Extended Discrete Interaction Model: Plasmonic Excitations of Silver Nanoparticles
2019
Zakomirnyi, Vadim I. | Rinkevicius, Zilvinas | Baryshnikov, Glib V. | Sørensen, Lasse K. | Ågren, Hans
We present a new atomistic model for plasmonic excitations and optical properties of metallic nanoparticles, which collectively describes their complete response in terms of fluctuating dipoles and charges that depend on the local environment and on the morphology of the composite nanoparticles. Being atomically dependent, the total optical properties, the complex polarizability, and the plasmonic excitation of a cluster refer to the detailed composition and geometric characteristics of the cluster, making it possible to explore the role of the material, alloy mixing, size, form shape, aspect ratios, and other geometric factors down to the atomic level and making it useful for the design of plasmonic particles with particular strength and field distribution. The model is parameterized from experimental data and, at present, practically implementable for particles up to more than 10 nm (for nanorods even more), thus covering a significant part of the gap between the scales where pure quantum calculations are possible and where pure classical models based on the bulk dielectric constant apply. We utilized the method to both spherical and cubical clusters along with nanorods where we demonstrate both the size, shape, and ratio dependence of plasmonic excitations and connect this to the geometry of the nanoparticles using the plasmon length.
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