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通过自参考分子阿秒光钟探测共振光电离时间延迟

Probing Resonant Photoionization Time Delay by Self-Referenced Molecular Attoclock.

作者信息

Tong Jihong, Liu Xiwang, Dong Wenhui, Jiang Wenyu, Zhu Ming, Xu Yidan, Zuo Zitan, Lu Peifen, Gong Xiaochun, Song Xiaohong, Yang Weifeng, Wu Jian

机构信息

State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai 200241, China.

School of Science and Center for Theoretical Physics, Hainan University, Haikou 570288, China.

出版信息

Phys Rev Lett. 2022 Oct 21;129(17):173201. doi: 10.1103/PhysRevLett.129.173201.

DOI:10.1103/PhysRevLett.129.173201
PMID:36332237
Abstract

Attosecond time-resolved electron tunneling dynamics have been investigated by using attosecond angular streaking spectroscopy, where a clock reference to the laser field vector is required in atomic strong-field ionization and the situation becomes complicated in molecules. Here we reveal a resonant ionization process via a transient state by developing an electron-tunneling-site-resolved molecular attoclock in Ar-Kr^{+}. Two distinct deflection angles are observed in the photoelectron angular distribution in the molecular frame, corresponding to the direct and resonant ionization pathways. We find the electron is temporally trapped in the Coulomb potential wells of the Ar-Kr^{+} before finally releasing into the continuum when the electron tunnels through the internal barrier. By utilizing the direct tunneling ionization as a self-referenced arm of the attoclock, the time delay of the electron trapped in the resonant state is revealed to be 3.50±0.04  fs. Our results give an impetus to exploring the ultrafast electron dynamics in complex systems and also endow a semiclassical presentation of the electron trapping dynamics in a quantum resonant state.

摘要

通过阿秒角条纹光谱法研究了阿秒时间分辨电子隧穿动力学,在原子强场电离中需要一个相对于激光场矢量的时钟参考,而在分子中情况变得复杂。在此,我们通过在Ar-Kr⁺中开发一种电子隧穿位点分辨的分子阿秒时钟,揭示了一种通过瞬态的共振电离过程。在分子坐标系中的光电子角分布中观察到两个不同的偏转角,分别对应直接电离和共振电离路径。我们发现,当电子隧穿通过内部势垒时,它会暂时被困在Ar-Kr⁺的库仑势阱中,最终释放到连续态中。通过将直接隧穿电离用作阿秒时钟的自参考臂,发现被困在共振态的电子的时间延迟为3.50±0.04 fs。我们的结果为探索复杂系统中的超快电子动力学提供了动力,也为量子共振态中的电子俘获动力学提供了半经典描述。

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Femtosecond Time- and Spectrally Resolved Ion Photofragmentation Spectroscopy: Case Studies of Two Alkylbenzene Cations.飞秒时间分辨与光谱分辨离子光解离光谱:两种烷基苯阳离子的案例研究
J Phys Chem A. 2025 Jul 31;129(30):6845-6865. doi: 10.1021/acs.jpca.5c04149. Epub 2025 Jul 21.
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Coulomb focusing in attosecond angular streaking.阿秒角条纹中的库仑聚焦
Light Sci Appl. 2024 Sep 11;13(1):250. doi: 10.1038/s41377-024-01600-4.
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Tunnelling of electrons via the neighboring atom.电子通过相邻原子的隧穿。
Light Sci Appl. 2024 Jan 16;13(1):18. doi: 10.1038/s41377-023-01373-2.