Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure
Journal article, 2020

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. Although 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.

plasmon dephasing

time-dependent density functional theory

hot carriers

hot electrons

atomic scale

plasmon decay


Tuomas Rossi

Chalmers, Physics, Materials and Surface Theory

Paul Erhart

Chalmers, Physics, Condensed Matter and Materials Theory

Mikael Kuisma

University of Jyväskylä

ACS Nano

1936-0851 (ISSN) 1936-086X (eISSN)

Vol. 14 8 9963-9971

Towards nanoscale reality in plasmonic hot-carrier generation (RealNanoPlasmon)

European Commission (EC), 2019-04-01 -- 2021-03-31.

Subject Categories

Atom and Molecular Physics and Optics

Condensed Matter Physics





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DOI: 10.5281/zenodo.3927527

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