On the role of the filament length distribution in the mechanics of semiflexible networks

This paper explores the effects of filament length polydispersity on the mechanical properties of semiflexible crosslinked polymer networks. Extending previous studies on monodisperse networks, we compute numerically the response of crosslinked networks of elastic filaments of bimodal and exponential length distributions. These polydisperse networks are subject to the same affine to nonaffine (A/NA) transition observed previously for monodisperse networks, wherein the decreases in either crosslink density or bending stiffness lead to a shift from affine, stretching-dominated deformations to nonaffine, bending-dominated deformations. We find that the onset of this transition is generally more sensitive to changes in the density of longer filaments than shorter filaments, meaning that longer filaments have greater mechanical efficiency. Moreover, in polydisperse networks, mixtures of long and short filaments interact cooperatively to generally produce a nonaffine mechanical response closer to the affine prediction than comparable monodisperse networks of either long or short filaments. Accordingly, the mechanical affinity of polydisperse networks is dependent on the filament length composition. Overall, length polydispersity has the effect of sharpening and shifting the A/NA transition to lower network densities. We discuss the implications of these results on experimental observation of the A/NA transition, and on the design of advanced materials.