Yang Yizhang, Ren Hao, Zhang Ming, Zhou Shengpeng, Mu Xiangxu, Li Xiaokai, Wang Zhenzhen, Deng Ke, Li Mingxuan, Ma Pan, Li Zheng, Hao Xiaolei, Li Weidong, Chen Jing, Wang Chuncheng, Ding Dajun
Institute of Atomic and Molecular Physics and Jilin Provincial Key Laboratory of Applied Atomic and Molecular Spectroscopy, Jilin University, 130012, Changchun, China.
Institute of Theoretical Physics and Department of Physics, State Key Laboratory of Quantum Optics and Quantum Optics Devices, Collaborative Innovation Center of Extreme Optics, Shanxi University, 030006, Taiyuan, China.
Nat Commun. 2023 Aug 16;14(1):4951. doi: 10.1038/s41467-023-40628-9.
Neutral H formation via intramolecular hydrogen migration in hydrocarbon molecules plays a vital role in many chemical and biological processes. Here, employing cold target recoil ion momentum spectroscopy (COLTRIMS) and pump-probe technique, we find that the non-adiabatic coupling between the ground and excited ionic states of ethane through conical intersection leads to a significantly high yield of neutral H fragment. Based on the analysis of fingerprints that are sensitive to orbital symmetry and electronic state energies in the photoelectron momentum distributions, we tag the initial electronic population of both the ground and excited ionic states and determine the branching ratios of H formation channel from those two states. Incorporating theoretical simulation, we established the timescale of the H formation to be ~1300 fs. We provide a comprehensive characterization of H formation in ionic states of ethane mediated by conical intersection and reveals the significance of non-adiabatic coupling dynamics in the intramolecular hydrogen migration.
通过烃类分子内氢迁移形成中性氢在许多化学和生物过程中起着至关重要的作用。在此，我们采用冷靶反冲离子动量谱（COLTRIMS）和泵浦 - 探测技术，发现乙烷基态和激发态离子态之间通过锥形交叉的非绝热耦合导致中性氢碎片的产率显著提高。基于对光电子动量分布中对轨道对称性和电子态能量敏感的指纹分析，我们标记了基态和激发态离子态的初始电子布居，并确定了这两个态的氢形成通道的分支比。结合理论模拟，我们确定氢形成的时间尺度约为1300飞秒。我们全面表征了由锥形交叉介导的乙烷离子态中的氢形成，并揭示了非绝热耦合动力学在分子内氢迁移中的重要性。
