電極表面の第一原理計算

抄録

Since the electrode interface phenomena have multiscale nature in space and time, the multiscale model from quantum to continuum level should be considered. In this article we describe the structure of the Pt(111)/dipolar liquid interface and the adsorption of sulfur on electrified Au(111) surface. The structure of the Pt(111)/dipolar liquid interface has been investigated by fully self-consistent combination of the first-principles calculation based on quantum mechanics for the metal and the reference hypernetted-chain (RHNC) theory for the liquid. The electronic density profile for the metal, density and orientational structure of liquid molecules, and electrostatic potential across the interface are discussed in detail. A dense layer of liquid molecules, which is ordered in terms of orientation, is formed near the metal surface, but this surface-induced structure extends about only three molecular diameters from the surface. This result is in agreement with the recent experimental observations. For S adsorption on electrified Au(111) surface the screening of the electron at metal surface and the change of the adsorption energy of sulfur are discussed briefly.