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Abstract 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. 

ABSTRACT Commercial silicone elastomers are commonly used in soft materials research due to their easily tunable mechanical properties. However, conventional polydimethylsiloxane (PDMS) elastomers with moduli below ∼100 kPa contain uncrosslinked free molecules, which play a significant role in their behavior. To utilize these materials, it is important to quantify what role these free molecules play in the mechanical response before and after their removal. We present a simple and inexpensive extraction method that enables the removal of free molecules from a lightly crosslinked sheet of Sylgard 184, a commercially available PDMS elastomer. The materials can contain a majority of free molecules yet maintain a thin and flat geometry without fractures after extraction. Subsequently, we compare the modulus, maximum stretchability, and hysteresis behavior with mixing ratios ranging from 60:1 to 30:1, before and after extraction. We show that the modulus, maximum stretchability, and dissipation increase upon extraction. Moreover, our approach offers a route to prepare crosslinked silicone elastomers with a modulus as low as ∼20 kPa without free molecules from a commercially available kit. © 2020 Wiley Periodicals, Inc. J. Polym. Sci.2020,58, 343–351 

Small scale contact between a soft, liquid-coated layer and a stiff surface is common in many situations, from synovial fluid on articular cartilage to adhesives in humid environments. Moreover, many model studies on soft adhesive contacts are conducted with soft silicone elastomers, which possess uncrosslinked liquid molecules ( i.e. silicone oil) when the modulus is low. We investigate how the thickness of a silicone oil layer on a soft substrate relates to the indentation depth of glass microspheres in contact with crosslinked PDMS, which have a modulus of <10 kPa. The particles indent into the underlying substrate more as a function of decreasing oil layer thickness. This is due to the presence of the liquid layer at the surface that causes capillary forces to pull down on the particle. A simple model that balances the capillary force of the oil layer and the minimal particle–substrate adhesion with the elastic and surface tension forces from the substrate is proposed to predict the particle indentation depth.