Atomic orbital alignment and coherence in N2O photodissociation at 193.3 nm

Strong recoil-frame orbital alignment is observed in the (OD2)-D-1 product following photodissociation of N2O at 193.3 nm. Velocity map imaging allows for investigation of the angular distribution of this alignment, providing insight into the dynamics in the frame of the molecule. Analysis of the results using a rigorous quantum mechanical theory yields alignment anisotropy parameters having direct physical significance. This alignment is dominated by strong incoherent parallel and perpendicular contributions. In addition, evidence is shown of a contribution from a perpendicular coherence. These results provide detailed insight into the dynamics of the photodissociation process and the nature of the electronic transitions responsible for the initial excitation.