The nanoscale manipulation of matter allows properties to be created in a material that would be difficult or even impossible to achieve in the bulk state. Progress towards such functional nanoscale architectures requires the development of methods to precisely locate nanoscale objects in three dimensions and for the formation of rigorous structure-function relationships across multiple size regimes (beginning from the nanoscale). Here, we use DNA as a programmable ligand to show that two- and three-dimensional mesoscale superlattice crystals with precisely engineered optical properties can be assembled from the bottom up. The superlattices can transition from exhibiting the properties of the constituent plasmonic nanoparticles to adopting the photonic properties defined by the mesoscale crystal (here a rhombic dodecahedron) by controlling the spacing between the gold nanoparticle building blocks. Furthermore, we develop a generally applicable theoretical framework that illustrates how crystal habit can be a design consideration for controlling far-field extinction and light confinement in plasmonic metamaterial superlattices.

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