A1 Journal article (refereed)
Hot-Carrier Generation in Plasmonic Nanoparticles : The Importance of Atomic Structure (2020)

Rossi, T. P., Erhart, P., & Kuisma, M. (2020). Hot-Carrier Generation in Plasmonic Nanoparticles : The Importance of Atomic Structure. ACS Nano, 14(8), 9963-9971. https://doi.org/10.1021/acsnano.0c03004

JYU authors or editors

Kuisma, Mikael

Publication details

All authors or editors: Rossi, Tuomas P.; Erhart, Paul; Kuisma, Mikael

Journal or series: ACS Nano

ISSN: 1936-0851

eISSN: 1936-086X

Publication year: 2020

Volume: 14

Issue number: 8

Pages range: 9963-9971

Publisher: American Chemical Society (ACS)

Publication country: United States

Publication language: English

DOI: https://doi.org/10.1021/acsnano.0c03004

Research data link: https://doi.org/10.5281/zenodo.3927527

Publication open access: Openly available

Publication channel open access: Partially open access channel

Publication is parallel published (JYX): https://jyx.jyu.fi/handle/123456789/71233

Web address of parallel published publication (pre-print): https://arxiv.org/pdf/2002.12087.pdf

Abstract

Metal nanoparticles are attractive for plasmon-enhanced generation of hot carriers, which may be harnessed in photochemical reactions. In this work, we analyze the coherent femtosecond dynamics of photon absorption, plasmon formation, and subsequent hot-carrier generation through plasmon dephasing using first-principles simulations. We predict the energetic and spatial hot-carrier distributions in small metal nanoparticles and show that the distribution of hot electrons is very sensitive to the local structure. Our results show that surface sites exhibit enhanced hot-electron generation in comparison to the bulk of the nanoparticle. While the details of the distribution depend on particle size and shape, as a general trend lower-coordinated surface sites such as corners, edges, and {100} facets exhibit a higher proportion of hot electrons than higher-coordinated surface sites such as {111} facets or the core sites. The present results thereby demonstrate how hot carriers could be tailored by careful design of atomic-scale structures in nanoscale systems.

Keywords: plasmons; surface plasmons; nanoparticles

Free keywords: localized surface plasmon; plasmon decay; plasmon dephasing; time-dependent density-functional theory; hot electrons; hot carriers; atomic-scale

Fields of science: