Facile Stratification-Enabled Emergent Hyper-Reflectivity in Cholesteric Liquid Crystals

Cholesteric liquid crystals (CLCs) are chiral photonic materials with selective reflection in terms of wavelength and polarization. Helix engineering is often required in order to produce desired properties for CLC materials to be employed for beam steering, light diffraction, scattering, and adaptive or broadband reflection. Here, we demonstrate a novel photopolymerization-enforced stratification (PES)-based strategy to realize helix engineering in a chiral CLC system with initially one handedness of molecular rotation throughout the layer. PES plays a crucial role in driving the chiral dopant bundle consisting of two chiral dopants of opposite handedness to spontaneously phase separate and create a CLC bilayer structure that reflects left- and right-handed circularly polarized light (CPL). The initially hidden chiral information therefore becomes explicit, and hyper-reflectivity, i.e., reflecting both left- and right-handed CPL, successfully emerges from the designed CLC mixture. The PES mechanism can be applied to structure a wide range of liquid crystal (LC) and polymer materials. Moreover, the engineering strategy enables facile programming of the center wavelength of hyper-reflection, patterning, and incorporating stimuli-responsiveness in the optical device. Hence, the engineered hyper-reflective CLCs offer great promise for future applications, such as digital displays, lasing, optical storage, and smart windows.