Reversible Supra‐Folding of User‐Programmed Functional DNA Nanostructures on Fuzzy Cationic Substrates
Résumé
Programmable DNA base pairing is a powerful way to build user-defined nanostructured assemblies, such as DNA origamis and DNA nanogrids. Although two-dimensional (2D) origamis of virtually any desired shape can now be quickly and easily produced, attaining further levels of organization, actuation or dynamics is still a desired challenge. Here we report that, upon adsorption on a soft cationic substrate prepared by layer-by-layer deposition of polyelectrolytes, both 2D origamis and DNA nanogrids undergo a rapid higher-order transition of folding into threedimensional (3D) compact structures (origamis) or well-defined µmlong ribbons (nanogrids), a process we refer to as supra-folding. We show that the supra-folding mechanism is mainly of electrostatic nature through on-surface inter-polyelectrolyte complexation, thus requiring enough fuzziness of the substrate to allow 3D reconfiguration instead of conventional flat adsorption. Interestingly the electrostatic nature of this actuation makes it reversible: once supra-folded, origamis can be switched back on the surface into their 2D original shape through addition of heparin, a highly charged anionic polyelectrolyte known as an efficient competitor of DNApolyelectrolyte complexation. Orthogonal to DNA base-pairing principles, this reversible structural reconfiguration is also versatile; we show in particular that i) it is compatible with various origami shapes, ii) it perfectly preserves fine structural details as well as sitespecific functionality, and iii) it can be applied to dynamically address the spatial distribution of origami-tethered proteins.
Domaines
Chimie
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