Ultrafast Science, Volume. 1, Issue 1, 9837107(2021)

Ultrafast Hole Deformation Revealed by Molecular Attosecond Interferometry

Yindong Huang1,2, Jing Zhao1, Zheng Shu3, Yalei Zhu1, Jinlei Liu1, Wenpu Dong4, Xiaowei Wang1, Zhihui Lü1, Dongwen Zhang1, Jianmin Yuan1,5、*, Jing Chen3,6、*, and Zengxiu Zhao1、*
Author Affiliations
  • 1Department of Physics, National University of Defense Technology, Changsha, Hunan, China
  • 2Innovation Laboratory of Terahertz Biophysics, National Innovation Institute of Defense Technology, BeijingChina
  • 3Institute of Applied Physics and Computational Mathematics, Beijing, China
  • 4Hypervelocity Aerodynamics Institute, China Aerodynamics Research and Development Center, Mianyang, Sichuan, China
  • 5Graduate School of China Academic of Engineering Physics, BeijingChina
  • 6Shenzhen Key Laboratory of Ultra Intense Laser and Advanced Material Technology, Center for Advanced Material Diagnostic Technology, and College of Engineering Physics, Shenzhen Technology University, Shenzhen, China
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    Understanding the evolution of molecular electronic structures is the key to explore and control photochemical reactions and photobiological processes. Subjected to strong laser fields, electronic holes are formed upon ionization and evolve in the attosecond timescale. It is crucial to probe the electronic dynamics in real time with attosecond-temporal and atomic-spatial precision. Here, we present molecular attosecond interferometry that enables the in situ manipulation of holes in carbon dioxide molecules via the interferometry of the phase-locked electrons (propagating in opposite directions) of a laser-triggered rotational wave packet. The joint measurement on high-harmonic and terahertz spectroscopy (HATS) provides a unique tool for understanding electron dynamics from picoseconds to attoseconds. The optimum phases of two-color pulses for controlling the electron wave packet are precisely determined owing to the robust reference provided with the terahertz pulse generation. It is noteworthy that the contribution of HOMO-1 and HOMO-2 increases reflecting the deformation of the hole as the harmonic order increases. Our method can be applied to study hole dynamics of complex molecules and electron correlations during the strong-field process. The threefold control through molecular alignment, laser polarization, and the two-color pulse phase delay allows the precise manipulation of the transient hole paving the way for new advances in attochemistry.

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    Yindong Huang, Jing Zhao, Zheng Shu, Yalei Zhu, Jinlei Liu, Wenpu Dong, Xiaowei Wang, Zhihui Lü, Dongwen Zhang, Jianmin Yuan, Jing Chen, Zengxiu Zhao. Ultrafast Hole Deformation Revealed by Molecular Attosecond Interferometry[J]. Ultrafast Science, 2021, 1(1): 9837107

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    Paper Information

    Category: Research Articles

    Received: Mar. 25, 2021

    Accepted: May. 7, 2021

    Published Online: Sep. 15, 2023

    The Author Email: Yuan Jianmin (jmyuan@nudt.edu.cn), Chen Jing (chen_jing@iapcm.ac.cn), Zhao Zengxiu (zhao.zengxiu@gmail.com)

    DOI:10.34133/2021/9837107

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