Ring polymer dynamics and tumbling-stretch transitions in planar mixed flows.

Abstract

The properties of dilute polymer solutions are governed by the conformational dynamics of individual polymers which can be perturbed in the presence of an applied flow. Much of our understanding of dilute solutions comes from studying how flows manipulate the molecular features of polymer chains out of equilibrium, primarily focusing on linear polymer chains. Recently there has been an emerging interest in the dynamics of nonlinear architectures, particularly ring polymers, which exhibit surprising out-of-equilibrium dynamics in dilute solutions. In particular, it has been observed that hydrodynamics can couple to topology in planar elongational and shear flows, driving molecular expansion in the nonflow direction that is not observed for linear chains. In this paper, we extend our understanding of dilute ring polymer dynamics to mixed flows, which represent flow profiles intermediate between simple shear or planar elongation. We map the conformational behaviors at a number of flow geometries and strengths, demonstrating transitions between coiled, tumbling, and stretched regimes. Indeed, these observations are consistent with how linear chains respond to mixed flows. For both linear and ring polymers, we observe a marked first-order-like transition between tumbling and stretched polymers that we attribute to a dynamic energy barrier between the two states. This manifests as bimodal extension distributions in a narrow range of flow strengths and geometries, with the primary difference between rings and linear chains being the presence of molecular expansion in the vorticity direction.