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An ultralight stand-alone plasmonic paint that can color large-scale objects is produced. 

Nanostructured plasmonic materials can lead to the extremely compact pixels and color filters needed for next-generation displays by interacting with light at fundamentally small length scales. However, previous demonstrations suffer from severe angle sensitivity, lack of saturated color, and absence of black/gray states and/or are impractical to integrate with actively addressed electronics. Here, we report a vivid self-assembled nanostructured system which overcomes these challenges via the multidimensional hybridization of plasmonic resonances. By exploiting the thin-film growth mechanisms of aluminum during ultrahigh vacuum physical vapor deposition, dense arrays of particles are created in near-field proximity to a mirror. The sub-10-nm gaps between adjacent particles and mirror lead to strong multidimensional coupling of localized plasmonic modes, resulting in a singular resonance with negligible angular dispersion and ∼98% absorption of incident light at a desired wavelength. The process is compatible with arbitrarily structured substrates and can produce wafer-scale, diffusive, angle-independent, and flexible plasmonic materials. We then demonstrate the unique capabilities of the strongly coupled plasmonic system via integration with an actively addressed reflective liquid crystal display with control over black states. The hybrid display is readily programmed to display images and video. 

Abstract Nanostructured materials have enabled new ways of controlling the light–matter interaction, opening new routes for exciting applications, in display technologies and colorimetric sensing, among others. In particular, metallic nanoparticles permit the production of color structures out of colorless materials. These plasmonic structural colors are sensitive to the environment and thus offer an interesting platform for sensing. Here, a self‐assembly of aluminum nanoparticles in close proximity of a mirror is spaced by an ultrathin poly(N‐isopropylacrylamide) (PNIPAM) layer. Hybridizing the plasmonic system with the active polymer layer, a thermoresponsive gap‐plasmon architecture is formed that transduces changes in the temperature and relative humidity of the environment into color changes. By harnessing the environmentally induced structural changes of PNIPAM, it was estimated from the finite difference time domain simulation that the resonance can be tuned 7 nm per every 1 nm change in thickness, resulting in color variation. Importantly, these fully reversible changes can be used for reusable powerless humidity and temperature colorimetric sensing. Crucially if condensation on the structure happens, the polymer layer is deformed beyond recovery and the colors are washed away. We leverage this effect to produce tamper‐proof dew labels that a straightforward smartphone app can read by taking a picture.