Molecular Dynamics Simulations of Short-Chain Branched Bimodal Polyethylene: Topological Characteristics and Mechanical Behavior

Abstract

It has previously been shown that polyethylene (PE) with a bimodal molar mass distribution has a high fracture toughness. Our approach has been to use coarse-grained (CG) molecular dynamics (MD) simulations to investigate the effects of including short-chain branches in the high molar mass fraction of bimodal PE on topological features and mechanical behavior of the material. The CG potentials were derived, validated, and utilized to simulate melt equilibration, cooling, crystallization, and mechanical deformation. Crystallinity, tie chain, and entanglement concentrations were continuously monitored. During crystallization, the branched bimodal systems disentangled to a lesser degree and ended up with a higher entanglement density than the linear bimodal systems simulated in our previous study. The increase in entanglement concentration was proportional to the content of the branched high molar mass fraction. A significantly higher tie chain concentration was obtained in the short-chain branched bimodal s...