Comparative investigations of surface instabilities (sharkskin) of a linear and a long-chain branched polyethylene

An experimental study of the physical origin and the mechanisms of the sharkskin instability is presented. Extrusion flows through a slit die are studied for two materials: a linear low density polyethylene (LLDPE) which exhibits sharkskin instability for flow rates larger than an onset value and a low density polyethylene (LDPE) which does not show any instability over a broad range of flow rates. By combining laser-Doppler velocimetry (LDV) with rheological measurements in both uniaxial extension and shear, the distributions of tensile and shear stresses in extrusion flows are measured for both materials. The experimentally measured flow fields appear to be qualitatively similar for both the unstable (LLDPE) and stable case (LDPE): around the die exit the flow accelerates near the boundaries and decelerates around the flow axis. The fields of the axial gradients of the axial velocity component are, however, quite different in the two cases. In the unstable case there exists a strongly non-uniform transversal distribution of velocity gradients near the die exit. This non-uniformity of the distribution of gradients is significantly smaller in the stable case. Significant differences in the extensional rheological properties of the two materials are found as well. Due to its branched structure, the LDPE is able to sustain higher tensile stresses prior to failure. Measurements of the distributions of tensile stresses around the die exit reveal a stress boundary layer and a stress imbalance between the boundaries and the bulk. The magnitude of the stress imbalance exceeds the melt strength in the experiments with the LLDPE which causes the failure of the material in the superficial layers and results in the emergence of the sharkskin instability. In the experiments with the LOPE, the magnitude of the stress imbalance remains smaller than the melt strength which explains the lack of an instability. The measured shear stresses around the die exit are significantly smaller than the tensile stresses, suggesting that the shear component of the flow plays no significant role in the emergence of the sharkskin instability. (C) 2010 Elsevier B.V. All rights reserved.