Tunable plasmonic coupling in self-assembled binary nanocrystal superlattices studied by correlated optical microspectrophotometry and electron microscopy.

We study the plasmonic properties of self-assembled binary nanocrystal superlattices (BNSLs) using correlated optical microspectrophotometry and electron microscopy performed on individual BNSL domains. The strength of near-field couplings between adjacent plasmonic nanocrystals (NCs) can be systematically engineered by varying the NC size, composition, and the lattice symmetry of BNSLs, leading to broadband spectral tunability of the collective plasmonic response of BNSLs across the entire visible spectrum. Self-assembled multicomponent NC superlattices represent a versatile platform for the rational design of macroscopic three-dimensional plasmonic metamaterials with emergent optical characteristics.