Self-constructed multiple plasmonic hotspots on an individual fractal to amplify broadband hot electron generation

Xi Wang, Changxu Liu, Congcong Gao, Kaili Yao, Seyed Shayan Mousavi Masouleh, Rodrigo Berté, Haoran Ren, Leonardo de S. Menezes, Emiliano Cortés, Isobel C. Bicket, Haiyu Wang, Ning Li, Zhenglong Zhang, Ming Li, Wei Xie, Yifu Yu, Yurui Fang, Shunping Zhang, Hongxing Xu, Alberto VomieroYongchang Liu, Gianluigi A. Botton, Stefan A. Maier, Hongyan Liang

Research output: Contribution to journalArticlepeer-review

2 Citations (Scopus)

Abstract

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.
Original languageEnglish
Pages (from-to)10553–10564
Number of pages12
JournalACS Nano
Volume15
Issue number6
Early online date11 Jun 2021
DOIs
Publication statusPublished - 22 Jun 2021
Externally publishedYes

Keywords

  • dendritic fractal
  • broadband hot electron generation
  • plasmonic resonances
  • electron energy loss spectroscopy
  • plasmon-assisted photocatalysis

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