Plutonium isotopes and 241Am in the atmosphere of Lithuania: A comparison of different source terms

137Cs, 241Am and Pu isotopes collected in aerosol samples during 1994–2011 were analyzed with special emphasis on better understanding of Pu and Am behavior in the atmosphere. The results from long-term measurements of 240Pu/239Pu atom ratios showed a bimodal frequency distribution with median values of 0.195 and 0.253, indicating two main sources contributing to the Pu activities at the Vilnius sampling station. The low Pu atom ratio of 0.141 could be attributed to the weapon-grade plutonium derived from the nuclear weapon test sites. The frequency of air masses arriving from the North-West and North-East correlated with the Pu atom ratio indicating the input from the sources located in these regions (the Novaya Zemlya test site, Siberian nuclear plants), while no correlation with the Chernobyl region was observed. Measurements carried out during the Fukushima accident showed a negligible impact of this source with Pu activities by four orders of magnitude lower as compared to the Chernobyl accident. The activity concentration of actinides measured in the integrated sample collected in March–April, 2011 showed a small contribution of Pu with unusual activity and atom ratios indicating the presence of the spent fuel of different origin than that of the Chernobyl accident. ► Sources of artificial airborne radioactivity were examined. ► The main Pu source originated from the global fallout. ► Fukushima accident had no significant impact on the area. ► Pu atom ratio frequency distribution showed a new source. ► Among analyzed sources are Sellafield, Chernobyl, Novaya Zemlya and Semipalatinsk.