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A dissipative pathway for the structural evolution of DNA fibres
Abstract
Biochemical networks interconnect, grow and evolve to express new properties as different chemical pathways are selected during a continuous cycle of energy consumption and transformation. In contrast, synthetic systems that push away from equilibrium usually return to the same self-assembled state, often generating waste that limits system recyclability and prevents the formation of adaptable networks. Here we show that annealing by slow proton dissipation selects for otherwise inaccessible morphologies of fibres built from DNA and cyanuric acid. Using single-molecule fluorescence microscopy, we observe that proton dissipation influences the growth mechanism of supramolecular polymerization, healing gaps within fibres and converting highly branched, interwoven networks into nanocable superstructures. Just as the growth kinetics of natural fibres determine their structural attributes to modulate function, our system of photoacid-enabled depolymerization and repolymerization selects for healed materials to yield organized, robust fibres. Our method provides a chemical route for error-checking, distinct from thermal annealing, that improves the morphologies and properties of supramolecular materials using out-of-equilibrium systems.
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“Because of the noncovalent nature of DNA nanostructures, they can be reconfigured using established strategies, including strand displacement,26 thermal annealing,105 and pH changes.106”
From Emerging Approaches to DNA Data Storage: Challenges and Prospects (2022) · cites this paper as [106]
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All‐in‐One Photoacid Generators with Green/Red‐light Responsiveness and Cooperative Functionality
Guo, H., Zhang, Z., Chen, Y., Yang, H., Deng, L., Dai, J., Cong, M., Wang, B., Qu, D., Zhu, W., et al. (2025) · Angewandte Chemie · doi:10.1002/ange.202425313 · Cited by 1
Fang, X., Zheng, J., Gao, W., Liu, Z., Li, X., Li, C., Gao, T., & Zhang, R. (2025) · Coordination Chemistry Reviews · doi:10.1016/j.ccr.2025.217525 · Cited by 1
Peng, S., Chang, Y., Zeng, X., Lai, R., Yang, M., Wang, D., Zhou, X., & Shao, Y. (2023) · Analytica Chimica Acta · doi:10.1016/j.aca.2022.340777 · Cited by 1
Optically Controlled Construction of Three‐Dimensional Protein Arrays
Liu, Q., Zhou, Y. J., Shaukat, A., Meng, Z., Kyllönen, D., Seitz, I., Langerreiter, D., Kuntze, K., Priimägi, A., Zheng, L., et al. (2023) · Angewandte Chemie · doi:10.1002/ange.202303880 · Cited by 1
Solra, M., Kapila, R., Das, S., Bhatt, P., & Rana, S. (2024) · Angewandte Chemie · doi:10.1002/ange.202400348 · Cited by 1
Large, tunable and reversible pH changes by spiropyran photoacidsPreprint
Wimberger, L., Prasad, S. K. K., Andréasson, J., Schmidt, T. W., & Beves, J. E. (2021) · doi:10.33774/chemrxiv-2021-gppx1-v2
Fuel-Driven Formation of Covalent Basket CagesPreprint
Badjić, J. D., Gunawardana, V. W. L., Finnegan, T. J., Ward, C. R., & Moore, C. E. (2022) · Research Square · doi:10.21203/rs.3.rs-1299975/v1
Metadata
- Authors
- Rizzuto, F. J., Platnich, C. M., Luo, X., Shen, Y., Dore, M. D., Lachance-Brais, C., Guarné, A., Cosa, G., & Sleiman, H. F.
- Affiliations
- McGill University (CA)
- Corresponding author
- Sleiman, Hanadi F.
- ORCID
- Venue
- Nature Chemistry
- Published
- 2021-08-09
- Volume
- 13
- Issue
- 9
- Pages
- 843-849
- ISSN
- 1755-4330 (ISSN-L)
- 1755-4349
- OpenAlex
- W3192049880
- Cited by
- 120
- References
- 48
- Citations by year
- 2026: 17 · 2025: 25 · 2024: 19 · 2023: 29 · 2022: 22 · 2021: 8
- FWCI
- 6.12
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Nature Chemistry (publishedVersion)
- PubMed (publishedVersion)
- Funders
- Canadian Institutes of Health Research
- Topics
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Advanced biosensing and bioanalysis techniques
- Physical Sciences › Materials Science › Biomaterials › Supramolecular Self-Assembly in Materials
- Physical Sciences › Chemistry › Organic Chemistry › Supramolecular Chemistry and Complexes
- Keywords
- cyanuric acid, dissipative systems, supramolecular polymerization, repolymerization, hierarchical assembly, error detection, single-molecule fluorescence microscopy
- MeSH terms
- DNA, Hydrogen-Ion Concentration, Indoles, Light, Triazines, Polymerization
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