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 教授受到实验物理化学项目的资助，进行凝聚相化学反应中能量重新分配的实验。 这些研究令人感兴趣的原因有两个：首先，了解液相中能量弛豫和化学反应之间的相互作用对于生物过程非常重要。 其次，一致控制反应的前景将是另一个重要成果。该提案旨在研究溶液中己三烯、环己二烯和脱氢胆固醇等多原子分子的分子内振动弛豫的速率和程度。 然后，首席研究员建议检查热分子和溶剂之间相互作用的性质。 该提案的成功成果将是用于预测、解释和/或控制溶液中化学反应结果的模型。 这项工作是独一无二的，因为 PI 能够在深紫外产生 30 fs 脉冲。 研究能量流过分子的路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。 在深紫外中使用超短激光脉冲使得小分子可以用于这些研究。 人们认为，溶液中反应相干控制的首次演示将在小分子中进行，因为可用于分散能量的途径较少，因此，能量更有可能被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生成的最新进展，使飞化学的新领域成为可能。