Supporting Information Single-Molecule Observation of the Photoregulated Conformational Dynamics of DNAOrigami Nanoscissors

We demonstrate direct observation of the dynamic opening and closing behavior of photocontrollable DNA origami nanoscissors using high-speed atomic force microscopy (HS-AFM). First the conformational change between the open and closed state controlled by adjustment of surrounding salt concentration could be directly observed during AFM scanning. Then light-responsive moieties were incorporated into the nanoscissors to control these structural changes by photoirradiation. Using photoswitchable DNA strands, we created a photoresponsive nanoscissors variant and were able to distinguish between the open and closed conformations after respective irradiation with ultraviolet (UV) and visible (Vis) light by gel electrophoresis and AFM imaging. Additionally, these reversible changes in shape during photoirradiation were directly visualized using HS-AFM. Moreover, four photoswitchable nanoscissors were assembled into a scissor-actuator-like higher-order object, the configuration of which could be controlled by the open and closed switching induced by irradiation with UV and Vis light.

[1]  Friedrich C. Simmel,et al.  Oberflächenunterstützte großflächige Anordnung von DNA‐Origami‐Kacheln , 2014 .

[2]  Yangyang Yang,et al.  Dynamic assembly/disassembly processes of photoresponsive DNA origami nanostructures directly visualized on a lipid membrane surface. , 2014, Journal of the American Chemical Society.

[3]  Friedrich C Simmel,et al.  Nucleic acid based molecular devices. , 2011, Angewandte Chemie.

[4]  A. Turberfield,et al.  Direct observation of stepwise movement of a synthetic molecular transporter. , 2011, Nature nanotechnology.

[5]  H. Dietz,et al.  Dynamic DNA devices and assemblies formed by shape-complementary, non–base pairing 3D components , 2015, Science.

[6]  Masayuki Endo,et al.  Single-molecule imaging of dynamic motions of biomolecules in DNA origami nanostructures using high-speed atomic force microscopy. , 2014, Accounts of chemical research.

[7]  Yangyang Yang,et al.  Single-molecule visualization of the hybridization and dissociation of photoresponsive oligonucleotides and their reversible switching behavior in a DNA nanostructure. , 2012, Angewandte Chemie.

[8]  Tomoko Emura,et al.  A Photoregulated DNA-Based Rotary System and Direct Observation of Its Rotational Movement. , 2017, Chemistry.

[9]  Na Liu,et al.  A light-driven three-dimensional plasmonic nanosystem that translates molecular motion into reversible chiroptical function , 2016, Nature Communications.

[10]  Friedrich C. Simmel,et al.  Nukleinsäure‐basierte molekulare Werkzeuge , 2011 .

[11]  Itamar Willner,et al.  DNA switches: from principles to applications. , 2015, Angewandte Chemie.

[12]  M. Komiyama,et al.  Nanomechanical DNA origami 'single-molecule beacons' directly imaged by atomic force microscopy , 2011, Nature communications.

[13]  N. Seeman,et al.  A nanomechanical device based on the B–Z transition of DNA , 1999, Nature.

[14]  Akinori Kuzuya,et al.  Nanomechanical molecular devices made of DNA origami. , 2014, Accounts of chemical research.

[15]  N. Seeman,et al.  A robust DNA mechanical device controlled by hybridization topology , 2002, Nature.

[16]  Itamar Willner,et al.  DNA-Schalter: Grundlagen und Anwendungen , 2015 .

[17]  Xingguo Liang,et al.  A supra-photoswitch involving sandwiched DNA base pairs and azobenzenes for light-driven nanostructures and nanodevices. , 2009, Small.

[18]  Itamar Willner,et al.  Switchable reconfiguration of nucleic acid nanostructures by stimuli-responsive DNA machines. , 2014, Accounts of chemical research.

[19]  A. Kuzyk,et al.  Reconfigurable 3D plasmonic metamolecules. , 2014, Nature materials.

[20]  Xingguo Liang,et al.  Synthesis of azobenzene-tethered DNA for reversible photo-regulation of DNA functions: hybridization and transcription , 2007, Nature Protocols.

[21]  Jing Pan,et al.  A synthetic DNA motor that transports nanoparticles along carbon nanotubes. , 2014, Nature nanotechnology.

[22]  Yangyang Yang,et al.  Photo-controllable DNA origami nanostructures assembling into predesigned multiorientational patterns. , 2012, Journal of the American Chemical Society.

[23]  Masayuki Endo,et al.  State-of-the-art high-speed atomic force microscopy for investigation of single-molecular dynamics of proteins. , 2014, Chemical reviews.

[24]  Keiichi Namba,et al.  Photoresponsive DNA nanocapsule having an open/close system for capture and release of nanomaterials. , 2014, Chemistry.

[25]  Hai-Jun Su,et al.  Programmable motion of DNA origami mechanisms , 2015, Proceedings of the National Academy of Sciences.

[26]  F. Simmel,et al.  Surface-assisted large-scale ordering of DNA origami tiles. , 2014, Angewandte Chemie.

[27]  Hai-Jun Su,et al.  Mechanical design of DNA nanostructures. , 2015, Nanoscale.

[28]  P. Rothemund,et al.  Engineering and mapping nanocavity emission via precision placement of DNA origami , 2016, Nature.

[29]  Adam H. Marblestone,et al.  Rapid prototyping of 3D DNA-origami shapes with caDNAno , 2009, Nucleic acids research.