In this project in the Physical Chemistry program of the Chemistry Division, Professor Patrick Vaccaro of Yale University will perform a series of experiments which combine the methods of Degenerate -Four-Wave-Mixing and Stimulated-Emission-Pumping. The chemistry of isomerization will be studied on disulfur monoxide and isocyanogen. A state-specific study of the proton transfer in malonaldehyde will also be carried out. Emphasis will be placed upon the identification and characterization of any vibrational mode selectivity that accompanies intramolecular rearrangement of chemical bonds. This research is in the broad area of molecular structure and dynamics. Its purpose is to explore the underlying impetus for chemical transformations. Information obtained from these experiments on vibrationally excited polyatomic species will provide insight into unimolecular processes which play a critical role in chemistry, including isomerization and hydrogen migration.