Influence of Solvent-Solute Interact#ins on Molecular Dynamics

本研究是物理化学实验的一部分， 程序，应用皮秒和飞秒时间分辨 光谱技术用于溶剂化动力学的研究， 电子转移反应，振动和定向 弛豫和扩散控制反应。这些研究 将阐明溶解的分子之间的相互作用 和它们的周围环境影响分子弛豫， 反应性 中等尺寸的晶体的振动弛豫途径 分子在各种溶剂中的研究将通过 利用可调谐性、灵敏度和 激光系统的时间分辨率。不均匀程度 振动线形的加宽将通过使用 一种拉曼回波技术，其中一对脉冲激发 振动态的相干叠加。这种系统 直到第二脉冲对使振动重新定相。 在第二延迟之后，斯托克斯探测相位相干性。 由第三激光脉冲引起的散射。的起源 电荷转移反应中的非指数衰减将是 研究了特别是，非平衡初始 在强绝热电子转移反应中， 探讨了

This research, part of the experimental Physical Chemistry Program, applies picosecond and femtosecond time resolved spectroscopic techniques to the study of solvation dynamics, electron transfer reactions, vibrational and orientational relaxation, and diffusion controlled reactions. These studies will elucidate how the interactions between dissolved molecules and their surroundings influence molecular relaxation and reactivity. The pathways of vibrational relaxation of medium-sized molecules in a variety of solvents will be investigated by taking advantage of improvements in tunability, sensitivity and time resolution of laser systems. The extent of inhomogeneous broadening in vibrational lineshapes will be examined by using a Raman echo technique in which a pair of pulses excite a coherent superposition of vibrational states. Such a system evolves until a second pulse pair rephases the vibrations. After a second delay the phase coherence is probed by Stokes scattering induced by a third laser pulse. The origin of nonexponential decays in charge transfer reactions will be studied. In particular, the role of a non-equilibrium initial state in strongly adiabatic electron transfer reactions will be explored.