Photoinduced Reaction Dynamics in Weakly Bound Complexes

俄亥俄州立大学的Anne McCoy得到了理论与计算化学计划的支持，从理论上研究弱束缚团簇中的光引发过程。以下三类过程将被研究：(1)二元配合物的紫外光解离解引起双分子反应，(2)通过振动激发一个簇分子在配合物中引起的反应动力学，以及(3)簇大小对IHI与氩原子簇的过渡态动力学和水簇与氩原子的光解离的影响。团簇中光引发过程的研究在理论上和计算上都提出了严峻的挑战。本研究的一个重要组成部分将涉及开发近似方法，使动力学研究中至少一些经典自由度的处理成为可能，以及研究用于传播动力学的混合量子/经典方法。分子簇提供了一个实验室，通过它，分子之间的相互作用可以在实验和理论上进行检查。团簇不能简单地认为是其组成分子的总和，因为团簇环境通常会改变络合分子的化学反应。本研究将从理论上探索聚类化学反应，其中许多可以与当前感兴趣的相关实验结果进行比较。

Anne McCoy of the Ohio State University is supported by the Theoretical and Computational Chemistry Program to investigate photoinitiated processes in weakly bound clusters theoretically. The following three categories of processes will be examined: (1) ultraviolet photodissociation of binary complexes in which the dissociation induces a bimolecular reaction, (2) reaction dynamics photoinduced in complexes by vibrationally exciting one of the cluster molecules, and (3) cluster size effects on transition state dynamics of IHI clustered with argon atoms and the photodissociation of water clusters with argon atoms. Studies of photoinitiated processes in clusters pose serious challenges theoretically and computationally. A significant component of this research will involve developing approximate approaches that will enable treatments of at least some of the degrees of freedom classically in the dynamics studies, as well as investigating hybrid quantum/classical methods for propagating the dynamics. Clusters of molecules provide a laboratory through which interactions between molecules can be examined both experimentally and theoretically. Clusters cannot be considered simply as the sum of their constituent molecules, as the cluster environment generally changes chemical reactions of the complexed molecules. This research will explore theoretically cluster chemical reactions, many of which can be compared to related experimental results of current interest.