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Programmable Dynamic Steady States in ATP-Driven Non-Equilibrium DNA Systems

preprint
submitted on 05.06.2019 and posted on 07.06.2019 by Laura Heinen, Andreas Walther

Inspired by the dynamics of the dissipative self-assembly of microtubules, chemically fueled synthetic systems with transient lifetimes are emerging for non-equilibrium materials design. However, realizing programmable or even adaptive structural dynamics has proven challenging because it requires synchronization of energy uptake and dissipation events within true steady states, which remains difficult to orthogonally control in supramolecular systems. Here, we demonstrate full synchronization of both events by ATP-fueled activation and dynamization of covalent DNA bonds via an enzymatic reaction network of concurrent ligation and cleavage. Critically, the average bond ratio and the frequency of bond exchange are imprinted into the energy dissipation kinetics of the network and tunable through its constituents. We introduce temporally and structurally programmable dynamics by polymerization of transient, dynamic covalent DNA polymers with adaptive steady-state properties in dependence of ATP fuel and enzyme concentrations. This approach enables generic access to non-equilibrium soft matter systems with adaptive and programmable dynamics.

Funding

European Research Council 677960

History

Email Address of Submitting Author

andreas.walther@makro.uni-freiburg.de

Institution

University of Freiburg

Country

Germany

ORCID For Submitting Author

0000-0003-2170-3306

Declaration of Conflict of Interest

no conflict of interests to declare

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