Light-Powered, yet Chemically Fueled, Dissipative DNA Systems with Transient Lifecycles

Fuel-driven dissipative self-assemblies are gaining ground for creating life-like, active and adaptive materials with autonomous behavior. However, up to now there is a lack for simple external control mechanisms of the transient behavior of the steady-state properties, at best using high spatiotemporal resolution. Here, we introduce the first examples of an externally controlled, chemically fueled transient self-assembly system that is ultimately powered using different colors of light. We demonstrate this concept for the programming of the transient lifecycle behaviors of ATP-dissipating, enzymatically controlled, dynamic covalent DNA polymerizations using controlled photolysis of properly designed caged ATP derivatives. Multiple uncaging, as well as wavelength-orthogonal activation are achieved by storing caged fuels as latent energy sources inside the system. We anticipate that this approach can be generalize to other ATP-dissipating self-assemblies and other chemical fuels to achieve versatile spatiotemporal control.