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 () and Peixiang Lu ()
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Min Li: Huazhong University of Science and Technology
Ming Zhang: Peking University
Oriol Vendrell: Universität Heidelberg
Zhenning Guo: Peking University
Qianru Zhu: Huazhong University of Science and Technology
Xiang Gao: Huazhong University of Science and Technology
Lushuai Cao: Huazhong University of Science and Technology
Keyu Guo: Huazhong University of Science and Technology
Qin-Qin Su: Huazhong University of Science and Technology
Wei Cao: Huazhong University of Science and Technology
Siqiang Luo: Huazhong University of Science and Technology
Jiaqing Yan: Huazhong University of Science and Technology
Yueming Zhou: Huazhong University of Science and Technology
Yunquan Liu: Peking University
Zheng Li: Peking University
Peixiang Lu: Huazhong University of Science and Technology

Nature Communications, 2021, vol. 12, issue 1, 1-6

Abstract: 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 $${{\rm{CH}}}_{4}^{+}$$ CH 4 + cation in symmetry space. It is unraveled that the Jahn-Teller deformation from C3v to C2v 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 C2v structure involving complex revival process of multiple vibrational pathways of the $${{\rm{CH}}}_{4}^{+}$$ CH 4 + cation.

Date: 2021
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DOI: 10.1038/s41467-021-24309-z

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