Abstract
DNA origami is a widely used DNA nanotechnology that allows construction of two-dimensional and three-dimensional nanometric shapes. The designability and rigidity of DNA origami make it an ideal material for construction of topologically linked molecules such as catenanes, which are attractive for their potential as motors and molecular machines. However, a general method for production of topologically linked DNA origami has been lacking. Here, we show that catenated single-stranded DNA circles can be produced and used as a universal scaffold for the production of topologically linked (catenated) DNA origami structures where the individual linked structures can be of any arbitrary design. Assembly of these topologically linked DNA origami structures is achieved via a simple one-pot annealing protocol.
Highlights
Linked molecules such as catenanes and rotaxanes are challenging and fascinating targets in supramolecular chemistry.[1]
The enzyme catalyzes a site-specific recombination of negatively supercoiled circular DNA at the res sites to form a supercoiled catenane,[43] while the reverse reaction occurs in the case of the relaxed substrate.[39]
All topologically linked DNA origami structures produced to date are only able to form the topological linkage by a “gap-closing” reaction whereby one DNA origami structure “wraps around” the other through the action of staple strands, i.e., by using base pairing
Summary
Linked molecules such as catenanes and rotaxanes are challenging and fascinating targets in supramolecular chemistry.[1]. They achieved particular prominence after Sauvage’s demonstration of the templated approach to molecular catenane synthesis in 19832,3 with Stoddart demonstrating a rotaxane almost a decade later.[4]. The scaffold strand is thousands of bases long, providing enough material for the construction of complex, rigid structures such as dynamic containers whose opening can be programmed in response to stimuli.[8,9]. While customization of scaffolds can be challenging, numerous examples have been reported, including those that are shortened,[10,11] extended,[12−14] or otherwise modified to provide arbitrary length and sequences.[15−18] Efforts to connect together discrete DNA origami structures have included hybridization of sticky ends[19] or base stacking[7,20−22] and have achieved gigadalton-scale structures[23] and fully addressable semimicrometer-scale tiles.[24] DNA origami is a DNA nanotechnology in which a long single-stranded DNA “scaffold” is shaped by the action of many short “staple” strands, which bind to cognate sequences distributed throughout the scaffold.[6,7] Typically, the scaffold strand is thousands of bases long, providing enough material for the construction of complex, rigid structures such as dynamic containers whose opening can be programmed in response to stimuli.[8,9] While customization of scaffolds can be challenging, numerous examples have been reported, including those that are shortened,[10,11] extended,[12−14] or otherwise modified to provide arbitrary length and sequences.[15−18] Efforts to connect together discrete DNA origami structures have included hybridization of sticky ends[19] or base stacking[7,20−22] and have achieved gigadalton-scale structures[23] and fully addressable semimicrometer-scale tiles.[24]
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