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Nonlinear extensional flows are common in polymer processing, but they remain challenging theoretically because dramatic stretching of chains deforms the entanglement network far from equilibrium. Here, we present coarse-grained simulations of extensional flows in entangled polymer melts for Rouse-Weissenberg numbers Wiₑ=0. 06-52 and Hencky strains ε≥6. Simulations reproduce experimental trends in extensional viscosity with time, rate, and molecular weight. Studies of molecular structure reveal an elongation and thinning of the confining tube with increasing Wiₑ. The rising stress is quantitatively consistent with the decreasing entropy of chains at the equilibrium entanglement length. Molecular weight dependent trends in viscosity are related to a crossover from the Newtonian limit to a high rate limit that scales differently with chain length.
O’Connor et al. (Thu,) studied this question.