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Ultrafast imaging of spontaneous symmetry breaking in a photoionized molecular system

Author

Listed:
  • Min Li

    (Huazhong University of Science and Technology)

  • Ming Zhang

    (Peking University
    University of Science and Technology Beijing)

  • 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
    Wuhan Institute of Technology
    CAS Center for Excellence in Ultra-intense Laser Science)

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.

Suggested Citation

  • 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 & Peixi, 2021. "Ultrafast imaging of spontaneous symmetry breaking in a photoionized molecular system," Nature Communications, Nature, vol. 12(1), pages 1-6, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-24309-z
    DOI: 10.1038/s41467-021-24309-z
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    Cited by:

    1. Ivica Živković & Jian-Rui Soh & Oleg Malanyuk & Ravi Yadav & Federico Pisani & Aria M. Tehrani & Davor Tolj & Jana Pasztorova & Daigorou Hirai & Yuan Wei & Wenliang Zhang & Carlos Galdino & Tianlun Yu, 2024. "Dynamic Jahn-Teller effect in the strong spin-orbit coupling regime," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Xiaochun Gong & Étienne Plésiat & Alicia Palacios & Saijoscha Heck & Fernando Martín & Hans Jakob Wörner, 2023. "Attosecond delays between dissociative and non-dissociative ionization of polyatomic molecules," Nature Communications, Nature, vol. 14(1), pages 1-8, December.

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