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Echo in a single vibrationally excited molecule
Nature Physics ( IF 19.6 ) Pub Date : 2020-01-20 , DOI: 10.1038/s41567-019-0762-7
Junjie Qiang , Ilia Tutunnikov , Peifen Lu , Kang Lin , Wenbin Zhang , Fenghao Sun , Yaron Silberberg , Yehiam Prior , Ilya Sh. Averbukh , Jian Wu

Echoes occur in many physical systems, typically in inhomogeneously broadened ensembles of nonlinear objects. They are often used to eliminate the effects of dephasing caused by interactions with the environment as well as to enable the observation of proper, inherent object properties. Here, we report the experimental observation of quantum wave-packet echoes in a single, isolated molecule. The entire dephasing–rephasing cycle occurs without any inhomogeneous spread of molecular properties, or any interaction with the environment, and offers a way to probe the internal coherent dynamics of single molecules. In our experiments, we impulsively excite a vibrational wave packet in an anharmonic molecular potential and observe its oscillations and eventual dispersion with time. A second, delayed pulse gives rise to an echo—a partial recovery of the initial coherent oscillations. The vibrational dynamics of single molecules is visualized by a time-delayed probe pulse dissociating them, one at a time. Two mechanisms for the echo formation are discussed: a.c. Stark-induced molecular potential shaking and creation of a depletion-induced ‘hole’ in the nuclear spatial distribution. The single-molecule wave-packet echoes may lead to the development of new tools for probing ultrafast intramolecular processes in various molecules.



中文翻译:

单个振动激发分子中的回声

回声出现在许多物理系统中,通常出现在非线性对象的非均匀展宽集合中。它们通常用于消除由与环境相互作用引起的相位差影响,以及能够观察适当的、固有的对象属性。在这里,我们报告了对单个孤立分子中量子波包回波的实验观察。整个去相位-重新相位循环的发生没有任何分子特性的不均匀扩散,或与环境的任何相互作用,并提供了一种探索单个分子内部相干动力学的方法。在我们的实验中,我们在非谐分子势中冲动地激发振动波包,并观察它的振荡和最终随时间的色散。一秒,延迟脉冲产生回波——初始相干振荡的部分恢复。单个分子的振动动力学通过一个时间延迟的探针脉冲来可视化,一次一个地解离它们。讨论了回声形成的两种机制:ac Stark 引起的分子势振动和在核空间分布中产生耗尽引起的“空洞”。单分子波包回波可能会导致开发用于探测各种分子中超快分子内过程的新工具。斯塔克诱导的分子势振动和在核空间分布中产生耗尽诱导的“空洞”。单分子波包回波可能会导致开发用于探测各种分子中超快分子内过程的新工具。斯塔克诱导的分子势振动和在核空间分布中产生耗尽诱导的“空洞”。单分子波包回波可能会导致开发用于探测各种分子中超快分子内过程的新工具。

更新日期:2020-01-20
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