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Brachiation of a polymer chain in the presence of a dynamic network

Pamela C. Cai, Brad A. Krajina, and Andrew J. Spakowitz
Phys. Rev. E 102, 020501(R) – Published 6 August 2020

Abstract

The viscoelastic behavior of a physically crosslinked gel involves a spectrum of molecular relaxation processes, which at the single-chain level involve the chain undergoing transient hand-to-hand motion through the network. We develop a self-consistent theory for describing transiently associating polymer solutions that captures these complex dynamics. A single polymer chain transiently binds to a viscoelastic background that represents the polymer network formed by surrounding polymer chains. The viscoelastic background is described in the equation of motion as a memory kernel, which is self-consistently determined based on the predicted rheological behavior from the chain itself. The solution to the memory kernel is translated into rheological predictions of the complex modulus over a wide range of frequencies to capture the time-dependent behavior of a physical gel. Using the loss tangent predictions, a phase diagram is shown for the sol-gel transition of polymers with dynamic association affinities. This theory provides a predictive, molecular-level framework for the design of associating gels and supramolecular assemblies with targeted rheological properties.

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  • Received 2 March 2020
  • Accepted 8 July 2020

DOI:https://doi.org/10.1103/PhysRevE.102.020501

©2020 American Physical Society

Physics Subject Headings (PhySH)

Polymers & Soft Matter

Authors & Affiliations

Pamela C. Cai1, Brad A. Krajina1, and Andrew J. Spakowitz1,2,3,4

  • 1Department of Chemical Engineering, Stanford University, Stanford, California 94305, USA
  • 2Department of Materials Science, Stanford University, Stanford, California 94305, USA
  • 3Department of Applied Physics, Stanford University, Stanford, California 94305, USA
  • 4Biophysics Program, Stanford University, Stanford, California 94305, USA

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Issue

Vol. 102, Iss. 2 — August 2020

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