Abstract

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.

Highlights

  • Polymer plays an increasingly important role in industry from structural materials such as in the aerospace field to functional materials such as the polymer coating of electrodes [1,2,3,4,5,6,7,8,9,10]

  • Tube model simplifies the dynamics by describing the movement of one single chain in a tube, formed by constraints imposed by surrounding chains [15,16]

  • Masubuchi et al [33] reproduce the probe rheology data reported by Matsumiya et al [30] using primitive chain network (PCN) model, which describes the dynamics of the network formed by the primitive chains and is used extensively in literature [34,35,36,37,38]

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Summary

Introduction

Polymer plays an increasingly important role in industry from structural materials such as in the aerospace field to functional materials such as the polymer coating of electrodes [1,2,3,4,5,6,7,8,9,10]. Masubuchi et al [33] reproduce the probe rheology data reported by Matsumiya et al [30] using primitive chain network (PCN) model, which describes the dynamics of the network formed by the primitive chains and is used extensively in literature [34,35,36,37,38]. Their results agree with the experiment well. Bidisperse melts are simulated and results agree with published experimental data, which validate the ability of this lifetime version model

Model and methodology
Results
The lifetime distribution and application of lifetime version SSp
Conclusion
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