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Ordering transitions in micrometer-thick films of nematic liquid crystals driven by self-assembly of ganglioside GM1.

ABSTRACT: We report an investigation of the self-assembly of the monosialoganglioside (GM(1)) at interfaces formed between aqueous solutions of 10 microM GM(1) (at 25 degrees C) and micrometer-thick films of the nematic liquid crystal (LC) 4'-pentyl-4-cyanobiphenyl (5CB). We observe the process of spontaneous transfer of GM(1) onto the interfaces to be accompanied by continuous ordering transitions within the micrometer-thick films of the LC. At saturation coverage, the GM(1) orders the LC in an orientation that is perpendicular to the interface, an orientation that is similar to that caused by phospholipids such as dilauroylphosphatidylcholine (DLPC). This result suggests an interaction between the LC and GM(1) that is dominated by the hydrophobic tails of the GM(1). Relative to DLPC, however, we observe the dynamics of the LC ordering transition driven by GM(1) to be slow (2 h for DLPC versus 100 h for GM(1)). To provide insight into the origins of the slow dynamics of the GM(1)-induced ordering transition in the LC, we performed two additional measurements. First, we quantified the time-dependent adsorption of GM(1) at the LC interface by using fluorescently-labeled GM(1). Second, we used the Langmuir-Schaefer method to transfer preorganized monolayers of GM(1) from an air-water interface to the aqueous-LC interface. Results obtained from these two experiments are consistent with a physical picture in which the final stages of spontaneous adsorption/ordering of GM(1) at the aqueous-LC interface dictate the dynamics of the LC ordering transition. This rate limiting process underlying the ordering transition was substantially accelerated by heating the system above the phase transition temperature of GM(1)(26 degrees C), suggesting that the phase state of the GM(1) micellar aggregates in bulk solution strongly influences the kinetics of the final stages of ordering/adsorption of GM(1) at the LC interface. Overall, these results and others presented in this manuscript reveal that it is possible to decorate interfaces of a nematic LC with GM(1), and that the assembly of GM(1) at these interfaces impacts the dynamic and equilibrium ordering of the LC.

SUBMITTER: Lin IH

PROVIDER: S-EPMC2778293 | biostudies-literature | 2009 Aug

REPOSITORIES: biostudies-literature

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Ordering transitions in micrometer-thick films of nematic liquid crystals driven by self-assembly of ganglioside GM1.

Lin I-Hsin IH Meli Maria-Victoria MV Abbott Nicholas L NL

Journal of colloid and interface science 20090408 1

We report an investigation of the self-assembly of the monosialoganglioside (GM(1)) at interfaces formed between aqueous solutions of 10 microM GM(1) (at 25 degrees C) and micrometer-thick films of the nematic liquid crystal (LC) 4'-pentyl-4-cyanobiphenyl (5CB). We observe the process of spontaneous transfer of GM(1) onto the interfaces to be accompanied by continuous ordering transitions within the micrometer-thick films of the LC. At saturation coverage, the GM(1) orders the LC in an orientati ...[more]

PMID: 19428021

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Project description:We report that phospholipid vesicles incorporating ligands, when captured from solution onto surfaces presenting receptors for these ligands, can trigger surface-induced orientational ordering transitions in nematic phases of 4'-pentyl-4-cyanobiphenyl (5CB). Specifically, whereas avidin-functionalized surfaces incubated against vesicles composed of 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC) were observed to cause the liquid crystal (LC) to adopt a parallel orientation at the surface, the same surfaces incubated against biotinylated vesicles (DOPC and 1,2-dioleoyl-sn-glycero-3-phosphoethanolamine-N-(biotinyl) (biotin-DOPE)) caused the homeotropic (perpendicular) ordering of the LC. The use of a combination of atomic force microscopy (AFM), ellipsometry and quantitative fluorimetry, performed as a function of vesicle composition and vesicle concentration in solution, revealed the capture of intact vesicles containing 1% biotin-DOPE from buffer at the avidin-functionalized surfaces. Subsequent exposure to water prior to contact with the LC, however, resulted in the rupture of the majority of vesicles into interfacial multilayer assemblies with a maximum phospholipid loading set by random close packing of the intact vesicles initially captured on the surface (5.1 ± 0.2 phospholipid molecules/nm(2)). At high concentrations of biotinylated lipid (>10% biotin-DOPE) in the vesicles, the limiting lipid loading was measured to be 4.0 ± 0.3 phospholipid molecules/nm(2), consistent with the maximum phospholipid loading set by the spontaneous formation of a bilayer during incubation with the biotinylated vesicles. We measured the homeotropic ordering of the LC on the surfaces independently of the initial morphology of the phospholipid assembly captured on the surface (intact vesicle, planar multilayer). We interpret this result to infer the reorganization of the phospholipid bilayers either prior to or upon contact with the LCs such that interactions of the acyl chains of the phospholipid and the LC dominate the ordering of the LC, a conclusion that is further supported by quantitative measurements of the orientation of the LC as a function of the phospholipid surface density (>1.8 molecules/nm(2) is required to cause the homeotropic ordering of the LC). These results and others presented herein provide fundamental insights into the interactions of phospholipid-decorated interfaces with LCs and thereby provide guidance for the design of surfaces on which phospholipid assemblies captured through ligand-receptor recognition can be reported via ordering transitions in LCs.

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.

Dataset Information

Ordering transitions in micrometer-thick films of nematic liquid crystals driven by self-assembly of ganglioside GM1.

Publications

Ordering transitions in micrometer-thick films of nematic liquid crystals driven by self-assembly of ganglioside GM1.

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