Bypassing Thermalization Losses through Ultrafast Interfacial Charge Transfer in Plasmonic Nanocavities for Water Oxidation.
- 1Institute for Solar Fuels, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Berlin14109, Germany.
- 2State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian116023, China.
- 3Institut für Chemie, Technische Universität Berlin, Berlin10623, Germany.
Abstract
Spatially inhomogeneous plasmonic heterostructures concentrate light into nanoscale volumes and offer powerful routes for plasmon-mediated solar energy conversion. However, how hot carriers evolve and lose energy under such extreme nanophotonic confinement, particularly during interfacial transfer, remains largely unexplored. Here, we demonstrate that rationally engineered plasmonic nanocavities with intense nanoscopic field localization provide a unique platform to bypass these energy-loss channels by enabling nonthermal charge injection on a sub-40 fs time scale. Using polarization-resolved and time-resolved multiphoton photoemission spectroscopy, we reveal that the intense localized fields arising from plasmon-cavity mode coupling establish an accelerated and direct electron transfer channel across the interface. This behavior is accompanied by a distinctive inversion of the polarization dependence and by photon-energy-independent spectral features, confirming charge injection occurring prior to thermalization. Furthermore, the emergence of three-photon photoemission indicates a fundamental reconfiguration of the hot carrier generation and relaxation landscape resulting from the nanoscopic electric field within the plasmonic nanocavity. These insights establish a microscopic understanding of how interfacial charge transfer contributes to the enhanced water-oxidation activity in plasmonic nanocavity systems, offering a guiding framework for the development of advanced plasmonic photocatalysts and optoelectronic interfaces.
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BibTeX
@article{gao2026bypassing,
title = {{Bypassing Thermalization Losses through Ultrafast Interfacial Charge Transfer in Plasmonic Nanocavities for Water Oxidation.}},
author = {Yuying Gao and Christian Höhn and Jiajun Wang and Markus Wollgarten and Holger Kropf and Fengtao Fan and Can Li and Roel van de Krol and Dennis Friedrich},
journal = {Journal of the American Chemical Society},
year = {2026},
month = sep,
doi = {10.1021/jacs.6c09174},
url = {https://europepmc.org/article/MED/42915560},
note = {CC BY},
}
RIS
TY - JOUR
TI - Bypassing Thermalization Losses through Ultrafast Interfacial Charge Transfer in Plasmonic Nanocavities for Water Oxidation.
AU - Yuying Gao
AU - Christian Höhn
AU - Jiajun Wang
AU - Markus Wollgarten
AU - Holger Kropf
AU - Fengtao Fan
AU - Can Li
AU - Roel van de Krol
AU - Dennis Friedrich
PY - 2026
DA - 2026/09/01
JO - Journal of the American Chemical Society
DO - 10.1021/jacs.6c09174
UR - https://europepmc.org/article/MED/42915560
AB - Spatially inhomogeneous plasmonic heterostructures concentrate light into nanoscale volumes and offer powerful routes for plasmon-mediated solar energy conversion. However, how hot carriers evolve and lose energy under such extreme nanophotonic confinement, particularly during interfacial transfer, remains largely unexplored. Here, we demonstrate that rationally engineered plasmonic nanocavities with intense nanoscopic field localization provide a unique platform to bypass these energy-loss channels by enabling nonthermal charge injection on a sub-40 fs time scale. Using polarization-resolved and time-resolved multiphoton photoemission spectroscopy, we reveal that the intense localized fields arising from plasmon-cavity mode coupling establish an accelerated and direct electron transfer channel across the interface. This behavior is accompanied by a distinctive inversion of the polarization dependence and by photon-energy-independent spectral features, confirming charge injection occurring prior to thermalization. Furthermore, the emergence of three-photon photoemission indicates a fundamental reconfiguration of the hot carrier generation and relaxation landscape resulting from the nanoscopic electric field within the plasmonic nanocavity. These insights establish a microscopic understanding of how interfacial charge transfer contributes to the enhanced water-oxidation activity in plasmonic nanocavity systems, offering a guiding framework for the development of advanced plasmonic photocatalysts and optoelectronic interfaces.
SN - 0002-7863
SN - 1520-5126
ER -