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Abstract
Plasmonic materials are promising photocatalysts as they are well suited to convert light into hot carriers and heat. Hot electron transfer is suggested as the driving force in many plasmon-driven reactions. However, to date, there are no direct molecular measures of the rate and yield of plasmon-To-molecule electron transfer or energy of these electrons on the timescale of plasmon decay. Here, we use ultrafast and spectroelectrochemical surface-enhanced Raman spectroscopy to quantify electron transfer from a plasmonic substrate to adsorbed methyl viologen molecules. We observe a reduction yield of 2.4 to 3.5% on the picosecond timescale, with plasmon-induced potentials ranging from 3.1 to 4.5 mV. Excitingly, some of these reduced species are stabilized and persist for tens of minutes. This work provides concrete metrics toward optimizing material molecule interactions for efficient plasmon-driven photocatalysis.
Original language | English (US) |
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Article number | e2305932120 |
Journal | Proceedings of the National Academy of Sciences of the United States of America |
Volume | 120 |
Issue number | 44 |
DOIs | |
State | Published - 2023 |
Bibliographical note
Publisher Copyright:© 2023 National Academy of Sciences. All rights reserved.
MRSEC Support
- Shared
PubMed: MeSH publication types
- Journal Article
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University of Minnesota Materials Research Science and Engineering Center (DMR-2011401)
Leighton, C. (PI) & Lodge, T. (CoI)
THE NATIONAL SCIENCE FOUNDATION
9/1/20 → 8/31/26
Project: Research project