Decoding polymer self-dynamics using a two-step approach

Zhiqiang Shen, Jan-Michael Y. Carrillo, Bobby G. Sumpter, and Yangyang Wang
Phys. Rev. E 106, 014502 – Published 11 July 2022

Abstract

The self-correlation function and corresponding self-intermediate scattering function in Fourier space are important quantities for describing the molecular motions of liquids. This work draws attention to a largely overlooked issue concerning the analysis of these space-time density-density correlation functions of polymers. We show that the interpretation of non-Gaussian behavior of polymers is generally complicated by intrachain averaging of distinct self-dynamics of different segments. By the very nature of the mathematics involved, the averaging process not only conceals critical dynamical information, but also contributes to the observed non-Gaussian dynamics. To fully expose this issue and provide a thorough benchmark of polymer self-dynamics, we perform analyses of coarse-grained molecular dynamics simulations of linear and ring polymer melts as well as several theoretical models using a “two-step” approach, where interchain and intrachain averagings of segmental self-dynamics are separated. While past investigations primarily focused on the average behavior, our results indicate that a more nuanced approach to polymer self-dynamics is clearly required.

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  • Received 19 April 2022
  • Accepted 22 June 2022

DOI:https://doi.org/10.1103/PhysRevE.106.014502

©2022 American Physical Society

Physics Subject Headings (PhySH)

  1. Research Areas
  1. Physical Systems
Polymers & Soft Matter

Authors & Affiliations

Zhiqiang Shen, Jan-Michael Y. Carrillo, Bobby G. Sumpter, and Yangyang Wang*

  • Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA

  • *wangy@ornl.gov

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Issue

Vol. 106, Iss. 1 — July 2022

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