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

在这个由美国国家科学基金会理论与计算化学计划支持的研究项目中，高水平的从头算理论，使用良好的轨道基集和相关波函数，被应用于过渡金属化学的广泛问题，涵盖了从只有6个原子的简单过渡金属配合物到完整催化循环的研究。对过渡金属配合物活化H-H键和C-H键进行了系统的比较。对现有从头算方法的改进包括使用有效核心势的计算技术的进一步发展。分子电子结构理论的现代方法应用于过渡金属化学。详细的计算将进行小分子系统，表现出基本的键合原理。更大规模的现实模型计算也将进行。这项研究的特点是将高度严谨的理论应用于如此大的分子系统。这些利用超级计算机进行的计算有望对过渡金属配合物催化的典型化学反应中发生的分子事件产生可靠和更详细的图像。这种催化过程广泛应用于化学工业。希望和期望是，这项研究最终将有利于这些行业。

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.