Theoretical Studies of Inorganic and Organometallic Systems

有了化学系理论和计算化学项目的这笔赠款，霍尔教授将使用从头算全梯度几何优化技术，包括多组态自洽场和组态相互作用方法来解决目前无机和有机金属化学中感兴趣的问题。他将在三个领域继续开发方法。为了缩短在多处理计算机上求解的时间，他将继续编写并行代码，其中的梯度部分现已完成。为了处理大量的电子和轨道，他将对完全活跃空间多组态自洽场技术进行修改。最后，他将继续使用和提高对巴德拓扑学分析方法的理解。所研究的体系涉及催化中的三个基本步骤：氧化加成、取代和迁移插入。具体地说，他将研究几个关于C-H激活性质的重要问题。所使用的方法将使他能够得出关于一组密切相关的分子的结论，这些分子具有适度的基组和中等程度的电子相关性。霍尔教授将进行理论计算，帮助理解催化过程中重要的一些化学反应的基本步骤。

With this grant in the Theoretical and Computational Chemistry Program of the Chemistry Division, Professor Hall will use ab initio full-gradient geometry optimization techniques, including multiconfiguration self-consistent-field and configuration interaction methods to solve problems of current interest in inorganic and organometallic chemistry. He will continue methods development in three areas. To improve the time to solution on multiprocessing computers, he will continue working on parallel code of which the gradient section is now complete. In order to handle large numbers of electrons and orbitals, he will implement a modification of the complete active space multiconfiguration self-consistent-field technique. Lastly, he will continue the use of and improve the understanding of the topological method of analysis due to Bader. The systems to be studied are related to three fundamental steps in catalysis: oxidative-addition, substitution, and migratory-insertion. Specifically, he will examine several important questions about the nature of the C-H activation. The methods to be utilized will allow him to draw conclusions about a group of closely related molecules with modest basis sets and a moderate degree of electron correlation. %%% Professor Hall will perform theoretical compuations that will aid in understanding the elementary steps in a number of chemical reactions that are important in catalytic processes.