Chiral Pearlescent Cellulose Nanocrystals Films with Broad‐Range Tunable Optical Properties for Anti‐Counterfeiting Applications

Abstract Pearlescent materials are of technological importance in a diverse array of industries from cosmetics to premium paints; however, chiral pearlescent materials remain unexplored. Here, chiral pearlescent films with on‐demand iridescence and metallic appearance are simply organized by leveraging vertical pressure to direct the self‐assembly of cellulose nanocrystals. The films are formed with a bilayer planar anchored left‐handed chiral nematic architecture, in which the bottom layer is featured with a vertical gradient pitch, and the top layer is featured with a uniform pitch. Simultaneous reflection of the rainbow colors and an on‐demand color of left‐handed polarized light with angle‐dependent wavelength and polarization state accounts for the unique optical phenomenon based on experimental observation and theoretical analysis. Such chiroptical property can be readily tuned with architectural design, enabling reproducible optical appearance with high fidelity. Bringing the pearlescence, iridescence, and specular reflection together endows cellulose nanocrystal films with rich and tunable chiroptical properties that can be used for anti‐counterfeiting applications. The current work marks the beginning of chiral pearlescent materials from renewable resources, while the pressure‐directed self‐assembly provides a step toward scalable production.