Water activity in lamellar stacks of lipid bilayers: "Hydration forces" revisited

Water activity and its relationship with interactions stabilising lamellar stacks of mixed lipid bilayers in their fluid state are investigated by means of osmotic pressure measurements coupled with small-angle x-ray scattering. The (electrically-neutral) bilayers are composed of a mixture in various proportions of lecithin, a zwitterionic phospholipid, and Simulsol, a non-ionic cosurfactant with an ethoxylated polar head. For highly dehydrated samples the osmotic pressure profile always exhibits the "classical" exponential decay as hydration increases but, depending on Simulsol to lecithin ratio, it becomes either of the "bound" or "unbound" types for more water-swollen systems. A simple thermodynamic model is used for interpreting the results without resorting to the celebrated but elusive "hydration forces"Comment: 24 pages, 12 figures. Accepted for publication in The European Physical Journal

The study the properties structurals and elastics of phases lamellar of lipid.

Lamellar systems composed of lipid bilayers have been widely used as model system\ud for investigating properties of biological membranes, interactions between membranes and with biomolecules. The composition of the membrane determines its\ud three dimensional shape and its properties such as rigidity and compressibility\ud which play an important role on membrane fusion, protein adhesion, interactions\ud between proteins, etc. We present a systematic study of a lamellar system composed of lecithin and a commercial co-surfactant (Simusol), which is a mixture of\ud ethoxylated fatty acids. Using X ray scattering and a new procedure to fit X-ray\ud experimental data, we determine relevant parameters characterizing the lamellar\ud structure, varying membrane composition from 100% of lecithin to 100% of Simulsol. We present experimental data illustrating the swelling behavior for the membrane of different compositions and the respective behavior of the Caillé parameter.\ud From and GISAXS experiments on oriented films under controlled humidity we investigate the compressibility of the lamellar phase and the effect of incorporating\ud co-surfactant. Combining the Caillé parameter and compressibility studies we determine the bending rigidity of membranes. The results obtained with this experimental approach and new procedure to fit X-ray experimental allows us to identify\ud structural changes in the bilayer depending both on hydration and co-surfactant\ud content, with implications on elastic properties of membranes

Disordered protein-graphene oxide co-assembly and supramolecular biofabrication of functional fluidic devices

Supramolecular chemistry offers an exciting opportunity to assemble materials with molecular precision. However, there remains an unmet need to turn molecular self-assembly into functional materials and devices. Harnessing the inherent properties of both disordered proteins and graphene oxide (GO), we report a disordered protein-GO co-assembling system that through a diffusion-reaction process and disorder-to-order transitions generates hierarchically organized materials that exhibit high stability and access to non-equilibrium on demand. We use experimental approaches and molecular dynamics simulations to describe the underlying molecular mechanism of formation and establish key rules for its design and regulation. Through rapid prototyping techniques, we demonstrate the system's capacity to be controlled with spatio-temporal precision into well-defined capillary-like fluidic microstructures with a high level of biocompatibility and, importantly, the capacity to withstand flow. Our study presents an innovative approach to transform rational supramolecular design into functional engineering with potential widespread use in microfluidic systems and organ-on-a-chip platforms

Stabilising lamellar stacks of lipid bilayers with soft confinement and steric effects

Structure and interactions stabilising the lamellar stack of mixed lipid bilayers in their fluid state are investigated by means of small-angle X-ray scattering. The (electrically neutral) bilayers are composed of a mixtures of lecithin, a zwitterionic phospholipid, and Simulsol, a non-ionic cosurfactantwith an ethoxylated polar head. The soft confinement of the bilayer hydrophilic components is varied by changing hydration and bilayer composition, as well as the length of the cosurfactant polar head. Structural transitions are observed at low hydration, in the stacking order for the longer cosurfactant,and in the mixed bilayers for the shorter one. At higher hydration, the swelling of the lamellar stacks occurs with a significant, but continuous evolution in the mixed bilayer structure. The bilayer structural changes are discussed in analogy with the so-called “brush-to-mushroom” transition induced by lateralconfinement, relevant for long linear polymers grafted onto rigid surfaces, taking also into account the role of vertical confinement