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Real-Time Observation Of Molecular Spinning With Angular High-Harmonic Spectroscopy, Lixin He, Pengfei Lan, Anh-Thu Le, Baoning Wang, Bincheng Wang, Xiaosong Zhu, Peixiang Lu, C. D. Lin

Physics Faculty Research & Creative Works

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. The observed frequency shift in HHG is demonstrated to arise from the …