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WIREs Nanomed Nanobiotechnol
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Long‐range assembly of DNA into nanofibers and highly ordered networks

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Long‐range assembly of DNA currently comprises both top‐down and bottom‐up methods. The top‐down techniques consist of physical alignment of DNA and lithographic patterning to organize DNA on surfaces. The bottom‐up approaches include lipid‐and polymer–DNA co‐assembly, the self‐assembly of DNA amphiphiles, and the remarkably specific and versatile methods of DNA nanotechnology. DNA‐based materials possess unprecedented molecular control and may offer innovative solutions in the fields of nanotechnology, sensing, nanomedicine, as well as optical and electronic devices. To realize the potential of these materials, a number of hurdles must be addressed. Bridging the gap between top‐down fabrication and bottom‐up assembly is of critical importance to the successful development of functional DNA‐based technology. A profound understanding of both regimes is necessary to achieve this goal. WIREs Nanomed Nanobiotechnol 2013, 5:266–285. doi: 10.1002/wnan.1218

The authors have declared no conflicts of interest for this article.

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Figure 1.

(a) Hydrogen bonding between base pairs (A with T and C with G). (b) DNA duplexes with A‐, B‐, and Z‐forms. (c) Chemical structure and cartoon representation of a G‐quadruplex, an i‐motif, and a DNA triple helix. (Reprinted with permission from Ref 4. Copyright 2006 Oxford University Press; Reprinted with permission from Ref 5. Copyright 1993 Macmillan Publishers Ltd; Reprinted with permission from Ref 6. Copyright 2012 American Chemical Society)

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Figure 2.

(a) Molecular combing of DNA strands on a surface. (Reprinted with permission from Ref 19. Copyright 2010 IOP Publishing Ltd) (b) Covalent immobilization of DNA strands on lithographically patterned surfaces. (Reprinted with permission from Ref 20. Copyright 1996 Oxford University Press) (c) DNA lines with 50‐nm resolution were patterned using a subtraction printing method. (Reprinted with permission from Ref 21. Copyright 2009 American Chemical Society) (d) Highly ordered arrays achieved by controlled microdroplet dewetting of DNA‐containing solutions. (Reprinted with permission from Ref 22. Copyright 2008 Macmillan Publishers Ltd) (e) Dip‐pen nanolithography is used to precisely deliver DNA‐SH molecules with an atomic force microscopy tip to a gold surface. (Reprinted with permission from Ref 23. Copyright 2002 American Chemical Society)

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Figure 3.

(a) Shapes of individual lipid surfactants and of their self‐assemblies. (Reprinted with permission from Ref 38. Copyright 2009 BioMed Central) (b) Reversible structural switching of DNA–dimethyldidodecylammonium bromide films in the wet and dry states. (Reprinted with permission from Ref 39. Copyright 2009 American Chemical Society) (c) Breath figure technique to prepare honeycomb structures with lipid–DNA films. (Reprinted with permission from Ref 10. Copyright 2011 John Wiley and Sons) (d) Temperature and conductivity dependence of a DNA–lipid film. (Reprinted with permission from Ref 10. Copyright 2011 John Wiley and Sons) (e) Layer‐by‐layer assembly mechanism of DNA films by consecutive adsorption of DNA and poly(allylamine). (Reprinted with permission from Ref 40. Copyright 1993 American Chemical Society)

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Figure 4.

(a) Self‐assembly of nucleoside phosphocholine DNA amphiphiles into helical fibers. (Reprinted with permission from Ref 55. Copyright 2004 American Chemical Society) (b) Single‐stranded DNA‐templated self‐assembly of polyethylene oxide‐functionalized nucleosides. (Reprinted with permission from Ref 61. Copyright 2007 American Chemical Society) (c) DNA–polypropylene oxide (PPO) conjugates self‐assemble into a micelle with a PPO core and single‐stranded DNA corona. The micelle shape shifts into a rod upon addition of a long DNA strand. (Reprinted with permission from Ref 62. Copyright 2007 John Wiley and Sons) (d) A polyethylene glycol–DNA brush block copolymer can shape shift between spherical and cylindrical micelles depending on the specific DNA input. (Reprinted with permission from Ref 63. Copyright 2010 John Wiley and Sons) (e) Long‐range assembly of DNA into fibers and networks through phase separation of DNA strands functionalized with oligoethylene glycol dendrons. (Reprinted with permission from Ref 64. Copyright 2009 American Chemical Society)

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Figure 5.

Tile‐based assembly of DNA lattices. (Reprinted with permission from Ref 71. Copyright 2006 John Wiley and Sons) (a) Sticky‐end assembly of DNA four‐way junctions. (Reprinted with permission from Ref 69. Copyright 2003 Macmillan Publishers Ltd) (b) Lattices formed from planar double crossover (DX) and DX triangle tiles. (Reprinted with permission from Ref 72. Copyright 1998 Macmillan Publishers Ltd; Reprinted with permission from Ref 73. Copyright 2004 American Chemical Society) (c) Lattices assembled from three‐ and six‐helix bundles. (Reprinted with permission from Ref 74. Copyright 2005 American Chemical Society; Reprinted with permission from Ref 75. Copyright 2005 American Chemical Society) (d) Lattices from cross‐shaped, 3‐point, 5‐point, and 6‐point motifs and T‐junction molecules. (Reprinted with permission from Ref 76. Copyright 2003 AAAS; Reprinted with permission from Ref 77. Copyright 2005 American Chemical Society; Reprinted with permission from Ref 78. Copyright 2008 National Academy of Sciences, U.S.A.; Reprinted with permission from Ref 79. Copyright 2006 American Chemical Society; Reprinted with permission from Ref 80. Copyright 2009 John Wiley and Sons) (e) 3D macroscopic DNA crystals built from tensegrity triangles. (Reprinted with permission from Ref 81. Copyright 2009 Macmillan Publishers Ltd) (f) Patterning of gold nanoparticle lines with defined separation on a DX tile array. (Reprinted with permission from Ref 82. Copyright 2004 American Chemical Society) (g) Assembly of lattices from RNA tectosquares. (Reprinted with permission from Ref 83. Copyright 2004 AAAS)

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Figure 6.

DNA origami. (a) DNA origami design and atomic force microscopy characterization. (Reprinted with permission from Ref 107. Copyright 2006 Macmillan Publishers Ltd) (b) Assembly of larger origami structures from ‘2D DNA jigsaw pieces’. (Reprinted with permission from Ref 110. Copyright 2011 American Chemical Society) (c) DNA origami nanoflask. (Reprinted with permission from Ref 112. Copyright 2011 AAAS) (d) Single‐stranded tile approach to the assembly of complex two‐dimensional shapes. (Reprinted with permission from Ref 113. Copyright 2012 Macmillan Publishers Ltd) (e) Label‐free detection of RNA targets on DNA origami chips. (Reprinted with permission from Ref 114. Copyright 2008 AAAS)

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Figure 7.

DNA nanotubes. (a) Nanotubes assembled from DX tiles. (Reprinted with permission from Ref 122. Copyright 2004 American Chemical Society) (b) Nanotubes assembled from a single DNA strand composed of four palindromic domains. (Reprinted with permission from Ref 123. Copyright 2006 John Wiley and Sons) (c) Nanotubes assembled by giving curvature to a DX tile array using a porphyrin‐DNA connector. (Reprinted with permission from Ref 124. Copyright 2005 John Wiley and Sons) (d) DX tile arrays with parallel lines of gold nanoparticles (AuNPs) transform into a nanotube displaying different nanoparticle arrangements. (Reprinted with permission from Ref 125. Copyright 2009 AAAS) (e) Covalently linked DNA nanotubes synthesized by orthogonal stepwise cross‐linking of bis‐thiolated/bis‐aminated circular DNA units. (Reprinted with permission from Ref 126. Copyright 2010 American Chemical Society) (f) Nanotubes made from 6HB building blocks joined by sticky‐end cohesion. (Reprinted with permission from Ref 75. Copyright 2005 American Chemical Society) (g) Nanotubes with monodisperse circumferences. (Reprinted with permission from Ref 127. Copyright 2008 AAAS.) (h) Single‐ and double‐stranded nanotubes made from triangular or square cyclic rungs.128 (i) Encapsulation and release of AuNPs in DNA nanotubes composed of alternating large and small capsules. (Reprinted with permission from Ref 129. Copyright 2010 Macmillan Publishers Ltd) (j) Metal–DNA nanotubes formed from triangular rungs containing copper‐stabilized chiral junctions. (Reprinted with permission from Ref 130. Copyright 2011 John Wiley and Sons) (k) DNA nanotubes built upon a template strand produced by rolling circle amplification (RCA nanotubes). (Reprinted with permission from Ref 131. Copyright 2012 American Chemical Society) (l) RCA nanotubes functionalized with block copolymer–DNA conjugates that form micellar aggregates. (Reprinted with permission from Ref 132. Copyright 2012 Royal Society of Chemistry)

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James F. Leary

James F. Leary
has been contributing to nanomedical research and technologies throughout his career. Such contributions include the invention of high-speed flow cytometry, cell sorting techniques, and rare-event methods. Dr. Leary’s current research spans across three general areas in nanomedicine. The first is the development of high-throughput single-cell flow cytometry and cell sorting technologies. The second explores BioMEMS technologies. These include miniaturized cell sorters, portable devices for detection of microbial pathogens in food and water, and artificial human “organ-on-a-chip” technologies which consists of developing cell culture chips capable of simulating the activities and mechanics of entire organs and organ systems. His third area of research aims at developing smart nano-engineered systems for single-cell drug or gene delivery for nanomedicine. Dr. Leary currently holds nine issued U.S. Patents with four currently pending, and he has received NIH funding for over 25 years.

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