Observation of Coherent and Incoherent Dissociation Mechanisms in the Angular Distribution of Atomic Photofragment Alignment

We have analyzed the recoil angle dependence of chlorine atom angular momentum alignment for the dissociation of chlorine molecules at 355 nm. This angular distribution was isolated from ion image measurements, which map a three-dimensional velocity vector distribution of state-selectively-ionized photofragments into a two-dimensional spatial distribution. Using a general quantum mechanical method to simulate the alignment angular distribution, we show that there are clear contributions to alignment from both incoherent and coherent components of a perpendicular optical transition in the molecule.