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 |
| 巻 | 113 |
| 発行部数 | 3 |
| DOI | |
| 出版物ステータス | Published - 2013 2 5 |
| 外部発表 | Yes |
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ASJC Scopus subject areas
- Condensed Matter Physics
- Atomic and Molecular Physics, and Optics
- Physical and Theoretical Chemistry
これを引用
Semiquantal molecular dynamics simulations of hydrogen-bond dynamics in liquid water using spherical Gaussian wave packets. / Ono, Junichi; Hyeon-Deuk, Kim; Ando, Koji.
：: International Journal of Quantum Chemistry, 巻 113, 番号 3, 05.02.2013, p. 356-365.研究成果: Article
}
TY - JOUR
T1 - Semiquantal molecular dynamics simulations of hydrogen-bond dynamics in liquid water using spherical Gaussian wave packets
AU - Ono, Junichi
AU - Hyeon-Deuk, Kim
AU - Ando, Koji
PY - 2013/2/5
Y1 - 2013/2/5
N2 - 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.
AB - 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.
KW - hydrogen bond dynamics
KW - molecular dynamics simulation
KW - quantum effects
UR - http://www.scopus.com/inward/record.url?scp=84872913741&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84872913741&partnerID=8YFLogxK
U2 - 10.1002/qua.24146
DO - 10.1002/qua.24146
M3 - Article
AN - SCOPUS:84872913741
VL - 113
SP - 356
EP - 365
JO - International Journal of Quantum Chemistry
JF - International Journal of Quantum Chemistry
SN - 0020-7608
IS - 3
ER -