Ultrafast Studies of Chemical Reactions in Simple Liquids

查尔斯·哈里斯教授得到了理论和计算化学项目的资助，研究溶剂对多原子单分子分解反应动力学的影响。他计划系统地研究各种多原子分子的皮秒和飞秒单分子解离反应，包括过渡金属羰基在液态氙气、氪和其他简单的超临界溶剂中的解离反应，如一氧化碳和二氧化碳。这项研究的实验部分的主要重点将是确定溶剂密度和温度对与液态反应相关的各个步骤的定量影响。此外，还将继续进行理论研究，包括使用分子动力学和广义朗之万动力学模拟反应。大多数实际重要的化学反应都发生在溶液中。众所周知，在溶液中发生的反应受到反应物种与溶剂分子相互作用的影响，溶剂分子往往将反应物分子封闭在溶剂笼中。然而，对溶剂对化学反应影响的理论理解还不是很清楚。Harris教授的研究将有助于阐明溶剂分子影响溶液中化学反应的机理，并将有助于改进理论以提高我们对这一重要现象的理解。

Professor Charles Harris is supported by a grant from the Theoretical and Computational Chemistry Program to study solvent effects on reaction dynamics of polyatomic unimolecular decomposition reactions. He plans to systematically investigate the picosecond and femtosecond unimolecular dissociation reactions of a variety of polyatomic molecules including transition metal carbonyls in liquid xenon, krypton and other simple supercritical solvents such as carbon monoxide and carbon dioxide. The primary focus of the experimental part of the research will be to determine the quantitative effect of the solvent density and temperature on the individual steps associated with the liquid state reactions. In addition, theoretical studies will be pursued which will include simulating the reactions using molecular dynamics and generalized Langevin dynamics. %%% Most chemical reactions of practical importance take place in solution. It is known that the reactions which occur in solution are influenced by the interaction of the reacting species with the solvent molecules which tend to enclose the reactant molecules in solvent cages. Nevertheless, the theoretical understanding of the effects of solvent on a chemical reaction are not well understood. The research being performed by Professor Harris will help to elucidate the mechanism by which solvent molecules influence chemical reactions in solution, and will lead to improved theories for improving our understanding of this important phenomenon.