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.
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