Polyhedra Self-Assembled from DNA Tripods and Characterized with 3D DNA-PAINT

Engineering Larger DNA Structures Several approaches now exist for the self-assembly of DNA into nanostructures. For example, three-arm DNA tripods can be assembled into larger wireframe polyhedra, but for the most complicated shapes, assembly yields can be low, apparently because the flexibility of smaller tripods allows for misassembly. Iinuma et al. (p. 65, published online 13 March) now show that larger, stiffer tripods that have controlled arm lengths and interarm angles can be designed to form a wide variety of open wireframe polyhedra—including tetrahedra, cubes, and hexagonal prisms, with edges 100 nanometers in length. Stiff DNA tripod units enabled the assembly of wireframe polyhedra with edges 100 nanometers in length. DNA self-assembly has produced diverse synthetic three-dimensional polyhedra. These structures typically have a molecular weight no greater than 5 megadaltons. We report a simple, general strategy for one-step self-assembly of wireframe DNA polyhedra that are more massive than most previous structures. A stiff three-arm-junction DNA origami tile motif with precisely controlled angles and arm lengths was used for hierarchical assembly of polyhedra. We experimentally constructed a tetrahedron (20 megadaltons), a triangular prism (30 megadaltons), a cube (40 megadaltons), a pentagonal prism (50 megadaltons), and a hexagonal prism (60 megadaltons) with edge widths of 100 nanometers. The structures were visualized by means of transmission electron microscopy and three-dimensional DNA-PAINT super-resolution fluorescent microscopy of single molecules in solution.

[1]  N. Seeman,et al.  Synthesis from DNA of a molecule with the connectivity of a cube , 1991, Nature.

[2]  N. Seeman,et al.  Construction of a DNA-Truncated Octahedron , 1994 .

[3]  H. P. Kao,et al.  Tracking of single fluorescent particles in three dimensions: use of cylindrical optics to encode particle position. , 1994, Biophysical journal.

[4]  N. Seeman,et al.  Design and self-assembly of two-dimensional DNA crystals , 1998, Nature.

[5]  William M. Shih,et al.  A 1.7-kilobase single-stranded DNA that folds into a nanoscale octahedron , 2004, Nature.

[6]  E. Winfree,et al.  Algorithmic Self-Assembly of DNA Sierpinski Triangles , 2004, PLoS biology.

[7]  Russell P. Goodman,et al.  Rapid Chiral Assembly of Rigid DNA Building Blocks for Molecular Nanofabrication , 2005, Science.

[8]  P. Rothemund Folding DNA to create nanoscale shapes and patterns , 2006, Nature.

[9]  R. Hochstrasser,et al.  Wide-field subdiffraction imaging by accumulated binding of diffusing probes , 2006, Proceedings of the National Academy of Sciences.

[10]  S. Hell Far-Field Optical Nanoscopy , 2007, Science.

[11]  Russell P. Goodman,et al.  A self-assembled DNA bipyramid. , 2007, Journal of the American Chemical Society.

[12]  Faisal A. Aldaye,et al.  Modular access to structurally switchable 3D discrete DNA assemblies. , 2007, Journal of the American Chemical Society.

[13]  C. Mao,et al.  Hierarchical self-assembly of DNA into symmetric supramolecular polyhedra , 2008, Nature.

[14]  G. von Kiedrowski,et al.  Self-assembly of a DNA dodecahedron from 20 trisoligonucleotides with C(3h) linkers. , 2008, Angewandte Chemie.

[15]  C. Mao,et al.  Conformational flexibility facilitates self-assembly of complex DNA nanostructures , 2008, Proceedings of the National Academy of Sciences.

[16]  Mark Bates,et al.  Three-Dimensional Super-Resolution Imaging by Stochastic Optical Reconstruction Microscopy , 2008, Science.

[17]  Hao Yan,et al.  Scaffolded DNA origami of a DNA tetrahedron molecular container. , 2009, Nano letters.

[18]  J. Kjems,et al.  Self-assembly of a nanoscale DNA box with a controllable lid , 2009, Nature.

[19]  Atanu Basu,et al.  Icosahedral DNA nanocapsules by modular assembly. , 2009, Angewandte Chemie.

[20]  J. Lippincott-Schwartz,et al.  Interferometric fluorescent super-resolution microscopy resolves 3D cellular ultrastructure , 2009, Proceedings of the National Academy of Sciences.

[21]  Shawn M. Douglas,et al.  Self-assembly of DNA into nanoscale three-dimensional shapes , 2009, Nature.

[22]  Hua Yang,et al.  Metal-nucleic acid cages. , 2009, Nature chemistry.

[23]  Chengde Mao,et al.  Symmetry controls the face geometry of DNA polyhedra. , 2009, Journal of the American Chemical Society.

[24]  Pamela E. Constantinou,et al.  From Molecular to Macroscopic via the Rational Design of a Self-Assembled 3D DNA Crystal , 2009, Nature.

[25]  F. Simmel,et al.  Single-molecule kinetics and super-resolution microscopy by fluorescence imaging of transient binding on DNA origami. , 2010, Nano letters.

[26]  Tim Liedl,et al.  A Structurally Variable Hinged Tetrahedron Framework from DNA Origami , 2011, Journal of nucleic acids.

[27]  Luvena L. Ong,et al.  Three-Dimensional Structures Self-Assembled from DNA Bricks , 2012, Science.

[28]  F. Simmel,et al.  DNA-based self-assembly of chiral plasmonic nanostructures with tailored optical response , 2011, Nature.

[29]  Shawn M. Douglas,et al.  A Logic-Gated Nanorobot for Targeted Transport of Molecular Payloads , 2012, Science.

[30]  P. Yin,et al.  Complex shapes self-assembled from single-stranded DNA tiles , 2012, Nature.

[31]  Peng Yin,et al.  Submicrometre geometrically encoded fluorescent barcodes self-assembled from DNA. , 2012, Nature chemistry.

[32]  T. G. Martin,et al.  Synthetic Lipid Membrane Channels Formed by Designed DNA Nanostructures , 2012, Science.

[33]  Philip Tinnefeld,et al.  Fluorescence Enhancement at Docking Sites of DNA-Directed Self-Assembled Nanoantennas , 2012, Science.

[34]  Hao Yan,et al.  Interenzyme substrate diffusion for an enzyme cascade organized on spatially addressable DNA nanostructures. , 2012, Journal of the American Chemical Society.

[35]  Philipp C Nickels,et al.  DNA origami nanopillars as standards for three-dimensional superresolution microscopy. , 2013, Nano letters.

[36]  Chengde Mao,et al.  Self-assembly of DNA nanoprisms with only two component strands. , 2013, Chemical communications.

[37]  V. Linko,et al.  The enabled state of DNA nanotechnology. , 2013, Current opinion in biotechnology.

[38]  Hao Yan,et al.  DNA Gridiron Nanostructures Based on Four-Arm Junctions , 2013, Science.

[39]  Johannes B. Woehrstein,et al.  Multiplexed 3D Cellular Super-Resolution Imaging with DNA-PAINT and Exchange-PAINT , 2014, Nature Methods.