Primitive chain network simulations for the interrupted shear response of entangled polymeric liquids

Abstract

The non-linear viscoelastic response under interrupted shear flows is one of the interesting characteristics of entangled polymers. In particular, the stress overshoot in the resumed shear has been discussed concerning the recovery of the entanglement network in some studies. In this study, we performed multichain slip-link simulations to observe the molecular structure of an entangled polymer melt. After confirming the reasonable reproducibility of our simulation with the literature data, we analyzed the molecular characteristics following the decoupling approximation. We reasonably found that the segment orientation dominates the stress overshoot even under the resumed shear with minor contributions from the segment stretch and entanglement density. We defined the mitigation function for the recovery of the stress overshoot as a function of the rest time and compared it with the relaxation of the molecular quantities after the initial shear. As a result, we have found that the mitigation of the stress overshoot coincides with the relaxation of entanglement density.