Quantum unidirectional rotation directly imaged with molecules.

Quantum unidirectional rotation directly imaged with molecules.
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DOI:
10.1126/sciadv.1400185
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发表时间:
2015-07
期刊:
影响因子:
13.6
通讯作者:
Ohshima Y
Ohshima Y
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Mizuse K;Kitano K;Hasegawa H;Ohshima Y

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高分辨率成像充分表征了方向控制分子旋转动力学的量子力学特征。最近出现了一种相干激发的具有定向旋转角动量的气相分子系综,作为一种合适的微观系统,可以说明与具有明确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、偏斜的激光脉冲调节,从而将动态手性引入系统。随后的时空传播由新开发的库仑爆炸成像装置跟踪。从观察到的分子电影中,当整体保持沿一个方向旋转时,波包的时间依赖性详细节点结构、瞬时对准、角色散和波包复兴分数得到了充分表征。目前的方法提供了量子体系中单向旋转的准确视图,将利用其捕获分子波包的高度结构化时空演化的能力来指导更复杂的分子操作。
High resolution imaging fully characterizes quantum-mechanical signatures of direction-controlled molecular rotational dynamics. 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.