Hierarchical Organization of Structurally Colored Cholesteric Phases of Cellulose via 3D Printing

Structural color—a widespread phenomenon observed throughout nature is caused by light interference from ordered phases of matter. While state‐of‐the‐art nanofabrication techniques can produce structural organization in small areas, cost‐effective and scalable techniques are still lacking to generate tunable color at sub‐micron length scales. In this work, structurally colored hydroxypropyl cellulose filaments are produced with a suppressed angular color response by 3D printing. The systematic study of the morphology of the filaments reveals the key stages in the induction of a two‐degree hierarchical order through 3D printing. The first degree of order originated from the changing of the cholesteric pitch at a few hundred nm scale via chemical modification and tuning of the solid content of the lyotropic phase. Upon 3D printing, the secondary hierarchical order of periodic wrinkling is introduced through the Helfrich–Hurault deformation of the shear‐aligned cholesteric phases. In single‐layered filaments, four morphological zones with varying orders of wrinkles are identified. Detailed morphological characterization is carried out using SEM to shed light on the mechanism of the wrinkling behavior. Through this work, the possibility of modifying the wrinkling behavior is demonstrated and thus the angle dependence of the color response by changing the printing conditions. Here, the fabrication of a two‐degree ordered structure is demonstrated by 3D printing of hydroxypropyl cellulose (HPC), which enables a simple production method for colorful samples with supressed angular dependence. The helicoids formed in this lyotropic phase give rise to structural coloration, while the optical behavior is controlled through shear forces induced by 3D printing that leads to periodic wrinkling.