Tight cohesion between glycolipid membranes results from balanced water–headgroup interactions

Membrane systems that naturally occur as densely packed membrane stacks contain high amounts of glycolipids whose saccharide headgroups display multiple small electric dipoles in the form of hydroxyl groups. Experimentally, the hydration repulsion between glycolipid membranes is of much shorter range than that between zwitterionic phospholipids whose headgroups are dominated by a single large dipole. Using solvent-explicit molecular dynamics simulations, here we reproduce the experimentally observed, different pressure-versus-distance curves of phospholipid and glycolipid membrane stacks and show that the water uptake into the latter is solely driven by the hydrogen bond balance involved in non-ideal water/sugar mixing. Water structuring effects and lipid configurational perturbations, responsible for the longer-range repulsion between phospholipid membranes, are inoperative for the glycolipids. Our results explain the tight cohesion between glycolipid membranes at their swelling limit, which we here determine by neutron diffraction, and their unique interaction characteristics, which are essential for the biogenesis of photosynthetic membranes.