Adsorption and diffusion on a stepped surface: Atomic hydrogen on Pt(211)
Adsorption and diffusion on a stepped surface: Atomic hydrogen on Pt(211)
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DOI：
10.1063/1.1755664
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发表时间：
2004-06-22
影响因子：
4.4
通讯作者：
Baerends, EJ
中科院分区：
文献类型：
--
作者：
Olsen, RA;Badescu, SC;Baerends, EJ
我们提出了原子氢与阶梯表面（Pt(211) 表面）相互作用的密度泛函理论计算。使用表面的平板表示，在广义梯度近似水平上进行计算。这是计算原子或分子与金属表面相互作用的最先进方法，然而只有很少的研究使用它来研究原子或分子与阶梯表面的相互作用，并且据我们所知，没有一个研究考虑氢与阶梯铂表面的相互作用。我们的目标是启动对此主题的系统研究。我们计算了H/Pt(211)系统的完整三维势能面(PES)以及H的振动能带结构和振动本征函数。在台阶边缘上发现了桥键氢的PES的深度全局最小值，这与类似H/Pt(533)系统的实验结果一致。全局最小值处的所有局部振动激励均已确定，这将有助于解释该（或类似）系统的未来实验。此外，根据计算的 PES 和振动能带结构，我们确定了扩散实验的解释或建模的许多结果，这些实验研究了原子氢扩散在阶梯状铂表面上的覆盖范围和方向依赖性。 (C) 2004 年美国物理研究所。
We present density functional theory calculations for atomic hydrogen interacting with a stepped surface, the Pt(211) surface. The calculations have been performed at the generalized gradient approximation level, using a slab representation of the surface. This is the state-of-the-art method for calculating the interaction of atoms or molecules with metal surfaces, nevertheless only few studies have used it to study atoms or molecules interacting with stepped surfaces, and none, to the best of our knowledge, have considered hydrogen interacting with stepped platinum surfaces. Our goal has been to initiate a systematic study of this topic. We have calculated the full three-dimensional potential energy surface (PES) for the H/Pt(211) system together with the vibrational band structure and vibrational eigenfunctions of H. A deep global minimum of the PES is found for bridge-bonded hydrogen on the step edge, in agreement with experimental results for the similar H/Pt(533) system. All the local vibrational excitations at the global minimum have been identified, and this will serve as a helpful guide to the interpretation of future experiments on this (or similar) system(s). Furthermore, from the calculated PES and vibrational band structure, we identify a number of consequences for the interpretation or modelling of diffusion experiments studying the coverage and directional dependence of atomic hydrogen diffusion on stepped platinum surfaces. (C) 2004 American Institute of Physics.