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Filming movies of attosecond charge migration in single molecules with high harmonic spectroscopy

Author

Listed:
  • Lixin He

    (Huazhong University of Science and Technology
    Optical Valley Laboratory)

  • Siqi Sun

    (Huazhong University of Science and Technology)

  • Pengfei Lan

    (Huazhong University of Science and Technology
    Optical Valley Laboratory)

  • Yanqing He

    (Huazhong University of Science and Technology)

  • Bincheng Wang

    (Huazhong University of Science and Technology)

  • Pu Wang

    (Huazhong University of Science and Technology)

  • Xiaosong Zhu

    (Huazhong University of Science and Technology
    Optical Valley Laboratory)

  • Liang Li

    (Huazhong University of Science and Technology
    Optical Valley Laboratory)

  • Wei Cao

    (Huazhong University of Science and Technology
    Optical Valley Laboratory)

  • Peixiang Lu

    (Huazhong University of Science and Technology
    Optical Valley Laboratory
    CAS Center for Excellence in Ultra-intense Laser Science)

  • C. D. Lin

    (Kansas State University)

Abstract

Electron migration in molecules is the progenitor of chemical reactions and biological functions after light-matter interaction. Following this ultrafast dynamics, however, has been an enduring endeavor. Here we demonstrate that, by using machine learning algorithm to analyze high-order harmonics generated by two-color laser pulses, we are able to retrieve the complex amplitudes and phases of harmonics of single fixed-in-space molecules. These complex dipoles enable us to construct movies of laser-driven electron migration after tunnel ionization of N2 and CO2 molecules at time steps of 50 attoseconds. Moreover, the angular dependence of the migration dynamics is fully resolved. By examining the movies, we observe that electron holes do not just migrate along the laser polarization direction, but may swirl around the atom centers. Our result establishes a general scheme for studying ultrafast electron dynamics in molecules, paving a way for further advance in tracing and controlling photochemical reactions by femtosecond lasers.

Suggested Citation

  • Lixin He & Siqi Sun & Pengfei Lan & Yanqing He & Bincheng Wang & Pu Wang & Xiaosong Zhu & Liang Li & Wei Cao & Peixiang Lu & C. D. Lin, 2022. "Filming movies of attosecond charge migration in single molecules with high harmonic spectroscopy," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-32313-0
    DOI: 10.1038/s41467-022-32313-0
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