Structure and Dynamics of the Instantaneous Water/Vapor Interface Revisited by Path-Integral and Ab Initio Molecular Dynamics Simulations

被引：65

作者：

Kessler, Jan ^{[1
,2
]}

Elgabarty, Hossam ^{[1
,2
]}

Spura, Thomas ^{[3
]}

Karhan, Kristof ^{[3
]}

Partovi-Azar, Pouya ^{[3
]}

Hassanali, Ali A. ^{[4
]}

Kuehne, Thomas D. ^{[3
,5
,6
]}

机构：

[1] Johannes Gutenberg Univ Mainz, Inst Phys Chem, D-55128 Mainz, Germany

[2] Johannes Gutenberg Univ Mainz, Ctr Computat Sci, D-55128 Mainz, Germany

[3] Univ Paderborn, Dept Chem, Dynam Condensed Matter, D-33098 Paderborn, Germany

[4] Abdus Salam Int Ctr Theoret Phys, I-34151 Trieste, Italy

[5] Paderborn Ctr Parallel Comp, D-33098 Paderborn, Germany

[6] Inst Lightweight Design Hybrid Syst, D-33098 Paderborn, Germany

来源：

JOURNAL OF PHYSICAL CHEMISTRY B | 2015年 / 119卷 / 31期

关键词：

LIQUID-VAPOR INTERFACE; FREQUENCY GENERATION SPECTROSCOPY; WATER-SURFACE; VIBRATIONAL SPECTROSCOPY; THEORETICAL-ANALYSIS; SPECTRUM; FRACTIONATION; ORIENTATION; DEPENDENCE; MIXTURES;

D O I：

10.1021/acs.jpcb.5b04185

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：

The structure and dynamics of the water/vapor interface is revisited by means of path-integral and secondgeneration Car Parrinello ab initio molecular dynamics simulations in conjunction with an instantaneous surface definition [Willard, A. P.; Chandler, D. J. Phys. Chem. B 2010, 114, 1954]. In agreement with previous studies, we find that one of the OH bonds of the water molecules in the topmost layer is pointing out of the water into the vapor phase, while the orientation of the underlying layer is reversed. Therebetween, an additional water layer is detected, where the molecules are aligned parallel to the instantaneous water surface.

引用

页码：10079 / 10086

页数：8

共 101 条

[11] Nuclear quantum effects and hydrogen bond fluctuations in water [J].