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Controlling Fragment Competition on Pathways to Addressable Self-Assembly

Madge, Jim; Bourne, David; Miller, Mark A.

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Authors

Jim Madge

David Bourne



Abstract

Addressable self-assembly is the formation of a target structure from a set of unique molecular or colloidal building-blocks, each of which occupies a defined location in the target. The requirement that each type of building-block appears exactly once in each copy of the target introduces severe restrictions on the combinations of particles and on the pathways that lead to successful self-assembly. These restrictions can limit the efficiency of self-assembly and the final yield of the product. In particular, partially formed fragments may compete with each other if their compositions overlap, since they cannot be combined. Here, we introduce a "completability" algorithm to quantify competition between self-assembling fragments and use it to deduce general principles for suppressing the effects of fragment incompatibility in the self-assembly of small addressable clusters. Competition originates from loops in the bonding network of the target structure, but loops may be needed to provide structural rigidity and thermodynamic stability. An optimal compromise can be achieved by careful choice of bonding networks and by promoting semi-hierarchical pathways that rule out competition between early fragments. These concepts are illustrated in simulations of self-assembly in two contrasting addressable targets of 20 unique components each.

Citation

Madge, J., Bourne, D., & Miller, M. A. (2018). Controlling Fragment Competition on Pathways to Addressable Self-Assembly. Journal of Physical Chemistry B (Soft Condensed Matter and Biophysical Chemistry), 122(42), 9815-9825. https://doi.org/10.1021/acs.jpcb.8b08096

Journal Article Type Article
Acceptance Date Sep 26, 2018
Online Publication Date Sep 26, 2018
Publication Date Oct 25, 2018
Deposit Date Sep 26, 2018
Publicly Available Date Sep 26, 2019
Journal Journal of Physical Chemistry B (Soft Condensed Matter and Biophysical Chemistry)
Print ISSN 1520-6106
Electronic ISSN 1520-5207
Publisher American Chemical Society
Peer Reviewed Peer Reviewed
Volume 122
Issue 42
Pages 9815-9825
DOI https://doi.org/10.1021/acs.jpcb.8b08096

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Copyright Statement
This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry B, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpcb.8b08096.







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