Reconstruction of 131I radioactive contamination in Ukraine caused by the Chernobyl accident using atmospheric transport modelling

The evaluation of ¹³¹I air and ground contamination field formation in the territory of Ukraine was made using the model of atmospheric transport LEDI (Lagrangian–Eulerian DIffusion model). The ¹³¹I atmospheric transport over the territory of Ukraine was simulated during the first 12 days after the accident (from 26 April to 7 May 1986) using real aerological information and rain measurement network data. The airborne ¹³¹I concentration and ground deposition fields were calculated as the database for subsequent thyroid dose reconstruction for inhabitants of radioactive contaminated regions. The small-scale deposition field variability is assessed using data of ¹³⁷Cs detailed measurements in the territory of Ukraine. The obtained results are compared with available data of radioiodine daily deposition measurements made at the network of meteorological stations in Ukraine and data of the assessments of ¹³¹I soil contamination obtained from the ¹²⁹I measurements.     

Mesoscale modelling of radioactive contamination formation in Ukraine caused by the Chernobyl accident

This work is devoted to the reconstruction of time-dependent radioactive contamination fields in the territory of Ukraine in the initial period of the Chernobyl accident using the model of atmospheric transport LEDI (Lagrangian-Eulerian DIffusion model). The modelling results were compared with available 137Cs air and ground contamination measurement data. The 137Cs atmospheric transport over the territory of Ukraine was simulated during the first 12 days after the accident (from 26 April to 7 May 1986) using real aerological information and rain measurement network data. The detailed scenario of the release from the accidental unit of the Chernobyl nuclear plant has been built (including time-dependent radioactivity release intensity and time-varied height of the release). The calculations have enabled to explain the main features of spatial and temporal variations of radioactive contamination fields over the territory of Ukraine on the regional scale, including the formation of the major large-scale spots of radioactive contamination caused by dry and wet deposition.     

Improvements in modeling sagebrush concentrations of radioiodine released from the Hanford site

The Hanford Environmental Dose Reconstruction Project estimated the radiation dose to individuals from historical emissions of radioactive materials from the Hanford Site in Washington State. Project validation studies using predicted activity concentrations of 131I on sagebrush (Artemisia tridentata) showed a systematic underestimation against historical data during cold weather months, indicating a need for sagebrush model improvement. A deposition model for semi-volatile organic materials presented by Komp and McLachlen (Environ. Sci. Tech. 31 (1997) 886-890) is adapted here for gaseous iodine onto sagebrush. The deposition model includes a temperature-dependent term based on an integrated van't Hoff equation. Calibration data for the model are obtained from a release of 131I in 1963. Modeling results for releases in 1946 show a good match between historical data and predicted results using the new model. The new model shows improvement over interception-fraction type models, but requires plant-type-specific calibration data.     

Fallout in the New York metropolitan area following the chernobyl accident

In the metropolitan New York area, maximum concentrations in air of radioactive aerosol and gaseous debris from the Chernobyl accident of April 1986 were much lower than those measured in Europe. The observed maxima were: for gaseous ¹³¹I, 23mBq m⁻³; for aerosol samples, 20mBq m⁻³ of ¹³¹I and 9·mBq m⁻³ of ¹³⁷Cs. The data suggest that little gas-to-particle transformation of iodine occurred during transport of the radioactive cloud from the Ukraine to New York. The ratios of ¹⁰³Ru and other refractories to ¹³⁷Cs were low in the first debris sampled, debris which probably was emitted from Chernobyl in late April during the early stages of the accident. In subsequent samples these ratios were higher, presumably because debris from the later, hotter stages of the fire had reached our sampling sites. A significant fraction (25–40%) of the deposition of ¹³¹I and ¹³⁷Cs into our samplers and on grass was by dry deposition. The total deposition of Chernobyl ¹³⁷Cs in the area was <1% of that already present in the soil from fallout from past nuclear weapon tests. The highest concentration of ¹³¹I measured in fresh milk was about 1.5 B1 liter⁻¹, <0.1% of the US action level. The dose to the thyroid of a six-month-old infant who had fresh milk as a sole food source would be about 70 μGy (7 mrad).     

Validation of I ecological transfer models and thyroid dose assessments using Chernobyl fallout data from the Plavsk district, Russia

Within the project “Environmental Modelling for Radiation Safety” (EMRAS) organized by the IAEA in 2003 experimental data of ¹³¹I measurements following the Chernobyl accident in the Plavsk district of Tula region, Russia were used to validate the calculations of some radioecological transfer models. Nine models participated in the inter-comparison. Levels of ¹³⁷Cs soil contamination in all the settlements and ¹³¹I/¹³⁷Cs isotopic ratios in the depositions in some locations were used as the main input information. 370 measurements of ¹³¹I content in thyroid of townspeople and villagers, and 90 measurements of ¹³¹I concentration in milk were used for validation of the model predictions.A remarkable improvement in models performance comparing with previous inter-comparison exercise was demonstrated. Predictions of the various models were within a factor of three relative to the observations, discrepancies between the estimates of average doses to thyroid produced by most participant not exceeded a factor of ten.     

Cs contamination of the Techa river flood plain near the village of Muslumovo

The results of a radiometric survey of the Techa river flood plain near the village of Muslumovo in the Chelyabinsk region of Russia are presented. The observed territory extended 16.6 km along the riverbed, with a total area of 2.5 km². The collimated scintillation detector technique was applied to in situ field measurements of ¹³⁷Cs deposition on the soil. Maps of ¹³⁷Cs deposition and soil penetration depth were developed on the basis of approximately 5000 measurements. The total ¹³⁷Cs deposition within the surveyed territory has been estimated at 6.6 TBq. The means of the total ¹³⁷Cs soil depositions at half-kilometer sites on the flood plain and its distribution along the river have also been calculated. A maximum ¹³⁷Cs contamination above 7.5 MBq/m² is associated with a bank height up to 1 m above the usual water level. The data identify zones of intensive radionuclide sedimentation and transit zones.     

Probabilistic risk assessment for long-range atmospheric transport of radionuclides

A simplified means of probabilistic risk assessment (PRA) for long-range atmospheric transport based on a K-diffusion model is presented. In a case study, model parameters are estimated by comparing with the results of long-range atmospheric dispersion model calculations using one-year numerical weather prediction model data. It is found that the estimated ensemble mean provides a reasonable first approximation to the total dry and wet deposition from the one-year continuous release.     

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.     

Monitoring of radionuclides contamination of soils in Shatsk National Natural Park (Volyn region, Ukraine) during 1994-2001

The results of studies of radionuclide contamination of the soils in the western part of the territory of Shatsk National Natural Park (ShNNP), Volyn region, Ukraine, performed during 1994-2001 are presented. Based on the experimental results, the three-dimensional plot of the 137Cs density contamination for the soils at the territory under investigation has been constructed. The monitoring during 1994-2001 of the 137Cs vertical distributions in the different kinds of soils from the Park and the forecasting of the distribution changes of the depth down to 50 cm for the sod loamy sandy gleyed loamy sand soil of the Park up to 2086 have been performed.     

Prediction of SVOC vegetation and atmospheric concentrations using calculated deposition velocities

A simple modeling concept was previously applied to study air-foliage exchange of both polybrominated diphenyl ethers (PBDEs) and polycyclic aromatic hydrocarbons (PAHs) using field measurements. In this paper, the predictive capabilities of this framework were tested using an independent set of data collected at the same sampling location for a different time period. Firstly, atmospheric (particle-bound and gaseous phase) PBDE and PAH concentrations were used to predict their accumulation in spruce needles. Conversely, we used PBDE and PAH concentrations in vegetation to predict their atmospheric concentrations. In both cases, calculated and measured values showed good agreement, providing evidence that the developed framework and our derived deposition velocities can be used as a predictive tool for these two different classes of semi-volatile organic compounds.     

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.     

Airborne 131I at a background monitoring site

As part of an environmental surveillance program, measurements of 131I in samples of atmospheric aerosols were determined in week-long collection periods at 0.3 km and 1.5 km from a municipal-sewage sludge incinerator located in Albany, New York. During an 11-month period when the sampler was temporarily located near the incinerator, sampling canisters of activated charcoal nearly always contained detectable airborne 131I activity (range of 0.1-6.0 mBq m(-3)). In contrast, remote concentrations where the sample was normally located were near or below analytical detection limits, both before and after the 11-month relocation. Activities of wet and dry fallout at both locations were below detection limits. The source of 131I in the aerosols associated with the sewage sludge was likely excreta from patients following medical treatments at local hospitals.     

Use of AMS in the marine environment

In recent years, the field of AMS has expanded into many areas of science. This paper reviews a variety of applications of AMS in the marine environment, focusing particularly on recent developments and applications. Following a brief summary of the three main isotope techniques used in environmental studies: dating, tracing and source identification, a number of applications are considered. Traditional (14)C-dating is no longer the dominant application of AMS measurements, and together with measurements of (10)Be, (26)Al and (36)Cl, much of the research is now directed towards an understanding of global climate change via studies of oceanic circulation, atmospheric processes and past climates by cosmic ray exposure dating. Profiles of long-lived cosmogenic radionuclides in sediments and ice cores, as a function of depth and, thus, age, provide key information on past solar variability, production rate changes and atmospheric transport and deposition mechanisms. Useful paleoclimatic information may be derived from these archives both because deposition is influenced by climate and because solar activity (which influences production) and solar radiance (which influences climate) are correlated. In recent years, emphasis has been put on the development and application of AMS techniques for the measurement of heavier long-lived isotopes, including (99)Tc, (129)I, (236)U and other actinide isotopes. AMS combines ultra low detection limits and the possibility to analyse isotope ratios that can be difficult with traditional instruments and has been used in a number of applications on the consequences and uses of releases from nuclear energy. Finally, the use AMS in environmental sciences is expected to expand further in the foreseeable future with long-lived cosmogenic radionuclides contributing to a large body of knowledge on processes involving atmosphere, oceans, ice sheets, biosphere, soils and sediments.     

A validation study for the transport of 134Cs to strawberry

The paper presents results on model validation by field experiment for transport of 134Cs to strawberry. The transfer of 134Cs to herbaceous plants was investigated following a wet deposition after an acute release during 2000. Leaf-to-fruit, soil-to-fruit and direct fruit pathways were examined. The available meteorological and local soil information together with the experimental data were taken into account by the model RUVFRU. The processes are described by first order differential equations. In the case of foliar contamination scenarios measured and calculated results for fruit are in good agreement. However, the results of soil contamination scenarios provide large differences of up to three orders of magnitude between model predictions and experimental values for either fruit or other parts of the plant. The bias could be explained by the underestimation of the interception of the plant at the beginning of the season, in the soil contamination scenario. The model output permits prompt assessment of emergency situations and provides aid making decisions concerning mitigation of the consequences of the accident.     

Radiostrontium hot spot in the Russian Arctic: ground surface contamination by (90)Sr at the "Kraton-3" underground nuclear explosion site

Strontium-90 activity concentrations in surface soils and areal deposition densities have been studied at a site contaminated by an accidental release to atmosphere from the underground nuclear explosion "Kraton-3" conducted near the Polar Circle (65.9 degrees N, 112.3 degrees E) within the territory of the former USSR in 1978. In 2001-2002, the ground surface contamination at 14 plots studied ranged from 20 to 15 000 kBq m(-2), which significantly exceeds the value of 0.44 kBq m(-2) deduced for three background plots. The zone with substantial radiostrontium contamination extends, at least, 2.5 km in a north-easterly direction from the borehole. The average (137)Cs/(90)Sr ratio in the ground contamination originated from the "Kraton-3" fallout was estimated to be 0.55, which is significantly different from the ratio of 2.05 evaluated for background plots contaminated mostly from global fallout. Although vertical migration of (90)Sr in all undisturbed soil profiles studied is more rapid than that for (137)Cs, the depth of percolation of both radionuclides into the ground is mostly limited to the top 10-20 cm, which may be explained, primarily, by permafrost conditions. The horizontal migration rate of radiostrontium in the aqueous phase exceeds the radiocaesium migration rate by many times. This phenomenon seems to be a reason for the significant enrichment of the soil surface layers by radiostrontium at some sites, with variations occurring in accordance with small-scale irregularities of landscape.     

Model testing using data on 131I released from Hanford

The Hanford test scenario described an accidental release of 131I to the environment from the Hanford Purex Chemical Separations Plant in September 1963. Based on monitoring data collected after the release, this scenario was used by the Dose Reconstruction Working Group of BIOMASS to test models typically used in dose reconstructions. The primary exposure pathway in terms of contribution to human doses was ingestion of contaminated milk and vegetables. Predicted mean doses to the thyroid of reference individuals from ingestion of 131I ranged from 0.0001 to 0.8 mSv. For one location, predicted doses to the thyroids of two children with high milk consumption ranged from 0.006 to 2 mSv. The predicted deposition at any given location varied among participants by a factor of 5-80. The exercise provided an opportunity for comparison of assessment methods and conceptual approaches, testing model predictions against measurements, and identifying the most important contributors to uncertainty in the assessment result. Key factors affecting predictions included the approach to handling incomplete data, interpretation of input information, selection of parameter values, adjustment of models for site-specific conditions, and treatment of uncertainties.     

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.     

Reconstruction of atmospheric concentrations and deposition of uranium and decay products released from the former uranium mill at Uravan, Colorado

Radionuclide concentrations in air from uranium milling emissions were estimated for the town of Uravan, Colorado, USA and the surrounding area for a 49-yr period of mill operations beginning in 1936 and ending in 1984. Milling processes with the potential to emit radionuclides to the air included crushing and grinding of ores; conveyance of ore; ore roasting, drying, and packaging of the product (U(3)O(8)); and fugitive dust releases from ore piles, tailings' piles, and roads. The town of Uravan is located in a narrow canyon formed by the San Miguel River in western Colorado. Atmospheric transport modeling required a complex terrain model. Because historical meteorological data necessary for a complex terrain model were lacking, meteorological instruments were installed, and relevant data were collected for 1 yr. Monthly average dispersion and deposition factors were calculated using the complex terrain model, CALPUFF. Radionuclide concentrations in air and deposition on ground were calculated by multiplying the estimated source-specific release rate by the dispersion or deposition factor. Time-dependent resuspension was also included in the model. Predicted concentrations in air and soil were compared to measurements from continuous air samplers from 1979 to 1986 and to soil profile sampling performed in 2006. The geometric mean predicted-to-observed ratio for annual average air concentrations was 1.25 with a geometric standard deviation of 1.8. Predicted-to-observed ratios for uranium concentrations in undisturbed soil ranged from 0.67 to 1.22. Average air concentrations from 1936 to 1984 in housing blocks ranged from about 2.5 to 6 mBq m(-3) for (238)U and 1.5 to 3.5 mBq m(-3) for (230)Th, (226)Ra, and (210)Pb.     

Effects of model complexity on uncertainty estimates

In the Model Complexity working group of BIOMOVS II, models of varying complexity have been applied to a theoretical problem concerning downward transport of radionuclides in soils. The purpose was to study how uncertainty in model predictions varies with model complexity and how model simplifications can suitably be made. A scenario describing a case of surface contamination of a pasture soil was defined. Three different radionuclides with different environmental behavior and radioactive half-lives were considered: ¹³⁷Cs, ⁹⁰Sr and ¹²⁹I. A detailed specification of the parameters required by different kinds of models was given, together with reasonable values for the parameter uncertainty. A total of seven modelling teams participated in the study using 13 different models. Four of the modelling groups performed uncertainty calculations using nine different modelling approaches. The models ranged in complexity from analytical solutions of a 2-box model using annual average data to numerical models coupling hydrology and transport using data varying on a daily basis.     

High-resolution spatial analysis of stomatal ozone uptake in arable crops and pastures

Ozone effects on plants depend on atmospheric transport and stomatal uptake. Thus, ozone-risk assessments should use measured ozone concentrations and account for the influence of atmospheric conditions and soil moisture on stomatal and nonstomatal ozone deposition. This requires disaggregated data for the physical input parameters and species-specific data for specific stomatal conductance (g(s)). In this study, an approach was developed based on a resistance analogue transport model. This model requires interpolated routine-measuring data for ozone concentration at 3-5 m height, wind speed, precipitation, and soil moisture content as inputs to estimate the amount of ozone taken up by wheat (Triticum aestivum) and grass/clover pastures with a 1x1-km resolution. The model was applied to the area under agricultural production in Switzerland. Using data for June 1994, the calculations revealed that the median of the distribution of stomatal ozone uptake was 88% higher in wheat compared to grassland. This was mainly due to the higher maximum stomatal conductance in wheat. Because ozone flux to soil and to external plant surfaces was comparable in both vegetation types, the difference in the stomatal fluxes was mainly responsible for distinct differences in flux partitioning. In both cases, only about 11% of the total cumulative flux was absorbed by external plant surfaces, whereas the soil was a strong sink responsible for as much as 50% of the total flux into grasslands. The higher-ozone flux to wheat resulted in clearly lower-ozone concentrations at canopy height, but no significant correlation between cumulative canopy-level ozone exposure, expressed as accumulated exposure above 40 ppb (AOT40), and stomatal uptake was found. Thus, to estimate the ozone risk for crops using a flux-based approach may lead to results that differ substantially from those obtained with a concentration-based approach.