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Spectroscopy and dynamics of the hydrated electron at the water/air interface

Jordan, Caleb J. C.; Coons, Marc P.; Herbert, John M.; Verlet, Jan R. R.

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Authors

Caleb Jordan caleb.j.jordan@durham.ac.uk
PGR Student Doctor of Philosophy

Marc P. Coons

John M. Herbert



Abstract

The hydrated electron, e–(aq), has attracted much attention as a central species in radiation chemistry. However, much less is known about e–(aq) at the water/air surface, despite its fundamental role in electron transfer processes at interfaces. Using time-resolved electronic sum-frequency generation spectroscopy, the electronic spectrum of e–(aq) at the water/air interface and its dynamics are measured here, following photo-oxidation of the phenoxide anion. The spectral maximum agrees with that for bulk e–(aq) and shows that the orbital density resides predominantly within the aqueous phase, in agreement with supporting calculations. In contrast, the chemistry of the interfacial hydrated electron differs from that in bulk water, with e–(aq) diffusing into the bulk and leaving the phenoxyl radical at the surface. Our work resolves long-standing questions about e–(aq) at the water/air interface and highlights its potential role in chemistry at the ubiquitous aqueous interface.

Citation

Jordan, C. J. C., Coons, M. P., Herbert, J. M., & Verlet, J. R. R. (2024). Spectroscopy and dynamics of the hydrated electron at the water/air interface. Nature Communications, 15(1), Article 182. https://doi.org/10.1038/s41467-023-44441-2

Journal Article Type Article
Acceptance Date Dec 13, 2023
Online Publication Date Jan 2, 2024
Publication Date Jan 2, 2024
Deposit Date Jan 16, 2024
Publicly Available Date Jan 16, 2024
Journal Nature Communications
Electronic ISSN 2041-1723
Publisher Nature Research
Peer Reviewed Peer Reviewed
Volume 15
Issue 1
Article Number 182
DOI https://doi.org/10.1038/s41467-023-44441-2
Public URL https://durham-repository.worktribe.com/output/2085044
Additional Information Author Correction: Spectroscopy and dynamics of the hydrated electron at the water/air interface: https://doi.org/10.1038/s41467-024-44816-z