Probing the Birth and Ultrafast Dynamics of Hydrated Electrons at the Gold/Liquid Water Interface via an Optoelectronic Approach,Journal of the American Chemical Society

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Probing the Birth and Ultrafast Dynamics of Hydrated Electrons at the Gold/Liquid Water Interface via an Optoelectronic Approach
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-09-20 , DOI: 10.1021/jacs.0c08289
François Lapointe ₁ , Martin Wolf ₁ , R Kramer Campen _{1,

2} , Yujin Tong _{1,

2}

Affiliation

The hydrated electron has fundamental and practical significance in radiation and radical chemistry, catalysis, and radiobiology. While its bulk properties have been extensively studied, its behavior at solid/liquid interfaces is still unclear due to the lack of effective tools to characterize this short-lived species in between two condensed matter layers. In this study, we develop a novel optoelectronic technique for the characterization of the birth and structural evolution of solvated electrons at the metal/liquid interface with a femtosecond time resolution. Using this tool, we record for the first time the transient spectra (in a photon energy range from 0.31 to 1.85 eV) in situ with a time resolution of 50 fs revealing several novel aspects of their properties at the interface. Especially the transient species show state-dependent optical transition behaviors from being isotropic in the hot state to perpendicular to the surface in the trapped and solvated states. The technique will enable a better understanding of hot electron driven reactions at electrochemical interfaces.

中文翻译：

通过光电方法探测金/液水界面水合电子的诞生和超快动力学

水合电子在辐射和自由基化学、催化和放射生物学中具有基础和实际意义。虽然其整体特性已被广泛研究，但由于缺乏有效工具来表征两个凝聚态物质层之间的这种短寿命物种，其在固/液界面上的行为仍不清楚。在这项研究中，我们开发了一种新的光电技术，用于表征金属/液体界面处溶剂化电子的诞生和结构演化，具有飞秒时间分辨率。使用该工具，我们首次以 50 fs 的时间分辨率原位记录了瞬态光谱（光子能量范围从 0.31 到 1.85 eV），揭示了它们在界面上的几个新特性。特别是瞬态物质显示出状态相关的光学跃迁行为，从热态的各向同性到捕获态和溶剂化态下垂直于表面。该技术将有助于更好地了解电化学界面处的热电子驱动反应。

更新日期：2020-09-20

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