Ultrafast Studies of Energy Redistribution in Condensed Phase Chemical Reactions

凝聚相化学反应中能量再分配的超快研究

• 批准号: 0078972
• 负责人: Roseanne Sension
• 金额: $ 32.85万
• 依托单位: Regents of the University of Michigan - Ann Arbor
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2000
• 资助国家: 美国
• 起止时间: 2000-08-01 至 2006-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0078972&HistoricalAwards=false
• 关键词: Ultrafast; Studies; Energy; Redistribution; Condensed

Professor Roseanne Sension of the University of Michigan is funded by the Experimental Physical Chemistry program to perform experiments on energy redistribution in condensed phase chemical reactions. The reason why these studies are of interest is two-fold: first, understanding the interplay between energy relaxation and chemical reactions in the liquid phase is important in biological processes. Secondly, prospects of coherent control of reactions would be another important outcome. This proposal seeks to study the rate and extent of intramolecular vibrational relaxation in polyatomic molecules such as hexatriene, cyclohexadiene and dehydrocholesterol in solution. The PI then proposes to examine the nature of the interactions between a hot molecule and the solvent. A successful outcome of this proposal would be a model used to predict, interpret and/or control the outcome of chemical reactions in solution. The proposed work is unique because of the PI's ability to produce 30 fs pulses in the deep ultraviolet. Studying the pathways that energy flows through molecules and the flow rates provides information that is directly applicable to biological processes such as photosynthesis and vision. The use of ultrashort laser pulses in the deep ultraviolet makes small molecules accessible to these studies. It is thought that the first demonstrations of coherent control of reactions in solution will be in small molecules, since there are fewer pathways available to disperse the energy and, thus, it is more likely that the energy can be driven to the reaction of interest (bond breaking, for example.) These fundamental studies take advantage of recent advances in laser pulse generation that make possible the new field of femtochemistry.

密歇根大学的Roseanne Sension教授由实验物理化学计划资助，进行凝聚相化学反应中能量再分配的实验。 这些研究引起兴趣的原因有两个方面：首先，了解能量弛豫和液相化学反应之间的相互作用在生物过程中非常重要。 第二，协调一致地控制反应的前景将是另一个重要成果。该建议旨在研究多原子分子如溶液中的己三烯、环己二烯和脱氢胆固醇的分子内振动弛豫的速率和程度。 PI然后建议检查热分子和溶剂之间相互作用的性质。 这一提议的一个成功结果将是一个用于预测、解释和/或控制溶液中化学反应结果的模型。 拟议的工作是独一无二的，因为PI的能力，以产生30 fs的脉冲在深紫外线。 研究能量通过分子流动的途径和流速提供了直接适用于光合作用和视觉等生物过程的信息。 在深紫外线中使用超短激光脉冲使得小分子可以进行这些研究。 人们认为，溶液中反应的相干控制的第一个演示将是在小分子中，因为有更少的途径可用于分散能量，因此，更有可能将能量驱动到感兴趣的反应（例如，键断裂）。 这些基础研究利用了激光脉冲产生的最新进展，使飞秒化学这一新领域成为可能。