Resonance and Electronically Non-Adiabatic Effects in State-To-State Reaction Dynamics Using Massively Parallel Computers

使用大规模并行计算机的状态到状态反应动力学中的共振和电子非绝热效应

• 批准号: 9632816
• 负责人: Aron Kuppermann
• 金额: $ 26.85万
• 依托单位: California Institute of Technology
• 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: 1996-08-01 至 1998-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9632816&HistoricalAwards=false
• 关键词: Resonance; Electronically; Non; Adiabatic; Effects

In this project Professor Kuppermann of the California Institute of Technology is being supported by the Theoretical and Computational Chemistry Program of the Chemistry Division. The project involves the study of electronic non-adiabatic effects in state-to-state chemical reaction dynamics. The primary reaction used is the hydrogen exchange reaction between H + H2 and various isotopic variants. Other reactions considered include the reaction of F + H2, as well as O + H2. Various ways of treating and incorporating multiple electronic surfaces and non-adiabatic effects will be investigated. Considerable use is being made of massively parallel supercomputers. Special attention is being placed on the role of the `geometric phase` in influencing the reaction probabilities for such reactions. Elementary bimolecular chemical reactions are the basic steps of complex technologically important chemical systems, such as combustion processes, atmospheric chemistry, chemical lasers, and plasma reactors. These systems may involve many steps whose reagents are very frequently short-lived and in many instances cannot be isolated experimentally. Studying their cross sections and rates theoretically constitutes in such cases the best, if not the only, available approach. Such studies also elucidate their molecular level details and lead to a fundamental understanding of how they occur. The theoretical description of very simple gas-phase chemical reactions such as those between a hydrogen atom and a hydrogen molecule, and oxygen atom and hydrogen molecule are being advanced in this computational study which makes use of massively parallel computers.

在这个项目中，加州研究所的库珀曼教授 技术正在得到理论和计算的支持， 化学系的化学课程。 该项目涉及 态-态化学中电子非绝热效应研究 反应动力学 所用的主要反应是氢交换 H + H2和各种同位素变体之间的反应。 其他反应 考虑的反应包括F + H2以及O + H2。 各种 处理和结合多个电子表面的方法， 将研究非绝热效应。 相当大的使用正在 由大规模并行的超级计算机组成。 特别注意的是， 放在影响反应的“几何相”的作用上 这种反应的可能性。 基元双分子化学反应是复杂化学的基本步骤 技术上重要的化学系统，如燃烧过程， 大气化学、化学激光器和等离子体反应堆。 这些 系统可能涉及许多步骤，这些步骤的试剂非常频繁地 寿命短，在许多情况下不能通过实验分离。 从理论上研究它们的截面和速率， 这是最好的，如果不是唯一的，可用的方法。 这些研究还 阐明它们的分子水平细节，并导致一个基本的 了解它们是如何发生的。 理论描述非常 简单的气相化学反应，如氢气和氢气之间的反应， 原子和氢分子，氧原子和氢分子， 在这项计算研究中， 并行计算机