Spatial correlations of entangled polymer dynamics

Jihong Ma, Jan-Michael Y. Carrillo, Changwoo Do, Wei-Ren Chen, Péter Falus, Zhiqiang Shen, Kunlun Hong, Bobby G. Sumpter, and Yangyang Wang
Phys. Rev. E 104, 024503 – Published 26 August 2021

Abstract

The spatial correlations of entangled polymer dynamics are examined by molecular dynamics simulations and neutron spin-echo spectroscopy. Due to the soft nature of topological constraints, the initial spatial decays of intermediate scattering functions of entangled chains are, to the first approximation, surprisingly similar to those of an unentangled system in the functional forms. However, entanglements reveal themselves as a long tail in the reciprocal-space correlations, implying a weak but persistent dynamic localization in real space. Comparison with a number of existing theoretical models of entangled polymers suggests that they cannot fully describe the spatial correlations revealed by simulations and experiments. In particular, the strict one-dimensional diffusion idea of the original tube model is shown to be flawed. The dynamic spatial correlation analysis demonstrated in this work provides a useful tool for interrogating the dynamics of entangled polymers. Lastly, the failure of the investigated models to even qualitatively predict the spatial correlations of collective single-chain density fluctuations points to a possible critical role of incompressibility in polymer melt dynamics.

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  • Received 24 February 2021
  • Accepted 3 August 2021

DOI:https://doi.org/10.1103/PhysRevE.104.024503

©2021 American Physical Society

Physics Subject Headings (PhySH)

Polymers & Soft Matter

Authors & Affiliations

Jihong Ma1,*, Jan-Michael Y. Carrillo1, Changwoo Do2, Wei-Ren Chen2, Péter Falus3, Zhiqiang Shen1, Kunlun Hong1, Bobby G. Sumpter1, and Yangyang Wang1,†

  • 1Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
  • 2Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
  • 3Institut Laue-Langevin, B.P. 156, F-38042 Grenoble CEDEX 9, France

  • *Present address: Department of Mechanical Engineering, University of Vermont, Burlington, Vermont 05405, USA.
  • wangy@ornl.gov

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Vol. 104, Iss. 2 — August 2021

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