Surface-Charge Dependent Orientation of Water at the Interface of a Gold Electrode: A Cluster Study

被引:4
作者
Fazio, Gianluca [1 ,2 ]
Seifert, Gotthard [1 ,3 ]
Rapacioli, Mathias [4 ,5 ]
Tarrat, Nathalie [6 ,7 ]
Joswig, Jan-Ole [1 ]
机构
[1] Tech Univ Dresden, Theoret Chem, D-01062 Dresden, Germany
[2] Univ Milano Bicocca, Dipartimento Sci Mat, Milan, Italy
[3] Univ Witwatersrand, Mat Energy Res Grp, Johannesburg, South Africa
[4] Univ Toulouse, Lab Chim & Phys Quant LCPQ IRSAMC, 118 Route Narbonne, F-31062 Toulouse, France
[5] CNRS, 118 Route Narbonne, F-31062 Toulouse, France
[6] Univ Toulouse, CEMES, 29 Rue Jeanne Marvig, F-31055 Toulouse, France
[7] CNRS, 29 Rue Jeanne Marvig, F-31055 Toulouse, France
来源
ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS | 2018年 / 232卷 / 9-11期
关键词
DFTB; electrochemistry; gold electrode; metal/water interface; molecular dynamics; ELECTROCHEMICAL INTERFACE; ABSORPTION SPECTROSCOPY; SIMULATIONS; MOLECULES; SCHEME;
D O I
10.1515/zpch-2018-1136
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
A gold/water interface has been investigated with the DFT-based self-consistent-charge density-functional tight-binding (SCC-DFTB) method using a cluster model. Born-Oppenheimer molecular-dynamics simulations for mono-, bi-, and trilayers of water on the surface of a Au-55 cluster have been computed. We have demonstrated the applicability of this method to the study of the structural and dynamical properties of the gold/water-multilayer interface. The results of the simulations clearly show the charge-dependent orientation and the corresponding polarization of the water sphere around the gold cluster. However, it was also shown that this polarization is restricted almost only to the first solvation shell. This illustrates the rather short-range screening behavior of water. The present study builds the basis for further investigations of metal/electrolyte interfaces on a reliable atomistic level, avoiding the problems of spurious artifacts in models using periodic boundary conditions.
引用
收藏
页码:1583 / 1592
页数:10
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