Model study on the real-time detection of ultrafast nonadiabatic dynamics associated with the Wulf-Chappuis bands of ozone

Abstract

Model calculations on the cw absorption spectrum and femtosecond time-resolved stimulated-emission pump—probe spectra are reported for the Wulf—Chappuis bands of ozone. The model accounts for the three dimensional conical intersection of the 1A 2 and 1B 1 excited states and the associated singular non-Born—Oppenheimer coupling. Effects of dissociation into O+O 2 are modelled phenomenologically. It is demonstrated on the basis of this model that detailed information on the ultrafast nonadiabatic excited-state dynamics can be obtained by pump—probe spectroscopy with ultrashort pulses (pulse duration of the order of 10 fs).