Despite the central role of Na + and K + in physiological processes, it is still unclear whether they interact or alter physical properties of simple zwitterionic phospholipid bilayers at physiologically relevant concentrations. Here we report a difference in membrane permeability between Na + and K + , as measured with electrical impedance spectroscopy and tethered bilayer lipid membranes. We reveal that the differences in membrane permeability originate from distinct ion coordination by carbonyl oxygens at the phospholipid-water interface, altering the propensity for bilayer pore formation. Molecular Dynamics simulations showed differences in the coordination of Na + and K + at the phospholipid-water interface of zwitterionic phospholipid bilayers. The ability of Na + to conscript more phospholipids with a greater number of coordinating interactions causes a higher localised energy barrier for pore formation. These results provide evidence that ion specific interactions at the phospholipidwater interface can modulate physical properties of zwitterionic phospholipid bilayers.
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