Unimolecular Reaction Dynamics

单分子反应动力学

• 批准号: 9316640
• 负责人: C. Bradley Moore
• 金额: $ 104.22万
• 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: 1993
• 资助国家: 美国
• 起止时间: 1993-12-15 至 1997-11-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9316640&HistoricalAwards=false
• 关键词: Unimolecular; Reaction; Dynamics

The goal of this work is to understand the unimolecular reaction dynamics of the ground electronic states of small molecules and hence of their thermal unimolecular reactions. Three kinds of experiments will be conducted: 1) infrared spectroscopy of molecules activated with sufficient vibrational energy to dissociate, 2) direct measurement of dissociation rates in the range from 1 million to 100 billion per second, and 3) measurement of product energy state and angular momentum distributions and their scalar and vector correlations as a function of the initial quantum state of the activated molecule. Special emphasis will be given to two qualitatively different, prototype molecules- formyl fluoride and ketene. The dynamics of chemical reactions stands at the forefront of investigations in contemporary physical chemistry. The primary purpose of these investigations is to obtain a detailed, molecular level understanding of the energetics and dynamics of reaction processes. This involves the preparation of a molecule in defined electronic, vibrational, and rotational quantum states and observing not only the products of a reaction, but also how the total energy and angular momentum redistribute themselves among the various possible reaction channels followed by the parent molecule as it dissociates into fragments. In contrast to conventional methods in which chemical reactions can be only crudely controlled through variations of temperature and pressure, and in which all possible reaction channels are followed, a detailed, molecular level understanding of the reaction dynamics offers the possibility of close control of a reaction and thereby maximizing the efficiency of producing the desired reaction products. The present research will provide critical data which will allow the testing and further development of state-of-the-art theoretical models for various aspects of chemical reaction kinetics and dynamics.

本工作的目标是了解单分子反应动力学 小分子的基态电子态， 热单分子反应 三种实验将在 进行：1）红外光谱的分子活化与 足够的振动能解离，2）直接测量 解离速率在每秒100万到1000亿之间， 产物能态和角动量的测量 分布及其标量和矢量相关性， 激活分子的初始量子态 特别强调 将被赋予两种性质不同的原型分子--甲酰基 氟化物和乙烯酮。 化学反应的动力学处于 当代物理化学研究。 主要目的 是为了获得一个详细的，分子水平的 理解反应过程的能量学和动力学。 这涉及到制备一种具有特定电子结构的分子， 振动和转动量子态，不仅观察到 反应的产物，而且如何总能量和角动量 动量在各种可能的反应中重新分配 当母体分子解离成 片段与传统方法相比， 反应只能粗略地通过改变 温度和压力，并且其中所有可能的反应通道都 其次，详细的，分子水平的理解的反应 动力学提供了密切控制反应的可能性， 从而使产生所需反应的效率最大化 产品. 目前的研究将提供关键数据， 允许测试和进一步发展最先进的理论 化学反应动力学和动力学的各个方面的模型。