Structural criterion for the onset of rigidity in a colloidal gel

Abstract: Identifying the necessary conditions for the onset of rigidity in a gel remains a challenge. It has been suggested that local particle coordination could be used to establish such conditions, but rigid gels occur for various coordination numbers. Combining simulations, oscillatory rheology, and a percolation analysis, for particles where the valence can be controlled, we find that the onset of rigidity coincides with the percolation of particles with three or more bonds, which arises after the connectivity percolation. We show that the rigidity results from an interplay of bonding and non-bonding interactions, providing insight into low-valence colloidal gel rigidity.