Acceleration of self-consistent field convergence in ab initio molecular dynamics simulation with multiconfigurational wave function

Masaki Okoshi, Hiromi Nakai

    Research output: Contribution to journalArticle

    2 Citations (Scopus)

    Abstract

    The Lagrange interpolation of molecular orbital (LIMO) method, which reduces the number of self-consistent field iterations in ab initio molecular dynamics simulations with the Hartree-Fock method and the Kohn-Sham density functional theories, is extended to the theory of multiconfigurational wave functions. We examine two types of treatments for the active orbitals that are partially occupied. The first treatment, as denoted by LIMO(C), is a simple application of the conventional LIMO method to the union of the inactive core and the active orbitals. The second, as denoted by LIMO(S), separately treats the inactive core and the active orbitals. Numerical tests to compare the two treatments clarify that LIMO(S) is superior to LIMO(C). Further applications of LIMO(S) to various systems demonstrate its effectiveness and robustness. © 2014 Wiley Periodicals, Inc. The Lagrange interpolation of molecular orbital (LIMO) method, which accelerates the self-consistent field (SCF) convergence in ab initio molecular dynamics simulations, is extended to the multiconfigurational (MC) wave function theories, including the complete active space SCF and restricted active space SCF methods. The reduction in the number of SCF iterations of 20-70% is achieved by the MC-type LIMO method.

    Original languageEnglish
    Pages (from-to)1473-1480
    Number of pages8
    JournalJournal of Computational Chemistry
    Volume35
    Issue number20
    DOIs
    Publication statusPublished - 2014 Jul 30

    Fingerprint

    Lagrange Interpolation
    Molecular orbitals
    Wave functions
    Wave Function
    Molecular Dynamics Simulation
    Molecular dynamics
    Interpolation
    Computer simulation
    Iteration
    Density Functional
    Accelerate
    Density functional theory
    Union
    Robustness

    Keywords

    • ab initio molecular dynamics simulation
    • acceleration technique
    • Lagrange interpolation technique
    • multiconfigurational wave function theory
    • self-consistent field convergence

    ASJC Scopus subject areas

    • Chemistry(all)
    • Computational Mathematics

    Cite this

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    title = "Acceleration of self-consistent field convergence in ab initio molecular dynamics simulation with multiconfigurational wave function",
    abstract = "The Lagrange interpolation of molecular orbital (LIMO) method, which reduces the number of self-consistent field iterations in ab initio molecular dynamics simulations with the Hartree-Fock method and the Kohn-Sham density functional theories, is extended to the theory of multiconfigurational wave functions. We examine two types of treatments for the active orbitals that are partially occupied. The first treatment, as denoted by LIMO(C), is a simple application of the conventional LIMO method to the union of the inactive core and the active orbitals. The second, as denoted by LIMO(S), separately treats the inactive core and the active orbitals. Numerical tests to compare the two treatments clarify that LIMO(S) is superior to LIMO(C). Further applications of LIMO(S) to various systems demonstrate its effectiveness and robustness. {\circledC} 2014 Wiley Periodicals, Inc. The Lagrange interpolation of molecular orbital (LIMO) method, which accelerates the self-consistent field (SCF) convergence in ab initio molecular dynamics simulations, is extended to the multiconfigurational (MC) wave function theories, including the complete active space SCF and restricted active space SCF methods. The reduction in the number of SCF iterations of 20-70{\%} is achieved by the MC-type LIMO method.",
    keywords = "ab initio molecular dynamics simulation, acceleration technique, Lagrange interpolation technique, multiconfigurational wave function theory, self-consistent field convergence",
    author = "Masaki Okoshi and Hiromi Nakai",
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    language = "English",
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    T1 - Acceleration of self-consistent field convergence in ab initio molecular dynamics simulation with multiconfigurational wave function

    AU - Okoshi, Masaki

    AU - Nakai, Hiromi

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    Y1 - 2014/7/30

    N2 - The Lagrange interpolation of molecular orbital (LIMO) method, which reduces the number of self-consistent field iterations in ab initio molecular dynamics simulations with the Hartree-Fock method and the Kohn-Sham density functional theories, is extended to the theory of multiconfigurational wave functions. We examine two types of treatments for the active orbitals that are partially occupied. The first treatment, as denoted by LIMO(C), is a simple application of the conventional LIMO method to the union of the inactive core and the active orbitals. The second, as denoted by LIMO(S), separately treats the inactive core and the active orbitals. Numerical tests to compare the two treatments clarify that LIMO(S) is superior to LIMO(C). Further applications of LIMO(S) to various systems demonstrate its effectiveness and robustness. © 2014 Wiley Periodicals, Inc. The Lagrange interpolation of molecular orbital (LIMO) method, which accelerates the self-consistent field (SCF) convergence in ab initio molecular dynamics simulations, is extended to the multiconfigurational (MC) wave function theories, including the complete active space SCF and restricted active space SCF methods. The reduction in the number of SCF iterations of 20-70% is achieved by the MC-type LIMO method.

    AB - The Lagrange interpolation of molecular orbital (LIMO) method, which reduces the number of self-consistent field iterations in ab initio molecular dynamics simulations with the Hartree-Fock method and the Kohn-Sham density functional theories, is extended to the theory of multiconfigurational wave functions. We examine two types of treatments for the active orbitals that are partially occupied. The first treatment, as denoted by LIMO(C), is a simple application of the conventional LIMO method to the union of the inactive core and the active orbitals. The second, as denoted by LIMO(S), separately treats the inactive core and the active orbitals. Numerical tests to compare the two treatments clarify that LIMO(S) is superior to LIMO(C). Further applications of LIMO(S) to various systems demonstrate its effectiveness and robustness. © 2014 Wiley Periodicals, Inc. The Lagrange interpolation of molecular orbital (LIMO) method, which accelerates the self-consistent field (SCF) convergence in ab initio molecular dynamics simulations, is extended to the multiconfigurational (MC) wave function theories, including the complete active space SCF and restricted active space SCF methods. The reduction in the number of SCF iterations of 20-70% is achieved by the MC-type LIMO method.

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