The availability of metamaterials with properties that can be actively tuned is crucial for the future development of various metamaterial-based technologies. Here we show that by using silver nanoparticles equipped with a thermally responsive organic coating a metamaterial is obtained with reversibly switchable properties. The material investigated exhibits dynamic self-assembly resulting from temperature-dependent changes of organic coating shape, which translates to a switchable spatial distribution of the silver nanoparticles. This in turn strongly influences the optical properties of the entire material. The measured optical characteristics of the material are in excellent agreement with theoretical calculations, which allow us to use the latter to predict a dynamically tunable epsilon-near-zero behaviour of the metamaterial. The suggested methodology opens new routes for tunable metamaterials that operate in the visible region and will enable various applications for soft-matter-based optical devices.

Spontaneous formation of smectic and columnar structures was observed when spherical gold nanoparticles were functionalized with mesogenic thiols (see layered structure and X-ray pattern of a sample in smectic phase). The particle ordering is stimulated by softening of the interparticle potential and flexibility for deformation of the grafting layer.

The availability of helical assemblies of plasmonic nanoparticles with precisely controlled and tunable structures can play a key role in the future development of chiral plasmonics and metamaterials. Here, a strategy to efficiently yield helical structures based on the cooperative interactions of liquid crystals and gold nanoparticles in thin films is developed. These nanocomposites exhibit exceptional long‐range hierarchical order across length scales, which results from the growth mechanism of nanoparticle‐coated twisted nanoribbons and their ability to form organized bundles. The helical assembly formation is governed by the presence of rationally functionalized nanoparticles. Importantly, the thickness of the achieved nanocomposites can be reversibly reconfigured owing to the polymorphic nature of the liquid crystal. The versatility of the proposed approach is demonstrated by preparing helices assembled from nanoparticles of different geometries and dimensions (spherical and rod‐like). The described strategy may become an enabling technology for structuring nanoparticle assemblies with high precision and fabricating optically active materials.

On the GO: The basal plane allylic alcohol functionality of graphite oxide (GO) can be converted into N,N‐dimethylamide groups through an Eschenmoser–Claisen sigmatropic rearrangement by using N,N‐dimethylacetamide dimethyl acetal. Subsequent saponification of these groups affords the carboxylic acids (see picture), which, when deprotonated, electrostatically stabilize the graphene sheets in an aqueous environment.