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Time-resolved infrared-ultraviolet double resonance (IR-UV DR) spectroscopy is used to study the kinetics of collision-induced state-to-state molecular energy transfer between rovibrational states in the 12700-cm −1  4ν CH  manifold of the electronic ground state of acetylene (C 2 H 2 ). Particular initial and final rovibrational  J -states are prepared and monitored by a pair of tunable laser pulses (IR PUMP and UV PROBE) and the kinetic results recorded by continuously varying the time delay between those pulses at a set sample pressure. After allowing for collision-induced quenching of fluorescence and mass transfer from the IR-UV optical excitation zone (by beam flyout and diffusion), an array of kinetic data for  J -resolved energy-transfer channels can be interpreted by means of a mechanistically structured master-equation model. This paper focuses on kinetics derived by probing C 2 H 2  in its 4ν CH  J  = 12 state (which is affected by intramolecular perturbations and implicated in unusual collision-induced quasi-continuous background effects) and  J -resolved collision-induced rovibrational energy transfer with both even Δ J  and (supposedly forbidden) odd Δ J .

zeitschrift für physikalische chemie

Rovibrational Energy Transfer in the 4ν CH  Manifold of Acetylene, Viewed by IR-UV Double Resonance Spectroscopy. 3. State-to-State  J -Resolved Kinetics