Optical Properties of Self‐Assembled Cellulose Nanocrystals Films Suspended at Planar–Symmetrical Interfaces

Hierarchically structured materials comprising rod‐like, chiral, nanoparticles are commonly encountered in nature as they can form assemblies with exceptional optical and mechanical characteristics. These include cellulose nanocrystals (CNCs), which have a large potential for the fabrication of bioinspired materials mimicking those advanced properties. Fine‐tuning the optomechanical properties of assemblies obtained from CNCs hinges on the transformations from suspensions of liquid crystals to long‐range order in the dry state. So far, associated transitions have been studied using trivial interfaces such as planar substrates. Such transitions are explored as they evolve onto meshed supports. The meshed substrate offers a complex topology, as is encountered in nature, for the formation of CNCs films. The CNCs self‐assembly occurs under confinement and support of the framework bounding the mesh openings. This leads to coexisting suspended and supported nanoparticle layers exhibiting nematic and/or chiral nematic order. Optical microscopy combined with crossed polarizers indicate that the formation of the suspended films occurs via intermediate gelation or kinetic arrest of CNCs across the mesh's open areas. The formation of self‐standing, ultrathin films of CNCs with tunable optical properties, such as selective reflections in the visible range (structural color), is demonstrated by using the presented simple and scalable approach.