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Since the lipid raft model was developed at the end of the last century, itbecame clear that the specific molecular arrangements of phospholipidassemblies within a membrane have profound implications in a vast range ofphysiological functions. Studies of such condensed lipid islands in modelsystems using fluorescence and Brewster angle microscopies have shown a widerange of sizes and morphologies, with suggestions of substantial in-planemolecular anisotropy and mesoscopic structural chirality. Whilst thesevariations can significantly alter many membrane properties including itsfluidity, permeability, and molecular recognition, the details of the in-planemolecular orientations underlying these traits remain largely unknown. Here, weuse phase-resolved sum-frequency generation microscopy on model membranes ofphospholipid monolayers with mixed molecular chirality, which form micron-scalecircular domains of condensed lipids, to fully determine theirthree-dimensional molecular structure. We find that the domains possess curvedmolecular directionality with spiralling mesoscopic packing. By comparingdifferent enantiomeric mixtures, both the molecular and spiral turningdirections are shown to depend on the lipid chirality, but with a cleardeviation from mirror symmetry in the formed structures. This demonstratesstrong enantioselectivity in the domain growth process, which has potentialconnections to the evolution of homochirality in all living organisms as wellas implications for enantioselective drug design.

Spiralling molecular structures and chiral selectivity in model membranes