Using ion imaging to analyze higher-order moments of the angular distributions of photofragments

We investigate the effect of the hexadecapole (K=4) polarization moment on the spatial distributions of angular momenta for atoms produced during the photodissociation of diatomic or triatomic molecules by polarized radiation. We derive general expressions for the angular distributions of the atomic density matrix for K = 2, 4 and expressions for the corresponding anisotropy parameters that contain all information on the photodissociation dynamics. We show that these anisotropy parameters can be experimentally determined by using ion imaging. We consider oxygen atoms in the ¹ D ₂ state aligned with respect to the orbital angular momentum as an example and provide ion images of the signals that correspond to the population of the atomic magnetic sublevels ¦m¦ = 0, 1, 2. We show the contributions from the second-and fourth-rank state multipoles to the angular distributions of the atomic density matrix to be comparable in magnitude and significantly different in form.