Superficial and bottom sediment samples from 83 European mountain lakes, ranging from Norway to the Pyrenees and East Europe, were tested for estrogenic compounds by the recombinant yeast assay. The results showed widespread potential estrogenic activity arriving at remote lakes. Tatra Mountains (Slovakia) and Scotland Highlands were the regions with the highest prevalence of lakes with high estrogenic values. Comparison of the estrogenic activity in the superficial layer of sediments with pre-industrial age sections showed that estrogenic compounds were predominantly deposited in recent times. Chemical analysis showed that highly estrogenic sediments were significantly enriched in both polycyclic aromatic hydrocarbons (PAH) and organochlorine compounds. For PAH, enrichment ratios in highly estrogenic samples versus nonestrogenic ones were inversely correlated with the vapor pressure value for each compound, indicating a significant relationship between estrogenicity and accumulation of less volatile PAH. Two PAH of predominantly diagenetic origin, retene and perylene, did not show specific enrichment in estrogenic samples. Principal component analysis revealed a strong correlation between estrogenic activity and the presence of contaminants of anthropogenic origin. These data reveal significant amounts of estrogenic compounds in remote lakes, relate them to the overall human activity, and suggest that they may affect organisms inhabiting these ecosystems.

Abstract. Bulk atmospheric deposition samples were collected between 2004 and 2007 at four high-altitude European sites encompassing east (Skalnaté Pleso), west (Lochnagar), central (Gossenköllesee) and south (Redòn) regions, and analysed for legacy and current-use organochlorine compounds (OCs). Polychlorobiphenyls (PCBs) generally showed the highest deposition fluxes in the four sites, between 112 and 488 ng m −2 mo −1 , and hexachlorobenzene (HCB) the lowest, a few ng m −2 mo −1 . Among pesticides, endosulfans were found at higher deposition fluxes (11-177 ng m −2 mo −1 ) than hexachlorocyclohexanes (HCHs) (17-66 ng m −2 mo −1 ) in all sites except Lochnagar that was characterized by very low fluxes of this insecticide.

1. Sediment extracts from 63 European remote lakes were tested for the presence of ligands of the aryl hydrocarbon receptor (AhR), using a yeast-based bioassay. The lakes belong to different European mountain regions in Central Norway, Scotland, Piedmont (Italy), Tyrol (Austria and Italy) and the Julian Alps (Slovenia). 2. AhR ligand activity varied about 40-fold among the examined lakes, with Scotland having the highest proportion of lakes with high AhR ligand activity, whereas samples with low AhR ligand activity predominate in the Julian Alps. 3. AhR ligand activity in sediment samples correlated with the concentration of several environmentally relevant compounds, including polycyclic aromatic hydrocarbons, hexachlorobenzene and several polychlorobiphenyl ether congeners. These correlations suggest an anthropogenic origin for the detected AhR ligands, rather than being generated from natural processes. 4. We conclude that pollutants deposited in remote lakes by atmospheric processes are active AhR ligands at the concentrations found in these lakes. Given the high toxicity associated with ectopic activation of AhR in different animal systems, this activity may represent a significant risk for the exposed fauna.

Abstract. Bulk atmospheric deposition samples were collected between 2004 and 2007 at four high altitude European sites encompassing east (Skalnaté pleso), west (Lochnagar), central (Gossenköllesee) and south (Redòn) regions, and analysed for legacy and current-use organochlorine compounds (OCs). Polychlorobiphenyls (PCBs) generally showed the highest deposition fluxes in the four sites, between 112 and 488 ng m−2 mo−1, and hexachlorobenzene (HCB) the lowest, a few ng m−2 mo−1. Among pesticides, endosulfans were found at higher deposition fluxes (11–177 ng m−2 mo−1) than hexachlorocyclohexanes (HCHs) (17–66 ng m−2 mo−1) in all sites except Lochnagar that was characterized by very low fluxes of this insecticide. Comparison of the present measurements with previous determinations in Redòn (1997–1998 and 2001–2002) and Gossenköllesee (1996–1998) provided for the first time an assessment of the long-term temporal trends in OC atmospheric deposition in the European background areas. PCBs showed increasing deposition trends while HCB deposition fluxes remained nearly constant. Reemission of PCBs from soils or as consequence of glacier melting and subsequent precipitation and trapping of the volatilized compounds may explain the observed PCB trends. This process does not occur for HCB due to its high volatility which keeps most of this pollutant in the gas phase. A significant decline of pesticide deposition was observed during this studied decade (1996–2006) which is consistent with the restriction in the use of these compounds in most of the European countries. In any case, degassing of HCHs or endosulfans from ice melting to the atmosphere should be limited because of the low Henry's law constants of these compounds that will retain them dissolved in the melted water. Investigation of the relationship between air mass trajectories arriving at each site and OC deposition fluxes showed no correlation for PCBs, which is consistent with diffuse pollution from unspecific sources as the predominant origin of these compounds in these remote sites. In contrast, significant correlations between current-use pesticides and air masses flowing from the south were observed in Gossenköllesee, Lochnagar and Redòn. In the case of Redòn, the higher proportion of air masses from the south occurred in parallel to higher temperatures, which did not allow to discriminating between these two determinant factors of pesticide deposition. However, in Gossenköllesee and Lochnagar, the relationship between pesticide concentration and southern air masses was univocal reflecting the impact of regions with intensive agricultural activities.