Distribution and flux of 238Pu, 239,240Pu, 241Am, 137Cs and 210Pb to high arctic lakes in the Thule district (Greenland)

Environmental samples (soil, sediment and lake water) in the Thule area (NW Greenland) have been studied to assess the contamination of radionuclides originating from a nuclear weapons accident (the Thule accident in 1968). Four lakes were chosen at different distances from the point of impact with the Thule air base community situated in between. The sedimentation rates in the lakes varied from 0.4 mm a(-1) (5 mg cm(-2) a(-1)) to 1.6 mm a(-1) (82 mg cm(-2) a(-1)). With these sedimentation rates, it is not possible to resolve the (239,240)Pu global fallout peak from a possible (239,240)Pu "accident" peak in the sediment depth profiles. However, the (239,240)Pu/(137)Cs and the (238)Pu/(239,240)Pu ratios agreed well with global fallout ratios, indicating that plutonium originating from the accident had not reached these lakes. This also indicates that the Thule air base community has probably only been exposed to radionuclides from the accident to a very limited extent. A limited study showed that (210)Pb could not be used as a normalizing nuclide to explain the transport of transuranic elements from the catchment area to the lake, i.e. (210)Pb has a different transport mechanism from that of the transuranic elements studied in this investigation.     

Determining the Chernobyl impact on sediments of a pre-Alpine lake with a very comprehensive set of data

Man-made and natural radionuclides in Lake Wallersee were determined in the pre-Alpine environment at the northern slope of the Alps, which was heavily affected by the Chernobyl fallout in May 1986. The objective of this study was to get knowledge of location and quantity of man-made radionuclide input (especially (137)Cs) generated in the Chernobyl accident to lake sediments. Eleven sediment cores were sampled and activity depth profiles of (137)Cs and (210)Pb were determined with 5mm depth-resolution. The Chernobyl fallout produced an extreme (137)Cs peak in the sediment cores providing an excellent time marker. The chronological interpretation of deeper sediment layers was done by radiochemical analysis of (90)Sr and (239+240)Pu, which were released during atmospheric weapons' tests in the 1950s and 1960s. This allowed a complete chronological analysis of the sediment cores with a very compact set of data.     

Determination of Cs in the water system of a pre-Alpine lake

The aim of this study was to measure the ¹³⁷Cs activity derived from the Chernobyl accident in the water system of Lake Wallersee, a pre-Alpine lake in Austria within an area highly contaminated by the Chernobyl fallout.     

Formation of radioactivity enriched soils in mountain areas

A field study was carried out in the Mercantour Mountains at 2200 m altitude to investigate the processes of soil enrichment in atmospheric Chernobyl (137)Cs. Soils with high (137)Cs activities have been collected in the pasture areas with frequently measured (137)Cs activity values of the order of 7000 Bq m(-2). At some single spots (about 6% of the studied area), activity in soils reached 300000 Bq m(-2), which represents 44% of the (137)Cs of the total area. Data further showed that spatial distribution of Cs depends widely on its origin: Chernobyl Cs is mainly concentrated in "enriched" soils, whereas older Cs and (241)Am fallout from nuclear weapons tests (NWTs) and natural atmospheric (210)Pb in soils is less heterogeneously distributed.In order to elucidate the processes which have led to the enrichment in Chernobyl (137)Cs in the Alps in May of 1986, we have studied the repartition of atmospheric (7)Be isotope (half-life=53.3 d) in the pasture compartments (soil, litter, grass, and snow). Snow (7)Be data give evidence that fallout enrichment is related to snow accumulation (snow drift). The transfer of beryllium occurs rapidly to the grass and litter, where the strongest pollutant accumulations were measured. However, (7)Be transport to the soil required more than 8 months.     

Analysis of radiocaesium in the Lebanese soil one decade after the Chernobyl accident

Fallout from the Chernobyl reactor accident due to the transport of a radioactive cloud over Lebanon in the beginning of May 1986 was studied 12 years after the accident for determining the level of (137)Cs concentration in soil. Gamma spectroscopy measurements were performed by using coaxial high sensitivity HPGe detectors. More than 90 soil samples were collected from points uniformly distributed throughout the land of Lebanon in order to evaluate their radioactivity. The data obtained showed a relatively high (137)Cs activity per surface area contamination, up to 6545Bqm(-2) in the top soil layer 0-3cm. The average activity of (137)Cs in the top soil layer 0-3cm in depth was 59.7Bqkg(-1) dry soil ranging from 15 to 119Bqkg(-1) dry soil. The horizontal variability was found to be about 45% between the sampling sites. The depth distribution of total (137)Cs activity in soil showed an exponential decrease. Estimation of the annual effective dose due to external radiation from (137)Cs contaminated soil for selected sites gave values ranging from 19.3 to 91.6 micro Svy(-1).     

Inventories of fallout 210Pb and 137Cs radionuclides in moorland and woodland soils around Edinburgh urban area (UK)

Inventories of fallout (210)Pb and (137)Cs have been measured in moorland and woodland soils around the Edinburgh urban area, using a high purity germanium detector. The (210)Pb inventories in moorland soils were relatively uniform, with a mean value of 2520+/-270Bqm(-2). The mean (137)Cs inventory in moorland soils varied greatly from 1310 to 2100Bqm(-2), with a mean value of 1580+/-310Bqm(-2). The variability was ascribed mainly to the non-uniform distribution of fallout Chernobyl (137)Cs. The mean (210)Pb and (137)Cs inventories in woodland canopy soils were found to be 3630+/-380Bqm(-2) and 2510+/-510Bqm(-2), respectively. At sites for which both moorland and woodland data were available, the mean inventories provided fairly similar average enhancements of (47+/-7)% and (46+/-18)% of (210)Pb and (137)Cs under woodland canopy soils relative to open grassland soils, respectively. The enhancement factors are broadly in line with other independent findings in literature. Enhancement of both (210)Pb and (137)Cs in woodland soils relative to moorland soils is, in part, due to deposition by impaction during air turbulence, wash-off, gravitational settling and deposition during leaf senescence. Results of this study suggest that these processes affect both (210)Pb and (137)Cs carrier aerosols in a similar way.     

Ecological half-life of 137Cs in lichens in an alpine region

About 17 years after the Chernobyl accident, lichen samples were collected in an alpine region in Austria (Bad Gastein), which was heavily contaminated by the Chernobyl fallout. Measured 137Cs activity concentrations in selected lichens (Cetraria islandica, Cetraria cucullata, and Cladonia arbuscula) ranged from 100 to 1100 Bq kg(-1) dry weight, depending on lichen species and sampling site. Ecological half-lives for 137Cs in different lichen samples, obtained by comparison with earlier measurements of the same lichen species at the same site, ranged from 2 to 6 years, with average values between 3 and 4 years. Comparison with earlier studies indicated that ecological half-lives hardly changed during the last 10 years, suggesting that ecological clearance mechanisms (e.g. washout or soil transfer) did not vary substantially at the selected sampling area.     

A 10-year study of the 137Cs distribution in soil and a comparison of Cs soil inventory with precipitation-determined deposition

During a 10-year period, 1988-1998, surface soil samples have been collected at Blentarp in southern Sweden and analysed for 137Cs from the Chernobyl accident and from the nuclear weapons tests. The distance between the sampling plots on the different sampling occasions has been no more than 3 m. The results show that the depth distribution of 137Cs is very similar for each of the sampling occasions, indicating that the caesium migration at this site is very small. The total activity measured in the soil cores is in agreement with the calculated activity of 137Cs deposited at the site after nuclear weapons tests and the Chernobyl accident, based on air activity concentration and the amount of precipitation. The calculated deposition of 137Cs originating from the bomb tests amounts to 1.41 kBq m-2 for the period 1962-1986, which is in agreement with the activity of nuclear weapons fallout measured in the soil samples (1.60 kBq m-2 as a mean value of the first four years of sampling). The calculated activity of 137Cs of Chernobyl origin was 0.79 kBq m-2, which agrees well with the value of 0.79 kBq m-2 measured in the soil samples in 1988.     

Vertical distributions of 210Pb excess, 7Be and 137Cs in selected grass covered soils in Southeast Queensland, Australia

Net accumulated areal activity densities and profiles of (210)Pb(ex), (7)Be and (137)Cs in the surface 10 cm of the soil are reported for eight sites in Southeast Queensland, Australia. Areal activity densities of (210)Pb(ex) and (7)Be varied from 1,080 to 4,100 Bqm(-2) and from 176 to 778 Bqm(-2), respectively. A significant (p < 0.001) portion of the variance (R(2) > 0.99) in their vertical distributions was explained by depth in the profile using an exponential function. Around 85% of accumulated (210)Pb(ex) was present in the surface 10 cm of the soil. Beryllium-7 was mainly confined to the grass and surface 2 cm of the soil. Average penetration half-depths of 3.6 +/- 0.2 and 0.3 +/- 0.1cm were determined for (210)Pb(ex) and (7)Be, respectively. Areal activity densities of global fallout (137)Cs varied from 10 to 361 Bqm(-2). Its signal was well mixed within the surface 10 cm. Comparison of the measured (137)Cs values to the estimated input value for the region ( approximately 490 Bqm(-2)) and profiling of a 1m deep soil core suggests a vertical migration of (137)Cs over the past decades. The paleo-radon activity flux determined from the (210)Pb(ex) areal activity density (5.1 +/- 0.9 mBqm(-2) s(-1)) was not statistically different to that measured using activated charcoal cups (5.5 +/- 0.4 mBqm(-2) s(-1)), tending to suggest that Southeast Queensland is neither a net source nor a net sink of (210)Pb-bearing aerosols.     

Lake fish as the main contributor of internal dose to lakeshore residents in the Chernobyl contaminated area

Two field expeditions in 1996 studied 137Cs intake patterns and its content in the bodies of adult residents from the village Kozhany in the Bryansk region, Russia, located on the shore of a drainless peat lake in an area subjected to significant radioactive contamination after the 1986 Chernobyl accident. The 137Cs contents in lake water and fish were two orders of magnitude greater than in local rivers and flow-through lakes, 10 years after Chernobyl radioactive contamination, and remain stable. The 137Cs content in lake fish and a mixture of forest mushrooms was between approximately 10-20 kBq/kg, which exceeded the temporary Russian permissible levels for these products by a factor of 20-40. Consumption of lake fish gave the main contribution to internal doses (40-50%) for Kozhany village inhabitants Simple countermeasures, such as Prussian blue doses for dairy cows and pre-boiling mushrooms and fish before cooking, halved the 137Cs internal dose to inhabitants, even 10 years after the radioactive fallout.     

210Pb and 137Cs as chronometers for salt marsh accretion in the Venice Lagoon - links to flooding frequency and climate change

Five salt marsh sediment cores from different parts of the Venice Lagoon were studied to determine their depositional history and its relationship with the environmental changes occurred during the past approximately 100 years. X-radiographs of the cores show no disturbance related to particle mixing. Accretion rates were calculated using a constant flux model applied to excess (210)Pb distributions in the cores. The record of (137)Cs fluxes to the sites, determined from (137)Cs profiles and the (210)Pb chronologies, shows inputs from the global fallout of (137)Cs in the late 1950s to early 1960s and the Chernobyl accident in 1986. Average accretion rates in the cores are comparable to the long-term average rate of mean sea level rise in the Venice Lagoon ( approximately 0.25 cm y(-1)) except for a core collected in a marsh presumably affected by inputs from the Dese River. Short-term variations in accretion rate are correlated with the cumulative frequency of flooding, as determined by records of Acqua Alta, in four of the five cores, suggesting that variations in the phenomena causing flooding (such as wind patterns, storm frequency and NAO) are short-term driving forces for variations in marsh accretion rate.     

Analysis of Factors Determining Accumulation of 137Cs by Woody Plants

The accumulation of ¹³⁷Cs by coniferous (Pinus sylvestris) and deciduous (Betula pendula) trees was studied in the area contaminated with radioactive products after the Chernobyl accident. The availability of ¹³⁷Cs to woody plants is determined by its vertical distribution in the soil profile, the proportion of its exchangeable form, and the distribution of tree roots in the soil. The index of biological availability of ¹³⁷C in the soil is proposed, and its linear dependence on the coefficients of ¹³⁷Cs transfer to wood is demonstrated.     

Distribution of pre- and post-Chernobyl radiocaesium with particle size fractions of soils

The association of radiocaesium with particle size fractions separated by sieving and settling from soils sampled eight years after the Chernobyl accident has been determined. The three size fractions were: <2 microm, 2-63 microm and >63 microm. 137Cs in the soil samples was associated essentially with the finer size fractions, which generally showed specific activities 3-5 times higher than the bulk samples. Activity ratios of 134Cs/137Cs in the clay-sized fractions appear to be lower with respect to the corresponding values in bulk soil samples. This result indicates that some differences still exists in the particle size distribution between 137Cs originating from nuclear weapons, which has been in the soil for decades after fallout, and 137Cs coming from the Chernobyl accident, eight years after the deposition event. This behaviour could be related to "ageing" processes of radiocaesium in soils.     

Comparative analysis of (239)Pu, (137)Cs, (210)Pb and (40)K spatial distributions in the top soil layer at the Baltic coast

This paper presents the results of an investigation into the spatial distribution of radionuclides of artificial ((239,240)Pu, (137)Cs) and natural ((210)Pb, (40)K) origins in the upper (0-5 cm) soil layers on the Baltic coastline of Lithuania ( approximately 5 km(2) area). The samples were analysed by gamma ray spectrometry and combined radiochemical procedures. The highest (210)Pb, (239,240)Pu and (137)Cs activity concentrations were determined in the forest samples, whereas (40)K activity was rather homogeneous across the study area. Relatively high (239,240)Pu and (40)K activity concentrations were determined along the surf zone. The (210)Pb and (137)Cs activity concentrations showed a gradual increase from the surf zone to the forest. The average activity concentrations of (239,240)Pu, (137)Cs, (210)Pb and (40)K in the beach and forest samples, respectively, were as follows: 0.32+/-0.08 and 0.74+/-0.14; 50+/-4 and 1190+/-50; 4.7+/-2.0 and 48+/-6; 186+/-15 and 216+/-17 Bq/kg.     

238Pu, 239,240Pu, 241Am, 90Sr and 137Cs in soils around nuclear research centre Rez, near Prague

Forty-four soil samples were taken around the nuclear research centre Rez, near Prague. The mean activity concentrations of 238Pu, 239,240Pu, 241Am, 90Sr and 137Cs in uncultivated soil were 0.010, 0.26, 0.12, 2.7 and 23 Bq.kg(-1), respectively. Contents of radionuclides in cultivated soil were lower and in forest soil higher than in uncultivated soil. The mean activity ratios of 238Pu/239,240Pu, 241Am/239,240Pu, 90Sr/239,240Pu and 239,240Pu/137Cs in uncultivated soil were 0.041, 0.47, 10.9 and 0.013, respectively. The mean activity ratios in cultivated and forest soils were close to the values given above. It follows from the results that the source of 239,240Pu, 90Sr and 137Cs in the studied area is deposition from atmospheric nuclear tests, in the case of 137Cs also deposition from Chernobyl accident. The contribution of the research centre effluents was not proved for these radionuclides. Increased activity ratio of 241Am/239,240Pu indicates the presence of 241Am in the soils studied emanating from sources other than nuclear tests. Uniform distribution of the 241Am/239,240Pu activity ratio around the nuclear research centre and the absence of an area with evidently higher activity ratio, including at sites lying in the main wind direction, suggest that the additional activity of 241Am does not originate from the nuclear research centre. The additional source might be the deposition following the Chernobyl accident.     

Deposition and distribution of Chernobyl fallout fission products and actinides in a Russian soil profile

In this article the distribution of fission products and actinides in a soil profile from Novo Bobovicky in Russia, which was contaminated due to the Chernobyl nuclear power plant accident, is described. The ground deposition of long-lived fission products determined by gamma-spectrometry was (recalculated to 26 April 1986) 1600 kBq (137)Cs/m(2), 900 kBq (134)Cs/m(2) and 60 kBq (125)Sb/m(2). Of these radionuclides (137)Cs shows the dominating activity at the present time. After 6.5 years 90% of the Cs and Sb activity was contained in the upper 4 cm. A (239,240)Pu ground deposition of 77.4+/-8.0 Bq/m(2) was determined by alpha-spectrometry. The (238)Pu/(239,240)Pu activity ratio of 0.30+/-0.03 and (241)Pu/(239,240)Pu activity ratio of 115+/-14 (in 1986) measured in the soil profile, indicates that the analysed Pu originates mainly from the Chernobyl accident. The average (234)U/(238)U activity ratio of 1.06+/-0.29 indicates that the uranium in this soil is dominated by naturally occurring uranium.The alpha- and beta-autoradiography revealed that the activity is mainly present in particulate form. It could further be observed that the spots containing alpha- or beta-activity originated from different particles. A comparison of alpha-autoradiography with the bulk Pu and Am activity showed that 92% of the alpha-activity was present as clearly detectable alpha-spots.The beta-active particles, located by beta-autoradiography were correlated with gamma-spectrometric measurements and contained only (137)Cs. These hot spots ranged from 0.02 to 0.15 Bq.It could be concluded that the vertical transport of (137)Cs and fuel fragments occurs mainly by movement of particles through the soil. It could also be concluded that the fuel fragments found, in this soil were depleted in respect to Cs, Sb and Eu.Comparison of the analysed (238)Pu/(239,240)Pu, (241)Pu/(239,240)Pu and (241)Am/(239,240)Pu ratios with the ratios calculated with ORIGEN-S code gave an estimate of the average burn-up of the fuel particles to be in the range of 11-12 GWd/tU.The results presented in this article are valid for this single soil profile and should not be generalised unless validated in a more rigorous study of a larger number of soil profiles.     

Post-depositional redistribution and gradual accumulation of 137Cs in a riparian wetland ecosystem in Sweden

After the Chernobyl accident, high activity concentrations of (137)Cs (>1 MBq m(-2)) were detected in a riparian swamp in the central-eastern part of Sweden. The objective of this study was to clarify the redistribution processes behind the accumulation of (137)Cs in the wetland. A mass balance budget of (137)Cs was calculated based on soil and sediment samples and reports in the literature. Results showed that accumulation occurred over several years. Of all the (137)Cs activity discharged between 1986 and 2002 from the upstream lake, 29% was estimated to be retained in the wetland. In 2003, measurements showed that 17 kBq m(-2) sedimented on the stream banks of the wetland. Continuing overbank sedimentation by spring flooding prolongs the time that the wetland will contain high activity concentrations of (137)Cs. Consequently, organisms living in wetlands serving as sinks for (137)Cs may become exposed over long time periods to high activity concentrations.     

Inventories of Pu, Cs, and excess Pb in sediments from freshwater and brackish lakes in Rokkasho, Japan, adjacent to a spent nuclear fuel reprocessing plant

We investigated the vertical profiles of ^239+240Pu, ¹³⁷Cs, and excess ²¹⁰Pb (²¹⁰Pb_ex) in sediment core samples obtained from two freshwater lakes and two brackish lakes situated near the first commercial spent nuclear fuel reprocessing plant in Rokkasho, Japan, before the final test of the plant using actual spent nuclear fuel. The inventory of ^239+240Pu in those lakes was larger than that in soil in Rokkasho, which indicated the inflow of ^239+240Pu from the catchment area in addition to direct deposition on the lake surfaces. The ¹³⁷Cs inventory in sediments of the brackish lakes was lower than that in the soil, which showed that part of the ¹³⁷Cs was removed from the sediments by the brackish water or that it was not deposited into the sediments, because of the high solubility of Cs in brackish water. The ¹³⁷Cs inventory in sediments of the freshwater lakes was higher than that of the brackish lakes, and comparable with that in soil except for one core sample out of four. The ^239+240Pu/¹³⁷Cs ratio in freshwater lake sediments was higher than that in soil, and that indicated that part of the ¹³⁷Cs was lost from the sediments. The low inventory of ¹³⁷Cs may be attributable to competition for absorption sites in sediments with ammonium ions formed in the reducing environment which occurs from summer to fall in the sediments. Those data will be used as background data on the artificial radionuclides in the lakes to assess the effect of released radionuclides on their concentrations.     

Vertical distribution and inventories of 137Cs in the Syrian soils of the eastern Mediterranean region

Vertical distribution and inventories of (137)Cs have been determined using radiocesium distributions in presumably undistributed soil profiles, collected from 36 sites distributed all over Syria (eastern Mediterranean region). Vertical distributions of (137)Cs in the collected profiles were found to be strongly correlated with soil type and five groups were identified. Based on these profiles, total (137)Cs inventory (bomb test and Chernobyl) varied between 320 Bq m(-2) and 9,647 Bq m(-2). Geographical mapping of (137)Cs inventories showed that the highest values were found in the coastal, middle and north-east regions of Syria indicating that Chernobyl atmospheric contribution to the total (137)Cs deposition in the region is predominant. In contrast, the lowest values were found in the south-east region (Syrian Badia), where a relatively uniform distribution was observed, which may only be attributed to the past global nuclear bomb test. The measured inventories were also compared with a mathematical model for estimating bomb derived (137)Cs reference inventories.     

Radionuclide tracing of water masses and processes in the water column and sediment in the Algerian Basin

Caesium-137 and (239,240)PU were analysed in the water column along the Algerian coast. The (137)Cs activity concentration in surface water increased from the west to the east from 1.6 to 3.3 mBq L(-1), documenting a presence of Modified Atlantic Water (MAW) in the region. Higher concentrations observed in deep waters may be due to an intrusion of Levantine Intermediate Water (LIW), which has been carrying higher levels of (137)Cs from Chernobyl accident. The (239,240)Pu sub-surface concentration peaked at about 250 m water depth as a result of biogeochemical processes in the water column. The observed (239,240)Pu/(137)Cs activity ratio at the surface (0.003) was significantly lower than that in global fallout (0.04). This decrease exceeds that expected from radioactive decay of (137)Cs, and confirms that Pu due to its adsorption on sinking particles is more effectively removed from surface layers than is (137)Cs. An increase of the (239,240)Pu/(137)Cs activity ratio with depth suggests that (239,240)Pu, similarly as (137)Cs, should be also transported by advection to maintain the observed ratios in deep waters. An intrusion of LIW may enhance therefore both the (137)Cs and (239,240)Pu concentrations in deep waters. The average (238)Pu/(239+240)Pu activity ratio in seawater was 0.03+/-0.02, confirming a global fallout origin of Pu in the Algerian Basin. Caesium-137 and (239,240)Pu inventories in the water column were estimated to be from 2.7+/-0.5 kBq m(-2) to 3.8+/-0.7 kBq m(-2), and from 13.8+/-2.6 Bq m(-2) to 41+/-7B qm(-2), respectively. The (137)Cs massic activities in surface sediment were almost constant, the average activity was 9.0+/-0.8 Bq kg(-1). Sedimentation rates obtained using the (210)Pb method were from 0.1 to 0.7 cm y(-1), and resulting penetration depths of (137)Cs in the sediment cores were from 15 to over 40 cm. The (137)Cs peaks found in the sediment cores were associated with the Chernobyl accident (1986) and global fallout (1964). The (137)Cs inventories in the sediment were increasing from the west (180 Bq m(-2)) to the east (350 Bq m(-2)).