Entangled polymer melts exhibit a variety of flow instabilities that limit production rates in industrial applications. We present both experimental and computational findings, using flow of monodisperse linear polystyrenes in a contraction-expansion geometry, which illustrate the formation and development of one such flow instability. This viscoelastic disturbance is first observed at the slit outlet and subsequently produces large-scale fluid motions upstream. A numerical linear stability study using the molecular structure based Rolie-Poly model confirms the instability and identifies important parameters within the model, which gives physical insight into the underlying mechanism. Chain stretch was found to play a critical role in the instability mechanism, which partially explains the effectiveness of introducing a low-molecular weight tail into a polymer blend to increase its processability. There are numerous types of experimentally observed instability in polymer melt flow; a recent review [1] highlights three forms observed in extrusion that occur at increasing rates of flow. The first two are "sharkskin" instabilities, which develop due to free surface effects, and "stick-spurt" or "stick-slip" instabilities, which result from material compression and stick-slip at the wall. While the mechanisms underlying the formation of these first two are relatively well understood [2,3], the third class, termed "volume instability", is less so [4]. This instability in converging flows for extrusion and injection moulding has been known for many years, and an empiricism has been developed. But as yet there is no understanding of the underlying physics of the problem, and the inherent connection between the viscoelastic instability and the molecular polymer dynamics. Understanding the underlying physical process would greatly enhance industry's ability to define efficient processing conditions. This letter outlines recent work in which we created an idealised model flow, related to the engineering flows in that the essential elements are present, but simplified so that the experimental variables are well-controlled and so the whole flow field can be modelled. We have use molecularly well-characterised materials (building on previous work for monodisperse materials under tightly controlled flow conditions [5,6]) so that the connection between viscoelastic properties and molecular structure can be maintained without empirical fitting. Through these careful *