Plasmonic structures can be constructed from precise numbers of well-defined metal nanoparticles that are held together with molecular linkers, templates or spacers. Such structures could be used to concentrate, guide and switch light on the nanoscale in sensors and various other devices. DNA was first used to rationally design plasmonic structures in 1996, and more sophisticated motifs have since emerged as effective and versatile species for guiding the assembly of plasmonic nanoparticles into structures with useful properties. Here we review the design principles for plasmonic nanostructures, and discuss how DNA has been applied to build finite-number assemblies (plasmonic molecules), regularly spaced nanoparticle chains (plasmonic polymers) and extended two- and three-dimensional ordered arrays (plasmonic crystals).

We introduce the first plasmonic palette utilizing color generation strategies for photorealistic printing with aluminum nanostructures. Our work expands the visible color space through spatially mixing and adjusting the nanoscale spacing of discrete nanostructures. With aluminum as the plasmonic material, we achieved enhanced durability and dramatically reduced materials costs with our nanostructures compared to commonly used plasmonic materials such as gold and silver, as well as size regimes scalable to higher-throughput approaches such as photolithography and nanoimprint lithography. These advances could pave the way toward a new generation of low-cost, high-resolution, plasmonic color printing with direct applications in security tagging, cryptography, and information storage.

Free-standing nanoparticle superlattices (suspended highly ordered nanoparticle arrays) are ideal for designing metamaterials and nanodevices free of substrate-induced electromagnetic interference. Here, we report on the first DNA-based route towards monolayered free-standing nanoparticle superlattices. In an unconventional way, DNA was used as a 'dry ligand' in a microhole-confined, drying-mediated self-assembly process. Without the requirement of specific Watson-Crick base-pairing, we obtained discrete, free-standing superlattice sheets in which both structure (inter-particle spacings) and functional properties (plasmonic and mechanical) can be rationally controlled by adjusting DNA length. In particular, the edge-to-edge inter-particle spacing for monolayered superlattice sheets can be tuned up to 20 nm, which is a much wider range than has been achieved with alkyl molecular ligands. Our method opens a simple yet efficient avenue towards the assembly of artificial nanoparticle solids in their ultimate thickness limit--a promising step that may enable the integration of free-standing superlattices into solid-state nanodevices.

Metal nanostructures can be designed to scatter different colours depending on the polarization of the incident light. Such spectral control is attractive for applications such as high-density optical storage, but challenges remain in creating microprints with a single-layer architecture that simultaneously enables full-spectral and polarization control of the scattered light. Here we demonstrate independently tunable biaxial colour pixels composed of isolated nanoellipses or nanosquare dimers that can exhibit a full range of colours in reflection mode with linear polarization dependence. Effective polarization-sensitive full-colour prints are realized. With this, we encoded two colour images within the same area and further use this to achieve depth perception by realizing three-dimensional stereoscopic colour microprint. Coupled with the low cost and durability of aluminium as the functional material in our pixel design, such polarization-sensitive encoding can realize a wide spectrum of applications in colour displays, data storage and anti-counterfeiting technologies.