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Self-Constructed Multiple Plasmonic Hotspots on an Individual Fractal to Amplify Broadband Hot Electron Generation

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.
- Ca Foscari University of Venice Italy
- Dalian Polytechnic University China (People's Republic of)
- Central South University China (People's Republic of)
- University of Paris-Saclay France
- Imperial College London United Kingdom
Chemical Sciences not elsewhere classified, Physiology, F300, H600, Information Systems not elsewhere classified, broadband hot electron generation; dendritic fractal; electron energy loss spectroscopy; plasmon-assisted photocatalysis; plasmonic resonances, Marine Biology, Microbiology, 530, Mathematical Sciences not elsewhere classified, broadband hot electron generation, fractal, dendritic fractal, Genetics, electron generation, Nanoscience & Nanotechnology, Molecular Biology, plasmonic, Pharmacology, Evolutionary Biology, electron energy loss spectroscopy, Ecology, ab initio simulation, 541, Amplify Broadband Hot Electron Gene., 620, resonance, plasmonic resonances, broadband, hotspot, plasmon-assisted photocatalysis, Self-Constructed Multiple Plasmonic., Physical Sciences not elsewhere classified, Biotechnology, Biological Sciences not elsewhere classified
Chemical Sciences not elsewhere classified, Physiology, F300, H600, Information Systems not elsewhere classified, broadband hot electron generation; dendritic fractal; electron energy loss spectroscopy; plasmon-assisted photocatalysis; plasmonic resonances, Marine Biology, Microbiology, 530, Mathematical Sciences not elsewhere classified, broadband hot electron generation, fractal, dendritic fractal, Genetics, electron generation, Nanoscience & Nanotechnology, Molecular Biology, plasmonic, Pharmacology, Evolutionary Biology, electron energy loss spectroscopy, Ecology, ab initio simulation, 541, Amplify Broadband Hot Electron Gene., 620, resonance, plasmonic resonances, broadband, hotspot, plasmon-assisted photocatalysis, Self-Constructed Multiple Plasmonic., Physical Sciences not elsewhere classified, Biotechnology, Biological Sciences not elsewhere classified
citations This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).43 popularity This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.Top 1% influence This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).Top 10% impulse This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.Top 1%
