Large-Area, Highly Crystalline DNA-Assembled Metasurfaces Exhibiting Widely Tunable Epsilon-Near-Zero Behavior

Metasurfaces prepared via bottom-up nanoparticle assembly enable the deliberate manipulation of light in the optical regime, resulting in media with various engineered optical responses. Here, we report a scalable method to grow highly crystalline 2D metasurfaces composed of colloidal gold nanocubes, over macroscopic areas, using DNA-mediated assembly under equilibrium conditions. Using an effective medium description, we predict that these plasmonic metasurfaces behave as dielectric media with high refractive indices that can be dynamically tuned by tuning DNA length. Furthermore, we predict that, when coupled with an underlying thin gold film, the real permittivity of these metasurfaces exhibits a crossover region between positive and negative values, known as the epsilon-near-zero (ENZ) condition, which can be tuned between 1.5 and 2.6 μm by changing DNA length. Optical characterization performed on the DNA-assembled metasurfaces reveals that the predicted optical properties agree well with the measured response. Overall, we propose an efficient method for realizing large-area plasmonic metasurfaces that enable dynamic control over optical characteristics. High-index and ENZ metasurfaces operating in the telecommunications regime could have significant implications in high-speed optical computing, optical communications, optical imaging, and other areas.