Accelerating Cellulose Nanocrystal Assembly into Chiral Nanostructures

Cellulose nanocrystal (CNC) suspensions self-assembled into chiral nematic liquid crystals. This property has enabled the development of versatile optical materials with fascinating properties. Nevertheless, the scale-up production and commercial success of chiral nematic CNC superstructures face significant challenges. Fabrication of chiral nematic CNC nanostructures suffers from a ubiquitous pernicious trade-off between uniform chiral nematic structure and rapid self-assembly. Specifically, the chiral nematic assembly of CNCs is a time-consuming, spontaneous process that involves the organization of particles into ordered nanostructures as the solvent evaporates. This review is driven by the interest in accelerating chiral nematic CNC assembly and promoting a long-range oriented chiral nematic CNC superstructure. To start this review, the chirality origins of CNC and CNC aggregates are analyzed. This is followed by a summary of the recent advances in stimuli-accelerated chiral nematic CNC self-assembly procedures, including evaporation-induced self-assembly, continuous coating, vacuum-assisted self-assembly, and shear-induced CNC assembly under confinement. In particular, stimuli-induced unwinding, alignment, and relaxation of chiral nematic structures were highlighted, offering a significant link between the accelerated assembly approaches and uniform chiral nematic nanostructures. Ultimately, future opportunities and challenges for rapid chiral nematic CNC assembly are discussed for more innovative and exciting applications.