Nonlinear Rheological Behaviors in Polymer Melts after Step Shear
YJ Ruan and YY Lu and LJ An and ZG Wang, MACROMOLECULES, 52, 4103-4110 (2019).
DOI: 10.1021/acs.macromol.9b00392
Using molecular dynamics simulation, we investigate the evolution of chain conformation, stress relaxation, and fracture for a polymer melt between two walls after step shear. We find that the characteristic overlap time for the reduced relaxation moduli and the time that the stretched primitive chain retracts to its equilibrium length are both much longer than the Rouse time. Importantly, we observe significant fracture-like flow after shear cessation. While there is considerable randomness in the location of the fracture plane and the magnitude of displacement from sample to sample, our analysis suggests that the randomness is not due to thermal noise, but may reflect inherent structural and dynamic heterogeneity in the entangled polymer network.
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