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

Junichi Ono, Kim Hyeon-Deuk, Koji Ando

研究成果: Article

7 引用 (Scopus)

抄録

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.

元の言語English
ページ(範囲)356-365
ページ数10
ジャーナルInternational Journal of Quantum Chemistry
113
発行部数3
DOI
出版物ステータスPublished - 2013 2 5
外部発表Yes

Fingerprint

Wave packets
wave packets
Molecular dynamics
Hydrogen bonds
hydrogen bonds
molecular dynamics
Water
Computer simulation
Liquids
Bond number
liquids
water
simulation
Trajectories
trajectories
Potential energy
Power spectrum
retraining
power spectra
Hydrogen

ASJC Scopus subject areas

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

これを引用

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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.",
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