TY - JOUR
T1 - Self-Constructed Multiple Plasmonic Hotspots on an Individual Fractal to Amplify Broadband Hot Electron Generation
AU - Wang, Xi
AU - Liu, Changxu
AU - Gao, Congcong
AU - Yao, Kaili
AU - Masouleh, Seyed
AU - Berté, Rodrigo
AU - Ren, Haoran
AU - Menezes, Leonardo
AU - Cortés, Emiliano
AU - Bicket, Isobel
AU - Wang, Haiyu
AU - Li, Ning
AU - Zhang, Zhenglong
AU - Li, Ming
AU - Xie, Wei
AU - Yu, Yifu
AU - Fang, Yurui
AU - Zhang, Shunping
AU - Xu, Hongxing
AU - Vomiero, Alberto
AU - Liu, Yongchang
AU - Botton, Gianluigi
AU - Maier, Stefan
AU - Liang, Hongyan
N1 - Research funded by National Natural Science Foundation of China (NSFC No. 51771132)
PY - 2021/6/22
Y1 - 2021/6/22
N2 - 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.
AB - 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.
KW - broadband hot electron generation
KW - dendritic fractal
KW - electron energy loss spectroscopy
KW - plasmon-assisted photocatalysis
KW - plasmonic resonances
UR - http://www.scopus.com/inward/record.url?scp=85108891316&partnerID=8YFLogxK
U2 - 10.1021/acsnano.1c03218
DO - 10.1021/acsnano.1c03218
M3 - Article
SN - 1936-0851
VL - 15
SP - 10553
EP - 10564
JO - ACS Nano
JF - ACS Nano
IS - 6
ER -
