Real-Time Observation of Molecular Spinning with Angular High-Harmonic Spectroscopy

He, Lixin; Lan, Pengfei; Le, Anh-Thu; Wang, Baoning; Wang, Bincheng; Zhu, Xiaosong; Lu, Peixiang; Lin, C.  D.

doi:10.1103/physrevlett.121.163201

Real-Time Observation of Molecular Spinning with Angular High-Harmonic Spectroscopy

Journal Article · Mon Oct 15 00:00:00 EDT 2018 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.121.163201· OSTI ID:1610049

He, Lixin ^[1]; Lan, Pengfei ^[2]; Le, Anh-Thu ^[3]; Wang, Baoning ^[2]; Wang, Bincheng ^[2]; Zhu, Xiaosong ^[2]; Lu, Peixiang ^[4]; Lin, C. D. ^[3]

Huazhong University of Science and Technology, Wuhan (China); DOE/OSTI
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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Kansas State Univ., Manhattan, KS (United States)

Sponsoring Organization:: USDOE Office of Science (SC); National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: FG02-86ER13491

OSTI ID:: 1610049

Alternate ID(s):: OSTI ID: 1478569

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 16 Vol. 121; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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