Multiple Light Control Mechanisms in ATP-Fueled Non-equilibrium DNA Systems.

Area of Science:

• Biomolecular Engineering
• Supramolecular Chemistry
• Synthetic Biology

Background:

• Fuel-driven self-assemblies offer programmable temporal behavior via reaction networks.
• Existing external control mechanisms for transient behaviors are limited, often relying on light.
• Modulating system components with different wavelengths remains a significant challenge.

Purpose of the Study:

• To introduce light control in ATP-fueled dynamic covalent DNA polymerization systems.
• To demonstrate wavelength-dependent modulation of system components (fuel and building blocks).
• To enable navigation along different trajectories based on light input.

Main Methods:

• Utilized ATP-fueled dynamic covalent DNA polymerization.
• Incorporated an enzymatic reaction network with concurrent ATP-powered ligation and restriction.
• Introduced caged ATP derivatives and caged DNA building blocks for light activation.
• Employed different light wavelengths to control specific components.

Main Results:

• Achieved light-activated fueling of DNA polymerization systems.
• Demonstrated wavelength-dependent self-sorting of structures and behaviors.
• Showcased the ability to transition between different dynamic steady states using specific wavelengths.
• Established the first examples of light control in this type of system.

Conclusions:

• Light control, particularly using different wavelengths, is feasible for complex dynamic covalent DNA systems.
• Caged components provide a versatile platform for external modulation of autonomous materials.
• This work opens avenues for designing sophisticated, wavelength-addressable autonomous materials and systems.