Autonomous and Programmable Reorganization of DNA‐Based Polymers Using Redox Chemistry**

Abstract

AbstractWe demonstrate here a strategy that allows the programmable and autonomous reorganization of self‐assembled DNA polymers using redox chemistry. We have rationally designed different DNA monomers (tiles) that can co‐assemble into tubular structures. The tiles can be orthogonally activated/deactivated with disulfide‐linked DNA fuel strands that are degraded over time upon reduction because of the presence of a reducing agent in the system. The concentration of the disulfide fuels determines the activation kinetics of each DNA tile, which controls the degree of order/disorder in the formed co‐polymer. The disulfide‐reduction pathway can be employed together with enzymatic fuel‐degradation pathways providing an additional level of control in the re‐organization of DNA structures. Taking advantage of the different pH‐sensitivities of disulfide‐thiol and enzymatic reactions, we show that we can control the order in DNA‐based co‐polymers as a function of pH.