Channel Coupling Dynamics of Deep-Lying Orbitals in Molecular High-Harmonic Generation

Zheng Shu, Hongjing Liang, Yichen Wang, Shilin Hu, Shi Chen, Haifeng Xu, Ri Ma, Dajun Ding, and Jing Chen
Phys. Rev. Lett. 128, 183202 – Published 6 May 2022
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Abstract

Investigation on structures in the high-harmonic spectrum has provided profuse information of molecular structure and dynamics in intense laser fields, based on which techniques of molecular ultrafast dynamics imaging have been developed. Combining ab initio calculations and experimental measurements on the high-harmonic spectrum of the CO2 molecule, we find a novel dip structure in the low-energy region of the harmonic spectrum which is identified as fingerprints of participation of deeper-lying molecular orbitals in the process and decodes the underlying attosecond multichannel coupling dynamics. Our work sheds new light on the ultrafast dynamics of molecules in intense laser fields.

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  • Received 18 September 2021
  • Revised 15 February 2022
  • Accepted 15 April 2022

DOI:https://doi.org/10.1103/PhysRevLett.128.183202

© 2022 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Zheng Shu1,*, Hongjing Liang2,*, Yichen Wang2, Shilin Hu3,†, Shi Chen4, Haifeng Xu2, Ri Ma2,‡, Dajun Ding2, and Jing Chen1,5,§

  • 1Institute of Applied Physics and Computational Mathematics, P.O. Box 8009, Beijing 100088, China
  • 2Institute of Atomic and Molecular Physics, Jilin University, Changchun 130012, China
  • 3Guangdong Provincial Key Laboratory of Quantum Metrology and Sensing School of Physics and Astronomy, Sun Yat-Sen University (Zhuhai Campus), Zhuhai 519082, China
  • 4Center for Applied Physics and Technology, HEDPS, and School of Physics, Peking University, Beijing 100871, China
  • 5Shenzhen Key Laboratory of Ultraintense Laser and Advanced Material Technology, Center for Advanced Material Diagnostic Technology, and College of Engineering Physics, Shenzhen Technology University, Shenzhen 518118, China

  • *These authors contributed equally to this work.
  • hushlin@mail.sysu.edu.cn
  • rma@jlu.edu.cn
  • §chen_jing@iapcm.ac.cn

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Issue

Vol. 128, Iss. 18 — 6 May 2022

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