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

The evaluation of (131)I 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 (131)I 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 (131)I 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 (137)Cs 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 (131)I soil contamination obtained from the (129)I 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.     

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).     

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.     

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.     

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.     

Fallout deposition at Monaco following the chernobyl accident

Increased atmospheric radioactivity from the Chernobyl accident was first detected on air filters taken in Monaco on 30 April 1986, with maximum activities of 10, 2·9, 1·5 and 0·84 Bqm^dash3 for ¹³²Te, ¹³¹ I, ¹³⁷Cs and ¹³⁴Cs, respectively, occurring about 1–3 May 1986. About one week later the activities had fallen to about 1% of peak values. A total of 33 radioisotopes were detected. The integrated inventories were significantly less than at other sites to the east. Preliminary results of plutonium analyses are also presented, together with other deposition data in rain and soil.     

The comparison of generic model predictions with chernobyl fallout data on the transfer of radioiodine over the air-pasture-cow-milk pathway

Data have been collected on concentrations of ¹³¹I in air, vegetation and milk from numerous locations receiving Chernobyl fallout. Time-integrated concentrations derived from these data are used to compare predictions from generic models used for routine environmental radiological assessments. In general, the models markedly overestimated the transfer of ¹³¹I over the air-grass-cow-milk pathway. The reasons for this overestimate appear to be related to a combination of different factors, among which overestimation of the dry deposition velocity assumed for elemental ¹³¹I, overestimation of the interception and retention of wet-deposited ¹³¹I by pasture vegetation and overestimation of the cow's diet-to-milk transfer coefficient appear to be most important. The low transfer of Chernobyl ¹³¹I from air to milk indicates that the direct inhalation of contaminated air by humans may be more important in determining the ¹³¹I exposure to large populations than the consumption of contaminated cow's milk. Radiological assessments conducted prior to the Chernobyl accident have typically assumed that ¹³¹I exposure would be dominated by the consumption of milk. The consumption of milk, however, is still of dominant importance for the exposure of critical population subgroups composed of infants and small children.     

Modeling of Cs migration in soils using an 80-year soil archive: role of fertilizers and agricultural amendments

An 80-year soil archive, the 42-plot experimental design at the INRA in Versailles (France), is used here to study long-term contamination by ¹³⁷Cs atmospheric deposition and the fate of this radioisotope when associated with various agricultural practices: fallow land, KCl, NH₄(NO₃), superphosphate fertilizers, horse manure and lime amendments. The pertinence of a simple box model, where radiocaesium is supposed to move downward by convectional mechanisms, is checked using samples from control plots which had been neither amended, nor cultivated since 1928. This simple model presents the advantage of depending on only two parameters: α, a proportional factor allowing the historical atmospheric ¹³⁷Cs fluxes to be reconstructed locally, and k, an annual loss coefficient from the plow horizon. Another pseudo-unknown is however necessary to run the model: the shape of historical ¹³⁷Cs deposition, but this function can be easily computed by merging several curves previously established by other surveys. A loss of ∼1.5% per year from the plow horizon, combined with appropriate fluxes, provides good concordance between simulated and measured values. In the 0–25 cm horizon, the residence half time is found to be ∼18 yr (including both migration and radioactive decay). Migration rate constants are also calculated for some plots receiving continuous long-term agricultural treatments. Comparison with the control plots reveals significant influence of amendments on ¹³⁷Cs mobility in these soils developed from a unique genoform.     

Medical radioisotopes in the environment – following the pathway from patient to river sediment

Motivated by the detection of ¹³¹I in river sediment in routine long-term surveillance samples, a systematic short-term study of the wastewater treatment chain was planned and conducted. Inflow, effluent and primary sludge were collected on a daily basis during two weeks at a regional wastewater treatment plant. Samples were investigated by gamma spectroscopy. Four medically used isotopes could be identified (¹³¹I and ^99mTc regularly, ¹⁵³Sm and ¹²³I sporadically). The concentration levels coincide well with literature data for ¹³¹I, and with our own long-term data for ¹³¹I and ^99mTc for the same plant. Cosmogenic ⁷Be activity in primary sludge correlated well with rainfall intensity. Surface sediment was sampled at low tide at both shores of the river, up- and downstream of the plant. ¹³¹I was identified in all samples, with a sharp maximum (about 100 Bq kg⁻¹ d.m.) at the discharge point of the plant and lower levels elsewhere, decreasing monotonically in downstream direction. ⁷Be and ¹³⁷Cs showed the same behaviour, but no peak at the discharge point. Predictions from simple equilibrium models for the transport and sedimentation of ¹³¹I show good agreement with the experimental data and suggest that the wastewater treatment plant is the main source for this isotope.     

Dose assessment for marine biota and humans from discharge of (131)I to the marine environment and uptake by algae in Sydney, Australia

Iodine-131 reaches the marine environment through its excretion to the sewer by nuclear medicine patients followed by discharge through coastal and deepwater outfalls. ¹³¹I has been detected in macroalgae, which bio-accumulate iodine, growing near the coastal outfall of Cronulla sewage treatment plant (STP) since 1995. During this study, ¹³¹I levels in liquid effluent and sludge from three Sydney STPs as well as in macroalgae (Ulva sp. and Ecklonia radiata) growing near their shoreline outfalls were measured. Concentration factors of 176 for Ulva sp. and 526 for E. radiata were derived. Radiation dose rates to marine biota from ¹³¹I discharged to coastal waters calculated using the ERICA dose assessment tool were below the ERICA screening level of 10 μGy/hr. Radiation dose rates to humans from immersion in seawater or consumption of Ulva sp. containing ¹³¹I were three and two orders of magnitude below the IAEA screening level of 10 μSv/year, respectively.     

A review and test of predictive models for the bioaccumulation of radiostrontium in fish

Empirical relations between the ⁹⁰Sr concentration factor (CF) and the calcium concentration in freshwater aquatic systems have previously been determined in studies based on data obtained prior to the Chernobyl accident. The purpose of the present research is to review and compare these models, and to test them against a database of post-Chernobyl measurements from rivers and lakes in Ukraine, Russia, Belarus and Finland. It was found that two independently developed models, based on pre-Chernobyl empirical data, are in close agreement with each other, and with empirical data. Testing of both models against new data obtained after the Chernobyl accident confirms the models’ predictive ability. An investigation of the influence of fish size on ⁹⁰Sr accumulation showed no significant relationship, though the data set was somewhat limited.     

Evaluation of Monte Carlo-based calibrations of HPGe detectors for in situ gamma-ray spectrometry

The aim of this work was to evaluate the use of Monte Carlo-based calibrations for in situ gamma-ray spectrometry. We have performed in situ measurements at five different sites in Sweden using HPGe detectors to determine ground deposition activity levels of ¹³⁷Cs from the 1986 Chernobyl accident. Monte Carlo-calculated efficiency calibration factors were compared with corresponding values calculated using a more traditional semi-empirical method. In addition, results for the activity ground deposition were also compared with activity densities found in soil samples. In order to facilitate meaningful comparisons between the different types of results, the combined standard uncertainty of in situ measurements was assessed for both calibration methods. Good agreement, both between the two calibration methods, and between in situ measurements and soil samples, was found at all five sites. Uncertainties in in situ measurements for the given measurement conditions, about 20 years after the fallout occurred, were found to be in the range 15–20% (with a coverage factor k = 1, i.e. with a confidence interval of about 68%).     

Transfer of Chernobyl-derived 134Cs, 137Cs, 131I and 103Ru from flowers to honey and pollen

The activity concentrations of ¹³⁷Cs, ¹³⁴Cs, ¹³¹I and ¹⁰³Ru were determined separately in honey and pollen samples collected from a single bee colony during several months after the deposition of Chernobyl fallout. The source of each honey and pollen sample was determined by pollen analysis. Although the activity concentrations in honey and pollen varied with time, the concentrations of ¹³⁷Cs and ¹³⁴Cs were, in general, higher in pollen than in honey. For ¹⁰³Ru and ¹³¹I, these differences were comparatively small. The mean ¹³¹ I/¹³⁷Cs and ¹⁰³Ru/¹³⁷Cs ratios were about one order of magnitude higher in honey than in pollen. The mean ¹³¹I/¹⁰³Ru ratio was about the same for honey and pollen. This observation, in the light of the corresponding nuclide ratios found in the deposition, suggests that ¹³⁷Cs, ¹³⁴Cs, ¹³¹I and ¹⁰³Ru were taken up by the plant leaves and transported to nectar and pollen. The higher activity concentrations of ¹³⁷Cs and ¹³⁴Cs in pollen, relative to honey, indicate that these radionuclides behave analogously to potassium, which is also found in higher quantities in pollen.     

Evidence of the radioactive fallout in the center of Asia (Russia) following the Fukushima Nuclear Accident

It was recently reported that radioactive fallout due to the Fukushima Nuclear Accident was detected in environmental samples collected in the USA and Greece, which are very far away from Japan. In April-May 2011, fallout radionuclides (¹³⁴Cs, ¹³⁷Cs, ¹³¹I) released in the Fukushima Nuclear Accident were detected in environmental samples at the city of Krasnoyarsk (Russia), situated in the center of Asia. Similar maximum levels of ¹³¹I and ¹³⁷Cs/¹³⁴Cs and ¹³¹I/¹³⁷Cs ratios in water samples collected in Russia and Greece suggest the high-velocity movement of the radioactive contamination from the Fukushima Nuclear Accident and the global effects of this accident, similar to those caused by the Chernobyl accident.     

Cocaine and cannabinoids in the atmosphere of Northern Europe cities,comparison with Southern Europe and wastewater analysis

This study reports the first investigation of atmospheric illicit drug concentrations in Northern Europe using measurements of cocaine and cannabinoids in Amsterdam, London and Stockholm. Further, these measurements were compared to those made in Rome to explore the geographical and inter-city variability. Co-located measurements of atmospheric particulate mass and PAHs were used to help describe and interpret the illicit drug measurements with respect to atmospheric dispersion. Cocaine concentrations ranged from 0.03 to 0.14 ng/m³ in Amsterdam, from 0.02 to 0.33 ng/m³ in London and were below quantification limit (3 pg/m³) in Stockholm. Cannabinol was the only cannabinoid molecule detected in the three cities. During this campaign, London reported the highest concentrations of cocaine and meaningful differences were detected between the urban background and city centre London sites. Mean cocaine concentrations measured in Amsterdam during March 2011 were also compared with those measured simultaneously in eight Italian cities. The cocaine concentration in Amsterdam was comparable to that measured at an urban background in Milan and at a densely populated site in Florence. Although correlating atmospheric concentrations directly with drug prevalence is not possible using current data, links between concentrations of cocaine and estimates of abuse prevalence assessed by the more routinely used wastewater analysis were also examined. A statistically significant correlation was found between the two sets of data (R² = 0.66; p = 0.00131). Results confirmed that meteorology, population rate and habits of consumption influence the atmospheric concentrations of drugs. If these confounding factors were better controlled for, the techniques described here could became an easy and cost effective tool to index the impact of cocaine abuse in the area; especially where local hot spots need to be identified.     

Inventory and vertical migration of 90Sr fallout and 137Cs/90Sr ratio in Spanish mainland soils

In this paper the inventory of ⁹⁰Sr in 34 points distributed along the Spanish peninsular territory is presented. Obtained values range between 173 Bq/m² and 2047 Bq/m². From these data set and those ¹³⁷Cs data obtained in a previous work the ¹³⁷Cs/⁹⁰Sr activity ratio has been established, laying this value between 0.9 and 3.6. Also the migration depth of both radionuclides has been analysed obtaining for ¹³⁷Cs an average value 57% lower than that obtained for ⁹⁰Sr.Additionally, this paper presents the results obtained in 11 sampling points in which the activity vertical profile has been measured. These profiles have been analysed to state the behaviour of strontium in soils and after, by using a convective-diffusive model, the parameters of the model which governs the vertical migration of ⁹⁰Sr in the soil, v (apparent convection velocity) and D (apparent diffusion coefficient) have been evaluated. Mean values obtained are 0.20 cm/year and 3.67 cm²/year, respectively.     

Inverse modeling of Asian Rn flux using surface air Rn concentration

When used with an atmospheric transport model, the ²²²Rn flux distribution estimated in our previous study using soil transport theory caused underestimation of atmospheric ²²²Rn concentrations as compared with measurements in East Asia. In this study, we applied a Bayesian synthesis inverse method to produce revised estimates of the annual ²²²Rn flux density in Asia by using atmospheric ²²²Rn concentrations measured at seven sites in East Asia. The Bayesian synthesis inverse method requires a prior estimate of the flux distribution and its uncertainties. The atmospheric transport model MM5/HIRAT and our previous estimate of the ²²²Rn flux distribution as the prior value were used to generate new flux estimates for the eastern half of the Eurasian continent dividing into 10 regions.The ²²²Rn flux densities estimated using the Bayesian inversion technique were generally higher than the prior flux densities. The area-weighted average ²²²Rn flux density for Asia was estimated to be 33.0 mBq m⁻² s⁻¹, which is substantially higher than the prior value (16.7 mBq m⁻² s⁻¹). The estimated ²²²Rn flux densities decrease with increasing latitude as follows: Southeast Asia (36.7 mBq m⁻² s⁻¹); East Asia (28.6 mBq m⁻² s⁻¹) including China, Korean Peninsula and Japan; and Siberia (14.1 mBq m⁻² s⁻¹). Increase of the newly estimated fluxes in Southeast Asia, China, Japan, and the southern part of Eastern Siberia from the prior ones contributed most significantly to improved agreement of the model-calculated concentrations with the atmospheric measurements. The sensitivity analysis of prior flux errors and effects of locally exhaled ²²²Rn showed that the estimated fluxes in Northern and Central China, Korea, Japan, and the southern part of Eastern Siberia were robust, but that in Central Asia had a large uncertainty.     

Po-210 and Pb-210 as atmospheric tracers and global atmospheric Pb-210 fallout: a review

Over the past ∼5 decades, the distribution of ²²²Rn and its progenies (mainly ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Po) have provided a wealth of information as tracers to quantify several atmospheric processes that include: i) source tracking and transport time scales of air masses; ii) the stability and vertical movement of air masses iii) removal rate constants and residence times of aerosols; iv) chemical behavior of analog species; and v) washout ratios and deposition velocities of aerosols. Most of these applications require that the sources and sink terms of these nuclides are well characterized.Utility of ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Po as atmospheric tracers requires that data on the ²²²Rn emanation rates is well documented. Due to low concentrations of ²²⁶Ra in surface waters, the ²²²Rn emanation rates from the continent is about two orders of magnitude higher than that of the ocean. This has led to distinctly higher ²¹⁰Pb concentrations in continental air masses compared to oceanic air masses. The highly varying concentrations of ²¹⁰Pb in air as well the depositional fluxes have yielded insight on the sources and transit times of aerosols. In an ideal enclosed air mass (closed system with respect to these nuclides), the residence times of aerosols obtained from the activity ratios of ²¹⁰Pb/²²²Rn, ²¹⁰Bi/²¹⁰Pb, and ²¹⁰Po/²¹⁰Pb are expected to agree with each other, but a large number of studies have indicated discordance between the residence times obtained from these three pairs. Recent results from the distribution of these nuclides in size-fractionated aerosols appear to yield consistent residence time in smaller-size aerosols, possibly suggesting that larger size aerosols are derived from resuspended dust. The residence times calculated from the ²¹⁰Pb/²²²Rn, ²¹⁰Bi/²¹⁰Pb, and ²¹⁰Po/²¹⁰Pb activity ratios published from 1970’s are compared to those data obtained in size-fractionated aerosols in this decade and possible reasons for the discordance is discussed with some key recommendations for future studies.The existing global atmospheric inventory data of ²¹⁰Pb is re-evaluated and a ‘global curve’ for the depositional fluxes of ²¹⁰Pb is established. A current global budget for atmospheric ²¹⁰Po and ²¹⁰Pb is also established. The relative importance of dry fallout of ²¹⁰Po and ²¹⁰Pb at different latitudes is evaluated. The global values for the deposition velocities of aerosols using ²¹⁰Po and ²¹⁰Pb are synthesized.     

Evaluation and assessment of 25 years of environmental radioactivity monitoring data at Tarapur (India) nuclear site

The evaluation and assessment of monitoring data generated over a period of 1983-2007 (25 years) of a nuclear facility is presented. Time trends of particulate radioactivity, correlation between ¹³⁷Cs in discharge canal seawater and station discharged activity and correlation of ¹³⁷Cs, ⁶⁰Co, and ¹³¹I in marine species such as sponge and Nerita (gastropod) and corresponding discharged activity are discussed. The concentration of ¹³⁷Cs and ¹³¹I in seawater versus biota are discussed. A good correlation between ¹³⁷Cs in seawater and ¹³⁷Cs in liquid waste discharged was observed (R² = 0.8, p < 0.001). Similarly, correlation was good for Nerita and discharged concentration of ¹³⁷Cs, ¹³¹I and ⁶⁰Co (R² = 0.55-0.73 and p < 0.001). The measurements over the years indicated that there is no accumulation of radionuclides in either the terrestrial or aquatic environments. The mean ¹³⁷Cs decreased from the pre-operational levels: 7.0-3.6 Bq kg⁻¹ in soil, 0.91-0.016 Bq L⁻¹ in milk and 0.28-0.036 Bq kg⁻¹ in vegetation. Similarly, the mean ⁹⁰Sr in these matrixes decreased from 3.9 to 0.26 Bq kg⁻¹; 0.37-0.011 Bq L⁻¹ and 0.34-0.022 Bq kg⁻¹ respectively. Cesium-137 of about 700 μBq m⁻³ was measured in the air filter disks during 1986 and there was a decrease of three orders of magnitude in concentration over the 25 years. The evaluation of environmental data indicated that the radionuclide concentrations and potential impacts, in terms of effective dose to the members of public, have significantly reduced since 1969.