Topological digestion drives time-varying rheology of entangled DNA fluids

Abstract

Understanding and controlling the rheology of polymeric fluids that are out-of-equilibrium is a fundamental problem in biology and industry. For example, to package, repair, and replicate DNA, cells use enzymes to constantly manipulate DNA topology, length, and structure. Inspired by this impressive feat, we combine experiments with theory and simulations to show that complex fluids of entangled DNA display a rich range of non-equilibrium material properties when undergoing enzymatic reactions that alter their topology and size. We reveal that while enzymatically-active fluids of linear DNA display universal viscous thinning, circular DNA fluids - undergoing the same non-equilibrium process - display thickening with a rate and degree that can be tuned by the DNA and enzyme concentrations. Our results open the way for the topological functionalization of DNA-based materials via naturally occurring enzymes to create a new class of "topologically-active" materials that can autonomously alter their rheological properties in a programmable manner.