期刊
NANOSCALE
卷 14, 期 7, 页码 2816-2825出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1nr04699c
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资金
- Consejo Nacional de Investigaciones Cientificas y Tecnicas (CONICET) [PIP 112-2017-0100892CO, PICT-2017-1605]
- Secretaria de Ciencia y Tecnologia de la Universidad Nacional de Cordoba (SECYT-UNC)
- European Union's Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant [895747]
- Marie Curie Actions (MSCA) [895747] Funding Source: Marie Curie Actions (MSCA)
The injection of plasmon-induced hot carriers in the Au-TiO2 system has been studied and it is found that pure electronic features contribute significantly to the stability of electron-hole separation, leading to photocatalytic dissociation.
The harnessing of plasmon-induced hot carriers promises to open new avenues for the development of clean energies and chemical catalysis. The extraction of carriers before thermalization and recombination is of fundamental importance to obtain appealing conversion yields. Here, hot carrier injection in the paradigmatic Au-TiO2 system is studied by means of electronic and electron-ion dynamics. Our results show that pure electronic features (without considering many-body interactions or dissipation to the environment) contribute to the electron-hole separation stability. These results reveal the existence of a dynamic contribution to the interfacial potential barrier (Schottky barrier) that arises at the charge injection pace, impeding electronic back transfer. Furthermore, we show that this charge separation stabilization provides the time needed for the charge to leak to capping molecules placed over the TiO2 surface triggering a coherent bond oscillation that will lead to a photocatalytic dissociation. We expect that our results will add new perspectives to the interpretation of the already detected long-lived hot carrier lifetimes and their catalytical effect, and concomitantly to their technological applications.
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