Surface‐Assisted Large‐Scale Ordering of DNA Origami Tiles

Abstract

The arrangement of DNA-based nanostructures into extended higher order assemblies is an important step towards their utilization as functional molecular materials. We herein demonstrate that by electrostatically controlling the adhesion and mobility of DNA origami structures on mica surfaces by the simple addition of monovalent cations, large ordered 2D arrays of origami tiles can be generated. The lattices can be formed either by close-packing of symmetric, non-interacting DNA origami structures, or by utilizing blunt-end stacking interactions between the origami units. The resulting crystalline lattices can be readily utilized as templates for the ordered arrangement of proteins.

Evolution of Structural DNA Nanotechnology

“…Hexagon, square, hexagonal‐shaped, and diamond‐shaped superstructures with dimensions up to 220 nm × 375 nm were assembled via annealing. Besides these methods, surface‐assisted hierarchical assemblies of DNA origami and tiles that yield large high‐quality lattices have been demonstrated . These techniques can be realized on biological membranes and on MICA substrates, but they often need careful tuning of salt concentration for the optimal binding and assembly results.…”

From Nano to Macro through Hierarchical Self‐Assembly: The DNA Paradigm

“…B) This has been experimentally demonstrated by use of a molecular seed consisting of six different types of DNA tiles growing longitudinally into zigzag ribbons of fixed width and variable length . C) Hierarchical assembly of DNA units can be mediated by electrostatic interactions and enhanced diffusion mobility at a liquid–solid interface, by use either of a mica surface, or of D) and E) a lipid bilayer as support. Regular structures with inert edges are prone to associate into closed‐packed structures, whereas base‐stacking interactions at the edges mainly lead to extended 2D crystals.…”

“…However, above a certain limit the strong binding of the DNA to the mica beneath generates a higher electrostatic friction, thus reducing surface diffusion mobility and therefore the percentage of lattice formation. A compromise between DNA stability and surface mobility can be achieved by the addition of monovalent cations, such as sodium ions, which partially replace magnesium ions and form a more diffusive charge layer (Figure C, left) . By this strategy, DNA origami tiles with inert edges and regular shapes, such as rectangles or triangles, were associated into closed‐packed structures (Figure C, middle).…”

“…In another work, twist‐corrected cross‐shaped tiles were grown into large 2D crystals on top of SLBs by taking advantage of blunt‐end stacking interactions and enhanced surface‐mediated mobility (Figure E, left) . Inert edges instead resulted in formation of closed‐packed arrays (Figure E, right), as also previously demonstrated for naked mica‐mediated assembly . Similarly, the adsorption/desorption rates and thus the diffusion properties of the single monomers could be manipulated by the percentage of monovalent cations, such as sodium or potassium ions, thus revealing the essential role played by the electrostatic interactions at the surface–DNA interface.…”

A Self‐Assembling Two‐Dimensional Protein Array is a Versatile Platform for the Assembly of Multicomponent Nanostructures

“…DNA, RNA, peptides, and proteins have all been used to create building blocks that self‐ or co‐associate into well‐defined supramolecular assemblies directly upon mixing, or following a change in the external milieu (e.g., pH, temperature, or buffer composition). The resulting structures may be one, two, or three‐dimensional, composed of a single or of multiple species, and they may require additional elements such as inorganic or biological interfaces to reach a final assembled state …”