Chemisorption on Metal Surfaces via Density Functional Theory Embedding of Ab Initio Finite Cluster Calculations

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The Theoretical and Computational Chemistry program is supporting a research effort where a hybrid electronic structure technique will be developed by Prof. E.A. Carter of UCLA that first utilizes density functional theory to obtain an accurate electron density distribution for a metal, which then is used (along with its corresponding orbital representation) to provide a set of Coulomb and exchange operators that describe the interaction of the infinite metal surface and bulk crystal with a chemisorption region (composed of a few metal atoms and an adsorbed molecule). The chemisorption region is then described using a local multireference configuration interaction method in the presence of the embedding Coulomb and exchange field derived from density functional theory. The goal is to develop and test this hybrid DFT/CI method, with the hope that it will provide the most accurate means yet of studying chemisorption on metal surfaces from first principles theories. A new theory involving a mixture of quantum chemistry and solid state physics techniques will be developed. The theory utilizes quantum physics known for its accuracy in describing metals and quantum chemistry known for its accuracy in describing metal-molecule chemical bonds. These taken together are expected to provide the most accurate means yet of modelling chemical reactions that occur on metal surfaces. Many important industrial technologies rely on such reactions and it is hoped that the new theory will help optimize such technologies further.