Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 48, Pages 20296-20301Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c09503
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Funding
- Associazione Italiana per la Ricerca sul Cancro, AIRC [21965]
- European Research Council, ERC [819160]
- Italian Ministry of Education and Research [2017E44A9P]
- European Union [896962]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC-0010595]
- Marie Curie Actions (MSCA) [896962] Funding Source: Marie Curie Actions (MSCA)
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The study demonstrates a strategy to allow for the spontaneous reconfiguration of self-assembled DNA polymers using RNA as chemical fuel. By designing orthogonally addressable DNA building blocks, the researchers can temporarily deactivate and reactivate the building blocks to control the final composition of the polymer. This approach suggests a novel route towards developing biomolecular materials that support autonomous spatial reorganization of multiple components through engineered chemical reactions.
We demonstrate a strategy that allows for the spontaneous reconfiguration of self-assembled DNA polymers exploiting RNA as chemical fuel. To do this, we have rationally designed orthogonally addressable DNA building blocks that can be transiently deactivated by RNA fuels and subtracted temporarily from participation in the self-assembly process. Through a fine modulation of the rate at which the building blocks are reactivated we can carefully control the final composition of the polymer and convert a disordered polymer in a higher order polymer, which is disfavored from a thermodynamic point of view. We measure the dynamic reconfiguration via fluorescent signals and confocal microscopy, and we derive a kinetic model that captures the experimental results. Our approach suggests a novel route toward the development of biomolecular materials in which engineered chemical reactions support the autonomous spatial reorganization of multiple components.
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