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Two-dimensional arrays of plasmonic nanoparticles at interfaces are promising candidates for novel optical metamaterials. Such systems materialise from ‘top–down’ patterning or ‘bottom–up’ self-assembly of nanoparticles at liquid/liquid or liquid/solid interfaces. Here, we present a comprehensive analysis of an extended effective quasi-static four-layer-stack model for the description of plasmon-resonance-enhanced optical responses of such systems. We investigate in detail the effects of the size of nanoparticles, average interparticle separation, dielectric constants of the media constituting the interface, and the nanoparticle position relative to the interface. Interesting interplays of these different factors are explored first for normally incident light. For off-normal incidence, the strong effects of the polarisation of light are found at large incident angles, which allows to dynamically tune the reflectance spectra. All the predictions of the theory are tested against full-wave simulations, proving this simplistic model to be adequate within the quasi-static limit. The model takes seconds to calculate the system’s optical response and makes it easy to unravel the effect of each system parameter. This helps rapid rationalization of experimental data and understanding of the optical signals from these novel ‘metamaterials’, optimised for light reflection or harvesting.

Theory of tailorable optical response of two-dimensional arrays of plasmonic nanoparticles at dielectric interfaces