Abstract
Fluorescence-detected Raman-ultraviolet double resonance spectroscopy enables state-selective investigations of vibrational energy transfer in gas-phase acetylene, C2H2. Pulsed coherent Raman excitation of the (v2 + v4 - v4) rovibrational hot band of C2H2(g) is followed by rovibronic probing of collision-induced population transfer to the v2 vibrational level. This time-resolved spectroscopic technique provides novel kinetic and mechanistic information on the quasi-elastic intermolecular V−V transfer process: C2H2(v2 + v4) + C2H2(v = 0) → C2H2(v2) + C2H2(v4). The state-to-state second-order rate constant for this process is measured and its relevance to the dynamics of vibrational energy transfer is discussed. The results demonstrate the advantages of rotationally resolved double-resonance tecniques in elucidating vibrational energy transfer processes.
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