Fully Quantum Studies of Molecule-Surface Interactions at Finite Temperature

这项对吸附在固体表面上的分子的研究得到了 NSF理论和计算化学计划。 分子声子 用哈密顿算符对相互作用进行量子力学处理 它可以包括多个声子，以及受阻碍的平移， 分子的旋转和振动模式，以及所有可能的 这些自由度的相互作用。 弱（一个声子）和 可以描述强（多声子）相互作用。 的性质 关于脱附、弛豫和热原子的俘获态 化学治疗。 改变束流能量分量的影响 平行于表面也进行了研究。 在这项研究中使用计算机模型来研究 吸附在固体表面上的分子。 我们的目标是从根本上 表面化学原理的知识，这反过来又关系到 对于具有重要实际意义的化学过程，例如非均相 催化作用 计算机建模是一种广泛使用的理论工具， 研究这些过程。 这个研究项目的特殊作用是， 测试各种数学和物理近似的有效性 通常用于这些计算。 特别是， 量子力学，而不是经典力学，被应用， 分子与一个或多个声子（量子化晶格）的相互作用 振动）进行处理。

This study of molecules adsorbed on a solid surface is supported by the NSF Theoretical and Computational Chemistry program. The molecule-phonon interaction is treated quantum mechanically using a Hamiltonian operator that can include multiple phonons, as well as the hindered translational, rotational, and vibrational modes of the molecule, and all possible interactions of these degrees of freedom. Both weak (one phonon) and strong (multi-phonon) interactions can be described. The nature of the trapped state with regard to desorption, relaxation, and hot atom chemistry is treated. The effect of varying the component of beam energy parallel to the surface is also studied. Computer models are used in this research to study the motion of molecules adsorbed on solid surfaces. The goal is to gain fundamental knowledge of the principles of surface chemistry, which in turn relates to chemical processes of great practical importance such as heterogeneous catalysis. Computer modeling is a widely used theoretical tool for the study of such processes. The special role of this research project is to test the validity of various mathematical and physical approximations commonly employed in these computations. In particular, the laws of quantum mechanics, rather than classical mechanics, are applied, and the interaction of the molecule with one or more phonons (quantized lattice vibrations) are treated.