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Monitoring ultrafast vibrational dynamics of isotopic molecules with frequency modulation of high-order harmonics

Author

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  • Lixin He

    (Huazhong University of Science and Technology)

  • Qingbin Zhang

    (Huazhong University of Science and Technology)

  • Pengfei Lan

    (Huazhong University of Science and Technology)

  • Wei Cao

    (Huazhong University of Science and Technology)

  • Xiaosong Zhu

    (Huazhong University of Science and Technology)

  • Chunyang Zhai

    (Huazhong University of Science and Technology)

  • Feng Wang

    (Huazhong University of Science and Technology)

  • Wenjing Shi

    (Huazhong University of Science and Technology)

  • Muzi Li

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Xue-Bin Bian

    (Chinese Academy of Sciences)

  • Peixiang Lu

    (Huazhong University of Science and Technology
    Wuhan Institute of Technology)

  • André D. Bandrauk

    (Université de Sherbrooke)

Abstract

Molecules constituted by different isotopes are different in vibrational modes, making it possible to elucidate the mechanism of a chemical reaction via the kinetic isotope effect. However, the real-time observation of the vibrational motion of isotopic nuclei in molecules is still challenging due to its ultrashort time scale. Here we demonstrate a method to monitor the nuclear vibration of isotopic molecules with the frequency modulation of high-order harmonic generation (HHG) during the laser-molecule interaction. In the proof-of-principle experiment, we report a red shift in HHG from H2 and D2. The red shift is ascribed to dominant HHG from the stretched isotopic molecules at the trailing edge of the laser pulse. By utilizing the observed frequency shift, the laser-driven nuclear vibrations of H2 and D2 are retrieved. These findings pave an accessible route toward monitoring the ultrafast nuclear dynamics and even tracing a chemical reaction in real time.

Suggested Citation

  • Lixin He & Qingbin Zhang & Pengfei Lan & Wei Cao & Xiaosong Zhu & Chunyang Zhai & Feng Wang & Wenjing Shi & Muzi Li & Xue-Bin Bian & Peixiang Lu & André D. Bandrauk, 2018. "Monitoring ultrafast vibrational dynamics of isotopic molecules with frequency modulation of high-order harmonics," Nature Communications, Nature, vol. 9(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-03568-3
    DOI: 10.1038/s41467-018-03568-3
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