Dynamic and Reversible Decoration of DNA-Based Scaffolds.

We demonstrate here an approach to achieve dynamic and reversible decoration of DNA-based scaffolds. To do this, we employ rationally engineered DNA tiles containing enzyme-responsive strands covalently conjugated to different molecular labels. These strands are designed to be recognized and degraded by specific enzymes (i.e., Ribonuclease H, RNase H or Uracil DNA Glycosylase, UDG) inducing their spontaneous de-hybridization from the assembled tile and replacement by a new strand conjugated to a different label. Multiple enzyme-responsive strands that specifically respond to different enzymes allow for dynamic, orthogonal, and reversible decoration of the DNA structures. As a proof-of-principle of our strategy, we demonstrate the possibility to orthogonally control the distribution of different labels (i.e., fluorophores and small molecules) on the same scaffold without crosstalk. By doing so we obtain DNA scaffolds that display different antibodies recognition patterns. Our approach offers the possibility to control the decoration of higher-order supramolecular assemblies (including origami) with several functional moieties to achieve functional biomaterials with improved adaptability, precision, and sensing capabilities. This article is protected by copyright. All rights reserved.