This article describes a systematic investigation of a discontinuous interfacial stick-slip transition (SST) in simple shear of monodisperse entangled 1,4-polybutadiene (PBD) and polyisoprene (PIP) melts with different molecular weights and architecture, using a specially designed controlled-force shear rheometer. The magnitude of the transition is found to be determined by the level of chain entanglement. Specifically, the dependence of extrapolation length b on molecular weight as b similar to M-w(3.4) and of the melt viscosity as b similar to eta is consistent with the observations based on capillary rheometric studies [X. Yang et al., Rheol. Acta 37, 415-423 (1998)]. The interfacial nature of the flow behavior is explicitly demonstrated by a surface treatment of the shearing plates and dependence of the abrupt increase of the apparent shear rate on the gap distance as well as by particle tracking velocimetry. The critical stress for different molecular weights of PBD and PIP is about 0.2 and 0.1 MPa, respectively, independent of molecular weight and architecture. These results are consistent with the previous conclusion of an interfacial SST as the origin of the discontinuous spurt flow behavior observed with pressure-driven capillary rheometry. The critical stress for the SST is found to be lower in simple shear flow. Finally, chain architecture is observed to also influence the magnitude of the SST apart from the level of chain entanglement. (c) 2006 The Society of Rheology.
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