Ambient silver concentration anomaly in the Finnish arctic lower atmosphere

Mean silver concentrations in weekly particle samples collected at Kevo, northern Finland, were determined for the period of October 1964-March 1978 by neutron activation analysis. Two distinct periods were observed in the silver concentration levels over this time frame. During 19641970, mean weekly silver concentration levels were found in the range of 0.01-190 ng/m(3) with an arithmetic mean of 2.19 ng/m(3). A few very high silver concentration levels (>10 ng/m(3)) were observed in this period, some of which simultaneously occurred with some of the highest bromine and iodine concentration levels. During 1971-1978, silver concentration levels were in the range of 0.02-0.89 ng/m(3) with a mean value of 0.09 ng/m(3). The observed concentration levels in the later period matched well the data from the early 1990s reported at Sevettijarvi, northern Finland, about 60 km east of Kevo. Data analysis, historical records for this region, and residence time analysis (RTA) using wind back-trajectories show that occasional smelting of silver-rich Norilsk ores at the Nikel smelter, Kola Peninsula, was probably a significant contributor to elevated mean silver concentration levels during 1964-1970. RTA alone was not able to unambiguously identify the most probable source region for highest silver impacts at Kevo due to the weekly integrated nature of the samples collected. Critical examination of wind back-trajectories (24 per day) for specific high silver, bromine, and iodine concentration weeks was carried out to supplement the ensemble RTA analysis (2 back-trajectories per day). The supplemental back-trajectory analysis revealed that deposition of the smelter component silver as well as the sea components (bromine and iodine) could occur together at Kevo during these weekly sampling periods. The study implies that data from weekly integrated samples are insufficiently time-resolved for RTA methods alone to unambiguously resolve the sources contributing to ambient atmospheric concentrations at Kevo, Finland.