Molecular assemblies of highly PEG-ylated phospholipids are important in many biomedical applications. We study sterically stabilized micelles (SSM) of self-assembled DSPE-PEG2000 in pure water and isotonic HEPES buffered saline solution. The observed SSM sizes of 2 – 15 nm largely depend on the solvent and the lipid concentration used. The critical micelle concentration (CMC) of DSPE-PEG2000 is ≈ 10 times higher in water than in buffer and the viscosity of the dispersion dramatically increases with the lipid concentration. To explain the experimentally observed results, we perform atomistic molecular dynamics simulations of the solvated SSM. Our modeling reveal that the observed assemblies have very different aggregation numbers of Nagg ≈ 90 (saline solution) and Nagg < 8 (water), due to very different screening of their charged −PO4− groups. We also demonstrate that the micelle cores can inflate and their corona highly fluctuate, allowing thus storage and delivery of molecules with different chemistry.

the explicit bilayer ensembles are in very good agreement with experiment. (Crossing angles from the implicit simulations are incorrect.) The predicted helix packing residues differ from experiment. It is possible the 100 ns simulation times are insufficient for a sampling of helix rotation and thereby a satisfactory determination of the residues involved in helix-helix packing.