The Influence of Adsorbate-Adsorbate Interactions on the Dynamics of Interfacial Hydrogen

布朗大学的吉米·多尔和罗德岛大学的大卫·弗里曼得到了理论和计算化学项目的资助，他们将继续研究吸附-吸附相互作用对界面氢动力学的影响。Doll和Freeman发展了吸附振动线型的动态路径积分理论，并将其应用于氢在不同金属表面上的吸附研究，如Ni(111)。用嵌入原子模型的结果解释了振动光谱的实验结果。目前的研究计划建立在这些结果的基础上，通过使用从头算电子结构计算来改进相互作用势。北卡罗来纳州立大学的Whitten和他的同事开发的嵌入的团簇方法将被用来开发更现实的从头算相互作用势，用于动力学路径积分计算。应用将包括氢在Ni(111)、Ni(110)、Cu(110)和W(110)上的研究以及氢在Ni、Cu和W团簇上的离域吸附的研究。这些计算将被用来解释布朗大学的彼得·韦伯获得的实验数据。金属中的储氢和氢脆是重要的技术问题。多尔和弗里曼的基础工作很有可能为基于分子的理解这些现象提供重要的理论见解。

Jimmie Doll from Brown University and David Freeman from University of Rhode Island are supported by a grant from the Theoretical and Computational Chemistry Program to continue their research on the influence of adsorbate-adsorbate interactions on the dynamics of interfacial hydrogen. Doll and Freeman have developed a dynamical path integral theory for adsorbate vibrational lineshapes and applied it to studies of Hydrogen adsorbed on various metal surfaces such as Ni(111). Results using the embedded atom model have been used to elucidate experimental results obtained from vibrational spectroscopy. The current research program builds upon these results by improving upon the interaction potentials through the use of ab initio electronic structure calculations. The embedded cluster methods developed by Whitten and coworkers at North Carolina State University will be employed to develop more realistic ab initio interaction potentials for use in the dynamical path integral calculations. Applications will include studies of Hydrogen on Ni(111), Ni(110), Cu(110) and W(110) as well as delocalization of hydrogen adsorption on Ni, Cu and W clusters. The calculations will be used to interpret experimental data obtained by Peter Weber of Brown University. Hydrogen storage in metals and hydrogen embrittlement are important technological problems. The fundamental work of Doll and Freeman has a very good probability of providing significant theoretical insights into a molecular based understanding of these phenomena.