Programmed Two-Dimensional Self-Assembly of Multiple DNA Origami Jigsaw Pieces

Abstract

T he unique structural motifs and molecular recognition properties of DNA make it a promising template for building nanostructures. 1Ϫ4 Using a long single-stranded DNA as a template, a novel strategy, the so-called DNA origami method, has been developed for the preparation of various two-dimensional (2D) and three-dimensional (3D) nanostructures with defined size. 5Ϫ12 In addition, these origami nanostructures have been used as a platform for the nanopatterning of proteins, nanoparticles, transition metals, and other functional components into deliberately designed arrangements. 13Ϫ20 They can also act as templates for the growth of nanowires, aid in the structural determination of proteins, and provide new platforms for genomic applications. 21 However, these structures offer a relatively small area, which is not sufficient for the precise positioning of functional molecules, and a larger assembly with a size of a few micrometers is required for the preparation of practical devices. For instance, conventional photolithography techniques require a size domain of 1 m. Although programmed DNA and RNA assemblies with the size of around 10Ϫ20 nm have been achieved, 22Ϫ24 strategies for the construction of defined larger assemblies are limited.The size of the origami was first expanded by Rothemund with the assembly of triangular origami into a hexagon with a yield of Ͻ2%. 5 Later, 3D heterotrimers in the shape of a wireframe icosahedron were reported with no information about the yield of the assembled structures. 10 We have recently developed a new method to scale up DNA origami using jigsaw pieces (JPs) and successfully prepared a unidirectional DNA assembly. 25 However, the 2D construction of origami tiles is critical for the development of DNA origami technology. The 2D scale-up of the origami structure was recently initiated using small DNA tiles with a size of 16 nm ϫ17 nm as folding staples. 26 Apart from these examples, there is no report for the preparation of larger origami structures (particularly 2D structures), and hence the development of new methods with added advantages is urgently required.In this work, we demonstrate a new route for the 2D extension of DNA origami using multiple JPs by programmed selfassembly, the spontaneous association of components into organized 2D structures using noncovalent interactions. By altering the shape of our previous origami structure, 25 we have designed nine different JPs, each of which is a 24-helix tile ( Figure 1A), containing (i) sequence-programmed connection sites, a tenon, and corresponding mortise, to allow assembly along the 10.1021/nn1031627© XXXX American Chemical Society ABSTRACT We demonstrate a novel strategy of self-assembly to scale up origami structures in twodimensional (2D) space using multiple origami structures, named "2D DNA jigsaw pieces", with a specially designed shape. For execution of 2D self-assembly along the helical axis (horizontal direction), sequence-programmed tenon and mortise were introduced to promote selective connections vi...

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