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

07 June 2019, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

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.

Keywords

DNA Nanoscience
Active Matter
Autonomous Systems
Dynamic Systems
Systems Chemistry
ATP fueled systems
dynamic covalent bond
non-equilibrium
life-like systems

Supplementary materials

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