Eitan Geva of the University of Michigan is supported by an award from the Chemical Theory, Models and Computational Methods program to carry out research on the development of theoretical and computational tools that would provide an atomistically detailed description of a wide range of nonequilibrium electronic, vibrational and conformational processes and their spectroscopic signature. This study involves method development in the context of recent experimental measurements of vibrational energy relaxation rates of polar and ionic species in polar and protic solvents, multidimensional infrared spectra of the hydroxyl stretch in alcohols and of the carbonyl stretch in metal-carbonyl complexes and solvent effects on isomerization rates in liquid solution. These studies also involve collaborations with experimentalists and theorists who are colleagues in Geva's department.
Vibrational and electronic relaxation is inherent to nearly all processes that are important in chemistry, including many that have relevance to biological systems. Nonlinear optical spectroscopic techniques are powerful probes of the structure and dynamics of complex systems. Theoretical methods, such as those developed by the PI and his research group, are indispensible for interpreting these spectra. The work is having a broader impact through the training of students at all levels, curriculum development and the dissemination of computer codes.