Publication date: 15th May 2025
Core-shell tin-doped indium oxide nanocrystals (ITO NCs)—with the tin dopants incorporated selectively in either the core or shell—exhibit two spectrally distinct localized surface plasmon resonances (LSPR) resulting from the interfaces between the surrounding environment and NC surface and between the core and shell. Simulations reveal highly concentrated electric near fields at the core-shell interface under incident infrared light resonant with the higher energy “core mode” and at the shell-surroundings interface under light resonant with the lower energy “surface mode.” The frequency of these modes can be tuned by varying the Sn-doping concentration and relative dimensions of the core and shell during synthesis, which changes the radial distribution of free electrons. Previous work has shown that ITO NCs assembled into ordered lattices display a collective plasmon mode, resulting from the dipole-dipole coupling of individual NCs, that is redshifted from the LSPR of individual NCs measured in a colloidal solution. Thin patterned assemblies of nanostructures like NC monolayers that give rise to new properties like collective plasmon modes are called metasurfaces. We hypothesized that more broadly tunable spectral and near-field properties could be achieved in metasurfaces by leveraging the additional tunability of core-shell NCs compared to uniformly-doped ITO NCs. In this work, we assemble core-shell ITO NCs into monolayers and observe large and small relative redshifts of the surface and core modes, respectively. Utilizing polarized light at various incident angles, we demonstrate the emergence of spectral peaks due to in- and out-of-plane collective resonances derived from both the “core” and “surface” modes of the individual NCs. We use finite element method simulations to reproduce redshift trends and in- and out-of-plane mode intensity variations for core-shell monolayers and visualize surface charge densities and local electric field distributions at resonant frequencies. Finally, these metasurfaces can be incorporated in photonic structures to further sculpt the electric field distribution and target spectral characteristics of interest for applications ranging from passive cooling to optical switching.
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