Preliminary evaluation of (135)Cs/(137)Cs as a forensic tool for identifying source of radioactive contamination

Ratios of the fission products (135)Cs and (137)Cs were determined in soil and sediment samples contaminated from three different sources, to assess the use of (135)Cs/(137)Cs as an indicator of source of radioactive contamination. Soil samples from the Chernobyl exclusion zone were found to have to be heavily depleted in (135)Cs ((135)Cs/(137)Cs approximately 0.45), indicative of a high thermal neutron flux at the source. Sludge samples from a nuclear waste treatment pond were found to have a (135)Cs/(137)Cs ratio of approximately 1, whereas sediment collected downstream from a nuclear reactor was highly variable in both (137)Cs activity and (135)Cs/(137)Cs ratio. Comparison of these preliminary results of variability in radiocaesium isotope ratios with reports of Pu isotope ratios suggests (135)Cs/(137)Cs similarly varies with fuel and reactor conditions, and may be used to corroborate other methods of characterizing radioactive contamination.     

In situ gamma-ray spectrometry in forests: determination of kerma rate in air from 137Cs

Continental margins are important areas to be considered when studying the distributions and depositions of pollutants, both conventional and radioactive. Coastal sediments accumulate most of those contaminants which can be introduced following atmospheric and/or fluvial pathways. Moreover, their residence times within the water column are usually shortened due to their affinity to associate with the downward falling particulate matter, more abundant at shallower depths. In this paper the distribution profiles and inventories of plutonium, americium and cesium are detailed, providing useful information about recent sedimentation phenomena such as sediment mixing, slumping processes and bioturbation. Unsupported 210Pb data are used as reliable indicators of enhanced/reduced deposition events. Also, the calculated inventories have enabled the estimation of the radiological contribution of the Spanish Mediterranean margin to the total radioactivity deposited onto the Mediterranean sea floor.     

A theoretical description of diffusion and migration of 137Cs in soil.

Careful measurements of activity concentrations of 137Cs in soil samples taken layer by layer in autumn of 1999 in Slovenia are confronted with a prediction based on the diffusion-convection equation with a boundary condition which--unlike the boundary conditions applied in the literature so far--conserves the deposited activity over time, except for the natural decay. It is shown that it is essential to consider the deposits from atmospheric nuclear weapons tests and the Chernobyl accident to arrive at a good fit to the measured data. The corresponding Green's function as well as the diffusion constant and migration speed based on the analysis are given.     

A comparison of three models of 137Cs transfer in forest ecosystems.

The predictions of three models of 137Cs transfer in forest ecosystems (FOA, LOGNAT and FORESTLAND) were compared. The scenario for the model-model comparison consisted of an acute dry deposition of 137Cs over a coniferous forest. The model predictions were subsequently compared (model-data comparison) with values derived from experimental data measured in forests of the Bryansk region in Russia that were contaminated by the Chernobyl accident and that have similar characteristics to the forests described in the scenario. The predictions of radiocaesium levels in the litter-soil layer, berries, needles, wood, whole tree and moose made with the models were in relatively good agreement with each other (within a factor of 1.4-2.9). The best agreement was observed for berries and moose and the worst for wood. There was also good agreement between the model predictions for the same variables and the experimental data (within a factor of 1.2 3.2). In this case, the best agreement was observed for the litter-soil layer and the worst for wood and the whole tree. Overall, at least for the studied scenario and for the first 10 years after deposition, any of the models can be used if the final aim is to estimate average concentrations in different forest components. The agreement between the model predictions worsens with time and there were differences in the form of the time dependencies predicted by the models, especially for wood. This may lead to larger differences between the model predictions and the experimental data for times beyond the period for which data were available for comparison (10 years after the deposition).     

A simplified 137Cs transport model for estimating erosion rates in undisturbed soil

(137)Cs is an artificial radionuclide with a half-life of 30.12 years which released into the environment as a result of atmospheric testing of thermo-nuclear weapons primarily during the period of 1950s-1970s with the maximum rate of (137)Cs fallout from atmosphere in 1963. (137)Cs fallout is strongly and rapidly adsorbed by fine particles in the surface horizons of the soil, when it falls down on the ground mostly with precipitation. Its subsequent redistribution is associated with movements of the soil or sediment particles. The (137)Cs nuclide tracing technique has been used for assessment of soil losses for both undisturbed and cultivated soils. For undisturbed soils, a simple profile-shape model was developed in 1990 to describe the (137)Cs depth distribution in profile, where the maximum (137)Cs occurs in the surface horizon and it exponentially decreases with depth. The model implied that the total (137)Cs fallout amount deposited on the earth surface in 1963 and the (137)Cs profile shape has not changed with time. The model has been widely used for assessment of soil losses on undisturbed land. However, temporal variations of (137)Cs depth distribution in undisturbed soils after its deposition on the ground due to downward transport processes are not considered in the previous simple profile-shape model. Thus, the soil losses are overestimated by the model. On the base of the erosion assessment model developed by Walling, D.E., He, Q. [1999. Improved models for estimating soil erosion rates from cesium-137 measurements. Journal of Environmental Quality 28, 611-622], we discuss the (137)Cs transport process in the eroded soil profile and make some simplification to the model, develop a method to estimate the soil erosion rate more expediently. To compare the soil erosion rates calculated by the simple profile-shape model and the simple transport model, the soil losses related to different (137)Cs loss proportions of the reference inventory at the Kaixian site of the Three Gorge Region, China are estimated by the two models. The over-estimation of the soil loss by using the previous simple profile-shape model obviously increases with the time period from the sampling year to the year of 1963 and (137)Cs loss proportion of the reference inventory. As to 20-80% of (137)Cs loss proportions of the reference inventory at the Kaixian site in 2004, the annual soil loss depths estimated by the new simplified transport process model are only 57.90-56.24% of the values estimated by the previous model.     

Aquatic mosses as a monitoring tool for 137Cs contamination in streams and rivers-a field study from central southern Norway

Mosses are frequently used as biomonitors for trace element pollution in the aquatic environment. The purpose of this study was to assess their usefulness as a tool in monitoring and in regional surveys of radioactive contamination. Specimens of the aquatic mosses, Fontinalis antipyretica and F. dalecarlica, were transplanted from non-contaminated areas to streams and rivers in the Norwegian Jotunheimen Mountains and neighbouring lowland areas that had received radioactive fallout after the Chernobyl accident. Equilibrium concentrations of 137Cs in the exposed mosses were reached after a few weeks. Two series from 20 streams in 1994 and 1996 show linear correlations between activities in water and moss samples and biomagnification ratios of 10(4) - 10(5). We conclude that mosses are better suited for monitoring purposes than water samples, because they provide values integrated over weeks while the radioactivity in surface waters can be subject to rapid variations according to hydrological events. The activity concentrations in aquatic mosses can be easily measured with good precision even when aqueous concentrations are below the limit of detection. Use of aquatic mosses also reduces the logistic problems of transporting large volumes of water, especially in areas inaccessible by road.     

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.     

Foliar contamination of Phaseolus vulgaris with aerosols of 137Cs, 85Sr, 133Ba and 123mTe: influence of plant development stage upon contamination and rain

As part of a requirement to improve the assessment of the impact of radioactive fallout on consumed agricultural products, bean plants at four development stages (seedlings, preflowering, late flowering and mature plants) were contaminated by dry deposition of (137)Cs, (85)Sr, (133)Ba and (123m)Te aerosols. The influence of two rain scenarios and of the development stage upon contamination on interception, retention, and translocation to pods was studied. Interception of the four radionuclides was almost identical and varied from 30 to 60% with increasing development stage. The most important rain parameter was the time which elapsed between contamination and the first rain. Whatever the development stage, rain washed off more cesium from the leaves when it occurred 2 days after the deposit (37% at the seedling stage, for example) rather than later on (6 days, 27%), due to rapid migration of Cs in the plant. The first rain washed off nearly 40% of Ba whatever the scenario. For later stages, Sr and Ba were more washed off by heavy weekly rains than by weak twice-a-week rains, perhaps because of the Sr/Ba-contaminated material loss associated with wash off (desquamation of cuticles). Te showed little wash off (less than 5%). Wash off decreased with an older development stage for a weak rain intensity, due to the superimposition of leaves. Heavy rains removed this shelter effect. At harvest, rain effect was no longer detectable as foliar activity was similar for both rain scenarios. Translocation factors (TF) for strontium and barium increased from 6 x 10(-3) to 1 x 10(-1) with the plant development stage upon contamination, whereas those for cesium remained almost unchanged between 2 x 10(-1) and 4 x 10(-1). Flowering is the most critical stage towards residual contamination in pods at harvest, with the exception of direct deposit on pods at the mature stage (TF values are one order of magnitude higher). TF value for Te was 6.5 x 10(-2) and was due to direct deposit. Modelling reflected the trends, through the differential values of the wash off and absorption coefficients, of what was reported for experimental results.     

Current contamination by 137Cs and 90Sr of the inhabited part of the Techa river basin in the Urals

Previous discharges of radioactivity from the Mayak Production Association plant in the Urals have resulted in considerable radionuclide contamination of the Techa River, and consequent high radiation doses during the late 1940s and 1950s to residents of villages along the Techa river. The most contaminated villages close to the site were evacuated in the period 1954-1962. The objective of this recent study was to conduct a preliminary assessment of the current radioactive contamination of soil, vegetation and foodstuffs in the two remaining villages closest to the Mayak site, Muslyumovo and Brodokalmak. The highest contamination levels in soil were found in the floodplain at 5.5 MBq m(-2) for 137Cs and 1.0 MBq m(-2) for 90Sr. Radionuclide contamination in soil of the villages was much lower, but exceeded that expected from global fallout. Data from 1207 measurements of 137Cs in milk and 1180 for 90Sr in milk for the period 1992-1999 were collated. There was no change with time in the 90Sr or 137Cs activity concentration in milk over the measured period. There were significantly higher 137Cs activity concentrations in milk sampled during the housed winter period in Muslyumovo compared with the grazing summer period, but compared to that for Brodokalmak or for either settlement for 90Sr. The highest measured activity concentrations in food products of 137Cs and 90Sr were found in river fish, waterfowl, poultry and milk. The measured activity concentrations of 137Cs and 90Sr in some animal products were higher than that expected from soil and vegetation from fields and pasture in the villages (not including the floodplain) confirming that the highly contaminated floodplains are contributing to contamination of some animal products.     

Ecological half-life of 137Cs in plants associated with a contaminated stream

Ecological half-life (Te) is a useful measure for studying the long-term decline of contaminants, such as radionuclides, in natural systems. The current investigation determined levels of radiocesium (137Cs) in two aquatic (Polygonum punctatum, Sagittaria latifolia) and three terrestrial (Alnus serrulata, Myrica cerifera, Salix nigra) plant species from a contaminated stream and floodplain on the U.S. Department of Energy's Savannah River Site. Current 137Cs levels in plants were used in conjunction with historical data to determine Te of 137Cs in each species. Median concentrations of 137Cs were highest in S. latifolia (0.84 Bq g(-1)) and lowest in M. cerifera (0.10 Bq g(-1)). Te's ranged from 4.85 yr in M. cerifera to 8.35 yr in S. nigra, both terrestrial species. Te's for all aquatic (6.30 yr) and all terrestrial (5.87) species combined were very similar. The Te's of the two aquatic primary producers (P. punctatum and S. latifolia) in the Steel Creek ecosystem were somewhat longer than Te values previously reported for some consumers from this ecosystem.     

137Cs in freshwater fish in Finland since 1986--a statistical analysis with multivariate linear regression models

The accident at the Chernobyl nuclear power plant in 1986 significantly elevated the 137Cs levels of fish in Finnish lakes. About 6200 fish samples from 390 lakes comprising 20 species have been analysed for 137Cs since 1986. The sizes of the lakes varied from a few hectares to about 1000 km2. Activity concentrations of 137Cs in fish still varied widely in 2003, from 16 to 6400 Bq/kg fresh weight. This paper presents the results of statistical analyses with multivariate linear regression models carried out on the empirical data collected since 1986. The statistical analysis resulted in separate models for two time periods describing temporal changes of 137Cs in fish. The explanatory variables were fish species with various feeding habits, the size class of the lake, municipal division, drainage area, time since the deposition and deposition level of the municipality. The calculated values for 137Cs in fish did not differ statistically significantly from the observed values in the validation data. The explanatory variables explained 58% (the first time period) and 72% (the second time period) of the total variability of 137Cs in fish.     

A rapid method for 90Sr determination in the presence of 137Cs in environmental samples

A rapid method for the determination of 90Sr in the presence of 137Cs using the Cherenkov radiation technique is described. The contribution of 137Cs to gross Cherenkov radiation (90Y + 137Cs) was examined for 137Cs /90Sr ratios ranging from 0.09 to 2.50 for 137Cs activities ranging from 2 to 1,211 Bq. Results from direct Cherenkov radiation measurement and results after radiochemical separation of 90Y from 90Sr for samples containing both 90Sr and 137Cs were compared. Errors below 5% were obtained for 137Cs /90Sr ratios lower than 1, when no separation was performed, independently of the activity level. However, errors between 10% and 35% were obtained for 137Cs/90Sr ratios higher than 1. In order to determine 90Sr activity in the presence of 137Cs using the Cherenkov technique, a multiple linear regression analysis model was established to correct the data for 137Cs content. The mathematical correction proposed was validated using 66 artificially contaminated lettuce samples in a laboratory experiment by taking into account the activity levels of 137Cs and 90Sr and the radionuclide ratios. Comparison of mathematically corrected radionuclide ratios with the results obtained without correction shows that, for radionuclide ratios higher than 1, error values for measuring 90Sr activity using the mathematical model were much smaller than when no radiochemical separation was performed. On the other hand, for ratios lower than 1, error values when measuring 90Sr activity with radiochemical separation were smaller than when mathematical correction was performed. In spite of this, the mathematical correction is an appropriate way of reducing the time needed to determine radiostrontium using the Cherenkov radiation technique. The method proposed could be a powerful tool for environmental research whenever the contents of 90Sr and 137Cs have to be determined.     

Bioaccumulation of 137Cs and 57Co by five marine phytoplankton species.

Under controlled laboratory conditions, we have examined the bioaccumulation of 137Cs and 57Co in three prymnesiophytes, the coccolithophorid Emiliania huxleyi and the noncalcareous species Isochrysis galbana and Phaeocystis globosa, and two diatoms Skeletonema costatum and Thalassiosira pseudonana. We measured the uptake in growing and non-growing cells and determined concentration factors on both volume and dry weight bases. For uptake of 57Co in non-growing cells, volume concentration factors (VCF) at equilibrium ranged from 0.2 x 10(3) for E. huxleyi to 4 x 10(3) for T. pseuedonana. For uptake of 137Cs in non-growing cells, the VCFs were low for all species and the uptake pattern seemed unsystematic. The results suggest that, in contrast to Co, the cycling and bioaccumulation of Cs in marine animals are unlikely to be affected by Cs accumulation in primary producers.     

Surface ground contamination and soil vertical distribution of 137Cs around two underground nuclear explosion sites in the Asian Arctic, Russia

Vertical distributions of 137Cs have been determined in vegetation-soil cores obtained from 30 different locations around two underground nuclear explosion sites--"Crystal" (event year - 1974) and "Kraton-3" (event year - 1978) in the Republic of Sakha (Yakutia), Russia. In 2001-2002, background levels of 137Cs surface contamination densities on control forest plots varied from 0.73 to 0.97 kBq m(-2) with an average of 0.84+/-0.10 kBq m(-2) and a median of 0.82 kBq m(-2). 137Cs ground contamination densities at the "Crystal" site ranged from 1.3 to 64 kBq m(-2); the activity gradually decreased with distance from the borehole. For "Kraton-3", residual surface contamination density of radiocaesium varied drastically from 1.7 to 6900 kBq m(-2); maximal 137Cs depositions were found at a "decontaminated" plot. At all forest plots, radiocaesium activity decreased throughout the whole vertical soil profile. Vertical distributions of 137Cs in soil for the majority of the plots sampled (n=18) can be described using a simple exponential function. Despite the fact that more than 20 years have passed since the main fallout events, more than 80% of the total deposited activity was found in the first 5 cm of the vegetation-soil cores from most of the forested landscapes. The low annual temperatures, clay-rich soil type with neutral pH, and presence of thick lichen-moss carpet are the factors which may hinder 137Cs transport down the soil profile.     

Levels of 137Cs in muddy sediments on the seabed in the Bay of Cadiz (Spain). Part II. Model of vertical migration of (137)Cs

This second part of the study reports the development of a model to describe the vertical migration of the artificial radioisotope (137)Cs in the sediment column on the seabed of the Bay of Cadiz. The application of the model provides an overall picture of the process of sedimentation in the Inner Bay of Cadiz. The spatial distribution of the rate of sedimentation enables us to study the sources of sediments and the means by which the sediments have been transported. A method has been derived from the rate of sedimentation to perform the dating of the layers of sediment. The model describes the behaviour of (137)Cs in the area under study, taking into account the time of residence in the zones that are the source of accumulation, the origin of the sedimentary material, together with the diffusion of the radionuclide in the sediment of the seabed.     

Intra-cultivar variability of the soil-to-grain transfer of fallout 137Cs and 90Sr for winter wheat

Differences between the root uptake of fallout radionuclides by different cultivars ('inter-cultivar' variability) growing on the same field may be influenced not only by genetic differences of the cultivars, but also by the spatial variability of the soil-to-grain transfer within the cultivation area of each cultivar. This 'intra-cultivar' variability was investigated in 2001 and 2002 for 137Cs and 90Sr using three winter wheat cultivars with four replicates for each cultivar at three different sites in Bavaria, Germany. The intra-cultivar variability proved to be in the same range as the inter-cultivar variability which was determined earlier at the same sites for both radionuclides. An ANOVA of the 137Cs data set revealed that the variability of the 137Cs soil-to-grain transfer was caused by the soil and climate (year) at the field sites and the interaction of cultivar and field. A significant contribution of the factor 'cultivar' alone to the variability could not be detected. This may be due to the complex environmental conditions to which plants are exposed in field experiments. To find wheat cultivars with minimal uptake of fallout radionuclides it may be better to examine the molecular mechanisms of their root uptake in order to identify targets for breeding "safer" plants.     

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 ¹³⁷Cs concentrations in different plant species and in species nested in certain site types, and to study the regional distribution of ¹³⁷Cs 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 ¹³⁷Cs concentrations in different site types differed significantly. The mean ¹³⁷Cs 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 ¹³⁷Cs more efficiently than plant species of mineral soil forests. A particularly efficient collector of ¹³⁷Cs 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 ¹³⁷Cs were found in Southern Lapland and the lowest in Northern Lapland. Today, the concentrations of ¹³⁷Cs 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 ¹³⁷Cs in reindeer meat.     

Concentration ratios for small mammals collected from the exposed sediments of a 137Cs contaminated reservoir

(137)Cs concentration ratios were computed for small mammals collected from the dried sediments of a partially drained, contaminated reservoir. Soil (137)Cs activity concentrations were heterogeneous on small and large spatial scales and had a geometric mean of 253 (range 23-2110) Bq/kg dry weight. Mean (137)Cs activity concentrations in composite cotton rat Sigmodon hispidus and cotton mouse Peromyscus gossypinus samples averaged 2480 (range 556-6670) and 471 (range 96-1000) Bq/kg whole body dry weight, respectively. About 50% of the variance in cotton rat tissue (137)Cs activity was explained by variation in soil (137)Cs activity. Soil-to-animal dry weight concentration ratios averaged 6.0 for cotton rats and 1.2 for cotton mice and were generally similar to (137)Cs concentration ratios for herbivorous, homeothermic animals from other contaminated ecosystems. In the RESRAD-BIOTA dose model, the default wet-weight concentration ratio for (137)Cs in terrestrial animals is 110 resulting in an estimate of internal and external radiation doses to terrestrial biota that is 44 times more than the dose calculated with the actual measured wet-weight concentration ratio for cotton rats (1.6). These results show that site-specific concentration ratios can significantly affect the estimation of dose.