Mizuse Kenta, Kitano Kenta, Hasegawa Hirokazu, Ohshima Yasuhiro
Institute for Molecular Science, National Institutes of Natural Sciences and SOKENDAI (The Graduate University for Advanced Studies), Okazaki 444-8585, Japan.
Department of Physics and Mathematics, Aoyama Gakuin University, Sagamihara, Kanagawa 252-5258, Japan.
Sci Adv. 2015 Jul 3;1(6):e1400185. doi: 10.1126/sciadv.1400185. eCollection 2015 Jul.
A gas-phase molecular ensemble coherently excited to have an oriented rotational angular momentum has recently emerged as an appropriate microscopic system to illustrate quantum mechanical behavior directly linked to classical rotational motion, which has a definite direction. To realize an intuitive visualization of such a unidirectional molecular rotation, we report high-resolution direct imaging of direction-controlled rotational wave packets in nitrogen molecules. The rotational direction was regulated 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, time-dependent detailed nodal structures, 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.
最近，一种被相干激发以具有定向旋转角动量的气相分子系综，已成为一种合适的微观系统，可直接展示与具有确定方向的经典旋转运动直接相关的量子力学行为。为了实现这种单向分子旋转的直观可视化，我们报告了氮分子中方向控制旋转波包的高分辨率直接成像。旋转方向由一对延时、偏振倾斜的激光脉冲调节，从而给系统引入动态手性。随后通过新开发的库仑爆炸成像装置跟踪时空传播。从观察到的分子影像中，在系综保持单向旋转的同时，波包随时间变化的详细节点结构、瞬时排列、角色散和分数复兴都得到了充分表征。本方法为量子体系中的单向旋转提供了精确视图，利用其捕捉分子波包高度结构化时空演化的能力，将指导更复杂的分子操纵。
