A force-level theory of the rheology of entangled rod and chain polymer liquids. I. Tube deformation, microscopic yielding, and the nonlinear elastic limit

Schweizer, Kenneth S.; Sussman, Daniel M.

doi:10.1063/1.4968516

A force-level theory of the rheology of entangled rod and chain polymer liquids. I. Tube deformation, microscopic yielding, and the nonlinear elastic limit

Journal Article · Sun Dec 04 23:00:00 EST 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4968516· OSTI ID:1465673

Schweizer, Kenneth S. ^[1]; Sussman, Daniel M. ^[2]

Univ. of Illinois, Urbana, IL (United States). Dept. of Materials Science. Dept. of Chemistry; Department of Materials Science and Department of Chemistry, University of Illinois, 1304 West Green Street, Urbana, Illinois 61801, USA
Syracuse Univ., NY (United States). Dept. of Physics

In this paper, we employ a first-principles-based, force-level approach to construct the anharmonic tube confinement field for entangled fluids of rigid needles, and also for chains described at the primitive-path (PP) level in two limiting situations where chain stretch is assumed to either be completely equilibrated or unrelaxed. The influence of shear and extensional deformation and polymer orientation is determined in a nonlinear elastic limit where dissipative relaxation processes are intentionally neglected. For needles and PP-level chains, a self-consistent analysis of transverse polymer harmonic dynamical fluctuations predicts that deformation-induced orientation leads to tube weakening or widening. In contrast, for deformed polymers in which chain stretch does not relax, we find tube strengthening or compression. For all three systems, a finite maximum transverse entanglement force localizing the polymers in effective tubes is predicted. The conditions when this entanglement force can be overcome by an externally applied force associated with macroscopic deformation can be crisply defined in the nonlinear elastic limit, and the possibility of a “microscopic absolute yielding” event destroying the tube confinement can be analyzed. For needles and contour-relaxed PP chains, this force imbalance occurs at a stress of order the equilibrium shear modulus and a strain of order unity, corresponding to a mechanically fragile entanglement tube field. However, for unrelaxed stretched chains, tube compression stabilizes transverse polymer confinement, and there appears to be no force imbalance. These results collectively suggest that the crossover from elastic to irreversible viscous response requires chain retraction to initiate disentanglement. Finally, we qualitatively discuss comparisons with existing phenomenological models for nonlinear startup shear, step strain, and creep rheology experiments.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Illinois, Urbana, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: FG02-07ER46471

OSTI ID:: 1465673

Alternate ID(s):: OSTI ID: 1334367

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 21 Vol. 145; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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A force-level theory of the rheology of entangled rod and chain polymer liquids. I. Tube deformation, microscopic yielding, and the nonlinear elastic limit

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