TY - JOUR

T1 - Mode-coupling theory of entangled polymer fluids

AU - Schweizer, Kenneth S.

AU - Szamel, Grzegorz

N1 - Funding Information:
We thank G.Agrawa1, J.F.Douglas, N.Fatkullin, G.Fleischer, M.Fuchs, F.Fujara, S.Granick, C.J.Grayce, G.S.Grest, M.F.Herman, K.Kawasaki, R.Kimmich, H.H.Winter, and R.P.Wool for helpful discussions andlor correspondence. We are grateful to Dr. C. Singh for preparing Figure 1. This work was supported in part by the U.S. National Science Foundation through the Materials Research Laboratory at the University of Illinois via grant NSF-DMR-89-20538 and by the U. S. Department of Energy via Sandia National Laboratories CRADA # 1078.

PY - 1995/7/1

Y1 - 1995/7/1

N2 - A microscopic mode-coupling theory of entangled linear chain polymer melts and solutions has been developed. Coupled generalized Langevin equations of motion for the segments of a tagged polymer are derived and two new fluctuating cage forces emerge associated with intermolecular excluded volume and chain connectivity. In the long chain limit the theory analytically predicts the emergence of a plateau shear modulus, anomalous diffusion and relaxation, self-similiar viscoelastic repsonse, and molecular weight and polymer density dependent renormalization of transport coefficients. These predictions are in general accord with experiments. Crossover from bare Rouse dynamics to entangled behavior, and the significant corrections due to finite chain lengths, are both addressed. Analogies with critical slowing down and the ideal dynamical glass transition, and connections with the phenomenological reptation/tube approach, are discussed.

AB - A microscopic mode-coupling theory of entangled linear chain polymer melts and solutions has been developed. Coupled generalized Langevin equations of motion for the segments of a tagged polymer are derived and two new fluctuating cage forces emerge associated with intermolecular excluded volume and chain connectivity. In the long chain limit the theory analytically predicts the emergence of a plateau shear modulus, anomalous diffusion and relaxation, self-similiar viscoelastic repsonse, and molecular weight and polymer density dependent renormalization of transport coefficients. These predictions are in general accord with experiments. Crossover from bare Rouse dynamics to entangled behavior, and the significant corrections due to finite chain lengths, are both addressed. Analogies with critical slowing down and the ideal dynamical glass transition, and connections with the phenomenological reptation/tube approach, are discussed.

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U2 - 10.1080/00411459508203941

DO - 10.1080/00411459508203941

M3 - Article

AN - SCOPUS:84972876900

SN - 0041-1450

VL - 24

SP - 947

EP - 977

JO - Transport Theory and Statistical Physics

JF - Transport Theory and Statistical Physics

IS - 6-8

ER -