Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 144, Issue 27, Pages 12272-12279Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c03506
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Funding
- National Science and Engineering Research Council of Canada (NSERC)
- Australian Research Council (ARC)
- Fonds de Recherche Nature et Technologies (FRQNT)
- Canada Foundation for Innovation (CFI)
- Canada Research Chairs Program
- Canada Council for the Arts
- Cottrell Scholar of the Research Corporation
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The sequence and length of single-stranded DNA directly influence the self-assembly of sequence-defined DNA block copolymers. Changing only the sequence of DNA can result in different structures, and the secondary structure of poly(adenine) DNA strands drives a temperature-dependent polymerization and assembly mechanism.
The self-assembly of block copolymers is often rationalized by structure and microphase separation; pathways that diverge from this parameter space may provide new mechanisms of polymer assembly. Here, we show that the sequence and length of single-stranded DNA directly influence the self-assembly of sequence-defined DNA block copolymers. While increasing the length of DNA led to predictable changes in self assembly, changing only the sequence of DNA produced three distinct structures: spherical micelles (spherical nucleic acids, SNAs) from flexible poly(thymine) DNA, fibers from semirigid mixed-sequence DNA, and networked superstructures from rigid poly(adenine) DNA. The secondary structure of poly(adenine) DNA strands drives a temperature-dependent polymerization and assembly mechanism: copolymers stored in an SNA reservoir form fibers after thermal activation, which then aggregate upon cooling to form interwoven networks. DNA is often used as a programming code that aids in nanostructure addressability and function. Here, we show that the inherent physical and chemical properties of single-stranded DNA sequences also make them an ideal material to direct self-assembled morphologies and select for new methods of supramolecular polymerization.
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