Structure and Strength at Immiscible Polymer Interfaces

Abstract: Thermal welding of polymer-polymer interfaces is important for integrating polymeric elements into devices. When two different polymers are joined, the strength of the weld depends critically on the degree of immiscibility. We perform large-scale molecular dynamics simulations of the structure-strength relation at immiscible polymer interfaces. Our simulations show that immiscibility arrests interdiffusion and limits the equilibrium interfacial width. Even for weakly immiscible films, the narrow interface is unable to transfer stress upon deformation as effectively as the bulk material, and chain pullout at the interface becomes the dominant failure mechanism. This greatly reduces the interfacial strength. The weak response of immiscible interfaces is shown to arise from an insufficient density of entanglements across the interface. We demonstrate that there is a threshold interfacial width below which no significant entanglements can form between opposite sides to strengthen the interface.