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* Theoretical Molecular Biophysics Group, Max-Planck-Institute for Biophysical Chemistry, Göttingen, Germany; and Membrane Biophysics and Thermodynamics Group, Max-Planck-Institute for Biophysical Chemistry, Göttingen, Germany
Correspondence: Address reprint requests to H. Grubmüller, Tel.: 49-551-201-1763; Fax: 49-551-201-1089; E-mail: hgrubmu{at}gwdg.de; and T. Heimburg, Tel.: 49-551-201-1412; Fax: 49-551-201-1501; E-mail: theimbu{at}gwdg.de.
Electrostatic interactions govern structural and dynamical properties of membranes and can vary considerably with the composition of the aqueous buffer. We studied the influence of sodium chloride on a pure POPC lipid bilayer by fluorescence correlation spectroscopy experiments and molecular dynamics simulations. Increasing sodium chloride concentration was found to decrease the self-diffusion of POPC lipids within the bilayer. Self-diffusion coefficients calculated from the 100 ns simulations agree with those measured on a millisecond timescale, suggesting that most of the relaxation processes relevant for lipid diffusion are faster than the simulation timescale. As the dominant effect, the molecular dynamics simulations revealed a tight binding of sodium ions to the carbonyl oxygens of on average three lipids leading to larger complexes with reduced mobility. Additionally, the bilayer thickens by 
2 Å, which increases the order parameter of the fatty acyl chains. Sodium binding alters the electrostatic potential, which is largely compensated by a changed polarization of the aqueous medium and a lipid dipole reorientation.
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