Theory of Chemical Dynamics

加州大学伯克利分校的威廉·米勒（William Miller）得到了理论与计算化学项目（Theoretical and Computational Chemistry Program）的支持，致力于发展能够提供化学动力学定量描述的理论概念和方法，这是一种“从头算化学动力学”，类似于电子结构理论的从头算量子化学。这些方法在特定化学系统中的新应用将用于说明或演示新的方法和概念。计算反应通量相关函数以给出化学反应速率是这项工作的中心主题，使用半经典（SC）初始值表示（IVR）方法探索稀有气团中的过程将继续进行。总体目标是将SC-IVR方法转换为一种形式，使其适用于几乎所有可以进行经典分子动力学模拟的系统。这项研究旨在探索一种潜在的通用化学动力学处理方法的发展，包括对非常小的粒子很重要的量子力学效应。这种方法可以提高在固体和溶液中发生的化学过程的预测能力，从而对化学、生物学和物理学的重要领域产生影响。

William Miller of the University of California, Berkeley, is supported by the Theoretical and Computational Chemistry Program to develop theoretical concepts and methodologies that can provide a quantitative description of chemical dynamics, a kind of "ab initio chemical dynamics" akin to the ab initio quantum chemistry of electronic structure theory. New applications of these approaches to specific chemical systems will be carried out to illustrate or demonstrate the new methods and concepts. Computation of reactive flux correlation functions to give chemical reaction rates is a central topic for this effort, and exploration of processes in rare gas clusters using semiclassical (SC) initial value representation (IVR) approaches will continue. The overall goal is to cast the SC-IVR methodology in a form that will make it practical for virtually all systems for which classical molecular dynamics simulation is possible.This research aims to explore the development of a potentially universal treatment of chemical dynamics, including the quantum mechanical effects that are important for very small particles. This approach may improve the predictive capabilities for chemical processes that occur in solids and solutions, with resulting impact in important areas of chemistry, biology, and physics.