Transition of surface-interface creasing in bilayer hydrogels.

Controlling the morphologies and properties of the surface and/or interface of bimaterials consisting of soft polymers provides new opportunities in many engineering applications. Crease is a widely observed deformation mode in nature and engineering applications for soft polymers where the smooth surface folds into a region of self-contact with a sharp tip, usually induced by the instability from mechanical compression or swelling. In this work, we explore the competition mechanisms between surface and interface creases through numerical simulations and experimental studies on bilayer hydrogels. The surface or interface crease of the bilayer hydrogels under swelling is governed by both the modulus ratio (M2/M1) and the height ratio (H2/H1). Through extensive numerical simulations, we find that the interface crease of the bilayer hydrogels can only occur at a moderate modulus ratio (24 < M2/M1 < 96) and a large height ratio (H2/H1 ≥ 8). Guided by this phase diagram, our experiments confirm that both surface and interface creases can be generated by swelling triggered instability, and the transition of surface to interface creases occurs at the critical value of the height ratio (H2/H1) between 5 and 10. Such an observation is in good agreement with our numerical predictions. Fundamental understandings on the switching between the surface and interface creases provide new insights into the design of highly tunable soft materials and devices over a wide range of length scales.