Exploring Mode Selective Behavior in the Dissociation Dynamics of Vibrationally Excited Molecules

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The Experimental Physical Chemistry Program supports Amitabha Sinha of The University of California - San Diego in his continuing studies on the influence of initial vibrational state selection on the dissociation dynamics of molecules. Using vibrational overtone-overtone double resonance, he can prepare HOCl in specific rovibrational states on the ground electronic state surface and investigate the expected non-statistical behavior. Photodissociation dynamics of molecules (e.g., CH3I and H2O) occurring on excited electronic states will also be investigated, with the goal to better understand the coupling of vibrational motion with nearly degenerate electronic excited states. The study of chemical reactions and their associated reaction dynamics stands at the forefront of contemporary physical chemistry. The goal of the present study is to understand how various molecular vibrations having similar total energy but corresponding to different intramolecular distribution of the excitation influence chemical reactivity. Measurements in which the excited states are fully resolved yield data which allow detailed comparisons with current theoretical models and promise to provide new insights into the factors that influence selectivity in chemical reactions.