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Published December 2014 | Supplemental Material + Published
Journal Article Open

Optimized Assembly and Covalent Coupling of Single-Molecule DNA Origami Nanoarrays


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/SiO_2 substrates has been achieved, but conditions for optimal assembly have not been characterized, and the method requires high Mg^(2+) 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 Mg^(2+)-free solution conditions.

Additional Information

© 2014 American Chemical Society. ACS Editors' Choice - This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes. Received for review October 21, 2014 and accepted November 20, 2014. Publication Date (Web): November 20, 2014. We acknowledge financial support from the Army Research Office award W911NF-11-1-0117 and the U.S. National Science Foundation for Expeditions in Computing funding for the Molecular Programming Project (Nos. 0832824 and 1317694, http://molecular-programming.org) and Office of Naval Research Award N000141410702. We acknowledge the gift of aminopropyl silatrane from G. Lovely. We thank S. Guo of Bruker Nano Surfaces for fast scan AFM movies. We thank D. Fygenson, J. Sorensen, T. del Bonis-O'Donnell, S. Woo, and members of Winfree lab for discussions. E-beam lithography was performed in the Kavli Nanoscience Institute at Caltech; nanoimprinting was performed in the UCSB Nanofabrication Facility.

Attached Files

Published - nn506014s.pdf

Supplemental Material - nn506014s_si_001.pdf

Supplemental Material - nn506014s_si_002.mov

Supplemental Material - nn506014s_si_003.mov

Supplemental Material - nn506014s_si_004.mov

Supplemental Material - nn506014s_si_005.mov

Supplemental Material - nn506014s_si_006.zip


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