Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 30, Pages 16693-16699Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202106010
Keywords
DNA; framework nucleic acid; FRET; hybridization kinetics; self-assembly
Categories
Funding
- National Natural Science Foundation of China [92056117, 21934007, 21904087, 22004058, 21834007]
- National Key R&D Program of China [2016YFA0400900]
- Science and Technology Commission of Shanghai Municipality [19ZR1474600]
- Postdoctoral Science Foundation of China [2018M641995]
- Key Research Program of Frontier Sciences [QYZDJ-SSW-SLH031]
- Open Large Infrastructure Research of CAS, Chinese Academy of Sciences
- LU Jiaxi International Team of the Chinese Academy of Sciences
- K. C. Wong Foundation at Shanghai Jiao Tong University
- Innovative research team of high-level local universities in Shanghai
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The limitations in engineering electric double layers in physiological fluids have hindered the extensive study of long-range electrostatic interactions beyond biomolecular interaction interfaces. However, experimental and theoretical studies have shown that long-range Coulomb interactions play a crucial role in DNA hybridizations. Encapsulating protein and gold nanoparticles with different charges allows for modulation of hybridization kinetics, potentially leading to new strategies for gene regulation and nucleic acid detection.
Long-range electrostatic interactions beyond biomolecular interaction interfaces have not been extensively studied due to the limitation in engineering electric double layers in physiological fluids. Here we find that long-range electrostatic interactions play an essential role in kinetic modulation of DNA hybridizations. Protein and gold nanoparticles with different charges are encapsulated in tetrahedral frameworks to exert diverse electrostatic effects on site-specifically tethered single DNA strands. Using this strategy, we have successfully modulated the hybridization kinetics in both bulk solution and single molecule level. Experimental and theoretical studies reveal that long-range Coulomb interactions are the key factor for hybridization rates. This work validates the important role of long-range electrostatic forces in nucleic acid-biomacromolecule complexes, which may encourage new strategies of gene regulation, antisense therapy, and nucleic acid detection.
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