Publication date: 22nd July 2026
Cellulose nanocrystals (CNCs) are promising renewable building blocks for chiral optoelectronic materials because of their outstanding thermomechanical properties and their ability to self-assemble into cholesteric liquid-crystalline phases [1]. This chiral organization can be retained in solid films through evaporation-induced self-assembly (EISA), producing photonic structures with characteristic dimensions that interact with UV and visible light. CNCs derived from the cellulose I allomorphs typically possess a right-handed twist along their longitudinal axis and form left-handed cholesteric phases. In contrast, CNCs obtained from cellulose II allomorphs [1, 2] have been reported to display an opposite particle twist and can generate right-handed liquid-crystalline phases, providing opportunities to control the handedness of chiral photonic films. Here, we present our recent work on the preparation, surface modification, and self-assembly of CNC allomorphs obtained from plant and bacterial cellulose sources. In addition to native cellulose I nanocrystals, Mercerization and ethylenediamine treatments were used to produce cellulose II and cellulose III allomorphs [3-5] respectively. The reducing end groups of the nanocrystals were subsequently functionalized with methoxypolyethylene glycol (mPEG) amines. This end-selective modification introduces steric interactions and may generate depletion effects, offering an additional strategy for controlling liquid-crystalline phase behavior without uniformly altering the nanocrystal surface. Using atomic force microscopy (AFM), polarized optical microscopy (POM), and circular dichroism (CD) spectroscopy, we investigate how crystal allomorph, nanocrystal morphology, polymer grafting, surface chemistry, and confinement influence chiral self-assembly and optical response. Our findings demonstrate that the handedness and structural characteristics of CNC-based cholesteric phases can be tuned through such complementary approaches. Polymer-tethered CNC allomorphs [1, 4] therefore provide a versatile bottom-up platform for the development of sustainable chiral photonic and optoelectronic materials, with potential applications in chiral plasmonics [5], optical sensing, and heterogeneous enantioselective catalysis.
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