Chemically tailored dielectric-to-metal transition for the design of metamaterials from nanoimprinted colloidal nanocrystals.

We demonstrate optical metamaterial design using colloidal gold nanocrystal building blocks. In the solid state, chemically exchanging the nanocrystals' surface-capping molecules provides a tailorable dielectric-to-metal transition exhibiting a 10(10) range in DC conductivity and dielectric permittivity ranging from everywhere positive to everywhere negative throughout the visible-to-near-IR. Direct, wide-area nanoimprinting of subwavelength superstructures at room temperature, on plastic and glass substrates, affords plasmonic resonances ranging from 660 to 1070 nm, in agreement with numerical simulations.