Combined Molecular Dynamics Simulation and Rouse Model Analysis of Static and Dynamic Properties of Unentangled Polymer Melts with Different Chain Architectures

Pu Yao; Lu-Kun Feng; Hong-Xia Guo

doi:10.1007/s10118-020-2489-4

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Combined Molecular Dynamics Simulation and Rouse Model Analysis of Static and Dynamic Properties of Unentangled Polymer Melts with Different Chain Architectures

ARTICLE | Updated：2020-09-29

- Combined Molecular Dynamics Simulation and Rouse Model Analysis of Static and Dynamic Properties of Unentangled Polymer Melts with Different Chain Architectures
- Combined Molecular Dynamics Simulation and Rouse Model Analysis of Static and Dynamic Properties of Unentangled Polymer Melts with Different Chain Architectures
- Chinese Journal of Polymer Science 2021年39卷第4期页码：512-524
- Affiliations：
  
  a.Beijing National Laboratory for Molecular Sciences, Joint Laboratory of Polymer Sciences and Materials, State Key Laboratory of Polymer Physics and Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
  b.University of Chinese Academy of Sciences, Beijing 100049, China
- Author bio：
  
  hxguo@iccas.ac.cn
- Funds：
  
  This work was financially supported by the National Natural Science Foundation of China (Nos. 21790343, 21574142, and 21174154) and the National Key Research and Development Program of China (No. 2016YFB1100800).
- DOI：10.1007/s10118-020-2489-4
  中图分类号：
- 收稿：2020-07-18，
  
  修回：2020-7-28，
  
  录用：2020-7-31，
  
  网络首发：2020-09-29，
  
  纸质出版：2021-01-01
- Accepted：
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Yao, P.; Feng, L. K.; Guo, H. X. Combined molecular dynamics simulation and rouse model analysis of static and dynamic properties of unentangled polymer melts with different chain architectures. Chinese J. Polym. Sci. 2021, 39, 512–524

Pu Yao, Lu-Kun Feng, Hong-Xia Guo. Combined Molecular Dynamics Simulation and Rouse Model Analysis of Static and Dynamic Properties of Unentangled Polymer Melts with Different Chain Architectures[J]. Chinese Journal of Polymer Science, 2021, 39(4): 512-524.
Yao, P.; Feng, L. K.; Guo, H. X. Combined molecular dynamics simulation and rouse model analysis of static and dynamic properties of unentangled polymer melts with different chain architectures. Chinese J. Polym. Sci. 2021, 39, 512–524 DOI： 10.1007/s10118-020-2489-4.

Pu Yao, Lu-Kun Feng, Hong-Xia Guo. Combined Molecular Dynamics Simulation and Rouse Model Analysis of Static and Dynamic Properties of Unentangled Polymer Melts with Different Chain Architectures[J]. Chinese Journal of Polymer Science, 2021, 39(4): 512-524. DOI： 10.1007/s10118-020-2489-4.

摘要

Abstract

Chain architecture effect on static and dynamic properties of unentangled polymers is explored by molecular dynamics simulation and Rouse mode analysis based on graph theory. For open chains

although they generally obey ideal scaling in chain dimensions

local structure exhibits nonideal behavior due to the incomplete excluded volume (EV) screening

the reduced mean square internal distance (MSID) can be well described by Wittmer’ theory for linear chains and the resulting chain swelling is architecture dependent

i.e

the more branches a bit stronger swelling. For rings

unlike open chains they are compact in term of global sizes. Due to EV effect and nonconcatenated constraints their local structure exhibits a quite different non-Gaussian behavior from open chains

i.e

reduced MSID curves do not collapse to a single master curve and fail to converge to a chain-length-independent constant

which makes the direct application of Wittmer’s theory to rings quite questionable. Deviation from ideality is further evidenced by limited applicability of Rouse prediction to mode amplitude and relaxation time at high modes as well as the non-constant and mode-dependent scaled Rouse mode amplitudes

while the latter is architecture-dependent and even molecular weight dependent for rings. The chain relaxation time is architecture-dependent

but the same scaling dependence on chain dimensions does hold for all studied architectures. Despite mode orthogonality at static state

the role of cross-correlation in orientation relaxation increases with time and the time-dependent coupling parameter rises faster for rings than open chains even at short time scales it is lower for rings.

关键词

Keywords

references

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