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ACS Nano. 2014 Dec 23;8(12):12030-40. doi: 10.1021/nn506014s. Epub 2014 Dec 9.

Optimized assembly and covalent coupling of single-molecule DNA origami nanoarrays.

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Departments of †Bioengineering, ‡Computer Science, and §Computation & Neural Systems, California Institute of Technology , Pasadena, California 91125, United States.


Artificial DNA nanostructures, such as DNA origami, have great potential as templates for the bottom-up fabrication of both biological and nonbiological nanodevices at a resolution unachievable by conventional top-down approaches. However, because origami are synthesized in solution, origami-templated devices cannot easily be studied or integrated into larger on-chip architectures. Electrostatic self-assembly of origami onto lithographically defined binding sites on Si/SiO2 substrates has been achieved, but conditions for optimal assembly have not been characterized, and the method requires high Mg2+ concentrations at which most devices aggregate. We present a quantitative study of parameters affecting origami placement, reproducibly achieving single-origami binding at 94±4% of sites, with 90% of these origami having an orientation within ±10° of their target orientation. Further, we introduce two techniques for converting electrostatic DNA-surface bonds to covalent bonds, allowing origami arrays to be used under a wide variety of Mg2+-free solution conditions.


DNA nanotechnology; directed self-assembly; nanoarray; single molecule; surface diffusion

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