How to measure a complete set of polarization-dependent differential cross sections in a scattering experiment with aligned reagents?

Polarization-dependent differential cross section (PDDCS) is one of the three-vector correlations (k, k′, j) in molecular collisions, which provides the most detailed insights into the steric requirements of chemical reactions, i.e., how the reactivity depends on the polarization of reagents. Only quite recently has such quantity been fully realized experimentally in the study of the reaction of the aligned CHD3(v1 = 1, |jK⟩ = |10⟩) molecules with Cl(2P3/2) atoms. Theoretically, PDDCS is a relatively new concept; experimental realization of the theoretical construct requires some careful considerations that are not readily available in the literature. Here, we present the “know-how” behind the full PDDCS measurements to fill the gaps and to provide a clear roadmap for future applications. To make the connection apparent between the methodology presented here and the stereodynamics revealed in previous reports, the same Cl + aligned CHD3 reaction is used for illustration.