Liquid droplets at interfaces may exhibit zero or nonzero contact angles corresponding to complete and partial wetting, respectively. As one varies a certain control parameter such as temperature or liquid composition, the system may undergo a transition from complete to partial wetting. Such transitions have been found and intensively studied for fluid-fluid interfaces in binary mixtures 1 and for liquids at solid substrates.2 Furthermore, liquid droplets at chemically patterned or topographically structured substrate surfaces can undergo morphological wetting transitions, 3 which reflect the freedom of contact angles for pinned contact lines.
4In this article, we provide the first experimental evidence that a transition between complete and partial wetting can also occur for an aqueous solution encapsulated within a lipid vesicle, i.e., for an aqueous solution in contact with a freely suspended lipid membrane.Lipid vesicles have long been recognized as models for the cell membrane and have been widely applied to study properties of lipid membranes.5 Recently, it has been found that giant unilamellar vesicles (several tens of microns in size and encapsulating volumes on the order of picoliters) loaded with aqueous solutions of watersoluble polymers may exhibit several spatial compartments formed by phase separation within the vesicle interior. 6,7 Thus, these artificial cell-like systems are a biomimetic setup for studying molecular crowding, fractionation, and protein sorting in cells. 6 We encapsulate an aqueous solution composed of 4.05% poly-(ethyleneglycol) (PEG) (molecular weight 8000 g/mol) and 2.22% dextran (molecular weight between 400 and 500 kDa) within giant vesicles, where 0.52% of the total dextran is labeled with fluorescein isothiocyanate and the composition of the aqueous solution is given in weight fractions. This solution is in the one-phase state at room temperature (see phase diagram in the Supporting Information). The vesicles are prepared in this solution using the method of electroformation (see Supporting Information). The membrane consists of 95.9% 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC), 4.0% galbeta1-3galnacbeta1-4(neuacalpha2-3)galbeta1-4glcbeta1-1′-cer (G M1 Ganglioside) and 0.1% 1,2-dipalmitoyl-sn-glycero-3-phosphoethanolamine-N-(lissamine rhodamine B sulfonyl) (DPPE-Rhod) with the membrane composition given in mole fractions.In order to obtain vesicles containing two phases, we raise the polymer concentration above the binodal (see Supporting Information) by deflation, i.e., by exposing the vesicles to a hypertonic medium. In order to balance the resulting osmotic pressure, water is forced out of the vesicle, the polymer concentration inside increases and phase separation occurs. To eliminate the fluorescence signal outside the vesicles and to make them sediment to the bottom of the chamber, they were first diluted in an isotonic solution containing 4.41% PEG and 1.45% dextran. The osmolarity of the medium was then increased stepwise (in 10-20% osmotic increments) by i...