Plasmon nanoparticle superlattices as optical-frequency magnetic metamaterials.

Nanocrystal superlattices have emerged as a new platform for bottom-up metamaterial design, but their optical properties are largely unknown. Here, we investigate their emergent optical properties using a generalized semi-analytic, full-field solver based on rigorous coupled wave analysis. Attention is given to superlattices composed of noble metal and dielectric nanoparticles in unary and binary arrays. By varying the nanoparticle size, shape, separation, and lattice geometry, we demonstrate the broad tunability of superlattice optical properties. Superlattices composed of spherical or octahedral nanoparticles in cubic and AB(2) arrays exhibit magnetic permeabilities tunable between 0.2 and 1.7, despite having non-magnetic constituents. The retrieved optical parameters are nearly polarization and angle-independent over a broad range of incident angles. Accordingly, nanocrystal superlattices behave as isotropic bulk metamaterials. Their tunable permittivities, permeabilities, and emergent magnetism may enable new, bottom-up metamaterials and negative index materials at visible frequencies.