Fracture in elongational flow of two low-density polyethylene melts

Samples of two commercial low-density polyethylene melts were investigated with respect to their fracture behavior in controlled uniaxial extensional flow at constant strain rate in a filament stretching rheometer. In order to assess the possible influence of grain boundaries on fracture, the samples were prepared by three different types of pre-treatment: by compression molding of (1) virgin pellets used as received, (2) pellets homogenized in a twin-screw extruder, and (3) pellets that were milled into powder by cryogenic grinding under liquid nitrogen. The elongational stress growth data were analyzed by the Extended Hierarchical Multi-mode Molecular Stress Function (EHMMSF) model developed by Wagner et al. (Rheol. Acta 61, 281-298 (2022)) for long-chain branched (LCB) polymer melts. The EHMMSF model quantifies the elongational stress growth including the maximum in the elongational viscosity of LDPE melts based solely on the linear-viscoelastic relaxation spectrum and two nonlinear material parameters, the dilution modulus G_D and a characteristic stretch parameter \({\overline{\lambda}}_m\). Within experimental accuracy, model predictions are in excellent agreement with the elongational stress growth data of the two LDPE melts, independent of the preparation method used. At sufficiently high strain rates, the fracture of the polymer filaments was observed and is in general accordance with the entropic fracture criterion implemented in the EHMMSF model. High-speed videography reveals that fracture is preceded by parabolic crack opening, which is characteristic for elastic fracture and which has been observed earlier in filament stretching of monodisperse polystyrene solutions. Here, for the first time, we demonstrate the appearance of a parabolic crack opening in the fracture process of polydisperse long-chain branched polyethylene melts.