Regulating the Polymerization of DNA Structures via Allosteric Control of Monomers

Abstract

Regulation of self-assembly is crucial in constructing structural biomaterials, such as tunable DNA nanostructures. Traditional tuning of self-assembled DNA nanostructures was mainly conducted by introducing external stimuli after the assembly process. Here, we explored the allosteric assembly of DNA structures via introducing external stimuli during the assembly process to produce structurally heterogeneous polymerization products. We demonstrated that ethidium bromide (EB), a DNA intercalator, could increase the left-handed out-of-plane chirality of curved DNA structures. Then, EB and double strands were introduced as competing stimuli to transform monomers into allosteric conformations, leading to three different polymerization products. The steric trap between different polymerization products promoted the polymerized structures to keep their geometric properties, like chirality, under varying intensity of external stimuli. Our strategy harnesses allosteric effects for assembly of DNA-based materials and is expected to expand the design space for advanced control in synthetic materials.

Endogenous miRNA and K+ Co-Activated Dynamic Assembly of DNA Coacervates for Intracellular miRNA Imaging and Mitochondrial Intervention

“…Most coacervates rely on polyelectrolyte interactions, and interactions between highly programmable molecules are rarely studied. DNA is an ideal highly programmable biomaterial to construct static or dynamic nanostructures due to its outstanding biocompatibility and addressability. − For example, Walther and his co-workers reported temperature-induced poly­(adenine)-rich ssDNA LLPS behavior, forming droplets with well-defined structures . Unfortunately, the method requires high-temperature annealing and is unsuitable for biological applications.…”

Programming the morphology of DNA origami crystals by magnesium ion strength

“…In crystallization of DNA tensegrity triangles, changes in the Mg 2+ strength impact the structure of resulting crystals by affecting the monomer arrangement propensities ( 40 ), and additionally, can dynamically induce the crystal expansion and contraction ( 41 ). Furthermore, related studies have elucidated the role of Mg 2+ and ethidium bromide (EB) in the complete formation and heterogeneous polymerization of DNA origami constructs ( 42 , 43 ). Building upon these studies, our work shows that Mg 2+ -dictated phase transitions impart allosterism on the shape of the DOF crystals, wherein SH and FCC lattices externally express hexagonal prism (HP) crystals and crystals characterized by triangular facets (CCTF), respectively.…”