DNA Framework‐Engineered Long‐Range Electrostatic Interactions for DNA Hybridization Reactions

Abstract

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.H ere we find that long-range electrostatic interactions play an essential role in kinetic modulation of DNAh ybridizations.P rotein and gold nanoparticles with different charges are encapsulated in tetrahedral frameworks to exert diverse electrostatic effects on sitespecifically tethered single DNAs trands.U sing 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.T his work validates the important role of long-range electrostatic forces in nucleic acid-biomacromolecule complexes,whichmay encourage new strategies of gene regulation, antisense therapy, and nucleic acid detection.

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“…Formula for ionisation degree of chains α = α max K a /[ k (K a / k + b*n + bath exp(‐φ))] (α max , welling degree; K a , acid dissociation constant; k , water molarity; b, a decrease in ionization degree driven by ion‐pairs; n + bath , positive ions fraction; φ is dimensionless electrostatic potential), accounts for screening of functional groups by surrounding segments and formation of ion‐pairs (Drozdov, Sanporean, & deClaville Christiansen, 2016). Types of anions (e.g., F − , Cl − , Br − and I − ), cations (Na + , K + and Li + ) and biopolymer (polyampholyte and polyelectrolyte) matter and have different screen effect on the electrostatic attractive forces, resulting in the various behaviours (Manning, 1969; Kudaibergenov, 1999; Lee & Chiu, 2002; Gao, Gawel, & Stokke, 2014), including swelling, collapsing and stability; high ionic strengths could largely screened charges (Wielema & Engberts, 1990; Qu et al ., 2021). Salt screens the charge repulsion on large scales that extends the chain of polyelectrolyte, and only at higher salt concentrations the charge attraction that compacts the polyampholyte locally, is screened, causing the chain to swell (Dobrynin, Colby, & Rubinstein, 2004).…”