Molecular Relaxation and Radiative Processes

Shaul Mukamel教授得到了理论和计算化学项目的资助，以开发帮助我们了解气相团簇、溶液和分子晶体的非线性光学性质的理论。对非线性光学性质的进一步了解对于发展新的激光光学光谱材料和技术是非常重要的。本文主要研究了在Liouville空间中利用密度矩阵技术对分子辐射过程进行动力学描述的发展和应用。这项技术允许直接计算热平均可观量。三阶非线性响应函数的理论模型正在建立中，该函数描述了广泛的四波混频和相关光谱。在超音速束流和凝聚相中的飞秒泵浦探测光谱、极性溶剂中的介电涨落、电子转移过程中的超交换、分子团簇中的辐射衰变过程以及分子晶体中的激子输运和延迟效应等方面都有应用。

Professor Shaul Mukamel is supported by a grant from The Theoretical and Computational Chemistry Program to develop theories which help us to understand nonlinear optical properties of gas phase clusters, solutions, and molecular crystals. A further understanding of nonlinear optical properties is very important in the development of new laser optical spectroscopic materials and techniques. The research is focused on the development and application of a dynamical description of molecular radiative processes using density matrix techniques in Liouville space. This technique permits the direct calculation of thermally averaged observables. Theoretical models are being constructed for the third order nonlinear response function which describes a broad range of four wave mixing and related spectroscopies. Applications are being made to femtosecond pump-probe spectroscopy in supersonic beams and in condensed phases, dielectric fluctuations in polar solvents, superexchange in electron transfer processes, radiative decay processes in molecular clusters, and exciton transport and retardation effects in molecular crystals.