title: Dynamic and Progressive Control of DNA Origami Conformation by Modulating DNA Helicity with Chemical Adducts.
abstract: DNA origami has received enormous attention for its ability to program complex nanostructures with a few nanometer precision. Dynamic origami structures that change conformation in response to environmental cues or external signals hold great promises in sensing and actuation at the nanoscale. The reconfiguration mechanism of existing dynamic origami structures is mostly limited to single-stranded hinges and relies almost exclusively on DNA hybridization or strand displacement. Here, we show an alternative approach by demonstrating on-demand conformation changes with DNA-binding molecules, which intercalate between base pairs and unwind DNA double helices. The unwinding effect modulates the helicity mismatch in DNA origami, which significantly influences the internal stress and the global conformation of the origami structure. We demonstrate the switching of a polymerized origami nanoribbon between different twisting states and a well-constrained torsional deformation in a monomeric origami shaft. The structural transformation is shown to be reversible, and binding isotherms confirm the reconfiguration mechanism. This approach provides a rapid and reversible means to change DNA origami conformation, which can be used for dynamic and progressive control at the nanoscale.
authors.affiliation: School of Mechanical Engineering, Purdue University , West Lafayette, Indiana 47907, United States.
authors.forename: Haorong
authors.initials: H
authors.lastname: Chen
authors.affiliation: School of Mechanical Engineering, Purdue University , West Lafayette, Indiana 47907, United States.
authors.forename: Hanyu
authors.initials: H
authors.lastname: Zhang
authors.affiliation: School of Mechanical Engineering, Purdue University , West Lafayette, Indiana 47907, United States.
authors.forename: Jing
authors.initials: J
authors.lastname: Pan
authors.affiliation: School of Mechanical Engineering, Purdue University , West Lafayette, Indiana 47907, United States.
authors.forename: Tae-Gon
authors.initials: TG
authors.lastname: Cha
authors.affiliation: Department of Chemistry and Chemical Engineering, Chalmers University of Technology , SE-412 96 Gothenburg, Sweden.
authors.forename: Shiming
authors.initials: S
authors.lastname: Li
authors.affiliation: Department of Chemistry and Chemical Engineering, Chalmers University of Technology , SE-412 96 Gothenburg, Sweden.
authors.forename: Joakim
authors.initials: J
authors.lastname: Andréasson
authors.affiliation: School of Mechanical Engineering, Purdue University , West Lafayette, Indiana 47907, United States.
authors.forename: Jong Hyun
authors.initials: JH
authors.lastname: Choi
mesh_terms: D004247:DNA; D049329:Nanostructures; D036103:Nanotechnology; D009690:Nucleic Acid Conformation
chemical_list: D004247:DNA
keywords: DNA binding; DNA origami; conformation change