Flow birefringence study of sharkskin and stress relaxation in polybutadiene melts

In this paper we report rheo-optical and rheological observations made through a transparent slit die attached to a capillary rheometer. We find that the flow birefringence signal oscillates periodically near the die exit when sharkskin-like extrudate distortion is present. In contrast, steady behavior is observed in the die inland region. Specifically, the flow birefringence varies at the die exit with a period identical to that measured directly from the sharkskin extrudate. We also show that the exit flow instability leading to sharkskin can be observed directly through cross-polarizers in terms of the temporal change of the retardation order. We demonstrate that the same kind of interfacial flow instability can occur at a boundary discontinuity within the die land where the upper portion of a clean die wall meets the lower portion of a polysiloxane-coated die wall. Finally, stress relaxation upon the cessation of the slit die flow of two polybutadiene melts is studied through time-dependent flow birefringence measurements. The stress relaxation is then correlated with sharkskin time scales to describe the role of relaxation in sharkskin ridge formation.