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Direct observation and rational design of nucleation behavior in addressable self-assembly

: Sajfutdinow, Martin; Jacobs, William M.; Reinhardt, Aleks; Schneider, Christoph; Smith, David M.

Fulltext ()

Proceedings of the National Academy of Sciences of the United States of America : PNAS 115 (2018), No.26, pp.E5877-E5886
ISSN: 0027-8424
ISSN: 1091-6490
Journal Article, Electronic Publication
Fraunhofer IZI ()
coarse-grained simulation; DNA nanotechnology; dynamic light scattering; nucleation; self-assembly

To optimize a self-assembly reaction, it is essential to understand the factors that govern its pathway. Here, we examine the influence of nucleation pathways in a model system for addressable, multicomponent self-assembly based on a prototypical “DNA-brick” structure. By combining temperature-dependent dynamic light scattering and atomic force microscopy with coarse-grained simulations, we show how subtle changes in the nucleation pathway profoundly affect the yield of the correctly formed structures. In particular, we can increase the range of conditions over which self-assembly occurs by using stable multisubunit clusters that lower the nucleation barrier for assembling subunits in the interior of the structure. Consequently, modifying only a small portion of a structure is sufficient to optimize its assembly. Due to the generality of our coarse-grained model and the excellent agreement that we find with our experimental results, the design principles reported here are likely to apply generically to addressable, multicomponent self-assembly. © 2018 National Academy of Sciences. All Rights Reserved.