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(2020)

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摘要
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 1.8S 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.
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关键词
hydrated electrons,ultrafast dynamics,gold/liquid water interface,water interface
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