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Spatial distribution of polychlorinated naphthalenes in air over the Great Lakes and air‐water gas exchange in Lake Ontario

High‐volume air sample were collected during research cruises of Lake Superior in August 1996 and May 1977 and of Lake Ontario (North America) in July and September 1998 and June 2000 and analyzed for polychlorinated naphthalenes (PCNs). Levels of tetra‐ to octachloronaphthalene (ΣPCN) varied spatially, with mean values (±SD) of 1.78 ± 0.74 and 1.46 ± 1.07 pg m−3 for Lake Superior in 1996 and 1997, respectively, and of 5.53 ± 2.19 and 5.60 ± 2.24 pg m−3 for Lake Ontario in 1998 and 2000, respectively. Evaporative sources were predominant, although combustion marker congeners such as tetrachloronaphthalenes 44 and 29 and pentachloronaphthalene 54 were present in most samples and were enhanced relative to technical PCN mixtures. The ΣPCN concentrations were higher in Lake Ontario samples collected in the western half of the lake and when winds were from the west. Greater proportions of the population and industrial areas are located around the western part of Lake Ontario. Water‐air fugacity ratios, calculated from air and water samples collected in June 2000, indicate that the trichloronaphthalenes are volatilizing from Lake Ontario, whereas the tetrachloronaphthalenes are close to equilibrium and the net deposition of tetrachloronaphthalenes can occur when the urban air plume influences levels over the lake.