Vibrational excitation and relaxation for a molecule adsorbed on a surface is investigated in connection with desorption/ dissociation processes. The population equations for a laser-driven anharmonic oscillator involving both energy-and phase-relaxation mechanisms are derived with the Zwanzig projector technique and eigenfunction-expansion method due to Weidlich. Phase relaxation is seen to assist in the excitation of the resonant active mode.

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Kinetic studies of the absorption and emission of triplet acetone and the absorption of the ketyl radical, following flash excitation of acetone in a variety of solvents, are reported as well as the quantum yields of acetone disappearance.Rate constants of triplet quenching are derived and the pathways of deactivation of triplet acetone in solution are discussed.

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