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测量环状-线性聚合物共混物中的拓扑约束松弛

Measuring Topological Constraint Relaxation in Ring-Linear Polymer Blends.

作者信息

Vigil Daniel L, Ge Ting, Rubinstein Michael, O'Connor Thomas C, Grest Gary S

机构信息

<a href="https://ror.org/01apwpt12">Sandia National Laboratories</a>, Albuquerque, New Mexico 87185, USA.

Department of Chemistry and Biochemistry, <a href="https://ror.org/02b6qw903">University of South Carolina</a>, Columbia, South Carolina 29208, USA.

出版信息

Phys Rev Lett. 2024 Sep 13;133(11):118101. doi: 10.1103/PhysRevLett.133.118101.

DOI:10.1103/PhysRevLett.133.118101
PMID:39331970
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12057411/
Abstract

Polymers are an effective test bed for studying topological constraints in condensed matter due to a wide array of synthetically available chain topologies. When linear and ring polymers are blended together, emergent rheological properties are observed as the blend can be more viscous than either of the individual components. This emergent behavior arises since ring-linear blends can form long-lived topological constraints as the linear polymers thread the ring polymers. Here, we demonstrate how the Gauss linking integral can be used to efficiently evaluate the relaxation of topological constraints in ring-linear polymer blends. For majority-linear blends, the relaxation rate of topological constraints depends primarily on reptation of the linear polymers, resulting in the diffusive time τ_{d,R} for rings of length N_{R} blended with linear chains of length N_{l} to scale as τ_{d,R}∼N_{R}^{2}N_{L}^{3.4}.

摘要

由于有大量可通过合成获得的链拓扑结构,聚合物是研究凝聚态物质中拓扑约束的有效试验平台。当线性聚合物和环状聚合物混合在一起时,会观察到新出现的流变特性,因为这种混合物可能比任何一种单独的组分更具粘性。这种新出现的行为之所以会出现,是因为当线性聚合物穿过环状聚合物时,环 - 线性聚合物混合物可以形成寿命较长的拓扑约束。在此,我们展示了高斯链环积分可如何用于有效评估环 - 线性聚合物混合物中拓扑约束的弛豫。对于多数为线性的混合物,拓扑约束的弛豫速率主要取决于线性聚合物的蠕动,导致与长度为(N_{l})的线性链混合的长度为(N_{R})的环的扩散时间(\tau_{d,R})按(\tau_{d,R} \sim N_{R}^{2}N_{L}^{3.4})缩放。