Theory of hot-carrier generation in bimetallic plasmonic catalysts
File(s)
Author(s)
Jin, Hanwen
Herran, Matias
Cortés, Emiliano
Lischner, Johannes
Type
Journal Article
Abstract
Bimetallic nanoreactors in which a plasmonic metal is used to funnel solar energy toward a catalytic metal have recently been studied experimentally, but a detailed theoretical understanding of these systems is lacking. Here, we present theoretical results of hot-carrier generation rates of different Au-Pd nanoarchitectures. In particular, we study spherical core-shell nanoparticles with a Au core and a Pd shell as well as antenna-reactor systems consisting of a large Au nanoparticle that acts as an antenna and a smaller Pd satellite nanoparticle separated by a gap. In addition, we investigate an antenna-reactor system in which the satellite is a core-shell nanoparticle. Hot-carrier generation rates are obtained from an atomistic quantum-mechanical modeling technique which combines a solution of Maxwell's equation with a tight-binding description of the nanoparticle electronic structure. We find that antenna-reactor systems exhibit significantly higher hot-carrier generation rates in the catalytic material than the core-shell system as a result of strong electric field enhancements associated with the gap between the antenna and the satellite. For these systems, we also study the dependence of the hot-carrier generation rate on the size of the gap, the radius of the antenna nanoparticle, and the direction of light polarization. Overall, we find a strong correlation between the calculated hot-carrier generation rates and the experimentally measured chemical activity for the different Au-Pd photocatalysts. Our insights pave the way toward a microscopic understanding of hot-carrier generation in heterogeneous nanostructures for photocatalysis and other energy-conversion applications.
Date Issued
2023-10-18
Date Acceptance
2023-09-01
Citation
ACS Photonics, 2023, 10 (10), pp.3629-3636
ISSN
2330-4022
Publisher
American Chemical Society
Start Page
3629
End Page
3636
Journal / Book Title
ACS Photonics
Volume
10
Issue
10
Copyright Statement
© 2023 The Authors. Published by American Chemical Society. This publication is licensed under
CC-BY 4.0.
CC-BY 4.0.
License URL
Identifier
https://www.ncbi.nlm.nih.gov/pubmed/37869558
Publication Status
Published
Coverage Spatial
United States
Date Publish Online
2023-09-15