New methods, applications and software tools in quantum reaction dynamics.

摘要

This dissertation is divided into two parts. Part I presents a theoretical study of new methodologies for accurate quantum reaction dynamics calculations. A novel approach, Reaction-Product Decoupling method, is described in details. This method aims at providing an efficient and flexible approach to obtaining state-to-state reaction information in rigorous quantum mechanical reaction dynamics calculations using a divide-and-conquer strategy. Its theoretical grounds, extensions and test results on benchmark systems are thoroughly discussed.; Also in Part I is a full-dimensional quantum mechanical study of a very important prototype reaction system: O(1 D) + H₂. This reaction plays an important role in many branches of chemistry and has been the focus of intensive study for decades. Works in this dissertation was the first rigorous full-dimensional quantum mechanical treatment on this reaction as far as the author is aware. The results provided a reliable and definitive reference for many other research works on this reaction, such as development of approximate methods and evaluation of the PES.; Part II describes a new computer software package DynaSolver, whose development the author has been in charge. DynaSolver is a software package for chemical reaction dynamics calculations with a modern Graphical User Interface. In this dissertation, its features and functionality are introduced. The ideas behind its design and implementation, its internal structure and some technical aspects are also presented. DynaSolver is a newly started project and we expect it to evolve into a very useful tool for the reaction dynamics community.