Aerosol-mediated transport of perfluorooctanoate (PFO) from a water body to the atmosphere and the subsequent emission of gas-phase perfluorooctanoic acid (PFOA) was investigated. The potential for this process to facilitate long-range transport of PFOA/PFO was assessed. In a laboratory experiment, aerosols were generated and collected from deionized, fresh, and ocean waters spiked with PFO and analyzed by LC-MS/MS. Gas-phase samples were also collected from the system and analyzed for PFOA. Aerosols were found to have significantly higher concentrations of PFO than the parent water body (< or = 80 times for ocean waters). The PFOA, at equilibrium with the PFO in the aqueous aerosol, partitioned rapidly (t 1/2 = 7.2 s) out of the aerosol droplet. This suggests that rainout rates are likely to be longer than previously hypothesized. These results imply that water bodies are not a permanent sink for atmospheric PFOA as previous studies have suggested. The occurrence of contamination in remote regions may not depend solely on the previously hypothesized indirect sources but also on the long-range transport, via the gas phase, of direct releases of PFOA to both the aquatic and atmospheric environments.