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Directly imaging excited state-resolved transient structures of water induced by valence and inner-shell ionisation

Author

Listed:
  • Zhenzhen Wang

    (Jilin University)

  • Xiaoqing Hu

    (Institute of Applied Physics and Computational Mathematics)

  • Xiaorui Xue

    (Xi’an Jiaotong University)

  • Shengpeng Zhou

    (Jilin University)

  • Xiaokai Li

    (Jilin University)

  • Yizhang Yang

    (Jilin University)

  • Jiaqi Zhou

    (Xi’an Jiaotong University)

  • Zheng Shu

    (Institute of Applied Physics and Computational Mathematics)

  • Banchi Zhao

    (Jilin University)

  • Xitao Yu

    (Jilin University)

  • Maomao Gong

    (University of Science and Technology of China
    Shaanxi Normal University)

  • Zhenpeng Wang

    (Institute of Applied Physics and Computational Mathematics
    University of Science and Technology of China)

  • Pan Ma

    (Jilin University)

  • Yong Wu

    (Institute of Applied Physics and Computational Mathematics
    Peking University)

  • Xiangjun Chen

    (University of Science and Technology of China)

  • Jianguo Wang

    (Institute of Applied Physics and Computational Mathematics)

  • Xueguang Ren

    (Xi’an Jiaotong University)

  • Chuncheng Wang

    (Jilin University)

  • Dajun Ding

    (Jilin University)

Abstract

Real-time imaging of transient structure of the electronic excited state is fundamentally critical to understand and control ultrafast molecular dynamics. The ejection of electrons from the inner-shell and valence level can lead to the population of different excited states, which trigger manifold ultrafast relaxation processes, however, the accurate imaging of such electronic state-dependent structural evolutions is still lacking. Here, by developing the laser-induced electron recollision-assisted Coulomb explosion imaging approach and molecular dynamics simulations, snapshots of the vibrational wave-packets of the excited (A) and ground states (X) of D2O+ are captured simultaneously with sub-10 picometre and few-femtosecond precision. We visualise that θDOD and ROD are significantly increased by around 50∘ and 10 pm, respectively, within approximately 8 fs after initial ionisation for the A state, and the ROD further extends 9 pm within 2 fs along the ground state of the dication in the present condition. Moreover, the ROD can stretch more than 50 pm within 5 fs along autoionisation state of dication. The accuracies of the results are limited by the simulations. These results provide comprehensive structural information for studying the fascinating molecular dynamics of water, and pave the way towards to make a movie of excited state-resolved ultrafast molecular dynamics and light-induced chemical reaction.

Suggested Citation

  • Zhenzhen Wang & Xiaoqing Hu & Xiaorui Xue & Shengpeng Zhou & Xiaokai Li & Yizhang Yang & Jiaqi Zhou & Zheng Shu & Banchi Zhao & Xitao Yu & Maomao Gong & Zhenpeng Wang & Pan Ma & Yong Wu & Xiangjun Che, 2023. "Directly imaging excited state-resolved transient structures of water induced by valence and inner-shell ionisation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41204-x
    DOI: 10.1038/s41467-023-41204-x
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    References listed on IDEAS

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