Tan Yuxin, Zhao Bin, Yuan Daofu, Li Fan, Yu Shanshan, Jin Mengda, Zhang Yu, Luo Chang, Chen Wentao, Wang Tao, Zhu Jikai, Wang Ziwei, Yang Tiangang, Liu Shu, Manthe Uwe, Wang Xingan, Zhang Dong H, Yang Xueming
State Key Laboratory of Chemical Reaction Dynamics and Department of Chemical Physics, University of Science and Technology of China, Hefei, China.
Department of Chemistry, College of Science, Southern University of Science and Technology, Shenzhen, China.
Nat Commun. 2025 Jul 1;16(1):5893. doi: 10.1038/s41467-025-61117-1.
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 + CH → HD + CH reaction, a benchmark polyatomic elementary reaction with CH 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 CH(v' = 1) product umbrella bending vibrational state is observed to scatter more in the sideways direction than the CH(v' = 0) one. By monitoring the wave functions on a dividing surface in the transition state region, the CH umbrella bending mode is established as a reporter mode that faithfully reveals how the D atom dynamically approaches CH 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.
分子的非反应部分如何影响多原子反应一直是众多研究兴趣的主题。在此，我们利用高分辨率交叉分子束装置和精确的七维波包方法，对D + CH → HD + CH反应进行了全面研究，该反应是以CH作为非反应部分的基准多原子基元反应。观察到有趣的现象：CH(v' = 1)产物伞形弯曲振动态的角分布在侧向方向上比CH(v' = 0)的散射更多。通过监测过渡态区域中分隔面上的波函数，CH伞形弯曲模式被确立为一种报告模式，它能如实揭示D原子在不同总角动量或碰撞参数下如何动态接近CH。这种报告模式的发现为详细研究多原子反应动力学提供了契机。
