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Nat Commun. 2018 Mar 16;9(1):1108. doi: 10.1038/s41467-018-03568-3.

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

Author information

1
Wuhan National Laboratory for Optoelectronics and School of Physics, Huazhong University of Science and Technology, 430074, Wuhan, China.
2
Wuhan National Laboratory for Optoelectronics and School of Physics, Huazhong University of Science and Technology, 430074, Wuhan, China. pengfeilan@hust.edu.cn.
3
State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, 430071, Wuhan, China.
4
University of Chinese Academy of Sciences, 100049, Beijing, China.
5
State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, 430071, Wuhan, China. xuebin.bian@wipm.ac.cn.
6
Wuhan National Laboratory for Optoelectronics and School of Physics, Huazhong University of Science and Technology, 430074, Wuhan, China. lupeixiang@hust.edu.cn.
7
Laboratory of Optical Information Technology, Wuhan Institute of Technology, 430205, Wuhan, China. lupeixiang@hust.edu.cn.
8
Laboratoire de chimie théorique, Département de Chimie, Université de Sherbrooke, Sherbrooke, J1K 2R1, Quebéc, Canada.

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.

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