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Photocontrollable Crystallization at the Topological Defect of a Liquid Crystalline Droplet.

ABSTRACT: Photocontrollable crystallization at topological defects in a liquid crystal (LC) droplet was demonstrated. The molecules dissolved in a surfactant solution outside the LC droplet were moved into the droplet via light absorption. Nuclei emerged tens of seconds after light irradiation and moved toward the topological defect located at the droplet center, thus forming a branch-shaped crystal. This phenomenon was reproduced for multiple different molecules; photoinduced migration, nucleation, and crystal formation were discussed as a plausible mechanism.

SUBMITTER: Sakai Y

PROVIDER: S-EPMC8697613 | biostudies-literature | 2021 Dec

REPOSITORIES: biostudies-literature

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Photocontrollable Crystallization at the Topological Defect of a Liquid Crystalline Droplet.

Sakai Yota Y Kusaki Hinako H Katayama Kenji K

ACS omega 20211209 50

Photocontrollable crystallization at topological defects in a liquid crystal (LC) droplet was demonstrated. The molecules dissolved in a surfactant solution outside the LC droplet were moved into the droplet via light absorption. Nuclei emerged tens of seconds after light irradiation and moved toward the topological defect located at the droplet center, thus forming a branch-shaped crystal. This phenomenon was reproduced for multiple different molecules; photoinduced migration, nucleation, and c ...[more]

PMID: 34963986

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Project description:We report an investigation of ordering transitions that are induced in water-dispersed, micrometer-sized droplets of a thermotropic liquid crystal (LC) by the bacterial lipopolysaccharide endotoxin. We reveal that the ordering transitions induced by endotoxin - from a bipolar state of the droplets to a radial state - are strongly dependent on the size of the LC droplets. Specifically, as the diameters of the LC droplets increase from 2 μm to above 10 μm (in phosphate buffered saline with an ionic strength of 90 mM and a pH of 7.2), we measured the percentage of droplets exhibiting a radial configuration in the presence of 100 pg/mL endotoxin to decrease from 98 ± 1 % to 3 ± 2 %. In addition, we measured a decrease in either the ionic strength or pH of the aqueous phase to reduce the percentage of droplets exhibiting a radial configuration in the presence of endotoxin. These results, when interpreted within the context of a simple thermodynamic model that incorporates the contributions of elasticity and surface anchoring to the free energies of the LC droplets, lead us to conclude that (i) the elastic constant K24 plays a central role in determining the size-dependent response of the LC droplets to endotoxin, and (ii) endotoxin-triggered ordering transitions occur only under solution conditions (pH, ionic strength) where the combined contributions of elasticity and surface anchoring to the free energies of the bipolar and radial configurations of the LC droplets are similar in magnitude. Our analysis also suggests that the presence of endotoxin perturbs the free energies of the LC droplets by ~10-17 J/droplet, which is comparable to the standard free energy of self-association of ~103 endotoxin molecules. These results, when combined with prior reports of localization of endotoxin at the center of LC droplets, are consistent with the hypothesis that self-assembly of endotoxin within micrometer-sized LC droplets provides the driving force for the ordering transitions. Overall, these results advance our understanding of ordering transitions triggered by the interactions of analytes with LC droplets and, more broadly, provide guidance to the design of LC droplet systems as the basis of stimuli-responsive soft materials.

Dataset Information

Photocontrollable Crystallization at the Topological Defect of a Liquid Crystalline Droplet.

Publications

Photocontrollable Crystallization at the Topological Defect of a Liquid Crystalline Droplet.

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