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The molecular arrangement of lipids and proteins within biomembranes andmonolayers gives rise to complex film morphologies as well as regions ofdistinct electrical surface potential, topographical and electrostaticnanoscale domains. To probe these nanodomains in soft matter is a challengingtask both experimentally and theoretically. This work addresses the effects ofcholesterol, lipid composition, lipid charge, and lipid phase on the monolayerstructure and the electrical surface potential distribution. Atomic ForceMicroscopy (AFM) was used to resolve topographical nanodomains and Kelvin ProbeForce Microscopy (KPFM) to resolve electrical surface potential of thesenanodomains in lipid monolayers. Model monolayers composed ofdipalmitoylphosphatidylcholine (DPPC), 1,2-dioleoyl-sn-glycero-3-phosphocholine(DOPC), 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine (POPC),1,2-dioleoyl-sn-glycero-3-[phospho-rac-(3-lysyl(1-glycerol))] (DOPG),sphingomyelin, and cholesterol were studied. It is shown that cholesterolchanges nanoscale domain formation, affecting both topography and electricalsurface potential. The molecular basis for differences in electrical surfacepotential was addressed with atomistic molecular dynamics (MD). MD simulationsqualitatively match the experimental results, with 100s of mV difference inelectrostatic potential between liquid-disordered bilayer (Ld, less cholesteroland lower chain order) and a liquid-ordered bilayer (Lo, more cholesterol andhigher chain order). Importantly, the difference in electrostatic propertiesbetween Lo and Ld phases suggests a new mechanism by which membrane compositioncouples to membrane function.

Molecular Dynamics simulations and Kelvin Probe Force microscopy to study of cholesterol-induced electrostatic nanodomains in complex lipid mixtures