Daisy Chain Rotaxanes Made from Interlocked DNA Nanostructures

Weigandt, Johannes; Chung, Chia‐Ling; Jester, Stefan‐S.; Famulok, Michael

doi:10.1002/anie.201601042

Cited by 30 publications

(20 citation statements)

References 48 publications

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“…[25][26][27][28][29][30] Rotaxanes have been used as molecular shuttles, [31,32] switches in molecular electronics, [33] control of chemical synthesis, [34] and force-generating components for molecular elevators [35] and pumps. [51] Subsequently, chemically more rigid, [52] light-switchable, [53] and Daisy-chain rotaxanes, [54] DNA-nanoparticle rotaxanes [55] as well as catalytically active rotaxanes [56] were demonstrated. [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.…”

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confidence: 99%

“…[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. [51] Subsequently, chemically more rigid, [52] light-switchable, [53] and Daisy-chain rotaxanes, [54] DNA-nanoparticle rotaxanes [55] as well as catalytically active rotaxanes [56] were demonstrated. [50] In 2010, DNA rotaxanes were reported.…”

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DNA Origami Catenanes Templated by Gold Nanoparticles

Peil

Zhan

Liu

2020

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molecule via a transition metal ion and subsequently closed by another crescentshaped molecule in a single cyclization reaction. In strategy B "entwining," two crescent-shaped molecules are linked together via a transition metal ion, followed by a double cyclization reaction to close them at once. In each case, the transition metal ion can be removed after serving its purpose, enabling the free relative movements of the two rings.Mechanically interlocked architectures are appealing building blocks for the realization of many functional devices. Importantly, they empower broad applications in nanomaterials, nanorobotics, and nanomachines. [18][19][20][21] For instance, catenanes have been exploited as switches, [22] rotary motors, [23,24] and sensors. [25][26][27][28][29][30] Rotaxanes have been used as molecular shuttles, [31,32] switches in molecular electronics, [33] control of chemical synthesis, [34] and force-generating components for molecular elevators [35] and pumps. [36] An alternative pathway to create topologically complex molecular architectures is structural DNA nanotechnology, which exploits DNA as both genetic and construction material. [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. [41,42] It was then followed by the construction of DNA catenanes, [43][44][45][46] rotary motors, [47,48] a biohybrid nanoengine, [49] and logic circuits. [50] In 2010, DNA rotaxanes were reported. [51] Subsequently, chemically more rigid, [52] light-switchable, [53] and Daisy-chain rotaxanes, [54] DNA-nanoparticle rotaxanes [55] as well as catalytically active rotaxanes [56] were demonstrated. 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. By contrast, DNA origami-based interlocked architectures possess much better structural rigidity. The first attempt to realize such catenanes was carried out by Yan and co-workers, who followed an innovative scheme of molecular kirigami. [57] In 2016, Simmel and co-workers reported switchable DNA origami rotaxanes with long-range on-axis motion. [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. DNA origami catenanes, which contain two, three or four interlocked rings are successfully created. In particular, the origami rings within the individual catenanes can be set free with respect to one another by releasing the interconnecting AuNPs through toehold-mediated strand displacement reactions.Mechanically interlocked molecules have marked a breakthrough in the field of topological chemistry and boosted the vigorous development of molecular machinery. As an archetypal example of the interlocked molecules, catenanes compri...

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DNA Origami Catenanes Templated by Gold Nanoparticles

Peil

Zhan

Liu

2020

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“…[3] Intrigued by the potential applications of rotaxanes as stimulus-responsive switches and the diverse conjugation chemistry compatible with DNA nanodevices [4] , several recent investigations have focused on assembly of rotaxanes from DNA. [3b, 5] …”

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DNA Origami Rotaxanes: Tailored Synthesis and Controlled Structure Switching

et al. 2016

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Mechanically interlocked supramolecular assemblies are appealing building blocks for creating functional nanodevices. Here we describe the multi-step assembly of massive DNA origami rotaxanes that are capable of programmable structural switching. We validated the topology and structural integrity of these rotaxanes by analyzing the intermediate and final products of various assembly routes using electrophoresis and electron microscopy. We further demonstrated two structural switching behaviors of our rotaxanes, both mediated by DNA hybridization. In the first mechanism, the translational motion of the macrocycle can be triggered or halted at either terminus. In the second mechanism, the macrocycle can be elongated after the completion of rotaxane assembly, giving rise to a unique structure that is otherwise difficult to access.

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“…An asymmetricr otaxane with aS ST-a nd ar ingshaped stopper featuring two stations for hybridization of the macrocycle to the axle was assembled. The macrocycle can be directedt owards one or the others tation upon triggering with fuel ODNs.Interlocked DNA architectures such as catenanes, [1] rotaxanes, [2] borromean rings, [3] daisy-chainr otaxanes, [4] or others represent useful components for constructing nanomechanical devices. [5] These have been used for variousp urposes such as simple or complex switches, shuttles, devices for performing molecular logic, or programmedr econfiguration of nanostructures.For example, a[ 3]pseudorotaxane [6] was assembled in which two single-stranded stations on an otherwise double-stranded DNA axle served as ah ybridization site for a1 05 base-pair dsDNA macrocycle and a1 26 base-paird sDNA macrocycle.…”

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“…Interlocked DNA architectures such as catenanes, [1] rotaxanes, [2] borromean rings, [3] daisy-chainr otaxanes, [4] or others represent useful components for constructing nanomechanical devices. [5] These have been used for variousp urposes such as simple or complex switches, shuttles, devices for performing molecular logic, or programmedr econfiguration of nanostructures.…”

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Single‐Stranded Tile Stoppers for Interlocked DNA Architectures

et al. 2016

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Interlocked DNA architectures are useful for DNA nanotechnology because of their mechanically bonded components, which can move relative to one another without disassembling. We describe the design, synthesis, and characterization of novel single-stranded tile (SST) stoppers for the assembly of interlocked DNA architectures. SST stoppers are shown to self-assemble into a square-shaped rigid structure upon mixing 97 oligodeoxynucleotide (ODN) strands. The structures are equipped with a sticky end that is designed for hybridization with the sticky ends of a dsDNA axle of a DNA rotaxane. Because the diameter of the macrocycle threaded onto the axle is 14 nm, the dimension of the square-shaped stopper was designed to be bulky enough to prevent the dethreading of the macrocycle. An asymmetric rotaxane with a SST- and a ring-shaped stopper featuring two stations for hybridization of the macrocycle to the axle was assembled. The macrocycle can be directed towards one or the other station upon triggering with fuel ODNs.

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Daisy Chain Rotaxanes Made from Interlocked DNA Nanostructures

Cited by 30 publications

References 48 publications

DNA Origami Catenanes Templated by Gold Nanoparticles

DNA Origami Catenanes Templated by Gold Nanoparticles

DNA Origami Rotaxanes: Tailored Synthesis and Controlled Structure Switching

Single‐Stranded Tile Stoppers for Interlocked DNA Architectures

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