Self-constructed multiple plasmonic hotspots on an individual fractal to amplify broadband hot electron generation.
File(s)0527 MS.docx (1.91 MB)
Accepted version
Author(s)
Type
Journal Article
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.
Date Issued
2021-06-22
Date Acceptance
2021-06-08
Citation
ACS Nano, 2021, 15 (6), pp.10553-10564
ISSN
1936-0851
Publisher
American Chemical Society
Start Page
10553
End Page
10564
Journal / Book Title
ACS Nano
Volume
15
Issue
6
Copyright Statement
© 2021 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Nano, after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsnano.1c03218
Sponsor
Engineering & Physical Science Research Council (E
Identifier
https://www.ncbi.nlm.nih.gov/pubmed/34114794
Grant Number
EP/M013812/1
Subjects
broadband hot electron generation
dendritic fractal
electron energy loss spectroscopy
plasmon-assisted photocatalysis
plasmonic resonances
Publication Status
Published
Coverage Spatial
United States
Date Publish Online
2021-06-11