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It has been unclear whether the role of water in the self-assembly of soft materials and biomolecules is influential or water is just a background medium. Here we investigate the correlation between hydration state of lipid membrane and structural phase transition of the membrane between lamellar and inverted-hexagonal phases, as an intermediate process of membrane fusion, by using the complementary techniques of X-ray scattering and terahertz (THz) spectroscopy. By comparing two lipid species, our results indicate that the structural changes of the lipid membrane depend on the behavior of the surrounding water, especially in the second hydration layer, in addition to the molecular shape of lipids. The water behaves differently at each membrane surface owing to the different hydrophilicities of the lipid head groups.
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