Molecular orbital propagation to accelerate self-consistent-field convergence in an ab initio molecular dynamics simulation

Teruo Atsumi, Hiromi Nakai

Research output: Contribution to journalArticle

13 Citations (Scopus)


Based on the idea of molecular orbital (MO) propagation, we propose a novel effective method for predicting initial guesses for the self-consistent-field calculations in direct ab initio molecular dynamics (AIMD) simulations. This method, called LIMO, adopts the Lagrange interpolation (LI) polynomial technique and predicts initial MO coefficients at the next AIMD step by using several previous results. Taking into account the crossing and/or mixing of MOs leads to orbital invariant formulas for the LIMO method. We also propose a simple method for determining the optimal degree of the LI polynomial, which corresponds to the number of previous steps. Numerical tests confirm that this proposed method is both effective and feasible.

Original languageEnglish
Article number094101
JournalJournal of Chemical Physics
Issue number9
Publication statusPublished - 2008 Mar 14


ASJC Scopus subject areas

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

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