水溶液中电子转移介导衰变的首次观测：一种新的离子对探针
First Observation of Electron Transfer Mediated Decay in Aqueous Solutions: A Novel Probe of Ion Pairing
摘要：
许多光谱技术的一个主要目标是提供当地化学环境的综合信息。电子转移介导衰变（ETMD）是一种敏感的环境探针，因为它通过电子和能量转移步骤积极参与这种非局部无辐射衰变过程。我们报告的第一个实验观察ETMD在液相中。利用液体射流X射线光电子能谱学，我们探讨了氯化锂水溶液，并检测到低能量电子明确出现的ETMD过程中的核心电离的锂+。我们用分子动力学和高级从头计算解释了实验结果。通过考虑各种溶剂化结构模型，我们表明，水分子和Cl-阴离子都可以参与ETMD，每个过程都有其特征光谱指纹。不同的离子缔合导致不同的光谱形状。ETMD光谱的独特的灵敏度的潜在应用的本地水化结构和离子配对进行了讨论。
英文摘要：
A major goal of many spectroscopic techniques is to provide comprehensive information on the local chemical environment. Electron transfer mediated decay (ETMD) is a sensitive probe of the environment since it is actively involved in this non-local radiationless decay process through electron and energy transfer steps. We report the first experimental observation of ETMD in the liquid phase. Using liquid-jet X-ray photoelectron spectroscopy we explore LiCl aqueous solution, and detect low-energy electrons unambiguously emerging from the ETMD processes of core-ionized Li+. We interpret the experimental results with molecular dynamics and high-level ab initio calculations. By considering various solvation-structure models we show that both water molecules and Cl- anions can participate in ETMD, with each process having its characteristic spectral fingerprint. Different ion associations lead to different spectral shapes. The potential application of the unique sensitivity of the ETMD spectroscopy to the local hydration structure and ion pairing is discussed.
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