Microscopic Picture of Cooperative Processes in Restructuring Gel Networks

Colloidal gel networks are disordered elastic solids that can form even in extremely dilute particle suspensions. With interaction strengths comparable to the thermal energy, their stress-bearing network can locally restructure via breaking and reforming interparticle bonds. This allows for yielding, self-healing, and adaptive mechanics under deformation. Designing such features requires controlling stress transmission through the complex structure of the gel and this is challenging because the link between local restructuring and overall response of the network is still missing. Here, we use a space resolved analysis of dynamical processes and numerical simulations of a model gel to gain insight into this link. We show that consequences of local bond breaking propagate along the gel network over distances larger than the average mesh size. This provides the missing microscopic explanation for why nonlocal constitutive relations are necessary to rationalize the nontrivial mechanical response of colloidal gels.

Stress localization, stiffening and yielding in a model colloidal gel

We use numerical simulations and an athermal quasi-static shear protocol to investigate the yielding of a model colloidal gel. Under increasing deformation, the elastic regime is followed by a significant stiffening before yielding takes place. A space-resolved analysis of deformations and stresses unravel how the complex load curve observed is the result of stress localization and that the yielding can take place by breaking a very small fraction of the network connections. The stiffening corresponds to the stretching of the network chains, unbent and aligned along the direction of maximum extension. It is characterized by a strong localization of tensile stresses, that triggers the breaking of a few network nodes at around 30% of strain. Increasing deformation favors further breaking but also shear-induced bonding, eventually leading to a large-scale reorganization of the gel structure at the yielding. At low enough shear rates, density and velocity profiles display significant spatial inhomogeneity during yielding in agreement with experimental observations.