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Based on non-equilibrium molecular dynamics simulations of entangled polymer melts, a recent Letter [Phys. Rev. Lett. $textbf{121}$, 047801 (2018), arXiv:1806.09509] claims that the rising extensional stress is quantitatively consistent with the decreasing entropy of chains at the equilibrium entanglement length. We point out that exactly the opposite is true: the intrachain entropic stress arising from individual entanglement strands generally does not agree with the total macroscopic stress. The conclusion of the Letter is based on an incomplete and questionable analysis of a limited range of the simulation trajectory. The opposite conclusion should have been drawn from their data, had they examined the full simulation trajectory in a proper way.
Nonlinear extensional flows are common in polymer processing but remain challenging theoretically because dramatic stretching of chains deforms the entanglement network far from equilibrium. Here, we present coarse-grained simulations of extensional
We present an extensive set of simulation results for the stress relaxation in equilibrium and step-strained bead-spring polymer melts. The data allow us to explore the chain dynamics and the shear relaxation modulus, $G(t)$, into the plateau regime
In addition to the terminal flow (the region I) and the shear thinning (the region II), we discover two new flow regions in capillary flow at the wall stress higher than the plateau modulus of the polymer. The region III violates the empirical Cox-Me
Following the Flory ideality hypothesis intrachain and interchain excluded volume interactions are supposed to compensate each other in dense polymer systems. Multi-chain effects should thus be neglected and polymer conformations may be understood fr
We present an effective and simple multiscale method for equilibrating Kremer Grest model polymer melts of varying stiffness. In our approach, we progressively equilibrate the melt structure above the tube scale, inside the tube and finally at the mo