Computational design of bimetallic core-shell nanoparticles for hot-carrier photocatalysis

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Title: Computational design of bimetallic core-shell nanoparticles for hot-carrier photocatalysis
Authors: Ranno, L
Dal Forno, S
Lischner, JC
Item Type: Journal Article
Abstract: Computational design can accelerate the discovery of new materials with tailored properties, but applying this approach to plasmonic nanoparticles with diameters larger than a few nanometers is challenging as atomistic first-principles calculations are not feasible for such systems. In this paper, we employ a recently developed material-specific approach that combines effective mass theory for electrons with a quasistatic description of the localized surface plasmon to identify promising bimetallic core-shell nanoparticles for hot-electron photocatalysis. Specifically, we calculate hot-carrier generation rates of 100 different core-shell nanoparticles and find that systems with an alkali-metal core and a transition-metal shell exhibit high figures of merit for water splitting and are stable in aqueous environments. Our analysis reveals that the high efficiency of these systems is related to their electronic structure, which features a two-dimensional electron gas in the shell. Our calculations further demonstrate that hot-carrier properties are highly tunable and depend sensitively on core and shell sizes. The design rules resulting from our work can guide experimental progress towards improved solar energy conversion devices.
Issue Date: 6-Jul-2018
Date of Acceptance: 18-Jun-2018
ISSN: 2057-3960
Publisher: Nature Publishing Group
Journal / Book Title: npj Computational Materials
Volume: 4
Copyright Statement: © The Author(s) 2018. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article ’ s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article ’ s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons. org/licenses/by/4.0/
Sponsor/Funder: Engineering & Physical Science Research Council (EPSRC)
Funder's Grant Number: EP/N005244/1
Keywords: Science & Technology
Physical Sciences
Chemistry, Physical
Materials Science, Multidisciplinary
Materials Science
Publication Status: Published
Article Number: ARTN 31
Appears in Collections:Faculty of Engineering
Condensed Matter Theory
Faculty of Natural Sciences

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