Mechanically Responsive Circularly Polarized Luminescence from Cellulose‐Nanocrystal‐Based Shape‐Memory Polymers

Abstract Stimulus‐responsive materials that display circularly polarized luminescence (CPL) have attracted great attention for application in chiral sensors and smart displays. However, due to difficulties in the regulation of chiral structures, fine control of CPL remains a challenge. Here, it is demonstrated that cellulose nanocrystal shape‐memory polymers (CNC‐SMPs) with luminescent components enable mechanically responsive CPL. The chiral nematic organization of CNCs in the material gives rise to a photonic bandgap. By manipulating the photonic bandgap or luminescence wavelengths of the luminescent CNC‐SMPs, precise control of CPL emission with varied wavelengths and high dissymmetry factors (g_lum) is achieved. Specifically, CPL emission can be switched reversibly by treating the luminescent CNC‐SMPs with hot‐pressing and recovery by heating. Pressure‐responsive CPL with tunable g_lum values is ascribed to the pressure‐responsive photonic bandgaps. Moreover, colorimetric and CPL‐active patterns are created by imprinting desired forms into SMP samples. This study demonstrates a novel way to fabricate smart CPL systems using biomaterials.