Ultrafast Studies of Chemical Reactions in Polyatomic Molecules in Simple Liquids

Charles Harris教授获得理论与计算化学计划的资助，对溶剂化对溶液中化学反应速率的影响进行实验和理论研究。他将使用各种实验方法，如瞬态泵-探针电子吸收光谱、瞬态拉曼散射和瞬态红外光谱，在皮秒和飞秒时间尺度上测量单分子解离和双分子重组率。他将研究的体系包括三原子、假三原子、单金属和双金属羰基以及取代多烯。在这些研究中使用的溶剂主要是单原子稀有气体液体。他还将使用广义朗格万和广义布朗动力学对正在研究的系统进行分子模拟。研究气相化学反应的理论已经相当发达了。我们对影响溶液中发生的化学反应的因素所知甚少，而大多数重要的化学反应都是在溶液中发生的。在这些非常基础的研究中，哈里斯将探索溶剂分子对溶液中由光的光子吸收引发的反应的影响。实验和理论的结合将使我们更好地了解影响溶液中化学反应的因素。

Professor Charles Harris is supported by a grant from the Theoretical and Computational Chemistry Program to conduct experimental and theoretical studies of the effects of solvation on the rates of chemical reactions in solution. He will measure unimolecular dissociation and bimolecular recombination rates on picosecond and femtosecond timescales using a variety of experimental methods such as transient pump-probe electronic absorption spectroscopy, transient Raman scattering, and transient IR spectroscopy. The systems he will study include triatomics, pseudotriatomics, mono- and di- metal carbonyls, and substituted polyenes. The solvents used in these studies are primarily monatomic rare gas liquids. He will also perform molecular simulations of the systems being studied using Generalized Langevin and Generalized Brownian dynamics. %%% Theories dealing with chemical reactions in the gas phase are quite well developed. Much less is known about the factors which influence chemical reactions occurring in solution, and this is where most important chemical reactions occur. In these very fundamental studies, Harris will explore the effects which solvent molecules have on reactions in solution which are initiated by absorption of a photon of light. The combination of experiment and theory will lead to a better understanding of the factors affecting chemical reactions in solution.