Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure
| Autor: | Rossi, Tuomas P., Erhart, Paul, Kuisma, Mikael |
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| Rok vydání: | 2020 |
| Předmět: | |
| Zdroj: | ACS Nano 14, 9963 (2020) |
| Druh dokumentu: | Working Paper |
| DOI: | 10.1021/acsnano.0c03004 |
| Popis: | 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. Comment: 10 pages, 4 figures |
| Databáze: | arXiv |
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