137Cs and isotopic ratios of Pu and U in lichens and mosses from Russian Arctic areas.

Knowledge of past anthropogenic sources of radionuclide contamination in Russian Arctic areas is important to assess the radioecological situation of these less-studied regions. Therefore, we investigated the sources of radionuclide contamination in Russian Arctic in the 1990s. Lichen and moss samples were collected from 1993 to 1996 in Kola Peninsula, Franz Josef Land, and few other locations. The activity concentration of 137Cs was determined from the archived samples by gamma spectrometry in 2020. After radiochemical separation of Pu and U isotopes from the lichens and mosses, mass ratios 240Pu/239Pu, 234U/238U, 235U/238U, and 236U/238U were determined by mass spectrometry. 137Cs activity concentrations at the sampling date were found to vary from 3.1 ± 1.4 (Inari, Finnish-Russian border) to 303 ± 7 (Kola Peninsula) Bq/kg. The ranges of isotopic ratios were 0.0592 ± 0.0007 to 0.253 ± 0.082 for 240Pu/239Pu, (4.89 ± 3.91) × 10-5 to (6.86 ± 0.04) × 10-5 for 234U/238U, 0.0072104(21) to 0.007376(41) for 235U/238U, and from below 1 × 10-7 to (2.65 ± 0.19) × 10-6 for 236U/238U, respectively. Based on the measured isotopic ratios and characteristic isotopic ratios of known contamination sources, the main Pu and U sources in the sampled lichens and mosses are global fallout, the Chernobyl accident, and possibly local nuclear activities. These results contribute to further understanding of past nuclear events and resulting nuclear contamination in Russian Arctic terrestrial areas.

Evaluation of 137Cs, 133Xe and 3H activity concentrations monitored in the Arctic atmosphere.

This paper provides a brief introduction to the Arctic atmospheric radioactivity monitoring network. A decade of monitoring results have shown the 137Cs background levels in Arctic air range from 0.05 to 1.50 µBq/m3. The monitoring stations have sufficient sensitivity to detect 137Cs brought to the atmosphere due to resuspension in local soil and reemissions from biomass burning in a daily temporal resolution. These observations can be used as tracers for atmospheric processes. The 133Xe measurements obtained at Yellowknife, Resolute and Spitsbergen could support other research into how air pollution problems arise across intercontinental distances. It will help develop and improve models capable of predicting the long-distance transport and deposition of trace gases in the Arctic. Rainwater monitoring data collected in Finnish Lapland since the 1960's indicate that 3H radioactivity concentrations reached natural background levels in early 2000s, typically around 1-2 Bq/L monthly, with an annual seasonal variation cycle consistent with the observed of other cosmogenic radionuclides.

Sediment profile dating and reconstructing nuclear events from annually laminated lake sediments in northern Finland.

The sediments deposited in Lake Kevojärvi (69°45N, 27°00'E) in northernmost Finland were investigated for radioactivity. Freeze cores recovered from the 35-m deep basin has preserved a distinct succession of annual laminations deposited between 1909 and 2015. The basic varve structure is composed of a detrital snowmelt layer and an organic-rich post-snowmelt layer lying on top of the snowmelt layer. The past nuclear events have been preserved in the lake sediment. In order to study these, sediment freeze with annual sediment laminations were recovered from the lake bottom and measured for gamma emitting radionuclides. A total of 53 sediment subsamples, each incorporating sediment from one to two varves i.e. sediment deposited during one to two years, were taken for gamma spectroscopy measurements using low-background HPGe detector system. The measurements showed large variations in 137Cs and 241Am concentrations between different laminae marking different nuclear events in history. This highly resolved profile revealed a detailed record of anthropogenic radioactive fallout from atmospheric nuclear weapons testing during 1950s and 1960s and the Chernobyl accident in 1986. The measured 137Cs concentrations varied between 0.6 and 229 Bq/kg dry weight (dw) while the measured 241Am concentrations varied between 0.6 and 6.4 Bq/kg dw. The 137Cs showed downward migration in the sediment column since 137Cs was also found in varves dating before 1945. The first clear increase in 137Cs concentration was observed in 1956 varve and the 137Cs concentrations were found to peak in the 1964, 1970 and 1986 varves. The 241Am was first observed in 1957 varve and the concentrations peaked in 1960-1962, 1964 and 1970 varves. This demonstrated that 241Am can be a complementary chronostratigraphic marker to 137Cs in sediment. A time delay of one to two years was observed between the years of intensive atmospheric nuclear weapons testing and the increased 137Cs and 241Am concentrations in the sediment varves. In the 210Pb concentrations long-time periods of low (~1930-1950 and ~1990-2000) and high concentrations (~1950-1980) were observed. The reason for large variation was the amount of sediment input. The Constant rate of supply (CRS) model results showed good agreement with the varve counting. The model results showed that the 210Pb deposition has been constant over the last 80 years and no effect of climate change to the 210Pb deposition was observed.

Deposition of naturally occurring 7Be and 210Pb in Northern Finland.

This study presents observations of naturally occurring 7Be and 210Pb in total deposition collected in three deposition sampling stations located in three towns in Northern Finland at Rovaniemi, Sodankylä and Ivalo. The deposition samples were measured in three-month intervals and the collected data covered the years from 1991 to 2017 in Rovaniemi and the years from 1999 to 2017 in Sodankylä and Ivalo. The 7Be deposition was observed to be dependent on the amount of precipitation where higher amount of precipitation meant higher 7Be deposition. The 7Be deposition showed a distinctive seasonal cycle where the highest 7Be deposition values were observed occur during July-September and the lowest values during January-March. From the annual total deposition 72-84% occurred during the months of April-September (2nd and 3rd quarters). The precipitation normalized enrichment factor (α) determined the excess or deficiency of 7Be relative to the amount of rain. The most excess of 7Be in the deposition was observed during April-June (2nd quarter) while the most 7Be depleted precipitation occurred during January-March (1st quarter). The large excess of 7Be in precipitation during April-June (2nd quarter) was an indication of injections of 7Be rich stratospheric air into troposphere. By using simultaneously collected 7Be aerosol concentration data at Rovaniemi and Ivalo, the 7Be deposition velocities were determined. The deposition velocities (VD) were also found to have a strong seasonal cycle where low velocities were observed during winter and higher ones during summer. The 7Be deposition time series were also compared with other time series that are known to affect ground level 7Be aerosol concentrations. These were precipitation, sunspot number (SSN), galactic cosmic ray flux (GCR), Arctic Oscillation (AO), North Atlantic Oscillation (NAO) and Scandinavian Pattern (SCAND) indices. The Pearson correlation and wavelet coherence (WTC) was used to analyze possible correlations between the time series. The analyses showed that the coherences were location dependent. Rovaniemi 7Be deposition data correlated strongly with rain and weakly with the SCAND index at the 6-8 year scale. The Sodankylä 7Be deposition data correlated strongly with the precipitation and SSN and GCR and weakly with AO and NAO indices. Ivalo 7Be deposition data correlated with strongly with 7Be aerosol concentration data, SSN, GCR and NAO index and weakly with the AO index. The WTC analysis revealed anti-phase coherences with the AO and NAO indices at 4-6 year scale. The 210Pb deposition data was sparse and only available from 2011 onwards. 210Pb deposition had a seasonal cycle where higher deposition values were observed during summer and lower ones deposition during winter. The annual 210Pb deposition was determined at Rovaniemi and Sodankylä during 2014. The values of 7Be/210Pb ratio was found to vary significantly seasonally, higher 7Be/210Pb ratios were measured during summer and lower ones during winter.

Derivation and validation of a novel Semi Empirical Deposition Estimation Model (SEDEM).

Predictive models are necessary in order to minimize potential damages in the event of a nuclear or radiological release. For this reason, a novel model for the calculation of both wet and dry deposition from airborne radioactivity is proposed. Full derivation of the model and the estimation of uncertainty are presented, and the validity of the model is evaluated by calculating deposition based on several measured airborne activities in different countries. The results are compared with the corresponding measured deposition activities and the predictive power of the model is found to be good, i.e. calculated depositions being within the limits of measurement uncertainty. Additionally, limitations of the model and possible sources of error in the calculations are discussed.

Transfer factors and effective half-lives of (134)Cs and (137)Cs in different environmental sample types obtained from Northern Finland: case Fukushima accident.

The Fukushima NPP accident caused a small but detectable cesium fallout in northern Finland, of the order of 1 Bq/m(2). This fallout transferred further to soil, water, flora and fauna. By using modern HPGe detector systems traces of (134)Cs from the Fukushima fallout were observed in various samples of biota. In northern Finland different types of environmental samples such as reindeer meat, berries, fish, lichens and wolf were collected during 2011-2013. The observed (134)Cs concentrations varied from 0.1 Bq/kg to a few Bq/kg. By using the known (134)Cs/(137)Cs ratio observed in Fukushima fallout the increase of the Fukushima accident to the (137)Cs concentrations was found to vary from 0.06 % to 6.9 % depending on the sample type. The aggregated transfer factors (Tag) and effective half-lives (Teff) for (134)Cs and (137)Cs were also determined and then compared with known values found from earlier studies which are calculated based on the fallout from the Chernobyl accident. Generally, the Tag and Teff values determined in this study were found to agree with the values found in the earlier studies. The Teff values were sample-type specific and were found to vary from 0.91 to 2.1 years for (134)Cs and the estimates for (137)Cs ranged between 1.6 and 19 years. Interestingly, the ground lichens had the longest Teff whereas the beard lichen had the shortest. In fauna, highest Tag values were determined for wolf meat ranging between 1.0 and 2.2 m(2)/kg. In flora, the highest Tag values were determined for beard lichens, ranging from 1.9 m(2)/kg to 3.5 m(2)/kg.

Artificial radionuclides in surface air in Finland following the Fukushima Dai-ichi nuclear power plant accident.

We present observations of radionuclides released during the Fukushima Dai-ichi nuclear power plant accident in ambient air and in deposition made in Finland during March-May 2011. The first observed fission product was (131)I, which arrived in Finland 8-9 days after the accident. Detections of (137)Cs and (134)Cs were made 2-3 days after the first (131)I observations. The highest concentrations of fission products in Finland were observed during March 31st and April 1st. The highest observed concentrations of the following isotopes were: (131)I (10.6 ± 0.4 mBq/m(3)), (134)Cs (0.397 ± 0.020 mBq/m(3)), (137)Cs (0.405 ± 0.017 mBq/m(3)), (136)Cs (28 ± 2 µBq/m(3)), (129)Te (129 ± 9 µBq/m(3)), (129m)Te (234 ± 20 µBq/m(3)), (132)Te (51 ± 3 µBq/m(3)) and (132)I (54 ± 3 µBq/m(3)). Generally, higher concentrations of fission product were observed in Southern Finland than in Northern Finland. The variations in the (137)Cs and (134)Cs activity concentration data suggest that three separate plumes passed over Finland with decreasing concentrations. The first plume, with highest cesium concentrations, passed over Finland during March 31st - April 2nd, the second plume during April 4th - 6th and the third and smallest one during April 10th - April 11th. Both aerosol and gaseous iodine fractions were sampled simultaneously and thus an accurate view of the behaviour of aerosol and gaseous fractions was obtained. Large variations between different fractions were observed with the gaseous fraction representing 65-98% of the total (131)I. The (134)Cs/(137)Cs ratio was determined to be 0.99 ± 0.10, which indicates a fuel burnup of approximately 30 MWd/t. The (136)Cs/(137)Cs and (129m)Te/(132)Te ratios were used to estimate the time lapse after the accident. The differences between true time lapse and the ones deduced from the isotope ratios were from the correct time lapse to 0-3 days for (136)Cs/(137)Cs and 5 days for (129m)Te/(132)Te, respectively. Radionuclides from the Fukuhisma Dai-ichi nuclear power plant were also observed in deposition samples. In Norther Finland, the total deposition of 0.28-0.62 Bq/m(2) for (137)Cs and 0.21-0.57 Bq/m(2) for (134)Cs was determined during March-May 2011. For (131)I the deposition of 8.5 ± 2.9 Bq/m(2) was determined at Rovaniemi from the samples from the sample collected during April 1st - 12th.

Selected anthropogenic and natural radioisotopes in the Barents Sea and off the western coast of Svalbard.

The Murmansk Marine Biological Institute (MMBI) performed high-latitude expeditions to the Barents Sea during 2007-2009 where a scientist from the Radiation and Nuclear Safety Authority (STUK) participated. The aim of the expeditions was to study and map the current radiological situation throughout the Barents Sea. In the expeditions, samples of seawater, sediment and biota were collected for radioactivity studies. The (90)Sr and (137)Cs isotopes were analysed from the seawater samples and no spatial distribution in the concentrations of (90)Sr and (137)Cs was found. The sediment samples were analysed for γ-emitting isotopes. In the statistical analysis performed only the (90)Sr was found to have no spatial distribution. In the (137)Cs concentrations two areas containing higher concentrations were observed: one in the western part of Svalbard and another in Franz Victoria Trough near the Franz Josef Land archipelago. The increase in the western coast of Svalbard suggests an Atlantic influence while in the Franz Victoria Trough source regions are possibly more complex. Since (137)Cs in marine sediments mainly originates from terrestrial sources, finding higher concentrations in the northern part of the Barents Sea may also suggest a contribution of (137)Cs carried by the ocean currents and by sea ice from the outside Barents Sea. In addition to γ spectrometric measurements, the sediment samples were radiochemically analysed for (210)Pb. It was found that the unsupported fraction of (210)Pb showed significant spatial variation. The fraction of unsupported (210)Pb was reduced to 40-70% near Bear Island, Edge Island and in the Franz Josef Land archipelago. In these regions the sea is typically covered with sea ice during winter. The relatively low fraction of unsupported (210)Pb is possibly caused by blocking of wet and dry deposition of (210)Pb onto the sea by winter sea ice. In biota samples, only small traces, at the level of 0.2 Bq/kg w.w. of (137)Cs, were found. When the (137)Cs concentrations found in cod and in haddock were compared with studies done in the early 1990's an effective half-life of (137)Cs in cod and in haddock was deduced. For cod the estimated effective half-life of (137)Cs was between 5.8 and 7.5 years and for haddock between 5.3 and 9.5 years. Similarly, the concentrations of naturally occurring (210)Po and (210)Pb were from 0.1 to 0.3 Bq/kg w.w. The (210)Po/(210)Pb ratio varied from 1.8 to 30 indicating a more efficient bioaccumulation of (210)Po than its precursor (210)Pb. The dose to humans eating Barents Sea fish was estimated. Even for people consuming large quantities of Barents Sea fish the annual dose was found to be below 20 µSv. The effective dose from anthropogenic (137)Cs was found to be less than 1% compared to the dose caused naturally occurring (210)Po and (210)Pb.

Concentrations of (137)Cs in summer pasture plants that reindeer feed on in the reindeer management area of Finland.

Samples of summer pasture plants that reindeer feed on were collected in order to study (137)Cs concentrations in different plant species and in species nested in certain site types, and to study the regional distribution of (137)Cs in the Finnish reindeer management area. Plant species were categorized by the site types of mineral soil forest (xeric heath forest and mesic heath forest) and peatland. A third category called 'other plant species' included plants with various site types, poorly determined species and species with poor statistics. The (137)Cs concentrations in different site types differed significantly. The mean (137)Cs concentrations of the whole reindeer management area in the xeric heath forest plant species was 44 ± 27 Bq/kg dw, in the mesic heath forest plant species 75 ± 59 Bq/kg dw and in the peatland plant species 219 ± 150 Bq/kg dw. The peatland species uptake (137)Cs more efficiently than plant species of mineral soil forests. A particularly efficient collector of (137)Cs was Trichophorum sp. It is suggested that Trichophorum sp. could be used as an indicator species for reindeer summer fodder plants. The highest concentrations of (137)Cs were found in Southern Lapland and the lowest in Northern Lapland. Today, the concentrations of (137)Cs in summer pasture plants that reindeer feed on in Finland are at such a level that there is no need to avoid any plant species. In the case of future nuclear fallout, reindeer grazing in peatlands would increase concentrations of (137)Cs in reindeer meat.

Effective half-lives of 134Cs and 137Cs in reindeer meat and in reindeer herders in Finland after the Chernobyl accident and the ensuing effective radiation doses to humans.

Monitoring of 137Cs in reindeer herders and in reindeer meat in Finnish Lapland began in the early 1960s and has continued until today. The monitoring of 137Cs in reindeer herders and in reindeer meat in the Halla area began after the Chernobyl accident. In this study, reindeer herders together with reindeer meat samples were monitored for gamma-emitting radionuclides from two separate areas in the Finnish reindeer management area, Northern Finland and the Halla area. The effective half-lives determined for 137Cs in reindeer meat were from 3.0 ± 1.7 to 5.1 ± 0.5 y. For 134Cs, the observed effective half-lives in reindeer meat were from 1.3 ± 0.2 to 1.5 ± 0.1 y. The effective half-lives among male and female reindeer herders in Northern Finland were 5.5 ± 1.3 and 4.4 ± 0.9 y, respectively, for the body-burden of 137Cs. In the Halla reindeer herding cooperative, located to the south of Finnish Lapland in the province of Kuusamo, the effective half-lives in the reindeer herders were shorter, about 1-2 y. The 134Cs × 137Cs-1 ratios decreased more rapidly in reindeer meat and also in humans in the Halla area than in Northern Finland. This implies faster removal of Chernobyl-derived cesium from the reindeer-man food chain in the Halla area. The contribution of Chernobyl fallout (percent) in reindeer meat was 70% and 80% in the Paistunturi and Ivalo cooperatives, respectively, and 50% and 80% in the western and eastern part of Halla cooperative, respectively. In humans, the contribution of Chernobyl fallout to 137Cs in whole-body content was 60% in Northern Finland and 80% in the Halla area. The mean committed effective doses of Cs for reindeer herders in Finnish Lapland decreased from 0.36 mSv y-1 in 1987 to 0.053 mSv y-1 in 2005.