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RESEARCH PRODUCT
Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure
Paul ErhartMikael KuismaTuomas P. Rossisubject
Materials scienceDephasingAtom and Molecular Physics and OpticsFOS: Physical sciencesGeneral Physics and AstronomyNanoparticlePhysics::Optics02 engineering and technology010402 general chemistry01 natural sciencesAtomic unitsArticleplasmon dephasingPhysics - Chemical PhysicsMesoscale and Nanoscale Physics (cond-mat.mes-hall)General Materials ScienceAbsorption (electromagnetic radiation)Plasmonatomic-scaleatomic scaleChemical Physics (physics.chem-ph)Plasmonic nanoparticlesCondensed Matter - Materials ScienceCondensed Matter - Mesoscale and Nanoscale Physicslocalized surface plasmonGeneral EngineeringMaterials Science (cond-mat.mtrl-sci)plasmon decay021001 nanoscience & nanotechnologyCondensed Matter Physicstime-dependent density-functional theory0104 chemical sciencespintaplasmonitplasmonittime-dependent density functional theoryChemical physicsFemtosecondnanohiukkasetAstrophysics::Earth and Planetary Astrophysicshot carriers0210 nano-technologyhot electronsLocalized surface plasmondescription
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.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2020-02-27 |