Onset of criticality in hyper-auxetic polymer networks

Abstract: Against common sense, auxetic materials expand or contract perpendicularly when stretched or compressed, respectively, by uniaxial strain, being characterized by a negative Poisson's ratio $\nu$. The amount of deformation in response to the applied force can be at most equal to the imposed one, so that $\nu=-1$ is the lowest bound for the mechanical stability of solids, a condition here defined as "hyper-auxeticity". In this work, we numerically show that ultra-low-crosslinked polymer networks under tension display hyper-auxetic behavior at a finite crosslinker concentration. At this point, the nearby mechanical instability triggers the onset of a critical-like transition between two states of different densities. This phenomenon displays similar features as well as important differences with respect to gas-liquid phase separation. Since our model is able to faithfully describe real-world hydrogels, the present results can be readily tested in laboratory experiments, paving the way to explore this unconventional phase behavior.