Femtosecond coincidence imaging of multichannel multiphoton dynamics

The novel technique of femtosecond time-resolved photoelectron-photoion coincidence imaging is applied to unravel dissociative ionization processes in a polyatomic molecule. Femtosecond coincidence imaging of CF3I photodynamics illustrates how competing multiphoton dissociation pathways can be distinguished, which would be impossible using photoelectron or ion imaging alone. Ion-electron energy correlations and photoelectron angular distributions reveal competing processes for the channel producing (e(-)+CF3++I). The molecular-frame photoelectron angular distributions of the two major pathways are strikingly different.