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Self-Constructed Multiple Plasmonic Hotspots on an Individual Fractal to Amplify Broadband Hot Electron Generation
School of Materials Science and Engineering, Tianjin University, Tianjin 300350, P.R. China; Key Laboratory of Efficient Utilization of Low and Medium Grade Energy, Ministry of Education, Tianjin University, Tianjin 300350, P.R. China.
Hybrid Nanosystems, Nanoinstitute Munich, Faculty of Physics, Ludwig-Maximilians-Universität München, D-80539 München, Germany.
School of Materials Science and Engineering, Tianjin University, Tianjin 300350, P.R. China.
School of Materials Science and Engineering, Tianjin University, Tianjin 300350, P.R. China.
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2021 (English)In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 15, no 6, p. 10553-10564Article in journal (Refereed) Published
Abstract [en]

Plasmonic nanoparticles are ideal candidates for hot-electron-assisted applications, but their narrow resonance region and limited hotspot number hindered the energy utilization of broadband solar energy. Inspired by tree branches, we designed and chemically synthesized silver fractals, which enable self-constructed hotspots and multiple plasmonic resonances, extending the broadband generation of hot electrons for better matching with the solar radiation spectrum. We directly revealed the plasmonic origin, the spatial distribution, and the decay dynamics of hot electrons on the single-particle level by using ab initio simulation, dark-field spectroscopy, pump–probe measurements, and electron energy loss spectroscopy. Our results show that fractals with acute tips and narrow gaps can support broadband resonances (400–1100 nm) and a large number of randomly distributed hotspots, which can provide unpolarized enhanced near field and promote hot electron generation. As a proof-of-concept, hot-electron-triggered dimerization of p-nitropthiophenol and hydrogen production are investigated under various irradiations, and the promoted hot electron generation on fractals was confirmed with significantly improved efficiency.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2021. Vol. 15, no 6, p. 10553-10564
Keywords [en]
dendritic fractal, broadband hot electron generation, plasmonic resonances, electron energy loss spectroscopy, plasmon-assisted photocatalysis
National Category
Condensed Matter Physics
Research subject
Experimental Physics
Identifiers
URN: urn:nbn:se:ltu:diva-85497DOI: 10.1021/acsnano.1c03218ISI: 000665748900121PubMedID: 34114794Scopus ID: 2-s2.0-85108891316OAI: oai:DiVA.org:ltu-85497DiVA, id: diva2:1567195
Note

Validerad;2021;Nivå 2;2021-07-14 (johcin);

Finansiär: National Natural Science Foundation of China (51771132); Alexander von Humboldt Foundation; Deutsche Forschungsgemeinschaft Centre of Excellence (EXC 2089/1 -390776260); Bavaria SolTech program; Lee−Lucas Chair in Physics; EPSRC Reactive Plasmonics Programme (EP/M013812/1); European Commission through the ERC Starting Grant CATALIGHT (802989)

Available from: 2021-06-16 Created: 2021-06-16 Last updated: 2021-12-13Bibliographically approved

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Vomiero, Alberto

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