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缠结管内高度缠结线性聚合物的协同动力学

Cooperative Dynamics of Highly Entangled Linear Polymers within the Entanglement Tube.

作者信息

Kruteva Margarita, Allgaier Jürgen, Monkenbusch Michael, Valiullin Rustem, Hoffmann Ingo, Richter Dieter

机构信息

Jülich Centre for Neutron Science (JCNS-1) and Institute for Biological Information Processing (IBI-8), Forschungszentrum Jülich GmbH, 52428 Jülich, Germany.

Felix Bloch Institute for Solid State Physics, Leipzig University, 04103 Leipzig, Germany.

出版信息

ACS Macro Lett. 2024 Mar 19;13(3):335-340. doi: 10.1021/acsmacrolett.3c00738. Epub 2024 Mar 1.

DOI:10.1021/acsmacrolett.3c00738
PMID:38427591
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10956489/
Abstract

We present a quantitative comparison of the dynamic structure factors from unentangled and strongly entangled poly(butylene oxide) (PBO) melts. As expected, the low molecular weight PBO displays Rouse dynamics, however, with very significant subdiffusive center-of-mass diffusion. The spectra from high molecular weight entangled PBO can be very well described by the dynamic structure factor based on the concept of local reptation, including the Rouse dynamics within the tube and allowing for non-Gaussian corrections. Comparing quantitatively the spectra from both polymers leads to the surprising result that their spectra differ only by the contribution of classical Rouse diffusion for the low molecular weight melt. The subdiffusive component is common for both the low and high molecular weight PBO melts, indicating that in both melts the same interchain potential is active, thereby supporting the validity of the Generalized Langevin Equation approach.

摘要

我们对未缠结和强缠结的聚环氧丁烷（PBO）熔体的动态结构因子进行了定量比较。正如预期的那样，低分子量的PBO呈现出Rouse动力学，然而，其质心扩散具有非常显著的亚扩散特性。基于局部蠕动概念的动态结构因子能够很好地描述高分子量缠结PBO的光谱，包括管内的Rouse动力学并考虑了非高斯校正。对两种聚合物的光谱进行定量比较得出了令人惊讶的结果：它们的光谱仅在低分子量熔体的经典Rouse扩散贡献方面存在差异。低分子量和高分子量PBO熔体都存在亚扩散成分，这表明在两种熔体中相同的链间势是活跃的，从而支持了广义朗之万方程方法的有效性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e16e/10956489/81fec84cce10/mz3c00738_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e16e/10956489/dc7d69580299/mz3c00738_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e16e/10956489/37375130e9c5/mz3c00738_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e16e/10956489/e8f5fcee5494/mz3c00738_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e16e/10956489/a66a4062b31d/mz3c00738_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e16e/10956489/81fec84cce10/mz3c00738_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e16e/10956489/dc7d69580299/mz3c00738_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e16e/10956489/37375130e9c5/mz3c00738_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e16e/10956489/e8f5fcee5494/mz3c00738_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e16e/10956489/a66a4062b31d/mz3c00738_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e16e/10956489/81fec84cce10/mz3c00738_0005.jpg

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本文引用的文献

1
Dynamic structure factors of polymer melts as observed by neutron spin echo: Direct comparison and reevaluation.通过中子自旋回波观察到的聚合物熔体的动态结构因子：直接比较和重新评估。
J Chem Phys. 2023 Jul 21;159(3). doi: 10.1063/5.0150811.
2
Chain Confinement and Anomalous Diffusion in the Cross over Regime between Rouse and Reptation.链约束和重排与蠕动之间转变区的异常扩散。
ACS Macro Lett. 2022 Dec 20;11(12):1343-1348. doi: 10.1021/acsmacrolett.2c00608. Epub 2022 Nov 21.
3
Anomalous Dynamics in Macromolecular Liquids.
Polymers (Basel). 2022 Feb 22;14(5):856. doi: 10.3390/polym14050856.
4
Cooperative Chain Dynamics of Tracer Chains in Highly Entangled Polyethylene Melts.高度缠结聚乙烯熔体中示踪链的协同链动力学
Phys Rev Lett. 2021 May 7;126(18):187801. doi: 10.1103/PhysRevLett.126.187801.
5
Localization of chain dynamics in entangled polymer melts.缠结聚合物熔体中链动力学的定位
Phys Rev E Stat Nonlin Soft Matter Phys. 2014 May;89(5):052603. doi: 10.1103/PhysRevE.89.052603. Epub 2014 May 27.
6
Cooperative dynamics in homopolymer melts: a comparison of theoretical predictions with neutron spin echo experiments.均聚物熔体中的协同动力学：理论预测与中子自旋回波实验的比较。
J Phys Chem B. 2008 Dec 18;112(50):16220-9. doi: 10.1021/jp807035z.
7
Cooperative dynamics in unentangled polymer fluids.非缠结聚合物流体中的协同动力学。
Phys Rev Lett. 2002 Jan 14;88(2):025901. doi: 10.1103/PhysRevLett.88.025901. Epub 2001 Dec 21.