Femtosecond electron transfer dynamics across the \(D_{2}O/Cs^{+}/Cu(111)\) interface

  • Hydrogen bonding is essential in electron transfer processes at water-electrode interfaces. We study the impact of the H-bonding of water as a solvent molecule on real-time electron transfer dynamics across a Cs\(^{+}\)-Cu(111) ion-metal interface using femtosecond time-resolved two-photon photoelectron spectroscopy. We distinguish in the formed water-alkali aggregates two regimes below and above two water molecules per ion. Upon crossing the boundary of these regimes, the lifetime of the excess electron localized transiently at the Cs\(^{+}\) ion increases from 40 to 60 femtoseconds, which indicates a reduced alkali-metal interaction. Furthermore, the energy transferred to a dynamic structural rearrangement due to hydration is reduced from 0.3 to 0.2 eV concomitantly. These effects are a consequence of H-bonding in water-water interaction and the beginning formation of a nanoscale water network. This binding is supported by real-space imaging of the solvatomers and vibrational frequency shifts of the OH stretch and bending modes calculated for these specific interfaces.

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Metadaten
Author:John ThomasGND, Jayita PatwariGND, Inga Christina LangguthGND, Christopher PenschkeORCiDGND, Ping ZhouGND, Karina MorgensternORCiDGND, Uwe BovensiepenGND
URN:urn:nbn:de:hbz:294-108209
DOI:https://doi.org/10.13154/294-10820
Parent Title (English):Journal of physical chemistry / C
Subtitle (English):The impact of hydrogen bonding
Publisher:ACS Publications
Place of publication:Washington, DC
Document Type:Article
Language:English
Date of Publication (online):2024/02/22
Date of first Publication:2023/11/17
Publishing Institution:Ruhr-Universität Bochum, Universitätsbibliothek
Tag:EXC 2033 RESOLV (Ruhr Explores Solvation)
Volume:127
Issue:48
First Page:23467
Last Page:23474
Note:
J. Phys. Chem. C 2023, 127, 48, 23467–23474
Publication Date: November 17, 2023
https://doi.org/10.1021/acs.jpcc.3c06172
Copyright © 2023 The Authors.
Published by American Chemical Society.
This publication is licensed under
CC-BY-NC-ND 4.0.
Note:
Cluster of Excellence RESOLV – EXC 2033 (ID: 390677874)
www.solvation.de
Institutes/Facilities:Lehrstuhl für Physikalische Chemie I
Dewey Decimal Classification:Naturwissenschaften und Mathematik / Chemie, Kristallographie, Mineralogie
faculties:Fakultät für Chemie und Biochemie
Licence (English):License LogoCreative Commons - CC BY-NC-ND 4.0 - Attribution-NonCommercial-NoDerivatives 4.0 International

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