Stress relaxation in network materials: the contribution of the network

Abstract

Stress relaxation in network materials with permanent crosslinks is due to the transport of fluid within the network (poroelasticity), the viscoelasticity of the matrix and the viscoelasticity of the network. While relaxation associated with the matrix was studied extensively, the contribution of the network remains unexplored. In this work we consider two and three-dimensional stochastic fiber networks with viscoelastic fibers and explore the dependence of stress relaxation on network structure. We observe that relaxation has two regimes – an initial exponential regime, followed by a stretched exponential regime – similar to the situation in other disordered materials. The stretch exponent is a function of density, fiber diameter and the network structure, and has a minimum at the transition between the affine and non-affine regimes of network behavior. The relaxation time constant of the first, exponential regime is similar to the relaxation time constant of individual fibers and is independent of network density and fiber diameter. The relaxation time constant of the second, stretched exponential regime is a weak function of network parameters. The stretched exponential emerges from the heterogeneity of relaxation dynamics on scales comparable with the mesh size, with higher heterogeneity leading to smaller stretch exponents. In composite networks of fibers whose relaxation time constant is selected from a distribution with set mean, the stretch exponent decreases with increasing the coefficient of variation of the fiber time constant distribution. As opposed to thermal glass formers and colloids, in these athermal systems the dynamic heterogeneity is introduced by the network structure and does not evolve during relaxation. While in thermal systems the control parameter is the temperature, in this athermal case the control parameter is a non-dimensional structural parameter which describes the degree of non-affinity of the network.