Long-range movement of large mechanically interlocked DNA nanostructures

Area of Science:

• Supramolecular Chemistry
• Nanotechnology
• Molecular Engineering

Background:

• Interlocked molecules like catenanes and rotaxanes, linked by mechanical bonds, enable large-scale movements.
• These properties make them promising for building artificial molecular machines and motors.

Purpose of the Study:

• To demonstrate the creation of large, rigid rotaxane structures using DNA origami.
• To enable modification of these structures for cargo or nanoparticle attachment.
• To develop a mechanism for controlling the movement of these DNA-based rotaxanes.

Main Methods:

• Utilizing DNA origami subunits to construct large, rigid rotaxane architectures.
• Employing multiple axle modules to achieve extended rotaxane lengths (up to 355 nm).
• Implementing a fuel/anti-fuel system to switch rotaxanes between mobile and fixed states.
• Creating extended pseudo-rotaxanes with DNA origami rings sliding along DNA filaments.
• Utilizing atomic force microscopy (AFM) for active movement and tracking of DNA origami rings.

Main Results:

• Successfully realized large, rigid rotaxane structures from DNA origami.
• Demonstrated the ability to functionalize these structures with molecular cargo or nanoparticles.
• Achieved rotaxane constructs with axle lengths up to 355 nm.
• Developed a fuel/anti-fuel mechanism to control the mobile/fixed states of the rotaxanes.
• Created pseudo-rotaxanes where rings slide over hundreds of nanometers along DNA filaments.
• Showcased active movement and AFM tracking of the sliding origami rings.

Conclusions:

• DNA origami provides a versatile platform for constructing complex, mechanically interlocked molecules.
• The developed fuel-based switching mechanism offers precise control over molecular machine states.
• These DNA-based rotaxanes and pseudo-rotaxanes represent significant advancements in nanoscale engineering and artificial molecular machines.