Functionalizing Designer DNA Crystals with a Triple‐Helical Veneer

DNA is a very useful molecule for the programmed self‐assembly of 2D and 3D nanoscale objects. 1 The design of these structures exploits Watson–Crick hybridization and strand exchange to stitch linear duplexes into finite assemblies. 2 – 4 The dimensions of these complexes can be increased by over five orders of magnitude through self‐assembly of cohesive single‐stranded segments (sticky ends). 5 , 6 Methods that exploit the sequence addressability of DNA nanostructures will enable the programmable positioning of components in 2D and 3D space, offering applications such as the organization of nanoelectronics, 7 the direction of biological cascades, 8 and the structure determination of periodically positioned molecules by X‐ray diffraction. 9 To this end we present a macroscopic 3D crystal based on the 3‐fold rotationally symmetric tensegrity triangle 3 , 6 that can be functionalized by a triplex‐forming oligonucleotide on each of its helical edges.