8G. Lujanien_e et al. / <strong>Journal</strong> <strong>of</strong> <strong>Environmental</strong> <strong>Radioactivity</strong> xxx (2012) 1e10Fig. 8. An example <strong>of</strong> 72 h air mass backward trajectories ended at Vilnius sampling site at 19 UTC at 20, 500, 1000 m AGL on 29 January, 1997, on 06 June, 1999 and on 03 February,2001 for 4 analyzed sectors (modified after De Cort et al., 1998).239,240Pu,241Am, nBq/m350 239,240 Pu40302010241 Am137 Cs4321137Cs, µBq/m 3005 6 7 8 9 10 11 12 1 2 3 4 5 6 72005-2006Fig. 9. Activity concentrations <strong>of</strong> 239,240 Pu and 241 Am in monthly aerosol samples andmonthly average activity concentrations <strong>of</strong> 137 Cs in 2005e2006 in Vilnius.Fig. 10. Alfa-spectrum <strong>of</strong> Pu isotopes separated from aerosol samples collectedbetween 23 March and 15 April.Please cite this article in press as: Lujanien_e, G., et al., Radionuclides from the Fukushima accident in the air over Lithuania: measurement andmodelling approaches, <strong>Journal</strong> <strong>of</strong> <strong>Environmental</strong> <strong>Radioactivity</strong> (2012), doi:10.1016/j.jenvrad.2011.12.004
G. Lujanien_e et al. / <strong>Journal</strong> <strong>of</strong> <strong>Environmental</strong> <strong>Radioactivity</strong> xxx (2012) 1e10 9(Hirose and Sugimura, 1990). This is approximately the same levelas observed in the aerosol samples collected in Vilnius.The activity ratio <strong>of</strong> 238 Pu/ 239,240 Pu detected at the Fukushimasite was reported to be 2 (TEPCO, 2011). Assuming the backgroundratio equal to the global fallout determined on the basis <strong>of</strong> the longtermmeasurements at the Vilnius site (Lujanien_e et al., 2009) wecan estimate the contribution <strong>of</strong> the Fukushima plutonium bysimple calculations (Hirose and Sugimura, 1990) using thefollowing equation:Fð%Þ ¼100$ðR M R G Þ=ðR F R G Þwhere F is the Fukushima originated 239,240 Pu fraction, R M , R G and R Fare the measured, global fallout and Fukushima derived ratios <strong>of</strong>238 Pu/ 239,240 Pu, respectively. According to these estimations thecontribution <strong>of</strong> the Fukushima derived 239,240 Pu is 59% or 26.4nBq/m 3 .The mean activity concentration <strong>of</strong> 137 Cs found in Vilniusduring the studied period was 118 mBq/m 3 . The background 137 Csactivity concentration can be estimated from the sample collectedone week before the accident and it was 0.7 0.1 mBq/m 3 . Fromthese estimations the mean Fukushima originated 239,240 Pu/ 137 Csratio could be 2$10 4 . The activity ratio <strong>of</strong> 239,240 Pu/ 137 Cs in theChernobyl originated hot particles was 2$10 2 . A fractionationduring the long-distance transport may have resulted in thevariation <strong>of</strong> the ratio at different locations (Pöllänen et al., 1997;Hirose and Sugimura, 1990). Further analyses (ICPMS and AMS)are in progress, which will help to explain Pu origin in thissample.4. ConclusionsFrom the presented data on variations <strong>of</strong> activity concentrations<strong>of</strong> studied radionuclides, from the analyses <strong>of</strong> meteorologicalsituation, and on the basis <strong>of</strong> the modelling exercises we canconclude that the complicated air mass transport, different arrivaltime, arrival height and downward air mass transport resulted intwo maxima <strong>of</strong> 131 I and 137 Cs activity concentrations in the nearsurfaceatmosphere. An increase in the 131 I and 137 Cs activityconcentrations up to 3800 mBq/m 3 and up to 1070 mBq/m 3 wasobserved on 28 March e 1 April and up to 500 mBq/m 3 and up to1000 mBq/m 3 was found on 3e4 April, respectively. In addition to131 I and 137 Cs, traces <strong>of</strong> other radionuclides were detected, and 132 I,132 Te, 129 Te, 129m Te and 136 Cs among them. The comparison <strong>of</strong> theChernobyl and Fukushima accidents indicated the higher activityconcentration <strong>of</strong> radionuclides by 4 orders <strong>of</strong> magnitude anda broader spectrum <strong>of</strong> radionuclides in the Chernobyl plume ascompared to the Fukushima one. Large collected air volumesallowed us to determine for the first time in Europe the activityratio and concentration <strong>of</strong> Fukushima derived 238 Pu and 239,240 Puisotopes. Approximately twice higher Pu activity concentration asexpected, and 238 Pu/ 239,240 Pu ratio not typical either for globalfallout or the Chernobyl accident was found in the integratedaerosol sample.AcknowledgementsThis research was partially supported by the Structural Funds <strong>of</strong>EU - the Research and Development Operational Program fundedby the ERDF (project No. 26240220004). 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Radioact. 7, 1e16.Masson, O., Baeza, A., Bieringer, J., Brudecki, K., Bucci, S., Cappai, M., Carvalho, F.P.,Connan, O., Cosma, C., Dalheimer, A., Didier, D., Depuydt, G., De Geer, L.E., DePlease cite this article in press as: Lujanien_e, G., et al., Radionuclides from the Fukushima accident in the air over Lithuania: measurement andmodelling approaches, <strong>Journal</strong> <strong>of</strong> <strong>Environmental</strong> <strong>Radioactivity</strong> (2012), doi:10.1016/j.jenvrad.2011.12.004
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