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Photoswitchable solvent-free DNA thermotropic liquid crystals toward self-erasable shape information recording biomaterials.

ABSTRACT: Soft thermotropic liquid crystals (TLCs) have advantages on processability and shape memory compared to hard solids and fluids. The development of photoswitchable soft TLCs based on biomolecules would afford reworkable shape information recording biomaterials for the areas requiring biocompatibility and degradability. In recent years, anhydrous DNA TLCs composed of DNA and ammonium surfactants have been receiving continuous attention. However, the photoswitchable phase transition has not been realized for soft DNA TLCs at room temperature, owing to the absence of functional ammonium surfactant. Herein, a new type of azobenzene-containing surfactant would be applied to the fabrication of soft DNA TLCs with photoresponsive physical properties. The double-chain design of the used surfactant and the use of DOAB as a dopant guarantee the soft state of DNA TLCs at r.t., which also facilitates the azobenzene isomerization by reducing the packing density of surfactants. With the assistance of photoisomerization of azobenzene, the reported DNA TLCs achieve reversible liquid crystal-isotropic liquid transition at temperatures below clearing points even at room temperature. The repeatable shape information recording and self-erasing tests indicate these DNA TLCs would be good shape information recording biomaterials in the future. This work also provides a useful strategy for designing photoresponsive soft biomaterials based on rigid biomolecules like DNA.

SUBMITTER: Zhang L

PROVIDER: S-EPMC8477207 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:We report that specific anions (of sodium salts) added to aqueous phases at molar concentrations can trigger rapid, orientational ordering transitions in water-immiscible, thermotropic liquid crystals (LCs; e.g., nematic phase of 4'-pentyl-4-cyanobiphenyl, 5CB) contacting the aqueous phases. Anions classified as chaotropic, specifically iodide, perchlorate, and thiocyanate, cause 5CB to undergo continuous, concentration-dependent transitions from planar to homeotropic (perpendicular) orientations at LC-aqueous interfaces within 20 s of addition of the anions. In contrast, anions classified as relatively more kosmotropic in nature (fluoride, sulfate, phosphate, acetate, chloride, nitrate, bromide, and chlorate) do not perturb the LC orientation from that observed without added salts (i.e., planar orientation). Surface pressure-area isotherms of Langmuir films of 5CB supported on aqueous salt solutions reveal ion-specific effects ranking in a manner similar to the LC ordering transitions. Specifically, chaotropic salts stabilized monolayers of 5CB to higher surface pressures and areal densities (12.6 mN/m at 27 Å(2)/molecule for NaClO(4)) and thus smaller molecular tilt angles (30° from the surface normal for NaClO(4)) than kosmotropic salts (5.0 mN/m at 38 Å(2)/molecule with a corresponding tilt angle of 53° for NaCl). These results and others reported herein suggest that anion-specific interactions with 5CB monolayers lead to bulk LC ordering transitions. Support for the proposition that these ion-specific interactions involve the nitrile group was obtained by using a second LC with nitrile groups (E7; ion-specific effects similar to 5CB were observed) and a third LC with fluorine-substituted aromatic groups (TL205; weak dipole and no ion-specific effects were measured). Finally, we also establish that anion-induced orientational transitions in micrometer-thick LC films involve a change in the easy axis of the LC. Overall, these results provide new insights into ionic phenomena occurring at LC-aqueous interfaces, and reveal that the long-range ordering of LC oils can amplify ion-specific interactions at these interfaces into macroscopic ordering transitions.

Project description:We report a study of the wetting and ordering of thermotropic liquid crystal (LC) droplets that are trapped (or "caged") within micrometer-sized cationic polymeric microcapsules dispersed in aqueous solutions of surfactants. When they were initially dispersed in water, we observed caged, nearly spherical droplets of E7, a nematic LC mixture, to occupy ?40% of the interior volume of the polymeric capsules [diameter of 6.7 ± 0.3 ?m, formed via covalent layer-by-layer assembly of branched polyethylenimine and poly(2-vinyl-4,4-dimethylazlactone)] and to contact the interior surface of the capsule wall at an angle of ?157 ± 11°. The internal ordering of LC within the droplets corresponded to the so-called bipolar configuration (distorted by contact with the capsule walls). While the effects of dodecyltrimethylammonium bromide (DTAB) and sodium dodecyl sulfate (SDS) on the internal ordering of "free" LC droplets are similar, we observed the two surfactants to trigger strikingly different wetting and configurational transitions when LC droplets were caged within polymeric capsules. Specifically, upon addition of SDS to the aqueous phase, we observed the contact angles (?) of caged LC on the interior surface of the capsule to decrease, resulting in a progression of complex droplet shapes, including lenses (? ? 130 ± 10°), hemispheres (? ? 89 ± 5°), and concave hemispheres (? < 85°). The wetting transitions induced by SDS also resulted in changes in the internal ordering of the LC to yield states topologically equivalent to axial and radial configurations. Although topologically equivalent to free droplets, the contributions that surface anchoring, LC elasticity, and topological defects make to the free energy of caged LC droplets differ from those of free droplets. Overall, these results and others reported herein lead us to conclude that caged LC droplets offer a platform for new designs of LC-droplet-based responsive soft matter that cannot be realized in dispersions of free droplets.

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Photoswitchable solvent-free DNA thermotropic liquid crystals toward self-erasable shape information recording biomaterials.

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