Article Hierarchical Self-Assembly of Disulfide-Linked Single-Stranded DNA into Stimuli-Responsive Pods

Volkan Kilinc ; Linawati Sutrisno SAMURAI ORCID (National Institute for Materials Science) ; Joel Henzie SAMURAI ORCID (National Institute for Materials Science) ; Emmanuel Picheau (National Institute for Materials Science) ; Yusuke Yamauchi ; Katsuhiko Ariga SAMURAI ORCID (National Institute for Materials Science) ; Jonathan P. Hill SAMURAI ORCID (National Institute for Materials Science)

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Volkan Kilinc, Linawati Sutrisno, Joel Henzie, Emmanuel Picheau, Yusuke Yamauchi, Katsuhiko Ariga, Jonathan P. Hill. Hierarchical Self-Assembly of Disulfide-Linked Single-Stranded DNA into Stimuli-Responsive Pods. Chemistry of Materials. 2026, 38 (4), 1968-1979. https://doi.org/10.1021/acs.chemmater.5c03128

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(abstract)

Controlling the large-scale assembly of charged biopolymers is a fundamental challenge in materials chemistry. Here, we report a chemical strategy that uses disulfide-linked single-stranded DNA (ssDNA) dimers as unique building blocks to drive the hierarchical self-assembly of functional DNA microstructures. Formed from short, random-sequence oligomers, these dimers first organize into DNA-salt composite nanobead condensates, which then serve as scaffolds for the assembly of uniform, microrod-shaped DNA condensates called DNA-pods. The key innovation of this work is the material's unique, cooperative structural transition. Upon thermal stimulation (>60 °C), dsDNA-pods undergo a rapid exfoliation into an expanded ssDNA network, a process driven by significant gains in configurational entropy and the relief of electrostatic repulsion. This establishes a new, accessible strategy for creating stimuli-responsive DNA materials through a chemistry-driven, sequence-independent pathway. We further demonstrate that these materials act as robust host matrices for encapsulating guest molecules like doxorubicin.

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Keyword: Stimuli-responsive DNA pods

Date published: 2026-02-24

Publisher: American Chemical Society (ACS)

Journal:

  • Chemistry of Materials (ISSN: 15205002) vol. 38 issue. 4 p. 1968-1979

Funding:

  • Ministry of Education, Culture, Sports, Science and Technology
  • Ministry of Education, Culture, Sports, Science and Technology JPMJER2003
  • Australian National Fabrication Facility
  • Ministry of Education, Culture, Sports, Science and Technology 20K05453
  • Ministry of Education, Culture, Sports, Science and Technology JP25H00898

Manuscript type: Publisher's version (Version of record)

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First published URL: https://doi.org/10.1021/acs.chemmater.5c03128

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Updated at: 2026-03-16 10:32:36 +0900

Published on MDR: 2026-03-16 17:54:57 +0900

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