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1.9).

Schematic illustration of DNA nanotechnology before the emergence of DNA origami.

      Source: Modified from Seeman [1].

      (c) Double crossover structure, in which two dsDNAs are connected by four‐way branched strands (crossover; arrows). Two‐dimensional periodic structure was formed by self‐assembly using two double‐crossover components (A‐tile and B‐tile* with hairpin) with sticky ends (complementary single‐stranded DNAs at the ends). AFM image of the self‐assembled 2D nanostructure.

      Source: Modified from Winfree et al. [10]

      (d) Dynamic open/close behavior of DNA tweezers operated by strand displacement using toehold containing DNA strands.

      Source: Modified from Yurke et al. [8].

      (e) PX‐JX2 device to exchange the bottom part of by insertion and removal of the strands. The structures can be observed in AFM images.

      Source: Yan et al. [9]/with permission of Springer Nature.

Schematic illustration of DNA origami.

      Source: Rothemund [6]/with permission of Springer Nature.

      The programmed arrangement of multiple DNA origami structures is an important technique for preparing larger structures, particularly in terms of integrating complex functions. We explored techniques for arranging multiple DNA origami components and developed methods to arrange rectangular DNA origami tiles horizontally in a programmed fashion [18]. Because the ends of the helical axes align at both edges of the DNA origami rectangles, origami tiles horizontally assemble via π‐interactions at the edges in a predictable fashion [18]. Specific concave and convex connectors were introduced into DNA origami tiles to precisely align neighboring tiles in a shape‐fitting manner. DNA tiles could be correctly assembled by shape and sequence complementarity, where the complementary strands were introduced into the concavity and the convex connectors. After self‐assembly of three, four, and five tiles, the DNA tiles were aligned and oriented in the same direction in a designed manner. For identification of the DNA tiles, hairpin markers were introduced onto individual tiles. After self‐assembly, judging from the order of the markers, the five tiles were aligned correctly. This method was further expanded vertically to form 2D assemblies.

      Rothemund and coworker created a programmed assembly system by controlling the positions of adhesive π‐stacking terminals for selective connection between rectangular tiles [19]. They showed that a relaxed edge with blunt ends can form a stable connection, as opposed to a stressed edge with the usual loop ends, which induces structural distortions. Multiple dsDNA terminals with blunt ends were introduced to assemble complementary edges of the counterpart tiles as a binary code. In addition, the complementarity of the edge shape effectively aligned the different tiles for one‐dimensional assemblies. The results indicate that the π‐stacking interactions between the complementary edges can control the programmed assembly of multiple different origami tiles.

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