Predicting the transfer of radiocaesium from organic soils to plants using soil characteristics

A model predicting plant uptake of radiocaesium based on soil characteristics is described. Three soil parameters required to determine radiocaesium bioavailability in soils are estimated in the model: the labile caesium distribution coefficient (kd1), K+ concentration in the soil solution [mK] and the soil solution-->plant radiocaesium concentration factor (CF, Bq kg-1 plant/Bq dm-3). These were determined as functions of soil clay content, exchangeable K+ status, pH, NH4+ concentration and organic matter content. The effect of time on radiocaesium fixation was described using a previously published double exponential equation, modified for the effect of soil organic matter as a non-fixing adsorbent. The model was parameterised using radiocaesium uptake data from two pot trials conducted separately using ryegrass (Lolium perenne) on mineral soils and bent grass (Agrostis capillaris) on organic soils. This resulted in a significant fit to the observed transfer factor (TF, Bq kg-1 plant/Bq kg-1 whole soil) (P < 0.001, n = 58) and soil solution K+ concentration (mK, mol dm-3) (P < 0.001, n = 58). Without further parameterisation the model was tested against independent radiocaesium uptake data for barley (n = 71) using a database of published and unpublished information covering contamination time periods of 1.2-10 years (transfer factors ranged from 0.001 to 0.1). The model accounted for 52% (n = 71, P < 0.001) of the observed variation in log transfer factor.     

Radiocaesium soil-to-wood transfer in commercial willow short rotation coppice on contaminated farm land

The feasibility of willow short rotation coppice (SRC) for energy production as a revaluation tool for severely radiocaesium-contaminated land was studied. The effects of crop age, clone and soil type on the radiocaesium levels in the wood were assessed following sampling in 14 existing willow SRC fields, planted on radiocaesium-contaminated land in Sweden following Chernobyl deposition. There was only one plot where willow stands of different maturity (R6S2 and R5S4: R, root age and S, shoot age) and clone (Rapp and L78183 both of age category R5S4) were sampled and no significant differences were found. The soils differed among others in clay fraction (3-34%), radiocaesium interception potential (515-6884 meq kg(-1)), soil solution K (0.09-0.95 mM), exchangeable K (0.58-5.77 meq kg(-1)) and cation exchange capacity (31-250 meq kg(-1)). The soil-to-wood transfer factor (TF) of radiocaesium differed significantly between soil types. The TF recorded was generally small (0.00086-0.016 kg kg(-1)), except for willows established on sandy soil (0.19-0.46 kg kg(-1)). Apart from the weak yet significant exponential correlation between the Cs-TF and the solid/liquid distribution coefficient (R2 = 0.54) or the radiocaesium interception potential, RIP (R2 = 0.66), no single significant correlations between soil characteristics and TF were found. The wood-soil solution 137Cs concentration factor (CF) was significantly related to the potassium concentration in the soil solution. A different relation was, however, found between the sandy Tr?dje soils (CF = 1078.8 x m(K)(-1.83), R2 = 0.99) and the other soils (CF = 35.75 x m(K)(-0.61), R2 =0.61). Differences in the ageing rate of radiocaesium in the soil (hypothesised fraction of bioavailable caesium subjected to fast ageing for Tr?dje soils only 1% compared to other soils), exchangeable soil K (0.8-1.8 meq kg(-1) for Tr?dje soils and 1.5-5.8 meq kg(-1) for the other soils) and the ammonium concentration in the soil solution (0.09-0.31 mM NH4+ for the Tr?dje soils compared to 0.003-0.11 mM NH4+ for the other soils) are put forward as potential factors explaining the higher CF and TF observed for the Tr?dje soils. Though from the dataset available it was not possible to unequivocally predict the Cs-soil-to-wood-transfer, the generally low TFs observed point to the particular suitability for establishment of SRC on radiocaesium-contaminated land.     

A simple method for the estimation of the bioavailability of radiocaesium from herbage contaminated by adherent soil

Adherent soil may contribute a large proportion of the radiocaesium content of sampled vegetation. Consequently, inadvertent ingestion of adherent soil can contribute significantly to the radiocaesium intake of grazing animals, and needs to be accounted for within radiological assessments. However, accurate estimation of the degree of soil adhesion on vegetation is acknowledged to be difficult. To determine the relative contributions of vegetation and soil to the radiocaesium contamination of milk and tissues, soil-specific estimation of radiocaesium bioavailability values would be required. Here we suggest that a previously developed in-vitro bioavailability assay (involving a 2 h extraction with 0.1 M stable CsCl) can be used to estimate the true absorption coefficient of radiocaesium associated with sampled vegetation directly. Using this technique, seasonal trends in bioavailability are demonstrated to vary in accordance with estimations of the degree of soil adherent to vegetation collected from an upland pasture. The use of this technique would negate the need for detailed measurements of the amount of soil adhering to sampled vegetation and soil-specific radiocaesium bioavailability assessments.     

Laboratory experiments to predict changes in radiocaesium root uptake after flooding events

Changes in soil solution composition after a flooding event were hypothesised to be one of the key factors in explaining changes in radiocaesium incorporation in the food chain in the areas affected by the Chernobyl accident. A laboratory methodology was set up to monitor changes in the soil solution composition after a sequence of flooding cycles. Experiments were performed using column and batch approaches on test soils with contrasting initial soil solution composition (high and low initial concentrations of K+). Results from column experiments indicated a potential increase in NH(4)(+) concentrations, a parameter which could lead to an increase in the radiocaesium root uptake. Batch results in the soil with high initial K+ concentration showed that after a number of flooding cycles, especially for high ratios of flooding solution/mass of soil, K+ concentration decreased sometimes below a threshold value (around 0.5-1 mmol l(-1)), a fact that could lead to an increase in radiocaesium transfer. For the soils with a low initial K+ concentration, the flooding solution increased K+ and NH(4)(+) values in the soil solution. The comparison of test soils with soils from Ukraine areas affected by flooding showed that the final stage in soil solution composition was similar in both cases, regardless of the initial composition of the soil solution. Moreover, the comparison with unflooded soils from the same area showed that potential changes in other soil parameters, such as (137)Cs activity concentration, clay content, and radiocaesium interception potential, RIP (a parameter that estimates the radiocaesium specific sorption capacity of a soil), should also be monitored for additional effects due to the flooding event. Therefore, the changes in the root uptake would depend on the resulting situation from changes in RIP, K+ and NH(4)(+) values in the soil solution.     

Radiocaesium contamination of meadow vegetation--time-dependent variability and influence of soil characteristics at grassland sites in Austria

Long-term trends of 137Cs and 40K concentrations in meadow grass and soil-plant transfer data at eight different sites in Upper Austria are presented. Geometric means of 137Cs TF-data and Tagg values vary between 0.03-1.06 and 0.0005-0.0184 depending on site, respectively. 40K results are less variable with TF values covering a range of 0.31-2.01. Only at one site was a significant decrease of 137Cs concentration (decay-corrected) in meadow vegetation observed during the observation period 1992-1999. Seasonal trends of 40K and 137Cs were investigated at one site in 1996. Both elements show decreasing concentrations in plants from beginning of May-July, followed by a peak in September. Although this pattern was not very pronounced, there are some hints that it may explain deviations of long-term trends in 137CS levels in grass caused by unusual weather conditions as indicated by phenological climate data (beginning of sweet cherry and black elder blossoming). Finally, TF values were correlated with soil characteristics, revealing a negative correlation of radiocaesium soil-plant transfer with soil pH, exchangeable and extractable fractions of Mg, Ca and Na as well as a positive correlation with exchangeable Al.     

Radiocaesium soil-to-plant transfer in tropical environments

In this work, soil-to-plant transfer factors of radiocaesium are predicted based on soil properties such as pH, organic matter content, exchangeable K+ and clay content valid for the tropical environments in Bangladesh, China and Japan, and using a previously published model. Due to insufficient data of soil properties in the selected regions, the average values of pH, organic matter content, exchangeable K+ and clay content were taken as the input model parameters within the ranges given for Asia. Nevertheless, a complete set of soil properties of Japanese soils was used to compare the measured and calculated TF values of radiocaesium for radish. The calculated TF values for radiocaesium are comparable with the measured values especially for leafy parts of a plant. However, calculated values for rice, an important crop in Asia are found to overestimate the measured values due to an overestimate of calculated CECs in soils in the selected regions. The empirical parameters used in the model need to be re-evaluated for the specific part of a plant and/or for a variety of different plants. Alternatively, a general conversion factor for each part of a plant and/or for a variety of different plants for a specific region is suggested for tropical environments.     

Effect of K and bentonite additions on Cs-transfer to ryegrass

Bentonite amendments are generally ineffective in reducing the soil-to-plant radiocaesium transfer but have previously been shown that bentonites in the K-form having been subjected to wetting-drying cycles had pronounced radiocaesium binding capacities. We have investigated the effect of wetting-drying (WD) on Radiocaesium Interception Potential (RIP) development in three K-bentonites and K-bentonite soil mixtures, using a variety of procedures: homogenisation of the bentonites with K through dialysis (K(B)), or partial transformation of the bentonite to the K-form in the presence of a solution of K2CO3 (K(L)) or in presence of solid K2CO3 (K(S)). Of the three strategies tested, addition of K2CO3 (solid) at a dose of 2 meq g(-1) clay and adding the K-bentonite mixtures to the soil resulted in the highest RIP increase after 20 WD cycles. The procedure giving the highest RIP yield is the most practical for further applications and was used in a pot experiment under greenhouse condition. When expressing the RIP increase of the soil-bentonite mixtures per unit bentonite added (RIP yield), 28- to 110-fold RIP increases were observed up to a value of approximately 60,000 meq kg(-1) (6 times higher than the RIP for illite). The beneficial effect following K-bentonite application was shown to be dependent both on a sorption enhancement effect (direct RIP effect) and fixation effects (indirect RIP effect). Greenhouse testing proved that the RIP effects observed in greenhouse could be predicted by making use of the sorption data from the laboratory tests. Optimum soil-amendment would be obtained with bentonites with high initial sorption RIP and a high sorption RIP increase when subjected to WD in the presence of potassium. Hypothised Transfer Factor (TF)-reductions of at least 10-fold could result when mixing approximately 1% bentonite, like Otay bentonite (RIP yield 99,000 meq kg(-1) after WD in presence of K if only fine particle size of <1mm considered) with the contaminated ploughing layer.     

Transfer factors of radioactive Cs,Sr, Mn,Co and Zn from Japanese soils to root and leaf of radish

Transfer factors (TFs) of some selected radionuclides from ten different Japanese soils to radish have been studied by radiotracer experiments. The geometric mean values of TFs (on a wet weight basis) of radioactive Cs, Sr, Co, Mn and Zn for edible parts of radish (tuber) were 0.0090. 0.029, 0.00094, 0.0034 and 0.067, respectively. TFs for leaf were higher than those for tuber. The geometric mean values of leaf/tuber ratios were 4.1 for Cs, 4.9 for Sr, 1.6 for Co, 11 for Mn and 1.9 for Zn. Most of the Cs TFs obtained for andosol, which is the most common arable soil in Japan, were higher than those for the other soils. This might be due to the high concentrations of organic matter and alophen in andosol. The obtained TFs were compared to reference values of IAEA Technical Report 364.     

Soil-to-plant transfer of radiocaesium for selected tropical plant species in Bangladesh

Soil-to-plant transfer factors (TF) of radiocaesium (137Cs) were determined under field condition for grassy vegetation grown in Bangladesh at contaminated land in the Atomic Energy Research Establishment (AERE) campus. TF values for rice, grass and grassy/root vegetations grown in the same type of soil were also measured under pot condition. TF values of 137Cs for grassy vegetation (2.4 x 10(-2) -4.2 x 10(-2) with an average of 3.1 x 10(-2) +/-0.005) obtained under field condition were slightly lower than the values for grass and grassy/root vegetations (2.9 x 10(-2) -6.6 x 10(-2) with an average of 4.8 x 10(-2) +/-0.01 for grass and grassy vegetations and 2.3 x 10(-2) -5.6 x 10(-2) with an average of 4.0 x 10(-2) +/-0.009 for root vegetations, respectively) obtained under pot condition. However, TF values (9.0 x 10(-3) -2.6 x 10(-2) with an average of 1.9 x 10(-2) +/-0.004) obtained for rice were about a factor of 4 lower than the values obtained for grass and grassy/root vegetations. When the properties of the AERE soils as input parameters were used in the soil-plant transfer model of Absalom, the estimated TF values (4.5 x 10(-2) -6.7 x 10(-2) with an average of 5.3 x 10(-2) +/-0.006) were consistent with the measured values obtained for grass and grassy vegetations under pot condition, however, the model overestimates the TF values for rice.     

Effect of external potassium (K) supply on the uptake of 137Cs by spring wheat (Triticum aestivum cv. Tonic): a large-scale hydroponic study.

A large-scale hydroponic experiment was carried out in a non-controlled greenhouse. Spring wheat plants were grown to maturity at four levels of external K concentration (2, 4, 20 and 40 mgl(-1)) and one concentration of radiocaesium (8 Bqml(-1)). Concentrations of K and radiocaesium in the growth solution were closely monitored, and replenishments were made upon depletion. K effectively competed with radiocaesium in terms of root uptake. Activity concentrations of radiocaesium in plants differed significantly between the four K treatments; the activity concentration at the lowest external K concentration being 100 times higher than that at the highest K level. The relationship between radiocaesium uptake and external K level could be described by a negative power function; this showed that when the K level reached around 12 mgl(-1), further increases in the external K level resulted only in slight changes in its inhibitory effect. As a result of this inhibitory effect of potassium supply, concentrations of radiocaesium in plant tissues, grains in particular, were greatly reduced at high external K concentration. Mechanisms involved in Cs-K interaction in root uptake are also discussed.     

Predictions of in situ solid/liquid distribution of radiocaesium in soils

Previous work has demonstrated that plant uptake of radiocaesium (RCs) is related to the activity concentration of RCs in soil solution, which is linked to the soil/soil solution distribution coefficient, K(D). The solid-liquid distribution of RCs is generally studied in soil suspensions in the laboratory and there are few reported measurements for in situ soil solutions. From a data set of 53 different soils (contaminated with either 134CsCl or 137CsCl) used in pot trials to investigate grass uptake of RCs, we analysed the variation of in situ K(D) with measured soil properties. The soils differed widely in % clay (0.5-58%), organic matter content (1.9-96%) and pH (2.4-7.0, CaCl2). The K(D) varied between 29 and 375,000 L kg-' (median 1460 L kg(-1)). Stepwise multiple regression analysis showed a significant correlation between the log K(D) and pH (p < 0.001), log %clay (p < 0.01) and log exchangeable K (p < 0.001) (overall R2 = 0.70). The in situ K(D) values were further compared to K(D)S predicted using an existing model, which assumes that RCs sorption occurs on specific sites and regular ion-exchange sites on the soil solid phase. Sorption of RCs on specific sites was quantified from the radiocaesium interception potential (RIP) measured for each soil and the soil solution concentrations of K+ and NH4+. The in situ log K(D) correlated well with the predicted K(D) (R2 = 0.85 before plant growth, R2 = 0.83 after plant growth). However, the observations were fivefold to eightfold higher than the predictions, particularly for the mineral soils. We attribute the under-prediction to the long contact times (minimum 4 weeks) between the RCs tracers and our experimental soils relative to the short (24 h) contact times used in RIP measurements. We conclude that our data confirmed the model but that ageing of RCs in soil is a factor that needs to be considered to better predict in situ KD values.     

Does soil adhesion matter when predicting radiocaesium transfer to animals?

A sward will often have significant amounts of soil adhered to the vegetation surfaces which will be ingested by grazing animals. If the soil is contaminated by radioactive fallout then it can serve as a dietary source of radionuclides, in addition to any root uptake by the plants. This study is an attempt to quantitatively assess the importance of soil adhesion as a source of radiocaesium to sheep using the RUINS model which simulates radiocaesium transfer in grazing systems.The method of simulating the contamination of vegetation surfaces used by the RUINS model is described, and the importance of the availability of radiocaesium associated with adhered soil relative to plant incorporated radiocaesium discussed. Two sets of simulations are presented: one in which the soil is treated as a medium providing a uniform availability of radiocaesium, and the second in which account is taken of the partitioning of radiocaesium in the soil between ‘fixed’ and ‘labile’ phases.The results demonstrate that, because of the reduced absorption in the gut of radiocaesium associated with soil, animals grazing pastures with significant amounts of radiocaesium associated with adhered soil will not be as contaminated as radiocaesium activity concentrations measured in bulk vegetation samples would suggest. Therefore, the extent of soil adhesion needs to be considered if predictions of radiocaesium contamination of animal products are to be made on the basis of measured activities of sampled vegetation. However, soil adhesion is unlikely to be a significant dietary source of available radiocaesium, unless the soil concerned exhibits an unusually high bioavailability of radiocaesium. Moreover the simulation results indicate that differences in availability between soil types observed experimentally are consistent with the partitioning between fixed and labile soil compartments made by the RUINS model.     

Uptake and elimination of radiocaesium in fish and the "size effect."

A number of hypotheses have previously been developed concerning the rates of uptake and elimination of radiocaesium (137Cs) in fish. These include the influence of potassium and other water chemical parameters on both uptake and elimination, and the effect of fish size on accumulation. In order to test these hypotheses, we have assembled a data set comprising more than 1,000 measurements of radiocaesium (137Cs) in predatory fish (perch, pike and brown trout) in nine European lakes during the years after Chernobyl. These data have been analysed using simple models for uptake and excretion of 137Cs in fish, showing that: 1. Fish-water concentration factors (CF) were inversely proportional to potassium [K+] concentration of the different lakes, in agreement with previous studies. 2. The uptake rate of 137Cs in fish was negatively correlated with lake [K+], but excretion rate was independent of [K+]. 3. Lower than expected CF values were found in one lake, Iso Valkj?rvi, Finland. This is attributed to inhibition of the K+ (and therefore 137Cs) high affinity transport system in aquatic plants and fish by low pH and/or low Ca2+. 4. The inclusion of fish weight as a parameter in our dynamic model significantly improves the ability of the model to fit the observed measurements of 137Cs. 5. The model developed from the above hypotheses was able to fit the data from nine different lakes to within approximately a factor of 3 of the observed values.     

Bioavailability of radiostrontium in soil: experimental study and modeling

Parameters related to 90Sr mobility in the soil-plant system are reported: exchangeable content, selectivity coefficient, and transfer factor. Large mobility of 90Sr in different soil types was shown. The fraction of exchangeable 90Sr varied between 70 and 90%. The selectivity coefficient K(C)(90Sr/Ca) values were in the range 1.3-2.5. The radionuclide transfer factors (TF) varied by a factor of 9.6 for barley seedlings and by a factor of 6.6 for lupine seedlings. The exchangeable Ca content was the determinant soil parameter responsible for differences in 90Sr biological availability. A static model was devised that describes 90Sr sorption from soil solution by soil and on the root surface. The parameter of 90Sr bioavailability (A) has been suggested. Parameter A was calculated from data on soil exchangeable Ca content and 90Sr mobility indicators--exchangeable fraction of the radionuclide and the selectivity coefficient K(C)(90Sr/Ca). A correlation was found between TF and parameter A.     

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.     

Long-term investigations of radiocaesium activity concentrations in carp in North Croatia after the Chernobyl accident

Long-term investigations of radiocaesium activity concentrations in carp in the Republic of Croatia are presented. The radiocaesium levels in carp decreased exponentially and the effective ecological half-life of (137)Cs was estimated to be about 1 year during 1987-2002 and 5 years during 1993-2005. The observed (134)Cs:(137)Cs activity ratio in carp was found to be similar to the ratio observed in other environmental samples. The concentration factor for carp (wet weight) was estimated to be 128+/-74 Lkg(-1), which is in reasonable agreement with model prediction based on K(+) concentrations in water. Estimated annual effective dose received by adult members of the Croatian population due to consumption of carp contaminated with (134)Cs and (137)Cs are small: per capita dose from this source during 1987-2005 was estimated to be 0.5+/-0.2 microSv. Due to minor freshwater fish consumption in Croatia and low radiocaesium activity concentrations in carp, it can be concluded that carp consumption was not a critical pathway for the transfer of radiocaesium from fallout to humans after the Chernobyl accident.     

Fibre crops as alternative land use for radioactively contaminated arable land

The transfer of radiocaesium, one of the most important and widespread contaminants following a nuclear accident, to the fibre crops hemp (Cannabis sativa L.) and flax (Linum usitatissimum L.) as well as the distribution of radiocaesium during crop conversion were studied for sandy soil under greenhouse and lysimeters conditions. Soil parameters did not unequivoqually explain the transfer factors (TF) observed. TFs to flax stems ranged from 1.34 to 2.80x10(-3) m2 kg(-1). TFs to seeds are about a factor of 4 lower. During the retting process for separating the fibres from the straw, more than 95% of the activity was removed with the retting water. For hemp, the TF to the stem was about 0.6x10(-3) m2 kg(-1). For hemp, straw and fibres were mechanically separated and TF to straw was about 0.5x10(-3) m2 kg(-1) and to fibres 1.0x10(-3) m2 kg(-1). Generally, the TFs to the useable plant parts both for hemp and flax, are low enough to allow for the production of clean end-products (fibre, seed oil, biofuel) even on heavily contaminated land. Given the considerable decontamination during retting, contamination levels in flax fibres would only exceed the exemption limits for fibre use after production in extreme contamination scenarios (>12,300kBq m(-2)). Since hemp fibres are mechanically separated, use of hemp fibres is more restricted (contamination <740kBq m(-2)). Use of stems as biofuel is restricted to areas with contamination levels of <250 and 1050kBq m(-2) for flax and hemp, respectively. Use of seeds for edible oil production and flour is possible almost without restriction for flax but due to the high TFs to seed observed for hemp (up to 3x10(-3) m2 kg(-1)) consumption of hemp seed products should be considered with care.     

On the influence of soil properties on the transfer of 137Cs from two soils (Chromic Luvisol and Eutric Fluvisol) to wheat and cabbage

Two types of soils (Eutric Fluvisol and Chromic Luvisol) and two crops (wheat and cabbage) were investigated for determination of the transfer of 137Cs from soil to plant. Measurements were performed using gamma-spectrometry. Results for the soil characteristics, transfer factors of the radionuclides (TF), and conversion factors (CF) (cabbage/wheat) were obtained. The transfer of 137Cs was higher for Chromic Luvisol for both the plants. Statistically significant dependence of TF of 137Cs on its concentration in soil was established for cabbage. Dependence between K content in the soil and the transfer factor of 137Cs was not found due to the high concentrations of available K. Use of bioconcentration factor (BCF) (ratio between the activity concentration of a radionuclide in a reference plant to its concentration in another plant) is demonstrated and proposed for risk assessment studies.     

Uptake and distribution of natural radioactivity in wheat plants from soil

The uptake of naturally occurring uranium, thorium, radium and potassium by wheat plant from two morphologically different soils of India was studied under natural field conditions. The soil to wheat grain transfer factors (TF) were calculated and observed to be in the range of 4.0 x 10(-4) to 2.1 x 10(-3) for 238U, 6.0 x 10(-3) to 2.4 x 10(-2) for 232Th, 9.0 x 10(-3) to 1.6 x 10(-2) for 226Ra and 0.14-3.1 for 40K. Observed ratios (OR) of radionuclides with respect to calcium have been calculated to explain nearly comparable TF values in spite of differences in soil concentration of the different fields. They also give an idea about the discrimination exhibited by the plant in uptake of essential and nonessential elements. The availability of calcium and potassium in soil for uptake affects the uranium, thorium and radium content of the plant. The other soil factors such as illite clays of alluvial soil which trap potassium in its crystal lattice and phosphates which form insoluble compounds with thorium are seen to reduce their availability to plants. A major percentage (54-75%) of total 238U, 232Th and 226Ra activity in the plant is concentrated in the roots and only about 1-2% was distributed in the grains, whereas about 57% of 40K activity accumulated in the shoots and 16% in the grains. The intake of radionuclides by consumption of wheat grains from the fields studied contributes a small fraction to the total annual ingestion dose received by man due to naturally existing radioactivity in the environment.