Abstract
AbstractDouble‐stranded DNA (dsDNA) fragments exhibit noncovalent attractive interactions between their tips. It is still unclear how DNA liquid crystal self‐assembly is affected by such blunt‐end attractions. It is demonstrated that stiff dsDNA fragments with moderate aspect ratio can specifically self‐assemble in concentrated aqueous solutions into different types of smectic mesophases on the basis of selectively screening of blunt‐end DNA stacking interactions. To this end, this type of attractions are engineered at the molecular level by constructing DNA duplexes where the attractions between one or both ends are screened by short hairpin caps. All‐DNA bilayer and monolayer smectic‐A type of phases, as well as a columnar phase, can be stabilized by controlling attractions strength. The results imply that the so far elusive smectic‐A in DNA rod‐like liquid crystals is a thermodynamically stable phase. The existence of the bilayer smectic phase is confirmed by Monte‐Carlo simulations of hard cylinders decorated with one attractive terminal site. This work demonstrates that DNA blunt‐ends behave as well‐defined monovalent attractive patches whose strength and position can be potentially precisely tuned, highlighting unique opportunities concerning the stabilization of nonconventional DNA‐based lyotropic liquid crystal phases assembled by all‐DNA patchy particles with arbitrary geometry and composition.
Highlights
Double-stranded DNA fragments exhibit noncovalent attractive terminate in a base-pair
The role of the weak blunt-end base stacking interactions in all-DNA lyotropic liquid crystals (LLC) self-assembly is investigated by both experiments and simulations
Our results unequivocally demonstrate that thermodynamically stable bilayer (Smb-A) and monolayer (Smm-A) smectic A-type of LLC phases in concentrated aqueoussaline solutions of rigid Double-stranded DNA (dsDNA) fragments can be stabilized by completely suppressing the attraction in the one (SC-duplex) or both (FC-duplex) tips of the DNA helices, respectively
Summary
Double-stranded DNA (dsDNA) fragments exhibit noncovalent attractive terminate in a base-pair (bp) These bluntend attractions originate from a combinainteractions between their tips. It is demonstrated that stiff dsDNA fragments with moderate aspect ratio can self-assemble in concentrated aqueous solutions into different types of smectic mesophases on the basis of selectively screening of blunt-end DNA stacking interactions. Together with the Watson–Crick base pairing[2] the blunt-end interactions are the most important contributions into the overall DNA double helix thermodynamic stability The existaddition, self-assembly studies on concentrated aqueous solutions of blunt-ended short B-form dsDNA and RNA helices have raised the hypothesis that these stacking forces could have influenced molecular evoence of the bilayer smectic phase is confirmed by Monte-Carlo simulations of lution in prebiotic environments.[4,5] More hard cylinders decorated with one attractive terminal site. Tional DNA-based lyotropic liquid crystal phases assembled by all-DNA patchy in the research area of DNA particles with arbitrary geometry and composition
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