Femtosecond Extreme Ultraviolet Photoelectron Spectroscopy of Organic Molecules in Aqueous Solution
Femtosecond Extreme Ultraviolet Photoelectron Spectroscopy of Organic Molecules in Aqueous Solution
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DOI：
10.1021/acs.jpclett.8b02937
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发表时间：
2018-11-15
影响因子：
5.7
通讯作者：
Kornilov, Oleg
中科院分区：
文献类型：
--
作者：
Hummert, Johan;Reitsma, Geert;Kornilov, Oleg
时间分辨价光电子能谱是研究气相超快分子动力学的成熟工具。在这里，我们展示了有机分子稀水溶液的时间分辨 XUV 光电子能谱，为将该方法应用于自然环境中有机分子的光动力学研究铺平了道路，迄今为止，这些研究只有所有光学瞬态光谱才能实现。我们记录样品分子喹啉黄 WS 的静态和时间分辨光电子能谱，分析其电子结构，并跟踪 400 nm 脉冲激发时的弛豫动力学。动力学表现出三个时间尺度，其中 250 +/- 70 fs 时间尺度归因于溶剂重排。 1.3 +/- 0.4 和 90 +/- 20 ps 两个较长的时间尺度可以与最近提出的密切相关分子喹酞酮中的超快激发态分子内质子转移相关。
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.