Orbital polarization from DC slice imaging: S(1D2) alignment in the photodissociation of ethylene sulfide

DC slice imaging [Rev. Sci. Instrum. 74 (2003) 2530], a recently developed high-resolution 'slicing' approach that directly provides the full 3D product distribution in imaging experiments, has been adapted to yield the absolute speed-dependent angular momentum alignment anisotropy parameters in a photodissociation experiment. We present the theoretical machinery for interpretation of a small basis set of sliced experimental images recorded under different laser polarization geometries and then demonstrate its application in the study of electronic orbital angular momentum alignment of excited state S(1D2) atoms following 193.3 nm photodissociation of ethylene sulfide. We find the slicing approach to be a highly sensitive and widely applicable technique for the study of orbital polarization, even in instances where the magnitude of such effects is small. The approach outlined here represents a direct route to the determination of recoil-angle dependent orbital alignment for a continuous range of photofragment kinetic energy release