Theoretical Studies of Structure and Reactions of Transition Metal Atoms, Ions, Complexes and Cluster Complexes

在NSF理论和计算化学项目的支持下，利用良好的轨道基组和相关波函数，高级从头计算理论被应用于过渡金属化学中的一系列问题，从简单的六个原子的过渡金属络合物到研究完整的催化循环。系统地比较了过渡金属络合物对H-H键和C-H键的活化作用。对现有从头算方法的改进包括进一步发展使用有效核心势的计算技术。将分子电子结构理论中的现代方法应用于过渡金属化学。对于表现出基本成键原理的小分子体系，将进行详细的计算。还将进行更大规模的真实模型计算。这项研究的特点是将高度严谨的理论应用于这样的大分子系统。这些使用超级计算机的计算预计将产生可靠和更详细的分子事件图，这些事件发生在过渡金属络合物催化的典型化学反应中。这种催化过程在化学工业中得到了广泛的应用。希望和期待的是，这项研究最终将使这些行业受益。

In this research project, supported by the NSF Theoretical and Computational Chemistry Program, high level ab initio theory, using good orbital basis sets and correlated wavefunctions, are applied to a broad range of problems in transition metal chemistry spanning the range of simple transition metal complexes with as few as six atoms to studies of full catalytic cycles. A systematic comparison will be carried out of H-H and C-H bond activation by transition metal complexes. Improvements to existing ab initio methodology include the further development of computational techniques using effective core potentials. Modern methods in molecular electronic structure theory are applied to transition metal chemistry. Detailed calculations will be carried out for small molecular systems which exhibit fundamental bonding principles. Much larger scale computations of realistic models will also be carried out. This research is distinguished by the application of highly rigorous theory to such large molecular systems. These computations using supercomputers are expected to yield a reliable and more detailed picture of the molecular events which occur during typical chemical reactions catalyzed by transition metal complexes. Such catalytic processes are widely employed in the chemical industry. The hope and expectation is that this research will eventually benefit these industries.