Femtosecond Studies of Chemical Reaction Dynamics in Simple Liquids

简单液体中化学反应动力学的飞秒研究

• 批准号: 9529105
• 负责人: Charles Harris
• 金额: $ 67.1万
• 依托单位: University of California-Berkeley
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 1996
• 资助国家: 美国
• 起止时间: 1996-04-01 至 2000-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9529105&HistoricalAwards=false
• 关键词: Femtosecond; Studies; Chemical; Reaction; Dynamics

Charles Harris is supported by a grant from the Theoretical and Computational Chemistry Program to continue his research in femtosecond studies of chemical reaction dynamics in simple liquids. Two main lines of research will be pursued. The first line of research involves the investigation of solute/solvent interactions of polyatomic molecules in solution using femtosecond and picosecond infrared and visible laser experiments as well as molecular dynamics simulations. This work will extend the work already completed on iodine in liquid krypton and xenon to diatomic molecules such as diatomic iodine anion, iodine chloride and iodine bromide in liquid krypton and xenon. Infrared pump and probe techniques will also be used to examine carbon-hydrogen stretching mode relaxation times of simple polyatomic as a function of pressure in krypton and xenon solvents. The second area of study involves the use of femtosecond and picosecond infrared and visible spectroscopic techniques to study reaction mechanisms of several organometallic compounds whose branching ratios and quantum yields are controlled by the ultrafast energy transfer between solute and solvent. These studies will encompass a broad range of mechanistic studies, including carbon-hydrogen and silicon-hydrogen bond activation in transition metal compounds and photochemical ring slippage of an aromatic ligand. Since many commercially important chemical reactions take place in solvents, it is important to understand the influence that such solvents have on the reaction dynamics. A number of effects, such as solvent cage effects, vibrational relaxation and quantum mechanical tunneling, that are not present in the gas phase, completely dominate condensed phase chemical reactions. It is important to develop reliable theories for model chemical systems that can then be applied to improving the efficiency of commercially important chemical reactions. The work that is being performed by Harris provides an important experimental basis for the development of such theories.

查尔斯·哈里斯得到了理论和 计算化学计划继续他的研究在飞秒 研究简单液体中的化学反应动力学。 两条主线 研究将继续进行。第一条研究路线涉及 多原子分子溶质/溶剂相互作用的研究 使用飞秒和皮秒红外和可见激光的解决方案 实验以及分子动力学模拟。 这项工作将 扩展已完成的关于液态氪和氙中碘的工作 双原子分子如双原子碘阴离子、氯化碘和 溴化碘在液态氪和氙中。 红外泵和探头 技术也将被用来检查碳氢伸缩模式 简单多原子的弛豫时间作为压力的函数， 氪和氙溶剂。 第二个研究领域涉及使用 飞秒和皮秒的红外和可见光谱 技术来研究几种有机金属的反应机理 这些化合物的支化比和量子产率由 溶质和溶剂之间的超快能量传递。 这些研究将 涵盖广泛的机械研究，包括 过渡金属中碳氢键和硅氢键的活化 化合物和芳香配体的光化学环滑移。 由于许多商业上重要的化学反应发生在 溶剂，重要的是要了解这种溶剂的影响， 对反应动力学的影响。 一些影响，如溶剂 笼效应、振动弛豫和量子力学隧穿， 不存在于气相中，完全支配冷凝 阶段化学反应。 发展可靠的理论很重要 用于模型化学系统，然后可以应用于改善 商业上重要的化学反应的效率。 的工作 哈里斯正在进行的一项研究为以下方面提供了重要的实验依据： 这些理论的发展。