An Experimental Investigation of Viscoelastic Flow in a Contraction Channel

In order to assess the predictive capability of the S–MDCPP model, which may describe the viscoelastic behavior of the low-density polyethylene melts, a planar contraction flow benchmark problem is calculated in this investigation. A pressure-stabilized iterative fractional step algorithm based on the finite increment calculus (FIC) method is adopted to overcome oscillations of the pressure field due to the incompressibility of fluids. The discrete elastic viscous stress splitting (DEVSS) technique in combination with the streamline upwind Petrov-Galerkin (SUPG) method are employed to calculate the viscoelastic flow. The equal low-order finite elements interpolation approximations for velocity-pressure-stress variables can be applied to calculate the viscoelastic contraction flows for LDPE melts. The predicted velocities agree well with the experimental results of particle imagine velocity (PIV) method, and the pattern of principal stress difference calculated by the S-MDCPP model has good agreement with the results measured by the flow induced birefringence (FIB) device. Numerical and experimental results show that the S-MDCPP model is capable of accurately capturing the rheological behaviors of branched polymers in complex flow.

Monodisperse Polymer Melts Crystallize via Structurally Polydisperse Nanoscale Clusters: Insights from Polyethylene

This study demonstrates that monodisperse entangled polymer melts crystallize via the formation of nanoscale nascent polymer crystals (i.e., nuclei) that exhibit substantial variability in terms of their constituent crystalline polymer chain segments (stems). More specifically, large-scale coarse-grain molecular simulations are used to quantify the evolution of stem length distributions and their properties during the formation of polymer nuclei in supercooled prototypical polyethylene melts. Stems can adopt a range of lengths within an individual nucleus (e.g., ∼1–10 nm) while two nuclei of comparable size can have markedly different stem distributions. As such, the attainment of chemically monodisperse polymer specimens is not sufficient to achieve physical uniformity and consistency. Furthermore, stem length distributions and their evolution indicate that polymer crystal nucleation (i.e., the initial emergence of a nascent crystal) is phenomenologically distinct from crystal growth. These results highlight that the tailoring of polymeric materials requires strategies for controlling polymer crystal nucleation and growth at the nanoscale.