Journal of Chemical Physics, Vol.100, No.2, 1040-1048, 1994
Interference Effects in the Photodissociation of Fno
Two-dimensional wave packet calculations on the photodissociation of FNO --> F + NO in the S-1 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 S-1 <-- S-0 transition rates.
Keywords:ULTRASHORT LASER-PULSES;ABSORPTION-SPECTRUM;CROSS-SECTION;STATE;CH3ONO;H2;PREDISSOCIATION;DISSOCIATION;DYNAMICS