Actively Induced Supercoiling Can Slow Down Plasmid Solutions by Trapping the Threading Entanglements

Harnessing the topology of ring polymers as a design motif in functional nanomaterials is becoming a promising direction in the field of soft matter. For example, the ring topology of DNA plasmids prevents the relaxation of excess twist introduced to the polymer, instead yielding helical supercoiled structures. In equilibrium semidilute solutions, tightly supercoiled rings relax faster than their torsionally relaxed counterparts, since the looser conformations of the latter allow for rings to thread through each other and entrain through entanglements. Here we use molecular simulations to explore a nonequilibrium scenario, in which a supercoiling agent, akin to gyrase enzymes, rapidly induces supercoiling in the suspensions of relaxed plasmids. The activity of the agent not only alters the conformational topology from open to branched, but also locks in threaded rings into supramolecular clusters, which relax very slowly. Ultimately, our work shows how the polymer topology under nonequilibrium conditions can be leveraged to tune dynamic behavior of macromolecular systems, suggesting a method to create a class of driven materials vitrified by activity.