Ultrafast Dynamics and Reactivity in Ground and Excited States: Beyond the Pump-probe Method

基态和激发态的超快动力学和反应性：超越泵浦探针方法

• 批准号: 0135581
• 负责人: Marcos Dantus
• 金额: $ 36.79万
• 依托单位: Michigan State University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2002
• 资助国家: 美国
• 起止时间: 2002-04-01 至 2005-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0135581&HistoricalAwards=false
• 关键词: Ultrafast; Dynamics; Reactivity; Ground; Excited

In this project funded by the Experimental Physical Chemistry Program of the Chemistry Division, Dantus will use three-pulse, four-wave mixing (FWM) non-linear spectroscopy to study the dynamics of wave packet motion in the ground and excited states of NO2, CF3NO, and N2O4. The purpose of the work is to investigate intramolecular vibrational energy redistribution (IVR) and curve crossing dynamics in polyatomic systems and thereby open up the way for more general, and wider ranging investigations than done heretofore on diatomics. Specific questions to be answered in this research are about the initial steps of energy dissipation and IVR in polyatomics, what is the nature of wave packet localization in phase space for multidimensional systems, and what is the ground state dynamics in systems with chemically significant amounts of energy, up to 12,000 cm-1.This project deals with fundamental questions of how energy absorbed into specific molecular energy states redistributes itself throughout a molecule in the course of time. A good understanding of these intramolecular processes may lead to the laser control of chemical reactions. This research is undertaken with students and postdoctoral research associates. They will acquire training and knowledge in one the forefront areas of contemporary physical chemistry in preparation for advanced studies or employment in industry, government or academia.

在这个由化学部实验物理化学计划资助的项目中，Dantus将使用三脉冲，四波混频（FWM）非线性光谱学来研究NO2，CF3NO和N2O4基态和激发态的波包运动动力学。这项工作的目的是研究多原子系统中的分子内振动能再分布（IVR）和曲线交叉动力学，从而开辟了一条道路，为更一般，更广泛的调查比迄今为止所做的电子学。在这项研究中要回答的具体问题是关于多原子中能量耗散和IVR的初始步骤，多维系统相空间中波包局域化的性质是什么，以及具有化学显着能量的系统中的基态动力学是什么，高达12，该项目涉及的基本问题是，吸收到特定分子能量状态的能量如何随着时间的推移在整个分子中重新分配。对这些分子内过程的深入理解可能会导致化学反应的激光控制。这项研究是与学生和博士后研究助理进行的。他们将获得当代物理化学前沿领域的培训和知识，为工业，政府或学术界的高级研究或就业做准备。