrides are calculated using the Dirac-Hartree-Fock method. The use of first-order perturbation theory is sufficient to obtain relativistic corrections for Ge, but the effects of spin-orbit interaction and other higher-order effects begin to show for Sn and become important for Pb. The energy of the reaction XH4 yields XH2 + H2 (X = Si, Ge, Sn, and Pb) is also calculated. The results are compared with relativistic effective core potential calculations, first-order perturbation theory calculations, and limited experimental data.

  16. Study of superdeformation at zero spin with Skyrme-Hartree-Fock method

    Energy Technology Data Exchange (ETDEWEB)

    Takahara, S.; Tajima, N.; Onishi, N. [Tokyo Univ. (Japan)

    1998-03-01

    Superdeformed (SD) bands have been studied extensively both experimentally and theoretically in the last decade. Since the first observation in {sup 152}Dy in 1986, SD bands have been found in four mass regions, i.e., A {approx} 80, 130, 150 and 190. While these SD bands have been observed only at high spins so far, they may also be present at zero spin like fission isomers in actinide nuclei: The familiar generic argument on the strong shell effect at axis ratio 2:1 does not assume rotations. If non-fissile SD isomers exist at zero spin, they may be utilized to develop new experimental methods to study exotic states, in a similar manner as short-lived high-spin isomers are planned to be utilized as projectiles of fusion reactions in order to populate very high-spin near-yrast states. They will also be useful to test theoretical models whether the models can describe correctly the large deformations of rare-earth nuclei without further complications due to rotations. In this report, we employ the Skyrme-Hartree-Fock method to study the SD states at zero spin. First, we compare various Skyrme force parameter sets to test whether they can reproduce the extrapolated excitation energy of the SD band head of {sup 194}Hg. Second, we systematically search large-deformation solutions with the SkM{sup *} force. The feature of our calculations is that the single-particle wavefunctions are expressed in a three-dimensional-Cartesian-mesh representation. This representation enables one to obtain solutions of various shapes (including SD) without preparing a basis specific to each shape. Solving the mean-field equations in this representation requires, however, a large amount of computation which can be accomplished only with present supercomputers. (author)

  17. Transport properties of isospin asymmetric nuclear matter using the time-dependent Hartree-Fock method

    Science.gov (United States)

    Umar, A. S.; Simenel, C.; Ye, W.

    2017-08-01

    Background: The study of deep-inelastic reactions of nuclei provides a vehicle to explore nuclear transport phenomena for a full range of equilibration dynamics. These investigations provide us the ingredients to model such phenomena and help answer important questions about the nuclear equation of state and its evolution as a function of neutron-to-proton (N /Z ) ratio. Purpose: The motivation is to examine the real-time dynamics of nuclear transport phenomena and its dependence on N /Z asymmetry from a microscopic point of view to avoid any pre-conceived assumptions about the involved processes. Method: The time-dependent Hartree-Fock (TDHF) method in full three dimensions is employed to calculate deep-inelastic reactions of 78Kr+208Pb and 92Kr+208Pb systems at 8.5 MeV/nucleon. The impact parameter and energy-loss dependence of relevant observables are calculated. In addition, the density-constrained TDHF method is used to compute excitation energies of the primary fragments. The statistical deexcitation code gemini is utilized to examine the final reaction products. Results: The kinetic energy loss and sticking times as a function of impact parameter are calculated. The final properties of the fragments (charge, mass, scattering angle, and kinetic energy) are computed. Their evolution as a function of energy loss is studied and various intra-relations are investigated. The fragment excitation energy sharing is computed. Conclusions: We find a smooth dependence of the energy loss, Eloss, on the impact parameter for both systems. However, the transfer properties for low Eloss values are very different for the two systems but become similar in the higher Eloss regime. The mean lifetime of the charge equilibration process, obtained from the final (N -Z )/A value of the fragments, is shown to be ˜0.5 zs. This value is slightly larger than (but of the same order as) the value obtained from reactions at Fermi energies.

  18. Solution of the Skyrme-Hartree-Fock-Bogolyubovequations in the Cartesian deformed harmonic-oscillator basis. (VIII) HFODD (v2.73y): A new version of the program

    Science.gov (United States)

    Schunck, N.; Dobaczewski, J.; Satuła, W.; Bączyk, P.; Dudek, J.; Gao, Y.; Konieczka, M.; Sato, K.; Shi, Y.; Wang, X. B.; Werner, T. R.

    2017-07-01

    We describe the new version (v2.73y) of the code HFODD which solves the nuclear Skyrme Hartree-Fock or Skyrme Hartree-Fock-Bogolyubov problem by using the Cartesian deformed harmonic-oscillator basis. In the new version, we have implemented the following new features: (i) full proton-neutron mixing in the particle-hole channel for Skyrme functionals, (ii) the Gogny force in both particle-hole and particle-particle channels, (iii) linear multi-constraint method at finite temperature, (iv) fission toolkit including the constraint on the number of particles in the neck between two fragments, calculation of the interaction energy between fragments, and calculation of the nuclear and Coulomb energy of each fragment, (v) the new version 200d of the code HFBTHO, together with an enhanced interface between HFBTHO and HFODD, (vi) parallel capabilities, significantly extended by adding several restart options for large-scale jobs, (vii) the Lipkin translational energy correction method with pairing, (viii) higher-order Lipkin particle-number corrections, (ix) interface to a program plotting single-particle energies or Routhians, (x) strong-force isospin-symmetry-breaking terms, and (xi) the Augmented Lagrangian Method for calculations with 3D constraints on angular momentum and isospin. Finally, an important bug related to the calculation of the entropy at finite temperature and several other little significant errors of the previous published version were corrected.

  19. Restricted Hartree Fock using complex-valued orbitals: A long-known but neglected tool in electronic structure theory

    Energy Technology Data Exchange (ETDEWEB)

    Small, David W.; Sundstrom, Eric J.; Head-Gordon, Martin [Department of Chemistry, University of California, Berkeley, California 94720, USA and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)

    2015-01-14

    Restricted Hartree Fock using complex-valued orbitals (cRHF) is studied. We introduce an orbital pairing theorem, with which we obtain a concise connection between cRHF and real-valued RHF, and use it to uncover the close relationship between cRHF, unrestricted Hartree Fock, and generalized valence bond perfect pairing. This enables an intuition for cRHF, contrasting with the generally unintuitive nature of complex orbitals. We also describe an efficient computer implementation of cRHF and its corresponding stability analysis. By applying cRHF to the Be + H{sub 2} insertion reaction, a Woodward-Hoffmann violating reaction, and a symmetry-driven conical intersection, we demonstrate in genuine molecular systems that cRHF is capable of removing certain potential energy surface singularities that plague real-valued RHF and related methods. This complements earlier work that showed this capability in a model system. We also describe how cRHF is the preferred RHF method for certain radicaloid systems like singlet oxygen and antiaromatic molecules. For singlet O{sub 2}, we show that standard methods fail even at the equilibrium geometry. An implication of this work is that, regardless of their individual efficacies, cRHF solutions to the HF equations are fairly commonplace.

  20. Restricted Hartree Fock using complex-valued orbitals: A long-known but neglected tool in electronic structure theory

    Science.gov (United States)

    Small, David W.; Sundstrom, Eric J.; Head-Gordon, Martin

    2015-01-01

    Restricted Hartree Fock using complex-valued orbitals (cRHF) is studied. We introduce an orbital pairing theorem, with which we obtain a concise connection between cRHF and real-valued RHF, and use it to uncover the close relationship between cRHF, unrestricted Hartree Fock, and generalized valence bond perfect pairing. This enables an intuition for cRHF, contrasting with the generally unintuitive nature of complex orbitals. We also describe an efficient computer implementation of cRHF and its corresponding stability analysis. By applying cRHF to the Be + H2 insertion reaction, a Woodward-Hoffmann violating reaction, and a symmetry-driven conical intersection, we demonstrate in genuine molecular systems that cRHF is capable of removing certain potential energy surface singularities that plague real-valued RHF and related methods. This complements earlier work that showed this capability in a model system. We also describe how cRHF is the preferred RHF method for certain radicaloid systems like singlet oxygen and antiaromatic molecules. For singlet O2, we show that standard methods fail even at the equilibrium geometry. An implication of this work is that, regardless of their individual efficacies, cRHF solutions to the HF equations are fairly commonplace.

  1. Influence of the Dirac-Hartree-Fock starting potential on the parity-nonconserving electric-dipole-transition amplitudes in cesium and thallium

    Science.gov (United States)

    Perger, W. F.; Das, B. P.

    1987-01-01

    The parity-nonconserving electric-dipole-transition amplitudes for the 6s1/2-7s1/2 transition in cesium and the 6p1/2-7p1/2 transition in thallium have been calculated by the Dirac-Hartree-Fock method. The effects of using different Dirac-Hartree-Fock atomic core potentials are examined and the transition amplitudes for both the length and velocity gauges are given. It is found that the parity-nonconserving transition amplitudes exhibit a greater dependence on the starting potential for thallium than for cesium.

  2. The Dirac equation in the algebraic approximation. IX. Matrix Dirac-Hartree-Fock calculations for the HeH and BeH ground states using distributed Gaussian basis sets

    NARCIS (Netherlands)

    Quiney, HM; Glushkov, VN; Wilson, S

    2004-01-01

    Using large component basis sets of distributed s-type Gaussian functions with positions and exponents optimized so as to support Hartree-Fock total energies with an accuracy approaching the sub-muhartree level, Dirac-Hartree-Fock-Coulomb calculations are reported for the ground states of the

  3. The dirac equation in the algebraic approximation : VIII. Comparison of finite basis set and finite element molecular Dirac-Hartree-Fock calculations for the H-2, LiH, and BH ground states

    NARCIS (Netherlands)

    Quiney, HM; Glushkov, VN; Wilson, S

    2002-01-01

    Using basis sets of distributed s-type Gaussian functions with positions and exponents optimized so as to support Hartree-Fock total energies with an accuracy approaching the sub-muHartree level, Dirac-Hartree-Fock-Coulomb calculations are reported for the ground states of the H-2, LiH, and BH

  4. Improvement of one-nucleon removal and total reaction cross sections in the Liège intranuclear-cascade model using Hartree-Fock-Bogoliubov calculations

    Science.gov (United States)

    Rodríguez-Sánchez, Jose Luis; David, Jean-Christophe; Mancusi, Davide; Boudard, Alain; Cugnon, Joseph; Leray, Sylvie

    2017-11-01

    The prediction of one-nucleon-removal cross sections by the Liège intranuclear-cascade model has been improved using a refined description of the matter and energy densities in the nuclear surface. Hartree-Fock-Bogoliubov calculations with the Skyrme interaction are used to obtain a more realistic description of the radial-density distributions of protons and neutrons, as well as the excitation-energy uncorrelation at the nuclear surface due to quantum effects and short-range correlations. The results are compared with experimental data covering a large range of nuclei, from carbon to uranium, and projectile kinetic energies. We find that the new approach is in good agreement with experimental data of one-nucleon-removal cross sections covering a broad range in nuclei and energies. The new ingredients also improve the description of total reaction cross sections induced by protons at low energies, the production cross sections of heaviest residues close to the projectile, and the triple-differential cross sections for one-proton removal. However, other observables such as quadruple-differential cross sections of coincident protons do not present any sizable sensitivity to the new approach. Finally, the model is also tested for light-ion-induced reactions. It is shown that the new parameters can give a reasonable description of the nucleus-nucleus total reaction cross sections at high energies.

  5. Solution of the Skyrme Hartree Fock Bogolyubov equations in the Cartesian deformed harmonic-oscillator basis. (V) HFODD(v2.08k)

    Science.gov (United States)

    Dobaczewski, J.; Olbratowski, P.

    2005-05-01

    We describe the new version (v2.08k) of the code HFODD which solves the nuclear Skyrme-Hartree-Fock or Skyrme-Hartree-Fock-Bogolyubov problem by using the Cartesian deformed harmonic-oscillator basis. Similarly as in the previous version (v2.08i), all symmetries can be broken, which allows for calculations with angular frequency and angular momentum tilted with respect to the mass distribution. In the new version, three minor errors have been corrected. New Version Program SummaryTitle of program: HFODD; version: 2.08k Catalogue number: ADVA Catalogue number of previous version: ADTO (Comput. Phys. Comm. 158 (2004) 158) Program summary URL:http://cpc.cs.qub.ac.uk/summaries/ADVA Program obtainable from: CPC Program Library, Queen's University of Belfast, N. Ireland Does the new version supersede the previous one: yes Computers on which this or another recent version has been tested: SG Power Challenge L, Pentium-II, Pentium-III, AMD-Athlon Operating systems under which the program has been tested: UNIX, LINUX, Windows-2000 Programming language used: Fortran Memory required to execute with typical data: 10M words No. of bits in a word: 64 No. of lines in distributed program, including test data, etc.: 52 631 No. of bytes in distributed program, including test data, etc.: 266 885 Distribution format:tar.gz Nature of physical problem: The nuclear mean-field and an analysis of its symmetries in realistic cases are the main ingredients of a description of nuclear states. Within the Local Density Approximation, or for a zero-range velocity-dependent Skyrme interaction, the nuclear mean-field is local and velocity dependent. The locality allows for an effective and fast solution of the self-consistent Hartree-Fock equations, even for heavy nuclei, and for various nucleonic ( n-particle n-hole) configurations, deformations, excitation energies, or angular momenta. Similar Local Density Approximation in the particle-particle channel, which is equivalent to using a zero

  6. Hartree-Fock study on the lower excited states of a Cu+ impurity in NaF using large embedded clusters

    NARCIS (Netherlands)

    Linker, G.J.; Broer, R.; Nieuwpoort, W.C.

    1996-01-01

    We report spin-restricted and symmetry-restricted Hartree-Fock cluster calculations on the lower excited states of a Cu+ impurity in NaF in order to investigate their dependence on cluster size. In contrast to previous work on smaller clusters, we found all states arising from the configurations

  7. A new representation of the many body wave function and its application as a post Hartree-Fock energy variation method

    OpenAIRE

    Uemura, Wataru

    2011-01-01

    In this paper, we introduce a new representation of many body electron wave function and a few calculation results of the ground state energies of many body systems using that representation, which is systematically better than the Hartree-Fock approximation.

  8. Self-consistent-field (SCF) and multiconfiguration (MC) Hartree-Fock (HF) methods in atomic calculations: Numerical integration approaches

    Science.gov (United States)

    Fischer, Charlotte Froese

    1986-06-01

    The self-consistent field (SCF) and multiconfiguration (MC) Hartree-Fock (HF) methods are reviewed. The emphasis is on the specification, design and implementation of these methods as a part of an atomic structure software package, dealing with wavefunction determination. Numerical integration approaches will be used throughout. After outlining a class of MCHF problems, the derivation of the MCHF equations is reviewed and some theory developed on the variation of the energy functional with respect to a rotation of the orbital basis among orbitals of the same symmetry. Various procedures are proposed and evaluated for dealing with cases where the radial basis for a given total energy is not unique. A numerical MC SCF procedure is described using a top-down approach. The overall algorithm will be outlined first with numerical details provided later. Finally some test cases are proposed.

  9. Collective excitations of a dilute Bose gas at finite temperature: time dependent Hartree-Fock-Bogoliubov theory

    Science.gov (United States)

    Boudjemâa, Abdelâali; Guebli, Nadia

    2017-10-01

    Using the time-dependent Hartree-Fock-Bogoliubov approach, where the condensate is coupled with the thermal cloud and the anomalous density, we study the equilibrium and the dynamical properties of three-dimensional quantum-degenerate Bose gas at finite temperature. Effects of the anomalous correlations on the condensed fraction and the critical temperature are discussed. In uniform Bose gas, useful expressions for the Bogoliubov excitations spectrum, the first and second sound, the condensate depletion and the superfluid fraction are derived. Our results are tested by comparing the findings computed by quantum Monte Carlo simulations. We present also a systematic investigation of the collective modes of a Bose condensate confined in an external trap. Our predictions are in qualitative agreement with previous experimental and theoretical results. We show in particular that our theory is capable of explaining the so-called anomalous behavior of the m=0 mode.

  10. Solution of the Skyrme-Hartree-Fock equations in the Cartesian deformed harmonic oscillator basis. (II) the program HFODD

    Energy Technology Data Exchange (ETDEWEB)

    Dobaczewski, J.; Dudek, J. [Strasbourg-1 Univ., 67 (France). Centre de Recherches Nucleaires; Dobaczewski, J. [Warsaw Univ. (Poland)

    1996-12-31

    We describe the code HFODD which solves the nuclear Skyrme-Hartree-Fock problem by using the deformed Cartesian harmonic oscillator basis. The user has a possibility of choosing among various symmetries of the nuclear HF problem for rotating or non-rotating nuclei; they vary from the non-axial parity-invariant nuclear shapes, through those also breaking the intrinsic parity, towards the least-restrictive case corresponding to only one symmetry plane. The code provides a solution for a complete superdeformed rotational band in an A{approx}150 nucleus within one CPU hour of the CRAY C-90 supercomputer or within two-three CPU hours of a fast workstation. (authors). 22 refs.

  11. Assessment of Time-dependent Unrestricted Hartree-Fock Method for Electron Dynamics in Intense Laser Fields

    Science.gov (United States)

    Sato, Takeshi; Ishikawa, Kenichi L.

    Time-dependent restricted and unrestricted Hartree-Fock (TD-RHF and TD-UHF) methods are comparatively assessed for the description of the electron dynamics in intense laser fields. These methods are applied to the one-dimensional H2 molecule exposed to an intense laser field, and compared to the results from the time-dependent Schrödinger (TDSE) equation. Around the equilibrium interatomic distance, where the initial RHF and UHF wavefunctions coincide, TD-UHF keeps an initial closed-shell, thus underestimates large amplitude electron motions. At a longer interatomic distance, where the UHF wavefunction differs from the RHF one, TD-UHF better reprodeces the TDSE result than TD-RHF does.

  12. Density functional theory, restricted Hartree - Fock simulations and FTIR, FT-Raman and UV-Vis spectroscopic studies on lamotrigine

    Science.gov (United States)

    Ramya, T.; Gunasekaran, S.; Ramkumaar, G. R.

    2013-10-01

    The Fourier Transform Infrared (FTIR) and FT Raman spectra of lamotrigine have been recorded in the region 4000-450 cm-1 and 4000-50 cm-1, respectively. The title compound is used as Antiepileptic drug. The optimized geometry, frequency, and intensities of the vibrational bands of the lamotrigine were obtained by Density Functional Theory (DFT) using B3LYP/631G** basis set and ab initio method at the restricted Hartree Fock/6-31** level. The harmonic vibrational frequencies, Natural population analysis, HOMO-LUMO energy gap, infra red intensities and Raman scattering activities, force constant were calculated by DFT and RHF methods. The quality of lamotrigine under different storage containers were analyzed using UV-Vis spectral technique.

  13. Coupled Perturbed Hartree-Fock Calculation of the Static Polarizability for Periodic Systems: Implementation in the CRYSTAL Code

    Science.gov (United States)

    Ferrero, M.; Rérat, Michel; Orlando, R.; Dovesi, R.

    2007-12-01

    The Coupled Perturbed Hartree-Fock (CPHF) scheme has been implemented in CRYSTAL06, periodic ab initio computer code that uses a gaussian type basis set, in order to obtain the polarizability of crystalline systems (3D), slabs (2D), polymers (1D) and, as a limiting case, molecules (0D). The formulation is presented, together with applications referring to diamond, silicon and SiC. It turns out that, for a given hamiltonian and basis set, high numerical accuracy can be achieved at relatively low cost compared to the Finite Field perturbation method (FF), that uses a saw-tooth electric potential. Correctness of the CPHF results was tested with reference to FF calculations with CRYSTAL.

  14. Arbitrary Angular Momentum Electron Repulsion Integrals with Graphical Processing Units: Application to the Resolution of Identity Hartree-Fock Method.

    Science.gov (United States)

    Kalinowski, Jaroslaw; Wennmohs, Frank; Neese, Frank

    2017-07-11

    A resolution of identity based implementation of the Hartree-Fock method on graphical processing units (GPUs) is presented that is capable of handling basis functions with arbitrary angular momentum. For practical reasons, only functions up to (ff|f) angular momentum are presently calculated on the GPU, thus leaving the calculation of higher angular momenta integrals on the CPU of the hybrid CPU-GPU environment. Speedups of up to a factor of 30 are demonstrated relative to state-of-the-art serial and parallel CPU implementations. Benchmark calculations with over 3500 contracted basis functions (def2-SVP or def2-TZVP basis sets) are reported. The presented implementation supports all devices with OpenCL support and is capable of utilizing multiple GPU cards over either MPI or OpenCL itself.

  15. MOLECULAR OPEN-SHELL CONFIGURATION-INTERACTION CALCULATIONS USING THE DIRAC-COULOMB HAMILTONIAN - THE F6-MANIFOLD OF AN EMBEDDED EUO69- CLUSTER

    NARCIS (Netherlands)

    VISSER, O; VISSCHER, L; AERTS, PJC; NIEUWPOORT, WC

    1992-01-01

    We present results of all-electron molecular relativistic (Hartree-Fock-Dirac) and nonrelativistic (Hartree-Fock) calculations followed by a complete open shell configuration interaction (COSCI) calculation on an EuO6(9-) cluster in a Ba2GdNbO6 crystal. The results include the calculated energies of

  16. Finite-temperature coupled-cluster, many-body perturbation, and restricted and unrestricted Hartree-Fock study on one-dimensional solids: Luttinger liquids, Peierls transitions, and spin- and charge-density waves

    Science.gov (United States)

    Hermes, Matthew R.; Hirata, So

    2015-09-01

    One-dimensional (1D) solids exhibit a number of striking electronic structures including charge-density wave (CDW) and spin-density wave (SDW). Also, the Peierls theorem states that at zero temperature, a 1D system predicted by simple band theory to be a metal will spontaneously dimerize and open a finite fundamental bandgap, while at higher temperatures, it will assume the equidistant geometry with zero bandgap (a Peierls transition). We computationally study these unique electronic structures and transition in polyyne and all-trans polyacetylene using finite-temperature generalizations of ab initio spin-unrestricted Hartree-Fock (UHF) and spin-restricted coupled-cluster doubles (CCD) theories, extending upon previous work [He et al., J. Chem. Phys. 140, 024702 (2014)] that is based on spin-restricted Hartree-Fock (RHF) and second-order many-body perturbation (MP2) theories. Unlike RHF, UHF can predict SDW as well as CDW and metallic states, and unlike MP2, CCD does not diverge even if the underlying RHF reference wave function is metallic. UHF predicts a gapped SDW state with no dimerization at low temperatures, which gradually becomes metallic as the temperature is raised. CCD, meanwhile, confirms that electron correlation lowers the Peierls transition temperature. Furthermore, we show that the results from all theories for both polymers are subject to a unified interpretation in terms of the UHF solutions to the Hubbard-Peierls model using different values of the electron-electron interaction strength, U/t, in its Hamiltonian. The CCD wave function is shown to encompass the form of the exact solution of the Tomonaga-Luttinger model and is thus expected to describe accurately the electronic structure of Luttinger liquids.

  17. Multiconfiguration Dirac-Hartree-Fock energy levels, oscillator strengths, transition probabilities, hyperfine constants and Landé g-factor of intermediate Rydberg series in neutral argon atom

    Science.gov (United States)

    Salah, Wa'el; Hassouneh, Ola

    2017-04-01

    We computed the energy levels, oscillator strengths f_{ij}, the radiative transition rates A_{ij}, the Landé g -factor, the magnetic dipole moment and the electric quadrupole hyperfine constants of the intermediate Rydberg series ns [k]J ( 4 ≤ n ≤ 6), nd [k]J (3 ≤ n ≤ 4), np [k]J (4 ≤ n ≤ 5) relative to the ground state 3p6 1S0 for neutral argon atom spectra. The values are obtained in the framework of the multiconfiguration Dirac-Hartree-Fock (MCDHF) approach. In this approach, Breit interaction, leading quantum electrodynamics (QED) effects and self-energy correction are taken into account. Moreover, these spectroscopic parameters have been calculated for many levels belonging to the configuration 3p54s, 3p55s, 3p56s, 3p53d, 3p54d, 3p54p, 3p55p as well as for transitions between levels 3p54s-3p54p, 3p54p-3p53d, 3p54p-3p55s, 3p55s-3p55p and 3p55p-3p56s. The large majority of the lines from the 4p-5s and 4p-3d, 5s-5p and 5p-6s transition arrays have been observed and the calculations are consistent with the J -file-sum rule. The obtained theoretical values are compared with previous experimental and theoretical data available in the literature. An overall satisfactory agreement is noticed allowing assessing the reliability of our data.

  18. Extension of the source-sink potential approach to Hartree-Fock and density functional theory: A new tool to visualize the ballistic current through molecules

    Science.gov (United States)

    Fias, Stijn; Stuyver, Thijs

    2017-11-01

    The recent source and sink potential approach by Pickup et al. [J. Chem. Phys. 143, 194105 (2015)] is extended to Hartree-Fock and density functional theory, allowing the calculation of the transmission and the visualization of ballistic currents through molecules at these levels of theory. This visualization allows the study of the transmission process in real-space, providing an important tool to better understand the conduction process.

  19. Relativistic effects on linear and nonlinear polarizabilities studied by effective-core potential, Douglas-Kroll, and Dirac-Hartree-Fock response theory

    DEFF Research Database (Denmark)

    Norman, Patrick; Schimmelpfennig, Bernd; Ruud, Kenneth

    2002-01-01

    A systematic investigation of a hierarchy of methods for including relativistic effects in the calculation of linear and nonlinear optical properties was carried out. The simple ECP method and the more involved spin-averaged Douglas-Kroll approximation were compared to benchmark results obtained ...... with the time-dependent Dirac-Hartree-Fock method. It was found that in many cases, the performance of the ECP method exceeds its rank....

  20. Spin polarization, orbital occupation and band gap opening in vanadium dioxide: The effect of screened Hartree-Fock exchange

    KAUST Repository

    Wang, Hao

    2014-07-01

    The metal-insulator transition of VO2 so far has evaded an accurate description by density functional theory. The screened hybrid functional of Heyd, Scuseria and Ernzerhof leads to reasonable solutions for both the low-temperature monoclinic and high-temperature rutile phases only if spin polarization is excluded from the calculations. We explore whether a satisfactory agreement with experiment can be achieved by tuning the fraction of Hartree Fock exchange (α) in the density functional. It is found that two branches of locally stable solutions exist for the rutile phase for 12.5%≤α≤20%. One is metallic and has the correct stability as compared to the monoclinic phase, the other is insulating with lower energy than the metallic branch. We discuss these observations based on the V 3d orbital occupations and conclude that α=10% is the best possible choice for spin-polarized VO2 calculations. © 2014 Elsevier B.V. All rights reserved.

  1. Spiral magnetism in the single-band Hubbard model: the Hartree-Fock and slave-boson approaches.

    Science.gov (United States)

    Igoshev, P A; Timirgazin, M A; Gilmutdinov, V F; Arzhnikov, A K; Irkhin, V Yu

    2015-11-11

    The ground-state magnetic phase diagram is investigated within the single-band Hubbard model for square and different cubic lattices. The results of employing the generalized non-correlated mean-field (Hartree-Fock) approximation and generalized slave-boson approach by Kotliar and Ruckenstein with correlation effects included are compared. We take into account commensurate ferromagnetic, antiferromagnetic, and incommensurate (spiral) magnetic phases, as well as phase separation into magnetic phases of different types, which was often lacking in previous investigations. It is found that the spiral states and especially ferromagnetism are generally strongly suppressed up to non-realistically large Hubbard U by the correlation effects if nesting is absent and van Hove singularities are well away from the paramagnetic phase Fermi level. The magnetic phase separation plays an important role in the formation of magnetic states, the corresponding phase regions being especially wide in the vicinity of half-filling. The details of non-collinear and collinear magnetic ordering for different cubic lattices are discussed.

  2. Crystal orbital calculation of coupled-perturbed Hartree-Fock dynamic (hyper)polarizabilities for polydiacetylene and polybutatriene

    Science.gov (United States)

    Gu, Feng Long; Aoki, Yuriko; Bishop, David M.

    2002-07-01

    Crystal orbital coupled-perturbed Hartree-Fock static and dynamic (hyper)polarizabilities for polydiacetylene (PDA) and polybutatriene (PBT) are computed. Geometry effects have been investigated. The static CPHF/6-31G second-order hyperpolarizability of PBT is 67 times larger than that of PDA using the optimized geometries at the HF/6-31G level. However, this factor is reduced to 17 with the optimized geometries at the MP2/6-311G* level. One of the bond length alternations (BLA), the difference between the single and double bond lengths (S/D), of PDA is the most sensitive factor for the (hyper)polarizabilities. It has been shown from the calculations that a smaller S/D produces a larger polarizability and second-order hyperpolarizability of PDA. Unlike PDA, two different BLAs of PBT are competing to change the values of polarizability and second-order hyperpolarizability. The dynamic second-order hyperpolarizabilities have been checked with the general dispersion expression by fitting the results to a polynomial. Our theoretical results can also be compared with experiment and possible reasons for the discrepancies are addressed.

  3. Molecular wave function and effective adiabatic potentials calculated by extended multi-configuration time-dependent Hartree-Fock method

    Energy Technology Data Exchange (ETDEWEB)

    Kato, Tsuyoshi; Ide, Yoshihiro; Yamanouchi, Kaoru [Department of Chemistry, School of Science, The University of Tokyo, 7-3-1, Hongo Bunkyo-ku, Tokyo, 113-0033 (Japan)

    2015-12-31

    We first calculate the ground-state molecular wave function of 1D model H{sub 2} molecule by solving the coupled equations of motion formulated in the extended multi-configuration time-dependent Hartree-Fock (MCTDHF) method by the imaginary time propagation. From the comparisons with the results obtained by the Born-Huang (BH) expansion method as well as with the exact wave function, we observe that the memory size required in the extended MCTDHF method is about two orders of magnitude smaller than in the BH expansion method to achieve the same accuracy for the total energy. Second, in order to provide a theoretical means to understand dynamical behavior of the wave function, we propose to define effective adiabatic potential functions and compare them with the conventional adiabatic electronic potentials, although the notion of the adiabatic potentials is not used in the extended MCTDHF approach. From the comparison, we conclude that by calculating the effective potentials we may be able to predict the energy differences among electronic states even for a time-dependent system, e.g., time-dependent excitation energies, which would be difficult to be estimated within the BH expansion approach.

  4. Transferability and accuracy by combining dispersionless density functional and incremental post-Hartree-Fock theories: Noble gases adsorption on coronene/graphene/graphite surfaces.

    Science.gov (United States)

    de Lara-Castells, María Pilar; Bartolomei, Massimiliano; Mitrushchenkov, Alexander O; Stoll, Hermann

    2015-11-21

    The accuracy and transferability of the electronic structure approach combining dispersionless density functional theory (DFT) [K. Pernal et al., Phys. Rev. Lett. 103, 263201 (2009)] with the method of increments [H. Stoll, J. Chem. Phys. 97, 8449 (1992)], are validated for the interaction between the noble-gas Ne, Ar, Kr, and Xe atoms and coronene/graphene/graphite surfaces. This approach uses the method of increments for surface cluster models to extract intermonomer dispersion-like (2- and 3-body) correlation terms at coupled cluster singles and doubles and perturbative triples level, while periodic dispersionless density functionals calculations are performed to estimate the sum of Hartree-Fock and intramonomer correlation contributions. Dispersion energy contributions are also obtained using DFT-based symmetry-adapted perturbation theory [SAPT(DFT)]. An analysis of the structure of the X/surface (X = Ne, Ar, Kr, and Xe) interaction energies shows the excellent transferability properties of the leading intermonomer correlation contributions across the sequence of noble-gas atoms, which are also discussed using the Drude oscillator model. We further compare these results with van der Waals-(vdW)-corrected DFT-based approaches. As a test of accuracy, the energies of the low-lying nuclear bound states supported by the laterally averaged X/graphite potentials (X = (3)He, (4)He, Ne, Ar, Kr, and Xe) are calculated and compared with the best estimations from experimental measurements and an atom-bond potential model using the ab initio-assisted fine-tuning of semiempirical parameters. The bound-state energies determined differ by less than 6-7 meV (6%) from the atom-bond potential model. The crucial importance of including incremental 3-body dispersion-type terms is clearly demonstrated, showing that the SAPT(DFT) approach effectively account for these terms. With the deviations from the best experimental-based estimations smaller than 2.3 meV (1.9%), the accuracy of

  5. Transferability and accuracy by combining dispersionless density functional and incremental post-Hartree-Fock theories: Noble gases adsorption on coronene/graphene/graphite surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Lara-Castells, María Pilar de, E-mail: Pilar.deLara.Castells@csic.es; Bartolomei, Massimiliano [Instituto de Física Fundamental (C.S.I.C.), Serrano 123, E-28006 Madrid (Spain); Mitrushchenkov, Alexander O. [Laboratoire Modélisation et Simulation Multi Echelle, Université Paris-Est, MSME UMR 8208 CNRS, 5 bd Descartes, 77454 Marne-la-Vallée (France); Stoll, Hermann [Institut für Theoretische Chemie, Universität Stuttgart, D-70550 Stuttgart (Germany)

    2015-11-21

    The accuracy and transferability of the electronic structure approach combining dispersionless density functional theory (DFT) [K. Pernal et al., Phys. Rev. Lett. 103, 263201 (2009)] with the method of increments [H. Stoll, J. Chem. Phys. 97, 8449 (1992)], are validated for the interaction between the noble-gas Ne, Ar, Kr, and Xe atoms and coronene/graphene/graphite surfaces. This approach uses the method of increments for surface cluster models to extract intermonomer dispersion-like (2- and 3-body) correlation terms at coupled cluster singles and doubles and perturbative triples level, while periodic dispersionless density functionals calculations are performed to estimate the sum of Hartree-Fock and intramonomer correlation contributions. Dispersion energy contributions are also obtained using DFT-based symmetry-adapted perturbation theory [SAPT(DFT)]. An analysis of the structure of the X/surface (X = Ne, Ar, Kr, and Xe) interaction energies shows the excellent transferability properties of the leading intermonomer correlation contributions across the sequence of noble-gas atoms, which are also discussed using the Drude oscillator model. We further compare these results with van der Waals-(vdW)-corrected DFT-based approaches. As a test of accuracy, the energies of the low-lying nuclear bound states supported by the laterally averaged X/graphite potentials (X = {sup 3}He, {sup 4}He, Ne, Ar, Kr, and Xe) are calculated and compared with the best estimations from experimental measurements and an atom-bond potential model using the ab initio-assisted fine-tuning of semiempirical parameters. The bound-state energies determined differ by less than 6–7 meV (6%) from the atom-bond potential model. The crucial importance of including incremental 3-body dispersion-type terms is clearly demonstrated, showing that the SAPT(DFT) approach effectively account for these terms. With the deviations from the best experimental-based estimations smaller than 2.3 meV (1.9%), the

  6. Clustered Low-Rank Tensor Format: Introduction and Application to Fast Construction of Hartree-Fock Exchange.

    Science.gov (United States)

    Lewis, Cannada A; Calvin, Justus A; Valeev, Edward F

    2016-12-13

    We describe the clustered low-rank (CLR) framework for block-sparse and block-low-rank tensor representation and computation. The CLR framework exploits the tensor structure revealed by basis clustering; computational savings arise from low-rank compression of tensor blocks and performing block arithmetic in the low-rank form whenever beneficial. The precision is rigorously controlled by two parameters, avoiding ad-hoc heuristics, such as domains: one controls the CLR block rank truncation, and the other controls screening of small contributions in arithmetic operations on CLR tensors to propagate sparsity through expressions. As these parameters approach zero, the CLR representation and arithmetic become exact. As a pilot application, we considered the use of the CLR format for the order-2 and order-3 tensors in the context of the density fitting (DF) evaluation of the Hartree-Fock (exact) exchange (DF-K). Even for small systems and realistic basis sets, CLR-DF-K becomes more efficient than the standard DF-K approach, and it has significantly reduced asymptotic storage and computational complexities relative to the standard [Formula: see text] and [Formula: see text] DF-K figures. CLR-DF-K is also significantly more efficient-all while negligibly affecting molecular energies and properties-than the conventional (non-DF) [Formula: see text] exchange algorithm for applications to medium-sized systems (on the order of 100 atoms) with diffuse Gaussian basis sets, a necessity for applications to negatively charged species, molecular properties, and high-accuracy correlated wave functions.

  7. The positronium and the dipositronium in a Hartree-Fock approximation of quantum electrodynamics

    DEFF Research Database (Denmark)

    Sok, Jérémy Vithya

    2016-01-01

    The Bogoliubov-Dirac-Fock (BDF) model is a no-photon approximation of quantum electrodynamics. It allows to study relativistic electrons in interaction with the Dirac sea. A state is fully characterized by its one-body density matrix, an infinite rank non-negative projector. We prove the existenc...

  8. Gauge-Origin Independent Formulation and Implementation of Magneto-Optical Activity within Atomic-Orbital-Density Based Hartree-Fock and Kohn-Sham Response Theories

    DEFF Research Database (Denmark)

    Kjærgaard, Thomas; Jørgensen, Poul; Thorvaldsen, Andreas

    2009-01-01

    -orbital density-matrix based formulation of response theory and use London atomic orbitals to parametrize the magnetic field dependence. It yields a computational procedure which is both gauge-origin independent and suitable for linear-scaling at the level of time-dependent Hartree-Fock and density functional...... theory. The formulation includes a modified preconditioned conjugated gradient algorithm, which projects out the excited state component from the solution to the linear response equation. This is required when solving one of the response equations for the determination of the B term and divergence...

  9. EOMCC over excited state Hartree-Fock solutions (ESHF-EOMCC: An efficient approach for the entire ground state potential energy curves of higher-order bonds

    Directory of Open Access Journals (Sweden)

    Y. Sajeev

    2015-08-01

    Full Text Available The equation-of-motion coupled cluster (EOMCC method based on the excited state Hartree-Fock (ESHF solutions is shown to be appropriate for computing the entire ground state potential energy curves of strongly correlated higher-order bonds. The new approach is best illustrated for the homolytic dissociation of higher-order bonds in molecules. The required multireference character of the true ground state wavefunction is introduced through the linear excitation operator of the EOMCC method. Even at the singles and doubles level of cluster excitation truncation, the nonparallelity error of the ground state potential energy curve from the ESHF based EOMCC method is small.

  10. Computation of Second Harmonic Generation for Crystalline Urea and KDP. An ab Initio Approach through the Coupled Perturbed Hartree-Fock/Kohn-Sham Scheme.

    Science.gov (United States)

    Rérat, Michel; Maschio, Lorenzo; Kirtman, Bernard; Civalleri, Bartolomeo; Dovesi, Roberto

    2016-01-12

    The electronic second harmonic generation (SHG) tensor, d, of crystalline urea and potassium dihydrogen phosphate (KDP) is evaluated as a function of frequency using a Gaussian type basis set and the Coupled Perturbed Hartree-Fock (CPHF) and Kohn-Sham (CPKS) schemes as implemented in the CRYSTAL code. The results of various functionals, including LDA, GGA (PBE), and global and range-separated hybrids (B3LYP, PBE0, LC-BLYP), as well as Hartree-Fock, are compared. It is found that the calculated SHG intensity always decreases as the percentage of exact exchange increases. The hybrid functionals turn out to provide results that agree well with experiment. For urea and KDP the percentage of exact exchange determined by the inverse dielectric constant is too large. At 1064 nm the vibrational contribution for urea is found to be less than 5% of the total value. To the authors' knowledge, this is the first coupled (self-consistent) calculation of SHG for any periodic system.

  11. Axially deformed solution of the Skyrme-Hartree-Fock-Bogolyubov equations using the transformed harmonic oscillator basis (III) HFBTHO (v3.00): A new version of the program

    Science.gov (United States)

    Perez, R. Navarro; Schunck, N.; Lasseri, R.-D.; Zhang, C.; Sarich, J.

    2017-11-01

    intrinsic densities. In the present version of HFBTHO, the energy density derives either from the zero-range Skyrme or the finite-range Gogny effective two-body interaction between nucleons. Nuclear super-fluidity is treated at the Hartree-Fock-Bogolyubov (HFB) approximation. Constraints on the nuclear shape allows probing the potential energy surface of the nucleus as needed e.g., for the description of shape isomers or fission. The implementation of a local scale transformation of the single-particle basis in which the HFB solutions are expanded provide a tool to properly compute the structure of weakly-bound nuclei. Solution method: The program uses the axial Transformed Harmonic Oscillator (THO) single-particle basis to expand quasiparticle wave functions. It iteratively diagonalizes the Hartree-Fock-Bogolyubov Hamiltonian based on generalized Skyrme-like energy densities and zero-range pairing interactions or the finite-range Gogny force until a self-consistent solution is found. A previous version of the program was presented in M.V. Stoitsov, N. Schunck, M. Kortelainen, N. Michel, H. Nam, E. Olsen, J. Sarich, and S. Wild, Comput. Phys. Commun. 184 (2013) 1592-1604 with much of the formalism presented in the original paper M.V. Stoitsov, J. Dobaczewski, W. Nazarewicz, P. Ring, Comput. Phys. Commun. 167 (2005) 43-63. Additional comments: The user must have access to (i) the LAPACK subroutines DSYEEVR, DSYEVD, DSYTRF and DSYTRI, and their dependencies, which compute eigenvalues and eigenfunctions of real symmetric matrices, (ii) the LAPACK subroutines DGETRI and DGETRF, which invert arbitrary real matrices, and (iii) the BLAS routines DCOPY, DSCAL, DGEMM and DGEMV for double-precision linear algebra (or provide another set of subroutines that can perform such tasks). The BLAS and LAPACK subroutines can be obtained from the Netlib Repository at the University of Tennessee, Knoxville: http://netlib2.cs.utk.edu/.

  12. Spin contamination analogy, Kramers pairs symmetry and spin density representations at the 2-component unrestricted Hartree-Fock level of theory

    KAUST Repository

    Bučinský, Lukáš

    2015-05-11

    "Kramers pairs symmetry breaking" is evaluated at the 2-component (2c) Kramers unrestricted and/or general complex Hartree-Fock (GCHF) level of theory, and its analogy with "spin contamination" at the 1-component (1c) unrestricted Hartree-Fock (UHF) level of theory is emphasized. The GCHF "Kramers pairs symmetry breaking" evaluation is using the square of overlaps between the set of occupied spinorbitals with the projected set of Kramers pairs. In the same fashion, overlaps between α and β orbitals are used in the evaluation of "spin contamination" at the UHF level of theory. In this manner, UHF Š2 expectation value is made formally extended to the GCHF case. The directly evaluated GCHF expectation value of the Š2 operator is considered for completeness. It is found that the 2c GCHF Kramers pairs symmetry breaking has a very similar extent in comparison to the 1c UHF spin contamination. Thus higher excited states contributions to the 1c and 2c unrestricted wave functions of open shell systems have almost the same extent and physical consequences. Moreover, it is formally shown that a single determinant wave function in the restricted open shell Kramers case has the expectation value of K2 operator equal to the negative number of open shell electrons, while the eigenvalue of K2 for the series of simple systems (H, He, He*-triplet, Li and Li*-quartet) are found to be equal to minus the square of the number of open shell electrons. The concept of unpaired electron density is extended to the GCHF regime and compared to UHF and restricted open shell Hartree-Fock spin density. The "collinear" and "noncollinear" analogs of spin density at the GCHF level of theory are considered as well. Spin contamination and/or Kramers pairs symmetry breaking, spin populations and spin densities are considered for H2O+, Cl, HCl+, phenoxyl radical (C6H5O) as well as for Cu, Cu2+, Fe and the [OsCl5(1H-pyrazole)]- anion. The 1c and 2c unpaired electron density representation is found

  13. Aufbau derived from a unified treatment of occupation numbers in Hartree-Fock, Kohn-Sham and Natural Orbital theories with the Karush-Kuhn-Tucker conditions for the inequality constraints ni≤1 and ni≥0

    NARCIS (Netherlands)

    Giesbertz, K.J.H.; Baerends, E.J.

    2010-01-01

    In the major independent particle models of electronic structure theory-Hartree-Fock, Kohn-Sham (KS), and natural orbital (NO) theories-occupations are constrained to 0 and 1 or to the interval [0,1]. We carry out a constrained optimization of the orbitals and occupation numbers with application of

  14. Magnetic state of K0.8Fe1.6Se2 from a five-orbital Hubbard model in the Hartree-Fock approximation

    Energy Technology Data Exchange (ETDEWEB)

    Luo, Qinlong [ORNL; Nicholson, Andrew D [ORNL; Riera, J. A. [Universidad Nacional de Rosario; Yao, Dao-Xin [Sun Yat-Sen University, Guangzhou, China; Moreo, Adriana [ORNL; Dagotto, Elbio R [ORNL

    2011-01-01

    Motivated by the recent discovery of Fe-based superconductors close to an antiferromagnetic insulator in the experimental phase diagram, here the five-orbital Hubbard model (without lattice distortions) is studied using the real-space Hartree-Fock approximation, employing a 10 10 Fe cluster with Fe vacancies in a5 5 pattern. Varying the Hubbard and Hund couplings, and at electronic density n = 6.0, the phase diagram contains an insulating state with the same spin pattern as observed experimentally, involving 2 2 ferromagnetic plaquettes coupled with one another antiferromagnetically. The presence of local ferromagnetic tendencies is in qualitative agreement with Lanczos results for the three-orbital model also reported here. The magnetic moment 3 B /Fe is in good agreement with experiments. Several other phases are also stabilized in the phase diagram, in agreement with recent calculations using phenomenological models.

  15. Density functional theory, restricted Hartree-Fock simulations and FTIR, FT-Raman and UV-Vis spectroscopic studies on lamotrigine.

    Science.gov (United States)

    Ramya, T; Gunasekaran, S; Ramkumaar, G R

    2013-10-01

    The Fourier Transform Infrared (FTIR) and FT Raman spectra of lamotrigine have been recorded in the region 4000-450 cm(-1) and 4000-50 cm(-1), respectively. The title compound is used as Antiepileptic drug. The optimized geometry, frequency, and intensities of the vibrational bands of the lamotrigine were obtained by Density Functional Theory (DFT) using B3LYP/631G** basis set and ab initio method at the restricted Hartree Fock/6-31** level. The harmonic vibrational frequencies, Natural population analysis, HOMO-LUMO energy gap, infra red intensities and Raman scattering activities, force constant were calculated by DFT and RHF methods. The quality of lamotrigine under different storage containers were analyzed using UV-Vis spectral technique. Copyright © 2013 Elsevier B.V. All rights reserved.

  16. Molecular structures and vibrational frequencies of xanthine and its methyl derivatives (caffeine and theobromine) by ab initio Hartree-Fock and density functional theory calculations

    Science.gov (United States)

    Ucun, Fatih; Sağlam, Adnan; Güçlü, Vesile

    2007-06-01

    The molecular structures, vibrational frequencies and corresponding vibrational assignments of xanthine and its methyl derivatives (caffeine and theobromine) have been calculated using ab initio Hartree-Fock (HF) and density functional theory (B3LYP) methods with 6-31G(d, p) basis set level. The calculations were utilized to the CS symmetries of the molecules. The obtained vibrational frequencies and optimised geometric parameters (bond lengths and bond angles) were seen to be well agreement with the experimental data. The used scale factors which have been obtained the ratio of the frequency values of the strongest peaks in the calculated and experimental spectra seem to cause the gained vibrations well corresponding to the experimental ones. Theoretical infrared intensities and Raman activities are also reported.

  17. Beyond computational difficulties: Survey of the two decades from the elaboration to the extensive application of the Hartree-Fock method

    Science.gov (United States)

    Martinez, Jean-Philippe

    2017-11-01

    The Hartree-Fock method, one of the first applications of the new quantum mechanics in the frame of the many-body problem, had been elaborated by Rayner Douglas Hartree in 1928 and Vladimir Fock in 1930. Promptly, the challenge of tedious computations was being discussed and it is well known that the application of the method benefited greatly from the development of computers from the mid-to-late 1950s. However, the years from 1930 to 1950 were by no means years of stagnation, as the method was the object of several considerations related to its mathematical formulation, possible extension, and conceptual understanding. Thus, with a focus on the respective attitudes of Hartree and Fock, in particular with respect to the concept of quantum exchange, the present work puts forward some mathematical and conceptual clarifications, which played an important role for a better understanding of the many-body problem in quantum mechanics.

  18. Solution of the Skyrme-Hartree-Fock-Bogolyubov equations in the Cartesian deformed harmonic-oscillator basis.. (VII) HFODD (v2.49t): A new version of the program

    Science.gov (United States)

    Schunck, N.; Dobaczewski, J.; McDonnell, J.; Satuła, W.; Sheikh, J. A.; Staszczak, A.; Stoitsov, M.; Toivanen, P.

    2012-01-01

    -consistent Hartree-Fock equations, even for heavy nuclei, and for various nucleonic ( n-particle- n-hole) configurations, deformations, excitation energies, or angular momenta. Similarly, Local Density Approximation in the particle-particle channel, which is equivalent to using a zero-range interaction, allows for a simple implementation of pairing effects within the Hartree-Fock-Bogolyubov method. Solution method: The program uses the Cartesian harmonic oscillator basis to expand single-particle or single-quasiparticle wave functions of neutrons and protons interacting by means of the Skyrme effective interaction and zero-range pairing interaction. The expansion coefficients are determined by the iterative diagonalization of the mean-field Hamiltonians or Routhians which depend non-linearly on the local neutron and proton densities. Suitable constraints are used to obtain states corresponding to a given configuration, deformation or angular momentum. The method of solution has been presented in: [J. Dobaczewski, J. Dudek, Comput. Phys. Commun. 102 (1997) 166]. Reasons for new version: Version 2.49s of HFODD provides a number of new options such as the isospin mixing and projection of the Skyrme functional, the finite-temperature HF and HFB formalism and optimized methods to perform multi-constrained calculations. It is also the first version of HFODD to contain threading and parallel capabilities. Summary of revisions: Isospin mixing and projection of the HF states has been implemented. The finite-temperature formalism for the HFB equations has been implemented. The Lipkin translational energy correction method has been implemented. Calculation of the shell correction has been implemented. The two-basis method for the solution to the HFB equations has been implemented. The Augmented Lagrangian Method (ALM) for calculations with multiple constraints has been implemented. The linear constraint method based on the cranking approximation of the RPA matrix has been implemented. An

  19. Spin density distribution in open-shell transition metal systems: A comparative post-Hartree-Fock, Density Functional Theory and quantum Monte Carlo study of the CuCl2 molecule

    CERN Document Server

    Caffarel, Michel; Scemama, Anthony; Ramírez-Solís, Alejandro

    2014-01-01

    We present a comparative study of the spatial distribution of the spin density (SD) of the ground state of CuCl2 using Density Functional Theory (DFT), quantum Monte Carlo (QMC), and post-Hartree-Fock wavefunction theory (WFT). A number of studies have shown that an accurate description of the electronic structure of the lowest-lying states of this molecule is particularly challenging due to the interplay between the strong dynamical correlation effects in the 3d shell of the copper atom and the delocalization of the 3d hole over the chlorine atoms. It is shown here that qualitatively different results for SD are obtained from these various quantum-chemical approaches. At the DFT level, the spin density distribution is directly related to the amount of Hartree-Fock exchange introduced in hybrid functionals. At the QMC level, Fixed-node Diffusion Monte Carlo (FN-DMC) results for SD are strongly dependent on the nodal structure of the trial wavefunction employed (here, Hartree-Fock or Kohn-Sham with a particula...

  20. Test of a q-fractional V{sup (N-q)} Hartree-Fock potential for the calculation of double photoionization cross sections of neon

    Energy Technology Data Exchange (ETDEWEB)

    Kilin, V.A. [Tomsk Polytechnic University, Tomsk (Russian Federation); Lazarev, D.V.; Lazarev, Dm.A.; Zelichenko, V.M. [Tomsk Pedagogic University, Tomsk (Russian Federation); Amusia, M. Ya. [A.F. Ioffe Physico-Technical Institute, St. Petersburg (Russian Federation); Schartner, K.-H. [I Physikalisches Institut, Justus-Liebig-Universitaet, Giessen (Germany); Ehresmann, A.; Schmoranzer, H. [Fachbereich Physik, Universitaet Kaiserslautern, Kaiserslautern (Germany)

    2001-10-28

    The approach of a parametric V{sup (N-q)} Hartree-Fock potential with fractional q is developed and applied for the first time for the calculation of the double photoionization cross sections of Ne. A minimum of the squared difference between the length-form and velocity-form cross sections is used as a criterion for calculating the values of q. It is found that the minimization procedure leads to a practically exact equality of the length-form and velocity-form cross sections for the Ne III 2s{sup 2}2p{sup 4}[{sup 3}P,{sup 1}D,{sup 1}S], 2s{sup 1}2p{sup 5}[{sup 3}P,{sup 1}P] and 2s{sup 0}2p{sup 6}[{sup 1}S] states in the exciting-photon energy region from the double-ionization threshold up to 325 eV, if q is considered as a function of the exciting-photon energy. The calculated V{sup (N-q)} cross sections are in better agreement with the experimental data than those for the V{sup (N-1)} and V{sup (N-2)} potentials. (author)

  1. On site coulomb repulsion dominates over the non-local Hartree-Fock exchange in determining the band gap of polymers

    Science.gov (United States)

    Chattopadhyaya, Mausumi; Sen, Sabyasachi; Alam, Md. Mehboob; Chakrabarti, Swapan

    2014-02-01

    The present study deals with the relative performance of the various density functional approaches in evaluating the band gap of polymer materials. Several density functional approximations that includes pure generalized gradient approximated (GGA) functional, meta-GGA, hybrid and range separated hybrid functionals have been used to evaluate the electrical band gap or transport gap of the studied polymers and compared with that obtained using Hubbard U corrected GGA functional (GGA+U). It has been observed that the experimental band gap of the polymers studied is satisfactorily reproducible when GGA+U approach is adopted. The band gap analyses further suggest that range separated hybrid functional, CAM-B3LYP, largely overestimates the band gap of all the polymers studied while the performance of hybrid B3LYP functional and other range separated hybrid functional like HSE is moderate. Better performance of the GGA+U method clearly indicates that short range coulomb correlation plays more significant role over the non-local Hartree-Fock (HF) exchange in determining the electrical band gap of polymer materials. It is also noticeable that the Hubbard U parameter used for the various polymers under consideration is relatively large, indicating the semi-empirical nature of the GGA+U level of calculations. The present finding will help us design new low band gap polymer through estimating band gap by the GGA+U method and this could be very useful for solar cell research.

  2. Recommending Hartree-Fock theory with London-dispersion and basis-set-superposition corrections for the optimization or quantum refinement of protein structures.

    Science.gov (United States)

    Goerigk, Lars; Collyer, Charles A; Reimers, Jeffrey R

    2014-12-18

    We demonstrate the importance of properly accounting for London dispersion and basis-set-superposition error (BSSE) in quantum-chemical optimizations of protein structures, factors that are often still neglected in contemporary applications. We optimize a portion of an ensemble of conformationally flexible lysozyme structures obtained from highly accurate X-ray crystallography data that serve as a reliable benchmark. We not only analyze root-mean-square deviations from the experimental Cartesian coordinates, but also, for the first time, demonstrate how London dispersion and BSSE influence crystallographic R factors. Our conclusions parallel recent recommendations for the optimization of small gas-phase peptide structures made by some of the present authors: Hartree-Fock theory extended with Grimme's recent dispersion and BSSE corrections (HF-D3-gCP) is superior to popular density functional theory (DFT) approaches. Not only are statistical errors on average lower with HF-D3-gCP, but also the convergence behavior is much better. In particular, we show that the BP86/6-31G* approach should not be relied upon as a black-box method, despite its widespread use, as its success is based on an unpredictable cancellation of errors. Using HF-D3-gCP is technically straightforward, and we therefore encourage users of quantum-chemical methods to adopt this approach in future applications.

  3. Roothaan's approach to solve the Hartree-Fock equations for atoms confined by soft walls: Basis set with correct asymptotic behavior.

    Science.gov (United States)

    Rodriguez-Bautista, Mariano; Díaz-García, Cecilia; Navarrete-López, Alejandra M; Vargas, Rubicelia; Garza, Jorge

    2015-07-21

    In this report, we use a new basis set for Hartree-Fock calculations related to many-electron atoms confined by soft walls. One- and two-electron integrals were programmed in a code based in parallel programming techniques. The results obtained with this proposal for hydrogen and helium atoms were contrasted with other proposals to study just one and two electron confined atoms, where we have reproduced or improved the results previously reported. Usually, an atom enclosed by hard walls has been used as a model to study confinement effects on orbital energies, the main conclusion reached by this model is that orbital energies always go up when the confinement radius is reduced. However, such an observation is not necessarily valid for atoms confined by penetrable walls. The main reason behind this result is that for atoms with large polarizability, like beryllium or potassium, external orbitals are delocalized when the confinement is imposed and consequently, the internal orbitals behave as if they were in an ionized atom. Naturally, the shell structure of these atoms is modified drastically when they are confined. The delocalization was an argument proposed for atoms confined by hard walls, but it was never verified. In this work, the confinement imposed by soft walls allows to analyze the delocalization concept in many-electron atoms.

  4. Semi-empirical calculations of radiative decay rates in Mo II. A comparison between oscillator strength parametrization and core-polarization-corrected relativistic Hartree-Fock approaches

    Science.gov (United States)

    Bouazza, Safa; Palmeri, Patrick; Quinet, Pascal

    2017-09-01

    We present a semi-empirical determination of Mo II radiative parameters in a wide wavelength range 1716-8789 Å. Our fitting procedure to experimental oscillator strengths available in the literature permits us to provide reliable values for a large number of Mo II lines, predicting previously unmeasured oscillator strengths of lines involving 4d45p and 4d35s5p odd-parity configurations. The extracted transition radial integral values are compared with ab-initio calculations: on average they are 0.88 times the values obtained with the basic pseudo-relativistic Hartree Fock method and they agree well when core polarization effects are included. When making a survey of our present and previous studies and including also those given in the literature we observe as general trends a decreasing of transition radial integral values with filling nd shells of the same principal quantum numbers for ndk(n + 1)s → ndk(n + 1)p transitions.

  5. Resonant-convergent second-order nonlinear response functions at the levels of Hartree-Fock and Kohn-Sham density functional theory

    Science.gov (United States)

    Fahleson, Tobias; Norman, Patrick

    2017-10-01

    The second-order nonlinear (or cubic) response function is derived from the Ehrenfest theorem with inclusion made of the finite lifetimes of the excited states, representing the extension of the derivation of the quadratic response function in the same framework [P. Norman et al., J. Chem. Phys. 123, 194103 (2005)]. The resulting damped response functions are physically sound and converging also in near-resonance and resonance regions of the spectrum. Being an accurate approximation for small complex frequencies (defined as the sum of an optical frequency and an imaginary damping parameter), the polynomial expansion of the complex cubic response function in terms of the said frequencies is presented and used to validate the program implementation. In terms of approximate state theory, the computationally tractable expressions of the damped cubic response function are derived and implemented at the levels of Hartree-Fock and Kohn-Sham density functional theory. Numerical examples are provided in terms of studies of the intensity-dependent refractive index of para-nitroaniline and the two-photon absorption cross section of neon. For the latter property, a numerical comparison is made against calculations of the square of two-photon matrix elements that are identified from a residue analysis of the resonance-divergent quadratic response function.

  6. Roothaan’s approach to solve the Hartree-Fock equations for atoms confined by soft walls: Basis set with correct asymptotic behavior

    Energy Technology Data Exchange (ETDEWEB)

    Rodriguez-Bautista, Mariano; Díaz-García, Cecilia; Navarrete-López, Alejandra M.; Vargas, Rubicelia; Garza, Jorge, E-mail: jgo@xanum.uam.mx [Departamento de Química, División de Ciencias Básicas e Ingeniería, Universidad Autónoma Metropolitana-Iztapalapa, San Rafael Atlixco 186, Col. Vicentina, Iztapalapa C. P. 09340, México D. F., México (Mexico)

    2015-07-21

    In this report, we use a new basis set for Hartree-Fock calculations related to many-electron atoms confined by soft walls. One- and two-electron integrals were programmed in a code based in parallel programming techniques. The results obtained with this proposal for hydrogen and helium atoms were contrasted with other proposals to study just one and two electron confined atoms, where we have reproduced or improved the results previously reported. Usually, an atom enclosed by hard walls has been used as a model to study confinement effects on orbital energies, the main conclusion reached by this model is that orbital energies always go up when the confinement radius is reduced. However, such an observation is not necessarily valid for atoms confined by penetrable walls. The main reason behind this result is that for atoms with large polarizability, like beryllium or potassium, external orbitals are delocalized when the confinement is imposed and consequently, the internal orbitals behave as if they were in an ionized atom. Naturally, the shell structure of these atoms is modified drastically when they are confined. The delocalization was an argument proposed for atoms confined by hard walls, but it was never verified. In this work, the confinement imposed by soft walls allows to analyze the delocalization concept in many-electron atoms.

  7. Off-Mass-Shell Behaviors of Nucleon Self-Energies and the Gamow-Teller Sum Rule in the Relativistic Hartree-Fock Approach

    Science.gov (United States)

    Maruyama, T.

    2011-06-01

    The relativistic Hartree approximation predicts a deep attractive potential for antinucleon, which largely reduces the threshold energies of the nucleon-antinucleon (N{bar N}) production. This effect has played an important role in explaining the quenching of the Gamow-Teller (GT) strength because the quenched strength in the particle-hole excitation is partially taken by the {N{bar N}} production. On the other hand antiproton experiments do not reveal a deep attractive potential for antinucleon. In this paper, we study the energy dependence of the nucleon self-energies in the relativistic Hartree-Fock (RHF) approximation in off-mass-shell states. Then, we demonstrate that the antinucleon appearing in low-energy observables is in the off-mass-shell energy region and its properties are quite different from those at the on-mass-shell state. Furthermore, we show that the quenched amount of the GT strength is taken by not only the N{bar N} production but also the meson production through the imaginary part of the nucleon self-energy in the RHF approximation.

  8. Spin-free Dirac-Coulomb calculations augmented with a perturbative treatment of spin-orbit effects at the Hartree-Fock level.

    Science.gov (United States)

    Cheng, Lan; Stopkowicz, Stella; Gauss, Jürgen

    2013-12-07

    A perturbative approach to compute second-order spin-orbit (SO) corrections to a spin-free Dirac-Coulomb Hartree-Fock (SFDC-HF) calculation is suggested. The proposed scheme treats the difference between the DC and SFDC Hamiltonian as perturbation and exploits analytic second-derivative techniques. In addition, a cost-effective scheme for incorporating relativistic effects in high-accuracy calculations is suggested consisting of a SFDC coupled-cluster treatment augmented by perturbative SO corrections obtained at the HF level. Benchmark calculations for the hydrogen halides HX, X = F-At as well as the coinage-metal fluorides CuF, AgF, and AuF demonstrate the accuracy of the proposed perturbative treatment of SO effects on energies and electrical properties in comparison with the more rigorous full DC treatment. Furthermore, we present, as an application of our scheme, results for the electrical properties of AuF and XeAuF.

  9. Long-range corrected density functional theory with accelerated Hartree-Fock exchange integration using a two-Gaussian operator [LC-ωPBE(2Gau)].

    Science.gov (United States)

    Song, Jong-Won; Hirao, Kimihiko

    2015-10-14

    Since the advent of hybrid functional in 1993, it has become a main quantum chemical tool for the calculation of energies and properties of molecular systems. Following the introduction of long-range corrected hybrid scheme for density functional theory a decade later, the applicability of the hybrid functional has been further amplified due to the resulting increased performance on orbital energy, excitation energy, non-linear optical property, barrier height, and so on. Nevertheless, the high cost associated with the evaluation of Hartree-Fock (HF) exchange integrals remains a bottleneck for the broader and more active applications of hybrid functionals to large molecular and periodic systems. Here, we propose a very simple yet efficient method for the computation of long-range corrected hybrid scheme. It uses a modified two-Gaussian attenuating operator instead of the error function for the long-range HF exchange integral. As a result, the two-Gaussian HF operator, which mimics the shape of the error function operator, reduces computational time dramatically (e.g., about 14 times acceleration in C diamond calculation using periodic boundary condition) and enables lower scaling with system size, while maintaining the improved features of the long-range corrected density functional theory.

  10. Properties of Fermi liquids with a finite range interaction

    Energy Technology Data Exchange (ETDEWEB)

    Nozieres, P. (Institut Max von Laue - Paul Langevin (ILL), 38 - Grenoble (France))

    1992-04-01

    Following a suggestion of Khodel' and Shaginyan (KS), it is shown that a Hartree Fock description of Fermi liquids can lead to very strange results when the interaction has long range. For instance, the sharp drop of particle distribution at the Fermi level can be smeared over a finite k-range, with a flat plateau in the quasiparticle energy. In practice, such an effect appears as an artefact of the Hartree Fock approximation. The KS effect occurs only for an attraction, in which case it is hidden by superconductivity. Moreover, the enhanced quasiparticle collision rate makes the Hartree Fock approximation untenable. Finally, screening of a strong long range interaction is such that the instability threshold cannot be reached.

  11. ENERGY DERIVATIVES FOR CONFIGURATION INTERACTION WAVEFUNCTIONS

    Energy Technology Data Exchange (ETDEWEB)

    Dupuis, M.

    1980-09-01

    Equations providing the first and second derivatives of a configuration interaction (CI) energy with respect to an external parameter are provided. We assume no restriction on the form of the CI expansion built from molecular orbitals obtained in a multiconfiguration Hartree-Fock (MCHF) calculation. Also the coupled perturbed multi-configuration Hartree-Fock formalism is presented for a general MCHF wavefunction and provides the first order and second order changes of the molecular orbital expansion coefficients with respect to an external parameter.

  12. Properties of Fermi liquids with a finite range interaction

    Science.gov (United States)

    Nozières, Philippe

    1992-04-01

    Following a suggestion of Khodel' and Shaginyan (KS), it is shown that a Hartree Fock description of Fermi liquids can lead to very strange results when the interaction has long range. For instance, the sharp drop of particle distribution at the Fermi level can be smeared over a finite k-range, with a flat plateau in the quasiparticle energy. In practice, such an effect appears as an artefact of the Hartree Fock approximation. The KS effect occurs only for an attraction, in which case it is hidden by superconductivity. Moreover, the enhanced quasiparticle collision rate makes the Hartree Fock approximation untenable. Finally, screening of a strong long range interaction is such that the instability threshold cannot be reached. Partant d'une suggestion de Khodel' et Shaginyan (KS), on montre que la description d'un liquide de Fermi en Hartree Fock peut conduire à des résultats très étranges quand la portée de l'interaction est grande. Par exemple, la discontinuité de la distribution des particules au niveau de Fermi est étalée sur une bande de k finie, avec un plateau de l'énergie des quasiparticules. En fait, cet état est une conséquence de l'approximation de Hartree Fock. Il se produit seulement pour une attraction, auquel cas il est masqué par la supraconductivité. De plus, le renforcement des collisions entre quasiparticules rend l'approximation de Hartree Fock inutilisable. Enfin, l'écrantage d'une interaction forte et à longue portée ne permet pas d'atteindre le seuil d'instabilité.

  13. First Principles Hartree-Fock Description of Lithium Insertion in Oxides. I. The End Members TiO 2and LiTiO 2of the System Li xTiO 2

    Science.gov (United States)

    Mackrodt, W. C.

    1999-02-01

    First principles periodic Hartree-Fock calculations are reported for the P4 2/ mnm(rutile), I4 1/ amd(anatase), Pbca(brookite), Pnma(ramsdellite), Pcbn(colombite), Fdoverline3m(spinel), and Imma(orthorhombic) polymorphs of TiO 2, from which the predicted order of stability is The calculated difference in energy between the rutile and anatase structures is 0.02-0.06 eV, in good agreement with a recent local density approximation (LDA) estimate of 0.033 eV and an experiment enthalpy difference of 0.05 eV. The corresponding Hartree-Fock and LDA differences for the brookite structure are 0.06 and 0.058 eV, respectively. The calculated volumes, which are based on isotropic volume-optimized Hartree-Fock energies, are also in good agreement with recent LDA calculations and with experiment. Spin-unrestricted calculations are reported for the Fmoverline3m, Imma, Pnma, and P4 2/ mmmof LiTiO 2, where the stability is in the order The only reported phase for LiTiO 2is Fmoverline3m, for which the calculated volume is in good agreement with experiment. From the relative stabilities of TiO 2and LiTiO 2, the relative lithium insertion potentials corresponding to TiO 2 → LiTiO 2are deduced, with a maximum variation of 1.6 eV for the different polymorphic routes. The maximum voltage predicted is that for the Immaroute which is ˜1 eV larger than that for Pnma. Direct comparisons with the calculated energy for C2/ mLi 0.5MnO 2 → LiMnO 2lead to an estimate of the voltage for ImmaTiO 2 → LiTiO 2of ˜1.3 eV, which is ˜2.5 eV anodicto the Mn system. The corresponding values for the Pnmapolymorphic route are ˜3 and ˜3.5 eV, respectively. Mulliken population analyses indicate that lithium is completely ionized in LiTiO 2and that the charge transfer is predominantly to the oxygen sublattice. There is a rehybridization of the titanium valence orbitals leading to a slight increase in the 3 dpopulation and strong localization of spin density at the titanium sites with local moments of

  14. Multiparticle equations for interacting Dirac fermions in magnetically confined graphene quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Egger, Reinhold [Institut fuer Theoretische Physik, Heinrich-Heine-Universitaet, Universitaetsstrasse 1, D-40225 Duesseldorf (Germany); De Martino, Alessandro [Institut fuer Theoretische Physik, Universitaet zu Koeln, Zuelpicher Strasse 77, D-50937 Koeln (Germany); Siedentop, Heinz; Stockmeyer, Edgardo, E-mail: egger@thphy.uni-duesseldorf.d, E-mail: ademarti@thp.uni-koeln.d, E-mail: h.s@lmu.d, E-mail: stock@math.lmu.d [Mathematisches Institut, Ludwigs-Maximilians-Universitaet Muenchen, Theresienstrasse 39, D-80333 Muenchen (Germany)

    2010-05-28

    We study the energy of quasi-particles in graphene within the Hartree-Fock approximation. The quasi-particles are confined via an inhomogeneous magnetic field and interact via the Coulomb potential. We show that the associated functional has a minimizer and determines the stability conditions for the N-particle problem in such a graphene quantum dot.

  15. Multi-configuration Dirac-Hartree-Fock calculations of the transition rates of 2s22p2 - 2s2p3 and 2s2p3 - 2s22pnl (n ≥ 3) E1 transitions of N+

    Science.gov (United States)

    Shen, Xiaozhi; Liu, Juan; Zhou, Fuyang

    2016-10-01

    Wavefunctions were determined using the multi-configuration Dirac-Hartree-Fock method. The core-core, core-valence, valence correlation, Breit interaction and quantum electrodynamics effects, as well as some higher-order correlation effects, were considered to obtain accurate wavelengths (λ), oscillator strengths (gf) and transition rates (A) of 2s22p2 - 2s2p3, 2s2p3 - 2s22pnl (n ≥ 3) and 2s2p3 - 2s2p23s E1 transitions. The branching ratio of 2s2p3 5S^o_2 (namely Aλ2143.45/Aλ2139.68) based on the latest calculation of 2.462 ± 0.119 is recommended for the determination of a nebula's electron temperature and electron density. The largest calculated gf value of 2s2p3 - 2s22p4p is λ630.65, differing from that of λ1060.2 (i.e. 2s2p3 3P^o_2 - 2s22p4p 3S1) that was observed with the largest intensities in the Orion Nebula spectrum. In addition, the energy levels and the splittings of 2s2p3, the extremely difficult calculations of the rates of two-electron one-photon transitions as well as those of the very small intercombination A of 2s2p3 5S^o_2 were studied in detail. Because of the weak spin-orbit interaction, accurately calculating the levels 3P^o_{1,2,0} (or 3D^o_{3,2,1}) and their transition matrix elements is very sensitive to relativistic and electron correlation effects. A special case for this is when the transition operators synchronously applied to wavefunctions with regard to 2s2p3 3Po and 2s22pnl (n = 4) become extremely sensitive to some higher-order correlation effects.

  16. Homogeneous Ni Catalysts for H2 Oxidation and Production: An Assessment of Theoretical Methods, from Density Functional Theory to Post Hartree-Fock Correlated Wave-Function Theory

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Shentan; Raugei, Simone; Rousseau, Roger; Dupuis, Michel; Bullock, R. Morris

    2010-12-09

    A systematic assessment of theoretical methods applicable to the accurate characterization of catalytic cycles of homogeneous catalysts for H2 oxidation and evolution is reported. The key elementary steps involve heterolytic cleavage of the H-H bond and formation/cleavage of Ni-H and N-H bonds. In the context of density functional theory (DFT), we investigated the use of functionals in the generalized gradient approximation (GGA) as well as hybrid functionals. We compared the results with wave-function theories based on perturbation theory (MP2 and MP4) and on coupled-cluster expansions [CCD, CCSD, and CCSD(T)]. Our findings indicate that DFT results based on Perdew correlation functionals are in semiquantitative agreement with the CCSD(T) results, with deviations of only a few kilocalories/mole. On the other hand, the B3LYP functional is not even in qualitative agreement with CCSD(T). Surprisingly, the MP2 results are found to be extremely poor, in particular for the diproton Ni(0) and dihydride Ni(IV) species on the reaction potential energy surface. The Hartree-Fock reference wave function in MP2 theory gives a poor reference state description for these states that are electron rich on Ni, giving rise to erroneous MP2 energies. Finally, we present a detailed potential-energy diagram for the oxidation of H2 by these catalysts after accounting for the effects of solvation, as modeled by a polarizable continuum, and of free energy estimated at the harmonic level of theory.

  17. Gogny interactions with tensor terms

    Energy Technology Data Exchange (ETDEWEB)

    Anguiano, M.; Lallena, A.M.; Bernard, R.N. [Universidad de Granada, Departamento de Fisica Atomica, Molecular y Nuclear, Granada (Spain); Co' , G. [INFN, Lecce (Italy); De Donno, V. [Universita del Salento, Dipartimento di Matematica e Fisica ' ' E. De Giorgi' ' , Lecce (Italy); Grasso, M. [Universite Paris-Sud, Institut de Physique Nucleaire, IN2P3-CNRS, Orsay (France)

    2016-07-15

    We present a perturbative approach to include tensor terms in the Gogny interaction. We do not change the values of the usual parameterisations, with the only exception of the spin-orbit term, and we add tensor terms whose only free parameters are the strengths of the interactions. We identify observables sensitive to the presence of the tensor force in Hartree-Fock, Hartree-Fock-Bogoliubov and random phase approximation calculations. We show the need of including two tensor contributions, at least: a pure tensor term and a tensor-isospin term. We show results relevant for the inclusion of the tensor term for single-particle energies, charge-conserving magnetic excitations and Gamow-Teller excitations. (orig.)

  18. Percolative Mott Metal-Insulator Transition in the Doped Hubbard-Holstein model: Theoretical Results from Hartree-Fock and Slave Boson Approaches

    Science.gov (United States)

    Moradi Kurdestany, Jamshid

    Motivated by the current interest in the understanding of the Mott insulators away from half filling, observed in many perovskite oxides, we study the Mott metal-insulator transition in the doped Hubbard-Holstein model using the Hatree-Fock and slave-Boson approaches. The model contains both the Coulomb and the electron-lattice interactions, which are important ingredients in the physics of the perovskite oxides. In contrast to the half-filled Hubbard model, which always results in a single phase (either metallic or insulating), our results show that away from half-filling, a mixed phase of metallic and insulating regions occur.As the dopant concentration is increased, the metallic part progressively grows in volume, until it exceeds the percolation threshold, leading to percolative conduction. This happens above a critical dopant concentration, which, depending on the strength of the electron-lattice interaction, can be a significant fraction of unity. This means that the material could be insulating even for a substantial amount of doping, in contrast with the Nagaoka theorem, where a single hole destroys the insulating behavior of the half-filled Hubbard model. Our theory provides a framework for the understanding of the density-driven MIT observed in many complex oxides.

  19. Fermion Superfluidity And Confining Interactions

    CERN Document Server

    Galal, A A

    2004-01-01

    We study the pairing of Fermi systems with long-range, confining interparticle interactions. We solve the Cooper problem for a pair of fermions interacting via a regularized harmonic oscillator potential and determine the s-wave spectrum of bound states. Using a model of two interacting species of fermions, we calculate the ground state energy of the normal phase in the Hartree-Fock approximation and find that it is infrared (IR) divergent, due to a combination of the sharpness of the Fermi sea and the long-range nature of the interaction. We calculate the correlation energy in the normal phase using the random phase approximation (RPA) and demonstrate the cancellation of infrared divergences between the Hartree-Fock and RPA contributions. Introducing a variational wavefunction to study the superfluid phase, we solve the BCS equations using a Hartree-Fock-Bogoliubov (HFB) analysis to determine the wave-function, excitation gap, and other parameters of the superfluid phase. We show that the system crosses over...

  20. Effects of short-ranged interactions on the Kane-Mele model without discrete particle-hole symmetry

    Science.gov (United States)

    Lai, Hsin-Hua; Hung, Hsiang-Hsuan

    2014-04-01

    We study the effects of short-ranged interactions on the Z2 topological insulator phase, also known as the quantum spin Hall phase, in the Kane-Mele model at half-filling with staggered potentials, which explicitly breaks the discrete particle-hole symmetry. Within Hartree-Fock mean-field analysis, we conclude that the on-site repulsive interactions help stabilize the topological phase (quantum spin Hall) against the staggered potentials by enlarging the regime of the topological phase along the axis of the ratio of the staggered potential strength and the spin-orbit coupling. In sharp contrast, the on-site attractive interactions destabilize the topological phase. We also examine the attractive interaction case by means of the unbiased determinant projector quantum Monte Carlo and the results are qualitatively consistent with the Hartree-Fock picture.

  1. Shape evolution of Ne isotopes and Ne hypernuclei: The interplay of pairing and tensor interactions

    Directory of Open Access Journals (Sweden)

    Li A.

    2014-03-01

    Full Text Available We study tensor and pairing effects on the quadruple deformation of neon isotopes based on a deformed Skyrme-Hartree-Fock model with BCS approximation for the pairing channel. We extend the Skyrme-Hartree-Fock formalism for the description of hypernuclei adopting the recently-proposed ESC08b hyperon-nucleon interaction. It is found that the interplay of pairing and tensor interactions is crucial to derive the deformations in several neon isotopes. Especially, the shapes of 26,30Ne are studied in details in comparisons with experimentally observed shapes. Furthermore the deformations of the hypernuclei are compared with the corresponding neon isotopic cores in the presence of tensor force. We find the same shapes with somewhat smaller deformations for single Λ-hypernuclei compared with their core deformations.

  2. Molecular modeling studies of interactions between sodium polyacrylate polymer and calcite surface

    Science.gov (United States)

    Ylikantola, A.; Linnanto, J.; Knuutinen, J.; Oravilahti, A.; Toivakka, M.

    2013-07-01

    The interactions between calcite pigment and sodium polyacrylate dispersing agent, widely used in papermaking as paper coating components, were investigated using classical force field and quantum chemical approaches. The objective was to understand interactions between the calcite surface and sodium polyacrylate polymer at 300 K using molecular dynamics simulations. A quantum mechanical ab initio Hartree-Fock method was also used to obtain detailed information about the sodium polyacrylate polymer structure. The effect of water molecules (moisture) on the interactions was also examined. Calculations showed that molecular weight, branching and the orientation of sodium polyacrylate polymers influence the interactions between the calcite surface and the polymer. The force field applied, and also water molecules, were found to have an impact on all systems studied. Ab initio Hartree-Fock calculations indicated that there are two types of coordination between sodium atoms and carboxylate groups of the sodium polyacrylate polymer, inter- and intra-carboxylate group coordination. In addition, ab initio Hartree-Fock calculations of the structure of the sodium polyacrylate polymer produced important information regarding interactions between the polymers and carboxylated styrene-butadiene latex particles.

  3. Computational strong-field quantum dynamics. Intense light-matter interactions

    Energy Technology Data Exchange (ETDEWEB)

    Bauer, Dieter (ed.) [Rostock Univ. (Germany). Inst. fuer Physik

    2017-09-01

    This graduate textbook introduces the computational techniques to study ultra-fast quantum dynamics of matter exposed to strong laser fields. Coverage includes methods to propagate wavefunctions according to the time dependent Schroedinger, Klein-Gordon or Dirac equation, the calculation of typical observables, time-dependent density functional theory, multi configurational time-dependent Hartree-Fock, time-dependent configuration interaction singles, the strong-field approximation, and the microscopic particle-in-cell approach.

  4. Computational strong-field quantum dynamics intense light-matter interactions

    CERN Document Server

    2017-01-01

    This graduate textbook introduces the computational techniques to study ultra-fast quantum dynamics of matter exposed to strong laser fields. Coverage includes methods to propagate wavefunctions according to the time-dependent Schrödinger, Klein-Gordon or Dirac equation, the calculation of typical observables, time-dependent density functional theory, multi-configurational time-dependent Hartree-Fock, time-dependent configuration interaction singles, the strong-field approximation, and the microscopic particle-in-cell approach.

  5. The efficient evaluation of configuration interaction analytic energy second derivatives: Application to hydrogen thioperoxide, HSOH

    Science.gov (United States)

    Lee, Timothy J.; Handy, Nicholas C.; Rice, Julia E.; Scheiner, Andrew C.; Schaefer, Henry F., III

    1986-10-01

    We present an efficient reformulation of the analytic configuration interaction (CI) energy second derivative. Specifically, the Z-vector method of Handy and Schaefer is used to avoid solving the second order coupled perturbed Hartree-Fock (CPHF) equations. We have incorporated translational-rotational invariance into the new method. We present a more efficient method for the evaluation of the Y matrix contribution. The procedure which has been implemented can accommodate very large basis sets and CI expansions for any general restricted Hartree-Fock (RHF) reference wave function. As a test case, we apply the new procedure to the HSOH molecule using a double zeta plus polarization basis set. This leads to 50 contracted Gaussian basis functions and 116 403 configurations in the CI expansion. Harmonic vibrational frequencies and infrared intensities are predicted for HSOH and its deuterated isotopomers. The analytic method described herein requires only 56% of the central processor unit time used by a numerical method.

  6. Efficient evaluation of configuration interaction analytic energy second derivatives: Application to hydrogen thioperoxide, HSOH

    Energy Technology Data Exchange (ETDEWEB)

    Lee, T.J.; Handy, N.C.; Rice, J.E.; Scheiner, A.C.; Schaefer H.F. III

    1986-10-01

    We present an efficient reformulation of the analytic configuration interaction (CI) energy second derivative. Specifically, the Z-vector method of Handy and Schaefer is used to avoid solving the second order coupled perturbed Hartree--Fock (CPHF) equations. We have incorporated translational--rotational invariance into the new method. We present a more efficient method for the evaluation of the Y matrix contribution. The procedure which has been implemented can accommodate very large basis sets and CI expansions for any general restricted Hartree--Fock (RHF) reference wave function. As a test case, we apply the new procedure to the HSOH molecule using a double zeta plus polarization basis set. This leads to 50 contracted Gaussian basis functions and 116 403 configurations in the CI expansion. Harmonic vibrational frequencies and infrared intensities are predicted for HSOH and its deuterated isotopomers. The analytic method described herein requires only 56% of the central processor unit time used by a numerical method.

  7. Theoretical studies of molecular interactions

    Energy Technology Data Exchange (ETDEWEB)

    Lester, W.A. Jr. [Univ. of California, Berkeley (United States)

    1993-12-01

    This research program is directed at extending fundamental knowledge of atoms and molecules including their electronic structure, mutual interaction, collision dynamics, and interaction with radiation. The approach combines the use of ab initio methods--Hartree-Fock (HF) multiconfiguration HF, configuration interaction, and the recently developed quantum Monte Carlo (MC)--to describe electronic structure, intermolecular interactions, and other properties, with various methods of characterizing inelastic and reaction collision processes, and photodissociation dynamics. Present activity is focused on the development and application of the QMC method, surface catalyzed reactions, and reorientation cross sections.

  8. Diatomic interaction potential theory applications

    CERN Document Server

    Goodisman, Jerry

    2013-01-01

    Diatomic Interaction Potential Theory, Volume 2: Applications discusses the variety of applicable theoretical material and approaches in the calculations for diatomic systems in their ground states. The volume covers the descriptions and illustrations of modern calculations. Chapter I discusses the calculation of the interaction potential for large and small values of the internuclear distance R (separated and united atom limits). Chapter II covers the methods used for intermediate values of R, which in principle means any values of R. The Hartree-Fock and configuration interaction schemes des

  9. Microscopic study of superdeformed rotational bands in sup 1 sup 5 sup 1 Tb 21.60.Ev; 21.10.Re; 21.60.Jz; 27.70.+q; Superdeformation; Pairing; Hartree-Fock method; Woods-Saxon potential; Dynamical moments

    CERN Document Server

    El-Aouad, N; Dudek, J; Li, X; Luo, W D; Molique, H; Bouguettoucha, A; Byrski, T; Beck, F A; Curien, D; Duchêne, G; Finck, C; Kharraja, B

    2000-01-01

    Structure of eight experimentally known superdeformed bands in the nucleus sup 1 sup 5 sup 1 Tb is analyzed using the results of the Hartree-Fock and Woods-Saxon cranking approaches. It is demonstrated that far going detailed similarities between the two approaches exist and predictions related to the structure of rotational bands calculated within the two models are nearly parallel. An interpretation scenario for the structure of the superdeformed bands is presented and predictions related to the exit spins are made. Small but systematic discrepancies between experiment and theory, analyzed in terms of the dynamical moments, J sup ( sup 2 sup ) , are shown to exist. These discrepancies can be parametrized in terms of a scaling factor f, such that modifications J sup ( sup 1 sup ) sup , sup ( sup 2 sup )->fJ sup ( sup 1 sup ) sup , sup ( sup 2 sup ) together with the implied scaling of the frequencies omega->f sup - sup 1 omega, correspond systematically better with the experimental data (f approx =0.9) for b...

  10. Using cloud ice flux to parametrise large-scale lightning

    Directory of Open Access Journals (Sweden)

    D. L. Finney

    2014-12-01

    Full Text Available Lightning is an important natural source of nitrogen oxide especially in the middle and upper troposphere. Hence, it is essential to represent lightning in chemistry transport and coupled chemistry–climate models. Using ERA-Interim meteorological reanalysis data we compare the lightning flash density distributions produced using several existing lightning parametrisations, as well as a new parametrisation developed on the basis of upward cloud ice flux at 440 hPa. The use of ice flux forms a link to the non-inductive charging mechanism of thunderstorms. Spatial and temporal distributions of lightning flash density are compared to tropical and subtropical observations for 2007–2011 from the Lightning Imaging Sensor (LIS on the Tropical Rainfall Measuring Mission (TRMM satellite. The well-used lightning flash parametrisation based on cloud-top height has large biases but the derived annual total flash density has a better spatial correlation with the LIS observations than other existing parametrisations. A comparison of flash density simulated by the different schemes shows that the cloud-top height parametrisation has many more instances of moderate flash densities and fewer low and high extremes compared to the other parametrisations. Other studies in the literature have shown that this feature of the cloud-top height parametrisation is in contrast to lightning observations over certain regions. Our new ice flux parametrisation shows a clear improvement over all the existing parametrisations with lower root mean square errors (RMSEs and better spatial correlations with the observations for distributions of annual total, and seasonal and interannual variations. The greatest improvement with the new parametrisation is a more realistic representation of the zonal distribution with a better balance between tropical and subtropical lightning flash estimates. The new parametrisation is appropriate for testing in chemistry transport and chemistry

  11. X- rays and matter- the basic interactions

    DEFF Research Database (Denmark)

    Als-Nielsen, Jens

    2008-01-01

    In this introductory article we attempt to provide the theoretical basis for developing the interaction between X-rays and matter, so that one can unravel properties of matter by interpretation of X-ray experiments on samples. We emphasize that we are dealing with the basics, which means that we...... shall limit ourselves to a discussion of the interaction of an X-ray photon with an isolated atom, or rather with a single electron in a Hartree-Fock atom. Subsequent articles in this issue deal with more complicated - and interesting - forms of matter encompassing many atoms or molecules. To cite...

  12. Microscopic effective interaction between electrons: Application to sodium clusters

    Science.gov (United States)

    Lipparini, E.; Serra, Ll.; Takayanagi, K.

    1994-06-01

    The effects of short-range electronic correlations on the properties of sodium clusters are studied using the Brueckner g matrix as an effective interaction which describes the scattering of two electrons in the presence of a many-electron medium. The associated cluster Hamiltonian is solved within the Hartree-Fock approximation for the ground state and the dipole plasmon resonance is studied using the self-consistent random-phase approximation. Effects due to ionic core electrons are considered within the pseudojellium model of metal cluster, which goes beyond jellium by using ionic pseudo-Hamiltonians.

  13. Derivation of general analytic gradient expressions for density-fitted post-Hartree-Fock methods: An efficient implementation for the density-fitted second-order Møller-Plesset perturbation theory

    Science.gov (United States)

    Bozkaya, Uǧur

    2014-09-01

    General analytic gradient expressions (with the frozen-core approximation) are presented for density-fitted post-HF methods. An efficient implementation of frozen-core analytic gradients for the second-order Møller-Plesset perturbation theory (MP2) with the density-fitting (DF) approximation (applying to both reference and correlation energies), which is denoted as DF-MP2, is reported. The DF-MP2 method is applied to a set of alkanes, conjugated dienes, and noncovalent interaction complexes to compare the computational cost of single point analytic gradients with MP2 with the resolution of the identity approach (RI-MP2) [F. Weigend and M. Häser, Theor. Chem. Acc. 97, 331 (1997); R. A. Distasio, R. P. Steele, Y. M. Rhee, Y. Shao, and M. Head-Gordon, J. Comput. Chem. 28, 839 (2007)]. In the RI-MP2 method, the DF approach is used only for the correlation energy. Our results demonstrate that the DF-MP2 method substantially accelerate the RI-MP2 method for analytic gradient computations due to the reduced input/output (I/O) time. Because in the DF-MP2 method the DF approach is used for both reference and correlation energies, the storage of 4-index electron repulsion integrals (ERIs) are avoided, 3-index ERI tensors are employed instead. Further, as in case of integrals, our gradient equation is completely avoid construction or storage of the 4-index two-particle density matrix (TPDM), instead we use 2- and 3-index TPDMs. Hence, the I/O bottleneck of a gradient computation is significantly overcome. Therefore, the cost of the generalized-Fock matrix (GFM), TPDM, solution of Z-vector equations, the back transformation of TPDM, and integral derivatives are substantially reduced when the DF approach is used for the entire energy expression. Further application results show that the DF approach introduce negligible errors for closed-shell reaction energies and equilibrium bond lengths.

  14. Efficient Modeling of Coulomb Interaction Effect on Exciton in Crystal-Phase Nanowire Quantum Dot

    DEFF Research Database (Denmark)

    Taherkhani, Masoomeh; Gregersen, Niels; Mørk, Jesper

    2016-01-01

    The binding energy and oscillation strength of the ground-state exciton in type-II quantum dot (QD) is calculated by using a post Hartree-Fock method known as the configuration interaction (CI) method which is significantly more efficient than conventional methods like ab initio method. We show t...... that the Coulomb interaction between electron and holes in these structures considerably affects the transition dipole moment which is the key parameter of optical quantum gating in STIRAP (stimulated Raman adiabatic passage) process for implementing quantum gates [1], [2]....

  15. Phenomenology of near-threshold states: a practical parametrisation for the line shapes

    Directory of Open Access Journals (Sweden)

    Guo F.-K.

    2017-01-01

    Full Text Available In the last decade many states in the spectrum of charmonium and bottomonium have been observed experimentally above the lowest open-flavour threshold. Most of these states reside in the vicinity of strong thresholds and show properties that cannot be captured by simple quark models. Description and understanding of such exotic states is a challenge for the phenomenology of strong interactions, since it requires building adequate theoretical tools and approaches. In this work, a practical parametrisation for the line shapes of near threshold resonance(s is derived in the framework of a coupled-channel model which includes an arbitrary number of elastic and inelastic channels as well as of bare pole terms. Parameters of the distribution have a direct relation to phenomenology and the resulting analytical parametrisation is therefore ideally suited to harvest the full information content provided by the measurements and to establish a link between the experimental data and their theoretical interpretation.

  16. Phenomenology of near-threshold states: a practical parametrisation for the line shapes

    Science.gov (United States)

    Guo, F.-K.; Hanhart, C.; Kalashnikova, Yu. S.; Matuschek, P.; Mizuk, R. V.; Nefediev, A. V.; Wang, Q.; Wynen, J.-L.

    2017-03-01

    In the last decade many states in the spectrum of charmonium and bottomonium have been observed experimentally above the lowest open-flavour threshold. Most of these states reside in the vicinity of strong thresholds and show properties that cannot be captured by simple quark models. Description and understanding of such exotic states is a challenge for the phenomenology of strong interactions, since it requires building adequate theoretical tools and approaches. In this work, a practical parametrisation for the line shapes of near threshold resonance(s) is derived in the framework of a coupled-channel model which includes an arbitrary number of elastic and inelastic channels as well as of bare pole terms. Parameters of the distribution have a direct relation to phenomenology and the resulting analytical parametrisation is therefore ideally suited to harvest the full information content provided by the measurements and to establish a link between the experimental data and their theoretical interpretation.

  17. Pair Interaction Energy Decomposition Analysis for Density Functional Theory and Density-Functional Tight-Binding with an Evaluation of Energy Fluctuations in Molecular Dynamics.

    Science.gov (United States)

    Fedorov, Dmitri G; Kitaura, Kazuo

    2018-02-15

    Pair interaction energy decomposition analysis in the fragment molecular orbital (FMO) method is extended to treat density functional theory (DFT) and density-functional tight-binding (DFTB). Fluctuations of energy contributions are obtained from molecular dynamics simulations. Interactions at the DFT and DFTB levels are compared to the values obtained with Hartree-Fock, second-order Møller-Plesset (MP2), and coupled cluster methods. Hydrogen bonding in water clusters is analyzed. 200 ps NVT molecular dynamics simulations are performed with FMO for two ligands bound to the Trp-cage miniprotein (PDB 1L2Y ); the fluctuations of fragment energies and interactions are analyzed.

  18. Non-orthogonal configuration interaction for the calculation of multielectron excited states

    Energy Technology Data Exchange (ETDEWEB)

    Sundstrom, Eric J., E-mail: eric.jon.sundstrom@berkeley.edu; Head-Gordon, Martin [Department of Chemistry, University of California Berkeley, Berkeley, California 94720, USA and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)

    2014-03-21

    We apply Non-orthogonal Configuration Interaction (NOCI) to molecular systems where multielectron excitations, in this case double excitations, play a substantial role: the linear polyenes and β-carotene. We demonstrate that NOCI when applied to systems with extended conjugation, provides a qualitatively correct wavefunction at a fraction of the cost of many other multireference treatments. We also present a new extension to this method allowing for purification of higher-order spin states by utilizing Generalized Hartree-Fock Slater determinants and the details for computing 〈S{sup 2}〉 for the ground and excited states.

  19. Ab initio electron propagators in molecules with strong electron-phonon interaction: II. Electron Green's function.

    Science.gov (United States)

    Dahnovsky, Yuri

    2007-07-07

    Ab initio electron propagator methods are developed to study electronic properties of molecular systems with strong electron-electron and electron-phonon interactions. For the calculation of electron Green's functions we apply a canonical small polaron transformation that intrinsically contains strong electron-phonon effects. In the transformed Hamiltonian, the energy levels for the noninteracting particles are shifted down by the relaxation (solvation) energies. The Coulomb integrals are also renormalized by the electron-phonon interaction. For certain values of the electron-phonon coupling constants, the renormalized Coulomb integrals can be negative which implies the attraction between two electrons. Within the small polaron transformation we develop a diagrammatic technique for the calculation of electron Green's function in which the electron-phonon interaction is already included into the multiple phonon correlation functions. Since the decoupling of the phonon correlation functions is impossible, and therefore, a Wick's theorem for such correlation functions is invalid, there is no Dyson equation for the electron Green's function. To find the electron Green's function, we use different approximations. One of them is a link-cluster approximation that includes diagonal transitions for the renormalized zeroth Green's function. In the linked-cluster approach the Dyson equation is derived in the most general case, where the self-energy operator is an arbitrary functional (not only in the Hartree-Fock approximation). It is shown that even a Hartree-Fock electron (hole) is not a particle any longer. It is a quasiparticle with a finite lifetime that depends on energy of particle and hole states in different ways. As a consequence of this, a standard description of a Hartree-Fock approximation in terms of wave functions becomes inappropriate in this problem. To challenge the linked-cluster approximation we develop a different approach: a sequential propagation

  20. Role of spin-orbit interaction in the chemical potential of quantum dots in a magnetic field

    Science.gov (United States)

    Emperador, Agustí; Lipparini, E.; Pederiva, F.

    2004-09-01

    We have studied the relevance of spin-orbit coupling to the chemical potential of semiconductor dots submitted to a perpendicularly applied magnetic field B . The energy of the ground state of the dot is calculated within Hartree-Fock (HF), local spin-density functional theory (LSDA) and fixed phase quantum Monte Carlo (FP-DMC) and the interplay between spin-orbit and exchange-correlation interactions is carefully investigated. The results are compared with the experimental curves obtained by means of conductance spectroscopy.

  1. The Explicit Wake Parametrisation V1.0: a wind farm parametrisation in the mesoscale model WRF

    Directory of Open Access Journals (Sweden)

    P. J. H. Volker

    2015-11-01

    Full Text Available We describe the theoretical basis, implementation, and validation of a new parametrisation that accounts for the effect of large offshore wind farms on the atmosphere and can be used in mesoscale and large-scale atmospheric models. This new parametrisation, referred to as the Explicit Wake Parametrisation (EWP, uses classical wake theory to describe the unresolved wake expansion. The EWP scheme is validated for a neutral atmospheric boundary layer against filtered in situ measurements from two meteorological masts situated a few kilometres away from the Danish offshore wind farm Horns Rev I. The simulated velocity deficit in the wake of the wind farm compares well to that observed in the measurements, and the velocity profile is qualitatively similar to that simulated with large eddy simulation models and from wind tunnel studies. At the same time, the validation process highlights the challenges in verifying such models with real observations.

  2. Observations of surface momentum exchange over the marginal ice zone and recommendations for its parametrisation

    Directory of Open Access Journals (Sweden)

    A. D. Elvidge

    2016-02-01

    Full Text Available Comprehensive aircraft observations are used to characterise surface roughness over the Arctic marginal ice zone (MIZ and consequently make recommendations for the parametrisation of surface momentum exchange in the MIZ. These observations were gathered in the Barents Sea and Fram Strait from two aircraft as part of the Aerosol–Cloud Coupling And Climate Interactions in the Arctic (ACCACIA project. They represent a doubling of the total number of such aircraft observations currently available over the Arctic MIZ. The eddy covariance method is used to derive estimates of the 10 m neutral drag coefficient (CDN10 from turbulent wind velocity measurements, and a novel method using albedo and surface temperature is employed to derive ice fraction. Peak surface roughness is found at ice fractions in the range 0.6 to 0.8 (with a mean interquartile range in CDN10 of 1.25 to 2.85  ×  10−3. CDN10 as a function of ice fraction is found to be well approximated by the negatively skewed distribution provided by a leading parametrisation scheme (Lüpkes et al., 2012 tailored for sea-ice drag over the MIZ in which the two constituent components of drag – skin and form drag – are separately quantified. Current parametrisation schemes used in the weather and climate models are compared with our results and the majority are found to be physically unjustified and unrepresentative. The Lüpkes et al. (2012 scheme is recommended in a computationally simple form, with adjusted parameter settings. A good agreement holds for subsets of the data from different locations, despite differences in sea-ice conditions. Ice conditions in the Barents Sea, characterised by small, unconsolidated ice floes, are found to be associated with higher CDN10 values – especially at the higher ice fractions – than those of Fram Strait, where typically larger, smoother floes are observed. Consequently, the important influence of sea-ice morphology and floe size on

  3. Role of the Skyrme tensor force in heavy-ion fusion

    Directory of Open Access Journals (Sweden)

    Stevenson P. D.

    2015-01-01

    Full Text Available We make use of the Skyrme effective nuclear interaction within the time-dependent Hartree-Fock framework to assess the effect of inclusion of the tensor terms of the Skyrme interaction on the fusion window of the 16O–16O reaction. We find that the lower fusion threshold, around the barrier, is quite insensitive to these details of the force, but the higher threshold, above which the nuclei pass through each other, changes by several MeV between different tensor parametrisations. The results suggest that eventually fusion properties may become part of the evaluation or fitting process for effective nuclear interactions.

  4. Stochastic Parametrisations and Regime Behaviour of Atmospheric Models

    Science.gov (United States)

    Arnold, Hannah; Moroz, Irene; Palmer, Tim

    2013-04-01

    The presence of regimes is a characteristic of non-linear, chaotic systems (Lorenz, 2006). In the atmosphere, regimes emerge as familiar circulation patterns such as the El-Nino Southern Oscillation (ENSO), the North Atlantic Oscillation (NAO) and Scandinavian Blocking events. In recent years there has been much interest in the problem of identifying and studying atmospheric regimes (Solomon et al, 2007). In particular, how do these regimes respond to an external forcing such as anthropogenic greenhouse gas emissions? The importance of regimes in observed trends over the past 50-100 years indicates that in order to predict anthropogenic climate change, our climate models must be able to represent accurately natural circulation regimes, their statistics and variability. It is well established that representing model uncertainty as well as initial condition uncertainty is important for reliable weather forecasts (Palmer, 2001). In particular, stochastic parametrisation schemes have been shown to improve the skill of weather forecast models (e.g. Berner et al., 2009; Frenkel et al., 2012; Palmer et al., 2009). It is possible that including stochastic physics as a representation of model uncertainty could also be beneficial in climate modelling, enabling the simulator to explore larger regions of the climate attractor including other flow regimes. An alternative representation of model uncertainty is a perturbed parameter scheme, whereby physical parameters in subgrid parametrisation schemes are perturbed about their optimal value. Perturbing parameters gives a greater control over the ensemble than multi-model or multiparametrisation ensembles, and has been used as a representation of model uncertainty in climate prediction (Stainforth et al., 2005; Rougier et al., 2009). We investigate the effect of including representations of model uncertainty on the regime behaviour of a simulator. A simple chaotic model of the atmosphere, the Lorenz '96 system, is used to study

  5. Molecular equilibrium structures from experimental rotational constants and calculated vibration-rotation interaction constants

    DEFF Research Database (Denmark)

    Pawlowski, F; Jorgensen, P; Olsen, Jeppe

    2002-01-01

    A detailed study is carried out of the accuracy of molecular equilibrium geometries obtained from least-squares fits involving experimental rotational constants B(0) and sums of ab initio vibration-rotation interaction constants alpha(r)(B). The vibration-rotation interaction constants have been...... calculated for 18 single-configuration dominated molecules containing hydrogen and first-row atoms at various standard levels of ab initio theory. Comparisons with the experimental data and tests for the internal consistency of the calculations show that the equilibrium structures generated using Hartree......-Fock vibration-rotation interaction constants have an accuracy similar to that obtained by a direct minimization of the CCSD(T) energy. The most accurate vibration-rotation interaction constants are those calculated at the CCSD(T)/cc-pVQZ level. The equilibrium bond distances determined from these interaction...

  6. Quantum Monte Carlo study of the two-dimensional electron gas in presence of Rashba interaction

    Science.gov (United States)

    Ambrosetti, A.; Pederiva, F.; Lipparini, E.; Gandolfi, S.

    2009-09-01

    We introduce a variant to the diffusion Monte Carlo algorithm that can be employed to study the effects of the Rashba interaction in many-electron systems. Because of the spin-orbit nature of Rashba interaction a standard algorithm cannot be applied and therefore a specific imaginary time spin-dependent propagator has been developed and implemented following previous work developed in the framework of nuclear physics. We computed the ground-state energy of the two-dimensional electron gas at different densities for several values of the Rashba interaction strength as a function of “Rashba spin states” polarization. Comparison is given with analytically known Hartree-Fock results and for the system in absence of Coulomb interaction.

  7. Structural study and investigation of NMR tensors in interaction of dopamine with Adenine and guanine

    Directory of Open Access Journals (Sweden)

    Lingjia Xu

    2007-04-01

    Full Text Available The interaction of dopamine with adenine and guanine were studied at the Hartree-Fock level theory. The structural and vibrational properties of dopamine-4-N7GUA and dopamine-4-N3ADE were studied at level of HF/6-31G*. Interaction energies (ΔE were calculated to be -11.49 and -11.92 kcal/mol, respectively. Some of bond lengths, angels and tortions are compared. NBO studies were performed to the second-order and perturbative estimates of donor-acceptor interaction have been done. The procedures of gauge-invariant atomic orbital (GIAO and continuous-set-of-gauge-transformation (CSGT were employed to calculate isotropic shielding, chemical shifts anisotropy and chemical shifts anisotropy asymmetry and effective anisotropy using 6-31G* basis set. These calculations yielded molecular geometries in good agreement with available experimental data.

  8. Ab initio MCDHF calculations of electron-nucleus interactions

    Science.gov (United States)

    Bieroń, Jacek; Froese Fischer, Charlotte; Fritzsche, Stephan; Gaigalas, Gediminas; Grant, Ian P.; Indelicato, Paul; Jönsson, Per; Pyykkö, Pekka

    2015-05-01

    We present recent advances in the development of atomic ab initio multiconfiguration Dirac-Hartree-Fock theory, implemented in the GRASP relativistic atomic structure code. For neutral atoms, the deviations of properties calculated within the Dirac-Hartree-Fock (DHF) method (based on independent particle model of an atomic cloud) are usually dominated by electron correlation effects, i.e. the non-central interactions of individual electrons. We present the recent advances in accurate calculations of electron correlation effects in small, medium, and heavy neutral atoms. We describe methods of systematic development of multiconfiguration expansions leading to systematic, controlled improvement of the accuracy of the ab initio calculations. These methods originate from the concept of the complete active space (CAS) model within the DHF theory, which, at least in principle, permits fully relativistic calculations with full account of electron correlation effects. The calculations within the CAS model on currently available computer systems are feasible only for very light systems. For heavier atoms or ions with more than a few electrons, restrictions have to be imposed on the multiconfiguration expansions. We present methods and tools, which are designed to extend the numerical calculations in a controlled manner, where multiconfiguration expansions account for all leading electron correlation effects. We show examples of applications of the GRASP code to calculations of hyperfine structure constants, but the code may be used for calculations of arbitrary bound-state atomic properties. In recent years it has been applied to calculations of atomic and ionic spectra (transition energies and rates), to determinations of nuclear electromagnetic moments, as well as to calculations related to interactions of bound electrons with nuclear electromagnetic moments leading to violations of discrete symmetries.

  9. The interaction-strength interpolation method for main-group chemistry: benchmarking, limitations, and perspectives

    CERN Document Server

    Fabiano, E; Seidl, M; Della Sala, F

    2016-01-01

    We have tested the original interaction-strength-interpolation (ISI) exchange-correlation functional for main group chemistry. The ISI functional is based on an interpolation between the weak and strong coupling limits and includes exact-exchange as well as the G\\"orling-Levy second-order energy. We have analyzed in detail the basis-set dependence of the ISI functional, its dependence on the ground-state orbitals, and the influence of the size-consistency problem. We show and explain some of the expected limitations of the ISI functional (i.e. for atomization energies), but also unexpected results, such as the good performance for the interaction energy of dispersion-bonded complexes when the ISI correlation is used as a correction to Hartree-Fock.

  10. Effects of symmetry energy and momentum dependent interaction on low-energy reaction mechanisms

    Directory of Open Access Journals (Sweden)

    Zheng H.

    2016-01-01

    Full Text Available We study the dipole response associated with the Pygmy Dipole Resonance (PDR and the Isovector Giant Dipole Resonance (IVGDR, in connection with specific properties of the nuclear effective interaction (symmetry energy and momentum dependence, in the neutron-rich systems 68Ni, 132Sn and 208Pb. We perform our investigation within a microscopic transport model based on the Landau-Vlasov kinetic equation.We observe that the peak energies of PDR and IVGDR are shifted to higher values when employing momentum dependent interactions, with respect to the results obtained neglecting momentum dependence. The calculated energies are close to the experimental values and similar to the results obtained in Hartree-Fock (HF with Random Phase Approximation (RPA calculations.

  11. Thermodynamic instabilities of nuclear matter at finite temperature with finite range effective interactions

    Energy Technology Data Exchange (ETDEWEB)

    Ventura, J.; Polls, A.; Vinas, X.; Pi, M. (Barcelona Univ. (Spain). Dept. de Estructura y Constituyentes de la Materia); Hernandez, S. (Buenos Aires Univ. (Argentina). Dept. de Fisica)

    1992-08-03

    A systematic study of the equation of state for symmetric nuclear matter is performed in the framework of a finite-temperature density dependent Hartree-Fock method using the Gogny finite-range effective interaction. Special attention is devoted to the density and temperature dependence of the single-particle spectrum, the effective mass and the momentum distributions. The liquid-gas phase transition and the spinodal lines are discussed, in connection with the breakup of heated nucleus into small clusters that takes place in medium energy heavy ion reactions. The level density parameter, which has been derived by a low temperature expansion of the internal energy, is also discussed. Comparisons with previous calculations using zero range effective interactions are also made. (orig.).

  12. Spectral and thermodynamical properties of symmetric nuclear matter with Gogny interaction

    Energy Technology Data Exchange (ETDEWEB)

    Ventura, J. (Departament d' Estructura i Constituents de la Materia, Facultat de Fisica, Universitat de Barcelona, E-08028 Barcelona (Spain)); Polls, A. (Departament d' Estructura i Constituents de la Materia, Facultat de Fisica, Universitat de Barcelona, E-08028 Barcelona (Spain)); Vinas, X. (Departament d' Estructura i Constituents de la Materia, Facultat de Fisica, Universitat de Barcelona, E-08028 Barcelona (Spain)); Hernandez, E.S. (Departamento de Fisica, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, RA-1428 Buenos Aires (Argentina))

    1994-10-03

    The finite range effects of an effective force on the single particle properties and the particle-hole effective interaction are investigated in a wide interval of temperatures. The calculations are performed in a framework of a thermal Hartree-Fock method using the D1-Gogny density dependent interaction. First, the behaviour of the single particle potential, effective mass and the momentum distribution is discussed. The competition between statistical correlations and mean field effects is studied by analyzing the relative momentum distribution and the two-body distribution function. Secondly, a possible extension of the Landau Fermi liquid theory to finite temperatures is discussed in the context of symmetric nuclear matter. Special attention is devoted to the meaning of the Landau parameters and to the requirements for thermodynamic stability. In particular, the relation between the nuclear incompressibility and the F[sub 0][sup ss]-Landau amplitude at finite temperatures is carefully analyzed. ((orig.))

  13. Virtual Orbital Many-Body Expansions: A Possible Route towards the Full Configuration Interaction Limit.

    Science.gov (United States)

    Eriksen, Janus J; Lipparini, Filippo; Gauss, Jürgen

    2017-09-21

    It is demonstrated how full configuration interaction (FCI) results in extended basis sets may be obtained to within sub-kJ/mol accuracy by decomposing the energy in terms of many-body expansions in the virtual orbitals of the molecular system at hand. This extension of the FCI application range lends itself to two unique features of the current approach, namely, that the total energy calculation can be performed entirely within considerably reduced orbital subspaces and may be so by means of embarrassingly parallel programming. Facilitated by a rigorous and methodical screening protocol and further aided by expansion points different from the Hartree-Fock solution, all-electron numerical results are reported for H2O in polarized core-valence basis sets ranging from double-ζ (10 e, 28 o) to quadruple-ζ (10 e, 144 o) quality.

  14. Performance of the coupled cluster and DFT methods for through-space magnetic interactions of nitroxide dimer

    Science.gov (United States)

    Saito, Toru; Ito, Akira; Watanabe, Tomohiro; Kawakami, Takashi; Okumura, Mitsutaka; Yamaguchi, Kizashi

    2012-07-01

    We have performed comparisons of several theoretical methods focusing on the through-space interactions of the F2 molecule and nitroxide (dihydronitrosyl) dimer based on the exchange coupling constant. The restricted Hartree-Fock (RHF) based coupled cluster full singles, doubles, and triples (RHF-CCSDT) and approximations to it do not show the exponential decay with increasing intermolecular distance for both antiferromagnetic and ferromagnetic interactions. On the other hand, Mukherjee's multireference CCSD (MkCCSD) method and the unrestricted HF (UHF) based CCSD (UHF-CCSD) with an approximate spin-projection (AP) method give reliable results. The present benchmark calculations are expected to contribute to the selection of an appropriate density functional theory (DFT) exchange-correlation functionals for larger systems.

  15. Core polarization in coupled-cluster theory induced by a parity and time-reversal violating interaction

    Science.gov (United States)

    Latha, K. V. P.; Angom, Dilip; Chaudhuri, Rajat K.; Das, B. P.; Mukherjee, Debashis

    2008-02-01

    The effects of a parity and time-reversal violating potential, in particular the tensor-pseudotensor electron-nucleus interaction, are studied. We establish that selected terms representing the interplay of these effects and the residual Coulomb interaction in the coupled-cluster method are equivalent to the coupled-perturbed Hartree-Fock (CPHF). We have shown that the normal CPHF diagrams have a one-to-one correspondence in the coupled-cluster theory, but the CPHF pseudo diagrams are present in a subtle way. We have studied the pseudo diagrams in great detail and have shown explicitly their origin in the coupled-cluster theory. This is demonstrated by considering the case of the permanent electric dipole moment of atomic Hg, and our results are compared with the results of an earlier calculation.

  16. Core polarization in coupled-cluster theory induced by a parity and time-reversal violating interaction

    Energy Technology Data Exchange (ETDEWEB)

    Latha, K V P [Indian Institute of Astrophysics, Koramangala, Bangalore 560 034, Karnataka (India); Angom, Dilip [Physical Research Laboratory, Navarangapura, Ahmedabad 380 009, Gujarat (India); Chaudhuri, Rajat K [Indian Institute of Astrophysics, Koramangala, Bangalore 560 034, Karnataka (India); Das, B P [Indian Institute of Astrophysics, Koramangala, Bangalore 560 034, Karnataka (India); Mukherjee, Debashis [Indian Association of Cultivation of Science, Kolkata 700 032, West Bengal (India)

    2008-02-14

    The effects of a parity and time-reversal violating potential, in particular the tensor-pseudotensor electron-nucleus interaction, are studied. We establish that selected terms representing the interplay of these effects and the residual Coulomb interaction in the coupled-cluster method are equivalent to the coupled-perturbed Hartree-Fock (CPHF). We have shown that the normal CPHF diagrams have a one-to-one correspondence in the coupled-cluster theory, but the CPHF pseudo diagrams are present in a subtle way. We have studied the pseudo diagrams in great detail and have shown explicitly their origin in the coupled-cluster theory. This is demonstrated by considering the case of the permanent electric dipole moment of atomic Hg, and our results are compared with the results of an earlier calculation.

  17. Detailed Analysis of Configuration Interaction and Calculation of Radiative Transition Rates in Seven Times Ionized Tungsten (W VIII

    Directory of Open Access Journals (Sweden)

    Jérôme Deprince

    2015-06-01

    Full Text Available A new set of oscillator strengths and transition probabilities for EUV spectral lines of seven times ionized tungsten (W VIII is reported in the present paper. These results have been obtained using the pseudo-relativistic Hartree-Fock (HFR method combined with a semi-empirical optimization of the radial parameters minimizing the discrepancies between computed energy levels and available experimental data. The final physical model considered in the calculations has been chosen further to a detailed investigation of the configuration interaction in this atomic system characterized by complex configurations of the type 4f145s25p5, 4f145s25p4nl, 4f145s5p6, 4f135s25p6, 4f135s25p5nl and 4f125s25p6nl (nl = 5d, 6s.

  18. Description of odd-mass nuclei within the interacting boson-fermion model based on the Gogny energy density functional

    Science.gov (United States)

    Nomura, K.; Rodríguez-Guzmán, R.; Robledo, L. M.

    2017-07-01

    Spectroscopic properties of odd-mass nuclei are studied within the framework of the interacting boson-fermion model (IBFM) with parameters based on the Hartree-Fock-Bogoliubov (HFB) approximation. The parametrization D1M of the Gogny energy density functional (EDF) was used at the mean-field level to obtain the deformation energy surfaces for the considered nuclei in terms of the quadrupole deformations (β ,γ ). In addition to the energy surfaces, both single-particle energies and occupation probabilities were used as a microscopic input for building the IBFM Hamiltonian. Only three strength parameters for the particle-boson-core coupling are fitted to experimental spectra. The IBFM Hamiltonian is then used to compute the energy spectra and electromagnetic transition rates for selected odd-mass Eu and Sm nuclei as well as for 195Pt and 195Au. A reasonable agreement with the available experimental data is obtained for the considered odd-mass nuclei.

  19. Computational Modeling of Light Induced Transformations in Organic Molecule

    Science.gov (United States)

    2008-08-31

    ground states with restricted Hartree- Fock method ( RHF ). The energies of the excited states are found within the configuration interaction approach...isolated retinal. We calculated the potential energy vs torsion angle for the ground state S0 with Restricted Hartree-Fock ( RHF ) method and 7

  20. Fusion hindrance in heavy systems with time-dependent Hartree-Fock

    Science.gov (United States)

    Washiyama, Kouhei

    2017-11-01

    We analyze fusion hindrance in heavy systems, where the fusion probability around the Coulomb barrier is hindered compared with that in light and medium-mass systems. We perform simulations of central collisions around the Coulomb barrier in heavy systems with time-dependent Hartree‒Fock (TDHF) and find that the fusion hindrance is realized in TDHF simulations. We extract nucleus‒nucleus potential and energy dissipation in heavy systems by a method combining a microscopic TDHF evolution to a macroscopic collective equation of motion. We find that the extracted potentials exhibit a dynamical increase at small relative distances, while the extracted friction coefficients show rather a behavior similar to that in light and medium-mass systems. We find from our analysis that the dynamical increase in potential is a main contribution to this fusion hindrance.

  1. Spin-Excitation Mechanisms in Skyrme-Force Time-Dependent Hartree-Fock

    OpenAIRE

    Maruhn, J. A.; Reinhard, P. -G.; Stevenson, P. D.; Strayer, M. R.

    2006-01-01

    We investigate the role of odd-odd (with respect to time inversion) couplings in the Skyrme force on collisions of light nuclei, employing a fully three-dimensional numerical treatment without any symmetry restrictions and with modern Skyrme functionals. We demonstrate the necessity of these couplings to suppress spurious spin excitations owing to the spin-orbit force in free translational motion of a nucleus but show that in a collision situation there is a strong spin excitation even in spi...

  2. Recent developments and applications of multi-configuration Hartree-Fock methods. NRCC proceedings No. 10

    Energy Technology Data Exchange (ETDEWEB)

    Dupuis, M. (ed.)

    1981-02-01

    Twenty-seven papers are included in four sessions titled: generalized Fock operator methods, annihilation of single excitations methods, second-order MCSCF methods, and applications of MCHF methods. Separate abstracts were prepared for eight papers; one of the remaining had been previously abstracted. (DLC)

  3. Etude hartree-fock de la tautomerisation du 1azirene sous pression ...

    African Journals Online (AJOL)

    The lazirene molecule is a heterocyclic compound containing two carbon atoms, one nitrogen atom and three hydrogen atoms which one is on the nitrogen atom. The hydrogen pressure being represented by one molecule of dihydrogen, the reaction of the dihydrogen with the azirene in the presence of the palladium ...

  4. Hartree-Fock energy derivatives with respect to basis set exponents. Integral derivatives using Rys polynomials

    Science.gov (United States)

    Tonachini, Glauco; Schlegel, H. Bernhard

    1987-07-01

    The Rys polynomial method has been used to evaluate the first derivatives of the two electron integrals and the nuclear electron attraction integrals with respect to the Gaussian exponents. Gradients for the sulfur 6-31 G(d) basis set in HS-, H2S, H3S+, H2S2, H3CSH, H2CS, CS, H2SO, SO2 and SO3 have been evaluated to illustrate the effect of charge, multiple bonding and hypervalency on the basis set exponents.

  5. Properties of young contrails – a parametrisation based on large-eddy simulations

    Directory of Open Access Journals (Sweden)

    S. Unterstrasser

    2016-02-01

    adiabatic heating. The geometric depth H and total ice crystal number N of young contrails are highly variable and depend on many environmental and aircraft parameters. Both properties, H and N, affect the later properties of the evolving contrail–cirrus, as they control the extent of shear-induced spreading and sedimentation losses. In this study, we provide parametrisations of H and N after 5 min taking into account the effects of temperature, relative humidity, thermal stratification and aircraft type (mass, wing span, fuel burn. The parametrisations rely on a large data set of recent large-eddy simulations of young contrails. They are suited to be incorporated in larger-scale models in order to refine the present-day contrail initialisations by considering the processes that strongly affect the contrail evolution during the vortex phase.

  6. Baryons and baryonic matter in four-fermion interaction models

    Energy Technology Data Exchange (ETDEWEB)

    Urlichs, K.

    2007-02-23

    In this work we discuss baryons and baryonic matter in simple four-fermion interaction theories, the Gross-Neveu model and the Nambu-Jona-Lasinio model in 1+1 and 2+1 space-time dimensions. These models are designed as toy models for dynamical symmetry breaking in strong interaction physics. Pointlike interactions (''four-fermion'' interactions) between quarks replace the full gluon mediated interaction of quantum chromodynamics. We consider the limit of a large number of fermion flavors, where a mean field approach becomes exact. This method is formulated in the language of relativistic many particle theory and is equivalent to the Hartree-Fock approximation. In 1+1 dimensions, we generalize known results on the ground state to the case where chiral symmetry is broken explicitly by a bare mass term. For the Gross-Neveu model, we derive an exact self-consistent solution for the finite density ground state, consisting of a one-dimensional array of equally spaced potential wells, a baryon crystal. For the Nambu- Jona-Lasinio model we apply the derivative expansion technique to calculate the total energy in powers of derivatives of the mean field. In a picture akin to the Skyrme model of nuclear physics, the baryon emerges as a topological soliton. The solution for both the single baryon and dense baryonic matter is given in a systematic expansion in powers of the pion mass. The solution of the Hartree-Fock problem is more complicated in 2+1 dimensions. In the massless Gross-Neveu model we derive an exact self-consistent solution by extending the baryon crystal of the 1+1 dimensional model, maintaining translational invariance in one spatial direction. This one-dimensional configuration is energetically degenerate to the translationally invariant solution, a hint in favor of a possible translational symmetry breakdown by more general geometrical structures. In the Nambu-Jona-Lasinio model, topological soliton configurations induce a finite baryon

  7. Effective interactions for extreme isospin conditions; Interactions effectives pour des conditions extremes d`isospin

    Energy Technology Data Exchange (ETDEWEB)

    Chabanat, E.

    1995-01-01

    One of the main goal in nuclear physics research is the study of nuclei in extreme conditions of spin and isospin. The more performing tools for theoretical predictions in this field are microscopic methods such as the Hartree-Fock one based on independent particle approximation. The main ingredient for such an approach is the effective nucleon-nucleon interaction. The actual trend being the study of nuclei more and more far from the stability valley, it is necessary to cast doubt over the validity of usual effective interaction. This work constitute a study on the way one can construct a new interaction allowing some theoretical predictions on nuclei far from the stability. We have thus made a complete study of symmetric infinite nuclear matter and asymmetric one up to pure neutron matter. One shows that the asymmetry coefficient, which was considered until now as fixing isospin properties, is not sufficient to have a correct description of very exotic isospin states. A new type of constraint is shown for fixing this degree of freedom: the neutron matter equation of state. One include this equation of state, taken from a theoretical model giving a good description of radii and masses of neutron stars. One can thus expect to build up new Skyrme interaction with realistic properties of ground state of very neutron-rich nuclei. (author). 63 refs., 68 figs., 15 tabs.

  8. Compressibility enhancement in an almost staggered interacting Harper model

    Science.gov (United States)

    Friedman, Bat-el; Berkovits, Richard

    2015-03-01

    We discuss the compressibility in the almost staggered fermionic Harper model with repulsive interactions in the vicinity of half-filling. It has been shown by Kraus et al. [Phys. Rev. B 89, 161106(R) (2014)], 10.1103/PhysRevB.89.161106 that for spinless electrons and nearest neighbors electron-electron interactions the compressibility in the central band is enhanced by repulsive interactions. Here we would like to investigate the sensitivity of this conclusion to the spin degree of freedom and longer range interactions. We use the Hartree-Fock (HF) approximation, as well as the density matrix renormalization group (DMRG) calculation to evaluate the compressibility. In the almost staggered Harper model, the central energy band is essentially flat and separated from the other bands by a large gap and therefore, the HF approximation is rather accurate. In both cases the compressibility of the system is enhanced compared to the noninteracting case, although the enhancement is weaker due to the inclusion of Hubbard and longer ranged interactions. We also show that the entanglement entropy is suppressed when the compressibility of the system is enhanced.

  9. Impact of different wave physics parametrisations in ECMWF Earth System model

    Science.gov (United States)

    Bidlot, Jean-Raymond

    2017-04-01

    The global analyses and medium range forecasts from the European Centre for Medium range Weather Forecasts rely on a state of the art atmospheric model. In order to best represent the momentum exchange at the surface of the oceans, it is tightly coupled to an ocean wave model. Recently, an ocean model has been included as part of the operational medium range forecasting system. In this context, a first set of sea state effects on Upper Ocean mixing and dynamics was successfully added to the system. Impact of sea-state dependent momentum forcing, the Stokes-Coriolis force and the enhanced mixing by breaking ocean waves have been added. So far, the implementation of the coupled system was done with ECMWF own wave physics parametrisation, an evolution of the original WAM cycle-4 physics. The ST4 physics from WaveWatch 3 has already been implemented in ECWAM and is used by Météo France in their standalone configuration. Plans are to also introduce the ST6 version. A first assessment of the different parametrisations will be presented in the context of the fully coupled system.

  10. The impact of lightning on tropospheric ozone chemistry using a new global lightning parametrisation

    Directory of Open Access Journals (Sweden)

    D. L. Finney

    2016-06-01

    Full Text Available A lightning parametrisation based on upward cloud ice flux is implemented in a chemistry–climate model (CCM for the first time. The UK Chemistry and Aerosols model is used to study the impact of these lightning nitric oxide (NO emissions on ozone. Comparisons are then made between the new ice flux parametrisation and the commonly used, cloud-top height parametrisation. The ice flux approach improves the simulation of lightning and the temporal correlations with ozone sonde measurements in the middle and upper troposphere. Peak values of ozone in these regions are attributed to high lightning NO emissions. The ice flux approach reduces the overestimation of tropical lightning apparent in this CCM when using the cloud-top approach. This results in less NO emission in the tropical upper troposphere and more in the extratropics when using the ice flux scheme. In the tropical upper troposphere the reduction in ozone concentration is around 5–10 %. Surprisingly, there is only a small reduction in tropospheric ozone burden when using the ice flux approach. The greatest absolute change in ozone burden is found in the lower stratosphere, suggesting that much of the ozone produced in the upper troposphere is transported to higher altitudes. Major differences in the frequency distribution of flash rates for the two approaches are found. The cloud-top height scheme has lower maximum flash rates and more mid-range flash rates than the ice flux scheme. The initial Ox (odd oxygen species production associated with the frequency distribution of continental lightning is analysed to show that higher flash rates are less efficient at producing Ox; low flash rates initially produce around 10 times more Ox per flash than high-end flash rates. We find that the newly implemented lightning scheme performs favourably compared to the cloud-top scheme with respect to simulation of lightning and tropospheric ozone. This alternative lightning scheme shows spatial and

  11. Ensemble simulations with perturbed physical parametrisations: Pre-HyMeX case studies

    Science.gov (United States)

    Hally, A.; Fresnay, S.; Richard, E.; Lambert, D.

    2012-04-01

    During the last 15 or 20 years, ensemble prediction systems have made substantial progress and have become an indispensable tool in forecasting the probability of certain weather events. Recent improvements in computer-modelling have also allowed convection and other physically complex processes to be well represented within atmospheric models. This however has also led to more questions, such as the representation of uncertainties in the initial field, the definition of boundary conditions, along with other areas of incertitude in the model. The relative importance of each field remains to be investigated more vigorously in order to allow for further improvements in forecasting, especially for heavy rainfall episodes, which can have large social and economic consequences. This study focuses on model uncertainties related to cloud physics and turbulence parametrisations, which have been so far less studied than other areas such as boundary or initial state uncertainties. The sensitivity of the precipitation forecasts to the details of the parametrisation are assessed by (a) varying the tunable parameters of micro-physical and turbulence schemes of the model within their range of allowed values and (b) by introducing random perturbations on the factors which govern hydro-meteor and/or turbulent kinetic energy evolution. An ensemble of simulations was performed in order to find the optimum setting of the model in relation to the forecasting of precipitation events. Two different sets of initial and boundary conditions were used during the ensembles, one from the French forecasting model AROME and the other from the ECMWF analyses. This methodology was applied in particular to the cases of the 1st to the 5th of November 2011 and the 6th - 7th of September 2010 which prefigure the heavy precipitation events expected to occur during the HyMeX field campaign of Autumn 2012. The simulations were performed with the French research model MESO-NH. The results show that the

  12. Wind friction parametrisation used in emission models for wastewater treatment plants: A critical review.

    Science.gov (United States)

    Prata, Ademir A; Santos, Jane M; Timchenko, Victoria; Reis, Neyval C; Stuetz, Richard M

    2017-11-01

    Emission models are widely applied tools for estimating atmospheric emissions from wastewater treatment plants (WWTPs). The friction velocity u∗ is a key variable for the modelling of emissions from passive liquid surfaces in WWTPs. This work evaluated different parametrisations of u∗ for passive liquid surfaces at the scale of WWTP units, which present relatively small fetches, based on available wind friction and wave data measured at wind-wave tanks (fetches spanning from approximately 3 to 100 m, and wind speeds from 2 to 17 m s(-1)). The empirical correlation by Smith (1980; J. Phys. Oceanogr. 10, 709-726), which has been frequently adopted in air emission models (despite the fact that it was originally derived for the ocean) presented a general tendency to overestimate u∗, with significant (although not extreme) relative errors (mean and maximum errors of 13.5% and 36.6%, respectively); the use of Charnock's relation, with Charnock constant 0.010, performed in a very similar manner (mean and maximum errors of 13.3% and 37.8%, respectively). Better estimates of u∗ were achieved by parametrisations based on the significant wave steepness. Simplified correlations between the wind drag and the non-dimensional fetch were obtained. An approach was devised, comprising the use of Charnock's relation (with Charnock constant 0.010) and of these simplified correlations, depending on the ranges of frequency of the peak waves, fetch and wind speed. The proposed approach predicted u∗ with improved accuracy (mean, maximum and 95%-percentile relative errors of 6.6%, 16.7% and 13.9%, respectively), besides being able to incorporate the influence of the fetch in the wind drag, thus taking into account the size of the tanks in the WWTPs. Copyright © 2017 Elsevier Ltd. All rights reserved.

  13. Properties of young contrails – a parametrisation based on large-eddy simulations

    Directory of Open Access Journals (Sweden)

    S. Unterstrasser

    2016-02-01

    Full Text Available Contrail–cirrus is probably the largest climate forcing from aviation. The evolution of contrail–cirrus and its radiative impact depends not only on a multitude of atmospheric parameters, but also on the geometric and microphysical properties of the young contrails evolving into contrail–cirrus. The early evolution of contrails (t  <  5 min is dominated by an interplay of ice microphysics and wake vortex dynamics. Young contrails may undergo a fast vertical expansion due to a descent of the wake vortices and may lose a substantial fraction of their ice crystals due to adiabatic heating. The geometric depth H and total ice crystal number N of young contrails are highly variable and depend on many environmental and aircraft parameters. Both properties, H and N, affect the later properties of the evolving contrail–cirrus, as they control the extent of shear-induced spreading and sedimentation losses. In this study, we provide parametrisations of H and N after 5 min taking into account the effects of temperature, relative humidity, thermal stratification and aircraft type (mass, wing span, fuel burn. The parametrisations rely on a large data set of recent large-eddy simulations of young contrails. They are suited to be incorporated in larger-scale models in order to refine the present-day contrail initialisations by considering the processes that strongly affect the contrail evolution during the vortex phase.

  14. Interaction-induced phase transitions of type-II Weyl semimetals

    Science.gov (United States)

    Wang, Yi-Xiang; Li, Fuxiang; Bian, Baoan

    2017-10-01

    The study of Weyl semimetals (WSMs) lies at the forefront of the nontrivial topological phenomena in condensed-matter physics. In this work, we study the effect of on-site repulsive Hubbard interaction on the WSM system with a nonzero tilt at half filling. Within the Hartree-Fock mean-field approximation, we treat the Hubbard interaction self-consistently and find that the Fock exchange field vanishes, while the Hartree field can renormalize the topological mass, the tilt, and the Fermi velocity of the Weyl cones. When the renormalized tilt is larger than the renormalized Fermi velocity, the Hubbard interaction will induce the quantum phase transition from a type-I WSM to a type-II WSM. We then provide the interaction-induced phase diagrams of WSMs in different parametric spaces, in which the antiferromagnetic order at strong interaction is also considered. In addition, we analyze another model hosting two pairs of Weyl nodes, and similar results are obtained. The implications of these results are discussed.

  15. Analytic gradients in electronic structure theory

    Science.gov (United States)

    Shroll, Robert Marvin

    1997-10-01

    The energy gradients for the Hartree Fock ground state, Dirac-Hartree-Fock ground state, singles-only configuration interaction approximation to the first singlet excited state, and a set of restricted singles- only configuration interaction equations are presented. Algebraic approximations will be used in all of these state energy equation derivations. This leads us to a commonality between the various methods which is the need to calculate gradients with respect to basis set expansion coefficients. For the non-relativistic correlated energy states, these coefficient derivatives will be determined using Coupled Perturbed Hartree Fock (CPHF) theory. For the relativistic case, an analogous set of equations are presented which have been called the Coupled Perturbed Dirac-Hartree-Fock (CPDHF) equations.

  16. Interaction quench in the Holstein model: Thermalization crossover from electron- to phonon-dominated relaxation

    Science.gov (United States)

    Murakami, Yuta; Werner, Philipp; Tsuji, Naoto; Aoki, Hideo

    2015-01-01

    We study the relaxation of the Holstein model after a sudden switch-on of the interaction by means of the nonequilibrium dynamical mean field theory, with the self-consistent Migdal approximation as an impurity solver. We show that there exists a qualitative change in the thermalization dynamics as the interaction is varied in the weak-coupling regime. On the weaker interaction side of this crossover, the phonon oscillations are damped more rapidly than the electron thermalization time scale, as determined from the relaxation of the electron momentum distribution function. On the stronger interaction side, the relaxation of the electrons becomes faster than the phonon damping. In this regime, despite long-lived phonon oscillations, a thermalized momentum distribution is realized temporarily. The origin of the "thermalization crossover" found here is traced back to different behaviors of the electron and phonon self-energies as a function of the electron-phonon coupling. In addition, the importance of the phonon dynamics is demonstrated by comparing the self-consistent Migdal results with those obtained with a simpler Hartree-Fock impurity solver that neglects the phonon self-energy. The latter scheme does not properly describe the evolution and thermalization of isolated electron-phonon systems.

  17. Radio morphing - towards a full parametrisation of the radio signal from air showers

    Science.gov (United States)

    Zilles, A.; Charrier, D.; Kotera, K.; Le Coz, S.; Martineau-Huynh, O.; Medina, C.; Niess, V.; Tueros, M.; de Vries, K.

    2017-12-01

    Over the last decades, radio detection of air showers has been established as a detection technique for ultra-high-energy cosmic-rays impinging on the Earth's atmosphere with energies far beyond LHC energies. Today’s second-generation of digital radio-detection experiments, as e.g. AERA or LOFAR, are becoming competitive in comparison to already standard techniques e.g. fluorescence light detection. Thanks to a detailed understanding of the physics of the radio emission in extensive air showers, simulations of the radio signal are already successfully tested and applied in the reconstruction of cosmic rays. However the limits of the computational power resources are easily reached when it comes to computing electric fields at the numerous positions requested by large or dense antenna arrays. In the case of mountainous areas as e.g. for the GRAND array, where 3D shower simulations are necessary, the problem arises with even stronger acuity. Therefore we developed a full parametrisation of the emitted radio signal on the basis of generic shower simulations which will reduce the simulation time by orders of magnitudes. In this talk we will present this concept after a short introduction to the concept of the radio detection of air-shower induced by cosmic rays.

  18. Di-nucleon structures in homogeneous nuclear matter based on two- and three-nucleon interactions

    Energy Technology Data Exchange (ETDEWEB)

    Arellano, Hugo F. [University of Chile, Department of Physics - FCFM, Santiago (Chile); CEA, DAM, DIF, Arpajon (France); Isaule, Felipe [University of Chile, Department of Physics - FCFM, Santiago (Chile); Rios, Arnau [University of Surrey, Department of Physics, Faculty of Engineering and Physical Sciences, Guildford (United Kingdom)

    2016-09-15

    We investigate homogeneous nuclear matter within the Brueckner-Hartree-Fock (BHF) approach in the limits of isospin-symmetric nuclear matter (SNM) as well as pure neutron matter at zero temperature. The study is based on realistic representations of the internucleon interaction as given by Argonne v{sub 18}, Paris, Nijmegen I and II potentials, in addition to chiral N{sup 3}LO interactions, including three-nucleon forces up to N{sup 2}LO. Particular attention is paid to the presence of di-nucleon bound states structures in {sup 1}S{sub 0} and {sup 3}SD{sub 1} channels, whose explicit account becomes crucial for the stability of self-consistent solutions at low densities. A characterization of these solutions and associated bound states is discussed. We confirm that coexisting BHF single-particle solutions in SNM, at Fermi momenta in the range 0.13-0.3 fm{sup -1}, is a robust feature under the choice of realistic internucleon potentials. (orig.)

  19. The nature of three-body interactions in DFT: Exchange and polarization effects

    Science.gov (United States)

    Hapka, Michał; Rajchel, Łukasz; Modrzejewski, Marcin; Schäffer, Rainer; Chałasiński, Grzegorz; Szcześniak, Małgorzata M.

    2017-08-01

    We propose a physically motivated decomposition of density functional theory (DFT) 3-body nonadditive interaction energies into the exchange and density-deformation (polarization) components. The exchange component represents the effect of the Pauli exclusion in the wave function of the trimer and is found to be challenging for density functional approximations (DFAs). The remaining density-deformation nonadditivity is less dependent upon the DFAs. Numerical demonstration is carried out for rare gas atom trimers, Ar2-HX (X = F, Cl) complexes, and small hydrogen-bonded and van der Waals molecular systems. None of the tested semilocal, hybrid, and range-separated DFAs properly accounts for the nonadditive exchange in dispersion-bonded trimers. By contrast, for hydrogen-bonded systems, range-separated DFAs achieve a qualitative agreement to within 20% of the reference exchange energy. A reliable performance for all systems is obtained only when the monomers interact through the Hartree-Fock potential in the dispersion-free Pauli blockade scheme. Additionally, we identify the nonadditive second-order exchange-dispersion energy as an important but overlooked contribution in force-field-like dispersion corrections. Our results suggest that range-separated functionals do not include this component, although semilocal and global hybrid DFAs appear to imitate it in the short range.

  20. Hartree-fock-slater method for materials science the DV-X alpha method for design and characterization of materials

    CERN Document Server

    Adachi, H; Kawai, J

    2006-01-01

    Molecular-orbital calculations for materials design such as alloys, ceramics, and coordination compounds are now possible for experimentalists. Molecuar-orbital calculations for the interpretation of chemical effect of spectra are also possible for experimentalists. The most suitable molecular-orbital calculation method for these purpose is the DV-Xa method, which is robust in such a way that the calculation converges to a result even if the structure of the molecule or solid is impossible in the pressure and temperature ranges on earth. This book specially addresses the methods to design novel materials and to predict the spectralline shape of unknown materials using the DV-Xa molecular-orbital method, but is also useful for those who want to calculate electronic structures of materials using any kind of method.

  1. Manifestation of many-body interactions in the integer quantum Hall effect regime

    Science.gov (United States)

    Oswald, Josef; Römer, Rudolf A.

    2017-09-01

    We use the self-consistent Hartree-Fock approximation for numerically addressing the integer quantum Hall (IQH) regime in terms of many-body physics at higher Landau levels (LL). The results exhibit a strong tendency to avoid the simultaneous existence of partly filled spin-up and spin-down LLs. Partly filled LLs appear as a mixture of coexisting regions of full and empty LLs. We obtain edge stripes with approximately constant filling factor ν close to half-odd filling at the boundaries between the regions of full and empty LLs, which we explain in terms of the g -factor enhancement as a function of a locally varying ν across the compressible stripes. The many-particle interactions follow a behavior as it would result from applying Hund's rule for the occupation of the spin split LLs. The screening of the disorder and edge potential appears significantly reduced as compared to screening based on a Thomas-Fermi approximation. For addressing carrier transport, we use a nonequilibrium network model (NNM) that handles the lateral distribution of the experimentally injected nonequilibrium chemical potentials μ .

  2. The effect of exchange interaction on quasiparticle Landau levels in narrow-gap quantum well heterostructures.

    Science.gov (United States)

    Krishtopenko, S S; Gavrilenko, V I; Goiran, M

    2012-04-04

    Using the 'screened' Hartree-Fock approximation based on the eight-band k·p Hamiltonian, we have extended our previous work (Krishtopenko et al 2011 J. Phys.: Condens. Matter 23 385601) on exchange enhancement of the g-factor in narrow-gap quantum well heterostructures by calculating the exchange renormalization of quasiparticle energies, the density of states at the Fermi level and the quasiparticle g-factor for different Landau levels overlapping. We demonstrate that exchange interaction yields more pronounced Zeeman splitting of the density of states at the Fermi level and leads to the appearance of peak-shaped features in the dependence of the Landau level energies on the magnetic field at integer filling factors. We also find that the quasiparticle g-factor does not reach the maximum value at odd filling factors in the presence of large overlapping of spin-split Landau levels. We advance an argument that the behavior of the quasiparticle g-factor in weak magnetic fields is defined by a random potential of impurities in narrow-gap heterostructures. © 2012 IOP Publishing Ltd

  3. Li interactions with the B40 fullerene and its application in Li-ion batteries: DFT studies

    Science.gov (United States)

    Moradi, Morteza; Bagheri, Zargham; Bodaghi, Ali

    2017-05-01

    The interaction of Li and Li+ with a B40 all-boron fullerene was theoretically investigated at the B3LYP, and Minnesota 2006 levels of theory. It was found that, unexpectedly, the interaction Li+ cation with the electron deficient B40 fullerene is stronger than the Li atom. It indicates that the B40 fullerene does not act as a conventional Lewis acid because of its highly correlated structure. Frontier molecular orbitals, partial density of states, and natural bond orbital analyses were used to discuss this unusual behavior. Our calculations indicate that this behavior makes the B40 fullerene more appropriate for application in the Li-ion batteries as anode material. The calculated cell voltage is about 530 mV. Also, it was found that Hartree Fock (HF) exchange percentage of density functionals has a reverse effect on the adsorption energies of Li and Li+. This energy is increased and decreased, respectively, for Li+ and Li adsorptions by increasing %HF exchange. Finally, a potential energy surface for Li and Li+ penetration into B40 fullerene was predicted.

  4. Evaluation of a convective-microphysics parametrisation package in Tropical MJO-conditions

    Science.gov (United States)

    Van Ginderachter, Michiel

    2015-04-01

    The physical parametrisations inside the ALARO (ALADIN - AROME) NWP model are centred around the 3MT (Modular, Multi-scale, Microphysics and Transport) scheme. 3MT touches so many aspects of the feedbacks that determine the model-atmosphere's behaviour that it is difficult to characterise it synthetically, but it is aimed to tackle the typical convection grey-zone problems. Key elements to do so are scale-awareness, prognostic closure and no distinction of the origin of condensation from the microphysical point of view. The aim of the study is to test the ALARO model, which is developed and tuned mainly for mid-latitude weather, in the tropics. More precisely the model will be evaluated in the framework of the Madden-Julian Oscillation (MJO). This framework is chosen because it really targets the key concepts of the 3MT-scheme since the coupling between small-scale convective motions, mesoscale convective clusters, and the planetary scale waves appears to be fundamental to the MJO. The period of interest is chosen to be April 2009, which is a part of the well documented "Year of Tropical Convection" MJO case and the domain is centred around the Indian Ocean. Model runs were performed in two ways, the first one being a continuous run, where the model was initialized from the ECMWF re-analysis and runs freely for the whole month with coupling every six hours to the re-analysis. For the second run, the model is re-initialized every 24 houres (also coupled every six hours) from the re-analysis. As a first indication precipitation fields are analysed and compared with satellite data. First results look promising, especially for the daily re-initialized runs. Next cloudiness as well as vertical transport fluxes will be investigated. As a final step we will try to recreate the MJO index based on the first two principal components of the Empirical Orthogonal Functions of outgoing longwave radiation, u-wind at 850 and 200 hPa.

  5. Improved Limits on Axionlike-Particle-Mediated P , T -Violating Interactions between Electrons and Nucleons from Electric Dipole Moments of Atoms and Molecules

    Science.gov (United States)

    Stadnik, Y. V.; Dzuba, V. A.; Flambaum, V. V.

    2018-01-01

    In the presence of P , T -violating interactions, the exchange of axionlike particles between electrons and nucleons in atoms and molecules induces electric dipole moments (EDMs) of atoms and molecules. We perform calculations of such axion-exchange-induced atomic EDMs using the relativistic Hartree-Fock-Dirac method including electron core polarization corrections. We present analytical estimates to explain the dependence of these induced atomic EDMs on the axion mass and atomic parameters. From the experimental bounds on the EDMs of atoms and molecules, including Cs 133 , Tl 205 , Xe 129 , Hg 199 , Yb 171 F 19 , Hf 180 F+ 19 , and Th 232 O 16 , we constrain the P , T -violating scalar-pseudoscalar nucleon-electron and electron-electron interactions mediated by a generic axionlike particle of arbitrary mass. Our limits improve on existing laboratory bounds from other experiments by many orders of magnitude for ma≳10-2 eV . We also place constraints on C P violation in certain types of relaxion models.

  6. Relativistic effects in the intermolecular interaction-induced nuclear magnetic resonance parameters of xenon dimer

    DEFF Research Database (Denmark)

    Hanni, Matti; Lantto, Perttu; Ilias, Miroslav

    2007-01-01

    Relativistic effects on the 129Xe nuclear magnetic resonance shielding and 131Xe nuclear quadrupole coupling (NQC) tensors are examined in the weakly bound Xe2 system at different levels of theory including the relativistic four-component Dirac-Hartree-Fock (DHF) method. The intermolecular intera...

  7. Full configuration interaction potential energy curves for the X (1)Sigma(g) (+), B (1)Delta(g), and B(') (1)Sigma(g) (+) states of C(2): a challenge for approximate methods.

    Science.gov (United States)

    Abrams, Micah L; Sherrill, C David

    2004-11-15

    The C(2) molecule exhibits unusual bonding and several low-lying excited electronic states, making the prediction of its potential energy curves a challenging test for quantum chemical methods. We report full configuration interaction results for the X (1)Sigma(g) (+), B (1)Delta(g), and B(') (1)Sigma(g) (+) states of C(2), which exactly solve the electronic Schrodinger equation within the space spanned by a 6-31G( *) basis set. Within the D(2h) subgroup used by most electronic structure programs, these states all have the same symmetry ((1)A(g)), and all three states become energetically close for interatomic distances beyond 1.5 A. The quality of several single-reference ab initio methods is assessed by comparison to the benchmark results. Unfortunately, even coupled-cluster theory through perturbative triples using an unrestricted Hartree-Fock reference exhibits large nonparallelity errors (>20 kcal mol(-1)) for the ground state. The excited states are not accurately modeled by any commonly used single-reference method, nor by configuration interaction including full quadruple substitutions. The present benchmarks will be helpful in assessing theoretical methods designed to break bonds in ground and excited electronic states.

  8. SU-E-J-93: Parametrisation of Dose to the Mucosa of the Anterior Rectal Wall in Transrectal Ultrasound Guided High-Dose-Rate Brachytherapy of the Prostate

    Energy Technology Data Exchange (ETDEWEB)

    Aitkenhead, A; Hamlett, L; Wood, D; Choudhury, A [The Christie Hospital NHS Foundation Trust, Manchester, Greater Manchester (United Kingdom)

    2014-06-01

    Purpose: In high-dose-rate (HDR) brachytherapy of the prostate, radiation is delivered from a number of radioactive sources which are inserted via catheter into the target volume. The rectal mucosa also receives dose during the treatment, which may lead to late toxicity effects. To allow possible links between rectal dose and toxicity to be investigated, suitable methods of parametrising the rectal dose are needed. Methods: During treatment of a series of 95 patients, anatomy and catheter locations were monitored by transrectal ultrasound, and target volume positions were contoured on the ultrasound scan by the therapist. The anterior rectal mucosal wall was identified by contouring the transrectal ultrasound balloon within the ultrasound scan. Source positions and dwell times, along with the dose delivered to the patient were computed using the Oncentra Prostate treatment planning system (TPS). Data for the series of patients were exported from the TPS in Dicom format, and a series of parametrisation methods were developed in a Matlab environment to assess the rectal dose. Results: Contours of the anterior rectal mucosa were voxelised within Matlab to allow the dose to the rectal mucosa to be analysed directly from the 3D dose grid. Dose parametrisations based on dose-surface (DSH) and dose-line (DLH) histograms were obtained. Both lateral and longitudinal extents of the mucosal dose were parametrised using dose-line histograms in the relevant directions. Conclusion: We have developed a series of dose parametrisations for quantifying the dose to the rectal mucosa during HDR prostate brachytherapy which are suitable for future studies investigating potential associations between mucosal dose and late toxicity effects. The geometry of the transrectal probe standardises the rectal anatomy, making this treatment technique particularly suited to studies of this nature.

  9. Parametrisation of the variety of human behaviour related to building energy consumption in the Town Energy Balance (SURFEX-TEB v. 8.2

    Directory of Open Access Journals (Sweden)

    R. Schoetter

    2017-07-01

    Full Text Available The anthropogenic heat flux can be an important part of the urban surface energy balance. Some of it is due to energy consumption inside buildings, which depends on building use and human behaviour, both of which are very heterogeneous in most urban areas. Urban canopy parametrisations (UCP, such as the Town Energy Balance (TEB, parametrise the effect of the buildings on the urban surface energy balance. They contain a simple building energy model. However, the variety of building use and human behaviour at grid point scale has not yet been represented in state of the art UCPs. In this study, we describe how we enhance the Town Energy Balance in order to take fractional building use and human behaviour into account. We describe how we parametrise different behaviours and initialise the model for applications in France. We evaluate the spatio-temporal variability of the simulated building energy consumption for the city of Toulouse. We show that a more detailed description of building use and human behaviour enhances the simulation results. The model developments lay the groundwork for simulations of coupled urban climate and building energy consumption which are relevant for both the urban climate and the climate change mitigation and adaptation communities.

  10. Molecular Interactions with Many-Body Perturbation Theory.

    Science.gov (United States)

    1981-09-11

    so-called coupled correlation, more than doubline the CHF result. Similariy,. he perturbed Hartree-Fock ( CPHF ) result [66, 671. The additional...a in mtis example. It is well known approach, one would have to distinguish between the CPHF that the single-excitation contributions to properties...Karplus. CHF (or CPHF ) sum certain categories t" evaluated, at several small (’mite-field strengths, from which single anddouble-excitation diagrams i the

  11. Equation of state of dense nuclear matter and neutron star structure from nuclear chiral interactions

    Science.gov (United States)

    Bombaci, Ignazio; Logoteta, Domenico

    2018-02-01

    Aims: We report a new microscopic equation of state (EOS) of dense symmetric nuclear matter, pure neutron matter, and asymmetric and β-stable nuclear matter at zero temperature using recent realistic two-body and three-body nuclear interactions derived in the framework of chiral perturbation theory (ChPT) and including the Δ(1232) isobar intermediate state. This EOS is provided in tabular form and in parametrized form ready for use in numerical general relativity simulations of binary neutron star merging. Here we use our new EOS for β-stable nuclear matter to compute various structural properties of non-rotating neutron stars. Methods: The EOS is derived using the Brueckner-Bethe-Goldstone quantum many-body theory in the Brueckner-Hartree-Fock approximation. Neutron star properties are next computed solving numerically the Tolman-Oppenheimer-Volkov structure equations. Results: Our EOS models are able to reproduce the empirical saturation point of symmetric nuclear matter, the symmetry energy Esym, and its slope parameter L at the empirical saturation density n0. In addition, our EOS models are compatible with experimental data from collisions between heavy nuclei at energies ranging from a few tens of MeV up to several hundreds of MeV per nucleon. These experiments provide a selective test for constraining the nuclear EOS up to 4n0. Our EOS models are consistent with present measured neutron star masses and particularly with the mass M = 2.01 ± 0.04 M⊙ of the neutron stars in PSR J0348+0432.

  12. Sensitivity of the WRF-Chem (V3.6.1) model to different dust emission parametrisation: assessment in the broader Mediterranean region

    Science.gov (United States)

    Flaounas, Emmanouil; Kotroni, Vassiliki; Lagouvardos, Konstantinos; Klose, Martina; Flamant, Cyrille; Giannaros, Theodore M.

    2017-08-01

    In this study we aim to assess the WRF-Chem model capacity to reproduce dust transport over the eastern Mediterranean. For this reason, we compare the model aerosol optical depth (AOD) outputs to observations, focusing on three key regions: North Africa, the Arabian Peninsula and the eastern Mediterranean. Three sets of four simulations have been performed for the 6-month period of spring and summer 2011. Each simulation set uses a different dust emission parametrisation and for each parametrisation, the dust emissions are multiplied with various coefficients in order to tune the model performance. Our assessment approach is performed across different spatial and temporal scales using AOD observations from satellites and ground-based stations, as well as from airborne measurements of aerosol extinction coefficients over the Sahara. Assessment over the entire domain and simulation period shows that the model presents temporal and spatial variability similar to observed AODs, regardless of the applied dust emission parametrisation. On the other hand, when focusing on specific regions, the model skill varies significantly. Tuning the model performance by applying a coefficient to dust emissions may reduce the model AOD bias over a region, but may increase it in other regions. In particular, the model was shown to realistically reproduce the major dust transport events over the eastern Mediterranean, but failed to capture the regional background AOD. Further comparison of the model simulations to airborne measurements of vertical profiles of extinction coefficients over North Africa suggests that the model realistically reproduces the total atmospheric column AOD. Finally, we discuss the model results in two sensitivity tests, where we included finer dust particles (less than 1 µm) and changed accordingly the dust bins' mass fraction.

  13. Homogeneous Ni catalysts for H2 Oxidation and Production: An Assessment of Theoretical Methods, from Density Functional Theory to Post Hartree-Fock Correlated Wave-Function Theory

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Shentan; Raugei, Simone; Rousseau, Roger J.; Dupuis, Michel; Bullock, R. Morris

    2010-12-09

    A systematic assessment of theoretical methods applicable to the accurate characterization of catalytic cycles of homogeneous catalysts for H2 oxidation and evolution is reported. For these catalysts, H2 bond breaking or formation involve di-hydrogen, di-hydride, hydride-proton, and di-proton complexes. The key elementary steps have heterolytic character. In the context of Density Functional Theory (DFT) we investigated the use of functionals in the generalized gradient approximation (GGA) as well as hybrid functionals. We compared the results with wavefunction theories based on perturbation theory (MP2 and MP4) and on coupled-cluster expansions (CCSD and CCSD(T)). Our findings suggest that DFT results based on Perdew functionals are in semi-quantitative agreement with the CCSD(T) results, with deviations of a few kcal/mol only. On the other hand, the B3LYP functional is not even in qualitative agreement with CCSD[T]. Surprisingly the MP2 results are found to be extremely poor, a finding that we attribute to the limited treatment in MP2 theory of dynamic electron correlation effects in Ni(0) oxidation state. This material is based upon work supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences.

  14. Nuclear structure with unitarily transformed two-body plus phenomenological three-body interactions

    Energy Technology Data Exchange (ETDEWEB)

    Guenther, Anneke

    2011-02-02

    The importance of three-nucleon forces for a variety of nuclear structure phenomena is apparent in various investigations. This thesis provides a first step towards the inclusion of realistic three-nucleon forces by studying simple phenomenological threebody interactions. The Unitary Correlation Operator Method (UCOM) and the Similarity Renormalization Group (SRG) provide two different approaches to derive soft phase-shift equivalent nucleon-nucleon (NN) interactions via unitary transformations. Although their motivations are quite different the NN interactions obtained with the two methods exhibit some similarities. The application of the UCOM- or SRG-transformed Argonne V18 potential in the Hartree-Fock (HF) approximation and including the second-order energy corrections emerging from many-body perturbation theory (MBPT) reveals that the systematics of experimental ground-state energies can be reproduced by some of the interactions considering a series of closed-shell nuclei across the whole nuclear chart. However, charge radii are systematically underestimated, especially for intermediate and heavy nuclei. This discrepancy to experimental data is expected to result from neglected three-nucleon interactions. As first ansatz for a three-nucleon force, we consider a finite-range three-body interaction of Gaussian shape. Its influence on ground-state energies and charge radii is discussed in detail on the basis of HF plus MBPT calculations and shows a significant improvement in the description of experimental data. As the handling of the Gaussian three-body interaction is time-extensive, we show that it can be replaced by a regularized three-body contact interaction exhibiting a very similar behavior. An extensive study characterizes its properties in detail and confirms the improvements with respect to nuclear properties. To take into account information of an exact numerical solution of the nuclear eigenvalue problem, the No-Core Shell Model is applied to

  15. MN15-L and MN-15: New Kohn-Sham Density Functionals with Board Accuracy for Main-Group and Transition Metal Chemistry and Noncovalent Interactions

    Science.gov (United States)

    Yu, Haoyu; He, Xiao; Truhlar, Donald G.; Donald G. Truhlar Team

    The accuracy of Kohn-Sham density functional theory depends on the exchange-correlation functional. Local functionals depending on only the density (ρ) , density gradient (grad), and possibly kinetic energy density (τ) have been popular because of their low cost and simplicity, but the most successful functionals for chemistry have involved nonlocal Hartree-Fock exchange (hybrid functionals). We have designed a new meta gradient approximation called MN15-L and a new hybrid meta gradient approximation called MN15 and tested them systematically for 17 absolute atomic energies, 51 noncovalent interaction energies, 56 data on transition metal atoms and molecules, and for 298 other atomic and molecular energetic data, including main-group and transition metal bond energies, ionization potentials, proton affinities, reaction barrier heights, hydrocarbon thermochemistry, excitation energies, and isomerization energies. When compared with 84 previous density MN15 and MN15-L give respectively the smallest and second smallest mean unsigned errors (MUEs, in kcal/mol) on all 422 data with errors for the 4 subsets above being: MN15: 6, 0.26, 4.4, 1.6; MN15-L: 7, 0.45, 4.3, 2.0. Third best: M06: 4, 0.35, 7.7, 2.2. Best previous local functional: M06-L: 7, 0.42, 6.0, 3.5. Other popular functionals: B3LYP: 18, 0.82, 8.2, 4.3; HSE06: 33, 0.58, 8.8, 3.6; TPSS: 18, 0.89, 7.25, 5.0; PBE, 47, 0.88, 9.1, 6.0. MN15-L also performs well for solid-state cohesive energies. This research is supported by the U.S. Department of Energy and inorganic catalyst design center from university of Minnesota.

  16. Microscopic evaluation of the nuclear dipole polarizability

    Energy Technology Data Exchange (ETDEWEB)

    Lipparini, E.; Orlandini, G.; Stringari, S.; Traini, M. (Trento Univ. (Italy). Dept. di Matematica e Fisica)

    1977-12-01

    The dipole polarizability sum rule has been evaluated by means of a restricted Hartree-Fock approach. The method leads to a simple and analytical expression for the dipole polarizability. Explicit calculations have been performed in /sup 16/O and /sup 40/Ca with different types of interaction.

  17. Structure of high spin states of 76Kr and 78Kr nuclei

    Indian Academy of Sciences (India)

    Following a fully self-consistent cranked Hartree-Fock-Bogoliubov (CHFB) approach with a pairing+quadrupole+hexadecapole model interaction Hamiltonian the structure of the yrast states of 76,78Kr nuclei is studied up to angular momentum = 24. Evolution of the shape with spin, and rotation alignment of proton as well ...

  18. A generalised model and calculation of the hyperfine interaction constant for anomalous muonium in the crystalline lattice of silicon

    Science.gov (United States)

    Myakenkaya, G. S.; Gutsev, G. L.; Samoylov, V. M.

    1991-02-01

    A new microscopic model of anomalous muonium for the elemental semiconductors is proposed. The relevant configuration consisting of both a diamagrentic molecule Si-Mu and an unpaired orbital e- is contained into a semivacancy of the real lattice. By using the unrestricted Hartree-Fock computational method the principal properties of the system are established. A dynamical version of the model together with a question on the formation of such system are discussed.

  19. Weak interactions in Graphane/BN systems under static electric fields—A periodic ab-initio study

    Energy Technology Data Exchange (ETDEWEB)

    Steinkasserer, Lukas Eugen Marsoner, E-mail: marsoner@zedat.fu-berlin.de [Institut für Chemie und Biochemie, Freie Universität Berlin, Takustraße 3, 14195 Berlin (Germany); MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Chemical and Physical Sciences, Victoria University of Wellington, P.O. Box 600, 6140 Wellington (New Zealand); Gaston, Nicola [MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Chemical and Physical Sciences, Victoria University of Wellington, P.O. Box 600, 6140 Wellington (New Zealand); Paulus, Beate [Institut für Chemie und Biochemie, Freie Universität Berlin, Takustraße 3, 14195 Berlin (Germany)

    2015-04-21

    Ab-initio calculations via periodic Hartree-Fock (HF) and local second-order Møller-Plesset perturbation theory (LMP2) are used to investigate the adsorption properties of combined Graphane/boron nitride systems and their response to static electric fields. It is shown how the latter can be used to alter both structural as well as electronic properties of these systems.

  20. 2-D reconstruction of atmospheric concentration peaks from horizontal long path DOAS tomographic measurements: parametrisation and geometry within a discrete approach

    Directory of Open Access Journals (Sweden)

    A. Hartl

    2006-01-01

    Full Text Available In this study, we theoretically investigate the reconstruction of 2-D cross sections through Gaussian concentration distributions, e.g. emission plumes, from long path DOAS measurements along a limited number of light paths. This is done systematically with respect to the extension of the up to four peaks and for six different measurement setups with 2-4 telescopes and 36 light paths each. We distinguish between cases with and without additional background concentrations. Our approach parametrises the unknown distribution by local piecewise constant or linear functions on a regular grid and solves the resulting discrete, linear system by a least squares minimum norm principle. We show that the linear parametrisation not only allows better representation of the distributions in terms of discretisation errors, but also better inversion of the system. We calculate area integrals of the concentration field (i.e. total emissions rates for non-vanishing perpendicular wind speed components and show that reconstruction errors and reconstructed area integrals within the peaks for narrow distributions crucially depend on the resolution of the reconstruction grid. A recently suggested grid translation method for the piecewise constant basis functions, combining reconstructions from several shifted grids, is modified for the linear basis functions and proven to reduce overall reconstruction errors, but not the uncertainty of concentration integrals. We suggest a procedure to subtract additional background concentration fields before inversion. We find large differences in reconstruction quality between the geometries and conclude that, in general, for a constant number of light paths increasing the number of telescopes leads to better reconstruction results. It appears that geometries that give better results for negligible measurement errors and parts of the geometry that are better resolved are also less sensitive to increasing measurement errors.

  1. Self-consistent description of the SHFB equations for 112Sn

    Science.gov (United States)

    Ghafouri, M.; Sadeghi, H.; Torkiha, M.

    2018-03-01

    The Hartree-Fock (HF) method is an excellent approximation of the closed shell magic nuclei. Pair correlation is essential for the description of open shell nuclei and has been derived for even-even, odd-odd and even-odd nuclei. These effects are reported by Hartree-Fock with BCS (HFBCS) or Hartree-Fock-Bogolyubov (HFB). These issues have been investigated, especially in the nuclear charts, and such studies have been compared with the observed information. We compute observations such as total binding energy, charge radius, densities, separation energies, pairing gaps and potential energy surfaces for neutrons and protons, and compare them with experimental data and the result of the spherical codes. In spherical even-even neutron-rich nuclei are considered in the Skyrme-Hartree-Fock-Bogolyubov (SHFB) method with density-dependent pairing interaction. Zero-range density-dependent interactions is used in the pairing channel. We solve SHF or SHFB equations in the spatial coordinates with spherical symmetry for tin isotopes such as 112Sn. The numerical accuracy of solving equations in the coordinate space is much greater than the fundamental extensions, which yields almost precise results.

  2. Consistent structures and interactions by density functional theory with small atomic orbital basis sets

    Science.gov (United States)

    Grimme, Stefan; Brandenburg, Jan Gerit; Bannwarth, Christoph; Hansen, Andreas

    2015-08-01

    A density functional theory (DFT) based composite electronic structure approach is proposed to efficiently compute structures and interaction energies in large chemical systems. It is based on the well-known and numerically robust Perdew-Burke-Ernzerhoff (PBE) generalized-gradient-approximation in a modified global hybrid functional with a relatively large amount of non-local Fock-exchange. The orbitals are expanded in Ahlrichs-type valence-double zeta atomic orbital (AO) Gaussian basis sets, which are available for many elements. In order to correct for the basis set superposition error (BSSE) and to account for the important long-range London dispersion effects, our well-established atom-pairwise potentials are used. In the design of the new method, particular attention has been paid to an accurate description of structural parameters in various covalent and non-covalent bonding situations as well as in periodic systems. Together with the recently proposed three-fold corrected (3c) Hartree-Fock method, the new composite scheme (termed PBEh-3c) represents the next member in a hierarchy of "low-cost" electronic structure approaches. They are mainly free of BSSE and account for most interactions in a physically sound and asymptotically correct manner. PBEh-3c yields good results for thermochemical properties in the huge GMTKN30 energy database. Furthermore, the method shows excellent performance for non-covalent interaction energies in small and large complexes. For evaluating its performance on equilibrium structures, a new compilation of standard test sets is suggested. These consist of small (light) molecules, partially flexible, medium-sized organic molecules, molecules comprising heavy main group elements, larger systems with long bonds, 3d-transition metal systems, non-covalently bound complexes (S22 and S66×8 sets), and peptide conformations. For these sets, overall deviations from accurate reference data are smaller than for various other tested DFT methods

  3. General aspects of the nucleon-nucleon interaction and nuclear matter properties

    Energy Technology Data Exchange (ETDEWEB)

    Plohl, Oliver

    2008-07-25

    The subject of the present thesis is at first the investigation of model independent properties of the nucleon-nucleon (NN) interaction in the vacuum concerning the relativistic structure and the implications for nuclear matter properties. Relativistic and non-relativistic meson-exchange potentials, phenomenological potentials s well as potentials based on effective field theory (EFT) are therefore mapped on a relativistic operator basis given by the Clifford Algebra. This allows to compare the various approaches at the level of covariant amplitudes where a remarkable agreement is found. Furthermore, the relativistic self-energy is determined in the Hartree-Fock (HF) approximation. The appearance of a scalar and vector field of several hundred MeV magnitude is a general feature of relativistic descriptions of nuclear matter. Within QCD sum rules these fields arise due to the density dependence of chiral condensates. We find that independent of the applied NN interaction large scalar and vector fields are generated when the symmetries of the Lorentz group are restored. In the framework of chiral EFT (chEFT) it is shown, that these fields are generated by short-range next-to-leading order (NLO) contact terms, which are connected to the spin-orbit interaction. To estimate the effect arising from NN correlations the equation of state of nuclear and neutron matter is calculated in the Brueckner-HF (BHF) approximation applying chEFT. Although, as expected, a clear over-binding is found (at NLO a saturating behavior is observed), the symmetry energy shows realistic properties when compared to phenomenological potentials (within the same approximation) and other approaches. The investigation of the pion mass dependence within chEFT at NLO shows that the magnitude of the scalar and vector fields persists in the chiral limit - nuclear matter is still bound. In contrast to the case of a pion mass larger than the physical one the binding energy and saturation density are

  4. Time dependent density matrix theory and effective interaction

    Energy Technology Data Exchange (ETDEWEB)

    Tohyama, Mitsuru [Kyorin Univ., Mitaka, Tokyo (Japan). School of Medicine

    1998-07-01

    A correlated ground state of {sup 16}O and an E2 giant resonance built on it are calculated using an extended version of the time-dependent Hartree-Fock theory called the time-dependent density-matrix theory (TDDM). The Skyrme force is used in the calculation of both a mean field and two-body correlations. It is found that TDDM gives reasonable ground-state correlations and a large spreading width of the E2 giant resonance when single-particle states in the continuum are treated appropriately. (author)

  5. Aurophilic Interactions from Wave Function, Symmetry-Adapted Perturbation Theory, and Rangehybrid Approaches.

    Science.gov (United States)

    Liu, Ru-Fen; Franzese, Christina A; Malek, Ryan; Żuchowski, Piotr S; Ángyán, János G; Szczȩśniak, Małgorzata M; Chałasiński, Grzegorz

    2011-08-09

    The aurophilic interaction is examined in three model systems Au2((3)Σg(+)), (AuH)2, and (HAuPH3)2 which contain interactions of pairs of the Au centers in the oxidation state (I). Several methods are employed ranging from wave function theory-based (WFT) approaches to symmetry-adapted perturbation theory (SAPT) and range-separated hybrid (RSH) density functional theory (DFT) methods. The most promising and accurate approach consists of a combination of the DFT and WFT approaches in the RSH framework. In this combination the short-range DFT handles the slow convergence of the correlation cusp, whereas the long-range WFT is best suited for the long-range correlation. Of the three tested RSH DFT methods, the one which uses a short-range exchange functional based on the Ernzerhof-Perdew exchange hole model with a range-separation parameter of 0.4 bohr(-1) seems to be the best candidate for treatment of gold. In combination with the long-range coupled cluster singles, doubles, and noniterative triples [CCSD(T)] treatment it places the strength of aurophilic bonding in (HAuPH3)2 at 5.7 kcal/mol at R = 3.09 Å. This value is somewhat larger than our best purely WFT result based on CCSD(T), 4.95 kcal/mol (R = 3.1 Å), and considerably smaller than the Hartree-Fock+dispersion value of 7.4 kcal/mol (R = 2.9 Å). The 5.7 kcal/mol estimate fits reasonably well within the prediction of the empirical relationship proposed by Schwerdtfeger et al. (J. Am. Chem. Soc.1998, 120, 6587). A direct computation of dispersion energy, including exchange corrections, results in values of ca. -9 kcal/mol for Au2((3)Σg(+)) and (AuH)2 and -13 kcal/mol for (HAuPH3)2 at the distance of a typical aurophilic bond, R = 3.0 Å.

  6. Explicit representation and parametrised impacts of under ice shelf seas in the z∗ coordinate ocean model NEMO 3.6

    Directory of Open Access Journals (Sweden)

    P. Mathiot

    2017-07-01

    Full Text Available Ice-shelf–ocean interactions are a major source of freshwater on the Antarctic continental shelf and have a strong impact on ocean properties, ocean circulation and sea ice. However, climate models based on the ocean–sea ice model NEMO (Nucleus for European Modelling of the Ocean currently do not include these interactions in any detail. The capability of explicitly simulating the circulation beneath ice shelves is introduced in the non-linear free surface model NEMO. Its implementation into the NEMO framework and its assessment in an idealised and realistic circum-Antarctic configuration is described in this study. Compared with the current prescription of ice shelf melting (i.e. at the surface, inclusion of open sub-ice-shelf cavities leads to a decrease in sea ice thickness along the coast, a weakening of the ocean stratification on the shelf, a decrease in salinity of high-salinity shelf water on the Ross and Weddell sea shelves and an increase in the strength of the gyres that circulate within the over-deepened basins on the West Antarctic continental shelf. Mimicking the overturning circulation under the ice shelves by introducing a prescribed meltwater flux over the depth range of the ice shelf base, rather than at the surface, is also assessed. It yields similar improvements in the simulated ocean properties and circulation over the Antarctic continental shelf to those from the explicit ice shelf cavity representation. With the ice shelf cavities opened, the widely used three equation ice shelf melting formulation, which enables an interactive computation of melting, is tested. Comparison with observational estimates of ice shelf melting indicates realistic results for most ice shelves. However, melting rates for the Amery, Getz and George VI ice shelves are considerably overestimated.

  7. A combined DFT and restricted open-shell configuration interaction method including spin-orbit coupling: application to transition metal L-edge X-ray absorption spectroscopy.

    Science.gov (United States)

    Roemelt, Michael; Maganas, Dimitrios; DeBeer, Serena; Neese, Frank

    2013-05-28

    A novel restricted-open-shell configuration interaction with singles (ROCIS) approach for the calculation of transition metal L-edge X-ray absorption spectra is introduced. In this method, one first calculates the ground state and a number of excited states of the non-relativistic Hamiltonian. By construction, the total spin is a good quantum number in each of these states. For a ground state with total spin S excited states with spin S' = S, S - 1, and S + 1 are constructed. Using Wigner-Eckart algebra, all magnetic sublevels with MS = S,..., -S for each multiplet of spin S are obtained. The spin-orbit operator is represented by a mean-field approximation to the full Breit-Pauli spin-orbit operator and is diagonalized over this N-particle basis. This is equivalent to a quasi-degenerate treatment of the spin-orbit interaction to all orders. Importantly, the excitation space spans all of the molecular multiplets that arise from the atomic Russell-Saunders terms. Hence, the method represents a rigorous first-principles approach to the complicated low-symmetry molecular multiplet problem met in L-edge X-ray absorption spectroscopy. In order to gain computational efficiency, as well as additional accuracy, the excitation space is restricted to single excitations and the configuration interaction matrix is slightly parameterized in order to account for dynamic correlation effects in an average way. To this end, it is advantageous to employ Kohn-Sham rather than Hartree-Fock orbitals thus defining the density functional theory∕ROCIS method. However, the method can also be used in an entirely non-empirical fashion. Only three global empirical parameters are introduced and have been determined here for future application of the method to any system containing any transition metal. The three parameters were carefully calibrated using the L-edge X-ray absorption spectroscopy spectra of a test set of coordination complexes containing first row transition metals. These

  8. Correlation energy and dispersion interaction in the ab initio potential energy curve of the neon dimer.

    Science.gov (United States)

    Bytautas, Laimutis; Ruedenberg, Klaus

    2008-06-07

    A close approximation to the empirical potential energy curve of the neon dimer is obtained by coupled-cluster singles plus doubles plus noniterative triples calculations by using nonaugmented correlation-consistent basis sets without counterpoise corrections and complementing them by three-term extrapolations to the complete basis set limit. The potential energy is resolved into a self-consistent-field Hartree-Fock contribution and a correlation contribution. The latter is shown to decay in the long-range region in accordance with the empirical dispersion expansion.

  9. Surfaces parametrised by the normals

    DEFF Research Database (Denmark)

    Gravesen, Jens

    2007-01-01

    the origin to the tangent plane and the surface is simply considered as the envelope of its family of tangent planes. Suppose we are given points and normals and we want a C^k-surface interpolating these data. The data gives the value and gradients of the support function at certain points (the given normals...

  10. Probing the pairing interaction through two-neutron transfer reactions

    Directory of Open Access Journals (Sweden)

    Margueron J.

    2012-12-01

    Full Text Available The treatment of the pairing interaction in mean-field-based models is addressed. In particular, the possibility to use pair transfers as A tool to better constrain this interaction is discussed. First, pairing inter-actions with various density dependencies (surface/volume mixing are used in the microscopic Hartree-Fock-Bogoliubov + quasiparticle random-phase approximation model to generate the form factors to be used in reaction calculations. Cross sections for (p,t two-neutron transfer reactions are calculated in the one-step zero-range distorted-wave Born approximation for some Tin isotopes and for incident proton energies from 15 to 35 MeV. Three different surface/volume mixings of A zero-range density-dependent pairing interaction are employed in the microscopic calculations and the sensitivity of the cross sections to the different mixings is analyzed. Differences among the three different theoretical predictions are found espacially for the nucleus 136Sn and they are more important at the incident proton energy of 15 MeV. We thus indicate (p,t two-neutron transfer reactions with very neutron-rich Sn isotopes and at proton energies around 15 MeV as good experimental cases where the surface/volume mixing of the pairing interaction may be probed. In the second part of the manuscript, ground-state to ground-state transitions are investigated. Approximations made to estimate two-nucleon transfer probabilities in ground-state to ground-state transitions and the physical interpretation of these probabilities are discussed. Probabilities are often calculated by approximating both ground states of the initial nucleus A and of the final nucleus A±2 by the same quasiparticle vacuum. We analyze two improvements of this approach. First, the effect of using two different ground states with average numbers of particles A and A±2 is quantified. Second, by using projection techniques, the role of particle number restoration is analyzed. Our analysis

  11. Three-dimensional TDHF calculation for reactions of unstable nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Ka-Hae; Otsuka, Takaharu [Tokyo Univ. (Japan). Dept. of Physics; Bonche, P.

    1998-07-01

    The fusion is studied for reactions between a stable and an unstable nuclei with neutron skin. The reactions {sup 16,28}O+{sup 40}Ca and {sup 16}O+{sup 16,28}O are taken as examples, and the three-dimensional time-dependent Hartree-Fock method with the full Skyrme interaction is used. It is confirmed that the fusion cross section in low-energy region is sensitive to the interaction used in the calculation. (author)

  12. The Importance of Three-Body Interactions in Molecular Dynamics Simulations of Water with the Fragment Molecular Orbital Method

    Energy Technology Data Exchange (ETDEWEB)

    Pruitt, Spencer R.; Nakata, Hiroya; Nagata, Takeshi; Mayes, Maricris; Alexeev, Yuri; Fletcher, Graham D.; Fedorov, Dmitri G; Kitaura, Kazuo; Gordon, M

    2016-04-12

    The analytic first derivative with respect to nuclear coordinates is formulated and implemented in the framework of the three-body fragment molecular orbital (FMO) method. The gradient has been derived and implemented for restricted Hartree-Fock, second-order Møller-Plesset perturbation, and density functional theories. The importance of the three-body fully analytic gradient is illustrated through the failure of the two-body FMO method during molecular dynamics simulations of a small water cluster. The parallel implementation of the fragment molecular orbital method, its parallel efficiency, and its scalability on the Blue Gene/Q architecture up to 262,144 CPU cores, are also discussed.

  13. Variational approach to the moment of inertia

    Energy Technology Data Exchange (ETDEWEB)

    Stringari, S.; Lipparini, E.

    1980-08-01

    We derive an approximate expression for the moment of inertia theta in the framework of the cranked Hartree-Fock theory. Our method allows for a detailed study of the role of spin-orbit and two-body nuclear potentials. In particular it is shown that in /sup 20/Ne the two-body interaction lowers by 30% the rigid value of theta. The irrotational and rigid values for the moment of inertia are obtained as special cases of the present approach.

  14. Description of magic nuclei properties in quasi-particle Lagrangian approach

    Energy Technology Data Exchange (ETDEWEB)

    Sapershtejn, Eh.E.; Khodel' , V.A.

    1983-10-01

    The quasi-particle Lagrangian method is applied to calculate characteristics of magic nuclei. It is shown that an account for the energy dependence of the effective nucleon interaction is essential for a simultaneous description of masses and radii of atomic nuclei and their single-particle spectra. The approach presented here incorporates the effects of the energy dependence naturally so one gets a better description of the totality of phenomena, than that provided by the Hartree-Fock method with effective forces.

  15. Description of the properties of magic nuclei in the quasiparticle Lagrangian approach

    Energy Technology Data Exchange (ETDEWEB)

    Sapershtein, E.; Khodel' , V.A.

    1983-10-01

    The quasiparticle Lagrangian method is used to calculate the characteristics of magic nuclei. It is shown that allowance for the effects of the energy dependence of the effective internucleon interaction is important for the simultaneous description of the masses, radii, and single-particle spectra of nuclei. The proposed approach incorporates these effects in a natural way, and thus provides a better description of the entire set of phenomena than the Hartree--Fock method with effective forces.

  16. The Noble Gas Dimers as a Probe of the Energetic Contributions of Dispersion and Short-Range Electron Correlation in Weakly-Bound Systems

    OpenAIRE

    Housden, Michael Philip; Pyper, Nicholas Charles

    2008-01-01

    Abstract The binding of the noble gas dimers is examined using a theory in which the Hartree-Fock interaction energy is augmented with both a short-range correlation term derived from the theory of a uniform electron-gas plus a dispersion energy damped according to the theory of Jabobi and Csanak. The good agreement between the predicted and experimental binding energies and equilibrium inter-nuclear separations confirms that this approach captures the essential physics of the int...

  17. Stretching and breaking of chemical bonds, correlation of electrons, and radical properties of covalent species

    OpenAIRE

    Sheka, Elena

    2014-01-01

    Chemical bonds are considered in light of correlation of valence electrons that is strengthened when the bond is dissociated. In the framework of the unrestricted Hartree-Fock single-reference version of the configuration interaction theory, effectively unpaired electrons lay the foundation of the electron correlation measure in terms of total number of the electrons (molecular chemical susceptibility). graphs and their singularities with respect to the interatomic distance allow presenting a...

  18. Calculation of the spectrum of the superheavy element Z=120

    OpenAIRE

    Dinh, T. H.; Dzuba, V. A.; Flambaum, V. V.; Ginges, J. S. M.

    2008-01-01

    High-precision calculations of the energy levels of the superheavy element Z=120 are presented. The relativistic Hartree-Fock and configuration interaction techniques are employed. The correlations between core and valence electrons are treated by means of the correlation potential method and many-body perturbation theory. Similar calculations for barium and radium are used to gauge the accuracy of the calculations and to improve the ab initio results.

  19. Benchmarking GW against exact diagonalization for semiempirical models

    DEFF Research Database (Denmark)

    Kaasbjerg, Kristen; Thygesen, Kristian Sommer

    2010-01-01

    captures around 65% of the ground-state correlation energy. The lowest lying excitations are overscreened by GW leading to an underestimation of electron affinities and ionization potentials by 0.15 eV on average corresponding to ∼3%. One-shot G0W0 calculations starting from Hartree-Fock reduce...... the screening and improve the low-lying excitation energies. The effect of the GW self-energy on the molecular excitation energies is shown to be similar to the inclusion of final-state relaxations in Hartree-Fock theory. We discuss the breakdown of the GW approximation in systems with short-range interactions...... (Hubbard models) where correlation effects dominate over screening/relaxation effects. Finally we illustrate the important role of the derivative discontinuity of the true exchange-correlation functional by computing the exact Kohn-Sham levels of benzene....

  20. Scattering resonances in a degenerate Fermi gas

    DEFF Research Database (Denmark)

    Challis, Katharine; Nygaard, Nicolai; Mølmer, Klaus

    2009-01-01

    We consider elastic single-particle scattering from a one-dimensional trapped two-component superfluid Fermi gas when the incoming projectile particle is identical to one of the confined species. Our theoretical treatment is based on the Hartree-Fock ground state of the trapped gas and a configur......We consider elastic single-particle scattering from a one-dimensional trapped two-component superfluid Fermi gas when the incoming projectile particle is identical to one of the confined species. Our theoretical treatment is based on the Hartree-Fock ground state of the trapped gas...... and a configuration-interaction description of the excitations. We determine the scattering phase shifts for the system and predict Fano-type scattering resonances that are a direct consequence of interatomic pairing. We describe the main characteristics of the scattering resonances and make a comparison...

  1. The nature of electron correlation in a dissociating bond

    Science.gov (United States)

    Hollett, Joshua W.; McKemmish, Laura K.; Gill, Peter M. W.

    2011-06-01

    We have constructed the unrestricted Hartree-Fock (UHF), restricted Hartree-Fock (RHF), and full configuration interaction (FCI) position and momentum intracules and holes for HṡṡṡH at bond lengths R from 1 to 10 bohrs. We trace the recently discovered inversion of the UHF position hole at intermediate R to over-localization of the spin-orbitals, and support this by a correlation energy component analysis. The RHF and UHF momentum holes are found to be more complicated; however their features are explained through decomposition of electron correlation effects. The UHF momentum hole is also found to invert and exhibits interesting behavior at large R. The RHF (but not UHF) and FCI momentum intracules exhibit Young-type interference patterns related to recent double photoionization experiments. Our analyses yield the most comprehensive picture to date of the behavior of the electrons during homolytic bond fission.

  2. Extended Thomas-Fermi approximation to the one-body density matrix

    Energy Technology Data Exchange (ETDEWEB)

    Soubbotin, V.B.; Vinas, X

    2000-02-28

    The one-body density matrix is derived within the Extended Thomas-Fermi approximation. This has been done starting from the Wigner-Kirkwood distribution function for a non-local single-particle potential. The links between this new approximation to the density matrix with former approaches available in the literature are widely discussed. The semiclassical counterpart of the Hartree-Fock energy at the Extended Thomas-Fermi level is also obtained in the case of a non-local one-body Hamiltonian. The semiclassical binding energies and root mean square radii are compared with those obtained using the Strutinsky averaged method. The full Hartree-Fock values are compared with those obtained using the Kohn-Sham scheme based on the different approximations to the density matrix considered in the text. Numerical applications are performed using the Gogny, Brink-Boeker and BDM3Y1{sup *} effective interactions.

  3. On the treatment of the center of mass motion in nuclear mean field theories

    Science.gov (United States)

    Schmid, K. W.; Grümmer, F.

    1990-03-01

    It is shown how the spurious components due to the center of mass motion can be eliminated from general Hartree-Fock-Bogoliubov quasi-particle configurations with the help of projection techniques. The problem how to restore the additional symmetries being broken by such configurations is discussed. An explicit formulation is given for the spherical Hartree-Fock problem with center of mass momentum projection before the variation. As an example for the application of this method the ground state of4He is studied using two different interactions, a microscopic two-body one as well as a phenomenological one including a Skyrme-type three-body force. The results are compared to those of the usual approximate treatment of the center of mass motion in Hartree-Fock calculations. It turns out that, at least for the chosen example, the latter yields a rather reasonable approximation to the correct total energy, single particle energy and even the mass density provided that it is calculated from a translationally invariant density operator.

  4. Tables Of Gaussian-Type Orbital Basis Functions

    Science.gov (United States)

    Partridge, Harry

    1992-01-01

    NASA technical memorandum contains tables of estimated Hartree-Fock wave functions for atoms lithium through neon and potassium through krypton. Sets contain optimized Gaussian-type orbital exponents and coefficients, and near Hartree-Fock quality. Orbital exponents optimized by minimizing restricted Hartree-Fock energy via scaled Newton-Raphson scheme in which Hessian evaluated numerically by use of analytically determined gradients.

  5. Shell evolution above Z ,N =50 within Skyrme density functional theory: The impact of deformation and tensor interactions

    Science.gov (United States)

    Shi, Yue

    2017-03-01

    Background: Recent years have seen considerable effort in associating the shell evolution (SE) for a chain of isotones or isotopes with the underlying nuclear interactions. In particular, it has been fairly well established that the tensor part of the Skyrme interaction is indispensable for understanding certain SE above Z ,N =50 shell closures, as a function of nucleon numbers. Purpose: The purpose of the present work is twofold: (1) to study the effect of deformation due to blocking on the SE above Z ,N =50 shell closures and (2) to examine the optimal parametrizations in the tensor part which gives a proper description of the SE above Z ,N =50 shell closures. Methods: I use the Skyrme-Hartree-Fock-Bogoliubov (SHFB) method to compute the even-even vacua of the Z =50 isotopes and N =50 isotones. For Sb and odd-A Sn isotopes, I perform calculations with a blocking procedure which accounts for the polarization effects, including deformations. Results: The blocking SHFB calculations show that the light odd-A Sb isotopes, with only one valence proton occupying down-sloping Ω =11 /2- and Ω =7 /2+ Nilsson orbits, assume finite oblate deformations. This reduces the energy differences between 11 /2- and 7 /2+ states by about 500 keV for 51Sb56 -66 , bringing the energy-difference curve closer to the experimental one. With une2t1 energy density functional (EDF), which differs from unedf2 parametrization by tensor terms, a better description of the slope of Δ e (π 1 h11 /2-π 1 g7 /2) as a function of neutron number has been obtained. However, the trend of Δ e (π 1 g7 /2-π 2 d5 /2) curve is worse using une2t1 EDF. Δ e (ν 3 s1 /2-ν 2 d5 /2) and Δ e (ν 1 g7 /2-ν 2 d5 /2) curve for N =50 isotones using une2t1 seems to be consistent with experimental data. The neutron SE of Δ e (ν 1 h11 /2-ν 1 g7 /2) and Δ e (ν 1 g7 /2-ν 2 d5 /2) for Sn isotopes are shown to be sensive to αT tensor parameter. Conclusions: Within the Skyrme self-consistent mean-field model

  6. The interaction of excited atoms and few-cycle laser pulses

    CERN Document Server

    Calvert, J E; Palmer, A J; Glover, R D; Tong, X M; Dolmatov, V K; Kheifets, A S; Bartschat, K; Litvinyuk, I V; Kielpinski, D; Sang, R T

    2016-01-01

    This work describes the first observations of the ionisation of neon in a metastable atomic state utilising a strong-field, few-cycle light pulse. We compare the observations to theoretical predictions based on the Ammosov-Delone-Krainov (ADK) theory and a solution to the time-dependent Schrodinger equation (TDSE). The TDSE provides better agreement with the experimental data than the ADK theory. We optically pump the target atomic species and demonstrate that the ionisation rate depends on the spin state of the target atoms and provide physically transparent interpretation of such a spin dependence in the frameworks of the spin-polarised Hartree-Fock and random-phase approximations.

  7. Parametrisation of the optical thickness of a Rayleigh atmosphere, for the 290-385 nm band.; Parametrizacion del espesor optico de una atmosfera de rayleigh para la banda UVA 290-385 nm. Determinacion de un factor de turbiedad para dicha banda en Valencia

    Energy Technology Data Exchange (ETDEWEB)

    Serrano, M. A; Bosca, J. V.; Canada, J.

    2004-07-01

    Parametrisation of the optical thickness of a Rayleigh atmosphere, for the 290-385 nm band of the solar spectrum, were obtained in relation to the relative air mass. A TB so-called factor has been defined as the factor to be multiplied the optical thickness of a Rayleigh atmosphere to produce the same attenuation to normal beam irradiance of this band. Finally with 18754 experimental measurements of global horizontal 290-385 nm irradiance, in Valencia taken in half an hour intervals, in cloudless conditions from January 1996 to December 2000 in Valencia, values of TB, have been determined. (Author)

  8. INTERACT

    DEFF Research Database (Denmark)

    Jochum, Elizabeth; Borggreen, Gunhild; Murphey, TD

    interaction between a human operator and an artificial actor or agent. We can apply insights from puppetry to develop culturally-aware robots. Here we describe the development of a robotic marionette theatre wherein robotic controllers assume the role of human puppeteers. The system has been built, tested...... including puppetry and dance. However, the aesthetics of these traditions vary across cultures and carry different associative and interpretive meanings. Puppetry offers a useful frame for understanding the relationship between abstract and imitative gestures and behavior, and instantiates the complex...

  9. Baryonic forces and hyperons in nuclear matter from SU(3) chiral effective field theory

    Energy Technology Data Exchange (ETDEWEB)

    Petschauer, Stefan Karl

    2016-02-12

    In this work the baryon-baryon interaction is studied at next-to-leading order in SU(3) chiral effective field theory and applied to hyperon-nucleon scattering. The properties of hyperons in isospin-symmetric as well as asymmetric nuclear matter are calculated within the Bruecker-Hartree-Fock formalism. Moreover, the leading three-baryon interaction is derived and its low-energy constants are estimated from decuplet intermediate states. We conclude, that chiral effective field theory is a well-suited tool to describe the baryonic forces.

  10. Neutron star properties derived from relativistic mean field

    CERN Document Server

    Beták, E; Urbanec, M

    2010-01-01

    The equation of state of asymmetric nuclear matter given by the parameterized form of the relativistic Brueckner-Hartree-Fock mean field with vector cross interaction is applied to construct spherically symmetric neutron star models. The masses and radii of the models are given as functions of the central energy density and compared with astrophysical data. The calculated radii appear to be confined to a narrow band between 12 and 13 km, nearly independent of the calculated masses. Our models are in agreement with known data and the ones with vector cross interaction cope well with the recent limitations imposed by the double pulsar J0737-3039.

  11. Theoretical chemistry advances and perspectives

    CERN Document Server

    Eyring, Henry

    1977-01-01

    Theoretical Chemistry: Advances and Perspectives, Volume 2 covers all aspects of theoretical chemistry.This book reviews the techniques that have been proven successful in the study of interatomic potentials in order to describe the interactions between complex molecules. The ground state properties of the interacting electron gas when a magnetic field is present are also elaborated, followed by a discussion on the Gellman-Brueckner-Macke theory of the correlation energy that has applications in atomic and molecular systems.This volume considers the instability of the Hartree-Fock ground state

  12. Spin-dependent semiconductor Bloch equations: Microscopic theory of Bir-Aronov-Pikus spin relaxation

    Science.gov (United States)

    Lechner, C.; Rössler, U.

    2005-10-01

    Semiconductor Bloch equations, in their extension including the spin degree of freedom of the carriers, are capable to describe spin dynamics on a microscopic level. In the presence of free holes, electron spins can flip simultaneously with hole spins due to electron-hole exchange interaction. This mechanism named after Bir, Aronov, and Pikus is described here by using the extended semiconductor Bloch equations [Phys. Status Solidi B 234, 385 (2002)] and considering carrier-carrier interaction beyond the Hartree-Fock truncation. As a result we derive microscopic expressions for spin-relaxation and spin-dephasing rates.

  13. Orbital dependent functionals: An atom projector augmented wave method implementation

    Science.gov (United States)

    Xu, Xiao

    This thesis explores the formulation and numerical implementation of orbital dependent exchange-correlation functionals within electronic structure calculations. These orbital-dependent exchange-correlation functionals have recently received renewed attention as a means to improve the physical representation of electron interactions within electronic structure calculations. In particular, electron self-interaction terms can be avoided. In this thesis, an orbital-dependent functional is considered in the context of Hartree-Fock (HF) theory as well as the Optimized Effective Potential (OEP) method and the approximate OEP method developed by Krieger, Li, and Iafrate, known as the KLI approximation. In this thesis, the Fock exchange term is used as a simple well-defined example of an orbital-dependent functional. The Projected Augmented Wave (PAW) method developed by P. E. Blochl has proven to be accurate and efficient for electronic structure calculations for local and semi-local functions because of its accurate evaluation of interaction integrals by controlling multiple moments. We have extended the PAW method to treat orbital-dependent functionals in Hartree-Fock theory and the Optimized Effective Potential method, particularly in the KLI approximation. In the course of study we develop a frozen-core orbital approximation that accurately treats the core electron contributions for above three methods. The main part of the thesis focuses on the treatment of spherical atoms. We have investigated the behavior of PAW-Hartree Fock and PAW-KLI basis, projector, and pseudopotential functions for several elements throughout the periodic table. We have also extended the formalism to the treatment of solids in a plane wave basis and implemented PWPAW-KLI code, which will appear in future publications.

  14. Study of the Location of Implanted Fluorine Atoms in Silicon and Germanium through Their Nuclear Quadrupole Interactions

    Science.gov (United States)

    Nunes, Stacie S.; Sulaiman, S.; Sahoo, N.; Das, T. P.; Frank, M.; Kreische, W.; Nielsen, K. B.

    1996-06-01

    Time Differential Perturbed Angular Distribution (TDPAD) measurements of the nuclear quadrupole hyperfine parameters for 19F* implanted into amorphous, polycrystalline and crystalline silicon and germanium are reported and reviewed. Two signals are observed in the crystalline materials (≈ 35 and 23 MHz in silicon, ≈ 33 and 27 MHz in germanium) while only one is detected in the amorphous and polycrystalline samples (≈ 22 MHz in silicon, ≈ 27 in germanium). Impurity sites in these materials were modeled using a Hartree-Fock cluster procedure. The Intrabond, Antibond, and Substitutional sites in the bulk were studied in both silicon and germanium. The ATOP and Intrabond Surface sites were also studied in silicon and the results extended to germa-nium. Lattice relaxation effects were incorporated by employing a geometry optimization method to obtain minimum energy configurations for the clusters modelling each site. The electronic wave functions were obtained for each optimized cluster by applying Unresctricted Hartree-Fock theory, and these wave functions were used to calculate the nuclear quadrupole hyperfine parameters at the site of the fluorine nucleus. Comparison of the theoretical hyperfine parameters to the experimental values indicates that 19F* located in the Intrabond and Intrabond surface sites could readily explain the higher frequency signal that has been observed. 19F* in the Antibond and the surface ATOP sites yield hyperfine parameters consistent with the low frequency signal observed in the crystalline materials and the single signal observed in the amorphous (or polycrystalline) materials. Examina-tion of these two sites, in view of other available experimental evidence including the temperature dependence of the TDPAD signals, leads to the conclusion that the lower frequency signal is due to 19F* implants which have come to rest at the site of dangling bonds in the bulk. These dangling bonds are created as a result of damage generated in the

  15. Electronic Green's functions in a T-shaped multi-quantum dot system

    OpenAIRE

    Tifrea, I.; Pal, G.; Crisan, M.

    2011-01-01

    We developed a set of equations to calculate the electronic Green's functions in a T-shaped multi-quantum dot system using the equation of motion method. We model the system using a generalized Anderson Hamiltonian which accounts for {\\em finite} intradot on-site Coulomb interaction in all component dots as well as for the interdot electron tunneling between adjacent quantum dots. Our results are obtained within and beyond the Hartree-Fock approximation and provide a path to evaluate all the ...

  16. Radiative Decay Rates for Electric Dipole, Magnetic Dipole and Electric Quadrupole Transitions in Triply Ionized Thulium (Tm IV

    Directory of Open Access Journals (Sweden)

    Saturnin Enzonga Yoca

    2017-09-01

    Full Text Available A new set of radiative decay parameters (oscillator strengths, transition probabilities for spectral lines in triply ionized thulium (Tm IV has been obtained within the framework of the pseudo-relativistic Hartree-Fock (HFR approach. The effects of configuration interaction and core-polarization have been investigated in detail and the quality of the results has been assessed through a comparison between different HFR physical models. The spectroscopic data listed in the present paper cover electric dipole as well as magnetic dipole and electric quadrupole transitions in a wide range of wavelengths from extreme ultraviolet to near infrared.

  17. Ab-initio study of the electronic structure of sup 1 sup 9 F implanted in GaAs and GaN crystals

    CERN Document Server

    Park, J H; Cho, H S; Shin, Y N

    1998-01-01

    We have studied the nuclear quadrupole interaction of a fluorine atom implanted in gallium arsenide and gallium nitride cluster models using the ab-initio Hartree-Fock theory. For the three possible fluorine sites in GaAs and GaN, we have determined the location of the implanted fluorine atom by using a self-consistent calculation, the electric field gradient at the implanted atom, and the electronic structure. Good agreement is found with experimental data wherever they are available. Predictions are made for the implanted fluorine site associated with the total energy and the electric field gradient which are expected to be measurable by a variety of experimental techniques.

  18. Gamow shell-model description of weakly bound and unbound nuclear states

    Energy Technology Data Exchange (ETDEWEB)

    Michel, N.; Nazarewicz, W. [Department of Physics and Astronomy, University of Tennessee, Knoxville, Tennessee 37996 (United States); Ploszajczak, M.; Rotureau, J. [Grand Accelerateur National d' Ions Lourds (GANIL), CEA/DSM- NRS/IN2P3, BP 55027, F-14076 Caen Cedex 05 (France)

    2004-12-01

    Recently, the shell model in the complex k-plane (the so-called Gamow Shell Model) has been formulated using a complex Berggren ensemble representing bound single-particle states, single-particle resonances, and non-resonant continuum states. In this framework, we shall discuss binding energies and energy spectra of neutron-rich helium and lithium isotopes. The single-particle basis used is that of the Hartree-Fock potential generated self-consistently by the finite-range residual interaction. (Author) 21 refs., 5 tabs., 2 figs.

  19. Ab initio study on the formation of triiodide CT complex from the reaction of iodine with 2,3-diaminopyridine.

    Science.gov (United States)

    Al-Hashimi, Nessreen A; Hussein, Yasser H A

    2010-01-01

    The charge transfer (CT) interaction between iodine and 2,3-diaminopyridine (DAPY) has been thoroughly investigated via theoretical calculations. A Hartree-Fock, 3-21G level of theory was used to optimize and calculate the Mullican charge distribution scheme as well as the vibrational frequencies of DAPY alone and both its CT complexes with one and two iodine molecules. A very good agreement was found between experiment and theory. New illustrations were concluded with a deep analysis and description for the vibrational frequencies of the formed CT complexes. The two-step CT complex formation mechanism published earlier was supported. Copyright 2009 Elsevier B.V. All rights reserved.

  20. Surface modelling on heavy atom crystalline compounds: HfO{sub 2} and UO{sub 2} fluorite structures

    Energy Technology Data Exchange (ETDEWEB)

    Evarestov, Robert [Department of Quantum Chemistry, St. Petersburg State University, 26 Universitetsky Prospect, Peterhof, St. Petersburg 198504 (Russian Federation)], E-mail: re1973@re1973.spb.edu; Bandura, Andrei; Blokhin, Eugeny [Department of Quantum Chemistry, St. Petersburg State University, 26 Universitetsky Prospect, Peterhof, St. Petersburg 198504 (Russian Federation)

    2009-01-15

    The study of the bulk and surface properties of cubic (fluorite structure) HfO{sub 2} and UO{sub 2} was performed using the hybrid Hartree-Fock density functional theory linear combination of atomic orbitals simulations via the CRYSTAL06 computer code. The Stuttgart small-core pseudopotentials and corresponding basis sets were used for the core-valence interactions. The influence of relativistic effects on the structure and properties of the systems was studied. It was found that surface properties of Mott-Hubbard dielectric UO{sub 2} differ from those found for other metal oxides with the closed-shell configuration of d-electrons.

  1. Nuclear mean fields through self-consistent semiclassical calculations

    Science.gov (United States)

    Bartel, J.; Bencheikh, K.

    Semiclassical expansions derived in the framework of the Extended Thomas-Fermi approach for the kinetic energy density τ( r) and the spin-orbit density J( r) as functions of the local density ρ( r) are used to determine the central nuclear potentials Vn( r) and Vp( r) of the neutron and proton distribution for effective interactions of the Skyrme type. We demonstrate that the convergence of the resulting semiclassical expansions for these potentials is fast and that they reproduce quite accurately the corresponding Hartree-Fock average fields.

  2. Signatures of quantum chaos in rare-earth elements: I. Characterization of the Hamiltonian matrices and coupling matrices of Ce I and Pr I using the statistical predictions of Random Matrix Theory

    Energy Technology Data Exchange (ETDEWEB)

    Cummings, A. [Physics Department, University College Dublin, Dublin (Ireland); Department of Mathematical Physics, National University of Ireland Maynooth, Kildare (Ireland); O' Sullivan, G. [Physics Department, University College Dublin, Dublin (Ireland); Heffernan, D.M. [Department of Mathematical Physics, National University of Ireland Maynooth, Kildare (Ireland); School of Theoretical Physics, Dublin Institute for Advanced Studies, Dublin (Ireland)

    2001-09-14

    Using the relativistic configuration interaction Hartree-Fock method the Hamiltonian matrices of Ce I, J=4{sup {+-}}, and Pr I, J=11/2{sup {+-}}, are studied. These matrices can be characterized as sparse, banded matrices, with a leading diagonal. Diagonalization of the Hamiltonian results in a set of energy eigenvalues and corresponding eigenvectors and the purpose of this investigation will be to characterize the Hamiltonian matrices and coupling matrices of Ce I and Pr I, for both ls and jj coupling representations, using various statistical predictions of Random Matrix Theory. (author)

  3. Ultrafast Processes in Atoms and Molecules: Integrated treatment of electronic and nuclear motion in ultrashort XUV pulses

    Energy Technology Data Exchange (ETDEWEB)

    McCurdy, C. William [Univ. of California, Davis, CA (United States). Dept. of

    2017-12-14

    This project made use of Multiconfiguration Time-Dependent Hartree-Fock method developed earlier in the McCurdy group in a series of novel applications of the method to ultrafast spectroscopic processes. MCTDHF treats the dynamics of a molecule or atom under the influence of an external field in manner that has all electrons active. That property distinguishes this method from the more popular (and much less computationally demanding) approaches for treating the electron dynamics of atoms and molecules in fields, such as the time-dependent “Configuration Interaction Singles” approximation or approaches that limit the treatment to either one or two-electron models.

  4. Mean field theory and boson expansion at finite temperature on the basis of the thermo field dynamics

    Science.gov (United States)

    Hatsuda, Tetsuo

    1989-02-01

    Thermo field dynamics (TFD) is applied to the general hamiltonian with two-body interaction. The Hartree-Fock-Bogoliubov (HFB) equation and RPA at finite temperature are derived by the approximate diagonalization of the time translational operator of TFD. A boson expansion theory at finite temperature is developed by introducing duplicated boson spaces as the image of the boson mapping. These methods are applied to the two-level Lipkin model in which the basic group is shown to become O(5) at finite temperature in place of SU(2).

  5. Finite-temperature treatment of ultracold atoms in a one-dimensional optical lattice

    Science.gov (United States)

    Wild, B. G.; Blakie, P. B.; Hutchinson, D. A. W.

    2006-02-01

    We consider the effects of temperature upon the superfluid phase of ultracold, weakly interacting bosons in a one-dimensional optical lattice. We use a finite-temperature treatment of the Bose-Hubbard model based upon the Hartree-Fock-Bogoliubov formalism, considering both a translationally invariant lattice and one with additional harmonic confinement. In both cases we observe an upward shift in the critical temperature for Bose condensation. For the case with additional harmonic confinement, this is in contrast with results for the uniform gas.

  6. Computational Study of Environmental Effects in the Adsorption of DMMP, Sarin, and VX on gamma-Al2O3: Photolysis and Surface Hydroxylation

    Science.gov (United States)

    2008-11-01

    phase molecule) at the restricted Hartree-Fock ( RHF ) level using the configuration interaction singles43 ap- proach with STO-3G basis sets. Irradiation of...the Brønsted acidity of OH on δ- and θ-Al2O3 by computing the deprotonation energy (ΔEdp) at the RHF level using small cluster models and effective-core...clusters at the RHF /3-21G level. Deprotonation energies (Table 1) were obtained here using the DFT methods and hydroxylated clusters described above

  7. Metallic ferromagnetism in the systems with strongly correlated electrons

    Directory of Open Access Journals (Sweden)

    L.Didukh

    2005-01-01

    Full Text Available The present paper considers the ground state ferromagnetic ordering in narrow-band models with strongly correlated electrons, in particular, in a single-band generalized Hubbard model with correlated hopping and interatomic exchange interaction, as well as in a double orbitally degenerate Hubbard model with correlated hopping. The effective Hamiltonians of these models are treated by means of variants of generalized Hartree-Fock approximations, in which the quasi-particle energy spectra are obtained. The ground state energy, critical electron concentration and magnetization are calculated for some types of density of states. The mechanisms of ferromagnetic ordering stability in the narrow-band materials are discussed.

  8. Electronic structure of the 3d metals. An investigation by L-shell-photoionisation

    Energy Technology Data Exchange (ETDEWEB)

    Richter, T.S.

    2007-12-03

    The 3d transition metal elements from Sc to Cu have been investigated by both photo electron emission and photo absorption. Experimental spectra in the 2p energy range are discussed based on atomic multiplet models and Hartree- Fock calculations. The samples have been evaporated from an electron bombardment crucible and excited/ionized by monochromatized synchrotron radiation. Fundamental effects and the main interactions which govern the electronic structure of the 3d metal atoms are covered. Common spectral features and trends in the series are discussed as well as the importance of many body electron correlation effects. (orig.)

  9. The Application of CPA to Calculations of the Mean Magnetic Moment in the Gd1-xNi, Gd1-xFe, Gd1xCox, and Y1-xCox Intermetallic Compounds

    DEFF Research Database (Denmark)

    Szpunar, B.; Kozarzewski, B.

    1977-01-01

    with a narrow d-band is considered. The magnetic moment of the alloy at zero temperature is calculated within the molecular field and Hartree-Fock approximations. Disorder is treated in the coherent potential approximation. Results are in good agreement with the experimental data obtained for the crystalline......Calculations are made of the mean magnetic moment per atom of the transition metal and the rare-earth metal in the intermetallic compounds, Gd1-x,Nix, Gd1-x Fex, Gd1-x Cox, and Y1-x Cox. A simple model of the disordered alloy consisting of spins localized on the rare-earth atoms and interacting...

  10. Singlet and triplet instability theorems

    Science.gov (United States)

    Yamada, Tomonori; Hirata, So

    2015-09-01

    A useful definition of orbital degeneracy—form-degeneracy—is introduced, which is distinct from the usual energy-degeneracy: Two canonical spatial orbitals are form-degenerate when the energy expectation value in the restricted Hartree-Fock (RHF) wave function is unaltered upon a two-electron excitation from one of these orbitals to the other. Form-degenerate orbitals tend to have isomorphic electron densities and occur in the highest-occupied and lowest-unoccupied molecular orbitals (HOMOs and LUMOs) of strongly correlated systems. Here, we present a mathematical proof of the existence of a triplet instability in a real or complex RHF wave function of a finite system in the space of real or complex unrestricted Hartree-Fock wave functions when HOMO and LUMO are energy- or form-degenerate. We also show that a singlet instability always exists in a real RHF wave function of a finite system in the space of complex RHF wave functions, when HOMO and LUMO are form-degenerate, but have nonidentical electron densities, or are energy-degenerate. These theorems provide Hartree-Fock-theory-based explanations of Hund's rule, a singlet instability in Jahn-Teller systems, biradicaloid electronic structures, and a triplet instability during some covalent bond breaking. They also suggest (but not guarantee) the spontaneous formation of a spin density wave (SDW) in a metallic solid. The stability theory underlying these theorems extended to a continuous orbital-energy spectrum proves the existence of an oscillating (nonspiral) SDW instability in one- and three-dimensional homogeneous electron gases, but only at low densities or for strong interactions.

  11. Nuclear structure for the crust of neutron stars and exotic nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Goegelein, Peter

    2007-07-01

    In this work the Skyrme Hartree-Fock and Relativistic Hartree--Fock approaches have been considered to describe the structure of nuclear systems ranging from finite nuclei, structures in the crust of neutron stars to homogeneous matter. Effects of pairing correlations and finite temperature are also taken into account. The numerical procedure in the cubic box is described for the Skyrme Hartree-Fock as well as the relativistic Hartree-Fock approach. And finally, results for the crust of neutron stars and exotic nuclei are presented and discussed. (orig.)

  12. Energy dependence of negatively charged pion production in proton-proton interactions at the CERN SPS

    CERN Document Server

    AUTHOR|(SzGeCERN)663936; Dominik, Wojciech; Gaździck, Marek

    2016-01-01

    This thesis presents inclusive spectra of the negatively charged pions produced in inelastic proton-proton interactions measured at five beam momenta: 20, 31, 40, 80 and 158 GeV/c. The measurements were conducted in the NA61/SHINE experiment at CERN using a system of five Time Projection Chambers. The negatively charged pion spectra were calculated based on the negatively charged hadron spectra. Contribution of hadrons other than the primary pions was removed using EPOS simulations. The results were corrected for effects related to detection, acceptance, reconstruction efficiency and the analysis technique. Two-dimensional spectra were derived as a function of rapidity and transverse momentum or transverse mass. The spectra were parametrised by widths of the rapidity distributions, inverse slope parameters of the transverse mass distributions, mean transverse masses and the total pion multiplicities. The negatively charged pion spectra in proton-proton interactions belong to a broad NA61/SHINE programme of se...

  13. {ital Ab} {ital initio} calculations of biomolecules

    Energy Technology Data Exchange (ETDEWEB)

    Les, A. [Department of Chemistry, University of Warsaw, 02-093 Warsaw (Poland)]|[Department of Chemistry, University of Arizona, Tucson, Arizona 85721 (United States); Adamowicz, L. [Department of Theoretical Chemistry, University of Lund, Lund, S-22100 (Sweden)]|[Department of Chemistry, University of Arizona, Tucson, Arizona 85721 (United States)

    1995-08-01

    {ital Ab} {ital initio} quantum mechanical calculations are valuable tools for interpretation and elucidation of elemental processes in biochemical systems. With the {ital ab} {ital initio} approach one can calculate data that sometimes are difficult to obtain by experimental techniques. The most popular computational theoretical methods include the Hartree-Fock method as well as some lower-level variational and perturbational post-Hartree Fock approaches which allow to predict molecular structures and to calculate spectral properties. We have been involved in a number of joined theoretical and experimental studies in the past and some examples of these studies are given in this presentation. The systems chosen cover a wide variety of simple biomolecules, such as precursors of nucleic acids, double-proton transferring molecules, and simple systems involved in processes related to first stages of substrate-enzyme interactions. In particular, examples of some {ital ab} {ital initio} calculations used in the assignment of IR spectra of matrix isolated pyrimidine nucleic bases are shown. Some radiation-induced transformations in model chromophores are also presented. Lastly, we demonstrate how the {ital ab}-{ital initio} approach can be used to determine the initial several steps of the molecular mechanism of thymidylate synthase inhibition by dUMP analogues.

  14. Ab initio calculations of biomolecules

    Science.gov (United States)

    Leś, Andrzej; Adamowicz, Ludwik

    1995-08-01

    Ab initio quantum mechanical calculations are valuable tools for interpretation and elucidation of elemental processes in biochemical systems. With the ab initio approach one can calculate data that sometimes are difficult to obtain by experimental techniques. The most popular computational theoretical methods include the Hartree-Fock method as well as some lower-level variational and perturbational post-Hartree Fock approaches which allow to predict molecular structures and to calculate spectral properties. We have been involved in a number of joined theoretical and experimental studies in the past and some examples of these studies are given in this presentation. The systems chosen cover a wide variety of simple biomolecules, such as precursors of nucleic acids, double-proton transferring molecules, and simple systems involved in processes related to first stages of substrate-enzyme interactions. In particular, examples of some ab initio calculations used in the assignment of IR spectra of matrix isolated pyrimidine nucleic bases are shown. Some radiation-induced transformations in model chromophores are also presented. Lastly, we demonstrate how the ab-initio approach can be used to determine the initial several steps of the molecular mechanism of thymidylate synthase inhibition by dUMP analogues.

  15. Effects of compositional defects on small polaron hopping in micas.

    Science.gov (United States)

    Rosso, Kevin M; Ilton, Eugene S

    2005-06-22

    Hartree-Fock calculations and electron transfer (ET) theory were used to model the effects of compositional defects on ET in the brucite-like octahedral sheet of mica. ET was modeled as an Fe(IIIII) valence interchange reaction across shared octahedral edges of the M2-M2 iron sublattice. The model entails the hopping of localized electrons and small polaron behavior. Hartree-Fock calculations indicate that substitution of F for structural OH bridges increases the reorganization energy lambda, decreases the electronic coupling matrix element V(AB), and thereby substantially decreases the hopping rate. The lambda increase arises from modification of the metal-ligand bond force constants, and the V(AB) decrease arises from reduction of superexchange interaction through anion bridges. Deprotonation of an OH bridge, consistent with a possible mechanism of maintaining charge neutrality during net oxidation, yields a net increase in the ET rate. Although substitution of Al or Mg for Fe in M1 sites distorts the structure of adjacent Fe-occupied M2 sites, the distortion has little net impact on ET rates through these M2 sites. Hence the main effect of Al or Mg substitution for Fe, should it occur in the M2 sublattice, is to block ET pathways. Collectively, these findings pave the way for larger-scale oxidation/reduction models to be constructed for realistic, compositionally diverse micas.

  16. BOOK REVIEW: Computational Atomic Structure

    Science.gov (United States)

    Post, Douglass E.

    1998-02-01

    The primary purpose of `Computational Atomic Structure' is to give a potential user of the Multi-Configuration Hartree-Fock (MCHF) Atomic Structure Package an outline of the physics and computational methods in the package, guidance on how to use the package, and information on how to interpret and use the computational results. The book is successful in all three aspects. In addition, the book provides a good overview and review of the physics of atomic structure that would be useful to the plasma physicist interested in refreshing his knowledge of atomic structure and quantum mechanics. While most of the subjects are covered in greater detail in other sources, the book is reasonably self-contained, and, in most cases, the reader can understand the basic material without recourse to other sources. The MCHF package is the standard package for computing atomic structure and wavefunctions for single or multielectron ions and atoms. It is available from a number of ftp sites. When the code was originally written in FORTRAN 77, it could only be run on large mainframes. With the advances in computer technology, the suite of codes can now be compiled and run on present day workstations and personal computers and is thus available for use by any physicist, even those with extremely modest computing resources. Sample calculations in interactive mode are included in the book to illustrate the input needed for the code, what types of results and information the code can produce, and whether the user has installed the code correctly. The user can also specify the calculational level, from simple Hartree-Fock to multiconfiguration Hartree-Fock. The MCHF method begins by finding approximate wavefunctions for the bound states of an atomic system. This involves minimizing the energy of the bound state using a variational technique. Once the wavefunctions have been determined, other atomic properties, such as the transition rates, can be determined. The book begins with an

  17. On the physical origin of the cation-anion intermediate bond in ionic liquids Part I. Placing a (weak) hydrogen bond between two charges.

    Science.gov (United States)

    Lehmann, Sebastian B C; Roatsch, Martin; Schöppke, Matthias; Kirchner, Barbara

    2010-07-21

    The intermediate bond forces in ionic liquids are investigated from static quantum chemical calculations at various methods and two basis sets. The experimentally observed red-shift of the donor-proton bond stretching frequency due to a bond elongation is confirmed by all methods. Comparing Hartree-Fock to second-order Møller-Plesset perturbation theory, the Hartree-Fock method gives in many cases an erroneous description of the geometries. Furthermore, the Hartree-Fock interaction energies can deviate up to 60 kJ mol(-1) from Møller-Plesset perturbation theory indicating the importance of dispersion interaction. While the usual trends of decreasing stability or interaction energies with increasing ion sizes are found, the geometries involving hydrogen atoms do not change this order of total interaction energies. Therefore, the hydrogen bond is not the most important interaction for ion pairs with regard to the total interaction energy. On the other hand, the different established analysis methods give rise to hydrogen bonding in several ion pairs. Charge analysis reveals the hydrogen-bonding character of the ion pair and shows, depending on the type of ions combined and further on the type of conformers considered, that a hydrogen bond can be present. The possibility of hydrogen bonding is also shown by an analysis of the frontier orbitals. Calculating potential energy surfaces and observing from this the change in the donor proton bond indicates that regular hydrogen bonds are possible in ion pairs of ionic liquids. Thereby, the maximum of bond elongation exceeds the one of a usual hydrogen bond by far. The more salt-like hydrogen-bonded ion pair [NH(4)][BF(4)] exhibits a steeper maximum than the more ionic liquid like ion pair [EtNH(3)][BF(4)]. The fact that imidazolium-based ionic liquids as [Emim][Cl] can display two faces, hydrogen bonding and purely ionic bonding, points to a disturbing rather than stabilizing role of hydrogen bonding on the interaction of

  18. A Phenomenological Equation of State of Strongly Interacting Matter with First-Order Phase Transitions and Critical Points

    Science.gov (United States)

    Typel, Stefan; Blaschke, David

    2018-02-01

    An extension of the relativistic density functional approach to the equation of state for strongly interacting matter is suggested which generalizes a recently developed modified excluded-volume mechanism to the case of temperature and density dependent available-volume fractions. A parametrisation of this dependence is presented for which at low temperatures and suprasaturation densities a first-order phase transition is obtained. It changes for increasing temperatures to a crossover transition via a critical endpoint. This provides a benchmark case for studies of the role of such a point in hydrodynamic simulations of ultrarelativistic heavy-ion collisions. The approach is thermodynamically consistent and extendable to finite isospin asymmetries that are relevant for simulations of neutron stars, their mergers and core-collapse supernova explosions.

  19. Many-body effects in Bose-Einstein condensates of dilute atomic gases

    Science.gov (United States)

    Esry, Brett Daniel

    The recent experimental achievement of Bose-Einstein condensation in a dilute alkali gas has spurred a great deal of interest among physicists from many fields. Dilute atomic gas experiments are particularly attractive, compared to experiments on the closely related phenomena of superfluidity and superconductivity, because a dilute gas is a weakly interacting system which is far more amenable to theoretical description. Experimentally, dilute gas experiments are advantageous because relatively straightforward and convenient diagnostics exist, using laser excitation of atomic transitions. As a result, dilute atomic gas experiments can be more completely understood using first principles theoretical treatments. I have adapted the Hartree-Fock, random phase, and configuration interaction approximations to describe systems of interacting bosons, and have shown that such systems can be treated accurately and efficiently within a particle number conserving approximation. In fact, the resulting approximations are remarkably similar to those made in the standard Bogoliubov approach and lead to largely the same equations. A key conclusion is that a system of interacting bosons can be treated in a manner analogous to that used to describe the electronic states of atoms. The hope is that the knowledge and intuition that have been gained from the extensive study of the atomic structure problem will ultimately lead to a deeper understanding of the quantum mechanical states of interacting, trapped atoms. In the course of this work, several phenomena are studied using both the Hartree-Fock approximation and the random phase approximation. The resulting analysis of the stability criteria for single and double condensates improves on results available in the literature in both cases. The double condensate ground state is explored for various hyperfine and isotopic combinations of rubidium in fully three-dimensional configurations for realistic numbers of atoms. Random phase

  20. QM AND AB INITIO INVESTIGATION ON THE HYDROGEN BONDING, NMR CHEMICAL SHIFTS AND SOLVENT EFFECTS ON THE DPPE

    Directory of Open Access Journals (Sweden)

    M. Monajjemi

    2010-06-01

    Full Text Available The hydrogen bonding effects that were produced from interaction of membrane lipid dipalmitoylphosphatidyl-ethanolamine (DPPE with 1-5 water molecules, has been theoretically  investigated through the quantum mechanical calculations at the Hartree-Fock level of theory and the 3-21G, 6-31G and 6-31G* basis sets with the computational package of Gaussian 98. According to the obtained results of the structural optimization of the isolated DPPE in the gas phase, we can see the evidences of interactions in the head group of this macromolecule (from the molecular point of view we have a proton transfer from the ammonium group to the phosphate oxygen of zwitterionic form. As we know that the hydrogen bonding of DPPE with water molecules which have surrounded its head group plays an important role in the permeability of DPPE. So, in order to understand the microscopic physico-chemical nature of this subject we have analyzed bond and torsion angles of DPPE before and after added water molecules.  In this paper we have theoretically studied the complexes DPPE with water molecules which have surrounded its head group. As mentioned before, this theoretically study has been done through Hartree-Fock level of theory by using simple basis sets. Theoretical data shows that the interaction of head group of DPPE with water molecules causes some changes in the geometry of DPPE which were explained by the contribution of zwitterionic form of DPPE macromolecule, and finally hydrated DPPE becomes stable complex. Comparison between theoretical and experimental geometry data of DPPE macromolecule shows that the calculation at the HF/3-21 level of theory produces results which they are in better agreement with the experimental data. Moreover the hydrogen bonding effects on the NMR shielding tensor of selected atoms in the hydrated complexes of DPPE were reported. The ";Gauge Including Atomic Orbitals"; (GIAO approaches within the SCF-Hartree-Fock approximation have

  1. Communication: generalization of Koopmans' theorem to optical transitions in the Hubbard model of graphene nanodots.

    Science.gov (United States)

    Sheng, Weidong; Luo, Kaikai; Zhou, Aiping

    2015-01-14

    Koopmans' theorem implies that the Hartree-Fock quasiparticle gap in a closed-shell system is equal to its single-particle energy gap. In this work, the theorem is generalized to optical transitions in the Hubbard model of graphene nanodots. Based on systematic configuration interaction calculations, it is proposed that the optical gap of a closed-shell graphene system within the Hubbard model is equal to its tight-binding single-particle energy gap in the absence of electron correlation. In these systems, the quasiparticle energy gap and exciton binding energy are found to be dominated by the long-range Coulomb interaction, and thus, both become small when only on-site Hubbard interactions are present. Moreover, the contributions of the quasiparticle and excitonic effects to the optical gap are revealed to nearly cancel each other, which results in an unexpected overlap of the optical and single-particle gaps of the graphene systems.

  2. Shell model calculations for exotic nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Brown, B.A. (Michigan State Univ., East Lansing, MI (USA)); Warburton, E.K. (Brookhaven National Lab., Upton, NY (USA)); Wildenthal, B.H. (New Mexico Univ., Albuquerque, NM (USA). Dept. of Physics and Astronomy)

    1990-02-01

    In this paper we review the progress of the shell-model approach to understanding the properties of light exotic nuclei (A < 40). By shell-model'' we mean the consistent and large-scale application of the classic methods discussed, for example, in the book of de-Shalit and Talmi. Modern calculations incorporate as many of the important configurations as possible and make use of realistic effective interactions for the valence nucleons. Properties such as the nuclear densities depend on the mean-field potential, which is usually separately from the valence interaction. We will discuss results for radii which are based on a standard Hartree-Fock approach with Skyrme-type interactions.

  3. Active appearance pyramids for object parametrisation and fitting.

    Science.gov (United States)

    Zhang, Qiang; Bhalerao, Abhir; Dickenson, Edward; Hutchinson, Charles

    2016-08-01

    Object class representation is one of the key problems in various medical image analysis tasks. We propose a part-based parametric appearance model we refer to as an Active Appearance Pyramid (AAP). The parts are delineated by multi-scale Local Feature Pyramids (LFPs) for superior spatial specificity and distinctiveness. An AAP models the variability within a population with local translations of multi-scale parts and linear appearance variations of the assembly of the parts. It can fit and represent new instances by adjusting the shape and appearance parameters. The fitting process uses a two-step iterative strategy: local landmark searching followed by shape regularisation. We present a simultaneous local feature searching and appearance fitting algorithm based on the weighted Lucas and Kanade method. A shape regulariser is derived to calculate the maximum likelihood shape with respect to the prior and multiple landmark candidates from multi-scale LFPs, with a compact closed-form solution. We apply the 2D AAP on the modelling of variability in patients with lumbar spinal stenosis (LSS) and validate its performance on 200 studies consisting of routine axial and sagittal MRI scans. Intervertebral sagittal and parasagittal cross-sections are typically used for the diagnosis of LSS, we therefore build three AAPs on L3/4, L4/5 and L5/S1 axial cross-sections and three on parasagittal slices. Experiments show significant improvement in convergence range, robustness to local minima and segmentation precision compared with Constrained Local Models (CLMs), Active Shape Models (ASMs) and Active Appearance Models (AAMs), as well as superior performance in appearance reconstruction compared with AAMs. We also validate the performance on 3D CT volumes of hip joints from 38 studies. Compared to AAMs, AAPs achieve a higher segmentation and reconstruction precision. Moreover, AAPs have a significant improvement in efficiency, consuming about half the memory and less than 10% of the training time and 15% of the testing time. Copyright © 2016 Elsevier B.V. All rights reserved.

  4. Microscopic Modeling of Intersubband Optical Processes in Type II Semiconductor Quantum Wells: Linear Absorption

    Science.gov (United States)

    Li, Jian-Zhong; Kolokolov, Kanstantin I.; Ning, Cun-Zheng

    2003-01-01

    Linear absorption spectra arising from intersubband transitions in semiconductor quantum well heterostructures are analyzed using quantum kinetic theory by treating correlations to the first order within Hartree-Fock approximation. The resulting intersubband semiconductor Bloch equations take into account extrinsic dephasing contributions, carrier-longitudinal optical phonon interaction and carrier-interface roughness interaction which is considered with Ando s theory. As input for resonance lineshape calculation, a spurious-states-free 8-band kp Hamiltonian is used, in conjunction with the envelop function approximation, to compute self-consistently the energy subband structure of electrons in type II InAs/AlSb single quantum well structures. We demonstrate the interplay of nonparabolicity and many-body effects in the mid-infrared frequency range for such heterostructures.

  5. AB INITIO INVESTIGATION OF 12-CROWN-4 AND BENZO-12-CROWN-4 COMPLEXES WITH Li+, Na+, K+, Zn2+, Cd2+, AND Hg2+

    Directory of Open Access Journals (Sweden)

    Yahmin Yahmin

    2010-06-01

    Full Text Available The structure and binding energies of 12-crown-4 and benzo-12-crown-4 complexes with Li+, Na+, K+, Zn2+, Cd2+, and Hg2+were investigated with ab initio calculations using Hartree-Fock approximation and second-order perturbation theory. The basis set used in this study is lanl2mb. The structure optimization of cation-crown ether complexes was evaluated at HF/lanl2mb level of theory and interaction energy of the corresponding complexes was calculated at MP2/lanl2mb level of theory (MP2/lanl2mb//HF/lanl2mb. Interactions of the crown ethers and the cations were discussed in term of the structure parameter of crown ether. The binding energies of the complexes show that all complex formed from transition metal cations is more stable than the complexes formed from alkali metal cations.   Keywords: 12-crown-4, benzo-12-crown-4, alkali metals, transition metals

  6. Quantum chemical study of reaction mechanism of [4+2]-cycloaddition between 2,3-dimethylbuta-1,3-diene and methyl acrylate

    Directory of Open Access Journals (Sweden)

    Yaroslav Kovalskyi

    2017-01-01

    Full Text Available The quantum-chemical modeling mechanism of the [4+2]-cycloaddition reaction of 2,3 dimethylbuta-1,3-diene and methyl acrylate was conducted. Its qualitative aspects were analyzed at the molecular level by the program MOPAC2012 and semiempirical method RM1. The potential energy surfaces of 2,3 dimethylbuta-1,3-diene and methyl acrylate [4+2] cycloaddition possible reaction pathways were constructed by restricted and unrestricted Hartree-Fock approximation. It has been established that the molecule of the final product methyl-3,4-dimethylcyclohex-3-encarboxylate has the half-chair shape, wherein the carboalkoxyl group is in the exo-orientation. Interaction between molecules of 2,3 dimethylbuta-1,3-diene and methyl acrylate occurs by a two-step mechanism more likely than one-step, since the activation parameters of this interaction maximum coincide with the experimental data.

  7. Self-Consistent Green Function Method in Nuclear Matter

    Directory of Open Access Journals (Sweden)

    Khaled S. A. Hassaneen

    2013-01-01

    Full Text Available Symmetric nuclear matter is studied within the Brueckner-Hartree-Fock (BHF approach and is extending to the self-consistent Green’s function (SCGF approach. Both approximations are based on realistic nucleon-nucleon interaction; that is, CD-Bonn potential is chosen. The single-particle energy and the equation of state (EOS are studied. The Fermi energy at the saturation point fulfills the Hugenholtz-Van Hove theorem. In comparison to the BHF approach, the binding energy is reduced and the EOS is stiffer. Both the SCGF and BHF approaches do not reproduce the correct saturation point. A simple contact interaction should be added to SCGF and BHF approaches to reproduce the empirical saturation point.

  8. Spontaneous formation of bright solitons in self-localized impurities in Bose-Einstein condensates

    Science.gov (United States)

    Boudjemâa, Abdelâali

    2016-04-01

    We study the formation of bright solitons in the impurity component of Bose-Einstein condensate-impurity mixture by using the time-dependent Hartree-Fock-Bogoliubov theory. While we assume the boson-boson and impurity-boson interactions to be effectively repulsive, their character can be changed spontaneously from repulsive to attractive in the presence of strong anomalous correlations. In such a regime the impurity component becomes a system of effectively attractive atoms leading automatically to the generation of bright solitons. We find that this soliton decays at higher temperatures due to the dissipation induced by the impurity-host and host-host interactions. We show that after a sudden increase of the impurity-boson strength a train of bright solitons is produced and this can be interpreted in terms of the modulational instability of the time-dependent impurity wave function.

  9. From small to medium and beyond: a pragmatic approach in predicting properties of Ne containing structures

    Science.gov (United States)

    Kupka, Teobald; Stachów, Michał; Nieradka, Marzena; Radula-Janik, Klaudia; Stobiński, Leszek; Kaminský, Jakub

    2014-03-01

    In this study, we outlined a pragmatic approach for structural studies leading to better understanding of polycarbon structures using 21Ne as a nuclear magnetic resonance (NMR) probe. 21Ne NMR parameters of a single neon atom and its dimer were predicted at the CCSD(T) level in combination with large basis sets. At a lower level of theory, an interaction of neon atom with 1,3-cyclopentadiene ring and with five- and six-membered rings in carbazole was studied using the restricted Hartree-Fock (RHF) and density functional theory (DFT) combined with smaller basis sets. The RHF and DFT modelling of neon interaction with nanosized objects were performed on cyclacenes and selected fullerenes.

  10. Reactions of Proton Halo Nuclei in a Relativistic Optical Potential

    CERN Document Server

    Rashdan, M

    2003-01-01

    The reaction cross section, sigma sub R; of the proton halo nuclei sup 1 sup 7 Ne and sup 1 sup 2 N on Si is calculated using an optical potential derived from the solution of the Dirac-Brueckner-Bethe-Goldstone equation, starting from the one-boson-exchange potential of Bonn. The nuclear densities are generated from self-consistent Hartree-Fock calculations using the recent Skyrme interaction SKRA. It is found that the enhancement in the reaction cross section found experimentally for the sup 1 sup 7 Ne + Si system in comparison to sup 1 sup 5 O + Si, where sup 1 sup 5 O has been considered as a core of sup 1 sup 7 Ne, is mainly due to the proton halo structure of sup 1 sup 7 Ne which increases the interaction, in the surface and tail regions. Glauber model calculations did not produce this enhancement in sigma sub R for proton halo nuclei

  11. Structures and spectra of gold nanoclusters and quantum dot molecules

    Science.gov (United States)

    Barnett, R. N.; Cleveland, C. L.; Häkkinen, H.; Luedtke, W. D.; Yannouleas, C.; Landman, U.

    Size-evolutions of structural and spectral properties in two types of finite systems are discussed. First we focus on energetics and structures of gold clusters, particularly AuN in the 40LSD) method, for a broad range of interdot distances and coupling strengths. A molecular orbital classification of the QDM states correlates between the united-dot and separated-dots limits. LSD addition energies and spin polarization patterns for QDM's in the entire coupling range are analyzed, guiding the construction of a constant interaction model. A generalization of the non-interacting-electrons Darwin-Fock model to QDM's is presented. Wigner crystallization of the electrons leading to formation of Wigner supermolecules is explored in both the field-free case and with a magnetic field using a spin-and-space unrestricted Hartree-Fock method.

  12. On the XFEL Schrödinger Equation: Highly Oscillatory Magnetic Potentials and Time Averaging

    KAUST Repository

    Antonelli, Paolo

    2014-01-14

    We analyse a nonlinear Schrödinger equation for the time-evolution of the wave function of an electron beam, interacting selfconsistently through a Hartree-Fock nonlinearity and through the repulsive Coulomb interaction of an atomic nucleus. The electrons are supposed to move under the action of a time dependent, rapidly periodically oscillating electromagnetic potential. This can be considered a simplified effective single particle model for an X-ray free electron laser. We prove the existence and uniqueness for the Cauchy problem and the convergence of wave-functions to corresponding solutions of a Schrödinger equation with a time-averaged Coulomb potential in the high frequency limit for the oscillations of the electromagnetic potential. © 2014 Springer-Verlag Berlin Heidelberg.

  13. Self-consistent approach for Bose-condensed atoms in optical lattices

    Directory of Open Access Journals (Sweden)

    V.I. Yukalov

    2013-06-01

    Full Text Available Bose atoms in optical lattices are considered at low temperatures and weak interactions, when Bose-Einstein condensate is formed. A self-consistent approach, based on the use of a representative statistical ensemble, is employed, guaranteeing a gapless spectrum of collective excitations and the validity of conservation laws. In order to show that the approach is applicable to both weak and tight binding, the problem is treated in the Bloch as well as in the Wannier representations. Both these ways result in similar expressions that are compared for the self-consistent Hartree-Fock-Bogolubov approximation. A convenient general formula for the superfluid fraction of atoms in an optical lattice is derived.

  14. Quark pair condensation and chiral symmetry breaking in QCD

    Energy Technology Data Exchange (ETDEWEB)

    Finger, J.R. (Massachusetts Inst. of Tech., Cambridge (USA)); Mandula, J.E. (Washington Univ., St. Louis, MO (USA))

    1982-05-17

    If the effective qanti q interaction strength due to gluon exchange becomes at least moderately strong beyond some distance g/sup 2//4..pi.. > 9/8, the perturbative vacuum becomes unstable to the creation of color singlet qanti q pairs, which indicates that the true vacuum contains a condensate of such pairs. We analyze the condensation by a coherent state variational procedure modeled after the BCS superconductor, and show that this method is equivalent to a self-consistent Hartree-Fock approximation to the Schwinger-Dyson equation for the quark propagator. The condensate leads to a spontaneous breakdown of chiral symmetry in the manner discussed by Nambu and Jona-Lasinio. The massive pseudoparticles with quark quantum numbers are identified with the 'constituent' quarks.

  15. Quark pair condensation and chiral symmetry breaking in QCD

    Science.gov (United States)

    Finger, Jonathan R.; Mandula, Jeffrey E.

    1982-05-01

    If the effective qoverlineq interaction strength due to gluon exchange becomes at least moderately strong beyond some distance g 2/4π > {9}/{8}, the perturbative vacuum becomes unstable to the creation of color singlet qoverlineq pairs, which indicates that the true vacuum contains a condensate of such pairs. We analyze the condensation by a coherent state variational procedure modeled after the BCS superconductor, and show that this method is equivalent to a self-consistent Hartree-Fock approximation to the Schwinger-Dyson equation for the quark propagator. The condensate leads to a spontaneous breakdown of chiral symmetry in the manner discussed by Nambu and Jona-Lasinio. The massive pseudoparticles with quark quantum numbers are identified with the "constituent" quarks.

  16. β-decay properties of neutron-deficient Pt, Hg, and Pb isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Sarriguren, P., E-mail: p.sarriguren@csic.es [Instituto de Estructura de la Materia, IEM-CSIC, Serrano 123, E-28006 Madrid (Spain); Boillos, J. M. [Instituto de Estructura de la Materia, IEM-CSIC, Serrano 123, E-28006 Madrid (Spain); Universidad de Santiago de Compostela, 15706 Santiago de Compostela (Spain); Moreno, O. [Center for Theoretical Physics, Laboratory for Nuclear Science and Department of Physics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 (United States); Moya de Guerra, E. [Departamento de Física Atómica, Molecular y Nuclear, Facultad de Ciencias Físicas, Universidad Complutense de Madrid, E-28040 Madrid (Spain)

    2015-10-15

    Neutron-deficient isotopes in the lead region are well established examples of the shape coexistence phenomenon in nuclei. In this work, bulk and decay properties, including deformation energy curves, charge mean square radii, Gamow-Teller (GT) strength distributions, and β-decay half-lives, are studied in neutron-deficient Pt, Hg, and Pb isotopes. The nuclear structure involved is described microscopically from deformed quasiparticle random-phase approximation calculations with residual interactions in both particle-hole and particle-particle channels, performed on top of a self-consistent deformed quasiparticle Skyrme Hartree-Fock basis. The sensitivity to deformation of the GT strength distributions in those isotopes is proposed as an additional complementary signature of the nuclear shape. The β-decay half-lives resulting from the GT strength distributions are compared to experiment to demonstrate the ability of the method.

  17. Fermionic Superfluids: From Cold Atoms To High Density Qcd Gapless (breached Pair) Superfluidity And Kaon Condensation

    CERN Document Server

    Forbes, M M

    2005-01-01

    In this thesis, we explore aspects of fermionic superfluidity through a mean-field approximation. Our framework is extremely general, includes both pairing and Hartree-Fock contributions, and is derived rigorously from a variational principle. This framework allows us to analyze a wide range of fermionic systems. In this thesis, we shall consider two-species non-relativistic atomic systems with various types of interactions, and relativistic QCD systems with 3 × 3 × 4 = 36 different quark degrees of freedom (3 colours, 3 flavours, and 4 relativistic degrees of freedom). We discuss properties of a new state of matter: gapless (Breached Pair) superfluidity, and include a summary of potential experimental realizations. We also present numerical results for a completely self-consistent approximation to the NJL model of high-density QCD and use these results to demonstrate a microscopic realization of kaon condensation. We describe how to match the mean-field approximation to the low-energy chi...

  18. Study of frequency- and temperature-dependent electrical transport in heavy fermion systems

    Science.gov (United States)

    Baral, P. C.

    2017-05-01

    This paper focuses on the frequency- and temperature-dependent electrical transport properties of heavy fermion (HF) systems. For this, Kondo lattice model (KLM) with Coulomb correlation between f-f electrons at the same site is considered. The Hamiltonian is treated in mean-field approximation (MFA) for the Kondo hybridization and Heisenberg-type interaction to get mean-field Hamiltonian and it is written after the Fourier transformation. The Hartree-Fock-type approximation is considered for the Coulomb repulsion between f-f electrons, the perturbed part of the Hamiltonian. The two Green’s functions for the conduction and f-electrons are calculated to define the self-energy. Then the frequency- and temperature-dependent optical conductivity and resistivity are calculated by using the Kubo’s formula within the linear dynamical response approach. They are studied by varying the model parameters. The anomalies and results obtained are compared with experimental data.

  19. Spectral investigation of highly ionized bismuth plasmas produced by subnanosecond Nd:YAG laser pulses

    Science.gov (United States)

    Wu, Tao; Higashiguchi, Takeshi; Li, Bowen; Arai, Goki; Hara, Hiroyuki; Kondo, Yoshiki; Miyazaki, Takanori; Dinh, Thanh-Hung; Dunne, Padraig; O'Reilly, Fergal; Sokell, Emma; O'Sullivan, Gerry

    2016-02-01

    The unresolved transition arrays (UTAs) emitted from laser produced bismuth (Bi) plasma sources show potential for single-shot live cell imaging. We have measured extreme ultraviolet spectra from bismuth laser produced plasmas in the 1-7 nm region using a λ = 1064 nm Nd:YAG laser with a pulse duration of 150 ps. Comparison of spectra obtained under different laser power densities with calculations using the Hartree-Fock with configuration interaction Cowan suite of codes and the UTA formalism, as well as consideration of previous predictions of isoelectronic trends, are employed to identify lines and a number of new features in spectra from Bi XXIII to Bi XLVII. The results show that Δn = 0, n = 4-4 emission from highly charged ions merges to form intense UTAs in the 4 nm region and Δn = 1, n = 4-5 resonance transitions UTAs dominate the 1-3 nm region of the Bi spectrum.

  20. Giant quadrupole resonances in time-dependent density-matrix theory

    CERN Document Server

    Tohyama, M

    1999-01-01

    Damping of an isoscalar giant quadrupole resonance (GQR) in sup 4 sup 0 Ca is studied using an extended version of the time-dependent Hartree--Fock theory known as the time-dependent density-matrix theory (TDDM). The Skyrme III force is used as an effective interaction for the calculation of both a mean-field potential and a two-body correlation function, and a correlated state is used as the ground state on which GQR is built. It is found that the calculated strength of GQR is split into a major component and a minor component. The spreading width of the major component is found small as compared with experimental data. A double giant quadrupole resonance (DGQR) is also studied in TDDM, and it is found that DGQR given in TDDM has properties of the double phonon state of GQR calculated in the random phase approximation.

  1. Fast and reliable ab initio calculation of crystal field splittings in lanthanide complexes

    Science.gov (United States)

    Hallmen, P. P.; Köppl, C.; Rauhut, G.; Stoll, H.; van Slageren, J.

    2017-10-01

    Ab initio calculations of crystal field splittings and magnetic properties of lanthanide complexes are usually performed using state-averaged complete active space self-consistent field (CASSCF) calculations and a subsequent spin-orbit calculation mixing the CASSCF wave functions (CASSCF/state interaction with spin-orbit coupling). Because this approach becomes very time-consuming for large molecules, simplifications have been proposed in the literature to determine the state-averaged orbitals by configuration-averaged Hartree-Fock (CAHF) instead of CASSCF. We present an approach which is an extension of the CAHF method. We combine the techniques of local density fitting with CAHF and achieve a significant speedup compared to CASSCF without loss in accuracy. To assess the performance of our method, we apply it to three well-known molecules, namely, Er[N(SiMe3)2]3, Er(trensal), and the double-decker (NBu4)+ [Er(Pc)2]-.

  2. Model-space approach to {sup 1}S{sub 0} neutron and proton pairing with the Bonn meson - exchange potentials

    Energy Technology Data Exchange (ETDEWEB)

    Elgaroey, Oe.; Engvik, L.; Osnes, E.; Hjort-Jensen, M.

    1996-03-01

    In this work the authors calculate neutron and proton energy gaps in neutron star matter using the Bonn meson exchange interactions and a model-space approach to the gap equation. This approach allows a consistent calculation of energy gaps and single particle energies with the model-space Brueckner-Hartree-Fock (MBHF) method, without double counting of two-particle correlations. Neutron energy gaps are calculated at zero and finite temperature. Proton energy gaps are calculated at beta equilibrium, and it is shown that the inclusion of muons has a significant effect. The results are compared with those of other works, and the implications for neutron star physics are briefly discussed. 18 refs., 15 figs., 1 tab.

  3. Image-charge-induced localization of molecular orbitals at metal-molecule interfaces

    DEFF Research Database (Denmark)

    Strange, M.; Thygesen, K. S.

    2012-01-01

    -conjugated molecular wire in contact with a metal surface. We find that image charge effects pull the frontier molecular orbitals toward the metal surface, while orbitals with higher or lower energy are pushed away. This affects both the size of the energetic image charge shifts and the coupling of the individual......Quasiparticle (QP) wave functions, also known as Dyson orbitals, extend the concept of single-particle states to interacting electron systems. Here we employ many-body perturbation theory in the GW approximation to calculate the QP wave functions for a semiempirical model describing a pi...... orbitals to the metal substrate. Full diagonalization of the QP equation and, to some extent, self-consistency in the GW self-energy, is important to describe the effect, which is not captured by standard density functional theory or Hartree-Fock. These results should be important for the understanding...

  4. Spiral magnetic order, non-uniform states and electron correlations in the conducting transition metal systems

    Science.gov (United States)

    Igoshev, P. A.; Timirgazin, M. A.; Arzhnikov, A. K.; Antipin, T. V.; Irkhin, V. Yu.

    2017-10-01

    The ground-state magnetic phase diagram is calculated within the Hubbard and s-d exchange (Kondo) models for square and simple cubic lattices vs. band filling and interaction parameter. The difference of the results owing to the presence of localized moments in the latter model is discussed. We employ a generalized Hartree-Fock approximation (HFA) to treat commensurate ferromagnetic (FM), antiferromagnetic (AFM), and incommensurate (spiral) magnetic phases. The electron correlations are taken into account within the Hubbard model by using the Kotliar-Ruckenstein slave boson approximation (SBA). The main advantage of this approach is a correct qualitative description of the paramagnetic phase: its energy becomes considerably lower as compared with HFA, and the gain in the energy of magnetic phases is substantially reduced.

  5. Quantum physics of light and matter a modern introduction to photons, atoms and many-body systems

    CERN Document Server

    Salasnich, Luca

    2014-01-01

    The book gives an introduction to the field quantization (second quantization) of light and matter with applications to atomic physics. The first chapter briefly reviews the origins of special relativity and quantum mechanics and the basic notions of quantum information theory and quantum statistical mechanics. The second chapter is devoted to the second quantization of the electromagnetic field, while the third chapter shows the consequences of the light field quantization in the description of electromagnetic transitions.In the fourth chapter it is analyzed the spin of the electron, and in particular its derivation from the Dirac equation, while the fifth chapter investigates the effects of external electric and magnetic fields on the atomic spectra (Stark and Zeeman effects). The sixth chapter describes the properties of systems composed by many interacting identical particles by introducing the Hartree-Fock variational method, the density functional theory, and the Born-Oppenheimer approximation. Finally,...

  6. Deformed shell model study of event rates for WIMP-73Ge scattering

    Science.gov (United States)

    Sahu, R.; Kota, V. K. B.

    2017-12-01

    The event detection rates for the Weakly Interacting Massive Particles (WIMP) (a dark matter candidate) are calculated with 73Ge as the detector. The calculations are performed within the deformed shell model (DSM) based on Hartree-Fock states. First, the energy levels and magnetic moment for the ground state and two low-lying positive parity states for this nucleus are calculated and compared with experiment. The agreement is quite satisfactory. Then the nuclear wave functions are used to investigate the elastic and inelastic scattering of WIMP from 73Ge; inelastic scattering, especially for the 9/2+ → 5/2+ transition, is studied for the first time. The nuclear structure factors which are independent of supersymmetric model are also calculated as a function of WIMP mass. The event rates are calculated for a given set of nucleonic current parameters. The calculation shows that 73Ge is a good detector for detecting dark matter.

  7. Dipole response in neutron-rich nuclei within self-consistent approaches using realistic potentials

    Directory of Open Access Journals (Sweden)

    Lo Iudice N.

    2015-01-01

    Full Text Available A nucleon-nucleon chiral potential with a corrective density dependent term simulating a three-body force is used in a self-consistent calculation of the dipole strength distribution in neutron-rich nuclei, with special attention to the low-lying spectra associated to the pygmy resonance. A Hartree-Fock-Bogoliubov basis is generated and adopted in Tamm-Dancoff and random-phase approximations and, then, in an equation of motion approach which includes a basis of two-phonon states. The direct use of the mentioned chiral potential improves the description of both giant and pygmy dipole modes with respect to other realistic interactions. Moreover, the inclusion of the two-phonon states induces a pronounced fragmentation of the giant resonance and enhances the density of the low-lying levels in the pygmy region in agreement with recent experiments.

  8. 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.

  9. Estudo das ligações de hidrogênio para dímeros formados pelas moléculas de H2O, NH3, HF, HCl e HBr através de cálculos baseados em primeiros princípios

    Directory of Open Access Journals (Sweden)

    Sergio Duvoisin Jr

    2011-09-01

    Full Text Available Hydrogen bond energies of fifteen dimers were calculated using the large basis set 6-311++G(3df,3pd, at Hartree-Fock (HF level including Møller-Plesset (MP2 calculations. The procedure for obtaining such energies were based on the dimer's energy rise provoked by increasing in intermolecular distance of the system component units. Deviations from a strictly linear hydrogen bond were investigated and rotational barriers were also computed allowing the calculation of the second order attractive interactions. In order to provide a more objective definition of hydrogen bond, a lower energy limit was proposed in place of the merely empirical parameters employed in the classical definition

  10. Fundamental and excited states of F-type centres in MgSiO{sub 3} perovskite

    Energy Technology Data Exchange (ETDEWEB)

    Stashans, Arvids, E-mail: arvids@utpl.edu.e [Grupo de Fisicoquimica de Materiales, Universidad Tecnica Particular de Loja, Apartado 11-01-608, Loja (Ecuador); Piedra, Lorena; Briceno, Tamara [Grupo de Fisicoquimica de Materiales, Universidad Tecnica Particular de Loja, Apartado 11-01-608, Loja (Ecuador); Escuela de Geologia y Minas, Universidad Tecnica Particular de Loja, Apartado 11-01-608, Loja (Ecuador)

    2010-10-15

    Quantum-chemical modelling based on the Hartree-Fock methodology and a periodic supercell model is done to study oxygen vacancy and F-type centres in the perovskite-type MgSiO{sub 3} crystal. The equilibrium geometry of defects is obtained, confirming the importance of electrostatic interaction in determination of atomic shifts. The calculated relaxation energies due to the defect formation are between 8 and 10 eV, thus evidencing favourability in the occurrence of such defects. The wave functions describing both F{sup +} and F centres are rather diffuse and the point defects are not well localised within the oxygen vacancy region. The {Delta} SCF computed absorption energies due to the F-type centres fall well within the ultraviolet spectrum, between 136 and 254 nm for the F{sup +} centre and between 163 and 248 nm for the F centre.

  11. Catalysis by transition metal compounds

    Energy Technology Data Exchange (ETDEWEB)

    Klein, D. L.

    1978-01-01

    The catalytic properties of cobalt oxide (Co0) were investigated theoretically. The interactions of atomic hydrogen with small clusters of atoms, representing cobalt oxide surfaces, were calculated using the ab initio Unrestricted Hartree-Fock (UHF) method. The electronic structure of the bulk solid was studied through band and cluster models. The bulk electronic structure computed predicts insulating behavior for cobalt oxide and agrees with experimental optical results. The ''perfect'' (100) cobalt oxide surface was determined not to chemisorb atomic hydrogen. Singly-ionized oxygen ions located near cation vacancies were found to chemisorb hydrogen, forming two-center covalent bonds. The effect of lattice defects on the creation of singly ionized oxygen ions was examined. A systematic procedure for the study of surface and bulk electronic properties was discussed.

  12. Microscopic Calculation of 240Pu Scission with a Finite-Range Effective Force

    Energy Technology Data Exchange (ETDEWEB)

    Younes, W; Gogny, D

    2009-05-04

    Hartree-Fock-Bogoliubov calculations of hot fission in {sup 240}Pu have been performed with a newly-implemented code that uses the D1S finite-range effective interaction. The hot-scission line is identified in the quadrupole-octupole-moment coordinate space. Fission-fragment shapes are extracted from the calculations. A benchmark calculation for {sup 226}Th is obtained and compared to results in the literature. In addition, technical aspects of the use of HFB calculations for fission studies are examined in detail. In particular, the identification of scission configurations, the sensitivity of near-scission calculations to the choice of collective coordinates in the HFB iterations, and the formalism for the adjustment of collective-variable constraints are discussed. The power of the constraint-adjustment algorithm is illustrated with calculations near the critical scission configurations with up to seven simultaneous constraints.

  13. Wave-packet propagation based calculation of above-threshold ionization in the x-ray regime

    CERN Document Server

    Tilley, Matthew; Santra, Robin

    2015-01-01

    We investigate the multi-photon process of above-threshold ionization for the light elements hydrogen, carbon, nitrogen and oxygen in the hard x-ray regime. Numerical challenges are discussed and by comparing Hartree-Fock-Slater calculations to configuration-interaction-singles results we justify the mean-field potential approach in this regime. We present a theoretical prediction of two-photon above-threshold-ionization cross sections for the mentioned elements. Moreover, we study how the importance of above-threshold ionization varies with intensity. We find that for carbon, at x-ray intensities around $10^{23}{\\rm Wcm}^{-2}$, two-photon above-threshold ionization of the K-shell electrons is as probable as one-photon ionization of the L-shell electrons.

  14. Entanglement and magnetism in high-spin graphene nanodisks

    Science.gov (United States)

    Hagymási, I.; Legeza, Ö.

    2018-01-01

    We investigate the ground-state properties of triangular graphene nanoflakes with zigzag edge configurations. The description of zero-dimensional nanostructures requires accurate many-body techniques since the widely used density-functional theory with local density approximation or Hartree-Fock methods cannot handle the strong quantum fluctuations. Applying the unbiased density-matrix renormalization group algorithm we calculate the magnetization and entanglement patterns with high accuracy for different interaction strengths and compare them to the mean-field results. With the help of quantum information analysis and subsystem density matrices we reveal that the edges are strongly entangled with each other. We also address the effect of electron and hole doping and demonstrate that the magnetic properties of triangular nanoflakes can be controlled by an electric field, which reveals features of flat-band ferromagnetism. This may open up new avenues in graphene based spintronics.

  15. GAS PHASE STRUCTURE AND STABILITY OF COMPLEX FORMED BY H2O, NH3, H2S AND THEIR METHYL DERIVATIVES WITH THE CATION CO2+

    Directory of Open Access Journals (Sweden)

    Cahyorini Kusumawardani

    2010-06-01

    Full Text Available Ab initio molecular orbital calculations at the Hartree-Fock-Self Consistent Field (HF-SCF have been performed in order to determine the structure and gas phase energies of complex formed by the Lewis bases of H2O, NH3, H2S and their methyl derivatives with the cation Co2+. The relative basicities of the base studied depend on both the substituent. The gas-phase interaction energies computed by the SCF method including electron correlation Møller-Plesset 2 (MP2 dan Configuration Iteration (CI were comparable in accuracy. The binding energies computed by these two methods reach the targeted chemical accuracy.   Keywords: ab initio calculation, cobalt complex, structure stability

  16. Pinning of fermionic occupation numbers.

    Science.gov (United States)

    Schilling, Christian; Gross, David; Christandl, Matthias

    2013-01-25

    The Pauli exclusion principle is a constraint on the natural occupation numbers of fermionic states. It has been suspected since at least the 1970s, and only proved very recently, that there is a multitude of further constraints on these numbers, generalizing the Pauli principle. Here, we provide the first analytic analysis of the physical relevance of these constraints. We compute the natural occupation numbers for the ground states of a family of interacting fermions in a harmonic potential. Intriguingly, we find that the occupation numbers are almost, but not exactly, pinned to the boundary of the allowed region (quasipinned). The result suggests that the physics behind the phenomenon is richer than previously appreciated. In particular, it shows that for some models, the generalized Pauli constraints play a role for the ground state, even though they do not limit the ground-state energy. Our findings suggest a generalization of the Hartree-Fock approximation.

  17. Addition and removal energies of circular quantum dots

    Science.gov (United States)

    Yuan, Fei; Novario, Samuel J.; Parzuchowski, Nathan M.; Reimann, Sarah; Bogner, S. K.; Hjorth-Jensen, Morten

    2017-10-01

    We present and compare several many-body methods as applied to two-dimensional quantum dots with circular symmetry. We calculate the approximate ground state energy using a harmonic oscillator basis optimized by Hartree-Fock (HF) theory and further improve the ground state energy using two post-HF methods: in-medium similarity renormalization group and coupled cluster with singles and doubles. With the application of quasidegenerate perturbation theory or the equations-of-motion method to the results of the previous two methods, we obtain addition and removal energies as well. Our results are benchmarked against full configuration interaction and diffusion Monte Carlo where available. We examine the rate of convergence and perform extrapolations to the infinite basis limit using a power-law model.

  18. Lifetime measurements using two-step laser excitation for high-lying even-parity levels and improved theoretical oscillator strengths in Y ii

    Science.gov (United States)

    Palmeri, P.; Quinet, P.; Lundberg, H.; Engström, L.; Nilsson, H.; Hartman, H.

    2017-10-01

    We report new time-resolved laser-induced fluorescence lifetime measurements for 22 highly excited even-parity levels in singly ionized yttrium (Y ii). To populate these levels belonging to the configurations 4d6s, 5s6s 4d5d, 5p2, 4d7s and 4d6d, a two-step laser excitation technique was used. Our previous pseudo-relativistic Hartree-Fock model (Biémont et al. 2011) was improved by extending the configuration interaction up to n = 10 to reproduce the new experimental lifetimes. A set of semi-empirical oscillator strengths extended to transitions falling in the spectral range λλ194-3995 nm, depopulating these 22 even-parity levels in Y ii, is presented and compared to the values found in the Kurucz's data base (Kurucz 2011).

  19. Small Atomic Orbital Basis Set First-Principles Quantum Chemical Methods for Large Molecular and Periodic Systems: A Critical Analysis of Error Sources.

    Science.gov (United States)

    Sure, Rebecca; Brandenburg, Jan Gerit; Grimme, Stefan

    2016-04-01

    In quantum chemical computations the combination of Hartree-Fock or a density functional theory (DFT) approximation with relatively small atomic orbital basis sets of double-zeta quality is still widely used, for example, in the popular B3LYP/6-31G* approach. In this Review, we critically analyze the two main sources of error in such computations, that is, the basis set superposition error on the one hand and the missing London dispersion interactions on the other. We review various strategies to correct those errors and present exemplary calculations on mainly noncovalently bound systems of widely varying size. Energies and geometries of small dimers, large supramolecular complexes, and molecular crystals are covered. We conclude that it is not justified to rely on fortunate error compensation, as the main inconsistencies can be cured by modern correction schemes which clearly outperform the plain mean-field methods.

  20. Evidence for a smooth onset of deformation in the neutron-rich Kr isotopes

    CERN Document Server

    Albers, M; Nomura, K; Blazhev, A; Jolie, J; Mucher, D; Bastin, B; Bauer, C; Bernards, C; Bettermann, L; Bildstein, V; Butterworth, J; Cappellazzo, M; Cederkall, J; Cline, D; Darby, I; Das Gupta, S; Daugas, J M; Davinson, T; De Witte, H; Diriken, J; Filipescu, D; Fiori, E; Fransen, C; Gaffney, L P; Georgiev, G; Gernhauser, R; Hackstein, M; Heinze, S; Hess, H; Huyse, M; Jenkins, D; Konki, J; Kowalczyk, M; Kroll, T; Krucken, R; Litzinger, J; Lutter, R; Marginean, N; Mihai, C; Moschner, K; Napiorkowski, P; Nara Singh, B S; Nowak, K; Otsuka, T; Pakarinen, J; Pfeiffer, M; Radeck, D; Reiter, P; Rigby, S; Robledo, L M; Rodriguez-Guzman, R; Rudigier, M; Sarriguren, P; Scheck, M; Seidlitz, M; Siebeck, B; Simpson, G; Thole, P; Thomas, T; Van de Walle, J; Van Duppen, P; Vermeulen, M; Voulot, D; Wadsworth, R; Wenander, F; Wimmer, K; Zell, K O; Zielinska, M

    2012-01-01

    The neutron-rich nuclei $^{94,96}$Kr were studied via projectile Coulomb excitation at the REX-ISOLDE facility at CERN. Level energies of the first excited 2$^{+}$ states and their absolute $E2$ transition strengths to the ground state are determined and discussed in the context of the $E(2^{+}_{1})$ and $B(E2;2^{+}_{1} \\rightarrow 0^{+}_{1})$ systematics of the krypton chain. Contrary to previously published results no sudden onset of deformation is observed. This experimental result is supported by a new proton-neutron interacting boson model calculation based on the constrained Hartree-Fock-Bogoliubov approach using the microscopic Gogny-D1M energy density functional.

  1. Collective properties of drip-line nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Hamamoto, I. [Univ. of Lund (Sweden); Sagawa, H. [Univ. of Aizu, Fukushima (Japan)

    1996-12-31

    Performing the spherical Hartree-Fock (HF) calculations with Skyrme interactions and, then, using RPA solved in the coordinate space with the Green`s function method, the authors have studied the effect of the unique shell structure as well as the very low particle threshold on collective modes in drip line nuclei. In this method a proper strength function in the continuum is obtained, though the spreading width of collective modes is not included. They have examined also one-particle resonant states in the obtained HF potential. Unperturbed particle-hole (p-h) response functions are carefully studied, which contain all basic information on the exotic behaviour of the RPA strength function in drip line nuclei.

  2. Møller Plesset evaluation of the static first hyperpolarizability of polymethineimine

    Science.gov (United States)

    Jacquemin, Denis; Champagne, Benoı̂t; André, Jean-Marie

    1998-02-01

    A finite oligomer approach is used to compute the longitudinal component of the static electronic first-hyperpolarizability per unit cell (Δ βL( N)) of polymethineimine. The longitudinal first hyperpolarizability ( β L) is calculated accounting for electron correlation effects via the Møller-Plesset partioning. The influences of the basis set size, of the order in electron-electron interactions up to which the electron correlation effects are accounted for and of the modification of the equilibrium geometry due to the inclusion of electron correlation are considered. Contrary to the Hartree-Fock level for which Δ βL( N) vs. N firstly presents a minimum then increases towards its polymeric value, at the MP2 level, Δ βL( N) evolves monotonically with chain length and its asymptotic value is 7.7 times larger than the CPHF results reaching the large value of 4.2×10 -30 esu g -1 mol.

  3. Structure factors for tunneling ionization rates of molecules

    DEFF Research Database (Denmark)

    Madsen, L.B.; Jensen, F.; Tolstikhin, O.I.

    2013-01-01

    of this factor, and hence the ionization rate, requires accurate values of the HOMO in the asymptotic region. Techniques for calculating the structure factors for molecules in the Hartree-Fock approximation are discussed. For diatomics, grid-based numerical Hartree-Fock calculations which reproduce the correct...... asymptotic tail of the HOMO are possible. However, for larger molecules, to solve the Hartree-Fock equations one should resort to basis-based approaches with too rapidly decaying Gaussian basis functions. A systematic study of the possibility to reproduce the asymptotic tail of the HOMO in calculations...

  4. Analysis of nondynamical correlation in the metal-ligand bond. Pauli repulsion and orbital localization in MnO - 4

    Science.gov (United States)

    Buijse, Marten A.; Baerends, Evert Jan

    1990-09-01

    The nondynamical correlation error in first row transition metal complexes is studied through calculations on the permanganate ion. The source of the error is the well-known Hartree-Fock failure in the weak-interaction limit, which is shown to exist for both the metal-ligand and the ligand-ligand bonds: the metal-ligand and the ligand-ligand distances are large compared to the size of the metal 3d and ligand 2p atomic orbitals (AO's). Pauli repulsion between ligand orbitals and 3s/3p orbitals prevent the metal-ligand and ligand-ligand distances to become small enough for efficient overlap and bonding. In multiply bonded systems the Hartree-Fock error does not show up in excessive electron repulsion, but leads to localization of the bonding orbitals (which sometimes requires symmetry breaking), resulting in a loss of covalent character. It is shown how, in the MnO-4 ion, the bonding electrons of E symmetry are localized on the oxygens while the T2 electrons are localized on the metal. The mechanism behind this (unphysical) localization is studied in detail, making use of a simple model system. The covalent character is reintroduced in configuration interaction or multiconfiguration self-consistent-field calculations: density is transferred from the ligand to the metal in the E bonds and vice versa in the T2 bonds. The total metal 3d occupation, however, remains unchanged. Several configuration selection schemes in the space of bonding, nonbonding, and antibonding orbitals are tested with the purpose to recover a large fraction of the nondynamical correlation error but still retain a manageable wave function. It is shown that the ``nonbonding'' O2p orbitals play an important role in the correlation process and cannot be excluded (kept closed) in a correlated calculation if quantatively correct results are required.

  5. Orbital momentum profiles and binding energy spectra for the complete valence shell of molecular fluorine

    Energy Technology Data Exchange (ETDEWEB)

    Zheng, Y.; Brion, C.E. [British Columbia Univ., Vancouver, BC (Canada). Dept. of Chemistry; Brunger, M.J.; Zhao, K.; Grisogono, A.M.; Braidwood, S.; Weigold, E. [Flinders Univ. of South Australia, Adelaide, SA (Australia). Electronic Structure of Materials Centre; Chakravorty, S.J.; Davidson, E.R. [Indiana Univ., Bloomington, IN (United States). Dept. of Chemistry; Sgamellotti, A. [Univ di Perugia (Italy). Dipartimento di Chimica; von Niessen, W. [Technische Univ. Braunschweig (Germany). Inst fuer Physikalische

    1996-01-01

    The first electronic structural study of the complete valence shell binding energy spectrum of molecular fluorine, encompassing both the outer and inner valence regions, is reported. These binding energy spectra as well as the individual orbital momentum profiles have been measured using an energy dispersive multichannel electron momentum spectrometer at a total energy of 1500 eV, with an energy resolution of 1.5 eV and a momentum resolution of 0.1 a.u. The measured binding energy spectra in the energy range of 14-60 eV are compared with the results of ADC(4) many-body Green`s function and also direct-Configuration Interaction (CI) and MRSD-CI calculations. The experimental orbital electron momentum profiles are compared with SCF theoretical profiles calculated using the target Hartree-Fock approximation with a range of basis sets and with Density Functional Theory predictions in the target Kohn-Sham approximation with non-local potentials. The truncated (aug-cc-pv5z) Dunning basis sets were used for the Density Functional Theory calculations which also include some treatment of correlation via the exchange and correlation potentials. Comparisons are also made with the full ion-neutral overlap amplitude calculated with MRSD-CI wave functions. Large, saturated basis sets (199-GTO) were employed for both the high level SCF near Hartree-Fock limit and MRSD-CI calculations to investigate the effects of electron correlation and relaxation. 66 refs., 9 tabs., 9 figs.

  6. Elementary quantum chemistry

    CERN Document Server

    Pilar, Frank L

    2003-01-01

    Useful introductory course and reference covers origins of quantum theory, Schrödinger wave equation, quantum mechanics of simple systems, electron spin, quantum states of atoms, Hartree-Fock self-consistent field method, more. 1990 edition.

  7. Properties of ground states of atomic nuclei in self-consistent theory of finite fermi-system

    Energy Technology Data Exchange (ETDEWEB)

    Sapershtejn, Eh.E.; Khodel' , V.A. (Gosudarstvennyj Komitet po Ispol' zovaniyu Atomnoj Ehnergii SSSR, Moscow. Inst. Atomnoj Ehnergii)

    1983-05-01

    Ground states of atomic nuclei are described within the framework of the self-consistent theory of finite Fermi systems. The developed approach is compared with the Hartree-Fock method with effective forces.

  8. Journal de la Recherche Scientifique de l'Universite de Lome - Vol 8 ...

    African Journals Online (AJOL)

    Etude hartree-fock de la tautomerisation du 1azirene sous pression d'hydrogene en presence du chlorure de palladium · EMAIL FULL TEXT EMAIL FULL TEXT DOWNLOAD FULL TEXT DOWNLOAD FULL TEXT. JB Mensah, AU Keuvi ...

  9. Ab-initio study of pure sup 7 sup 7 Se and sup 1 sup 2 sup 5 Te systems and of the sup 7 sup 7 Se nuclear quadrupole interaction in tellurium

    CERN Document Server

    Oh, Y K; Cho, H S

    1999-01-01

    Using the Hartree-Fock cluster procedure, we have studied the electric-field gradient tensors at the nuclear sites of sup 7 sup 7 Se and sup 1 sup 2 sup 5 Te in pure sup 1 sup 2 sup 5 Te systems and in tellurium crystalline system's with a sup 7 sup 7 Se impurity. From the results for the pure systems, sup 7 sup 7 Se in selenium and sup 1 sup 2 sup 5 Te in tellurium, using the observed quadrupole moments: Q( sup 7 sup 7 Se) 0.75 +- 0.07 barns and Q( sup 1 sup 2 sup 5 Te) = 0.35 +- 0.04 barns. Comparison is made with earlier values obtained by different methods. Using our calculated values of Q and the results of a study of the field-gradient tensors for sup 7 sup 7 Se in tellurium, the theoretical values of the quadrupole coupling constants are found to agree, within about 7 percent, with experiment. The calculated asymmetry parameters are also found to be in reasonable agreement with the experiment values, although the agreement not as close as in the case of the quadrupole -coupling constants. Directions fo...

  10. shape change in Hf, W and Os-isotopes: A non-relativistic Hartree ...

    Indian Academy of Sciences (India)

    Shape change in Hf, W and Os isotopes. 2. Formalisms. 2.1 Non-relativistic Hartree-Fock. Theoretically, the band structure of the Nilsson orbit [ЖТ3A]Ω , is studied with a well-known microscopic model, i.e., deformed Hartree-Fock and angular momentum projection [19,20]. In this calculation, axial symmetry of the ...

  11. Some properties of solid helium and helium nanoclusters using the effective HFD-like interaction potential: Adsorption and desorption inside carbon nanotube

    Science.gov (United States)

    Abbaspour, M.; Akbarzadeh, H.; Banihashemi, S. Z.; Sotoudeh, A.

    2018-02-01

    We have calculated the zero equation of state of solid helium using a two-body Hartree-Fock dispersion (HFD)-like potential from molecular dynamics (MD) simulation. To take many-body forces into account, our simple and accurate empirical expression is used with the HFD-like potential without requiring an expensive three-body calculation. This potential model also includes the quantum effects for helium at low temperatures. The results indicate that our effective HFD-like potential improves the prediction of the classical two-body results to get better agreement with experiment than many other two-body and three-body potentials of helium reported in the literature. We have also simulated the adsorption and desorption processes of the (He)55, (He)147, (He)309, (He)561, and (He)923 icosahedral nanoclusters confined into the different armchair and zigzag CNTs from 0 to 50 K using our effective model. We have observed an interesting phenomenon at 0 K for helium. The nanoclusters adsorb to the inner CNT wall as a melting process. But, the heavier noble gas clusters (such as Ne and Xe) show the different behavior than the He clusters. They form a multilayered solid structure into the CNT at zero temperature and adsorb into the inner wall of the CNT at higher temperatures. Our results for He clusters show that the absolute value of the adsorption energy increases as the size of the nanocluster increases. The desorption process begins at a certain temperature and represents itself by a jump in the configurational energy values. We have also investigated the structural and dynamical properties of the confined helium nanoclusters during the adsorption and desorption processes at different temperatures.

  12. Hyperons in dense matter

    Energy Technology Data Exchange (ETDEWEB)

    Dapo, Haris

    2009-01-28

    The hyperon-nucleon YN low momentum effective interaction (V{sub low} {sub k}) allows for an extensive study of the behavior of hyperons in dense matter, together with an investigation of effects of the presence of hyperons on dense matter. The first step towards this goal is the construction of the matrix elements for the hyperon-nucleon low momentum potential. In order to assess the different properties of hyperons within these potentials we calculate the hyperon single-particle potentials in the Hartree-Fock approximation for all of the interactions. Their dependence on both momentum and density, is studied. The single-particle potentials are then used to determine the chemical potential of hyperons in neutron stars. For nucleonic properties, the nucleon-nucleon V{sub low} {sub k} can be used with the caveat that the calculation of the ground-state energy of symmetric nuclear matter does not correctly reproduce the properties of matter at saturation. With the nucleon-nucleon V{sub low} {sub k} one is unable to reach the densities needed for the calculation of neutron star masses. To circumvent this problem we use two approaches: in the first one, we parametrize the entire nucleonic sector. In the second one, we replace only the three-body force. The former will enable us to study neutron star masses, and the latter for studying the medium's response to the external probe. In this thesis we take the external probe to be the neutrino. By combining this parametrization with the YN V{sub low} {sub k} potential, we calculate the equation of state of equilibrated matter. Performing the calculation in the Hartree-Fock approximation at zero temperature, the concentrations of all particles are calculated. From these we can ascertain at which densities hyperons appear for a wide range of parameters. Finally, we calculate the masses of neutron stars with these concentrations. For the calculation of the medium's response to an external probe, we replace the three

  13. Organic adsorbates on metal surfaces. PTCDA and NTCDA on AG(110)

    Energy Technology Data Exchange (ETDEWEB)

    Abbasi, Afshin

    2010-02-22

    Polyaromatic molecules functionalized with carboxylic groups have served as model systems for the growth of organic semiconducting films on a large variety of substrates. Most non-reactive substrates allow for a growth mode compatible with the bulk phase of the molecular crystal with two molecules in the unit cell, but some more reactive substrates including Ag(111) and Ag(110) can induce substantial changes in the first monolayer (ML). In the specific case of Ag(110), the adsorbate unit cell of both NTCDA and PTCDA resembles a brickwall structure, with a single molecule in the unit cell. From this finding, it can be concluded that the adsorbate-substrate interaction is stronger than typical inter-molecular binding energies in the respective bulk phases. In the present work, the interactions between small Ag(110) clusters and a single NTCDA or PTCDA molecule are investigated with different ab initio techniques. Four major ingredients contribute to the binding between adsorbate and substrate: Directional bonds between Ag atoms in the topmost layer and the oxygen atoms of the molecule, Pauli repulsion between filled orbitals of molecule and substrate, an attractive van-der-Waals interaction, and a negative net charge on the molecule inducing positive image charges in the substrate, resulting therefore in an attractive Coulomb interaction between these opposite charges. As both Hartree-Fock theory and density functional theory with typical gradient-corrected density functional do not contain any long range correlation energy required for dispersion interactions, we compare these approaches with the fastest numerical technique where the leading term of the van-der-Waals interaction is included, i.e. second order Moeller-Plesset theory (MP2). Both Hartree-Fock and density functional theory result in bended optimized geometries where the adsorbate is interacting mainly via the oxygen atoms, with the core of the molecule repelled from the substrate. Only at the MP2 level

  14. Interactive numerals

    Science.gov (United States)

    2017-01-01

    Although Arabic numerals (like ‘2016’ and ‘3.14’) are ubiquitous, we show that in interactive computer applications they are often misleading and surprisingly unreliable. We introduce interactive numerals as a new concept and show, like Roman numerals and Arabic numerals, interactive numerals introduce another way of using and thinking about numbers. Properly understanding interactive numerals is essential for all computer applications that involve numerical data entered by users, including finance, medicine, aviation and science. PMID:28484609

  15. Towards Efficient and Accurate Description of Many-Electron Problems: Developments of Static and Time-Dependent Electronic Structure Methods

    Science.gov (United States)

    Ding, Feizhi

    Understanding electronic behavior in molecular and nano-scale systems is fundamental to the development and design of novel technologies and materials for application in a variety of scientific contexts from fundamental research to energy conversion. This dissertation aims to provide insights into this goal by developing novel methods and applications of first-principle electronic structure theory. Specifically, we will present new methods and applications of excited state multi-electron dynamics based on the real-time (RT) time-dependent Hartree-Fock (TDHF) and time-dependent density functional theory (TDDFT) formalism, and new development of the multi-configuration self-consist field theory (MCSCF) for modeling ground-state electronic structure. The RT-TDHF/TDDFT based developments and applications can be categorized into three broad and coherently integrated research areas: (1) modeling of the interaction between moleculars and external electromagnetic perturbations. In this part we will first prove both analytically and numerically the gauge invariance of the TDHF/TDDFT formalisms, then we will present a novel, efficient method for calculating molecular nonlinear optical properties, and last we will study quantum coherent plasmon in metal namowires using RT-TDDFT; (2) modeling of excited-state charge transfer in molecules. In this part, we will investigate the mechanisms of bridge-mediated electron transfer, and then we will introduce a newly developed non-equilibrium quantum/continuum embedding method for studying charge transfer dynamics in solution; (3) developments of first-principles spin-dependent many-electron dynamics. In this part, we will present an ab initio non-relativistic spin dynamics method based on the two-component generalized Hartree-Fock approach, and then we will generalized it to the two-component TDDFT framework and combine it with the Ehrenfest molecular dynamics approach for modeling the interaction between electron spins and nuclear

  16. Floor interaction

    DEFF Research Database (Denmark)

    Petersen, Marianne Graves; Krogh, Peter; Ludvigsen, Martin

    2005-01-01

    Within architecture, there is a long tradition of careful design of floors. The design has been concerned with both decorating floors and designing floors to carry information. Ubiquitous computing technology offers new opportunities for designing interactive floors. This paper presents three...... different interactive floor concepts. Through an urban perspective it draws upon the experiences of floors in architecture, and provides a set of design issues for designing interactive floors....

  17. Interactive Timetabling

    OpenAIRE

    Muller, Tomas; Bartak, Roman

    2001-01-01

    Timetabling is a typical application of constraint programming whose task is to allocate activities to slots in available resources respecting various constraints like precedence and capacity. In this paper we present a basic concept, a constraint model, and the solving algorithms for interactive timetabling. Interactive timetabling combines automated timetabling (the machine allocates the activities) with user interaction (the user can interfere with the process of timetabling). Because the ...

  18. Playful Interaction

    DEFF Research Database (Denmark)

    2003-01-01

    The video Playful Interaction describes a future architectural office, and envisions ideas and concepts for playful interactions between people, materials and appliances in a pervasive and augmented working environment. The video both describes existing developments, technologies and designs...... as well as ideas not yet implemented such as playful modes of interaction with an augmented ball. Playful Interaction has been used as a hybrid of a vision video and a video prototype (1). Externally the video has been used to visualising our new ideas, and internally the video has also worked to inspire...

  19. Description of Weak Halogen Bonding Using Various Levels of Symmetry-Adapted Perturbation Theory Combined with Effective Core Potentials

    Directory of Open Access Journals (Sweden)

    Piotr Matczak

    2017-01-01

    Full Text Available The present work starts with providing a description of the halogen bonding (XB interaction between the halogen atom of MH3X (where M = C–Pb and X = I, At and the N atom of HCN. This interaction leads to the formation of stable yet very weakly bound MH3X⋯NCH complexes for which the interaction energy (Eint between MH3X and HCN is calculated using various symmetry-adapted perturbation theory (SAPT methods combined with the def2-QZVPP basis set and midbond functions. This basis set assigns effective core potentials (ECPs not only to the I or At atom directly participating in the XB interaction with HCN but also to the M atom when substituted with Sn or Pb. Twelve SAPT methods (or levels are taken into consideration. According to the SAPT analysis of Eint, the XB interaction in the complexes shows mixed electrostatic-dispersion nature. Next, the accuracy of SAPT Eint is evaluated by comparing with CCSD(T reference data. This comparison reveals that high-order SAPT2+(3 method and the much less computationally demanding SAPT(DFT method perform very well in describing Eint of the complexes. However, the accuracy of these methods decreases dramatically if they are combined with the so-called Hartree-Fock correction.

  20. Symmetry breaking and quantum correlations in finite systems: studies of quantum dots and ultracold Bose gases and related nuclear and chemical methods

    Science.gov (United States)

    Yannouleas, Constantine; Landman, Uzi

    2007-12-01

    Investigations of emergent symmetry breaking phenomena occurring in small finite-size systems are reviewed, with a focus on the strongly correlated regime of electrons in two-dimensional semiconductor quantum dots and trapped ultracold bosonic atoms in harmonic traps. Throughout the review we emphasize universal aspects and similarities of symmetry breaking found in these systems, as well as in more traditional fields like nuclear physics and quantum chemistry, which are characterized by very different interparticle forces. A unified description of strongly correlated phenomena in finite systems of repelling particles (whether fermions or bosons) is presented through the development of a two-step method of symmetry breaking at the unrestricted Hartree-Fock level and of subsequent symmetry restoration via post Hartree-Fock projection techniques. Quantitative and qualitative aspects of the two-step method are treated and validated by exact diagonalization calculations. Strongly-correlated phenomena emerging from symmetry breaking include the following. Chemical bonding, dissociation and entanglement (at zero and finite magnetic fields) in quantum dot molecules and in pinned electron molecular dimers formed within a single anisotropic quantum dot, with potential technological applications to solid-state quantum-computing devices. Electron crystallization, with particle localization on the vertices of concentric polygonal rings, and formation of rotating electron molecules (REMs) in circular quantum dots. Such electron molecules exhibit ro-vibrational excitation spectra, in analogy with natural molecules. At high magnetic fields, the REMs are described by parameter-free analytic wave functions, which are an alternative to the Laughlin and composite-fermion approaches, offering a new point of view of the fractional quantum Hall regime in quantum dots (with possible implications for the thermodynamic limit). Crystalline phases of strongly repelling bosons. In rotating

  1. Interactive benchmarking

    DEFF Research Database (Denmark)

    Lawson, Lartey; Nielsen, Kurt

    2005-01-01

    We discuss individual learning by interactive benchmarking using stochastic frontier models. The interactions allow the user to tailor the performance evaluation to preferences and explore alternative improvement strategies by selecting and searching the different frontiers using directional...... in the suggested benchmarking tool. The study investigates how different characteristics on dairy farms influences the technical efficiency....

  2. Kinesthetic Interaction

    DEFF Research Database (Denmark)

    Fogtmann, Maiken Hillerup; Fritsch, Jonas; Kortbek, Karen Johanne

    2008-01-01

    Within the Human-Computer Interaction community there is a growing interest in designing for the whole body in interaction design. The attempts aimed at addressing the body have very different outcomes spanning from theoretical arguments for understanding the body in the design process, to more...... practical examples of designing for bodily potential. This paper presents Kinesthetic Interaction as a unifying concept for describing the body in motion as a foundation for designing interactive systems. Based on the theoretical foundation for Kinesthetic Interaction, a conceptual framework is introduced...... to reveal bodily potential in relation to three design themes – kinesthetic development, kinesthetic means and kinesthetic disorder; and seven design parameters – engagement, sociality, movability, explicit motivation, implicit motivation, expressive meaning and kinesthetic empathy. The framework is a tool...

  3. Aesthetic Interaction

    DEFF Research Database (Denmark)

    Ludvigsen, Martin; Petersen, M.G.; Iversen, O.

    2004-01-01

    There is a growing interest in considering aesthetic aspects in the design of interactive systems. A set of approaches are emerging each representing different applications of the terminology as well as different inherent assumptions on the role of the user, designer and interaction ideals....... In this paper, we use the concept of Pragmatist Aesthetics to provide a framework for distinguishing between different approaches to aesthetics. Moreover, we use our own design cases to illustrate how pragmatist aesthetics is a promising path to follow in the context of designing interactive systems......, as it promotes aesthetics of use, rather than aesthetics of appearance. We coin this approach in the perspective of aesthetic interaction. Finally we make the point that aesthetics is not re-defining everything known about interactive systems. We provide a framework placing this perspective among other...

  4. Generalized Nambu-Jona-Lasinio model in flavour SU(3): Development and application. Verallgemeinertes Nambu-Jona-Lasinio-Modell in Flavour-SU(3): Entwicklung und Anwendung

    Energy Technology Data Exchange (ETDEWEB)

    Klimt, S.

    1989-12-19

    In this thesis the author tried to decribe important low-energy phenomena of the strong interactions by means of the Nambu-Jona-Lasinio model. The effective quark-quark interaction was thereby constructed in accordance with the basing symmetries and conserved currents of the QCD; the model possesses especially chiral SU(3){sub L} x SU(3){sub R} symmetry. In the framework of this approach properties of the quarks and the light mesons were studied. In the calculations for instance the Hartree-Fock approach for the quark propagator was used. Properties of the mesons were determined in the framework of a RPA calculation by solution of the Bethe-Salpeter equation for the quark-antiquark scattering matrix. All questions, which were treated here, concern aspects of the symmetry breaking of the QCD: At the one hand the explicit breaking of the chiral symmetry by finite, if also small quark current masses. Thereby was assumed that these can be described as low perturbation of the chiral limit of massless quarks; furthermore the breaking of the U(1){sub A} symmetry observed in nature. It was tried to regard this anomaly property of the QCD by an additional flavor-mixing and U(1){sub A} breaking determinant interaction. The last and most important point finally is the spontaneous breaking of the chiral symmetry and the generation of quark condensates in the QCD ground state by the interaction dynamics. (orig./HSI).

  5. Massive neutron star with strangeness in a relativistic mean-field model with a high-density cutoff

    Science.gov (United States)

    Zhang, Ying; Hu, Jinniu; Liu, Peng

    2018-01-01

    The properties of neutron stars with the strangeness degree of freedom are studied in the relativistic mean-field (RMF) model via including a logarithmic interaction as a function of the scalar meson field. This interaction, named the σ -cut potential, can largely reduce the attractive contributions of the scalar meson field at high density without any influence on the properties of nuclear structure around the normal saturation density. In this work, the TM1 parameter set is chosen as the RMF interaction, while the strengths of σ -cut potential are constrained by the properties of finite nuclei so that we can obtain a reasonable effective nucleon-nucleon interaction. The hyperons Λ ,Σ , and Ξ are considered in neutron stars within this framework, whose coupling constants with mesons are determined by the latest hyperon-nucleon and Λ -Λ potentials extracted from the available experimental data of hypernuclei. The maximum mass of neutron star can be larger than 2 M⊙ with these hyperons in the present framework. Furthermore, the nucleon mass at high density will be saturated due to this additional σ -cut potential, which is consistent with the conclusions obtained by other calculations such as Brueckner-Hartree-Fock theory and quark mean-field model.

  6. Programming Interactivity

    CERN Document Server

    Noble, Joshua

    2012-01-01

    Ready to create rich interactive experiences with your artwork, designs, or prototypes? This is the ideal place to start. With this hands-on guide, you'll explore several themes in interactive art and design-including 3D graphics, sound, physical interaction, computer vision, and geolocation-and learn the basic programming and electronics concepts you need to implement them. No previous experience is necessary. You'll get a complete introduction to three free tools created specifically for artists and designers: the Processing programming language, the Arduino microcontroller, and the openFr

  7. Application of the weak-field asymptotic theory to the analysis of tunneling ionization of linear molecules

    DEFF Research Database (Denmark)

    Madsen, Lars Bojer; Tolstikhin, Oleg I.; Morishita, Toru

    2012-01-01

    The recently developed weak-field asymptotic theory [ Phys. Rev. A 84 053423 (2011)] is applied to the analysis of tunneling ionization of a molecular ion (H2+), several homonuclear (H2, N2, O2) and heteronuclear (CO, HF) diatomic molecules, and a linear triatomic molecule (CO2) in a static...... Hartree-Fock wave functions for the diatomics, and a Hartree-Fock quantum chemistry wave function for CO2. The structure factors are expanded in terms of standard functions and the associated structure coefficients, allowing the determination of the ionization rate for any orientation of the molecule...... with respect to the field, are tabulated. Our results, which are exact in the weak-field limit for H2+ and, in addition, under the Hartree-Fock approximation for the diatomics, are compared with results from the recent literature....

  8. Electron correlation within the relativistic no-pair approximation

    DEFF Research Database (Denmark)

    Almoukhalalati, Adel; Knecht, Stefan; Jensen, Hans Jørgen Aa

    2016-01-01

    This paper addresses the definition of correlation energy within 4-component relativistic atomic and molecular calculations. In the nonrelativistic domain the correlation energy is defined as the difference between the exact eigenvalue of the electronic Hamiltonian and the Hartree-Fock energy...... electronic Hamiltonian, the Dirac-Coulomb Hamiltonian, has no bound solutions. Present-day relativistic calculations are carried out within the no-pair approximation, where the Dirac-Coulomb Hamiltonian is embedded by projectors eliminating the troublesome negative-energy solutions. Hartree-Fock calculations...... are carried out with the implicit use of such projectors and only positive-energy orbitals are retained at the correlated level, meaning that the Hartree-Fock projectors are frozen at the correlated level. We argue that the projection operators should be optimized also at the correlated level...

  9. Measurements of fluorescence and Coster-Kronig yields for 66Dy using synchrotron radiation induced selective photoionization method

    Science.gov (United States)

    Kaur, Rajnish; Kumar, Anil; Czyzycki, M.; Migliori, A.; Karydas, A. G.; Puri, Sanjiv

    2017-09-01

    The L shell fluorescence (ω1, ω2, ω3) and Coster-Kronig (f12, f13, f23) yields for 66Dy have been deduced from the Li (i = 1-3) sub-shell X-ray intensities measured at different incident photon energies across its Li absorption edge energies. Three sets of photoionization cross sections used for determination of these yields include two sets of theoretical values based on the non-relativistic Hartree-Fock-Slater model and the self-consistent Dirac-Hartree-Fock model, and the third one is that deduced from independently measured mass attenuation coefficients of 66Dy. The present experimental fluorescence and Coster-Kronig yields deduced using the self-consistent Dirac-Hartree-Fock model based photoionization cross sections have been found to be in good agreement with the semi-empirical values tabulated by Krause [1] and the Dirac-Hartree-Slater model based values.

  10. The role of electron correlations in the binding properties of Ca, Sr, and Ba

    Energy Technology Data Exchange (ETDEWEB)

    Belger, Dennis; Huesges, Zita; Voloshina, Elena; Paulus, Beate, E-mail: velena@chemie.fu-berlin.d [Institut fuer Chemie und Biochemie-Physikalische und Theoretische Chemie, Freie Universitaet Berlin, Takustrasse 3, 14195 Berlin (Germany)

    2010-07-14

    In order to apply wavefunction-based correlation methods to solids it is necessary to have reliable Hartree-Fock (HF) results for the infinite system of interest. We performed Hartree-Fock calculations for the group 2 heavy alkali-earth metals Ca, Sr, and Ba. For that, basis sets of valence-double-{zeta} quality have been optimized for the periodic systems. In all cases small-core pseudopotentials were used to deal with the scalar-relativistic effects. We determine the cohesive energies, the equilibrium volumes and the bulk moduli of the systems at the Hartree-Fock level and compare them with experimental data as well as the results of density functional theory calculations. Relativistic effects in the case of Ba are estimated by using a non-relativistic pseudopotential. The comparative HF versus the density functional theory (DFT) study of the electronic structures of Ca, Sr, and Ba has been performed.

  11. Interaction graphs

    DEFF Research Database (Denmark)

    Seiller, Thomas

    2016-01-01

    Interaction graphs were introduced as a general, uniform, construction of dynamic models of linear logic, encompassing all Geometry of Interaction (GoI) constructions introduced so far. This series of work was inspired from Girard's hyperfinite GoI, and develops a quantitative approach that should...... be understood as a dynamic version of weighted relational models. Until now, the interaction graphs framework has been shown to deal with exponentials for the constrained system ELL (Elementary Linear Logic) while keeping its quantitative aspect. Adapting older constructions by Girard, one can clearly define...... "full" exponentials, but at the cost of these quantitative features. We show here that allowing interpretations of proofs to use continuous (yet finite in a measure-theoretic sense) sets of states, as opposed to earlier Interaction Graphs constructions were these sets of states were discrete (and finite...

  12. Embarrassing Interactions

    DEFF Research Database (Denmark)

    Deterding, Sebastian; Lucero, Andrés; Holopainen, Jussi

    2015-01-01

    Wherever the rapid evolution of interactive technologies disrupts standing situational norms, creates new, often unclear situational audiences, or crosses cultural boundaries, embarrassment is likely. This makes embarrassment a fundamental adoption and engagement hurdle, but also a creative desig...... space for human-computer interaction. However, research on embarrassment in HCI has remained scattered and unsystematic so far. This workshop therefore convenes researchers and practitioners to assemble and advance the current state of research on embarrassing interactions.......Wherever the rapid evolution of interactive technologies disrupts standing situational norms, creates new, often unclear situational audiences, or crosses cultural boundaries, embarrassment is likely. This makes embarrassment a fundamental adoption and engagement hurdle, but also a creative design...

  13. Pairing correlations in an explicitly particle-number conserving approach

    CERN Document Server

    Pillet, N; Libert, J

    2002-01-01

    A method to treat pairing correlations in an explicitly particle-number conserving approach is proposed and discussed. It appears to be both tractable and reliable while using state of the art effective interactions, e.g. of the Skyrme type, for the particle-hole matrix elements. It corresponds to a highly truncated shell-model calculation approach. Its fast convergence in the particle-hole basis is due to the use of single-particle states stemming from an Hartree-Fock-like mean field defined from a one-body density matrix including self-consistently the one-body effect of the correlations. Results obtained in an non-fully consistent fashion, in that the residual interaction is mocked up by a delta interaction, are presented. They mainly confirm most of the physical properties underlying the BCS-like solutions, in particular the paramount importance of pair transfers. However in weak pairing situations, e.g. near subshell- or shell-closures, they provide a microscopic description quite at variance with the us...

  14. Computational investigation and synthesis of a sol-gel imprinted material for sensing application of some biologically active molecules

    Energy Technology Data Exchange (ETDEWEB)

    Atta, Nada F., E-mail: Nada_fah1@yahoo.com [Department of Chemistry, Faculty of Science, University of Cairo, Post Code 12613, Giza (Egypt); Hamed, Maher M.; Abdel-Mageed, Ali M. [Department of Chemistry, Faculty of Science, University of Cairo, Post Code 12613, Giza (Egypt)

    2010-05-14

    A hybrid sol-gel material was molecularly imprinted with a group of neurotransmitters. Imprinted material is a sol-gel thin film that is spin coated on the surface of a glassy carbon electrode. Imprinted films were characterized electrochemically using cyclic voltammetry (CV) and the encapsulated molecules were extracted from the films and complementary molecular cavities are formed that enable their rebind. The films were tested in their corresponding template solutions for rebinding using square wave voltammetry (SWV). Computational approach for exploring the primary intermolecular forces between templates and hydrolyzed form of the precursor monomer, tetraethylorthosilicate (TEOS), were carried out using Hartree-Fock method (HF). Interaction energy values were computed for each adduct formed between a monomer and a template. Analysis of the optimized conformations of various adducts could explain the mode of interaction between the templates and the monomer units. We found that interaction via the amino group is the common mode among the studied compounds and the results are in good agreement with the electrochemical measurements.

  15. High spin exotic states and new method for pairing energy; Etats exotiques a hauts spins et nouvelle methode pour l`energie d`appariement nucleaire

    Energy Technology Data Exchange (ETDEWEB)

    Molique, H.

    1996-01-19

    We present a new method called `PSY-MB`, initially developed in the framework of abstract group theory for the solution of the problem of strongly interacting multi-fermionic systems with particular to systems in an external rotating field. The validity of the new method (PSY-MB) is tested on model Hamiltonians. A detailed comparison between the obtained solutions and the exact ones is performed. The new method is used in the study of realistic nuclear Hamiltonians based on the Woods-Saxon potential within the cranking approximation to study the influence of residual monopole pairing interactions in the rare-earth mass region. In parallel with this new technique we present original results obtained with the Woods-Saxon mean-field and the self-consistent Hartree-Fock approximation in order to investigate such exotic effects as octupole deformations and hexadecapole C{sub 4}-polarizing deformations in the framework of high-spin physics. By developing these three approaches in one single work we prepare the ground for the nuclear structure calculations of the new generation - where the residual two-body interactions are taken into account also in the weak pairing limit. (author). 2370refs.

  16. Intuitive Understanding of σ Delocalization in Loose and σ Localization in Tight Helical Conformations of an Oligosilane Chain.

    Science.gov (United States)

    Jovanovic, Milena; Antic, Dean; Rooklin, David; Bande, Annika; Michl, Josef

    2017-06-01

    Conformational effects on the σ-electron delocalization in oligosilanes are addressed by Hartree-Fock and time-dependent density functional theory calculations (B3LYP, 6-311G**) at MP2 optimized geometries of permethylated uniformly helical linear oligosilanes (all-ω-Sin R2n+2 ) up to n=16 and for backbone dihedral angles ω=55-180°. The extent of σ delocalization is judged by the partition ratio of the highest occupied molecular orbital and is reflected in the dependence of its shape and energy and of UV absorption spectra on n. The results agree with known spectra of all-transoid loose-helix conformers (all-[±165]-Sin Me2n+2 ) and reveal a transition at ω≈90° from the "σ-delocalized" limit at ω=180° toward and close to the physically non-realizable "σ-localized" tight-helix limit ω=0 with entirely different properties. The distinction is also obtained in the Hückel Ladder H and C models of σ delocalization. An easy intuitive way to understand the origin of the two contrasting limits is to first view the linear chain as two subchains with alternating primary and vicinal interactions (σ hyperconjugation), one consisting of the odd and the other of the even σ(SiSi) bonds, and then allow the two subchains to interact by geminal interactions (σ conjugation). © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  17. Interaction Widget

    DEFF Research Database (Denmark)

    Ingstrup, Mads

    2003-01-01

    This pattern describes the idea of making a user interface of discrete, reusable entities---here called interaction widgets. The idea behind widgets is described using two perspectives, that of the user and that of the developer. It is the forces from these two perspectives that are balanced...... in the pattern. The intended audience of the pattern is developers and researchers within the field of human computer interaction....

  18. A benchmark study for the crown-type splashing dynamics of one- and two-component droplet wall-film interactions

    Science.gov (United States)

    Geppert, A.; Terzis, A.; Lamanna, G.; Marengo, M.; Weigand, B.

    2017-12-01

    The present paper investigates experimentally the impact dynamics of crown-type splashing for miscible two- and one-component droplet wall-film interactions over a range of Weber numbers and dimensionless film thicknesses. The splashing outcome is parametrised in terms of a set of quantifiable parameters, such as crown height, top and base diameter, wall inclination, number of fingers, and secondary droplet properties. The results show that the outcome of a splashing event is not affected by the choice of similar or dissimilar fluids, provided the dimensionless film thickness is larger than 0.1. Below this threshold, distinctive features of two-component interactions appear, such as hole formation and crown bottom breakdown. The observation of different crown shapes (e.g. V-shaped, cylindrical, and truncated-cone) confirms that vorticity production induces changes in the crown wall inclination, thus affecting the evolution of the crown height and top diameter. The evolution of the crown base diameter, instead, is mainly dependent on the relative importance of liquid inertia and viscous losses in the wall-film. The maximum number of liquid fingers decreases with increasing wall, film thickness, due to the enhanced attenuation of the effect of surface properties on the fingering process. The formation of secondary droplets is also affected by changes in the crown wall inclination. In particular, for truncated-cone shapes the occurrence of crown rim contraction induces a large scatter in the secondary droplet properties. Consequently, empirical models for the maximum number and mean diameter of the secondary droplets are derived for V-shaped crowns, as observed for the hexadecane-Hyspin interactions.

  19. The Parametrisation of Legal Terminology Concerning Child Maintenance Support in the Swedish and Polish Legal Systems

    Directory of Open Access Journals (Sweden)

    Hadryan Milena

    2017-03-01

    Full Text Available This paper deals with translating legal terminology concerning child maintenance from Polish to Swedish. The analysis covers selected terms regulated in the Polish civil law and their possible Swedish equivalents. The method used is based on the parameterisation of legal terms, which allows the specification of terms by selected parameters, which are understood as mutually exclusive properties. The parameterised equivalents are analysed in the context of various types of recipients. This provides the basis for the choice of appropriate translation strategies. The author also discusses pragmatic equivalents featured in Rikstermbanken, the Swedish national terminological database, and those used in practice.

  20. Fast simulation options in LHCb from ReDecay to fully parametrised

    CERN Multimedia

    Muller, Dominik

    2017-01-01

    With the steady increase in the precision of flavour physics measurements with data from Run 2 of the LHC, the LHCb experiment requires simulated data samples of ever increasing magnitude to study the detector response in detail. However, relying on an increase of computing resources available for the production of simulated samples will not suffice to achieve this goal. Therefore, multiple efforts are currently being investigated to reduce the time needed to simulate an event. This talk presents a summary of those efforts in LHCb, focusing on the newest developments: re-using parts of previously simulated events and a fully parametric detector description using the DELPHES framework. The former merges a simulation of an underlying event multiple times with signal decays simulated separately, achieving an order of magnitude increase in speed with identical precision. The latter provides a parametric solution replacing the full, GEANT4-based simulation, including the smearing of particles' energies, efficienci...

  1. Mediation in Different Areas of Chinese Legal Reality – Parametrisation of Selected Terminology

    Directory of Open Access Journals (Sweden)

    Grzybek Joanna

    2016-06-01

    Full Text Available The paper deals with terminological issues in legal translation. The author has researched the process of establishing equivalents for partially equivalent terminology, using the parametrical approach to legal translation. The research consists of the terminological analysis of the texts of mediation regulations formulated in Chinese and Polish. The objective was to establish translational equivalents in the case of significant differences between the legal systems of the above mentioned linguistic area. The research was financed from the research grant no. 2012/07/E/HS2/00678, titled: Parameterisation of legilinguistic translatology in the scope of civil law and civil procedure awarded by the National Science Centre of the Republic of Poland (Sonata Bis program.

  2. A combined experimental (IR, Raman and UV-Vis) and quantum chemical study of canadine

    Science.gov (United States)

    Joshi, Bhawani Datt; Srivastava, Anubha; Tandon, Poonam; Jain, Sudha; Ayala, A. P.

    2018-02-01

    Plant based natural products cover a major sector of the medicinal field, as such focus on plant research has been increased all over the world. As an attempt to aid that research, we have performed structural and spectroscopic analysis of a natural product, an alkaloid: canadine. Both ab initio Hartree-Fock (HF) and density functional theory (DFT) employing B3LYP using 6-311 ++G(d,p) basis set were used for the calculations. The calculated vibrational frequencies were scaled and compared with the experimental infrared and Raman spectra. The complete vibrational assignments were made using potential energy distribution. The structure-activity relation has also been interpreted by mapping electrostatic potential surface and evaluating the reactivity descriptors, which are valuable information for quality control of medicines and drug-receptor interactions. Natural bond orbital analysis has also been performed to understand the stability and hyperconjugative interactions of the molecule. Furthermore, UV-Vis spectra have been recorded in an ethanol solvent (EtOH) and the electronic property has been analyzed employing TD-DFT for both gaseous and solvent phase. The HOMO and LUMO calculation with their energy gap show that charge transfer occurs within the molecule. Additionally, the nonlinear optical properties of the title compound have been interpreted that predicts it's the best candidate for the NLO materials.

  3. Transport and current noise characteristics of a T-shape double-quantum-dot system

    Energy Technology Data Exchange (ETDEWEB)

    Brown, K; Tifrea, I [Department of Physics and Astronomy, California State University, Fullerton, CA 92834 (United States); Crisan, M [Department of Theoretical Physics, ' Babes-Bolyai' University, 40084 Cluj-Napoca (Romania)

    2009-05-27

    We consider the transport and the noise characteristics for the case of a T-shape double-quantum-dot system using the equation of motion method. Our theoretical results, obtained in an approximation equivalent to the Hartree-Fock approximation, account for non-zero on-site Coulomb interaction in both the detector and side dots. The existence of a non-zero Coulomb interaction implies an additional two resonances in the detector's dot density of states and thereafter affects the electronic transport properties of the system. The system's conductance presents two Fano dips as a function of the energy of the localized electronic level in the side dot. The Fano dips in the system's conductance can be observed for both strong (fast detector) and weak coupling (slow detector) between the detector dot and the external electrodes. Due to stronger electronic correlations, the noise characteristics in the case of a slow detector are much higher. This setup may be of interest for the practical realization of qubit states in quantum dot systems.

  4. Propagation of neutrinos in nuclear matter; Effets du milieu sur la propagation des neutrinos dans la matiere nucleaire

    Energy Technology Data Exchange (ETDEWEB)

    Margueron, J

    2001-07-01

    We study the elementary interactions between neutrinos and dense matter in a proto-neutron star. Equations of state obtained with different nuclear effective interactions (Skyrme, Gogny, Relativistic Lagrangians) are first discussed. Then, we characterize their stability in spin and isospin. We derive magnetic susceptibilities for all isospin asymmetry values as a function of Landau parameters G{sup {pi}}{sup {pi}}{sup '}{sub 0} (where {pi}, {pi}' = proton or neutron). From this work, we select a parametrization for each of the 3 effective forces: Sly230b,D1P,NL3. We calculate the pure neutron matter and asymmetric nuclear matter response functions with and without charge exchange, describing nuclear correlations in both approaches: non-relativistic (Hartree-Fock with Skyrme forces, then complete RPA) and relativistic (in the Hartree approximation). At the end, we calculate neutrino mean free paths neutral current and charged current reactions. Comparisons between relativistic and non-relativistic approaches allow us to identify relativistic effects in nuclear matter at densities as low as twice the saturation density. RPA correlations make the medium more transparent to neutrinos compared to free Fermi gas. The importance of the effective mass in mean free path calculations is also shown. (author)

  5. Spectroscopic, quantum mechanical and molecular docking studies of a new benzoxazole compound with an oxidoreductase enzyme and DNA

    Science.gov (United States)

    Zeyrek, Celal Tuğrul; Boyacioglu, Bahadir; Temiz-Arpaci, Özlem; Ünver, Hüseyin; Elmali, Ayhan

    2017-05-01

    The spectroscopic, theoretical molecular structure, full vibrational band assignments, MEP, NBO, frontier molecular orbitals, and NLO effects, and molecular docking studies of 5-ethylsulphonyl-2-(p-ethylphenyl)-benzoxazole, C17H17SO3N, (L) have been presented in this work. The quantum mechanical calculations have been performed by using the Hartree-Fock (HF)/6-311++G(d,p) and density functional theory (DFT) with the B3LYP/6-311++G(d,p) levels. Calculated vibrational frequencies have been compared with the experimental FT-IR spectra. The natural bond orbital (NBO) analysis has been performed to determine the hyper conjugative interactions. Frontier molecular orbitals have been defined to predict the chemical parameters of the L. The first order hyperpolarizability of L was calculated to find its role in nonlinear optics. Molecular docking of L with the oxidoreductase enzyme nicotinamide adenine dinucleotide phosphate (NADPH) exhibited the good binding affinity with energy of -8.8 kcal/mol. The molecular docking was also done to identify the interaction of L with the DNA.

  6. Numerical results on the short-range spin correlation functions in the ground state of the two-dimensional Hubbard model

    Science.gov (United States)

    Qin, Mingpu; Shi, Hao; Zhang, Shiwei

    2017-08-01

    Optical lattice experiments with ultracold fermion atoms and quantum gas microscopy have recently realized direct measurements of magnetic correlations at the site-resolved level. We calculate the short-range spin-correlation functions in the ground state of the two-dimensional repulsive Hubbard model with the auxiliary-field quantum Monte Carlo (AFQMC) method. The results are numerically exact at half filling where the fermion sign problem is absent. Away from half filling, we employ the constrained path AFQMC approach to eliminate the exponential computational scaling from the sign problem. The constraint employs unrestricted Hartree-Fock trial wave functions with an effective interaction strength U , which is optimized self-consistently within AFQMC. Large supercells are studied, with twist averaged boundary conditions as needed, to reach the thermodynamic limit. We find that the nearest-neighbor spin correlation always increases with the interaction strength U , contrary to the finite-temperature behavior where a maximum is reached at a finite U value. We also observe a change of sign in the next-nearest-neighbor spin correlation with increasing density, which is a consequence of the buildup of the long-range antiferromagnetic correlation. We expect the results presented in this paper to serve as a benchmark as lower temperatures are reached in ultracold atom experiments.

  7. Vibrational properties of organic donor-acceptor molecular crystals: Anthracene-pyromellitic-dianhydride (PMDA) as a case study

    KAUST Repository

    Fonari, A.

    2015-12-10

    We establish a reliable quantum-mechanical approach to evaluate the vibrational properties of donor-acceptor molecular crystals. The anthracene-PMDA (PMDA = pyromellitic dianhydride) crystal, where anthracene acts as the electron donor and PMDA as the electron acceptor, is taken as a representative system for which experimental non-resonance Raman spectra are also reported. We first investigate the impact that the amount of nonlocal Hartree-Fock exchange (HFE) included in a hybrid density functional has on the geometry, normal vibrational modes, electronic coupling, and electron-vibrational (phonon) couplings. The comparison between experimental and theoreticalRaman spectra indicates that the results based on the αPBE functional with 25%-35% HFE are in better agreement with the experimental results compared to those obtained with the pure PBE functional. Then, taking αPBE with 25% HFE, we assign the vibrational modes and examine their contributions to the relaxation energy related to the nonlocal electron-vibration interactions. The results show that the largest contribution (about 90%) is due to electron interactions with low-frequency vibrational modes. The relaxation energy in anthracene-PMDA is found to be about five times smaller than the electronic coupling.

  8. Effect of exact Coulomb-exchange calculations on band-head spectra of odd-proton nuclei

    Directory of Open Access Journals (Sweden)

    Koh Meng-Hock

    2017-01-01

    Full Text Available Previous calculations of band-head energy spectra of odd-mass heavy nuclei in the Hartree-Fock-plus-Bardeen-Cooper-Schrieffer (HF-BCS framework showed that the agreement with data is better for odd-neutron as compared to odd-proton nuclei. The reason for a poorer agreement with data for the latter have been ascribed to the possible usage of the Slater approximation in calculating the Coulomb-exchange term. In this work, we report the effect of exact Coulomb-exchange calculations on band-head energy spectra of two odd-proton nuclei (namely 237Np and 241Am as compared to the results obtained using the Slater approximation. We performed self-consistent blocking calculations while taking the breaking of time-reversal symmetry at the mean-field level into account due to the unpaired nucleon. The SkM* and SIII parametrizations of the Skyrme interaction have been employed to approximate the effective nucleon-nucleon interaction while a seniority force is used for the pairing channel. Contrary to what was expected, our preliminary results show no improvement on the band-head spectra as compared to data when the Coulomb-exchange term is calculated exactly.

  9. A new approach to barrier-top fission dynamics

    Directory of Open Access Journals (Sweden)

    Bertsch G.F.

    2016-01-01

    Full Text Available We proposed a calculational framework for describing induced fission that avoids the Bohr-Wheeler assumption of well-defined fission channels. The building blocks of our approach are configurations that form a discrete, orthogonal basis and can be characterized by both energy and shape. The dynamics is to be determined by interaction matrix elements between the states rather than by a Hill-Wheeler construction of a collective coordinate. Within our approach, several simple limits can be seen: diffusion; quantized conductance; and ordinary decay through channels. The specific proposal for the discrete basis is to use the Kπ quantum numbers of the axially symmetric Hartree-Fock approximation to generate the configurations. Fission paths would be determined by hopping from configuration to configuration via the residual interaction. We show as an example the configurations needed to describe a fictitious fission decay 32S → 16 O + 16 O. We also examine the geometry of the path for fission of 236U, measuring distances by the number of jumps needed to go to a new Kπ partition.

  10. Initial four-body forces in many-body calculations

    Energy Technology Data Exchange (ETDEWEB)

    Schulz, Stefan; Roth, Robert [Institut fuer Kernphysik, Technische Universitaet Darmstadt (Germany)

    2016-07-01

    For the ab-initio description of light and medium-mass nuclei, chiral effective field theory is used successfully. Improving the precision and uncertainty estimation of chiral forces, especially an improved description of medium-mass nuclei, requires consistent order-by-order calculations. Starting at N{sup 3}LO, chiral four-body forces play a role and their impact on nuclei beyond few-body systems is currently unknown. Even without initial four-body forces, transformations such as the similarity renormalization group induce many-body forces. We model the four-body forces using a simple contact interaction and investigate its effect on nuclear many-body observables, especially ground-state energies and radii, as well as correlations between them. The four-body forces are evaluated in a Jacobi harmonic oscillator (HO) basis and subsequently used in no-core shell model and Hartree-Fock calculations for light- and medium mass nuclei. Handling of chiral forces is identical to a contact interaction, once they are evaluated in a HO basis.

  11. Structure and stability of SnS2-based single- and multi-wall nanotubes

    Science.gov (United States)

    Bandura, Andrei V.; Evarestov, Robert A.

    2015-11-01

    Hybrid density functional method PBE0 which mixes the 75% Perdew-Burke-Ernzerhof and 25% Hartree-Fock exchange functional has been applied for investigation of the electronic and atomic structures of nanotubes obtained by rolling up of hexagonal layers of tin disulfide. Calculations have been performed on the basis of the localized atomic functions by means of the CRYSTAL09 computer code. The calculated strain energy of SnS2 single-wall nanotubes approximately obeys the R- 2 law (R is nanotube radius) of the classical elasticity theory. The SnS2 nanotube electronic band structures yield a semiconducting behavior. Band gap of single-wall nanotubes decreases linearly with R- 1. The dispersion force correction is found to be important for prediction of the multi-wall nanotube stability. The distance and interaction energy between the single-wall components of the double-wall nanotubes are proved to be close to the distance and interaction energy between layers in the bulk crystal. Analysis of the relaxed nanotube shape using the offered method demonstrates a small but noticeable deviation from completely cylindrical cross-section of the external walls in the armchair-like double- and triple-walled nanotubes.

  12. Structure and thermochemistry of ClO2 radicals

    Science.gov (United States)

    Francisco, J. S.; Sander, S. P.

    1993-01-01

    The structure of ClO2 has been calculated for the X 2A-double prime ground state using unrestricted Hartree-Fock (UHF), unrestricted second-order Moller-Plesset perturbation (UMP2), configuration interaction employing single and double excitation (CISD), and quadratic configuration interaction (QCI) ab initio molecular orbital methods. Calculations using UMP2 and CISD wave functions predict a ClO bond length of 1.728 +/- 0.01 A. The single-configuration-based QCI in the singles and doubles space with perturbation inclusion of triple substitutions, denoted QCISD(T), yield a ClO bond length of 2.205 A. The QCI results are consistent with results of Jensen (1990) who showed that the ClO bond length is 2.181 A using annihilated self-consistent methods (AUMP2). The thermochemistry of ClO2 radical has been calculated using MP2 and QCI methods employing an isodesmic scheme. Our scheme predicts the heat of formation for ClO2 at 0 K to be 24.6 +/- 2 kcal/mol.

  13. Vibrational properties of organic donor-acceptor molecular crystals: Anthracene-pyromellitic-dianhydride (PMDA) as a case study

    Energy Technology Data Exchange (ETDEWEB)

    Fonari, A.; Corbin, N. S.; Coropceanu, V., E-mail: jean-luc.bredas@kaust.edu.sa, E-mail: coropceanu@gatech.edu [School of Chemistry and Biochemistry and Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400 (United States); Vermeulen, D.; McNeil, L. E. [Department of Physics and Astronomy, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599-3255 (United States); Goetz, K. P.; Jurchescu, O. D. [Department of Physics, Wake Forest University, Winston-Salem, North Carolina 27109-7507 (United States); Bredas, J. L., E-mail: jean-luc.bredas@kaust.edu.sa, E-mail: coropceanu@gatech.edu [School of Chemistry and Biochemistry and Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400 (United States); Solar and Photovoltaics Engineering Research Center, Division of Physical Science and Engineering, King Abdullah University of Science and Technology, Thuwal 23955-6900 (Saudi Arabia)

    2015-12-14

    We establish a reliable quantum-mechanical approach to evaluate the vibrational properties of donor-acceptor molecular crystals. The anthracene-PMDA (PMDA = pyromellitic dianhydride) crystal, where anthracene acts as the electron donor and PMDA as the electron acceptor, is taken as a representative system for which experimental non-resonance Raman spectra are also reported. We first investigate the impact that the amount of nonlocal Hartree-Fock exchange (HFE) included in a hybrid density functional has on the geometry, normal vibrational modes, electronic coupling, and electron-vibrational (phonon) couplings. The comparison between experimental and theoretical Raman spectra indicates that the results based on the αPBE functional with 25%-35% HFE are in better agreement with the experimental results compared to those obtained with the pure PBE functional. Then, taking αPBE with 25% HFE, we assign the vibrational modes and examine their contributions to the relaxation energy related to the nonlocal electron-vibration interactions. The results show that the largest contribution (about 90%) is due to electron interactions with low-frequency vibrational modes. The relaxation energy in anthracene-PMDA is found to be about five times smaller than the electronic coupling.

  14. Mott metal-insulator transition in the doped Hubbard-Holstein model

    Science.gov (United States)

    Kurdestany, Jamshid Moradi; Satpathy, S.

    2017-08-01

    Motivated by the current interest in the understanding of the Mott insulators away from half-filling, observed in many perovskite oxides, we study the Mott metal-insulator transition in the doped Hubbard-Holstein model using the Hartree-Fock mean field theory. The Hubbard-Holstein model is the simplest model containing both the Coulomb and the electron-lattice interactions, which are important ingredients in the physics of the perovskite oxides. In contrast to the half-filled Hubbard model, which always results in a single phase (either metallic or insulating), our results show that away from half-filling, a mixed phase of metallic and insulating regions occurs. As the dopant concentration is increased, the metallic part progressively grows in volume, until it exceeds the percolation threshold, leading to percolative conduction. This happens above a critical dopant concentration δc, which, depending on the strength of the electron-lattice interaction, can be a significant fraction of unity. This means that the material could be insulating even for a substantial amount of doping, in contrast to the expectation that doped holes would destroy the insulating behavior of the half-filled Hubbard model. While effects of fluctuation beyond the mean field remain an open question, our results provide a starting point for the understanding of the density-driven metal-insulator transition observed in many complex oxides.

  15. Electronic Structure of Ligated CdSe Clusters: Dependence on DFT Methodology

    Energy Technology Data Exchange (ETDEWEB)

    Albert, VV; Ivanov, SA; Tretiak, S; Kilina, SV

    2011-07-07

    Simulations of ligated semiconductor quantum dots (QDs) and their physical properties, such as morphologies, QD-ligand interactions, electronic structures, and optical transitions, are expected to be very sensitive to computational methodology. We utilize Density Functional Theory (DFT) and systematically study how the choice of density functional, atom-localized basis set, and a solvent affects the physical properties of the Cd{sub 33}Se{sub 33} cluster ligated with a trimethyl phosphine oxide ligand. We have found that qualitative performance of all exchange-correlation (XC) functionals is relatively similar in predicting strong QD-ligand binding energy ({approx}1 eV). Additionally, all functionals predict shorter Cd-Se bond lengths on the QD surface than in its core, revealing the nature and degree of QD surface reconstruction. For proper modeling of geometries and QD-ligand interactions, however, augmentation of even a moderately sized basis set with polarization functions (e.g., LANL2DZ* and 6-31G*) is very important. A polar solvent has very significant implications for the ligand binding energy, decreasing it to 0.2-0.5 eV. However, the solvent model has a minor effect on the optoelectronic properties, resulting in persistent blue shifts up to {approx}0.3 eV of the low-energy optical transitions. For obtaining reasonable energy gaps and optical transition energies, hybrid XC functionals augmented by a long-range Hartree-Fock orbital exchange have to be applied.

  16. Proximity effects on the local magnetic moments of clusters V{sub 6}-V{sub 9} embedded in a Fe matrix

    Energy Technology Data Exchange (ETDEWEB)

    Sosa-Hernandez, E.M. [Departamento de Matematicas Aplicadas, Facultad de Contaduria y Administration, Universidad Autonoma de San Luis Potosi, Alvaro Obregon 64, 78000 San Luis Potosi, S.L.P. (Mexico); Alvarado-Leyva, P.G. [Departamento de Fisica, Facultad de Ciencias, Universidad Autonoma de San Luis Potosi Alvaro Obregon 64, 78000 San Luis Potosi, S.L.P. (Mexico)]. E-mail: pal@galia.fc.uaslp.mx

    2006-11-09

    The magnetic behavior of clusters V{sub 6}-V{sub 9} in bulk Fe is determined by using an electronic Hamiltonian which includes s, p and d electrons. The spin density distribution is calculated self-consistenly in the unrestricted Hartree-Fock approximation. The local magnetic moments are obtained at V and Fe atoms; the magnetic coupling between Fe and V atoms is antiferromagnetic-like. We consider two cases, the first case correspond to non-interacting clusters, the distance between them is infinity, and the another case, when the clusters are interacting, the separation between them is finite; in the first case, the magnetic order in V{sub 6} is ferromagnetic-like whereas for V{sub 9} the magnetic order is antiferromagnetic-like, in the second case we have found that the magnetic order is not well stablished in V{sub 6}. We have found that the magnetic order in the matrix is not broken by the presence of the V atoms, although the local magnetic moments of Fe atoms at the interface cluster-matrix, are reduced respect to Fe bulk magnetization (2.22{mu} {sub B}) [e.g. {mu} {sub Fe}(5) = 1.98{mu} {sub B} in V{sub 6}; {mu} {sub Fe}(3) 1.89{mu} {sub B} in V{sub 9}].

  17. Transport and current noise characteristics of a T-shape double-quantum-dot system.

    Science.gov (United States)

    Brown, K; Crisan, M; Tifrea, I

    2009-05-27

    We consider the transport and the noise characteristics for the case of a T-shape double-quantum-dot system using the equation of motion method. Our theoretical results, obtained in an approximation equivalent to the Hartree-Fock approximation, account for non-zero on-site Coulomb interaction in both the detector and side dots. The existence of a non-zero Coulomb interaction implies an additional two resonances in the detector's dot density of states and thereafter affects the electronic transport properties of the system. The system's conductance presents two Fano dips as a function of the energy of the localized electronic level in the side dot. The Fano dips in the system's conductance can be observed for both strong (fast detector) and weak coupling (slow detector) between the detector dot and the external electrodes. Due to stronger electronic correlations, the noise characteristics in the case of a slow detector are much higher. This setup may be of interest for the practical realization of qubit states in quantum dot systems.

  18. Interactive governance

    DEFF Research Database (Denmark)

    Sørensen, Eva; Torfing, Jacob; Peters, B. Guy

    Governance has become one of the most commonly used concepts in contemporary political science. It is, however, often used to mean a variety of different things. This book helps to clarify this conceptual muddle by concentrating on one variety of governance-interactive governance. The authors argue...... that although the state may remain important for many aspects of governing, interactions between state and society represent an important, and perhaps increasingly important, dimension of governance. These interactions may be with social actors such as networks, with market actors or with other governments......, but all these forms represent means of governing involving mixtures of state action with the actions of other entities.This book explores thoroughly this meaning of governance, and links it to broader questions of governance. In the process of explicating this dimension of governance the authors also...

  19. Programming Interactivity

    CERN Document Server

    Noble, Joshua

    2009-01-01

    Make cool stuff. If you're a designer or artist without a lot of programming experience, this book will teach you to work with 2D and 3D graphics, sound, physical interaction, and electronic circuitry to create all sorts of interesting and compelling experiences -- online and off. Programming Interactivity explains programming and electrical engineering basics, and introduces three freely available tools created specifically for artists and designers: Processing, a Java-based programming language and environment for building projects on the desktop, Web, or mobile phonesArduino, a system t

  20. Compton profiles and band structure calculations of IV-VI layered compounds GeS and GeSe

    Science.gov (United States)

    Rathor, A.; Sharma, V.; Heda, N. L.; Sharma, Y.; Ahuja, B. L.

    2008-04-01

    First ever isotropic experimental Compton profiles of GeS and GeSe are presented. Moreover, we present Compton profiles, energy bands and density of states (DOS) using Hartree-Fock, density functional and pseudopotential schemes. It is seen that the Hartree-Fock and density functional theories show a reasonable agreement with the experiment. The equal-valence-electron-density profiles show that GeS is more ionic than GeSe. We have also reported energy bands and DOS using full potential linearized augmented plane-wave method.

  1. A theoretical study on the photoionization of the valence orbitals of phosphine

    Directory of Open Access Journals (Sweden)

    Nascimento Edmar M.

    2006-01-01

    Full Text Available We report a theoretical study on the photoionization of phosphine in the static-exchange level and frozen core approximation, using the method of continued fractions. The main subject of the present study is to investigate in which extent the Hartree-Fock description of the target applied to molecular photoionization is valid. Also, the role played by multichannel coupling is analysed. Our study shows that single-channel Hartree-Fock calculations can provide reliable results except for photon energies near the photoionization threshold.

  2. 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...

  3. Hole trapping at Al impurities in silica: A challenge for density functional theories

    DEFF Research Database (Denmark)

    Lægsgaard, Jesper; Stokbro, Kurt

    2001-01-01

    The atomic geometry and electronic structure around a neutral substitutional Al impurity in silica is investigated using either the unrestricted Hartree-Fock (UHF) approximation, or Beckes three-parameter hybrid functional (B3LYP). It is found that the B3LYP functional fails to describe the struc......The atomic geometry and electronic structure around a neutral substitutional Al impurity in silica is investigated using either the unrestricted Hartree-Fock (UHF) approximation, or Beckes three-parameter hybrid functional (B3LYP). It is found that the B3LYP functional fails to describe...

  4. Cardiopulmonary interactions

    African Journals Online (AJOL)

    2006-08-28

    Aug 28, 2006 ... applications to a particular subspecialty,2-5 the reader is advised to have .... Using Ohm's law, it is known that PVR = (mean PAP – mean LAP)/Qp. PVR is determined by the interactions of the large capacitance vessels of the pulmonary arterial tree and ..... care setting, the application of this gas is usually.

  5. Explicit Interaction

    DEFF Research Database (Denmark)

    Löwgren, Jonas; Eriksen, Mette Agger; Linde, Per

    2006-01-01

    as an interpretation of palpability, comprising usability as well as patient empowerment and socially performative issues. We present a prototype environment for video recording during physiotherapeutical consultation which illustrates our current thoughts on explicit interaction and serves as material for further...

  6. Interacting Components

    NARCIS (Netherlands)

    Orlic, B.; Broenink, Johannes F.; Welch, Peter; Kerridge, Jon; Barnes, Fred

    2006-01-01

    SystemCSP is a graphical modeling language based on both CSP and concepts of component-based software development. The component framework of SystemCSP enables specification of both interaction scenarios and relative execution ordering among components. Specification and implementation of

  7. Interactive Television.

    Science.gov (United States)

    Bisesi, Michael; Felder, B. Dell

    1986-01-01

    Universities can offer opportunities for workers in high-technology fields to gain state-of-the-art information and skills without traveling to campus, through interactive television training. Careful organization and planning of such programs, including selection of effective faculty and remote site personnel, are essential to their success. (MSE)

  8. Interactive Storytelling

    DEFF Research Database (Denmark)

    Schoenau-Fog, Henrik; Reng, Lars

    2015-01-01

    This book constitutes the refereed proceedings of the 8th International Conference on Interactive Digital Storytelling, ICIDS 2015, held in Copenhagen, Denmark, in November/December 2015. The 18 revised full papers and 13 short papers presented together with 9 posters, 9 workshop descriptions...

  9. Interactive cinema : engagement and interaction

    NARCIS (Netherlands)

    Vosmeer, Mirjam; Schouten, Ben; Mitchell, Alex; Fernández-Vara, Clara; Thue, David

    2014-01-01

    Technologies that were initially developed to be applied within the domain of video games are currently being used in experiments to explore their meaning and possibilities for cinema and cinema audiences. In this position paper we examine how narrativity, interactivity and engagement are mutually

  10. A 2:2:2 Complex of Vanadium(V) with 4-(2-Thiazolylazo)orcinol and 2,3,5-Triphenyl-2H-Tetrazolium Chloride.

    Science.gov (United States)

    Gavazov, Kiril Blazhev; Delchev, Vassil Borisov; Mileva, Kremena Tomova; Stefanova, Teodora Stefcheva; Toncheva, Galya Kostadinova

    2016-01-01

    The complex formation in the vanadium(V)/4-(2-thiazolylazo)orcinol (TAO)/2,3,5-triphenyl-2H-tetrazolium chloride (TTC) liquid-liquid extraction-chromogenic system was studied. The chloroform-extracted complex has a composition of 2:2:2 under the optimum conditions (pH 4.8-5.2, extraction time 3 min, concentration of TAO 3.4 × 10(-4) mol dm(-3), and concentration of TTC 9.4 × 10(-4) mol dm(-3)) and could be regarded as a dimer (D) of two 1:1:1 species (S) presented by the formula (TT+)[VO2(TAO)]. The constant of extraction was calculated by two methods and some analytical characteristics were determined. The wavelength of maximum absorption (λmax), molar absorptivity (ελ) and fraction extracted (E) were found to be λ = 545 nm, ε545 = 1.97 × 10(4) dm(3) mol(-1) cm(-1), and E = 97.9%. The ground-state equilibrium geometries of the complexes S and D were optimized by quantum chemical Hartree-Fock calculations using 3-21G* basis functions. The bonding and interaction energies were calculated as well.

  11. Correlation functions for three-dimensional quantum dots from Diffusion Monte Carlo simulations

    Science.gov (United States)

    Vincent, Jordan; Wilkens, Tim; Martin, Richard

    2002-03-01

    We report diffusion Monte Carlo (DMC) simulations of interacting electrons in spherical and cylindrical quasi-2D quantum dots [1] to determine the low energy spin states and to search for transitions to "Wigner molecule" or "spin wave" type states that are the analogue of the Wigner crystal that occurs in the low density homogeneous gas [2] or an anitferromagnet. All calculations are performed at zero magnetic field. Our fixed-node DMC uses trial wavefunction of the Slater-Jastrow type, with orbitals obtained from density functional theory calculations using the LDA or the KLI approximation to exact exchange (which is very close to Hartree-Fock). Since such mean-field calculations lead to broken symmetry solutions, we use multiple determinant trial functions that properly restore the symmetry. Simulations of the density profile and correlation functions in the correlated system show that formation of Wigner molecule or spin wave type correlations are significantly reduced from those inferred from the mean field solutions. The effect of including the thrid dimension in the simulations of the quasi-2D systems is elucidated by comparing with analogous DMC calculations of Pederiva, Umrigar and Lipparini [3] for the same area density and 2D confining potential. [1] See, for example R. C. Ashoori, Nature 379, 413 (1996). [2] B. Tanatar and D. M. Ceperley, Phys. Rev. B 39, 5005 (1989). [3] F. Pederiva, C. J. Umrigar, and E. Lipparini, Phys. Rev. B 62, 8120 (2000).

  12. Density functional investigations of the properties and thermochemistry of UF6 and UF5 using valence-electron and all-electron approaches.

    Science.gov (United States)

    Batista, Enrique R; Martin, Richard L; Hay, P Jeffrey; Peralta, Juan E; Scuseria, Gustavo E

    2004-08-01

    The structural properties and thermochemistry of UF6 and UF5 have been investigated using both Hartree-Fock and density functional theory (DFT) approximations. Within the latter approach, the local spin-density approximation, the generalized gradient approximation, and hybrid density functionals were considered. To describe the uranium atom we employed small-core (60 electrons) and large-core (78 electrons) relativistic effective core potentials (RECPs), as well as the all-electron approximation based on the two-component third-order Douglas-Kroll-Hess Hamiltonian. For structural properties, we obtained very good agreement with experiment with DFT and both large and small-core RECPs. The best match with experiment is given by the hybrid functionals with the small-core RECP. The bond dissociation energy (BDE) was obtained from the relative energies of the fragments [UF6 --> UF5 + F], corrected for zero-point energy and spin-orbit interaction. Very good agreement was found between the BDE obtained from all-electron calculations and those calculated with the small-core RECP, while those from the large-core RECP are off by more than 50%. In order to obtain good agreement with experiment in the BDE it is imperative to work with hybrid density functionals and a small-core RECP. (c) 2004 American Institute of Physics.

  13. Finite Fermi systems theory and self-consistency relations

    Energy Technology Data Exchange (ETDEWEB)

    Khodel, V.A.; Saperstein, E.E. (Gosudarstvennyj Komitet po Ispol' zovaniyu Atomnoj Ehnergii SSSR, Moscow. Inst. Atomnoj Ehnergii)

    1982-12-01

    The self-consistent theory of the finite Fermi systems is outlined. This approach is based on the same Fermi liquid theory principles as the familiar theory for finite Fermi systems (FFS) by Migdal. We show that the basic Fermi system properties can be evaluated in terms of the quasiparticle Lagrangian Lsub(q) which incorporates the energy dependency effects. This Lagrangian is defined so that the corresponding Lagrange equations should coincide with the FFS theory equations of motion of the quasiparticles. The quasiparticle energy Esub(q) defined in the terms of the quasiparticle Lagrangian Lsub(q) according to the usual canonical rules is shown to be equal to the binding energy E/sub 0/ of the system. For a given Lagrangian Lsub(q) the particle densities in nuclei, the nuclear single-particle spectra, the low-lying collective states (LCS) properties, and the amplitude of the interquasiparticle interaction are also evaluated. The suggested approach is compared with the Hartree-Fock theory with effective forces.

  14. Assessment of quantum chemical methods and basis sets for excitation energy transfer

    Energy Technology Data Exchange (ETDEWEB)

    Fink, Reinhold F. [Institute of Physical Chemistry, University of Wuerzburg, Am Hubland, D-97074 Wuerzburg (Germany); Pfister, Johannes; Zhao Hongmei [Institute of Organic Chemistry, University of Wuerzburg, Am Hubland, D-97074 Wuerzburg (Germany); Engels, Bernd [Institute of Organic Chemistry, University of Wuerzburg, Am Hubland, D-97074 Wuerzburg (Germany)], E-mail: bernd@chemie.uni-wuerzburg.de

    2008-05-04

    The validity of several standard quantum chemical approaches and other models for the prediction of exciton energy transfer is investigated using the HOMO-LUMO excited states of benzene dimer as an example. The configuration interaction singles (CIS), time-dependent Hartree-Fock (TD-HF), time dependent density functional theroy (TD-DFT), and complete-active-space self-consistent-field (CASSCF) methods are applied with a supermolecule approach and compared to the previously established monomer transition density method and the ideal dipole approximation. Strong and physically incorrect admixture of charge-transfer states makes TD-DFT inappropriate for investigations of potential energy surfaces in such dimer systems. CIS, TD-HF and CASSCF perform qualitatively correct. TD-HF seems to be a particularly appropriate method due to its general applicability and overall good performance for the excited state and for transition properties. Double-zeta basis sets with polarisation functions are found to be sufficient to predict transfer rates of dipole allowed excitations. Efficient excitation energy transfer is predicted between degenerate excited states while avoided curve crossings of nearly spaced {pi}-aggregates are identified as a possible trapping mechanism.

  15. Merging symmetry projection methods with coupled cluster theory: Lessons from the Lipkin model Hamiltonian

    Energy Technology Data Exchange (ETDEWEB)

    Wahlen-Strothman, J. M. [Rice Univ., Houston, TX (United States); Henderson, T. H. [Rice Univ., Houston, TX (United States); Hermes, M. R. [Rice Univ., Houston, TX (United States); Degroote, M. [Rice Univ., Houston, TX (United States); Qiu, Y. [Rice Univ., Houston, TX (United States); Zhao, J. [Rice Univ., Houston, TX (United States); Dukelsky, J. [Consejo Superior de Investigaciones Cientificas (CSIC), Madrid (Spain). Inst. de Estructura de la Materia; Scuseria, G. E. [Rice Univ., Houston, TX (United States)

    2018-01-03

    Coupled cluster and symmetry projected Hartree-Fock are two central paradigms in electronic structure theory. However, they are very different. Single reference coupled cluster is highly successful for treating weakly correlated systems, but fails under strong correlation unless one sacrifices good quantum numbers and works with broken-symmetry wave functions, which is unphysical for finite systems. Symmetry projection is effective for the treatment of strong correlation at the mean-field level through multireference non-orthogonal configuration interaction wavefunctions, but unlike coupled cluster, it is neither size extensive nor ideal for treating dynamic correlation. We here examine different scenarios for merging these two dissimilar theories. We carry out this exercise over the integrable Lipkin model Hamiltonian, which despite its simplicity, encompasses non-trivial physics for degenerate systems and can be solved via diagonalization for a very large number of particles. We show how symmetry projection and coupled cluster doubles individually fail in different correlation limits, whereas models that merge these two theories are highly successful over the entire phase diagram. Despite the simplicity of the Lipkin Hamiltonian, the lessons learned in this work will be useful for building an ab initio symmetry projected coupled cluster theory that we expect to be accurate in the weakly and strongly correlated limits, as well as the recoupling regime.

  16. Shuffle dislocation induced magnetic moment in graphene

    Energy Technology Data Exchange (ETDEWEB)

    Lopez-Sancho, M.P., E-mail: pilar@icmm.csic.e [Instituto de Ciencia de Materiales de Madrid-CSIC, C/Sor Juana Ines de la Cruz 3, 28049 Madrid (Spain); Juan, F. de; Vozmediano, M.A.H. [Instituto de Ciencia de Materiales de Madrid-CSIC, C/Sor Juana Ines de la Cruz 3, 28049 Madrid (Spain)

    2010-05-15

    Graphene, a honeycomb arrangement of carbon atoms, is a promising material for nanoelectronics applications due to its unusual electronic properties. Recent experiments performed on suspended graphene indicate the existence of intrinsic defects on the samples. It is known that lattice defects such as vacancies or voids leaving unpaired atoms, lead to the formation of local magnetic moments (Vozmediano et al., 2005). The existence and ordering of these moments is largely determined by the bipartite character of the honeycomb lattice seen as two interpenetrating triangular sublattices. Dislocations made by pentagon-heptagon pairs or octagons with an unpaired atom have been studied recently and found to be stable in the graphene lattice (Carpio et al., 2008). These defects frustrate the sublattice structure and affect the magnetic properties of graphene. We study the magnetic properties of graphene in the presence of these defects. The system is described by a p{sub z} tight-binding model with electron-electron interactions modelled by a Hubbard term. Spin-polarized mean-field solutions are investigated within an unrestricted Hartree-Fock approximation.

  17. Regularity and approximability of electronic wave functions

    CERN Document Server

    Yserentant, Harry

    2010-01-01

    The electronic Schrödinger equation describes the motion of N-electrons under Coulomb interaction forces in a field of clamped nuclei. The solutions of this equation, the electronic wave functions, depend on 3N variables, with three spatial dimensions for each electron. Approximating these solutions is thus inordinately challenging, and it is generally believed that a reduction to simplified models, such as those of the Hartree-Fock method or density functional theory, is the only tenable approach. This book seeks to show readers that this conventional wisdom need not be ironclad: the regularity of the solutions, which increases with the number of electrons, the decay behavior of their mixed derivatives, and the antisymmetry enforced by the Pauli principle contribute properties that allow these functions to be approximated with an order of complexity which comes arbitrarily close to that for a system of one or two electrons. The text is accessible to a mathematical audience at the beginning graduate level as...

  18. A benchmark study of the two-dimensional Hubbard model with auxiliary-field quantum Monte Carlo method

    CERN Document Server

    Qin, Mingpu; Zhang, Shiwei

    2016-01-01

    Ground state properties of the Hubbard model on a two-dimensional square lattice are studied by the auxiliary-field quantum Monte Carlo method. Accurate results for energy, double occupancy, effective hopping, magnetization, and momentum distribution are calculated for interaction strengths of U/t from 2 to 8, for a range of densities including half-filling and n = 0.3, 0.5, 0.6, 0.75, and 0.875. At half-filling, the results are numerically exact. Away from half-filling, the constrained path Monte Carlo method is employed to control the sign problem. Our results are obtained with several advances in the computational algorithm, which are described in detail. We discuss the advantages of generalized Hartree-Fock trial wave functions and its connection to pairing wave functions, as well as the interplay with different forms of Hubbard-Stratonovich decompositions. We study the use of different twist angle sets when applying the twist averaged boundary conditions. We propose the use of quasi-random sequences, whi...

  19. Dynamical mean-field theory from a quantum chemical perspective.

    Science.gov (United States)

    Zgid, Dominika; Chan, Garnet Kin-Lic

    2011-03-07

    We investigate the dynamical mean-field theory (DMFT) from a quantum chemical perspective. Dynamical mean-field theory offers a formalism to extend quantum chemical methods for finite systems to infinite periodic problems within a local correlation approximation. In addition, quantum chemical techniques can be used to construct new ab initio Hamiltonians and impurity solvers for DMFT. Here, we explore some ways in which these things may be achieved. First, we present an informal overview of dynamical mean-field theory to connect to quantum chemical language. Next, we describe an implementation of dynamical mean-field theory where we start from an ab initio Hartree-Fock Hamiltonian that avoids double counting issues present in many applications of DMFT. We then explore the use of the configuration interaction hierarchy in DMFT as an approximate solver for the impurity problem. We also investigate some numerical issues of convergence within DMFT. Our studies are carried out in the context of the cubic hydrogen model, a simple but challenging test for correlation methods. Finally, we finish with some conclusions for future directions. © 2011 American Institute of Physics.

  20. Phase diagram of insulating crystal and quantum Hall states in ABC-stacked trilayer graphene

    Science.gov (United States)

    Côté, R.; Rondeau, Maxime; Gagnon, Anne-Marie; Barlas, Yafis

    2012-09-01

    In the presence of a perpendicular magnetic field, ABC-stacked trilayer graphene's chiral band structure supports a 12-fold degenerate N=0 Landau level (LL). Along with the valley and spin degrees of freedom, the zeroth LL contains additional quantum numbers associated with the LL orbital index n=0,1,2. Remote interlayer hopping terms and external potential difference ΔB between the layers lead to LL splitting by introducing a gap ΔLL between the degenerate zero-energy triplet LL orbitals. Assuming that the spin and valley degrees of freedom are frozen, we study the phase diagram of this system resulting from competition of the single particle LL splitting and Coulomb interactions within the Hartree-Fock approximation at integer filling factors. In some range [ΔLLc,1,ΔLLc,2] of the gap ΔLL, the uniform QH state is unstable to the formation of a crystal state at integer filling factors while outside of this range, the ground state is a uniform quantum Hall state where the electrons occupy the lowest unoccupied LL orbital index. The transition between the uniform and crystal states should be characterized by a Hall plateau transition as a function of ΔLL at a fixed filling factor. We also study the properties of this crystal state and discuss its experimental detection.

  1. Spectroscopic (FT-IR, FT-Raman, UV-Vis) analysis, conformational, HOMO-LUMO, NBO and NLO calculations on monomeric and dimeric structures of 4-pyridazinecarboxylic acid by HF and DFT methods

    Science.gov (United States)

    Eşme, A.; Sağdınç, S. G.

    2017-11-01

    In this study, the Fourier transform infrared (FT-IR) and Fourier transform Raman (FT-Raman) spectra of 4-pyridazinecarboxylic acid (4PCA) in solid phase were recorded and analyzed. Quantum chemical calculations of the optimized molecular structure, energies, conformational, UV-Vis, nonlinear optical (NLO) and natural bond orbital (NBO) analysis, molecular surfaces, Mulliken charges, and vibrational studies for 4PCA were performed using the ab initio Hartree-Fock (HF) and density functional theory (DFT/B3LYP) methods with 6-311++G(d,p) basis set. Obtained results on the geometric structure and vibrational frequencies are compared with observed data. The dimeric structure of 4PCA with DFT/B3LYP/6-311++G(d,p) level caused by the shifts of Osbnd H and Cdbnd O bands in the vibrational spectra of 4PCA were also studied. Moreover, the spectroscopic and theoretical results were compared with the corresponding properties for monomeric and dimeric structures of 4PCA. The calculated highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) energies also confirm that charge transfer occurs within the molecule. NBO analysis confirms the presence of intramolecular charge transfer and the hydrogen bonding interaction. The detailed vibrational assignments were performed with the HF and DFT calculations, and the potential energy distribution (PED) was obtained by the Vibrational Energy Distribution Analysis (VEDA4) program.

  2. NLO and NBO Analysis of Sarcosine-Maleic Acid by Using HF and B3LYP Calculations

    Directory of Open Access Journals (Sweden)

    N. Günay

    2013-01-01

    Full Text Available We report a theoretical study on molecular structure, vibrational spectra, nonlinear optical (NLO, and natural bond orbital (NBO analysis of sarcosine-maleic acid (C7H11NO6 in the ground state calculated by using the Hartree-Fock (HF and density functional method (DFT/B3LYP with 6–31++G(d,p basis set. We repeat NBO calculations with 6–31G(d,p basis set so as to see the diffuse function impact on NBO analysis. Stability of the molecule arising from hyper conjugative interactions and charge delocalization has been analyzed using NBO analysis. NBO analysis shows that there is a O–H⋯O and N–H⋯O hydrogen bond in the title compound, which is consistent with the conclusion obtained by the analysis of molecular structure. The calculated HOMO and LUMO energies show that charge transfer occurs within the molecule. Also, these results are supported by the NLO parameters. Finally, the calculated results were applied to simulate infrared and Raman spectra of the title compound which showed good agreement with experimental ones.

  3. Quantum and thermal fluctuations in a Raman spin-orbit-coupled Bose gas

    Science.gov (United States)

    Chen, Xiao-Long; Liu, Xia-Ji; Hu, Hui

    2017-07-01

    We theoretically study a three-dimensional weakly interacting Bose gas with Raman-induced spin-orbit coupling at finite temperature. By employing a generalized Hartree-Fock-Bogoliubov theory with Popov approximation, we determine a complete finite-temperature phase diagram of three exotic condensation phases (i.e., the stripe, plane-wave, and zero-momentum phases), against both quantum and thermal fluctuations. We find that the plane-wave phase is significantly broadened by thermal fluctuations. The phonon mode and sound velocity at the transition from the plane-wave phase to the zero-momentum phase are thoughtfully analyzed. At zero temperature, we find that quantum fluctuations open an unexpected gap in sound velocity at the phase transition, in stark contrast to the previous theoretical prediction of a vanishing sound velocity. At finite temperature, thermal fluctuations continue to significantly enlarge the gap, and simultaneously shift the critical minimum. For a Bose gas of 87Rb atoms at the typical experimental temperature, T =0.3 T0 , where T0 is the critical temperature of an ideal Bose gas without spin-orbit coupling, our results of gap opening and critical minimum shifting in the sound velocity are qualitatively consistent with the recent experimental observation [Ji et al., Phys. Rev. Lett. 114, 105301 (2015), 10.1103/PhysRevLett.114.105301].

  4. Generalized SU(3) Nambu-Jona-Lasinio model. Pt. 2; From current to constituent quarks

    Energy Technology Data Exchange (ETDEWEB)

    Vogl, U.; Lutz, M.; Klimt, S.; Weise, W. (Regensburg Univ. (Germany, F.R.). Inst. fuer Physik 1 - Theoretische Physik)

    1990-10-08

    We investigate the properties of constituent quarks, i.e. quarks dressed by their strong interactions, in a generalized Nambu-Jona-Lasinio model with N{sub f}=3 flavours. In the Hartree-Fock approximation, the step from structureless current quarks to massive constituent quarks is made through dynamical mass generation which implies spontaneous chiral symmetry breaking. We study, in particular, the quark scalar, vector and axial vector currents within this framework. We demonstrate that, a low energy and momentum transfers, single valence quarks are strongly screened by quark-antiquark polarization effects. For the electromagnetic currents, we recover relationships familiar from the vector meson dominance model. For the axial current, screening by J{sup {pi}}=1{sup +} quark-antiquark modes leads to an effective quark axial vector constant g{sub A}<1 which satisfies the Goldberger-Treiman relation at the quark level. The spin content of the proton is also discussed in this framework. We calculate quark magnetic moments and electromagnetic form factors and discuss their related sizes. (orig.).

  5. Manifestly Hermitian semiclassical expansion for the one-particle density matrix of a two-dimensional Fermi gas

    Science.gov (United States)

    Bencheikh, K.; van Zyl, B. P.; Berkane, K.

    2016-08-01

    The semiclassical ℏ expansion of the one-particle density matrix for a two-dimensional Fermi gas is calculated within the Wigner transform method of B. Grammaticos and A. Voros [Ann. Phys. (N.Y.) 123, 359 (1979), 10.1016/0003-4916(79)90343-9], originally developed in the context of nuclear physics. The method of Grammaticos and Voros has the virtue of preserving both the Hermiticity and idempotency of the density matrix to all orders in the ℏ expansion. As a topical application, we use our semiclassical expansion to go beyond the local-density approximation for the construction of the total dipole-dipole interaction energy functional of a two-dimensional, spin-polarized dipolar Fermi gas. We find a finite, second-order gradient correction to the Hartree-Fock energy, which takes the form ɛ (∇ρ ) 2/√{ρ } , with ɛ being small (|ɛ |≪1 ) and negative. We test the quality of the corrected energy by comparing it with the exact results available for harmonic confinement. Even for small particle numbers, the gradient correction to the dipole-dipole energy provides a significant improvement over the local-density approximation.

  6. Perspective: Kohn-Sham density functional theory descending a staircase

    Science.gov (United States)

    Yu, Haoyu S.; Li, Shaohong L.; Truhlar, Donald G.

    2016-10-01

    This article presents a perspective on Kohn-Sham density functional theory (KS-DFT) for electronic structure calculations in chemical physics. This theory is in widespread use for applications to both molecules and solids. We pay special attention to several aspects where there are both concerns and progress toward solutions. These include: 1. The treatment of open-shell and inherently multiconfigurational systems (the latter are often called multireference systems and are variously classified as having strong correlation, near-degeneracy correlation, or high static correlation; KS-DFT must treat these systems with broken-symmetry determinants). 2. The treatment of noncovalent interactions. 3. The choice between developing new functionals by parametrization, by theoretical constraints, or by a combination. 4. The ingredients of the exchange-correlation functionals used by KS-DFT, including spin densities, the magnitudes of their gradients, spin-specific kinetic energy densities, nonlocal exchange (Hartree-Fock exchange), nonlocal correlation, and subshell-dependent corrections (DFT+U). 5. The quest for a universal functional, where we summarize some of the success of the latest Minnesota functionals, namely MN15-L and MN15, which were obtained by optimization against diverse databases. 6. Time-dependent density functional theory, which is an extension of DFT to treat time-dependent problems and excited states. The review is a snapshot of a rapidly moving field, and—like Marcel Duchamp—we hope to convey progress in a stimulating way.

  7. Electronic properties of prismatic modifications of single-wall carbon nanotubes

    Science.gov (United States)

    Tomilin, O. B.; Muryumin, E. E.; Rodionova, E. V.; Ryskina, N. P.

    2018-01-01

    The article shows the possibility of target modifying the prismatic single-walled carbon nanotubes (SWCNTs) by regular chemisorption of fluorine atoms in the graphene surface. It is shown that the electronic properties of prismatic SWCNT modifications are determined by the interaction of π- and ρ(in-plane)-electron conjugation in the carbon-conjugated subsystems (tracks) formed in the faces. The contributions of π- and ρ(in-plane)-electron conjugation depend on the structural characteristics of the tracks. It was found that the minimum of degree deviation of the track from the plane of the prism face and the maximum of the track width ensure the maximum contribution of the π-electron conjugation, and the band gap of the prismatic modifications of the SWCNT tends to the band gap of the hydrocarbon analog of the carbon track. It is established that the maximum of degree deviation of the track from the plane of the prism face and the maximum of track width ensure the maximum contribution of the ρ(in-plane) electron interface, and the band gap of the prismatic modifications of the SWCNT tends to the band gap of the unmodified carbon nanotube. The calculation of the model systems has been carried out using an ab initio Hartree-Fock method in the 3-21G basis.

  8. Electronic structure of vitamin B12 within the framework of the Haldane-Anderson impurity model

    Science.gov (United States)

    Kandemir, Zafer; Mayda, Selma; Bulut, Nejat

    2015-03-01

    We study the electronic structure of vitamin B12 (cyanocobalamine C63H88CoN14O14P) by using the framework of the multi-orbital single-impurity Haldane-Anderson model of a transition-metal impurity in a semiconductor host. Here, our purpose is to understand the many-body effects originating from the transition-metal impurity. In this approach, the cobalt 3 d orbitals are treated as the impurity states placed in a semiconductor host which consists of the rest of the molecule. The parameters of the resulting effective Haldane-Anderson model are obtained within the Hartree-Fock approximation for the electronic structure of the molecule. The quantum Monte Carlo technique is then used to calculate the one-electron and magnetic correlation functions of this effective Haldane-Anderson model for vitamin B12. We find that new states form inside the semiconductor gap due to the on-site Coulomb interaction at the impurity 3 d orbitals and that these states become the highest occupied molecular orbitals. In addition, we present results on the charge distribution and spin correlations around the Co atom. We compare the results of this approach with those obtained by the density-functional theory calculations.

  9. Synthesis of diosgenin p-nitrobenzoate by Steglich method, its crystal structure and quantum chemical studies

    Science.gov (United States)

    Sethi, Arun; Bhatia, Akriti; Shukla, Dolly; Kumar, Abhinav; Sonker, Ravi; Prakash, Rohit; Bhatia, Gitika

    2012-11-01

    In the present study, a novel one pot synthetic route for the synthesis of diosgenin p-nitrobenzoate (2) is described from cheap, commercially available naturally occurring sapogenin-diosgenin. The molecular geometry, IR frequencies, Gauge-including atomic orbital (GIAO), 1H and 13C NMR chemical shifts of compound 2 has been calculated in the ground state by using the Hartree-Fock (HF) and density functional method (DFT/B3LYP) using 6-31G(d,p) basis set. The structure of diosgenin p-nitrobenzoate (2) has been confirmed by single crystal X-ray diffraction. The compound crystallizes in monoclinic form having space group P21 with cell parameters a = 7.719(2) Å, b = 8.425(2) Å and c = 22.578(6) Å, α = 90.00, β = 98.46 and γ = 90.00. The oxygen atoms O5 and O4 of the nitro and carbonyl ester, respectively display weak intermolecular N1sbnd O5⋯H7' and C1'dbnd O4⋯H4' interactions having dimensions of 2.61 and 2.59 Å, respectively to form intricate 1D network. The study of the electronic properties such as HOMO and LUMO energy were performed using time dependent DFT (TD-DFT) calculations. The calculated HOMO and LUMO energy values indicate that charge transfer takes place within the molecule. The compound was screened for cytotoxicity and anti-adipogenic activity.

  10. Ab initio calculation of UV-absorption spectra of chlorophyll a: Comparison study between RHF/CIS, TDDFT, and semi-empirical methods

    CERN Document Server

    Suendo, Veinardi

    2011-01-01

    Chlorophyll a is one the most abundant pigment on Earth, which is responsible for trapping the light energy to perform the photosynthesis process in green plants. This molecule is a metal-complex compound that consists of a porphyrins ring with high symmetry that acts as ligands with magnesium as the central ion. Chlorophyll a has been studied for many years from different point of views for both experimental and theoretical interests. In this study, the restricted Hartree-Fock configuration interaction single (RHF/CIS), time-dependent density functional theory (TDDFT) and some semi-empirical methods (CNDO/s and ZINDO) calculations were carried out and compared to reconstruct the UV-Vis absorption spectra of chlorophyll a. In some extend, the calculation results based on a single molecule calculation were succeeded to reconstruct the absorption spectra but required to be scaling and broaden to match the experimental one. Different computational methods (ab initio and semi-empirical) exhibits the differences i...

  11. The N=16 subshell closure; La fermeture de sous-couche N=16

    Energy Technology Data Exchange (ETDEWEB)

    Obertelli, A

    2005-09-01

    The sequence of magic numbers for stable nuclei is now well understood. However the magnitude of shell gap may evolve from stability to drip line. Several observables show that N = 16 neutron-rich isotones present a higher stability compared to their neighbors on the N-Z chart. The spectroscopy of the levels of Ne{sup 27}, involving sd and fp shells, has allowed us to study the evolution of the nuclear shells responsible for the structure changes in N 16 isotones. In this framework we have studied the neutron transfer reaction Ne{sup 26}(d,p)Ne{sup 27} by inverted kinematics at 9,7 MeV/u. A cryogenic D{sub 2} target (17 mg.cm{sup -2}) has been used. The use of the magnetic spectrometer Vamos and that of the Exogam photon detector in coincidence operating mode has allowed us to achieve the spectroscopy of Ne{sup 27}. The results show a reduction in the gap between sd and fp shells for N = 17 isotones as we go from stability toward the neutron drip line. We have also performed a theoretical study in mean-field theory and beyond it through configuration mixing so that we can see the evolution of the isospin of the N = 16 subshell's closure. We have used a HFB (Hartree-Fock-Bogoliubov) with the finite range D1S effective interaction. (A.C.)

  12. Ab initio many-body perturbation theory and no-core shell model

    Science.gov (United States)

    Hu, B. S.; Wu, Q.; Xu, F. R.

    2017-10-01

    In many-body perturbation theory (MBPT) we always introduce a parameter N shell to measure the maximal allowed major harmonic-oscillator (HO) shells for the single-particle basis, while the no-core shell model (NCSM) uses N maxℏΩ HO excitation truncation above the lowest HO configuration for the many-body basis. It is worth comparing the two different methods. Starting from “bare” and Okubo-Lee-Suzuki renormalized modern nucleon-nucleon interactions, NNLOopt and JISP16, we show that MBPT within Hartree-Fock bases is in reasonable agreement with NCSM within harmonic oscillator bases for 4He and 16O in “close” model space. In addition, we compare the results using “bare” force with the Okubo-Lee-Suzuki renormalized force. Supported by National Key Basic Research Program of China (2013CB834402), National Natural Science Foundation of China (11235001, 11320101004, 11575007) and the CUSTIPEN (China-U.S. Theory Institute for Physics with Exotic Nuclei) funded by the U.S. Department of Energy, Office of Science (DE-SC0009971)

  13. On the interplay of superconductivity and magnetism

    CERN Document Server

    Powell, B J

    2002-01-01

    We explore the exchange field dependence of the Hubbard model with a attractive, effective, pairwise, nearest neighbour interaction via the Hartree-Fock-Gorkov approximation. We derive a Ginzburg-Landau theory of spin triplet superconductivity in an exchange field. For microscopic parameters which lead to ABM phase superconductivity in zero field, the Ginzburg-Landau theory allows both an axial (A, A sub 1 or A sub 2) solution with the vector order parameter, d(k), perpendicular to the field, H, and an A phase solution with d(k) parallel to H. We study the spin-generalised Bogoliubov-de Gennes (BdG) equations for this model with parameters suitable for strontium ruthenate (Sr sub 2 RuO sub 4). The A sub 2 phase is found to be stable in a magnetic field. However, in the real material, spin-orbit coupling could pin the order parameter to the crystallographic c-axis which would favour the A phase for fields parallel to the c-axis. We show that the low temperature thermodynamic behaviour in a magnetic field could...

  14. Crystalline phases of bosons in rotating traps: Tonks-Girardeau gas on a ring.

    Science.gov (United States)

    Romanovsky, Igor; Yannouleas, Constantine; Landman, Uzi

    2006-03-01

    We analyze the systems of strongly repelling bosons in two-dimensional harmonic and ring-shaped traps as a function of the rotational frequency of the trap for neutral atoms (and of an applied magnetic field for charged bosons). Our two-step approach consists of breaking the rotational symmetry at the Hartree-Fock level and of subsequent symmetry restoration via projection techniques, thus taking into account correlations beyond the Gross-Pitaevskii (GP) solution. The bosons localize and form crystalline patterns both for a repulsive contact potential and a Coulomb interaction, as revealed via conditional probability distribution (CPD) analysis. This behavior of the bosons in the ring-shaped traps in the strong repulsion limit is similar to the behavior of fermions and is a manifestation of the fermionization phenomenon. We present calculations for the ground state energies as a function of the rotational frequency (or the strength of the magnetic field) and as a function of the repulsion strength. Phys. Rev. Lett.93, 230405 (2004)

  15. Psi4 1.1: An Open-Source Electronic Structure Program Emphasizing Automation, Advanced Libraries, and Interoperability.

    Science.gov (United States)

    Parrish, Robert M; Burns, Lori A; Smith, Daniel G A; Simmonett, Andrew C; DePrince, A Eugene; Hohenstein, Edward G; Bozkaya, Uğur; Sokolov, Alexander Yu; Di Remigio, Roberto; Richard, Ryan M; Gonthier, Jérôme F; James, Andrew M; McAlexander, Harley R; Kumar, Ashutosh; Saitow, Masaaki; Wang, Xiao; Pritchard, Benjamin P; Verma, Prakash; Schaefer, Henry F; Patkowski, Konrad; King, Rollin A; Valeev, Edward F; Evangelista, Francesco A; Turney, Justin M; Crawford, T Daniel; Sherrill, C David

    2017-07-11

    Psi4 is an ab initio electronic structure program providing methods such as Hartree-Fock, density functional theory, configuration interaction, and coupled-cluster theory. The 1.1 release represents a major update meant to automate complex tasks, such as geometry optimization using complete-basis-set extrapolation or focal-point methods. Conversion of the top-level code to a Python module means that Psi4 can now be used in complex workflows alongside other Python tools. Several new features have been added with the aid of libraries providing easy access to techniques such as density fitting, Cholesky decomposition, and Laplace denominators. The build system has been completely rewritten to simplify interoperability with independent, reusable software components for quantum chemistry. Finally, a wide range of new theoretical methods and analyses have been added to the code base, including functional-group and open-shell symmetry adapted perturbation theory, density-fitted coupled cluster with frozen natural orbitals, orbital-optimized perturbation and coupled-cluster methods (e.g., OO-MP2 and OO-LCCD), density-fitted multiconfigurational self-consistent field, density cumulant functional theory, algebraic-diagrammatic construction excited states, improvements to the geometry optimizer, and the "X2C" approach to relativistic corrections, among many other improvements.

  16. Do independent-particle-model broken-symmetry solutions contain more physics than the symmetry-adapted ones? The case of homonuclear diatomics.

    Science.gov (United States)

    Li, Xiangzhu; Paldus, Josef

    2009-02-28

    We explore spin-preserving, singlet stability of restricted Hartree-Fock (RHF) solutions for a number of closed-shell, homonuclear diatomics in the entire relevant range of internuclear separations. In the presence of such instabilities we explore the implied broken-symmetry (bs) solutions and check their stability. We also address the occurrence of vanishing roots rendered by the stability problem in the case of bs solutions. The RHF bs solutions arise primarily due to the symmetry breaking of the relevant, mostly frontier, molecular orbitals, which approach atomic-type orbitals in the dissociation limit. The resulting bs RHF solutions yield more realistic potential energy curves (PECs) than do the symmetry adapted (sa) solutions. These PECs are shown to be very similar to those rendered by the density functional theory (DFT). Moreover, the sa DFT solutions are found to be stable in a much wider range of internuclear separations than are the RHF solutions, and their bs analogs differ very little from the sa ones. Finally, we examine a possible usefulness of bs RHF solutions in post-HF correlated approaches to the many-electron problem, specifically in the limited configuration interaction and coupled-cluster methods.

  17. Diffusion energy profiles in silica mesoporous molecular sieves modelled with the fragment molecular orbital method

    Science.gov (United States)

    Roskop, Luke; Fedorov, Dmitri G.; Gordon, Mark S.

    2013-07-01

    The fragment molecular orbital (FMO) method is used to model truncated portions of mesoporous silica nanoparticle (MSN) pores. The application of the FMO/RHF (restricted Hartree-Fock) method to MCM-41 type MSNs is discussed and an error analysis is given. The FMO/RHF method is shown to reliably approximate the RHF energy (error ∼0.2 kcal/mol), dipole moment (error ∼0.2 debye) and energy gradient (root mean square [RMS] error ∼0.2 × 10-3 a.u./bohr). Several FMO fragmentation schemes are employed to provide guidance for future applications to MSN models. An MSN pore model is functionalised with (phenyl)propyl substituents and the diffusion barrier for benzene passing through the pore is computed by the FMO/RHF-D method with the Grimme dispersion correction (RHF-D). For the reaction coordinates examined here, the maximum FMO/RHF-D interaction energies range from -0.3 to -5.8 kcal/mol.

  18. Ab initio calculation of UV-absorption spectra of chlorophyll a: Comparison study between RHF/CIS, TDDFT, and semi-empirical methods

    Directory of Open Access Journals (Sweden)

    Veinardi Suendo

    2012-07-01

    Full Text Available Chlorophyll a is one the most abundant pigment on Earth that responsible for trapping the light energy to perform photosynthesis in green plants. This molecule has been studied for many years from different point of views in both experimental and theoretical interests. In this study, the restricted Hartree-Fock configuration interaction single (RHF/CIS, time-dependent density functional theory (TDDFT and several semi-empirical methods (CNDO/s and ZINDO calculations were carried out to reconstruct the UV-Vis absorption spectra of chlorophyll a. In some extend, the calculation results based on single molecule approach were succeeded to reconstruct the absorption spectra but required to be rescaled to fit the experimental one. In general, the semi-empirical methods provide better energy scaling factor that closer to unity. However, they lack of vertical transition fine features with respect to the spectrum obtained experimentally. Here, the ab initio calculations provide more complete features, especially the TDDFT at high level of basis sets that also has a good accuracy in the transition energies. The contribution of ground states and excited states orbitals in the main vertical transitions is discussed based on delocalization nature of the wavefunctions and the presence of solvent through polarizable continuum model (PCM.

  19. Magnetization orientation dependence of the quasiparticle spectrum and hysteresis in ferromagnetic metal nanoparticles

    Science.gov (United States)

    Cehovin, A.; Canali, C. M.; MacDonald, A. H.

    2002-09-01

    We use a microscopic Slater-Koster tight-binding model with short-range exchange and atomic spin-orbit interactions that realistically captures generic features of ferromagnetic metal nanoparticles to address the mesoscopic physics of magnetocrystalline anisotropy and hysteresis in nanoparticle-quasiparticle excitation spectra. Our analysis is based on qualitative arguments supported by self-consistent Hartree-Fock calculations for nanoparticles containing up to 260 atoms. Calculations of the total energy as a function of magnetization direction demonstrate that the magnetic anisotropy per atom fluctuates by several percent when the number of electrons in the particle changes by 1, even for the largest particles we consider. Contributions of individual orbitals to the magnetic anisotropy are characterized by a broad distribution with a mean more than two orders of magnitude smaller than its variance and with no detectable correlations between anisotropy contribution and quasiparticle energy. We find that the discrete quasiparticle excitation spectrum of a nanoparticle displays a complex nonmonotonic dependence on an external magnetic field, with abrupt jumps when the magnetization direction is reversed by the field, explaining recent spectroscopic studies of magnetic nanoparticles. Our results suggest the existence of a broad crossover from a weak spin-orbit coupling to a strong spin-orbit coupling regime, occurring over the range from approximately 200- to 1000-atom nanoparticles.

  20. Projector Augmented Wave formulation of orbital-dependent exchange-correlation functionals

    Science.gov (United States)

    Xu, Xiao; Holzwarth, N. A. W.

    2012-02-01

    The use of orbital-dependent exchange-correlation functionals within electronic structure calculations has recently received renewed attention for improving the accuracy of the calculations, especially correcting self-interaction errors. Since the Projector Augmented Wave (PAW) methodootnotetext P. Bl"ochl, Phys. Rev. B 50, 17953 (1994). is an efficient pseudopotential-like scheme which ensures accurate evaluation of all multipole moments of direct and exchange Coulomb integrals, it is a natural choice for implementing orbital-dependent formalisms. Using Fock exchange as an example of an orbital-dependent functional, we developed the formulation and numerical implementation of the approximate optimized effective potential formalism of Kreiger, Li, and Iafrate (KLI)ootnotetext J. B. Krieger, Y. Li, and G. J. Iafrate Phys. Rev. A 45, 101 (1992). within the PAW method, comparing results with the analogous Hartree-Fock treatment.ootnotetext Xiao Xu and N. A. W. Holzwarth, Phys. Rev. B 81, 245105 (2010); 84, 155113 (2011). Test results are presented for ground state properties of two well-known materials -- diamond and LiF. This formalism can be extended to treat orbital-dependent functionals more generally.

  1. Electron correlation in tunneling ionization of diatomic molecules: An application of the many-electron weak-field asymptotic theory with a generalized-active-space partition scheme

    Science.gov (United States)

    Yue, Lun; Bauch, Sebastian; Madsen, Lars Bojer

    2017-10-01

    The many-electron weak-field asymptotic theory (ME-WFAT) for static tunneling ionization [O. I. Tolstikhin et al., Phys. Rev. A 89, 013421 (2014), 10.1103/PhysRevA.89.013421] is applied to diatomic molecules. In the ME-WFAT, the dependence of the ionization rate on the molecular orientation with respect to the static field direction is determined by the structure factor, which in turn depends on the asymptotic tail of the Dyson orbital. We extract the latter by the time-dependent generalized-active-space configuration-interaction method [S. Bauch et al., Phys. Rev. A 90, 062508 (2014), 10.1103/PhysRevA.90.062508], which takes into account electron correlation effects systematically. Results for the orientation-dependent structure factor are presented for H2 and LiH. Compared to mean-field Hartree-Fock results, the inclusion of electron-electron correlation affects the structure factor, and hence the rate, even for these simple systems.

  2. Coupled cluster calculations of mean excitation energies of the noble gas atoms He, Ne and Ar and of the H2 molecule

    Science.gov (United States)

    Sauer, Stephan P. A.; Haq, Inam Ul; Sabin, John R.; Oddershede, Jens; Christiansen, Ove; Coriani, Sonia

    2014-03-01

    Using an asymmetric Lanczos chain algorithm for the calculation of the coupled cluster linear response functions at the coupled cluster singles and doubles (CCSD) and coupled cluster singles and approximate iterative doubles (CC2) levels of approximation, we have calculated the mean excitation energies of the noble gases He, Ne and Ar, and of the hydrogen molecule (H2). Convergence with respect to the one-electron basis set was investigated in detail for families of correlation-consistent basis sets including both augmentation and core-valence functions. We find that the electron correlation effects at the CCSD level change the mean excitation energies obtained at the uncorrelated Hartree-Fock level by about 1%. For the two-electron systems He and H2, our CCSD results (for a Lanczos chain length equal to the full excitation space), I0 = 42.28 eV (helium) and I0 = 19.62 eV (H2), correspond to full configuration interaction results and are therefore the exact, non-relativistic theoretical values for the mean excitation energy of these two systems within the Bethe theory for the chosen basis set and, in the case of H2, at the experimental equilibrium geometry.

  3. First-principles calculations on anharmonic vibrational frequencies of polyethylene and polyacetylene in the Gamma approximation.

    Science.gov (United States)

    Keçeli, Murat; Hirata, So; Yagi, Kiyoshi

    2010-07-21

    The frequencies of the infrared- and/or Raman-active (k=0) vibrations of polyethylene and polyacetylene are computed by taking account of the anharmonicity in the potential energy surfaces (PESs) and the resulting phonon-phonon couplings explicitly. The electronic part of the calculations is based on Gaussian-basis-set crystalline orbital theory at the Hartree-Fock and second-order Møller-Plesset (MP2) perturbation levels, providing one-, two-, and/or three-dimensional slices of the PES (namely, using the so-called n-mode coupling approximation with n=3), which are in turn expanded in the fourth-order Taylor series with respect to the normal coordinates. The vibrational part uses the vibrational self-consistent field, vibrational MP2, and vibrational truncated configuration-interaction (VCI) methods within the Gamma approximation, which amounts to including only k=0 phonons. It is shown that accounting for both electron correlation and anharmonicity is essential in achieving good agreement (the mean and maximum absolute deviations less than 50 and 90 cm(-1), respectively, for polyethylene and polyacetylene) between computed and observed frequencies. The corresponding values for the calculations including only one of such effects are in excess of 120 and 300 cm(-1), respectively. The VCI calculations also reproduce semiquantitatively the frequency separation and intensity ratio of the Fermi doublet involving the nu(2)(0) fundamental and nu(8)(pi) first overtone in polyethylene.

  4. The effects of strong correlations on the band structure of Ag_8SnSe_6 argyrodite

    Directory of Open Access Journals (Sweden)

    S.V. Syrotyuk

    2016-12-01

    Full Text Available The electronic energy band spectra, as well as partial and total density of electronic states of the crystal argyrodite Ag_8SnSe_6 have been evaluated within the projector augmented waves (PAW approach by means of the ABINIT code. The one-electron energies have been evaluated using two functionals for exchange-correlation energy. The first one is the generalized gradient approximation (GGA approach. The second one is the hybrid functional PBE0 composed of the semilocal GGA part and Hartree-Fock exact exchange non-local energy for strongly correlated 4d electrons of Ag atom. The second approach eliminates the Coulomb self-interaction of the Ag 4d electrons. This leads to a significant restructuring of the energy bands in the filled valence part and to an improved location of the Ag 4d-states on the energy scale, and the resulting value of the band gap is well compared with experiment. The effects of strong correlation on the electronic structure of the crystal argyrodite are considered here for the first time.

  5. Combined experimental and theoretical approaches to the molecular structure of 4-(1-formylnaphthalen-2-yloxy)phthalonitrile.

    Science.gov (United States)

    Tereci, Hidayet; Askeroğlu, İskender; Akdemir, Nesuhi; Uçar, İbrahim; Büyükgüngör, Orhan

    2012-10-01

    The novel compound 4-(1-formylnaphthalen-2-yloxy)phthalonitrile, C(19)H(10)N(2)O(2,) has been synthesized and characterized by IR, UV-vis, NMR and X-ray single-crystal determination. The title compound, is built up from two planar groups (naphthalen and phthalonitrile), with a dihedral angle of 64.10(4)° between them. The crystal structure is stabilized by weak C-H···O hydrogen-bond and π-π interactions. The structural and spectroscopic data of the compound in the ground state have been calculated using density functional theory (DFT) and Hartree-Fock (HF) with the 6-31G(d,p) basis set. The vibrational study was interpreted in terms of potential energy distribution (PED). The observed wave number in FT-IR spectra was analyzed and assigned to different normal modes of the molecule. Using the TD-DFT and TD-HF methods, electronic absorption spectra of the title compound were predicted and good agreement with the TD-DFT method and the experimental determination was found. Isotropic chemical shifts ((13)C and (1)H NMR) were calculated using the gauge-invariant atomic orbital (GIAO) method. The HOMO and LUMO analyses were used to elucidate information regarding charge transfer within the molecule. Copyright © 2012 Elsevier B.V. All rights reserved.

  6. A SAR and QSAR Study of New Artemisinin Compounds with Antimalarial Activity

    Directory of Open Access Journals (Sweden)

    Cleydson Breno R. Santos

    2013-12-01

    Full Text Available The Hartree-Fock method and the 6-31G** basis set were employed to calculate the molecular properties of artemisinin and 20 derivatives with antimalarial activity. Maps of molecular electrostatic potential (MEPs and molecular docking were used to investigate the interaction between ligands and the receptor (heme. Principal component analysis and hierarchical cluster analysis were employed to select the most important descriptors related to activity. The correlation between biological activity and molecular properties was obtained using the partial least squares and principal component regression methods. The regression PLS and PCR models built in this study were also used to predict the antimalarial activity of 30 new artemisinin compounds with unknown activity. The models obtained showed not only statistical significance but also predictive ability. The significant molecular descriptors related to the compounds with antimalarial activity were the hydration energy (HE, the charge on the O11 oxygen atom (QO11, the torsion angle O1-O2-Fe-N2 (D2 and the maximum rate of R/Sanderson Electronegativity (RTe+. These variables led to a physical and structural explanation of the molecular properties that should be selected for when designing new ligands to be used as antimalarial agents.

  7. Spontaneous symmetry breaking approach to La{sub 2}CuO{sub 4} properties: Hints for matching the Mott and Slater pictures

    Energy Technology Data Exchange (ETDEWEB)

    Cabo-Bizet, Alejandro [Departamento de Fisica, Centro de Aplicaciones Tecnologicas y Desarrollo, Nuclear (CEADEN), Calle 30, esq. a 5ta, La Habana (Cuba); Cabo Montes de Oca, Alejandro [Grupo de Fisica Teorica, Instituto de Cibernetica Matematematica y Fisica (ICIMAF), Calle E, No. 309, entre 13 y 15, Vedado, La Habana (Cuba)], E-mail: cabo@icmf.inf.cu

    2009-05-04

    Special solutions of the Hartree-Fock (HF) problem for Coulomb interacting electrons described by a simple model of the Cu-O planes in La{sub 2}CuO{sub 4} are presented. One of the mean field states obtained, is able to predict some of the most interesting properties of this material, such as its insulator character and the antiferromagnetic order. The natural appearance of pseudogaps in some states of this material is also indicated by another of the HF states obtained. These surprising results follow after eliminating spin and crystal symmetry restrictions usually imposed on the single particle HF orbitals, by employing the rotational invariant formulation of the HF scheme originally introduced by Dirac. Therefore, it is exemplified here, how up to know considered strong correlation effects, can be described by improving the HF solution of the considered system. In other words, it has been argued, that defining correlation effects as the ones shown by the system and not predicted by the HF best (lowest energy) solution, allows to explain important, up to know considered as strong correlation properties, as simple mean field ones. The discussion also helps to clarify the role of the antiferromagnetism and pseudogaps in the physical properties of the HTSC materials and indicates a promising way to start conciliating the Mott and Slater pictures in the physics of the transition metal oxides and other strongly correlated electron systems.

  8. Description of the giant monopole resonance in the even-A Sn112-124 isotopes within a microscopic model including quasiparticle-phonon coupling

    Science.gov (United States)

    Tselyaev, V.; Speth, J.; Krewald, S.; Litvinova, E.; Kamerdzhiev, S.; Lyutorovich, N.; Avdeenkov, A.; Grümmer, F.

    2009-03-01

    We have calculated the strength distributions of the isoscalar giant monopole resonance (ISGMR) in the even-A tin isotopes (A=112-124) that were recently measured in inelastic α scattering. The calculations were performed within two microscopic models: the quasiparticle random phase approximation (QRPA) and the quasiparticle time blocking approximation (QTBA), which is an extension of the QRPA including quasiparticle-phonon coupling. We used a self-consistent calculational scheme based on the Hartree-Fock+Bardeen-Cooper-Schrieffer approximation. Within the RPA the self-consistency is full. The single-particle continuum is also exactly included at the RPA level. The self-consistent mean field and the effective interaction are derived from the Skyrme energy functional. In the calculations, two Skyrme force parametrizations were used: T5 with a comparatively low value of the incompressibility modulus of infinite nuclear matter (K∞=202 MeV) and T6 with K∞=236 MeV. The T5 parametrization gives theoretical results for tin isotopes in good agreement with the experimental data including the resonance widths. The results of the ISGMR calculations in Zr90, Sm144, and Pb208 performed with these Skyrme forces are discussed and compared with the experiment.

  9. Quantum chemical density functional theory studies on the molecular structure and vibrational spectra of mannitol

    Science.gov (United States)

    Moorthi, P. P.; Gunasekaran, S.; Swaminathan, S.; Ramkumaar, G. R.

    2015-02-01

    A collective experimental and theoretical study was conducted on the molecular structure and vibrational spectra of mannitol. The FT-IR and FT-Raman spectra of mannitol were recorded in the solid phase. The molecular geometry, vibrational frequencies, thermodynamic functions and atomic charges of mannitol in the ground state have been calculated by using the ab initio HF (Hartree-Fock) and density functional methods (B3LYP) invoking cc-pVDZ basis set. The complete vibrational assignments were performed on the basis of Total Energy Distribution (TED) of the vibrational modes. The UV absorption spectra of the title compound dissolved in water. Natural bond orbital analysis has been carried out to explain the charge transfer or delocalization of charge due to the intra-molecular interactions. The 1H and 13C nuclear magnetic resonance (NMR) chemical shifts of the molecule were calculated by GIAO methods. The first order hyperpolarizability (β0) of this novel molecular system and related properties (β, α0 and Δα) of mannitol are calculated using B3LYP/cc-pVDZ and HF/cc-pVDZ methods on the finite-field approach. By using TD-DFT calculation, electronic absorption spectra of the title compound have been predicted and a good agreement with experimental one is established. In addition, the molecular electrostatic potential (MEP) have been investigated using theoretical calculations, the calculated HOMO and LUMO energies shows that the charge transfer within the molecule.

  10. Merging symmetry projection methods with coupled cluster theory: Lessons from the Lipkin model Hamiltonian.

    Science.gov (United States)

    Wahlen-Strothman, Jacob M; Henderson, Thomas M; Hermes, Matthew R; Degroote, Matthias; Qiu, Yiheng; Zhao, Jinmo; Dukelsky, Jorge; Scuseria, Gustavo E

    2017-02-07

    Coupled cluster and symmetry projected Hartree-Fock are two central paradigms in electronic structure theory. However, they are very different. Single reference coupled cluster is highly successful for treating weakly correlated systems but fails under strong correlation unless one sacrifices good quantum numbers and works with broken-symmetry wave functions, which is unphysical for finite systems. Symmetry projection is effective for the treatment of strong correlation at the mean-field level through multireference non-orthogonal configuration interaction wavefunctions, but unlike coupled cluster, it is neither size extensive nor ideal for treating dynamic correlation. We here examine different scenarios for merging these two dissimilar theories. We carry out this exercise over the integrable Lipkin model Hamiltonian, which despite its simplicity, encompasses non-trivial physics for degenerate systems and can be solved via diagonalization for a very large number of particles. We show how symmetry projection and coupled cluster doubles individually fail in different correlation limits, whereas models that merge these two theories are highly successful over the entire phase diagram. Despite the simplicity of the Lipkin Hamiltonian, the lessons learned in this work will be useful for building an ab initio symmetry projected coupled cluster theory that we expect to be accurate in the weakly and strongly correlated limits, as well as the recoupling regime.

  11. Application of the graphical unitary group approach to the energy second derivative for CI wave functions via the coupled perturbed CI equations

    Energy Technology Data Exchange (ETDEWEB)

    Fox, D.J.

    1983-10-01

    Analytic derivatives of the potential energy for Self-Consistent-Field (SCF) wave functions have been developed in recent years and found to be useful tools. The first derivative for configuration interaction (CI) wave functions is also available. This work details the extension of analytic methods to energy second derivatives for CI wave functions. The principal extension required for second derivatives is evaluation of the first order change in the CI wave function with respect to a nuclear perturbation. The shape driven graphical unitary group approach (SDGUGA) direct CI program was adapted to evaluate this term via the coupled-perturbed CI equations. Several iterative schemes are compared for use in solving these equations. The pilot program makes no use of molecular symmetry but the timing results show that utilization of molecular symmetry is desirable. The principles for defining and solving a set of symmetry adapted equations are discussed. Evaluation of the second derivative also requires the solution of the second order coupled-perturbed Hartree-Fock equations to obtain the correction to the molecular orbitals due to the nuclear perturbation. This process takes a consistently higher percentage of the computation time than for the first order equations alone and a strategy for its reduction is discussed.

  12. Increase of spin dephasing times in a 2D electron system with degree of initial spin polarization

    Science.gov (United States)

    Stich, D.; Korn, T.; Schulz, R.; Schuh, D.; Wegscheider, W.; Schüller, C.

    2008-03-01

    We report on time-resolved Faraday/Kerr rotation measurements on a high-mobility 2D electron system. A variable initial spin polarization is created in the sample by a circularly polarized pump pulse, and the spin polarization is tracked by measuring the Faraday/Kerr rotation of a time-delayed probe pulse. By varying the pump intensity, the initial spin polarization is changed from the low-polarization limit to a polarization degree of several percent. The observed spin dephasing time increases from less than 20 ps to more than 200 ps as the initial spin polarization is increased. To exclude sample heating effects, additional measurements with constant pump intensity and variable degree of circular polarization are performed. The results confirm the theoretical prediction by Weng and Wu [Phys. Rev. B 68 (2003) 075312] that the spin dephasing strongly depends on the initial spin polarization degree. The microscopic origin for this is the Hartree-Fock term in the Coulomb interaction, which acts as an effective out-of plane magnetic field.

  13. Effect of tensor correlations on the depletion of nuclear Fermi sea within the extended BHF approach

    Science.gov (United States)

    Yin, Peng; Dong, Jianmin; Zuo, Wei

    2017-11-01

    We have investigated the effect of tensor correlations on the depletion of the nuclear Fermi sea in symmetric nuclear matter within the framework of the extended Brueckner-Hartree-Fock approach by adopting the AV 18 two-body interaction and a microscopic three-body force. The contributions from various partial wave channels including the isospin-singlet T=0 channel, the isospin-triplet T=1 channel and the T=0 tensor 3 SD 1 channel have been calculated. The T=0 neutron-proton correlations play a dominant role in causing the depletion of nuclear Fermi sea. The T=0 correlation-induced depletion turns out to stem almost completely from the 3 SD 1 tensor channel. The isospin-singlet T=0 3 SD 1 tensor correlations are shown to be responsible for most of the depletion, which amounts to more than 70 percent of the total depletion in the density region considered. The three-body force turns out to lead to an enhancement of the depletion at high densities well above the empirical saturation density and its effect increases as a function of density. Supported by National Natural Science Foundation of China (11435014, 11175219), the 973 Program of China (2013CB834405) and the Knowledge Innovation Project (KJCX2-EW-N01) of the Chinese Academy of Sciences

  14. The role of electron-electron repulsion in the problem of epitaxial graphene on a metal: Simple estimates

    Science.gov (United States)

    Davydov, S. Yu.

    2017-08-01

    For single-layer graphene placed on a metal substrate, the influence of intra- and interatomic Coulomb repulsion of electrons ( U and G, respectively) on its phase diagram is considered in the framework of an extended Hartree-Fock theory. The general solution of the problem is presented, on the basis of which special cases allowing for analytical consideration are analyzed: free and epitaxial graphene with and without regard for the energy of the electron transition between neighboring atoms of graphene. Three regions of the phase diagram are considered: spin and charge density waves (SDW and CDW, respectively) and the semimetal (SM) state uniform in the spin and charge. The main attention is paid to undoped graphene. It is shown that the allowance for the interaction with a metal substrate expands the SM existence domain. However, in all the considered cases, the boundary between the SDW and CDW states is described by the equation U = zG, where z = 3 is the number of nearest neighbors in graphene. The widening of the SM state region also results from the doping of graphene, and the effect is independent of the sign of free carriers introduced into epitaxial graphene by the substrate. According to estimates made, the only state possible in the buffer layer is the metal-type SM state, whereas, in epitaxial graphene, the CDW state is possible. The influence of temperature on the phase diagram of epitaxial graphene is discussed.

  15. Interactive Macroeconomics

    Science.gov (United States)

    Di Guilmi, Corrado; Gallegati, Mauro; Landini, Simone

    2017-04-01

    Preface; List of tables; List of figures, 1. Introduction; Part I. Methodological Notes and Tools: 2. The state space notion; 3. The master equation; Part II. Applications to HIA Based Models: 4. Financial fragility and macroeconomic dynamics I: heterogeneity and interaction; 5. Financial fragility and macroeconomic Dynamics II: learning; Part III. Conclusions: 6. Conclusive remarks; Part IV. Appendices and Complements: Appendix A: Complements to Chapter 3; Appendix B: Solving the ME to solve the ABM; Appendix C: Specifying transition rates; Index.

  16. Interactive Governance

    DEFF Research Database (Denmark)

    Bang, Henrik

    2016-01-01

    Governance analysis has exploded in recent years, and it has become nearly impossible to tell what difference the concept and practice of governance makes from those of government and state. In addition governance analysis has been placed more and more in the shadow of the new institutionalisms and...... and growth. However, interactive governance is not a property or effect of institutions; nor does it apply solely to those individuals who seek success above everything else. It is connective more than individualistic or collectivistic in nature; and it manifests a governability capacity which...

  17. Interactive Workspaces

    DEFF Research Database (Denmark)

    Mogensen, Preben Holst

    Many application domains such as architecture, engineering, industrial design, city planning, environmental supervision, health care etc. share the properties of users working collaboratively with complex mixtures of physical and digital materials. Studies in such domains show that it is hard...... augmented reality, interactive building elements, and mobile devices to support new ways of working in a diversity of application domains with work situations ranging from individual work, through local collaboration, to distributed collaboration. The work situations may take place in offices/project rooms...

  18. Electromagnetic interactions

    CERN Document Server

    Bosanac, Slobodan Danko

    2016-01-01

    This book is devoted to theoretical methods used in the extreme circumstances of very strong electromagnetic fields. The development of high power lasers, ultrafast processes, manipulation of electromagnetic fields and the use of very fast charged particles interacting with other charges requires an adequate theoretical description. Because of the very strong electromagnetic field, traditional theoretical approaches, which have primarily a perturbative character, have to be replaced by descriptions going beyond them. In the book an extension of the semi-classical radiation theory and classical dynamics for particles is performed to analyze single charged atoms and dipoles submitted to electromagnetic pulses. Special attention is given to the important problem of field reaction and controlling dynamics of charges by an electromagnetic field.

  19. Ab initio and DFT study of Octanitrocubane. | Ejuh | Journal of the ...

    African Journals Online (AJOL)

    The molecular stability, structure, dipole moment, charge transfer, polarizability and energy of Octonitrocubane have been studied by using ab- initio Quantum Mechanical calculations. We have used the Restricted Hartree-Fock (RHF) and density functional Becke3LYP (B3LYP) theories by employing 6-31G, 6- 31++G** and ...

  20. Closed-shell variational quantum Monte Carlo simulation for the ...

    African Journals Online (AJOL)

    Closed-shell variational quantum Monte Carlo simulation for the electric dipole moment calculation of hydrazine molecule using casino-code. ... Nigeria Journal of Pure and Applied Physics ... The variational quantum Monte Carlo (VQMC) technique used in this work employed the restricted Hartree-Fock (RHF) scheme.

  1. Linear response at the 4-component relativistic level

    DEFF Research Database (Denmark)

    Saue, T.; Jensen, Hans Jørgen Aagaard

    2003-01-01

    The theory, implementation, and application of linear response at the 4-component relativistic closed-shell Hartree-Fock level based on the concept of quasienergy and time averaging are reported. As such, an efficient AO-driven algorithm is obtained by assigning specific Hermiticity and time reve...

  2. Octupole correlations in superdeformed nuclei; Correlations octupolaires dans les noyaux superdeformes

    Energy Technology Data Exchange (ETDEWEB)

    Dancer, H.; Meyer, J.; Perries, S. [Inst.. de Physique Nucleaire, Lyon-1 Univ., 69 - Villeurbanne (France); Bonche, P. [Service de Physique Theorique, CEA Centre d`Etudes de Saclay, 91 - Gif-sur-Yvette (France); Flocard, H. [Inst. de Physique Nucleaire, Paris-11 Univ., 91 - Orsay (France); Heenen, P.H. [Universite Libre de Bruxelles (Belgium)

    1998-12-31

    Octupole correlations have been investigated within the Generator Coordinate Method based upon Hartree-Fock plus BCS wavefunctions. GCM states corresponding to the q{sub 30} and q{sub 32} modes have been built up to describe the SD excited bands which have been recently observed as negative parity bands. (authors) 4 refs., 1 fig. Short communication

  3. Hydrodynamical approach to the difference between neutron and proton radii

    Energy Technology Data Exchange (ETDEWEB)

    Stringari, S.; Lipparini, E. (Trento Univ. (Italy). Dipartimento di Fisica)

    1982-11-11

    The difference between the neutron and proton radii is investigated using a hydrodynamical approach. A comparison with Hartree-Fock calculations and the predictions of the liquid droplet model is made. The role of the surface symmetry energy and of the Coulomb force is discussed in details.

  4. Charge exchange excitations in N not = Z nuclei: Vlasov and hydrodynamic equations

    Energy Technology Data Exchange (ETDEWEB)

    Lipparini, E.; Stringari, S.

    1987-06-01

    Macroscopic equations of motion for charge exchange reactions in N not = Z nuclei are derived starting from the time dependent Hartree-Fock theory. Application is made to the study of the dipole giant resonance in isospin channels and ..mu..- capture in N not = Z nuclei.

  5. Assessing the performance of the random phase approximation for exchange and superexchange coupling constants in magnetic crystalline solids

    DEFF Research Database (Denmark)

    Olsen, Thomas

    2017-01-01

    . It is found that the RPA can accurately correct the large errors introduced by Hartree- Fock, independent of the input orbitals used for the perturbative expansion. However, in most cases, accuracies similar to RPA can be obtained with DFT+ U, which is significantly simpler from a computational point of view....

  6. Microscopic study of low-lying collective bands in 77Kr

    Indian Academy of Sciences (India)

    The structure of the collective bands in 77Kr is investigated within our deformed shell model (DSM) based on Hartree-Fock states. The different levels are classified into collective bands on the basis of their (2) values. The calculated = 5/2+ ground band agrees reasonably well with the experiment. An attempt has been ...

  7. Attosecond photoionization dynamics in neon

    DEFF Research Database (Denmark)

    Omiste, Juan J.; Madsen, Lars Bojer

    2018-01-01

    We study the role of electron-electron correlation in the ground-state of Ne, as well as in photoionization dynamics induced by an attosecond XUV pulse. For a selection of central photon energies around 100 eV, we find that while the mean-field time-dependent Hartree-Fock method provides qualitat...

  8. Wigner’s phase-space function and atomic structure: II. Ground states for closed-shell atoms

    DEFF Research Database (Denmark)

    Springborg, Michael; Dahl, Jens Peder

    1987-01-01

    display and analyze the function for the closed-shell atoms helium, beryllium, neon, argon, and zinc in the Hartree-Fock approximation. The quantum-mechanical exact results are compared with those obtained with the approximate Thomas-Fermi description of electron densities in phase space....

  9. Open-ended response theory with polarizable embedding

    DEFF Research Database (Denmark)

    Steindal, Arnfinn Hykkerud; Beerepoot, Maarten T P; Ringholm, Magnus

    2016-01-01

    We present the theory and implementation of an open-ended framework for electric response properties at the level of Hartree-Fock and Kohn-Sham density functional theory that includes effects from the molecular environment modeled by the polarizable embedding (PE) model. With this new state-of-th...

  10. Browse Title Index

    African Journals Online (AJOL)

    Items 301 - 350 of 650 ... Vol 2, No 2 (2009), Future prospects for ethanol fuel use - a review, Abstract PDF. G Ahmed, S ... Vol 10, No 1 (2017), Geometry optimization and vibrational frequencies of tetracene molecule in gas phase and in methanol based on Density Funtional Theory and Restricted Hartree-Fock, Abstract PDF.

  11. Mean-field models and exotic nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Bender, M.; Buervenich, T.; Maruhn, J.A.; Greiner, W. [Inst. fuer Theoretische Physik, Univ. Frankfurt (Germany); Rutz, K. [Inst. fuer Theoretische Physik, Univ. Frankfurt (Germany)]|[Gesellschaft fuer Schwerionenforschung mbH, Darmstadt (Germany); Reinhard, P.G. [Inst. fuer Theoretische Physik, Univ. Erlangen (Germany)

    1998-06-01

    We discuss two widely used nuclear mean-field models, the relativistic mean-field model and the (nonrelativistic) Skyrme-Hartree-Fock model, and their capability to describe exotic nuclei. Test cases are superheavy nuclei and neutron-rich Sn isotopes. New information in this regime helps to fix hitherto loosely determined aspects of the models. (orig.)

  12. Density functional theory study of vibrational spectra, and ...

    Indian Academy of Sciences (India)

    The FTIR and FT Raman spectra of dacarbazine were recorded in the regions 4000-400 and 3500-100 cm-1, respectively. The optimized geometry, wavenumber, polarizability and several thermodynamic properties of dacarbazine were studied using ab initio Hartree-Fock, MP2 and DFT methods. A complete vibrational ...

  13. Download this PDF file

    African Journals Online (AJOL)

    pc

    (HOMO) and lowest unoccupied molecular orbital energy (LUMO) are very popular quantum chemical parameters. ... quantum mechanical calculations at the Restricted. Hartree-Fock (RHF) and Density Functional Theory ... amount of energy is needed to break them. On the other hand, at both levels of theory, the bonds.

  14. Ab initio calculations on 2,6-dimethylphenol and 4-(2,6-dimethylphenoxy)-2,6-dimethylphenol. Evidence of an important role for the phenoxonium cation in the copper-catalyzed oxidative phenol coupling reaction

    NARCIS (Netherlands)

    Baesjou, PJ; Driessen, WL; Challa, G; Reedijk, J

    1997-01-01

    Ab initio unrestricted Hartree-Fock calculations with a 6-31G* basis set were performed on 2, 6-dimethylphenol (DMP or monomer) and 4-(2, 6-dimethylphenoxy)-2, 6-dimethylphenol (dimer) to gain more insight into the mechanism of the copper-catalyzed oxidative phenol coupling reaction. Atomic charges

  15. Charge ordering and magnetism in quarter-filled Hubbard-Holstein model

    NARCIS (Netherlands)

    Kumar, S.; van den Brink, J.

    2008-01-01

    We study a two-dimensional Hubbard-Holstein model with phonons treated in the adiabatic limit. A Hartree-Fock decomposition is employed for the Hubbard term. A range of electronic densities are discussed with special emphasis on the quarter filling (n=0.5). We argue that the quarter-filled system is

  16. Relativistic versus non-relativistic mean field

    Science.gov (United States)

    Reinhard, Paul-Gerhard

    Three variants of the relativistic mean-field model (RMF) and the nonrelativistic Skyrme-Hartree-Fock model (SHF) are compared. Overall quality, predictive power, and correlations between observables are addressed using statistical analysis on the basis of least squares fits. Appropriate density dependence is a crucial ingredient for good performance of RMF. However, SHF shows still more flexibility particularly in the isovector channel.

  17. FROM NUCLEAR-MATTER TO FINITE NUCLEI .2. RELATIVISTIC THEORIES FOR FINITE NUCLEI

    NARCIS (Netherlands)

    BOERSMA, HF; MALFLIET, R

    We discuss various relativistic models describing ground-state properties of spherical nuclei. Relativistic mean-field and Hartree-Fock theories, which serve as a starting point for subsequent models, are reviewed. Using a density-dependent parametrization of the Dirac-Brueckner G matrix in nuclear

  18. LINE EMISSION FROM C6+, O8++LI ELECTRON-CAPTURE COLLISIONS

    NARCIS (Netherlands)

    OLSON, RE; PASCALE, J; HOEKSTRA, R

    1992-01-01

    Electron capture cross sections to nl sublevels have been calculated for 1-10 keV u-1 collisions of C6+ and O8+ projectiles on a Li target. The classical trajectory Monte Carlo method has been employed with the initial phase distributions for the Li(2s) target obtained from Hartree-Fock

  19. Bloch-Messiah theorem at finite temperature

    Science.gov (United States)

    Tanabe, K.; Sugawara-Tanabe, K.

    1991-03-01

    The Bloch-Messiah theorem is extended to the thermal Hartree-Fock-Bogoliubov (THFB) theory by making use of the thermo field dynamics. This enables us to define the correct order parameter describing the superconducting phase at finite temperature, and demonstrates consistency of the THFB formalism.

  20. Distributed Gaussian basis sets : Variationally optimized s-type sets for H-2, LiH, and BH

    NARCIS (Netherlands)

    Glushkov, VN; Wilson, S

    2002-01-01

    Distributed basis sets of s-type Gaussian functions are determined by invoking the variation principle for the Hartree-Fock ground states of the H-2, LiH, and BH molecules at their respective experimental equilibrium geometries. The calculated energy expectation values supported by these finite

  1. Elongation Cutoff Technique: Parallel Performance

    Directory of Open Access Journals (Sweden)

    Jacek Korchowiec

    2008-01-01

    Full Text Available It is demonstrated that the elongation cutoff technique (ECT substantially speeds up thequantum-chemical calculation at Hartree-Fock (HF level of theory and is especially wellsuited for parallel performance. A comparison of ECT timings for water chains with thereference HF calculations is given. The analysis includes the overall CPU (central processingunit time and its most time consuming steps.

  2. Auger yield calculations for medical radioisotopes

    Directory of Open Access Journals (Sweden)

    Lee Boon Q.

    2015-01-01

    Full Text Available Auger yields from the decays of 71Ge, 99mTc, 111In and 123–125I have been calculated using a Monte Carlo model of the Auger cascade that has been developed at the ANU. In addition, progress to improve the input data of the model has been made with the Multiconfiguration Dirac-Hartree-Fock method.

  3. Author Details

    African Journals Online (AJOL)

    Keuvi, AU. Vol 8, No 1 (2006): Serie E - Articles Etude hartree-fock de la tautomerisation du 1azirene sous pression d'hydrogene en presence du chlorure de palladium. Abstract. ISSN: 1027-1988. AJOL African Journals Online. HOW TO USE AJOL... for Researchers · for Librarians · for Authors · FAQ's · More about AJOL ...

  4. Page 1 974. B M Deb Table 1. Atomic kinetic energies (a.u.). Hartree ...

    Indian Academy of Sciences (India)

    N-representability criteria were satisfied by taking p(r) = db (r)'. Equation (17) then leads to the new nonlinear DFT equation (Deb and Ghosh 1983). - V+ Vird = u(b. (20). Equation (20) was solved numerically for Ne, Ar, Krand Xe, by using model potentials. This gave p(r) and E, in good agreement with Hartree-Fock results.

  5. THEORETICAL STUDY (AB INITIO AND DFT METHODS) ON ...

    African Journals Online (AJOL)

    Theoretical study on acidic dissociation constant of xylenol orange in aqueous solution. Bull. Chem. Soc. Ethiop. 2017, 31(1). 129 modeled. Hartree-Fock ab initio and density functional geometry optimizations were performed with the Gaussian 09 program. The optimizations were done using HF/6-31+G(d) method. The.

  6. Shape change in Hf, W and Os-isotopes: A non-relativistic Hartree ...

    Indian Academy of Sciences (India)

    Home; Journals; Pramana – Journal of Physics; Volume 62; Issue 4. Shape change in Hf, W and Os-isotopes: A non-relativistic Hartree-Fock versus relativistic Hartree approximation. Z Naik B K Sharma T K Jha P Arumugam S K Patra. Research Articles Volume 62 Issue 4 April 2004 pp 827-839 ...

  7. Ab initio computations on small copper compounds-CuO

    NARCIS (Netherlands)

    Boer, D.H.W. den; Kaleveld, E.W.

    1980-01-01

    Ab initio computations on CuO were performed with the Hartree-Fock method and a proper dissociation MC SCF procedure. In particular the influence of the GTO basis set for Cu in molecular computations has been studied. A potential energy curve and a Mulliken population analysis are presented. The

  8. Investigation of the Effects of Expectation Values for Radii on the ...

    Indian Academy of Sciences (India)

    2016-01-27

    Jan 27, 2016 ... Transition probabilities for some excited s–p and p–s transition arrays of neutral nitrogen have been calculated using the weakest bound electron potential model theory (WBEPMT) for the investigation of effects of expectation values of radii.We have used both numerical non-relativistic Hartree-Fock (NRHF) ...

  9. Massive Skyrmions in quantum Hall ferromagnets

    NARCIS (Netherlands)

    Abolfath, M.; Mullen, K.; Stoof, H.T.C.

    2001-01-01

    We apply the theory of elasticity to study the effects of Skyrmion mass on lattice dynamics in quantum Hall systems. We find that massive Skyrme lattices behave like a Wigner crystal in the presence of a uniform perpendicular magnetic field. We make a comparison with the microscopic Hartree-Fock

  10. Semiempirical and DFT Investigations of the Dissociation of Alkyl Halides

    Science.gov (United States)

    Waas, Jack R.

    2006-01-01

    Enthalpy changes corresponding to the gas phase heats of dissociation of 12 organic halides were calculated using two semiempirical methods, the Hartree-Fock method, and two DFT methods. These calculated values were compared to experimental values where possible. All five methods agreed generally with the expected empirically known trends in the…

  11. Role of nuclear spin-orbit coupling on the constitution of the outer crust of a nonaccreting neutron star

    Directory of Open Access Journals (Sweden)

    Chamel N.

    2017-01-01

    Full Text Available The role of the nuclear spin-orbit coupling on the equilibrium composition and on the equation of state of the outer crust of a nonaccreting neutron star is studied by employing a series of three different nuclear mass models based on the self-consistent Hartree-Fock-Bogoliubov method.

  12. On the applicability of deformed jellium model to the description of metal clusters

    DEFF Research Database (Denmark)

    Lyalin, Andrey G.; Matveentsev, Anton; Solov'yov, Ilia

    2003-01-01

    This work is devoted to the elucidation the applicability of jellium model to the description of alkali cluster properties on the basis of comparison the jellium model results with those derived from experiment and within ab initio theoretical framework. On the basis of the Hartree-Fock and local...

  13. a density functional theory study of substituted and bridged ...

    African Journals Online (AJOL)

    In this work the electronic and thermodynamic properties of both neutral and radical cationic oligothiophene chains with up to eight thiophene units, substituted and bridged oligothiophenes are investigated by performing hybrid DFT (BH and HLYP) and Hartree-Fock calculations using 6-31G* and 6-311G** basis sets.

  14. K X-ray relative transition probabilities for 23 <= Z <= 33

    CERN Document Server

    Chen Xi Meng; Liu Zhao Yuan; Ma Shu Xun; Zhang Hua Lin; Cai Xiao

    2003-01-01

    The K X-ray relative transition probabilities K beta/K alpha of some elements for atomic numbers 23 <= Z <= 33 induced by 3 MeV protons were measured. The experimental results are compared with the relativistic Hartree-Fock (RHF) calculations. Good agreements have been obtained considering the experimental error.

  15. Fission properties of the Barcelona-Catania-Paris energy density functional

    Energy Technology Data Exchange (ETDEWEB)

    Robledo, L M [Dep. Fisica Teorica (Modulo 15), Universidad Autonoma de Madrid, E-28049 Madrid (Spain); Baldo, M [Instituto Nazionale di Fisica Nucleare, Sezione di Catania, Via Santa Sofia 64, I-95123 Catania (Italy); Schuck, P [Institut de Physique Nucleaire, CNRS, UMR8608, F-91406 Orsay (France); Vinas, X, E-mail: luis.robledo@uam.es [Departament d' Estructura i Constituents de la Materia and Institut de Ciencies del Cosmos, Facultat de Fisica, Universitat de Barcelona, Diagonal 647, 08028 Barcelona (Spain)

    2011-09-16

    Fission properties of the Barcelona-Catania-Paris (BCP) energy density functional are explored by performing constrained mean field Hartree-Fock-Bogoliubov (HFB) calculations along the fission path. These calculations provide us with the quantities required to estimate the spontaneous fission half lives and fragment mass distribution. The results obtained are compared to experimental data and other calculations.

  16. Distributed Gaussian basis sets : Variationally optimized s-type sets for the open-shell systems HeH and BeH

    NARCIS (Netherlands)

    Glushkov, VN; Wilson, S

    2004-01-01

    Distributed basis sets of s-type Gaussian functions are determined by invoking the variation principle for the restricted open-shell matrix Hartree-Fock ground states of the open-shell molecular systems HeH and BeH for nuclear separations of 1.500 bohr and 2.500 bohr, respectively. The calculated

  17. Quantum theory of matter - cohesive and spectral properties. Final technical report, 1 July 1974--30 June 1975. [Quantium Chemistry Group, Uppsala Univ. Sweden

    Energy Technology Data Exchange (ETDEWEB)

    Loewdin, P.; Calais, J.L.; Goscinski, O.

    1976-12-01

    Contents: Combination of special relativity and quantum mechanics; Trace algebra and chemical kinetics; Characterization of truncated basis sets by means of error quotients; General spin orbitals in Hartree-Fock theory; Cohesive properties of ionic crystals; and Description of ionization and excitation by means of transition operators.

  18. RHF and DFT study of the optimized molecular structure and atomic ...

    African Journals Online (AJOL)

    Restricted HartreeFock (RHF) and Density Functional Theory (DFT) studies were carried out on the organic semi conductor material Pentacene. 6-31G and 6-31G* basis sets were used to optimize the molecule and compute the charge distribution at both levels of theory. The results show that the Carbon-Hydrogen bonds in ...

  19. effect of side chain length on the stability and structural properties of 3

    African Journals Online (AJOL)

    Preferred Customer

    PROPERTIES OF 3-(2',5'-DIALKOXYPHENYL)THIOPHENES: A THEORETICAL. STUDY ... applications of these materials in various electronic devices such as solar cells, electrochromic displays (ECD), light ... Hartree-Fock (HF) and Density Functional Theory (DFT) methods to understand the difference in stabilities and ...

  20. Author Details

    African Journals Online (AJOL)

    The effect of water solubles on Kelvin effects of the Maritime Polluted aerosols. Abstract PDF · Vol 10, No 1 (2017) - Articles Geometry optimization and vibrational frequencies of tetracene molecule in gas phase and in methanol based on Density Funtional Theory and Restricted Hartree-Fock Abstract PDF. ISSN: 2006-6996.

  1. Structural and vibrational spectral studies on hydrogen bonded salts ...

    Indian Academy of Sciences (India)

    compounds were optimized with the Density Functional Theory (DFT) using B3LYP function and the Hartree-. Fock (HF) level with a6-311++G(d ... which have more importance in the areas of molecular recognition, crystal engineering ... acceptor sites, viz., nitrogen and chlorine atoms in the present case. The present work ...

  2. Dirac-Fock atomic electronic structure calculations using different nuclear charge distributions

    NARCIS (Netherlands)

    Visscher, L; Dyall, KG

    1997-01-01

    Numerical Hartree-Fock calculations based on the Dirac-Coulomb Hamiltonian for the first 109 elements of the periodic table are presented. The results give the total electronic energy, as a function of the nuclear model that is used, for four different models of the nuclear charge distribution. The

  3. On the convergence of zero-point vibrational corrections to nuclear shieldings and shielding anisotropies towards the complete basis set limit in water

    DEFF Research Database (Denmark)

    Faber, Rasmus; Buczek, Aneta; Kupka, Teobald

    2017-01-01

    The method and basis set dependence of zero-point vibrational corrections (ZPVC) to NMR shielding constants and anisotropies has been investigated using water as a test system. A systematic comparison has been made using the Hartree-Fock (HF), second-order Møller-Plesset perturbation theory (MP2...

  4. Experimental studies on the K{beta}/K{alpha} intensity ratio of Zn at different thickness and pressure

    Energy Technology Data Exchange (ETDEWEB)

    Icelli, Orhan E-mail: orhan_icelli@hotmail.com; Erzeneoglu, Salih

    2004-01-15

    K{beta}/K{alpha} intensity ratios of Zn were measured at a photon excitation energy of 59.5 keV using a high-resolution Si(Li) detector for several thickness at different pressure. Present results were compared with theoretical data and other experimental values. The results were in good agreement theoretical values based on Hartree-Fock theory.

  5. On the importance of excited state dynamic response electron correlation in polarizable embedding methods

    DEFF Research Database (Denmark)

    Eriksen, Janus J.; Sauer, Stephan P. A.; Mikkelsen, Kurt Valentin

    2012-01-01

    We investigate the effect of including a dynamic reaction field at the lowest possible ab inito wave function level of theory, namely the Hartree-Fock (HF) Self-Consistent Field (SCF) level within the Polarizable Embedding (PE) formalism. We formulate HF based PE within the linear response theory...

  6. An ab initio SCF calculation of the polarizability tensor of sulphur dioxide

    Science.gov (United States)

    Bacskay, George G.

    1983-08-01

    The principal components of the static electric dipole polarizability have been calculated by an ab initio coupled perturbed Hartree-Fock (CPHF) method. The calculated components are sufficiently accurate so that a choice can be made between the two different sets of experimentally consistent values in favor of the negative anisotropy parameter αxx-ᾱ.

  7. Ab Initio Calculations of Oxosulfatovanadates

    DEFF Research Database (Denmark)

    Frøberg, Torben; Johansen, Helge

    1996-01-01

    Restricted Hartree-Fock and multi-configurational self-consistent-field calculations together with secondorder perturbation theory have been used to study the geometry, the electron density, and the electronicspectrum of (VO2SO4)-. A bidentate sulphate attachment to vanadium was found to be stabl...

  8. A theoretical study of the cohesion of noble gases on graphite.

    Science.gov (United States)

    Bichoutskaia, Elena; Pyper, Nicholas C

    2008-01-14

    The interactions of the noble gases with a graphene sheet are investigated theoretically. The short range repulsive interaction between the noble gas and each carbon atom is described using Hartree-Fock atomic densities and a local density functional theory with the exchange functional corrected for the finite range of the interaction by introducing a Rae-type correction depending on the effective number of electrons. The long range interactions are introduced as the sum of the Axilrod-Teller triple-dipole interaction plus the dipole-dipole and dipole-quadrupole dispersive attractions damped according to the theory of Jacobi and Csanak. The energy arising from the interactions between the permanent quadrupoles on the carbon atoms with the dipole they induce on the noble gas is negligible, being nonzero only on account of the atomistic structure of graphene. The mobile and delocalized nature of the graphene pi electrons causes the effective number of electrons to be around 500 rather than that of 12 appropriate for a system of entirely localized interactions with individual carbon atoms. Inclusion of the Axilrod-Teller term is required to obtain reliable predictions for the binding energies and equilibrium geometries. Absorption of a noble gas atom is predicted to occur at the site above the center of a six membered ring although this is preferred over two other sites by only about 5 meV. The methods presented for generating all the potentials can be applied to derive the interactions between any ion and carbon atom in the wall of a single-walled nanotube. Knowledge of these interactions is required to study the alkali halide nanocrystals encapsulated in single-walled carbon nanotubes of current interest.

  9. Separation of Methylene Blue Dye from Aqueous Solution Using Triton X-114 Surfactant

    Directory of Open Access Journals (Sweden)

    Arunagiri Appusamy

    2014-01-01

    Full Text Available In this study, the interaction energy between Triton X-114 surfactant + methylene blue or water and methylene blue + water was investigated using Hartree-Fock (HF theory with 6-31G* basis set. The results of structures and interaction energies show that these complexes have good physical and chemical interactions at atom and molecular levels. However, the Triton X-114 surfactant + methylene blue complex shows stronger molecular interaction compared to other complexes systems. The order of the interaction energy is 4303.472023 (Triton X-114 surfactant + water > -1222.962 (methylene blue + water > -3573.28 (Triton X-114 surfactant + methylene blue kJ·mole−1. Subsequently, the cloud point extraction was carried out for 15 ppm of methylene blue in a mixture at 313.15 and 323.15 K over the surfactant concentration range from 0.01 M to 0.1 M. From the measured data, the excess molar volume was calculated for both phases. The results show a positive deviation in the dilute phase and a negative deviation in the surfactant rich phase. It is confirmed that the interaction between Triton X-114 and methylene blue is stronger than other complex systems due to the presence of chemical and structural orientation. The concentration of dyes and surfactant in the feed mixture and temperature effect in both phases has been studied. In addition, the thermodynamics feasibility and efficiency of the process have also been investigated.

  10. Drug Interaction API

    Data.gov (United States)

    U.S. Department of Health & Human Services — The Interaction API is a web service for accessing drug-drug interactions. No license is needed to use the Interaction API. Currently, the API uses DrugBank for its...

  11. Reactions of exotic nuclei with the quark-meson coupling model

    Science.gov (United States)

    McRae, E.; Simenel, C.; Simpson, E. C.; Thomas, A. W.

    2017-11-01

    The nucleon-nucleon interaction is an important requirement for investigations of nuclear structure and reactions, as well as for astrophysical models such as r-process nucleosynthesis and neutron stars. The traditional approach to low-energy nuclear physics is to treat nucleons as immutable objects interacting via phenomenological forces. The use of phenomenological interactions, rather than one derived from a microscopic theory, raises questions as to the reliability of predictions for exotic regions of the nuclear chart. The quark-meson coupling (QMC) model uses a relativistic mean-field approach to provide a microscopically derived nucleon-nucleon interaction, which takes into account the quark structure of the nucleon. The Skyrme energy density functional is a popular phenomenological tool in studies of nuclear structure and reactions. In this work, the QMC density functional was used to produce a set of Skyrme parameterisations, in the hopes that they will give more reliable predictions for exotic nuclei. In conjunction with Hartree-Fock-Bogoliubov (HFB) calculations, the Skyrme-QMC (SQMC) parameterisations have been used to model the ground-state properties of individual nuclei and nucleus-nucleus potentials for Ca + Sn reactions. The SQMC parameterisation performs with an accuracy comparable to modern phenomenological functionals. From this, one can investigate the importance of the isovector terms of the nucleon-nucleon interaction, which are particularly significant for exotic, neutron-rich regions of the nuclear chart. One of the notable successes of the QMC model is its derivation of nuclear spin-orbit coupling. The isovector dependence of the spin-orbit equation of state is remarkably similar to that of the modern UNEDF1 phenomenological density functional. HFB calculations along the Sn isotopic chain reveal that the isovector properties of the spin-orbit term impact binding energies to a level that will be significant for astrophysical r

  12. Problem of interactions: electromagnetic particles interaction

    CERN Document Server

    Sannikov-Proskuryakov, S S

    2001-01-01

    The electromagnetic interactions between charged particles are derived on the basis of the particles dynamic theory, proposed in the work of Sannikov. The electromagnetic interactions exist only in the relativistic model of the bihamiltonian system, based on the Heisenberg algebra. Existence of this type of interactions is connected with the U sub e (1)-degeneration of the basic state of the relativistic bihamiltonian system, lying in the basis of the given theory

  13. Probing the selective separation of potassium ion from sodium ion with cyclopentadienyl anion as receptor: a computational study.

    Science.gov (United States)

    Desai, Mittal L; Si, Mrinal Kanti; Lo, Rabindranath; Ganguly, Bishwajit

    2015-08-01

    A systematic computational study has been carried out using post-Hartree-Fock and density functional theory methods on half sandwich (M-Cp), sandwich (Cp-M-Cp), inversed sandwich (M-Cp-M), and multi-decker chain complexes of alkali metal ions (Na(+), and K(+)). The binding affinity of cyclopentadienyl anion (Cp) with K(+) and Na(+) ions has been studied in half sandwich, sandwich, inversed sandwich, and multi-decker chain complexes. These complexes have been examined in the aqueous phase. The calculated results show that Cp anion can preferentially bind with Na(+) ion over K(+) ion in aqueous phase. The results obtained from DFT calculations have been compared with the crystal structures of Cp-Na and Cp-K complexes. The Bader's atoms in molecule (AIM) analysis were performed to characterize the non-covalent cation-π interactions in the Cp-M complexes. The calculated electron density at cage critical point indicates the strength of the Cp-M complexes. Energy decomposition analysis (EDA) has also been performed to investigate the origins of these interactions. The electrostatic interaction contributes significantly to the total interaction energy in Cp-M complexes. The relative stability difference of cyclopentadienyl anion (Cp) with K(+) and Na(+) ions in aqueous phase can be exploited for the separations from mixture such as sea bittern. The lower stability of K-Cp complex can induce to precipitate the K(+) ions more easily than the corresponding Na(+) ions. Graphical Abstract Potassium ion from sodium ion with cyclopentadienyl anion as receptor.

  14. A reversible monoamine oxidase inhibitor, toloxatone: comparison of its physicochemical properties with those of other inhibitors including brofaromine, harmine, R40519 and moclobemide

    Energy Technology Data Exchange (ETDEWEB)

    Moureau, F.; Wouters, J.; Depas, M.; Vercauteren, D.P.; Durant, F. [Facultes Universitaires Notre-Dame de la Paix, Namur (Belgium); Ducrey, F.; Koenig, J.J.; Jarreau, F.X. [Synthelabo Recherche, 92 - Rueil-Malmaison (France)

    1995-12-31

    Reversible, competitive and selective monoamine oxidase A inhibitors (MAO{sub A}Is) are an exciting new type of anti-depressants with a safe profile. The mechanism for reversible inhibition of MAO{sub A} at the molecular level is still unknown. The planar structure of most reversible MAO{sub A}Is and the well-defined acceptor power of flavin adenine dinucleotide (FAD), the cofactor of the enzyme, suggest that MAO{sub A}Is exert their inhibitory effect through charge-transfer interactions with the FAD. This hypothesis has been evaluated for Toloxatone 1, the first reversible MAO-AI marketed in France. In this work, we give evidence for the ability of other reversible MAO{sub A}Is, including Brofaromine 2, Harmine 3 and R40519 4 to interact with the flavin cofactor in comparison with Moclobemide 5, and we underline the physicochemical properties required for these interactions. First, the formation of a complex between each of the MAO{sub A}Is and riboflavin, a model of the flavin cofactor, is shown by electronic absorption spectroscopy. Essential electronic describers of MAO{sub A}Is, such as the molecular electrostatic potential and the topology of the frontier orbitals, are then calculated by the ab initio Hartree-Fock method and compared with those of previously studied Toloxatone. This confirms the electronic absorption spectroscopy results. Finally, the similarities between the different MAO{sub A}Is are underlined and an interaction model is discussed on the basis of a detailed analysis of the electronic describers of all the considered MAO{sub A}Is and the flavin nucleus. (authors). 49 refs., 14 figs., 3 tabs.

  15. Pairwise additivity of energy components in protein-ligand binding: The HIV II protease-Indinavir case

    Science.gov (United States)

    Ucisik, Melek N.; Dashti, Danial S.; Faver, John C.; Merz, Kenneth M.

    2011-08-01

    An energy expansion (binding energy decomposition into n-body interaction terms for n ≥ 2) to express the receptor-ligand binding energy for the fragmented HIV II protease-Indinavir system is described to address the role of cooperativity in ligand binding. The outcome of this energy expansion is compared to the total receptor-ligand binding energy at the Hartree-Fock, density functional theory, and semiempirical levels of theory. We find that the sum of the pairwise interaction energies approximates the total binding energy to ˜82% for HF and to >95% for both the M06-L density functional and PM6-DH2 semiempirical method. The contribution of the three-body interactions amounts to 18.7%, 3.8%, and 1.4% for HF, M06-L, and PM6-DH2, respectively. We find that the expansion can be safely truncated after n = 3. That is, the contribution of the interactions involving more than three parties to the total binding energy of Indinavir to the HIV II protease receptor is negligible. Overall, we find that the two-body terms represent a good approximation to the total binding energy of the system, which points to pairwise additivity in the present case. This basic principle of pairwise additivity is utilized in fragment-based drug design approaches and our results support its continued use. The present results can also aid in the validation of non-bonded terms contained within common force fields and in the correction of systematic errors in physics-based score functions.

  16. Comparative studies of density-functional approximations for light atoms in strong magnetic fields

    Science.gov (United States)

    Zhu, Wuming; Zhang, Liang; Trickey, S. B.

    2014-08-01

    For a wide range of magnetic fields, 0≤B≤2000 a.u., we present a systematic comparative study of the performance of different types of density-functional approximations in light atoms (2≤Z≤6). Local, generalized-gradient approximation (GGA; semilocal), and meta-GGA ground-state exchange-correlation (xc) functionals are compared on an equal footing with exact-exchange, Hartree-Fock (HF), and current-density-functional-theory (CDFT) approximations. Comparison also is made with published quantum Monte Carlo data. Though all approximations give qualitatively reasonable results, the exchange energies from local and GGA functionals are too negative for large B. Results from the Perdew-Burke-Ernzerhof ground-state GGA and Tao-Perdew-Staroverov-Scuseria (TPSS) ground-state meta-GGA functionals are very close. Because of confinement, self-interaction error in such functionals is more severe at large B than at B =0, hence self-interaction correction is crucial. Exact exchange combined with the TPSS correlation functional results in a self-interaction-free (xc) functional, from which we obtain atomic energies of comparable accuracy to those from correlated wave-function methods. Specifically for the B and C atoms, we provide beyond-HF energies in a wide range of B fields. Fully self-consistent CDFT calculations were done with the Vignale-Rasolt-Geldart (VRG) functional in conjunction with the PW92 xc functional. Current effects turn out to be small, and the vorticity variable in the VRG functional diverges in some low-density regions. This part of the study suggests that nonlocal, self-interaction-free functionals may be better than local approximations as a starting point for CDFT functional construction and that some basic variable other than the vorticity could be helpful in making CDFT calculations practical.

  17. Folding model study of the charge-exchange scattering to the isobaric analog state and implication for the nuclear symmetry energy

    Energy Technology Data Exchange (ETDEWEB)

    Khoa, Dao T.; Thang, Dang Ngoc [VINATOM, Institute for Nuclear Science and Technique, Hanoi (Viet Nam); Loc, Bui Minh [VINATOM, Institute for Nuclear Science and Technique, Hanoi (Viet Nam); University of Pedagogy, Ho Chi Minh City (Viet Nam)

    2014-02-15

    The Fermi transition (ΔL = ΔS = 0 and ΔT = 1) between the nuclear isobaric analog states (IAS), induced by the charge-exchange (p, n) or ({sup 3}He, t) reaction, can be considered as ''elastic'' scattering of proton or {sup 3}He by the isovector term of the optical potential (OP) that flips the projectile isospin. The accurately measured (p, n) or ({sup 3}He, t) scattering cross section to the IAS can be used, therefore, to probe the isospin dependence of the proton or {sup 3}He optical potential. Within the folding model, the isovector part of the OP is determined exclusively by the neutron-proton difference in the nuclear densities and the isospin dependence of the effective nucleon-nucleon (NN) interaction. Because the isovector coupling explicitly links the isovector part of the proton or {sup 3}He optical potential to the cross section of the charge-exchange (p, n) or ({sup 3}He, t) scattering to the IAS, the isospin dependence of the effective (in-medium) NN interaction can be well tested in the folding model analysis of these charge-exchange reactions. On the other hand, the same isospin- and density-dependent NN interaction can also be used in a Hartree-Fock calculation of asymmetric nuclear matter, to estimate the nuclear matter energy and its asymmetry part (the nuclear symmetry energy). As a result, the fine-tuning of the isospin dependence of the effective NN interaction against the measured (p, n) or ({sup 3}He, t) cross sections should allow us to make some realistic prediction of the nuclear symmetry energy and its density dependence. (orig.)

  18. beam-beam interaction

    CERN Multimedia

    2017-01-01

    The Beam 1 (represented in blue) and the Beam 2 (represented in red) are colliding with an angle at the Interaction Point (IP). The angle is needed to avoid unwanted multiple collisions along the interaction region. Despite of the separation introduced by the angle, the two beams interact via their electromagnetic field, the so called "beam-beam" interaction.

  19. Designing for mobile interaction

    DEFF Research Database (Denmark)

    Nazzi, Elena

    2009-01-01

    The theme of this PhD project is designing for mobile interaction with devices and services, for the accessing, making, and sharing of information, taking into account the dynamic physical and social settings that embrace this interaction. To narrow down this theme, the whole project focuses...... on the exploitation of social interaction --- in particular among senior citizens --- to enhance and support mobile interaction....

  20. Interaction for visualization

    CERN Document Server

    Tominski, Christian

    2015-01-01

    Visualization has become a valuable means for data exploration and analysis. Interactive visualization combines expressive graphical representations and effective user interaction. Although interaction is an important component of visualization approaches, much of the visualization literature tends to pay more attention to the graphical representation than to interaction.The goal of this work is to strengthen the interaction side of visualization. Based on a brief review of general aspects of interaction, we develop an interaction-oriented view on visualization. This view comprises five key as