用时间和角度分辨光电子能谱学成像电子动力学
Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy
摘要：
我们从理论上研究如何时间和角度分辨的光电子能谱可以应用于成像相干电子动力学分子。我们考虑一个过程，其中泵脉冲触发相干电子动力学的分子通过创建一个价电子空穴。超短极紫外（XUV）探测脉冲在分子中产生第二个电子空穴。有关电子动力学的信息是通过分析在一个固定的光电子能量的光电子发射概率的角分布。我们证明，严格的理论分析，考虑到由超短，宽带探测脉冲和电子-空穴相关效应引起的跃迁的不可逆性，是必要的时间和角度分辨光电子谱的解释。我们展示了如何从一个分子的时间和角度分辨的光电子光谱的傅立叶分析可以应用到以下的电子动力学考虑光电子分布从吲哚分子阳离子与相干电子动力学。
英文摘要：
We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a molecule by creating a valence electron hole. An ultrashort extreme ultraviolet (XUV) probe pulse creates a second electron hole in the molecule. Information about the electron dynamics is accessed by analyzing angular distributions of photoemission probabilities at a fixed photoelectron energy. We demonstrate that a rigorous theoretical analysis, which takes into account the indistinguishability of transitions induced by the ultrashort, broadband probe pulse and electron hole correlation effects, is necessary for the interpretation of time- and angle-resolved photoelectron spectra. We show how a Fourier analysis of time- and angle-resolved photoelectron spectra from a molecule can be applied to follow its electron dynamics by considering photoelectron distributions from an indole molecular cation with coherent electron dynamics.
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