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The ability to modulate the adhesion of soft materials on-demand is desired for broad applications ranging from tissue repair to soft robotics. Research effort has been focused on the chemistry and architecture of interfaces, leaving the mechanics of soft adhesives overlooked. Stimuli-responsive mechanisms of smart hydrogels could be leveraged for achieving stimuli-responsive hydrogel adhesives that respond mechanically to external stimuli. Such stimuli-responsive hydrogel adhesives involve complex chemomechanical coupling and interfacial fracture phenomena, calling for mechanistic understanding to enable rational design. Here, we combine experimental, computational, and analytical approaches to study a thermo-responsive hydrogel adhesive. Experimentally, we show that the adhesion and mechanical properties of a stimuli-responsive hydrogel adhesive are both enhanced by the application of a stimulus. Our analysis further reveals that the enhanced adhesion stems from the increased fracture energy of the bulk hydrogel and the insignificant residual stress on the adhesive–tissue interface. This study presents a framework for designing stimuli-responsive hydrogel adhesives based on the modulation of bulk properties and sheds light on the development of smart adhesives with tunable mechanics.

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Utilizing colloidal probe, lateral force microscopy and simultaneous confocal microscopy, combined with finite element analysis, we investigate how a microparticle starts moving laterally on a soft, adhesive surface. We find that the surface can form a self-contacting crease at the leading front, which results from a buildup of compressive stress. Experimentally, creases are observed on substrates that exhibit either high or low adhesion when measured in the normal direction, motivating the use of simulations to consider the role of adhesion energy and interfacial strength. Our simulations illustrate that the interfacial strength plays a dominating role in the nucleation of a crease. After the crease forms, it progresses through the contact zone in a Schallamach wave-like fashion. Interestingly, our results suggest that this Schallamach wave-like motion is facilitated by free slip at the adhesive, self-contacting interface within the crease.