Journal Article Quantum unidirectional rotation directly imaged with molecules

水瀬, 賢太  ,  Mizuse, Kenta  ,  大島, 康裕  ,  Ohshima, Yasuhiro  ,  Hasegawa, Hirokazu

Many interesting quantum aspects in molecular rotation have been unveiled by extensive real-time measurements, but rotational wave packets so far studied have no net oriented angular momentum, and they cannot be linked to any classical rotational motion having a definite sense of rotation. Here we report high-resolution direct imaging of ultrafast unidirectional molecular rotation. The direction-controlled rotational wave packet was induced by a pair of time-delayed, polarization-skewed laser pulses, introducing the dynamic chirality to the system. The subsequent spatiotemporal propagation was tracked by a newly developed Coulomb explosion imaging setup. From the observed molecular movie, instantaneous alignment, angular dispersion, and fractional revivals of the wave packet are fully characterized while the ensemble keeps rotating in one direction. The present approach, providing an accurate view on unidirectional rotation in quantum regime, will guide more sophisticated molecular manipulations, by utilizing its capability in capturing highly structured spatiotemporal evolution of molecular wave packets.

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