Spatial correlations of entangled polymer dynamics

Ma, Jihong; Carrillo, Jan Michael; Do, Changwoo; Chen, Wei-Ren; Falus, Peter; Shen, Zhiqiang; Hong, Kunlun; Sumpter, Bobby; Wang, Yangyang

doi:10.1103/PhysRevE.104.024503

Spatial correlations of entangled polymer dynamics

Journal Article · Thu Aug 26 00:00:00 EDT 2021 · Physical Review E

DOI:https://doi.org/10.1103/PhysRevE.104.024503· OSTI ID:1818717

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Univ. of Vermont, Burlington, VT (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Institut Laue-Langevin, Grenoble (France)

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. Furthermore, 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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1818717

Journal Information:: Physical Review E, Journal Name: Physical Review E Journal Issue: 2 Vol. 104; ISSN 2470-0045

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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