In this project, funded by the Experimental Physical Chemistry Program of the Chemistry Division, Professor Charles Harris and his students at the University of California, Berkeley will study elementary steps in complex chemical reactions using ultrafast pump-probe experiments and transient two-dimensional infrared spectroscopy. The experimental work will be combined with theoretical modeling to provide insights into the detailed microscopic mechanisms of several prototypical, organometallic reactions, including C-H and Si-H bond activation and the reactions of 17- and 19-electron species in ligand substitution and disproportionation. These studies promise to demonstrate the ability of ultrafast infrared techniques to improve our understanding of organometallic chemistry, including reactions of importance in catalysis. The research also will provide training in time-resolved spectroscopy and theoretical chemistry to graduate students and postdoctoral research associates.