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Published April 2014 | Published + Supplemental Material
Journal Article Open

Developmental Self-Assembly of a DNA Tetrahedron


Kinetically controlled isothermal growth is fundamental to biological development, yet it remains challenging to rationally design molecular systems that self-assemble isothermally into complex geometries via prescribed assembly and disassembly pathways. By exploiting the programmable chemistry of base pairing, sophisticated spatial and temporal control have been demonstrated in DNA self-assembly, but largely as separate pursuits. By integrating temporal with spatial control, here we demonstrate the "developmental" self-assembly of a DNA tetrahedron, where a prescriptive molecular program orchestrates the kinetic pathways by which DNA molecules isothermally self-assemble into a well-defined three-dimensional wireframe geometry. In this reaction, nine DNA reactants initially coexist metastably, but upon catalysis by a DNA initiator molecule, navigate 24 individually characterizable intermediate states via prescribed assembly pathways, organized both in series and in parallel, to arrive at the tetrahedral final product. In contrast to previous work on dynamic DNA nanotechnology, this developmental program coordinates growth of ringed substructures into a three-dimensional wireframe superstructure, taking a step toward the goal of kinetically controlled isothermal growth of complex three-dimensional geometries.

Additional Information

© 2014 American Chemical Society. ACS AuthorChoice - 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 July 23, 2013 and accepted February 19, 2014. Published online April 11, 2014. The authors thank C. Grun and E. Winfree for discussions, and D. Pastuszak for help with draft preparation. This work was funded by Office of Naval Research Grants N000141010827 and N000141310593, Office of Naval Research Young Investigator Program Award N000141110914, NIH Director's New Innovator Award 1DP2OD007292, NSF CAREER Award CCF1054898, NSF Grant CCF1162459, NSF Expedition in Computing Award CCF1317291, and Wyss Institute for Biologically Inspired Engineering Faculty Startup Fund to P.Y., and NIH 5R01CA140759, NIH P50 HG004071, the Molecular Programming Project (NSF-CCF-0832824 and NSF-CCF-1317694), and the Gordon and Betty Moore Foundation (GBMF2809) to N.A.P.; J.P.S. acknowledges a Graduate Research Fellowship from NSF and a J. Marshall & Jane H. Booker Graduate Scholarship from the Buttonwood Foundation, and D.Y.Z. is supported by NIH Transition to Independence Award 1K99EB015331.

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Published - nn4038223.pdf

Supplemental Material - nn4038223_si_001.pdf


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