Long-range movement of large mechanically interlocked DNA nanostructures

Abstract

Interlocked molecules such as catenanes and rotaxanes, connected only via mechanical bonds have the ability to perform large-scale sliding and rotational movements, making them attractive components for the construction of artificial molecular machines and motors. We here demonstrate the realization of large, rigid rotaxane structures composed of DNA origami subunits. The structures can be easily modified to carry a molecular cargo or nanoparticles. By using multiple axle modules, rotaxane constructs are realized with axle lengths of up to 355 nm and a fuel/anti-fuel mechanism is employed to switch the rotaxanes between a mobile and a fixed state. We also create extended pseudo-rotaxanes, in which origami rings can slide along supramolecular DNA filaments over several hundreds of nanometres. The rings can be actively moved and tracked using atomic force microscopy.

DNA Origami Rotaxanes: Tailored Synthesis and Controlled Structure Switching

“…However,the rotaxanes presented here are larger and more rigid than antecedent interlocked DNAn anodevices and harbor great potential for functionalization with am yriad of biomolecule cargos (e.g., proteins) and stimulus-responsive components.Moreover,the modular design and structure-switching properties of the rotaxanes open up new possibilities for producing otherwise entropically unfavorable DNAs tructures and for programmably altering rotaxane geometry and dynamics.S immel and coworkers recently made several multicomponent rotaxanes using adifferent assembly scheme. [13]…”

“…Moreover, the modular design and structural switching properties of the rotaxanes open up new possibilities both for producing otherwise entropically unfavorable DNA structures and for programmably altering rotaxane geometry and dynamics. Simmel et al recently made several multi-component rotaxanes using a different assembly scheme [13] .…”

Fold 2D Woven DNA Origami to Origami+ Structures

“…Since DNA origami strategy was invented in 2006, it has greatly promoted the development of DNA nanotechnology as it can be employed to prepare delicate 2D/3D nanostructures through systematic design, such as patterns, boxes, tubes, wheel and LEGOs, etc . Recently, functionalization of DNA origami has been developed rapidly by employing origami as scaffolds, for example, molecular robotics, chiral nanostructures, biomimetic nanopores, drug delivery systems, regulators for molecular assembly, etc . Currently, the construction of DNA origami is based on a woven method to fold a long single‐strand DNA by multiple smaller “staple” strands, which is mainly based on the organized packing of rigid DNA duplex and limit the complexity of the DNA assembly structures.…”

DNA Origami Catenanes Templated by Gold Nanoparticles

“…[37][38][39][40] The first topological DNA structures were demonstrated by Seeman and co-workers, who synthesized a variety of DNA knots and Borromean rings. [58] In this work, we experimentally demonstrate the hierarchical assembly of DNA origami catenanes templated by gold nanoparticles (AuNPs), taking inspirations from the transition metal-templated synthesis of catenanes developed by Sauvage and co-workers. [50] In 2010, DNA rotaxanes were reported.…”

“…[50] In 2010, DNA rotaxanes were reported. [58] In this work, we experimentally demonstrate the hierarchical assembly of DNA origami catenanes templated by gold nanoparticles (AuNPs), taking inspirations from the transition metal-templated synthesis of catenanes developed by Sauvage and co-workers. Despite being topologically well-defined, the as-fabricated DNA catenanes and rotaxanes were in general mechanically rather flexible and floppy, because they were made of single-or doublestranded DNA.…”