Flower-like Photonic Hydrogel with Superstructure Induced via Modulated Shear Field

Biological tissues usually have complex superstructures and elaborated functionalities. However, creating superstructures in soft and wet hydrogels is challenging because of the absence of effective approaches to control the molecular orientation. Here we introduce a method to create superstructures in photonic hydrogels comprising lamellar bilayers intercalated in the cross-linked polymer network. The orientation of lamellar bilayers in the photonic gel, which are sensitive to shear, is modulated by applying a gradient shear field on the precursor solution using a customized rheometer. The difference in orientation of lamellar bilayers leads to swelling mismatch in the radial direction, endowing the disk-shape hydrogel with a macroscopic flower-like shape with a central dome and an edge petal, along with a bright photonic color. By characterization of the swelling anisotropy of the radial profile, the shear rate required for the unidirectional orientation of lamellar bilayers was extracted. Moreover, a delayed polymerization experiment was designed to measure the lifetime of aligned lamellar bilayers, which reveals the domain size of lamellar bilayers in the precursor solution. Furthermore, we also demonstrated that the hydrogel flowers could fade and rebloom reversibly in response to external stimuli. This work presents a strategy to develop superstructures in hydrogels and sheds light on designing biomimetic materials with intricately architectural superstructure.