Spontaneous Wrinkle Formation on Hydrogel Surfaces Using Photoinitiator Diffusion from Oil-Water Interface

Patterning wrinkles on three-dimensional curved or enclosed surfaces can be challenging due to difficulties in application of uniform films and stresses on such structures. In this study, we demonstrate a simple one-step wrinkle-formation method on various hydrogel structures utilizing the oil-water interfaces. By diffusion of the photoinitiator from the oil phase to the prepolymer solution in water through the interface, a characteristic cross-linking gradient is set up in the hydrogel. Then, after photopolymerization, we observe diverse patterns of wrinkles upon changing the concentration of the hydrogel or photoinitiator. As the wrinkle formation via photoinitiator diffusion through the interface requires only UV exposure for polymerization, while taking advantage of the oil-water interfacial tension, wrinkles can be developed easily on various curved structures. In addition, we illustrate the formation of wrinkles on surfaces underneath another layer of polymer or on completely enclosed surfaces, which is difficult with conventional methods. We expect that our results will lead to production of novel microstructures and provide a platform for studying the morphogenesis of wrinkles found in nature such as in curved substrates and multilayers.