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Orientation-dependent stereo Wigner time delay and electron localization in a small molecule
Science ( IF 44.7 ) Pub Date : 2018-06-21 , DOI: 10.1126/science.aao4731
J. Vos 1 , L. Cattaneo 1 , S. Patchkovskii 2 , T. Zimmermann 3, 4 , C. Cirelli 1, 5 , M. Lucchini 1 , A. Kheifets 6 , A. S. Landsman 3, 4 , U. Keller 1
Affiliation  

Time and place of electron exit Until about a decade ago, laser-induced ionization was considered instantaneous. Since then, applications of attosecond laser pulses have shown multiple subtle and complex factors that influence the precise timing of electron ejection from atoms and surfaces. Vos et al. measured the corresponding attosecond dynamics of dissociative photoionization in a diatomic molecule, carbon monoxide. By imaging the charged fragments, the timing could be correlated with the specific spatial portion of the molecule from which the electron wave packet emerged. Science, this issue p. 1326 The precise timing of ionization in CO varies with respect to the portion of the molecule from which the electron emerges. Attosecond metrology of atoms has accessed the time scale of the most fundamental processes in quantum mechanics. Transferring the time-resolved photoelectric effect from atoms to molecules considerably increases experimental and theoretical challenges. Here we show that orientation- and energy-resolved measurements characterize the molecular stereo Wigner time delay. This observable provides direct information on the localization of the excited electron wave packet within the molecular potential. Furthermore, we demonstrate that photoelectrons resulting from the dissociative ionization process of the CO molecule are preferentially emitted from the carbon end for dissociative 2Σ states and from the center and oxygen end for the 2Π states of the molecular ion. Supported by comprehensive theoretical calculations, this work constitutes a complete spatially and temporally resolved reconstruction of the molecular photoelectric effect.

中文翻译:

小分子中取向相关的立体维格纳时间延迟和电子定位

电子退出的时间和地点 大约十年前,激光诱导电离被认为是瞬时的。从那时起,阿秒激光脉冲的应用显示出多种微妙而复杂的因素影响电子从原子和表面喷射的精确时间。沃斯等人。测量了双原子分子一氧化碳中解离光电离的相应阿秒动力学。通过对带电碎片进行成像,时间可以与电子波包出现的分子的特定空间部分相关联。科学,这个问题 p。1326 CO 中电离的精确时间因电子出现的分子部分而异。原子的阿秒计量已经进入了量子力学中最基本过程的时间尺度。将时间分辨光电效应从原子转移到分子会大大增加实验和理论挑战。在这里,我们显示取向和能量分辨测量表征分子立体 Wigner 时间延迟。这个可观测的提供了关于分子势内受激电子波包的定位的直接信息。此外,我们证明了由 CO 分子的解离电离过程产生的光电子优先从分子离子的解离 2Σ 态的碳端和分子离子的 2Π 态的中心和氧端发射。在综合理论计算的支持下,这项工作构成了分子光电效应的完整时空分辨重建。
更新日期:2018-06-21
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