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

作　　者：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 

机构地区：[1]School of Physics and Wuhan National Laboratory for Optoelectronics,Huazhong University of Scienceand Technology,Wuhan 430074,China [2]Key Laboratory of Computational Physics,Institute of Applied Physics and Computational Mathematics,Beijing 100088,China [3]School of Physics and Information Technology,Shaanxi Normal University,Xi'an 710119,China

出　　处：《Ultrafast Science》2024年第6期45-52,共8页超快科学(英文)

基　　金：supported by the National Key Research and Development Program of China(grant no.2023YFA1406800);the National Natural Science Foundation of China(grant nos.62275085,12021004,11934004,and 12104063).

摘　　要：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 O+2 molecule.We observe that the electron density changes its shape from that of a molecularσorbital to a nearly isotropic shape as the internuclear distance goes up to∼20?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.

关 键 词：electronic dynamics coupling interactions rotational dynamics coupled nuclear electronic dynamics coriolis coupling 

分 类 号：O561[理学—原子与分子物理]