Ultrafast Dynamics and Reactivity in Ground and Excited States: Beyond the Pump-probe Method

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In this project funded by the Experimental Physical Chemistry Program of the Chemistry Division, Dantus will use three-pulse, four-wave mixing (FWM) non-linear spectroscopy to study the dynamics of wave packet motion in the ground and excited states of NO2, CF3NO, and N2O4. The purpose of the work is to investigate intramolecular vibrational energy redistribution (IVR) and curve crossing dynamics in polyatomic systems and thereby open up the way for more general, and wider ranging investigations than done heretofore on diatomics. Specific questions to be answered in this research are about the initial steps of energy dissipation and IVR in polyatomics, what is the nature of wave packet localization in phase space for multidimensional systems, and what is the ground state dynamics in systems with chemically significant amounts of energy, up to 12,000 cm-1.This project deals with fundamental questions of how energy absorbed into specific molecular energy states redistributes itself throughout a molecule in the course of time. A good understanding of these intramolecular processes may lead to the laser control of chemical reactions. This research is undertaken with students and postdoctoral research associates. They will acquire training and knowledge in one the forefront areas of contemporary physical chemistry in preparation for advanced studies or employment in industry, government or academia.