Nuclear Quantum Effects in Water Reorientation and Hydrogen-Bond Dynamics

被引:49
|
作者
Wilkins, David M. [1 ]
Manolopoulos, David E. [2 ]
Pipolo, Silvio [3 ,4 ,6 ]
Laage, Damien [3 ,4 ]
Hynes, James T. [3 ,5 ]
机构
[1] Ecole Polytech Fed Lausanne, IMX, Lab Computat Sci & Modeling, CH-1015 Lausanne, Switzerland
[2] Univ Oxford, Phys & Theoret Chem Lab, South Parks Rd, Oxford OX1 3QZ, England
[3] UPMC Univ Paris 06, PSL Res Univ, PASTEUR, Ecole Normale Super,CNRS,Dept Chim, F-75005 Paris, France
[4] UPMC Univ Paris 06, Sorbonne Univ, CNRS, PASTEUR,ENS, F-75005 Paris, France
[5] Univ Colorado, Dept Chem & Biochem, Campus Box 215, Boulder, CO 80309 USA
[6] Univ Lille 1, Unite Catalyze & Chim Solide, F-59655 Villeneuve Dascq, France
来源
基金
美国国家科学基金会;
关键词
PROTON-TRANSFER REACTIONS; FREE-ENERGY RELATIONS; MOLECULAR-REORIENTATION; POLAR ENVIRONMENT; MECHANISM;
D O I
10.1021/acs.jpclett.7b00979
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We combine classical and ring polymer molecular dynamics simulations with the molecular jump model to provide a molecular description of the nuclear quantum effects (NQEs) on water reorientation and hydrogen-bond dynamics in liquid H2O and D2O. We show that while the net NQE is negligible in D2O, it leads to a similar to 13% acceleration in H2O dynamics compared to a classical description. Large angular jumps exchanging hydrogen-bond partners are the dominant reorientation pathway (just as in a classical description); the faster reorientation dynamics arise from the increased jump rate constant. NQEs do not change the jump amplitude distribution, and no significant tunneling is found. The faster jump dynamics are quantitatively related to decreased structuring of the 00 radial distribution function when NQEs are included. This is explained, via a jump model analysis, by competition between the effects of water's librational and OH stretch mode zero-point energies on the hydrogen-bond strength.
引用
收藏
页码:2602 / 2607
页数:6
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