Abstract
By means of triplet-triplet energy transfer to biacetyl, the population of the vibrationally relaxed triplet state T 0 1 of the alicyclic ketones cycloheptanone, cyclohexanone, and cyclopentanone was examined as a function of the excitation wavelength. This population, as measured in terms of the ketone triplet yield φ T(λ), was compared with the excitation energy dependence of the photochemical quantum yield. This comparison demonstrated that the main photochemical path of these ketones originates from higher vibrational levels of T 1. Thus, φ T(λ) reflects the branching ratio between a non-RRKM photochemical decay and the vibrational relaxation process to T 1. Moreover, φ T(λ) was found to decrease significantly in the order cycloheptanone > cyclohexanone > cyclopentanone. This observation reflects, at least in part, the influence of the internal degrees of freedom on the vibrational relaxation rate.
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