Concentration and specific activity of fallout 137Cs in extracted and particle-size fractions of cultivated soils

Fallout (137)Cs and stable Cs in soils were separated with two extractants (1M CH(3)COONH(4) solution and 0.8M CH(3)COONH(4) in 5% HNO(3) solution after H(2)O(2) oxidization). The residue remaining after removal of the oxidizable organic-bound fraction was separated into the particle-size fractions including clay, silt, fine sand and coarse sand with a sieving and sedimentation method. Then, the concentrations of (137)Cs and stable Cs in the extracted fractions and the particle-size fractions were determined. The (137)Cs contents in the exchangeable and organic-bound fractions in the soil were approximately 10 and 20%, respectively. The (137)Cs content in the strongly bound fraction was about 70%, and the concentration of (137)Cs in the clay was the richest among the particle-size fractions. The specific activity of (137)Cs (concentration ratio of fallout (137)Cs/stable Cs) decreased in the order exchangeable, organic-bound and strongly bound fractions. The data suggest that equilibrium between (137)Cs and stable Cs was not reached among those fractions, even though most of the (137)Cs that had been deposited on the soil was derived from fallout weapons tests that occurred several decades ago. The concentration of (137)Cs among the particle-size fractions in each soil was different, whereas the specific activity of (137)Cs in the particle-size fractions had a relatively similar value.     

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.     

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.     

Monitoring microbial biomass and respiration in different soils from the Czech Republic--a summary of results

The microbial biomass (Cbio), respiration (basal respiration (BR) and potential respiration (PR)), and derived indices for 520 independent soil samples of 117 different soils from the Czech Republic were statistically analysed. The broad range of soil samples allowed the stepwise breakdown of the database into six reasonable categories of soil: arable soils, loamy grassland soils, sandy grassland soils with weak organic matter content, sandy grassland soils with moderate organic matter content, forest soils with moderate organic matter content, and forest organic soils with rich organic matter content. Because soil microbiology lacks benchmarking values, the ranges of the microbial characteristics for these categories were stated and are presented here. The separation into soil groups narrowed the ranges enough to be useful for comparative purposes. The groups displayed significant differences in basal microbial parameters. The lowest microbial biomass was found in arable soils and grassland sandy soils with weak organic matter content. The highest microbial biomass was shown by loamy grassland soils and organic forest soils. Respiration displayed similar results to the microbial biomass. The derived indices revealed less significant differences confirming their inner-standard nature. The relationships between the soil contamination and microbial parameters were not explored because of the confounding effect of soil organic matter. However, it was not shown by the category of grassland sandy soils with weak organic matter content suggesting they could be especially suitable for the biomonitoring of harmful effects of chemicals on soil microorganisms.     

Soil to plant transfer of 137Cs and 60Co in Ferralsol, Nitisol and Acrisol

In this study, soil to plant transfer factor values were determined for 137Cs and 60Co in radish (Raphanus sativus), maize (Zea mays L.) and cabbage (Brassica oleracea L. var. capitata) growing in gibbsite-, kaolinite- and iron-oxide-rich soils. After 3 years of experiment in lysimeters it was possible to identify the main soil properties able to modify the soil to plant transfer processes, e.g. exchangeable K and pH, for 137Cs, and organic matter for 60Co. Results of sequential chemical extraction were coherent with root uptake and allowed the recognition of the role of iron oxides on 137Cs behaviour and of Mn oxides on 60Co behaviour. This information should provide support for adequate choices of countermeasures to be applied on tropical soils in case of accident or for remediation purposes.     

Effect of chemical pollution on forms of 137Cs, 90Sr and 239,240Pu in arctic soil studied by sequential extraction

The aim of the present study was to determine the forms of 137Cs, 90Sr and 239,240Pu occurring in different soil horizons using sequential extraction of samples taken from four sites located along a pollution gradient from the copper-nickel smelter at Monchegorsk in the Kola Peninsula, Russia, and from a reference site in Finnish Lapland in 1997. A selective sequential-leaching procedure was employed using a modification of the method of Tessier, Cambell and Bisson ((1979). Analytical Chemistry, 51, 844-851). For 137Cs the organic (O) and uppermost mineral (E1) layer were studied, for 90Sr and 239,240Pu only the uppermost organic layer (Of). The fraction of 137Cs occurring in readily exchangeable form in the organic layer was about 50% at the reference site and decreased as a function of pollution, being 15% at the most polluted site in the Kola Peninsula. There was a clear positive correlation in the O layer between the distance from the smelter and the percentage of 137Cs extracted in the readily exchangeable fraction (Spearman correlation rsp = 0.7805, p = 0.0001), whereas in the E1 layer no correlation was evident. The distribution of 90Sr in the Of layer was similar at all sites, with the highest amounts occurring in exchangeable form and bound to organic matter, whereas stable Sr showed a somewhat different distribution with the highest amount in the oxide fraction. Most of the 239,240Pu was bound to organic matter. Chemical pollution affected the exchangeable fraction of 239,240Pu, which was about 1% at the most polluted site and 4-6% at the other sites.     

Chemical availability of 137Cs and 90Sr in undisturbed lysimeter soils maintained under controlled and close-to-real conditions

Chemical availability of 137Cs and 90Sr was determined in four undisturbed soils in a lysimeter study three and four years after deposition to the soil surface. The study was part of a larger project on radionuclide soil-plant interactions under well-defined conditions. The soil types were loam, silt loam, sandy loam and loamy sand, and were representatives of important European soil and climatic conditions. The lysimeters were installed in greenhouses with climatic and hydrological control, and were contaminated with 137Cs and 90Sr in an aerosol mixture simulating fallout from a nuclear accident. Soil samples were taken from several depths in each soil in 1997 and 1998 and the samples were sequentially extracted with H2O, NH4Ac, NH2OH.HCl, H2O2 and HNO3. Extractability of 137Cs decreased in the order: HNO3 > R-esidual > or = NH4Ac > H2O2 > or = NH2OH.HCl > or = H2O. More than 80% was found in the acid digestible or residual fractions, and 11-17% in labile fractions. Soil type differences were small. Extractability of 90Sr decreased in the order: NH4Ac > NH2OH.HCl > HNO3 > H2O2 approximately H2O. 31-58% was found in easily available fractions. Differences between soil types were quite small. The results suggest that availability of 137Cs for plant uptake and migration is low, whereas availability of 90Sr is rather high.     

Use of 129I and 137Cs in soils for the estimation of 131I deposition in Belarus as a result of the Chernobyl accident

Using radioactivity measurements for 131I and 137Cs and nuclear activation analysis (NAA) or accelerator mass spectrometry (AMS) for 129I, ratios of 131I/137Cs and 129I/137Cs have been determined in soils from Belarus. We find that the pre-Chernobyl ratio of 129I/137Cs in Belarus is significantly larger than expected from nuclear weapons fallout. For the Chernobyl accident, our results support the hypothesis that there was relatively little fractionation of iodine and caesium during migration and deposition of the radioactive cloud. For sites having 137Cs > 300 Bq/kg, 129I can potentially give more reliable retroactive estimates of Chernobyl 131I deposition. However, our results suggest that 137Cs can also give reasonably good (+/-50%) estimates for 131I in Belarus.     

Radiocesium storage in soil microbial biomass of undisturbed alpine meadow soils and its relation to 137Cs soil-plant transfer

This study focuses on radiocesium storage in soil microbial biomass of undisturbed alpine meadow sites and its relation to the soil-to-plant transfer. Soil and plant samples were taken in August 1999 from an altitude transect (800-1600m.a.s.l.) at Gastein valley, Austria. Soil samples were subdivided into 3-cm layers for analyses of total, K(2)SO(4)-extractable and microbially stored (137)Cs. Microbial biomass was measured by the fumigation extraction method, and fungal biomass was quantified using ergosterol as biomarker molecule. In general, the quantity of (137)Cs stored in the living soil microbial biomass was relatively small. At the high-altitude meadows, showing high amounts of fungal biomass, microbially stored (137)Cs amounted to 0.64+/-0.14kBqm(-2) which corresponds to about 1.2-2.7% of the total (137)Cs soil inventory. At lower altitudes, microbial (137)Cs content was distinctly smaller and in most cases not measurable at all using the fumigation extraction method. However, a positive correlation between the observed soil-to-plant aggregated transfer factor, microbially stored (137)Cs and fungal biomass was found, which indicates a possible role of fungal biomass in the storage and turnover of (137)Cs in soils and in the (137)Cs uptake by plants.     

Resuspension and redistribution of radionuclides during grassland and forest fires in the Chernobyl exclusion zone: part I. Fire experiments

Controlled burning of experimental plots of forest or grassland in the Chernobyl exclusion zone has been carried out in order to estimate the parameters of radionuclide resuspension, transport and deposition during forest and grassland fires and to evaluate the working conditions of firemen. An increase of several orders of magnitude of the airborne radionuclide concentration was observed in the territory near the fire area. The resuspension factor for (137)Cs and (90)Sr was determined to range from 10(-6) to 10(-5) m(-1), and for the plutonium radionuclides from 10(-7) to 10(-6) m(-1) (related to the nuclides in the combustible biomass). These values are 2 orders of magnitude lower if they are calculated relatively to the total contamination density (including the nuclides in the soil). The radionuclide fallout along the plume axis is negligible in comparison to the existing contamination. However, the additional inhalation dose for firemen exposed in the affected area can reach the level of the additional external irradiation in the period of their mission. The plutonium nuclides constitute the dominating contribution to the inhalation dose.     

Radioactive contamination of tropical rainforest soils in Southern Costa Rica

Radionuclide content in soils from four locations in a tropical rainforest near Golfito in Southern Costa Rica was investigated. For comparison, two nearby locations in open grassland were also studied. From each site 5 soil cores down to a depth of 15 cm were taken. The median contamination with 137Cs was 584 Bq m-2 (reference date 1 January 1996) and the coefficient of variation (CV) was 50%. This contamination can be attributed to global fallout from atmospheric nuclear weapon tests between 1945 and 1980. The mean contamination is slightly lower than the value expected for the latitude (8 degrees 42': 700 Bq m-2), which may be explained by migration of radiocaesium to subsoil below 15 cm or by uptake into the living biomass. Out of the total variability of 50%, around 20% can be attributed to the sampling and measuring process uncertainties, thus leaving a 45% contribution of spatial variability. A significant difference between forest and meadow sites could be detected: the meadow sites showed lower radiocaesium soil inventories (median: 291 Bq m-2) than the forest sites (643 Bq m-2). This may be explained by the agricultural activities carried out on meadow sites which lead to an increased redistribution of caesium in the soil profile and therefore a larger fraction of the total 137Cs lying below 15 cm. Another reason for higher contamination levels under forest can be attributed to the high interception potential of dense tree canopies for dry deposition. Extrapolating the 137Cs concentration below the sampling horizon, i.e. accounting for the cut-off of the profiles by the sampling technique, results in an estimated mean of 710 Bq m-2 for the forest sites, which is very close to the expected figure. The mainly mineral part of the forest soil profiles was analysed for the 137Cs transport parameters, apparent convection velocity (v = 0.14 +/- 0.09 cm a-1) and apparent diffusion constant (D = 0.79 +/- 0.49 cm2 a-1). The maximum concentration can be found at 5.3 +/- 2.9 cm depth, the half-value depth being 7.4 +/- 1.3 cm. The mean 40K activity concentration was 175 Bq kg-1 dry matter (CV = 69%) and 226Ra and 228Ra concentrations of 9.90 Bq kg-1 (CV = 23%) and 7.93 Bq kg-1 (CV = 20%) have been found, respectively.     

Foliar and root uptake of 134Cs, 85Sr and 65Zn in processing tomato plants (Lycopersicon esculentum Mill.)

Rice is a staple food in Japan and other Asian countries, and the soil-to-plant transfer factor of 137Cs released into the environment is an important parameter for estimating the internal radiation dose from food ingestion. Soil and rice grain samples were collected from 20 paddy fields throughout Aomori Prefecture, Japan in 1996 and 1997, and soil-to-polished rice transfer factors were determined. The concentrations of 137Cs, derived from fallout depositions, stable Cs and K in paddy soils were 2.5-21 Bq kg(-1), 1.2-5.3 and 5000-13000 mg kg(-1), respectively. The ranges of 137Cs, stable Cs and K concentration in polished rice were 2.5-85 mBq kg(-1) dry wt., 0.0005-0.0065 and 580-910 mg kg(-1) dry wt., respectively. The geometric mean of soil-to-polished rice transfer factor of 137Cs was 0.0016, and its 95% confidence interval was 0.00021-0.012. The transfer factor of 137Cs was approximately 3 times higher than that of stable Cs at 0.00056, and they were well correlated. This implied that fallout 137Cs, mostly deposited up to the 1980s, is more mobile and more easily absorbed by plants than stable Cs in the soil, although the soil-to-plant transfer of stable Cs can be used for predicting the long-term transfer of 137Cs. The transfer factors of both 137Cs and stable Cs decreased with increasing K concentration in the soil. This suggests that K in the soil was a competitive factor for the transfers of both 137Cs and stable Cs from soil-to-polished rice. However, the transfer factors of 137Cs and stable Cs were independent of the amount of organic materials in soils.     

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.     

Accumulation of (137)Cs in Brazilian soils and its transfer to plants under different climatic conditions

The spatial distribution and behaviour of the global fallout (137)Cs in the tropical, subtropical and equatorial soil-plant systems were investigated at several upland sites in Brazil selected according to their climate characteristics, and to the agricultural importance. To determine the (137)Cs deposition density, undisturbed soil profiles were taken from 23 environments situated between the latitudes of 02 degrees N and 30 degrees S. Sampling sites located along to the equator exhibited (137)Cs deposition densities with an average value of 219Bqm(-2). Extremely low deposition densities of 1.3Bqm(-2) were found in the Amazon region. In contrast, the southern part of Brazil, located between latitudes of 20 degrees S and 34 degrees S, exhibited considerably higher deposition densities ranging from 140Bqm(-2) to 1620Bqm(-2). To examine the (137)Cs soil-to-plant transfer in the Brazilian agricultural products, 29 mainly tropical plant species, and corresponding soil samples were collected at 43 sampling locations in nine federal states of Brazil. Values of the (137)Cs concentration factor plant/soil exhibited a large range from 0.020 (beans) to 6.2 (cassava). Samples of some plant species originated from different collecting areas showed different concentration factors. The (137)Cs content of some plants collected was not measurable due to a very low (137)Cs concentration level found in the upper layers of the incremental soils. Globally, the soil-to-plant transfer of (137)Cs can be described by a logarithmic normal distribution with a geometric mean of 0.3 and a geometric standard deviation of 3.9.     

Radiocaesium fallout behaviour in volcanic soils in Iceland

The retention of 137Cs in various types of Andosols in Iceland was investigated. Soils were sampled at 29 sites with varying precipitation and environmental conditions. Samples were obtained from 0 to 5, 5 to 10, and 10 to 15 cm depths. The amount of radiocaesium present was quite variable, ranging between 300 and 4800 Bq m(-2) and correlated closely to total annual precipitation (r2=0.71). The majority of 137Cs, 82.7% on average, was retained in the uppermost 5 cm of the soil. The greatest penetration of 137Cs was observed for organic Histosols (76.3% in top 5 cm). The Icelandic Vitrisols (barren, poorly developed Andosols) are coarse grained with only 2-5% clay content and contain little organic matter (<1%). Yet these soils retained 74% of 137Cs in the top 5 cm. The results indicate that radiocaesium fallout is strongly retained by colloidal materials characteristic of Andosols, such as allophane and ferrihydrite. Most soils in Iceland are subject to severe and prolonged freezing and waterlogging; despite this, 137Cs is retained in the upper soil horizons and vertical migration is negligible in Icelandic Andosols. However, erosion and aeolian activity can markedly influence the amount and vertical distribution of radiocaesium in Icelandic soils.     

Distribution of environmental Cesium-137 in tree rings

Environmental ¹³⁷Cs concentrations in tree rings grown since 1914 and 1929 were measured and compared with the record of ¹³⁷Cs deposition from weapons fallout. ¹³⁷Cs was found in tree rings formed prior to 1945 when the first nuclear weapon test was conducted. The radiocesium record in wood is not correlated with that of fallout deposition.     

Deposition of 134,137Cs from Chernobyl fallout on Norway spruce and forest soil and its incorporation into spruce twigs

The aims of the present research are to describe the amounts, and the variation with time, of ¹³⁴Cs and ¹³⁷Cs in spruce-twigs (P. abies karst.) and in the soil of a spruce forest in Switzerland following deposition of the Chernobyl fallout. The activity of the twigs was subdivided into 3 compartments: the activity on their surfaces (i.e. the activity which can be removed from the twigs along with their natural wax coating), the activity incorporated into the needles and, finally, the activity incorporated into the wood. These compartments were separately sampled 6 times over a period from 54 to 233 days after the Chernobyl incident. Twigs which sprouted in two successive years (1985, 1986) were sampled and were found to show different behaviours. The activities associated with the 1986 twigs were roughly constant with time, while those of the 1985 twigs decreased exponentially, with half-lives around 150 days. The mean activity associated with 1 g (dry) of 1985 twigs is 724 mBq ¹³⁷Cs g⁻¹, of which 58% is incorporated into the twig wood, 17% into the needles and 25% associated with the adhering aerosol. ¹³⁷Cs on the surface of the needles was found to be water-insoluble. It is believed to be strongly adsorbed on to the soil-derived fraction of the aerosol residing on the needle surface and thus provides a tracer for studying the behaviour of natural aerosols on such surfaces.The same soil profile was measured before and after the Chernobyl incident, allowing direct comparison between nuclear weapons and Chernobyl fallout. The latter is mainly (56%) stored in the litter layer, with only 4% below a depth of 13 cm; it has penetrated into the soil to a much lesser extent than weapons fallout. The forest soil inventory of ¹³⁷Cs showed 2600 Bq m⁻² from nuclear weapons fallout and 6200 Bq m⁻² from Chernobyl.The ¹³⁴Cs/¹³⁷Cs activity ratio of the Chernobyl fallout was found to be 0·58 ± 0·01; the activity ratios in the different compartments investigated prove that incorporation of Cs into spruce occurred exclusively by uptake through the needles. A rough estimate indicates that in a spruce forest the activity stored in the twigs is half that stored in the soil.     

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.     

Contamination of Austrian soil with caesium-137

Austria ranks among the countries that have been most strongly affected by the Chernobyl fallout. The mean contamination with 137Cs is 21.0 kBq/m2, of which 18.7 kBq/m2 is due to the Chernobyl accident, whereas global fallout contributes 2.3 kBq/m2. Maximum values of total 137Cs contamination are nearly 200 kBq/m2. Total deposition of Chernobyl 137Cs on Austrian territory is 1.6 PBq or a fraction of around 2% of the 137Cs released from the reactor. 2115 measurements were used to draw the Austrian "caesium map". The geographical pattern of fallout distribution shows regional differences of contamination as high as 1:100.     

Distribution of 90Sr and 137Cs in Arctic soil profiles polluted by heavy metals

Effects of industrial pollution on the behaviour of radionuclides in spruce forest ecosystems were studied along a gradient from of a copper-nickel smelter in Monchegorsk, NW Russia. A reference site was situated in Lapland, Finland, 152 km west of Monchegorsk. Most of the total 137Cs activity in soil was in mineral (E and B) horizons, except at the reference site where the major part was still in the organic surface layer. Most of the total 90Sr activity still remaining in the soil profile was found in the surface layer, but the relative amount decreased with increasing level of industrial pollution. Pollutants from the smelter clearly affected the chemical speciation of radionuclides. Smaller amounts of exchangeable radionuclides were present in the organic surface layer at the most polluted sites. The decline of 137Cs with decreasing distance from the smelter correlated strongly with a similar depletion in exchangeable K and Mg. Total concentrations of 137Cs and 90Sr showed high correlations with exchangeable cations, particularly in the E and upper B horizon. A sudden change in behaviour of 137Cs in the lower B horizon may be associated with changes in clay mineralogy along the soil profile caused by weathering.