Fusion and fission of fluid amphiphilic bilayers

Abstract

The system water–oil (n-decane)–nonionic surfactant (C₁₂E₅) forms bilayer phases in a large concentration region, but, for a given oil-to-surfactant ratio, only in a narrow temperature range. In addition to the anisotropic lamellar phase (L_α) there is also, at slightly higher temperature, a sponge or L₃-phase where the bilayers build up an isotropic structure extending macroscopically in three dimensions. In this phase the bilayer mid-surface has a mean curvature close to zero and a negative Euler characteristic. In this paper we study how the bilayers in the lamellar and the sponge phase respond dynamically to sudden temperature changes. The monolayer spontaneous curvature depends sensitively on temperature and a change of temperature thus provides a driving force for a change in bilayer topology. The equilibration therefore involves kinetic steps of fusion/fission of bilayers. Such dynamic processes have previously been monitored by temperature jump experiments using light scattering in the sponge phase. These experiments revealed an extraordinarily strong dependence of the relaxation time on the bilayer volume fraction ϕ. At ϕ < 0.1 the relaxation times are so slow that experiments using deuterium nuclear magnetic resonance (²H-NMR) appear feasible. We here report on the first experiments concerned with the dynamics of the macroscopic phase transition sponge–lamellae by ²H-NMR. We find that the sponge-to-lamellae transition occurs through a nucleation process followed by domain growth involving bilayer fission at domain boundaries. In contrast, the lamellae-to-sponge transformation apparently occurs through a succession of uncorrelated bilayer fusion events.