Revealing umbrella bending as a reporter mode in the D+CH4 reaction

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Abstract
How the non-reacting moiety of a molecule influences a polyatomic reaction has been a topic of much research interest. Here we present a comprehensive investigation of the D + CH4 → HD + CH3 reaction, a benchmark polyatomic elementary reaction with CH3 as the non-reacting moiety, employing a high-resolution crossed molecular beams apparatus and an accurate seven-dimensional wave packet method. An interesting angular distribution of the CH3(v’ = 1) product umbrella bending vibrational state is observed to scatter more in the sideways direction than the CH3(v’ = 0) one. By monitoring the wave functions on a dividing surface in the transition state region, the CH3 umbrella bending mode is established as a reporter mode that faithfully reveals how the D atom dynamically approaches CH4 at different total angular momenta or impact parameters. This discovery of the reporter mode provides an opportunity for the detailed study of polyatomic reaction dynamics.

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