Bimodal colloids highlight the structural mirror of rigidity percolation and yielding

Abstract

In metastable particulate gels, it is tempting to believe that the dynamic similarities between the fluid-to-solid non-linear phase transition of rigidity percolation and the solid-to-fluid transition that occurs during yielding represent mirror images of the same continuous process. Even though these behaviors are clearly dynamically similar, their multi-scale nature makes it difficult to determine if they could also follow a unified structural pathway. We know from model monodisperse colloidal gels that both yielding and the elastic modulus seem to be heavily influenced by a small subset of topologically distinct singly-connected bridges linking mesoscale features. Here we use particle simulations to examine the participation of different classes of particle-level bonds and their contributions to the bulk mechanical response. We find that rigidity is disproportionately supported by singly connected intercluster bridges, whereas yielding localizes at bonds with high edge-betweenness centrality (EBC); strikingly, these independently identified populations substantially overlap and perform comparable mechanical roles. Bimodality exposes this correspondence by concentrating large-particle contacts in both populations, thereby providing a compositional label for the common backbone. Thus, rigidity and yielding are opposing mechanical manifestations of the same mesoscale structure: the intercluster bottlenecks that establish rigidity are also the sites at which rigidity is preferentially lost.