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Slip-spring simulations of different constraint release environments for linear polymer chains

机译:线性聚合物链的不同约束释放环境的防滑弹簧模拟

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The constraint release (CR) mechanism has important effects on polymer relaxation and the chains will show different relaxation behaviour in conditions of monodisperse, bidisperse and other topological environments. By comparing relaxation data of linear polyisoprene (PI) chains dissolved in very long matrix and monodisperse melts, Matsumiya et al. showed that CR mechanism accelerates both dielectric and viscoelastic relaxation (Matsumiya et al. 2013 Macromolecules 46 , 6067. ( doi:10.1021/ma400606n )). In this work, the experimental data reported by Matsumiya et al. are reproduced using the single slip-spring (SSp) model and the CR accelerating effects on both dielectric and viscoelastic relaxation are validated by simulations. This effect on viscoelastic relaxation is more pronounced. The coincidence for end-to-end relaxation and the viscoelastic relaxation has also been checked using probe version SSp model. A variant of SSp with each entanglement assigning a characteristic lifetime is also proposed to simulate various CR environment flexibly. Using this lifetime version SSp model, the correct relaxation function can be obtained with equal numbers of entanglement destructions by CR and reptation/contour length fluctuation (CLF) for monodisperse melts. Good agreement with published experiment data is also obtained for bidisperse melts, which validates the ability to correctly describe the CR environment of the lifetime version model.
机译:约束释放(CR)机制对聚合物松弛具有重要影响,并且链条将在单分散,双分散和其他拓扑环境条件下显示不同的松弛行为。通过比较溶解在非常长的基质和单分散熔体的线性聚异戊二烯(PI)链的弛豫数据,Matsumiya等。表明CR机制加速了介电和粘弹性松弛(Matsumiya等,2013年MacromoleCules 46,6067.(DOI:10.1021 / MA400606N))。在这项工作中,Matsumiya等人报告的实验数据。使用单滑弹簧(SSP)模型再现,并通过模拟验证了对介质和粘弹性松弛的CR加速效应。这种对粘弹性松弛的影响更加明显。使用探头SSP模型检查了端到端放松和粘弹性松弛的巧合。还提出了分配特征寿命的每个缠模的SSP变体来灵活地模拟各种CR环境。使用这种寿命版本SSP模型,可以通过CR和Reptation / Contour Length Flutumation(CLF)以相同的纠缠破坏来获得正确的弛豫功能,用于单分散熔体。对于出版的实验数据,还获得了良好的协议,用于指标熔体,这验证了正确描述了寿命版本模型的CR环境的能力。

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