Viscoelasticity of 3D actin networks dictated by the mechanochemical characteristics of cross-linkers

In this study, we report a computational investigation on how the mechanochemical characteristics of crosslinking molecules influence the viscoelasticity of three dimensional F-actin networks, an issue of key interest in analyzing the behavior of living cells and biological gels. In particular, it was found that the continuous breakage and rebinding of cross-linkers result in a locally peaked loss modulus in the rheology spectrum of the network, reflecting the fact that maximum energy dissipation is achieved when the driving frequency of the applied oscillating shear becomes comparable to the dissociation/association rate of crosslinking molecules. In addition, we showed that when subjected to constant rate of shear, an actin network can exhibit either strain hardening or softening depending on the ratio between the loading rate and unbinding speed of cross-linkers. A criterion for predicting the transition from softening to hardening was also obtained, in agreement with recent experiments. Finally, significant structural evolution was found to occur in random networks undergoing mechanical "training" (i.e. under a constant applied shear stress over a period of time), eventually leading to a pronounced anisotropic response of the network afterward which again is consistent with experimental observations.