Hardening and Softening Materials: the role of network topology in soft gels

The structural complexity of soft gels is at the origin of a versatile mechanical response that allows for large deformation, controlled elastic recovery, and toughness in the same material. A limit to exploiting the potential of such materials is the insufficient fundamental understanding of the microstructural origin of the bulk mechanical properties. Here we investigate the role of the network topology and of frozen-in stresses in a model gel through 3D numerical simulations. Our study links the topology of the network organization in space to the stress redistribution under shear and to its nonlinear rheological response preceding yielding and damage: our analysis elucidates how the network connectivity alone could be used to modify the gel mechanics at large strains, from strain-softening to hardening and even to a brittle response. These findings provide new insight for smart material design and for understanding the nontrivial mechanical response of a potentially wide range of technologically relevant materials.