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Two-dimensional wave packet calculations on the photodissociation of FNO→F+NO in the S1 state were carried out to analyze the asymmetric resonance line shapes (Fano profiles) in the absorption spectrum in terms of a continuum, a resonance, and an interference contribution. Vibrationally resolved partial cross sections were calculated which predict a strong variation of the vibrational state distribution in the NO fragment as a function of the energy in the vicinity of a resonance. This effect is due to a substantial interference contribution to the vibronic absorption cross section. The results were compared to recent experimental findings by Reisler and co-workers and to the Fano model applied to predissociation. Further, we simulated the excitation with a semi-infinite laser pulse to extract resonance energies from the time behavior of the calculated S1←S0 transition rates.
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Cotting et al. (1994) studied this question.
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