Quantum Simulation of Chemical Dynamics in Solution

彼得·罗斯基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，研究溶剂对非水溶剂中化学体系激发态动力学的影响。 环境动力学对溶质量子态振幅相干性和退相的作用将使用凝聚相动力学的瞬时简正模描述来探索。 应用包括研究甜菜碱-30在乙腈和甲醇溶剂中的光谱和电子转移动力学，以及四氰基乙烯和六亚甲基四胺之间的溶液相双分子络合物。 理论处理将被用来解释相当多的超快时间分辨和共振拉曼这些系统的数据。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过程的分子运动，并影响溶质内以及溶质与环境之间的能量流动。 详细了解分子的作用，溶剂化在化学反应中发挥的作用可能会有显着的影响，一些商业合成工艺的优化。

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.