Molecular Relaxation and Radiative Processes

Shaul Mukamel得到了理论和计算化学计划的资助，继续他在分子弛豫和辐射过程方面的研究。他将继续发展他的理论方法，在耦合的局域振动或电子发色团系统中设计和系统解释多维飞秒相关光谱。多脉冲核磁共振技术的可见光和红外类似物为复杂分子组装的结构和动力学、相互作用和松弛过程提供了新的快照探针。涉及分子对整形和定时辐射脉冲序列的响应的技术的基本理论概念将被开发。将测试用于模拟非线性响应函数的半经典方法。光谱学的经典振子描述将被开发出来，为设计实现与它们的核磁共振类似物相同目标的新的脉冲序列奠定基础，并提供一个计算和解释多维信号的框架。脉冲激光技术的出现与非线性光学技术的使用相结合，导致了大量探测气相和凝聚相分子体系的新方法。穆卡迈尔正在开发理论技术，这些技术是解释从这些实验获得的数据的核心。这些解释导致了许多关于凝聚相系统中的化学反应和溶剂化效应的重要见解，这些见解可以应用于理解生物系统。

Shaul Mukamel is supported by a grant from the Theoretical and Computational Chemistry Program to continue his research in molecular relaxation and radiative processes. He will continue his development of theoretical methods for the design and systematic interpretation of multidimensional femtosecond correlation spectroscopies in systems of coupled localized vibrational or electronic chromophores. Visible and infrared analogues of multiple-pulse NMR techniques provide novel snapshot probes into the structure as well as dynamics, interactions and relaxation processes of complex molecular assemblies. The fundamental theoretical concepts underlying techniques involving molecular responses to sequences of shaped and timed radiation pulses will be developed. Semiclassical methods for simulating nonlinear response functions will be tested. A classical-oscillator description of the spectroscopies will be developed, setting the stage for designing new pulse sequences that accomplish the same goals as their NMR analogues and providing a framework for computing and interpreting multidimensional signals.The advent of pulsed laser technology combined with the use of non-linear optical techniques has led to a large number of new methods to probe gas-phase and condensed-phase molecular systems. Mukamel is developing theoretical techniques that are central to the interpretation of the data obtained from these experiments. These interpretations lead to many important insights regarding chemical reactions and the effects of solvation in condensed phase systems that can have application to understanding biological systems.