Assembly of DNA 2D and 3D crystals critically relies on sticky-end cohesions among motifs, which require complementarity not only in sequence but also in geometry. For DNA motifs to self-assemble into crystals, they must be associated with each other in the proper geometry and orientation to ensure that the steric hindrance does not exist and prevent sticky ends from interacting. For DNA motifs with exactly the same pair of sticky-end sequences, by adjusting the length (the helical twisting, the geometry) of the motif branches, it is possible to engineer the assembly of these distinct motifs into different 2D patterns: either mix with one another to form “alloy” crystals or to self-sort and consequently separate from one another to segregate into isolated phases. By rationally designing the motif length to form 3D crystals, the screw axes and even the space group could be precisely predicted without solving the structures at all. In the end, the deposited structure with 2.2 Å resolution validated our design principle. The combination of this strategy and conventional sequence-focused assembly strategy could further expand the programming versatility of DNA self-assembly and pave the way for the structural determination of guest molecules and cascade chemical reactions within DNA platforms.

Engineering DNA 2D and 3D crystals by geometry, not sequence

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