A Coarse-Grained Molecular Model of Strain-Hardening for Polymers in the Marginally Glassy State

Nayak, Kapileswar; Read, Daniel J.; McLeish, Tom C.B.; Hine, Peter J.; Tassieri, Manlio

Abstract

We have developed a simple bead-spring model, intended to mimic the internal dynamics of individual polymer chains in the region of the glass transition temperature. Entanglement constraints on the chains are approximated by “sliplinks.” We model the chain dynamics using a dynamic Monte Carlo scheme, with a hop acceptance criterion based on the traversal of high energy barriers. We use this to address the recent experiments of Hine et al., which investigated the effects of melt processing on stress-strain behavior. Polystyrene samples were stretched, annealed at constant length for various times, then either subjected to shrinkage tests or further stress-strain tests. Our model reproduces, at a qualitative level, the observations of Hine et al. It indicates that whilst the initial (weak) strain hardening involves deformation of chain subunits smaller than the entanglement length, the transition to stronger strain hardening involves the “pulling tight” of a small fraction of chain strands trapped in between entanglements. The insights gained suggest a route towards development of molecular-based constitutive models for strain hardening in the glassy state, and specifically the effect of melt processing.

Citation

Nayak, K., Read, D. J., McLeish, T. C., Hine, P. J., & Tassieri, M. (2011). A Coarse-Grained Molecular Model of Strain-Hardening for Polymers in the Marginally Glassy State. Journal of Polymer Science Part B: Polymer Physics, 49(13), 920-938. https://doi.org/10.1002/polb.22263

• Journal Article Type: Article
• Publication Date: Jul 1, 2011
• Deposit Date: Oct 31, 2011
• Journal: Journal of Polymer Science Part B: Polymer Physics
• Print ISSN: 0887-6266
• Electronic ISSN: 1099-0488
• Publisher: Wiley
• Peer Reviewed: Peer Reviewed
• Volume: 49
• Issue: 13
• Pages: 920-938
• DOI: https://doi.org/10.1002/polb.22263
• Keywords: Drawing, Glass, Simulations, Strain-hardening, Stress.
• Public URL: https://durham-repository.worktribe.com/output/1504136