The role of crosslinking density in surface stress and surface energy of soft solids*

Surface stress and surface energy are two fundamental parameters that determine the surface properties of any material. While it is commonly believed that the surface stress and surface energy of liquids are identical, the relationship between the two parameters in soft polymeric gels remains debatable. In this work, we measured the surface stress and surface energy of soft silicone gels with varying crosslinking densities in soft wetting experiments. Above a critical crosslink density, $k_0$, the surface stress is found to increase significantly with crosslinking density while the surface energy, by contrast, remains unchanged. In this regime, we can estimate a non-zero surface elastic modulus that also increases with the ratio of crosslinkers. By comparing the surface mechanics of the soft gels to their bulk rheology, the surface properties near the critical density $k_0$ are found to be closely related to the underlying percolation transition of the polymer networks.