Understanding Mass Dependence of Glass Formation in Ring Polymers

Xiang-Yu Song; Zhen-Yue Yang; Qi-Lu Yuan; Shang-Wei Li; Zi-Qiang Tang; Yue-Tong Dong; Shi-Chun Jiang; Wen-Sheng Xu

doi:10.1007/s10118-023-3004-5

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Understanding Mass Dependence of Glass Formation in Ring Polymers

RESEARCH ARTICLE | Updated：2023-08-24

- Understanding Mass Dependence of Glass Formation in Ring Polymers
- Understanding Mass Dependence of Glass Formation in Ring Polymers
- 高分子科学（英文版） 2023年41卷第9期页码：1447-1461
- Affiliations：
  
  a.State Key Laboratory of Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
  b.School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China
  c.School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
- Author bio：
  
  scjiang@tju.edu.cn (S.C.J.)
  wsxu@ciac.ac.cn (W.S.X.)
- Funds：
  
  This work was financially supported by the National Natural Science Foundation of China (Nos. 22222307 and 21973089).
- DOI：10.1007/s10118-023-3004-5
  中图分类号：
- 收稿：2023-04-09，
  
  修回：2023-4-29，
  
  录用：2023-5-16，
  
  网络首发：2023-07-05，
  
  纸质出版：2023-09-01
- Accepted：
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Song, X. Y.; Yang, Z. Y.; Yuan, Q. L.; Li, S. W.; Tang, Z. Q.; Dong, Y. T.; Jiang, S. C.; Xu, W. S. Understanding mass dependence of glass formation in ring polymers. Chinese J. Polym. Sci. 2023, 41, 1447–1461

Xiang-Yu Song, Zhen-Yue Yang, Qi-Lu Yuan, et al. Understanding Mass Dependence of Glass Formation in Ring Polymers[J]. Chinese Journal of Polymer Science, 2023, 41(9): 1447-1461.
Song, X. Y.; Yang, Z. Y.; Yuan, Q. L.; Li, S. W.; Tang, Z. Q.; Dong, Y. T.; Jiang, S. C.; Xu, W. S. Understanding mass dependence of glass formation in ring polymers. Chinese J. Polym. Sci. 2023, 41, 1447–1461 DOI： 10.1007/s10118-023-3004-5.

Xiang-Yu Song, Zhen-Yue Yang, Qi-Lu Yuan, et al. Understanding Mass Dependence of Glass Formation in Ring Polymers[J]. Chinese Journal of Polymer Science, 2023, 41(9): 1447-1461. DOI： 10.1007/s10118-023-3004-5.

摘要

The present paper utilizes coarse-grained molecular dynamics simulation to investigate the glass formation of unknotted

nonconcatenated ring and linear polymer melts having variable molecular mass. It is demonstrated that the glass formation of ring polymers can quantitatively be described by the string model of glass formation.

Abstract

Having highly tunable molecular topology is one of the most important characteristics of polymers that provides these materials with a wide range of interesting and unique properties. In particular

ring polymers exhibit a number of properties that are markedly distinct from their linear counterparts. Here

we compare and contrast the glass formation of unknotted

nonconcatenated ring and linear polymer melts having variable molecular mass based on molecular dynamics simulations of a coarse-grained model. After revealing an unusual property in the structure of small rings

we discuss the mass dependence of the structural relaxation time determined from the self-intermediate scattering function over a wide range of temperatures in both ring and linear polymers. As a general trend

we find that the characteristic temperatures (

e.g.

the glass transition temperature) and fragility of glass formation increase with increasing molecular mass in linear polymers

but the mass dependences of these properties are rather weak in the family of ring polymer models considered

in broad accord with experimental measurements. Importantly

we show that the glass formation of ring polymers can quantitatively be described by the string model

a model that is broadly consistent with the entropy theory of glass formation and that takes the mass of string-like clusters as a molecular realization of the abstract cooperatively rearranging regions. This opens the possibility of applying the configurational entropy-based theories to describe the glass formation of ring polymers

once the ring topology is taken into account.

关键词

Keywords

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