Real-Time Observation of Molecular Spinning with Angular High-Harmonic Spectroscopy
Abstract
We demonstrate an angular high-harmonic spectroscopy method to probe the spinning dynamics of a molecular rotation wave packet in real time. With the excitation of two time-delayed, polarization-skewed pump pulses, the molecular ensemble is impulsively kicked to rotate unidirectionally, which is subsequently irradiated by another delayed probe pulse for high-order harmonic generation (HHG). The spatiotemporal evolution of the molecular rotation wave packet is visualized from the time-dependent angular distributions of the HHG yields and frequency shift measured at various polarization directions and time delays of the probe pulse. Here, the observed frequency shift in HHG is demonstrated to arise from the nonadiabatic effect induced by molecular spinning. Different from the previous spectroscopic and Coulomb explosion imaging techniques, the angular high-harmonic spectroscopy method can reveal additionally the electronic structure and multiple orbitals of the sampled molecule. All the experimental findings are well reproduced by numerical simulations. Further extension of this method would provide a powerful tool for probing complex polyatomic molecules with HHG spectroscopy.
- Authors:
-
- Huazhong University of Science and Technology, Wuhan (China)
- Kansas State Univ., Manhattan, KS (United States)
- Huazhong University of Science and Technology, Wuhan (China); Wuhan Institute of Technology (China)
- Publication Date:
- Research Org.:
- Kansas State Univ., Manhattan, KS (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 1610049
- Alternate Identifier(s):
- OSTI ID: 1478569
- Grant/Contract Number:
- FG02-86ER13491; 11627809; 11874165; 11704137; 11774109
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Letters
- Additional Journal Information:
- Journal Volume: 121; Journal Issue: 16; Journal ID: ISSN 0031-9007
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; physics; atomic & molecular processes in external fields
Citation Formats
He, Lixin, Lan, Pengfei, Le, Anh-Thu, Wang, Baoning, Wang, Bincheng, Zhu, Xiaosong, Lu, Peixiang, and Lin, C. D. Real-Time Observation of Molecular Spinning with Angular High-Harmonic Spectroscopy. United States: N. p., 2018.
Web. doi:10.1103/physrevlett.121.163201.
He, Lixin, Lan, Pengfei, Le, Anh-Thu, Wang, Baoning, Wang, Bincheng, Zhu, Xiaosong, Lu, Peixiang, & Lin, C. D. Real-Time Observation of Molecular Spinning with Angular High-Harmonic Spectroscopy. United States. https://doi.org/10.1103/physrevlett.121.163201
He, Lixin, Lan, Pengfei, Le, Anh-Thu, Wang, Baoning, Wang, Bincheng, Zhu, Xiaosong, Lu, Peixiang, and Lin, C. D. Mon .
"Real-Time Observation of Molecular Spinning with Angular High-Harmonic Spectroscopy". United States. https://doi.org/10.1103/physrevlett.121.163201. https://www.osti.gov/servlets/purl/1610049.
@article{osti_1610049,
title = {Real-Time Observation of Molecular Spinning with Angular High-Harmonic Spectroscopy},
author = {He, Lixin and Lan, Pengfei and Le, Anh-Thu and Wang, Baoning and Wang, Bincheng and Zhu, Xiaosong and Lu, Peixiang and Lin, C. D.},
abstractNote = {We demonstrate an angular high-harmonic spectroscopy method to probe the spinning dynamics of a molecular rotation wave packet in real time. With the excitation of two time-delayed, polarization-skewed pump pulses, the molecular ensemble is impulsively kicked to rotate unidirectionally, which is subsequently irradiated by another delayed probe pulse for high-order harmonic generation (HHG). The spatiotemporal evolution of the molecular rotation wave packet is visualized from the time-dependent angular distributions of the HHG yields and frequency shift measured at various polarization directions and time delays of the probe pulse. Here, the observed frequency shift in HHG is demonstrated to arise from the nonadiabatic effect induced by molecular spinning. Different from the previous spectroscopic and Coulomb explosion imaging techniques, the angular high-harmonic spectroscopy method can reveal additionally the electronic structure and multiple orbitals of the sampled molecule. All the experimental findings are well reproduced by numerical simulations. Further extension of this method would provide a powerful tool for probing complex polyatomic molecules with HHG spectroscopy.},
doi = {10.1103/physrevlett.121.163201},
journal = {Physical Review Letters},
number = 16,
volume = 121,
place = {United States},
year = {Mon Oct 15 00:00:00 EDT 2018},
month = {Mon Oct 15 00:00:00 EDT 2018}
}
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Figures / Tables:
FIG. 1: (a) Angular distribution of H21 from N2 as a function of the time delay of the probe pulse measured with the molecules excited by only the pump pulse P1 (the case of alignment). (b) Same as (a), but for the molecules excited by both pump pulses, P1 andmore »
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