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

Lixin He, Qingbin Zhang, Pengfei Lan (), Wei Cao, Xiaosong Zhu, Chunyang Zhai, Feng Wang, Wenjing Shi, Muzi Li, Xue-Bin Bian (), Peixiang Lu () and André D. Bandrauk
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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
Xue-Bin Bian: Chinese Academy of Sciences
Peixiang Lu: Huazhong University of Science and Technology
André D. Bandrauk: Université de Sherbrooke

Nature Communications, 2018, vol. 9, issue 1, 1-7

Abstract: 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.

Date: 2018
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DOI: 10.1038/s41467-018-03568-3

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