State-to-state integral cross sections for the inelastic scattering of CH(X 2Π)+He: Rotational rainbow and orbital alignment

Abstract

The state-to-state integral cross sections for the inelastic scattering of CH(X 2Π) with He were measured in a newly constructed crossed molecular beam machine. Use of laser-induced fluorescence in an unconventional flux mode of detection provided single fine-structure state specific detection of the products. Two types of measurements were performed to further our understanding of the collision dynamics of open shell systems: (1) the product state distribution at a fixed and well-defined collision energy and (2) the dependence on collision energy of product state-resolved cross sections. A qualitative understanding of the collision dynamics can be obtained by properly factoring out features dependent on the fine-structure states, i.e., effects involving individual Λ-doublet states and features dependent on the rotational level alone, i.e., effects remaining after summing over all four fine-structure states associated with a given rotational quantum number. As for the fine-structure effects, a preferential population of product Λ-doublet states with reflection symmetry Π(A″) was observed. The physical origin of this observed electronic orbital alignment can be attributed to a quantum interference phenomenon, as detailed in the accompanying paper. At the rotational level, the dominance of rotational rainbow scattering is unambiguously identified from both the existence of dynamical thresholds and a strong correlation between rotational level distributions at fixed translational energy and level specific excitation functions. These effects combined with other experimental observations lead us to visualize the CH+He scattering dynamics in a novel fashion. The collision can be regarded as a series of approximately independent sequential events each mediated by different regions of the interaction potential during the course of the whole encounter.