We study the deformation of a lipid membrane in response to a local pH modification. Experimentally, a basic solution is microinjected close to a giant unilamellar vesicle. A local deformation appears in the zone of the membrane that is closest to the micropipette, and relaxes when the injection is stopped. A theoretical description of this phenomenon is provided. It fully takes into account the spatiotemporal evolution of the concentration of hydroxide ions during and after the microinjection, as well as the linear dynamics of the membrane. This description applies to a local injection of any substance that reacts reversibly with the membrane lipids. We compare experimental data obtained in the domain of small deformations to the results of our linear description, and we obtain a good agreement between theory and experiments. In addition, we present direct experimental observations of the pH profile on the membrane during and after the microinjection, using pHsensitive fluorescent lipids.
Molecular assembly systems that have autonomous reproduction and Darwinian evolution abilities can be considered as minimal cell-like systems. Here we demonstrate the reproduction of cell-sized vesicles composed of AOT, i.e., sodium bis-(2-ethylhexyl) sulfosuccinate, coupled with an enzymatic polymerisation reaction occurring on the surface of the vesicles. The particular reaction used is the horseradish peroxidase-catalysed polymerisation of aniline with hydrogen peroxide as oxidant, which yields polyaniline in its emeraldine salt form (PANI-ES). If AOT micelles are added during this polymerisation reaction, the AOT-PANI-ES vesicles interact with the AOT molecules in the external solution and selectively incorporate them in their membrane, which leads to a growth of the vesicles. If the AOT vesicles also contain cholesterol, the vesicles not only show growth, but also reproduction. An important characteristic of this reproduction system is that the AOT-based vesicles encourage the synthesis of PANI-ES and PANI-ES promotes the growth of AOT vesicles.
We have investigated shape deformations of binary giant unilamellar vesicles (GUVs) composed of cone- and cylinder-shaped lipids. By coupling the spontaneous curvature of lipids with the phase separation, we demonstrated pore opening and closing in GUVs. When the temperature was set below the chain melting transition temperature of the cylinder-shaped lipid, the GUVs burst and then formed a single large pore, where the cone shape lipids form a cap at the edge of the bilayer to stabilize the pore. The pore closed when we increased the temperature above the transition temperature. The pore showed three types of shapes depending on the cone-shaped lipid concentration: simple circular, rolled-rim, and wrinkled-rim pores. These pore shape changes indicate that the distribution of the cone- and cylinder-shaped lipids is asymmetric between the inner and outer leaflets in the bilayer. We have proposed a theoretical model for a two-component membrane with an edge of bilayer where lipids can transfer between two leaflets. Using this model, we have reproduced numerically the observed shape deformations at the rim of pore.
Development of self-reproducing vesicle systems is the first step for autopoietic cycles. We established a model self-reproducing vesicle system without the membrane molecule synthesis route. The model vesicle composed of cylinder- and inverse-cone-shaped lipids formed inclusion vesicles inside the mother vesicle, and the inclusion vesicles were then expelled by a temperature cycling. By changing the vesicle composition, the mother vesicles showed a budding-type self-reproduction pathway. A key concept of this system is the coupling of the main-chain transition and the shape of lipids.
It is very challenging to construct protocells from molecular assemblies. An important step in this challenge is the achievement of vesicle dynamics that are relevant to cellular functions, such as membrane trafficking and self-reproduction, using amphiphilic molecules. Soft matter physics will play an important role in the development of vesicles that have these functions. Here, we show that simple binary phospholipid vesicles have the potential to reproduce the relevant functions of adhesion, pore formation and self-reproduction of vesicles, by coupling the lipid geometries (spontaneous curvatures) and the phase separation. This achievement will elucidate the pathway from molecular assembly to cellular life.
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