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• W2055106008 abstract "For metallic nanoparticles less than 10 nm in diameter, localized surface plasmon resonances (LSPRs) become sensitive to the quantum nature of conduction electrons. In this regime, experimental probes of size-dependent LSPRs are particularly challenging, and contradictory results are often reported. Unfortunately, quantum mechanical simulations based on time-dependent Kohn-Sham density functional theory (TD-KSDFT) are computationally too expensive to tackle metal particles larger than 2 nm. Herein, we present a time-dependent orbital-free density functional theory (TD-OFDFT) that accurately captures the dynamic response of electrons in the presence of realistic ionic potentials. The TD-OFDFT method offers a comparable accuracy as TD-KSDFT but with a much lower computational cost. Using TD-OFDFT, we study size-dependent LSPRs on Na nanoparticles with diameters from 0.7 to 12.3 nm. The optical absorption spectra exhibit a nonmonotonic behavior from blue shift to red shift and back to blue shift as the particle size decreases. Three principal plasmon modes are identified, and their physical origins are elucidated. Competing physical mechanisms responsible for the nonmonotonic size dependence are discussed. The TD-OFDFT provides a unified theoretical framework that bridges the gap between classical electromagnetic theory and quantum mechanical theory for plasmonics and nanophotonics." @default.
• W2055106008 created "2016-06-24" @default.
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• W2055106008 date "2014-03-20" @default.
• W2055106008 modified "2023-09-25" @default.
• W2055106008 title "Size-Dependent Plasmonic Resonances from Large-Scale Quantum Simulations" @default.
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• W2055106008 doi "https://doi.org/10.1021/jz500216t" @default.
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• W2055106008 hasPublicationYear "2014" @default.
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