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.
