In this project in the Experimental Physical Chemistry Program of the Chemistry Division, Vaccaro will study the spectroscopy, relaxation, and chemical reactivity of rovibrationally excited polyatomic molecules as a function of both the magnitude and type of excitation of the molecular framework. The first state-to-state measurements of polyatomic reaction dynamics will be performed. Novel multiple-resonance laser techniques will be used to prepare molecules in specific rotation-vibration states. %%% Studies of the reactivity of polyatomic molecules which contain chemically significant quantities of energy of excitation are important because of the information they can reveal about aeronomic and combustion-related processes. On a fundamental scientific level, these transient species can reveal much regarding the nature and origin of such phenomena as mode- or bond-specific chemistry and quantum chaos.