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

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 Chen, Jianguo Wang, Xueguang Ren (), Chuncheng Wang () and Dajun Ding ()
Additional contact information
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
Zhenpeng Wang: Institute of Applied Physics and Computational Mathematics
Pan Ma: Jilin University
Yong Wu: Institute of Applied Physics and Computational Mathematics
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

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-41204-x

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