Self-assembly and cooperative dynamics of a model colloidal gel network

Abstract: We study the assembly into a gel network of colloidal particles, via effective interactions that yield local rigidity and make dilute network structures mechanically stable. The self-assembly process can be described by a Flory-Huggins theory, until a network of chains forms, whose mesh size is on the order of, or smaller than, the persistence length of the chains. The localization of the particles in the network, akin to some extent to caging in dense glasses, is determined by the network topology, and the network restructuring, which takes place via bond breaking and recombination, is characterized by highly cooperative dynamics. We use NVE and NVT Molecular Dynamics as well as Langevin Dynamics and find a qualitatively similar time dependence of time correlations and of the dynamical susceptibility of the restructuring gel. This confirms that the cooperative dynamics emerge from the mesoscale organization of the network.