Probe molecule spectroscopy and hygroscopic growth curves characterize the morphology of surfactant-coated aerosol particles as a function of relative humidity (RH). This study focuses on particles composed of either potassium iodide or sodium chloride and sodium dodecyl sulfate (SDS). At high RH, these mixed particles assume a reverse micelle type structure, and at low RH, they comprise a solid core of either KI or NaCl coated with SDS and water. The deliquescence relative humidity (DRH) and efflorescence relative humidity (ERH) of the inorganic fraction of the mixed particles are very similar to those of the pure salts. The surface polarity and morphology sampled by the coumarin 314 probe molecule ranges from that of a water-organic interface to that of an ionic surface and depends strongly on the RH and the amount of SDS. When the SDS coverage of the droplet just prior to efflorescence reaches approximately one monolayer, a thin soap film persists on the surface to values of RH much lower than the ERH. Both the electronic spectroscopy and photoelectric charging efficiency show a separate efflorescence for this layer at RH < 5%. The spectroscopy further reveals that there is a hysteresis associated with this low RH phase transition for both KI and NaCl cores.