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The predissociation dynamics of the vibrationless level of the first Rydbergstate 6s (B 2E) state of CH3I has been studied by femtosecond-resolved velocitymap imaging of both the CH3 and I photofragments. The kinetic energydistributions of the two fragments have been recorded as a function of thepump-probe delay, and as a function of excitation within the umbrella andstretching vibrational modes of the CH3 fragment. These observations are madeby using (2+1) Resonant Enhanced MultiPhoton Ionization (REMPI) via the 3pz2A2" state of CH3 to detect specific vibrational levels of CH3. The vibrationalbranching fractions of the CH3 are recovered by using the individualvibrationally state-selected CH3 distributions to fit the kinetic energydistribution obtained by using nonresonant multiphoton ionization of either theI or CH3 fragment. The angular distributions and rise times of the twofragments differ significantly. These observations can be rationalized througha consideration of the alignment of the CH3 fragment and the effect of thisalignment on its detection efficiency. Two extra dissociation channels aredetected: one associated with Rydberg states near 9.2 eV that were observedpreviously in photoelectron studies, and one associated with photodissociationof the parent cation around 15 eV.

Time-resolved predissociation of the vibrationless level of the B state of CH3I