Local response dispersion method. II. Generalized multicenter interactions

Takeshi Sato, Hiromi Nakai

    Research output: Contribution to journalArticle

    71 Citations (Scopus)

    Abstract

    Recently introduced local response dispersion method [T. Sato and H. Nakai, J. Chem. Phys. 131, 224104 (2009)], which is a first-principles alternative to empirical dispersion corrections in density functional theory, is implemented with generalized multicenter interactions involving both atomic and atomic pair polarizabilities. The generalization improves the asymptote of intermolecular interactions, reducing the mean absolute percentage error from about 30% to 6% in the molecular C6 coefficients of more than 1000 dimers, compared to experimental values. The method is also applied to calculations of potential energy curves of molecules in the S22 database [P. Jurečka, Phys. Chem. Chem. Phys. 8, 1985 (2006)]. The calculated potential energy curves are in a good agreement with reliable benchmarks recently published by Molnar [J. Chem. Phys. 131, 065102 (2009)]. These improvements are achieved at the price of increasing complexity in the implementation, but without losing the computational efficiency of the previous two-center (atom-atom) formulation. A set of different truncations of two-center and three- or four-center interactions is shown to be optimal in the cost-performance balance.

    Original languageEnglish
    Article number194101
    JournalJournal of Chemical Physics
    Volume133
    Issue number19
    DOIs
    Publication statusPublished - 2010 Nov 21

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    Potential energy
    Atoms
    Computational efficiency
    Dimers
    Density functional theory
    potential energy
    interactions
    Molecules
    asymptotes
    curves
    atoms
    Costs
    dimers
    density functional theory
    costs
    formulations
    coefficients
    approximation
    molecules

    ASJC Scopus subject areas

    • Physics and Astronomy(all)
    • Physical and Theoretical Chemistry

    Cite this

    Local response dispersion method. II. Generalized multicenter interactions. / Sato, Takeshi; Nakai, Hiromi.

    In: Journal of Chemical Physics, Vol. 133, No. 19, 194101, 21.11.2010.

    Research output: Contribution to journalArticle

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