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

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...

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Main Authors: Yuxin Tan, Bin Zhao, Daofu Yuan, Fan Li, Shanshan Yu, Mengda Jin, Yu Zhang, Chang Luo, Wentao Chen, Tao Wang, Jikai Zhu, Ziwei Wang, Tiangang Yang, Shu Liu, Uwe Manthe, Xingan Wang, Dong H. Zhang, Xueming Yang
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-61117-1
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Summary: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.
ISSN:2041-1723