Semiquantal molecular dynamics simulations of hydrogen-bond dynamics in liquid water using spherical Gaussian wave packets

Junichi Ono, Kim Hyeon-Deuk, Koji Ando

Research output: Contribution to journalArticle

7 Citations (Scopus)

Abstract

A semiquantal (SQ) molecular dynamics (MD) simulation method using spherical Gaussian wave packets (WPs) is applied to a microscopic analysis of hydrogen-bond (H-bond) exchange dynamics in liquid water. We focus on the molecular jump mechanism of H-bond reorientation dynamics proposed from a classical MD simulation by Laage and Hynes (Science 2006, 311, 832). As a notable quantum effect, broadenings of both the oxygen and hydrogen WPs of jumping water are observed associated with the H-bond switching events. Nonetheless, quantum effects on averaged trajectories of structural parameters measured with respect to the WP centers are rather minor. A 1/f fluctuation of local H-bond number is observed in both SQ and classical simulations. This is obtained straightforwardly from the real-time trajectories, in contrast with the originally found 1/f fluctuation (Sasai et al., J. Chem. Phys. 1992, 96, 3045) of the total potential energies collected at quenched inherent structures. The quantum effects are found to accelerate the relaxation of H-bond number fluctuation, which is reflected in the region near the lower bound of the 1/f behavior in the power spectra. New developments in the implementation of SQMD simulations including all atoms are also described.

Original languageEnglish
Pages (from-to)356-365
Number of pages10
JournalInternational Journal of Quantum Chemistry
Volume113
Issue number3
DOIs
Publication statusPublished - 2013 Feb 5
Externally publishedYes

Keywords

  • hydrogen bond dynamics
  • molecular dynamics simulation
  • quantum effects

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Atomic and Molecular Physics, and Optics
  • Physical and Theoretical Chemistry

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