Quantum Simulation of Chemical Dynamics in Solution

Peter Rossky得到了理论和计算化学计划的资助，继续他对溶液中化学动力学的量子模拟的研究。他将继续发展理论和计算技术来研究溶剂对非水溶剂中化学体系激发态动力学的影响。利用凝聚相动力学的瞬时简正模描述，探讨环境动力学对溶质量子态振幅相干性和退相的影响。应用包括甜菜碱-30在乙腈和甲醇溶剂中的光谱和电子转移动力学的研究，以及四氰乙烯和六甲苯的溶液相双分子络合物的研究。理论处理将被用来解释这些系统相当大的超快时间分辨和共振拉曼数据。大多数化学反应发生在溶液中，这一事实为实验和理论研究提供了强大的动力，以阐明决定化学反应进程的分子运动，以及影响溶质内部和溶质与其环境之间的能量流动的分子运动。对溶剂化作用在化学反应中所起作用的详细分子理解可能会对一些商业合成过程的优化产生重大影响。

Peter Rossky is supported by a grant from the Theoretical and Computational Chemistry Program to continue his research on quantum simulation of chemical dynamics in solution. He will the continue the development of theoretical and computational techniques to study solvent effects on excited state dynamics of chemical systems in nonaqueous solvents. The role of environmental dynamics on solute quantum state amplitude coherence and dephasing will be explored using the instantaneous normal mode description of condensed phase dynamics. Applications include the study of the spectroscopy and electron transfer dynamics of betaine-30 in acetonitrile and methanol solvents and the solution phase bimolecular complex between tetracyanoethylene and hexamethylbenzene. Theoretical treatments will be used to interpret the considerable ultrafast time resolved and resonance Raman data for these systems. The fact that most chemical reactions occur in solution provides a strong impetus for both experimental and theoretical research to elucidate the molecular motions that determine the course of a chemical reaction and that influence the energy flow within the solute and between the solute and its environment. A detailed molecular understanding of the role that solvation plays in chemical reactions could have a significant impact on the optimization of a number of commercial synthetic processes.