Hierarchically Doped Plasmonic Nanocrystal Metamaterials

[Image: see text] Assembling plasmonic nanocrystals in regular superlattices can produce effective optical properties not found in homogeneous materials. However, the range of these metamaterial properties is limited when a single nanocrystal composition is selected for the constituent meta-atoms. Here, we show how continuously varying doping at two length scales, the atomic and nanocrystal scales, enables tuning of both the frequency and bandwidth of the collective plasmon resonance in nanocrystal-based metasurfaces, while these features are inextricably linked in single-component superlattices. Varying the mixing ratio of indium tin oxide nanocrystals with different dopant concentrations, we use large-scale simulations to predict the emergence of a broad infrared spectral region with near-zero permittivity. Experimentally, tunable reflectance and absorption bands are observed, owing to in- and out-of-plane collective resonances. These spectral features and the predicted strong near-field enhancement establish this multiscale doping strategy as a powerful new approach to designing metamaterials for optical applications.