Ultrafast Science, Volume. 4, Issue 1, 0073(2024)

Probing Coupled Rotational and Electronic Dynamics during Laser-Induced Molecular Fragmentation

Keyu Guo1,†... Xiaoqing Hu2,†, Min Li1,*, Cong-Cong Jia2, Songbin Zhang3, Chuanpeng Cao1, Wenhai Xie1, Wei Cao1, Kunlong Liu1, Yueming Zhou1, Yong Wu2,*, Jianguo Wang2 and Peixiang Lu1,* |Show fewer author(s)
Author Affiliations
  • 1School of Physics and Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, China.
  • 2Key Laboratory of Computational Physics, Institute of Applied Physics and Computational Mathematics, Beijing 100088, China.
  • 3School of Physics and Information Technology, Shaanxi Normal University, Xi'an 710119, China.
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    Coupled nuclear and electronic dynamics within a molecule are key to understanding a broad range of fundamental physical and chemical processes. Although probing the coupled vibrational and electronic dynamics was demonstrated, it has so far been challenging to observe the coupling interactions between the rotational and electronic degrees of freedom. Here, we report the first observation of Coriolis coupling, a coupling interaction between nuclear rotational angular momentum and electronic axial angular momentum, during laser-induced molecular fragmentation by tracing the electronic structure of a dissociating O2+ molecule. We observe that the electron density changes its shape from that of a molecular σ orbital to a nearly isotropic shape as the internuclear distance goes up to ∼20 Å, which results from the transition between nearly degenerate electronic states associated with different rotational angular momenta. Our experiment demonstrates that the breaking of a chemical bond does not occur suddenly during molecular dissociation. Instead, it lasts for a long time of several hundred femtoseconds due to the Coriolis coupling interaction. Our experiment can be extended to complicated molecules, holding the potential of revealing yet unobserved electron–nuclear coupling interactions during ultrafast processes.

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    Keyu Guo, Xiaoqing Hu, Min Li, Cong-Cong Jia, Songbin Zhang, Chuanpeng Cao, Wenhai Xie, Wei Cao, Kunlong Liu, Yueming Zhou, Yong Wu, Jianguo Wang, Peixiang Lu. Probing Coupled Rotational and Electronic Dynamics during Laser-Induced Molecular Fragmentation[J]. Ultrafast Science, 2024, 4(1): 0073

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    Paper Information

    Category: Research Articles

    Received: Mar. 27, 2024

    Accepted: Jul. 26, 2024

    Published Online: Dec. 13, 2024

    The Author Email: Li Min (mli@hust.edu.cn), Wu Yong (wu_yong@iapcm.ac.cn), Lu Peixiang (lupeixiang@hust.edu.cn)

    DOI:10.34133/ultrafastscience.0073

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