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Probing the Birth and Ultrafast Dynamics of Hydrated Electrons at the Gold/Liquid Water Interface via an Optoelectronic Approach

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Lapointe,  Francois
Physical Chemistry, Fritz Haber Institute, Max Planck Society;
National Research Council Canada;

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Wolf,  Martin
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Campen,  R. Kramer
Physical Chemistry, Fritz Haber Institute, Max Planck Society;
Faculty of Physics, University of Duisburg-Essen;

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Tong,  Yujin
Physical Chemistry, Fritz Haber Institute, Max Planck Society;
Faculty of Physics, University of Duisburg-Essen;

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Citation

Lapointe, F., Wolf, M., Campen, R. K., & Tong, Y. (2020). 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, 142(43), 18619-18627. doi:10.1021/jacs.0c08289.


Cite as: http://hdl.handle.net/21.11116/0000-0005-A1F9-C
Abstract
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 buried 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. We thus recorded for the first time their transient spectra (in a photon energy range from 0.31 to 1.85 eV) in situ with a time resolution of 50 fs. 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.