Hot-Carrier Generation in Plasmonic Nanoparticles : The Importance of Atomic Structure
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
Julkaistu sarjassa
ACS NanoPäivämäärä
2020Tekijänoikeudet
© 2020 the Authors
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.
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Julkaisija
American Chemical Society (ACS)ISSN Hae Julkaisufoorumista
1936-0851Asiasanat
Julkaisu tutkimustietojärjestelmässä
https://converis.jyu.fi/converis/portal/detail/Publication/41632525
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Suomen AkatemiaRahoitusohjelmat(t)
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We acknowledge financial support from the Knut and Alice Wallenberg Foundation (2014.0226, 2015.0055), the Swedish Research Council (2015-04153), and the Swedish Foundation for Strategic Research (RMA15-0052). T.P.R. acknowledges support from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 838996 and also thanks the Adlerbert Research Foundation and the Wilhelm and Martina Lundgren Foundation for support. M.K. acknowledges funding from Academy of Finland under grant No 295602. We acknowledge generous computational resources provided by the Swedish National Infrastructure for Computing (SNIC) at PDC (Stockholm), NSC (Linköping), and C3SE (Gothenburg) as well as by the CSC – IT Center for Science (Finland). ...Lisenssi
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