Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure
Artikel i vetenskaplig tidskrift, 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.

Författare

Tuomas Rossi

Chalmers, Fysik, Material- och ytteori

Paul Erhart

Chalmers, Fysik, Kondenserad materie- och materialteori

Mikael Kuisma

Jyväskylän Yliopisto

ACS Nano

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

Vol. 14 8 9963-

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

Europeiska kommissionen (EU), 2019-04-01 -- 2021-03-31.

Ämneskategorier

Atom- och molekylfysik och optik

Den kondenserade materiens fysik

DOI

10.1021/acsnano.0c03004

Relaterade dataset

DOI: 10.5281/zenodo.3927527

Mer information

Senast uppdaterat

2020-09-21