Time-resolved valence photoelectron spectroscopy is an established tool for studies of ultrafast molecular dynamics in the gas phase. Here we demonstrate time-resolved XUV photoelectron spectroscopy from dilute aqueous solutions of organic molecules, paving the way to application of this method to photodynamics studies of organic molecules in natural environments, which so far have only been accessible to all-optical transient spectroscopies. We record static and time-resolved photoelectron spectra of a sample molecule, quinoline yellow WS, analyze its electronic structure, and follow the relaxation dynamics upon excitation with 400 nm pulses. The dynamics exhibit three time scales, of which a 250 ± 70 fs time scale is attributed to solvent rearrangement. The two longer time scales of 1.3 ± 0.4 and 90 ± 20 ps can be correlated to the recently proposed ultrafast excited-state intramolecular proton transfer in a closely related molecule, quinophthalone.

中文翻译：

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飞秒的水溶液中有机分子的极紫外光电子能谱

时间分辨价电子光谱学是研究气相超快分子动力学的成熟工具。在这里，我们演示了从稀有机分子水溶液中分离出的时间分辨XUV光电子能谱，为该方法在自然环境中有机分子的光动力学研究中的应用铺平了道路，到目前为止，全光瞬态光谱学只能使用该方法。我们记录样品分子喹啉黄WS的静态和时间分辨光电子光谱，分析其电子结构，并在用400 nm脉冲激发时跟踪弛豫动力学。动力学表现出三个时标，其中250±70 fs时标归因于溶剂重排。两个较长的时间刻度为1.3±0。