Ultrafast imaging of spontaneous symmetry breaking in a photoionized molecular system

Min Li; Ming Zhang; Oriol Vendrell; Zhenning Guo; Qianru Zhu; Xiang Gao; Lushuai Cao; Keyu Guo; Qin-Qin Su; Wei Cao; Siqiang Luo; Jiaqing Yan; Yueming Zhou; Yunquan Liu; Zheng Li; Peixiang Lu

doi:10.1038/s41467-021-24309-z

Ultrafast imaging of spontaneous symmetry breaking in a photoionized molecular system

Nat Commun. 2021 Jul 9;12(1):4233. doi: 10.1038/s41467-021-24309-z.

Authors

Min Li^#¹, Ming Zhang^#^{2

3}, Oriol Vendrell⁴, Zhenning Guo², Qianru Zhu⁵, Xiang Gao⁵, Lushuai Cao⁵, Keyu Guo¹, Qin-Qin Su¹, Wei Cao⁶, Siqiang Luo¹, Jiaqing Yan¹, Yueming Zhou¹, Yunquan Liu⁷, Zheng Li⁸, Peixiang Lu^{9

10

11}

Affiliations

¹ Wuhan National Laboratory for Optoelectronics and School of Physics, Huazhong University of Science and Technology, Wuhan, China.
² State Key Laboratory for Mesoscopic Physics and Collaborative Innovation Center of Quantum Matter, School of Physics, Peking University, Beijing, China.
³ University of Science and Technology Beijing, Beijing, China.
⁴ Physikalisch-Chemisches Institut, Universität Heidelberg, Heidelberg, Germany.
⁵ MOE Key Laboratory of Fundamental Physical Quantities Measurement and Hubei Key Laboratory of Gravitation and Quantum Physics, PGMF and School of Physics, Huazhong University of Science and Technology, Wuhan, China.
⁶ Wuhan National Laboratory for Optoelectronics and School of Physics, Huazhong University of Science and Technology, Wuhan, China. weicao@hust.edu.cn.
⁷ State Key Laboratory for Mesoscopic Physics and Collaborative Innovation Center of Quantum Matter, School of Physics, Peking University, Beijing, China. yunquan.liu@pku.edu.cn.
⁸ State Key Laboratory for Mesoscopic Physics and Collaborative Innovation Center of Quantum Matter, School of Physics, Peking University, Beijing, China. zheng.li@pku.edu.cn.
⁹ Wuhan National Laboratory for Optoelectronics and School of Physics, Huazhong University of Science and Technology, Wuhan, China. lupeixiang@hust.edu.cn.
¹⁰ Hubei Key Laboratory of Optical Information and Pattern Recognition, Wuhan Institute of Technology, Wuhan, China. lupeixiang@hust.edu.cn.
¹¹ CAS Center for Excellence in Ultra-intense Laser Science, Shanghai, China. lupeixiang@hust.edu.cn.

^# Contributed equally.

Abstract

The Jahn-Teller effect is an essential mechanism of spontaneous symmetry breaking in molecular and solid state systems, and has far-reaching consequences in many fields. Up to now, to directly image the onset of Jahn-Teller symmetry breaking remains unreached. Here we employ ultrafast ion-coincidence Coulomb explosion imaging with sub-10 fs resolution and unambiguously image the ultrafast dynamics of Jahn-Teller deformations of [Formula: see text] cation in symmetry space. It is unraveled that the Jahn-Teller deformation from C_3v to C_2v geometries takes a characteristic time of 20 ± 7 fs for this system. Classical and quantum molecular dynamics simulations agree well with the measurement, and reveal dynamics for the build-up of the C_2v structure involving complex revival process of multiple vibrational pathways of the [Formula: see text] cation.

Abstract

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