We have investigated the shear-induced ordering of multilamellar vesicles (onions) in a nonionic surfactant (C(12)E(4)) system using a small-angle light scattering (shear-SALS) and a small-angle X-ray scattering (shear-SAXS) technique. In a narrow shear rate-temperature space, the onions form a two-dimensional (2D) hexagonally close-packed structure that shows characteristic hexagonal scattering patterns in both SALS and SAXS. In the dynamic phase diagram, the ordered onion phase is surrounded by disordered onion phase, indicating reentrant behavior against the temperature. The disorder-order transition is accompanied by a jump in onion size by a factor of 5-6. In the disordered onion phase, by applying a shear flow, the planar lamellar membranes transform to an intermediate structure, multilamellae cylinders or a coherent stripe buckling, and then the intermediate structure develops to the isotropic onions. On the other hand, in the ordered onion phase, the intermediate structure breaks to onions stretched in the shear velocity direction, and then the stretched onions aligned gradually to form the 2D hexagonal close packing.
We have investigated the entropic interactions between lamellar membranes and spherical colloidal particles using a small-angle neutron scattering (SANS) technique. By adding colloidal particles between lamellar sheets, the first lamellar peaks in SANS profiles become intense and the second and higher order Bragg peaks begin to appear, indicating that the membrane fluctuations are suppressed by the colloidal particles. We estimate the interlamellar interaction potential in the presence of the colloidal particles from the layer compressibility obtained by the SANS profile analysis and propose a phenomenological free energy model based on the restriction of membrane fluctuations. By further addition of the colloidal particles, the lamellar membranes transform to prolate micelles. In order to release the strong frustration due to the restriction of membrane fluctuations, the surfactant assemblies change the morphology from the two dimensional sheets to the one dimensional prolate micelles.
The effects of colloidal particles confined between lamellar membrane slits on interlamellar interactions have been investigated by small-angle neutron scattering. On addition of colloidal particles to a lamellar phase composed of a non-ionic surfactant, the first lamellar peak becomes sharper and higher-order peaks appear. Thus the colloidal particles suppress undulation fluctuations of lamellar membranes by their steric hindrance, which results in a repulsive interlamellar interaction. As the interlamellar distance decreases, the position of the Bragg peak shifts towards higher q [where q is the magnitude of scattering vector, given by q ¼ ð4=Þ sin , where 2 is the scattering angle and is the wavelength] and the peak intensity weakens. This tendency is completely opposite to the behavior of non-ionic surfactant lamellar phases, where the interlamellar interaction is governed by the Helfrich interaction. A phenomenological free-energy model is proposed based on the restriction of membrane fluctuations by colloidal particles. This model describes the experimental results well.
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