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Seeding the Self-Assembly of DNA Origamis at Surfaces

  • Huan H. Cao
    Huan H. Cao
    Chemistry and Chemical Biology, University of California, Merced, California 95343, United States
    More by Huan H. Cao
  • Gary R. Abel Jr.
    Gary R. Abel, Jr.
    Chemistry and Chemical Biology, University of California, Merced, California 95343, United States
  • Qufei Gu
    Qufei Gu
    Materials and Biomaterials Science and Engineering, University of California, Merced, California 95343, United States
    More by Qufei Gu
  • Gloria-Alexandra V. Gueorguieva
    Gloria-Alexandra V. Gueorguieva
    Chemistry and Chemical Biology, University of California, Merced, California 95343, United States
  • Yehan Zhang
    Yehan Zhang
    Chemistry and Chemical Biology, University of California, Merced, California 95343, United States
    More by Yehan Zhang
  • Warren A. Nanney
    Warren A. Nanney
    Chemistry and Chemical Biology, University of California, Merced, California 95343, United States
  • Eric T. Provencio
    Eric T. Provencio
    Chemistry and Chemical Biology, University of California, Merced, California 95343, United States
  • , and 
  • Tao Ye*
    Tao Ye
    Chemistry and Chemical Biology, University of California, Merced, California 95343, United States
    Materials and Biomaterials Science and Engineering, University of California, Merced, California 95343, United States
    *(T.Y.) Email: [email protected]
    More by Tao Ye
Cite this: ACS Nano 2020, 14, 5, 5203–5212
Publication Date (Web):February 13, 2020
https://doi.org/10.1021/acsnano.9b09348
Copyright © 2020 American Chemical Society

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    Abstract

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    Unlike supramolecular self-assembly methods that can organize many distinct components into designer shapes in a homogeneous solution (e.g., DNA origami), only relatively simple, symmetric structures consisting of a few distinct components have been self-assembled at solid surfaces. As the self-assembly process is confined to the surface/interface by mostly nonspecific attractive interactions, an open question is how these interfacial interactions affect multicomponent self-assembly. To gain a mechanistic understanding of the roles of the surface environment in DNA origami self-assembly, here we studied the oligonucleotide-assisted folding of a long single-stranded DNA (ssDNA scaffold) that was end-tethered to a dynamic surface, which could actively regulate the DNA–surface interactions. The results showed that even weak surface attractions can lead to defective structures by inhibiting the merging of multiple domains into complete structures. A combination of surface anchoring and deliberate regulation of DNA–surface interactions allowed us to depart from the existing paradigm of surface confinement via nonspecific interactions and enabled DNA origami folding to proceed in a solution-like environment. Importantly, our strategy retains the key advantages of surface-mediated self-assembly. For example, surface-anchored oligonucleotides could sequence-specifically initiate the growth of DNA origamis of specific sizes and shapes. Our work enables information to be encoded into a surface and expressed into complex DNA surface architectures for potential nanoelectronic and nanophotonic applications. In addition, our approach to surface confinement may facilitate the 2D self-assembly of other molecular components, such as proteins, as maintaining conformational freedom may be a general challenge in the self-assembly of complex structures at surfaces.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.9b09348.

    • Detailed notes on the effects of formamide on DNA–surface interactions in SMFS experiments, the effects of nonspecific interactions on folding at the surface, additional differences between folding in the solution phase and at the surface, additional SMFS/AFM data over different salt conditions, caDNAno designs, and DNA sequences (PDF)

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    Cited By

    This article is cited by 18 publications.

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