Swelling-Induced Interface Crease Instabilities at Hydrogel Bilayers

Abstract

Two dissimilar hydrogel layers bonded together become unstable when the compressive stresses due to diffusion-driven swelling of the layers reach a critical point and creases form at the interface. Although creasing instabilities observed on surfaces of soft solids subjected to large compressions are well studied, the transient nature and critical conditions for the emergence of interface creases as a result of swelling behavior of hydrogels remain elusive. Here, we investigate the formation and transient growth of interface creases in bilayer hydrogels through experimental and computational approaches. Equipped with a mixed isogeometric analysis that accounts for large swelling deformations along with dissipative fluid transport phenomena, we show that both the equilibrium and the transient characteristics of interface creases can be tuned by controlling the material properties, in contrast to the reported material-independent behavior of creases in elastomers. The effects of material parameters on the onset and growth of interface creases are quantified in terms of the critical swelling ratio and critical chemical potential, and these values are compared to the critical conditions for the emergence of wrinkling instabilities. In agreement with our experimental observations of swelling bilayer hydrogels, our computational results demonstrate that the formation of creases is energetically more favorable than wrinkle formation at the interface.