Long-term dynamics of radioactive <Superscript>90</Superscript>Sr and <Superscript>137</Superscript>Cs contamination of small mammals in the Chernobyl zone

Between 1986 and 1994, a decrease in nonalimentary ⁹⁰Sr and ¹³⁷Cs intake and changes in the accessibility of radionuclides in the soil-plant link of their cycle resulted in a 10-to 100-fold decrease in their specific activity (SA) in the bodies of small mammals inhabiting the Chernobyl zone, and a similar decrease was observed in the radionuclide transition factor (TF) in the soil-animal chain. Between 1995 and 2005, no consistent increase or decrease in SA or TF could be revealed against the background of a combined effect of different physicochemical and ecological factors. It is suggested that subsequent changes in the level of radioactive contamination of small mammals will generally reflect only the dynamics of physical ⁹⁰Sr and ¹³⁷Cs decay, but, nevertheless, seasonal and local variations in this level will be significant.     

Problems in predicting <Superscript>137</Superscript>Cs levels in lake waters of eastern Fennoscandia

With regard to data on two-year exposure of Chernobyl-derived ¹³⁷Cs in lakes with average depths ranging from 2 to 15 m, contamination of lake waters has been estimated using a sorption-diffusion model with ¹³⁷Cs distribution and diffusion coefficients of 4000 l/kg and 1.0 × 10⁻⁷ cm², respectively.     

Spatial Distribution of Heavy Metals and <Superscript>137</Superscript>Cs in Spruce Forest Soil under Conditions of Regional Pollution

The influence of horizontal structure of spruce forest on the spatial distribution of acid-soluble Zn, Cd, Pb compounds and ¹³⁷Cs in the litter and the humus horizon of soddy podzolic soil has been studied in the territory with the regional background level of industrial fallout. It has been found that the distribution pattern of Zn in the forest litter is a result of biogeochemical processes. The litter in fern–wood sorrel microplots contains increased amounts of Zn and Cd, while the contents of Pb and ¹³⁷Cs are decreased. The distribution patterns of Pb and ¹³⁷Cs in the litter are positively correlated with each other, since both elements are deposited from the atmosphere, and similar mechanisms account for their redistribution in the spruce forest ecosystem.     

Plutonium isotopes in surface air of Prague in 1986–2006

Monitoring of ^239,240Pu in surface air of Prague started in 1986 in connection with the Chernobyl accident. Measurable activities of 10–28 μBq m⁻³ were found from 29 April 1986 to 5 May 1986. In the most of the monitoring periods of 1987–1996, activities of ^239,240Pu in air were not measurable. Positive values for ^239,240Pu and ²³⁸Pu in air could be obtained after installation of an aerosol sampler with higher flow-rate in 1997. Activity concentrations of ^239,240Pu and ²³⁸Pu in Prague air in the most of quarters of 1997–2006 were in the range 0.53–5.06 and <0.16–1.10 nBq m⁻³, respectively. Seasonal fluctuations can be found in content of ^239,240Pu in air. Activity ratios of ²³⁸Pu/^239,240Pu in air are higher than those in top soil, so it can be supposed that ²³⁸Pu is coming to air of Prague also from other sources than resuspension of fallout from atmospheric nuclear tests.     

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.     

Concentrations of U,U, U,Th, Th,Th, Ra,Ra, Ra,Po, Pb and Pb in drinking water in Italy: reconciling safety standards based on measurements of gross α and β

Some important naturally occurring α- and β-radionuclides in drinking water samples collected in Italy were determined and the radiological quality evaluated. The mean activity concentrations (mBq L⁻¹) of the radionuclides in the water samples were almost in the order: 26 ± 36 (²³⁴U) > 21 ± 30 (²³⁸U) > 8.9 ± 15 (²²⁶Ra) > 4.8 ± 6.3 (²²⁸Ra) > 4.0 ± 4.1 (²¹⁰Pb) > 3.2 ± 3.7 (²¹⁰Po) > 2.7 ± 1.2 (²¹²Pb) > 1.4 ± 1.8 (²²⁴Ra) > 1.1 ± 1.3 (²³⁵U) > 0.26 ± 0.39 (²²⁸Th) > 0.0023 ± 0.0009 (²³⁰Th) > 0.0013 ± 0.0006 (²³²Th). The mean estimated dose (μSv yr⁻¹) to an adult from the water intake was in this order: 2.8 ± 3.3 (²¹⁰Po) > 2.4 ± 3.2 (²²⁸Ra) > 2.1 ± 2.1 (²¹⁰Pb) > 1.8 ± 3.1 (²²⁶Ra) > 0.94 ± 1.30 (²³⁴U) > 0.70 ± 0.98 (²³⁸U) > 0.069 ± 0.087 (²²⁴Ra) > 0.036 ± 0.044 (²³⁵U) > 0.014 ± 0.021 (²²⁸Th) > 0.012 ± 0.005 (²¹²Pb) > 0.00035 ± 0.00029 (²³⁰Th) > 0.00022 ± 0.00009 (²³²Th). It is obvious that ²¹⁰Po, ²²⁸Ra, ²¹⁰Pb and ²²⁶Ra are the most important dose contributors in the drinking water intake. As far as the seventeen brands of analysed drinking water were concerned, the committed effective doses were in the range of 2.81–38.5 μSv yr⁻¹, all well below the reference level of the committed effective dose (100 μSv yr⁻¹) recommended by the WHO. These data throw some light on the scale of the radiological impact on the public from some naturally occurring radionuclides in drinking water, and can also serve as a comparison for the dose contribution from artificial radionuclides released to the environment as a result of human practices. Based on the radionuclide composition in the analysed waters, comment was made on the new screening level for gross α activity in guidelines for drinking-water quality recommended by the WHO, 2004.     

Depth profile of ²³⁶U/²³⁸U in soil samples in La Palma, Canary Islands

The vertical distribution of the ²³⁶U/²³⁸U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the ²⁴⁰Pu/²³⁹Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA^® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios ²³⁶U/²³⁸U, ²⁴⁰Pu/²³⁹Pu and ²³⁶U/²³⁹Pu, respectively. The ²³⁶U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio ²⁴⁰Pu/²³⁹Pu indicated a global fallout signature we assume the same origin as the probable source for ²³⁶U. Our measured ²³⁶U/²³⁹Pu value of around 0.2 is within the expected range for this contamination source.     

Determination of U, Pu and Am isotopes in Irish Sea sediment by a combination of AMS and radiometric methods

Samples from a marine sediment core from the Irish Sea (54.416 N, 3.563 W) were analyzed for the isotopic composition of uranium, plutonium and americium by a combination of radiometric methods and AMS. The radiochemical procedure consisted of a Pu separation step by anion exchange, subsequent U separation by extraction chromatography using UTEVA^® and finally Am separation with TRU^® Resin.Additionally to radiometric determination of these isotopes by alpha spectrometry, the separated samples were also used for the determination of ²³⁶U/²³⁸U and plutonium isotope ratios by Accelerator Mass Spectrometry (AMS) at the VERA facility.     

Artificial radionuclides in the atmosphere over Lithuania

Measurements of airborne radioactive aerosol concentration were carried out on the basis of 1-3 days samples after the Chernobyl disaster and during the period of 1992-2003. Transport of "hot" particles of different composition resulted in the high activity concentrations of (137)Cs, (238)Pu, (239,240)Pu and (241)Am in the atmosphere in Vilnius at the end of April 1986. The (240)Pu/(239)Pu atom ratio showed clear evidence of non-global plutonium originating from the Chernobyl accident in the atmosphere over Lithuania. The (240)Pu/(239)Pu atom ratio ranged from 0.14 to 0.40 in monthly samples in Vilnius in 1995-2003. An increase in activity concentration of (137)Cs by a factor of 100 (up to 300 microBq/m(3)) was found following forest fires in the Ukraine and Belarus. However, no transport of the Chernobyl plutonium was observed and the (240)Pu/(239)Pu atom ratio in samples collected during the forest fires was found to be 0.229 and 0.185, respectively. The exponential decrease in the (240)Pu/(239)Pu atom ratio from 0.30 to 0.19 (mean values) was observed in 1995-2003.     

External gamma-ray dose rate and radon concentration in indoor environments covered with Brazilian granites

Health hazard from natural radioactivity in Brazilian granites, covering the walls and floor in a typical dwelling room, was assessed by indirect methods to predict external gamma-ray dose rates and radon concentrations. The gamma-ray dose rate was estimated by a Monte Carlo simulation method and validated by in-situ measurements with a NaI spectrometer. Activity concentrations of ²³²Th, ²²⁶Ra, and ⁴⁰K in an extensive selection of Brazilian commercial granite samples measured by using gamma-ray spectrometry were found to be 4.5-450 Bq kg⁻¹, 4.9-160 Bq kg⁻¹ and 190-2029 Bq kg⁻¹, respectively. The maximum external gamma-ray dose rate from floor and walls covered with the Brazilian granites in the typical dwelling room (5.0 m × 4.0 m area, 2.8 m height) was found to be 120 nGy h⁻¹, which is comparable with the average worldwide exposure to external terrestrial radiation of 80 nGy h⁻¹ due to natural sources, proposed by United Nations Scientific Committee on the Effects of Atomic Radiation. Radon concentrations in the room were also estimated by a simple mass balance equation and exhalation rates calculated from the measured values of ²²⁶Ra concentrations and the material properties. The results showed that the radon concentration in the room ventilated adequately (0.5 h⁻¹) will be lower than 100 Bq m⁻³, value recommended as a reference level by the World Health Organization.     

Comparative trends and seasonal variation of ⁷Be, ²¹⁰Pb and ¹³⁷Cs at two altitude sites in the central part of France

The atmospheric concentrations of ¹³⁷Cs, ²¹⁰Pb, and ⁷Be were measured over a three-year period at two research stations located less than 12 km apart and at different altitudes (puy de Dôme, 1465 m a.s.l. and Opme, 660 m a.s.l., France). Seasonal trends in all radionuclides were observed at both stations, with high concentration measured during the summer and low concentrations during the winter. The ²¹⁰Pb concentrations at both stations were similar to each other. Higher concentrations of both ⁷Be and ¹³⁷Cs were measured at puy de Dôme than at Opme. These observations can be explained by the stratospheric and upper tropospheric sources of ⁷Be and the long-range transportation of ¹³⁷Cs at high altitudes. Air mass origins during sampling periods were classified into several groups by their route to the stations (marine, marine modified, continental and mediterranean). We observed that ⁷Be concentrations were constant regardless of the air mass origins, unlike ¹³⁷Cs and ²¹⁰Pb concentrations that increased when influenced by continental air masses. Higher ⁷Be concentrations were observed when air masses were arriving from the upper troposphere than from the boundary layer, the opposite was observed for ¹³⁷Cs. The temporal trend in concentrations of ⁷Be shows good agreement with previous modelling studies suggesting that there is a good understanding of its sources and the atmospheric vertical mixing of this radionuclide. The sources and mixing of ²¹⁰Pb, however, seem to be more complex than it appeared to be in previous modelling studies.     

Cs, Pu concentrations and the Pu/Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary

A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of ¹³⁷Cs and plutonium (Pu) isotopes. The ¹³⁷Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the ¹³⁷Cs and ^239+240Pu. The shape of the vertical ¹³⁷Cs distribution in the sediment core was similar to that of the Pu. The maximum ¹³⁷Cs and ^239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average ²⁴⁰Pu/²³⁹Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the ²⁴⁰Pu/²³⁹Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The ¹³⁷Cs and ^239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m² and 407 ± 27 Bq/m², respectively. Approximately 40% of the ^239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure ²⁴⁰Pu/²³⁹Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.     

Fukushima fallout in Northwest German environmental media

Traces of short- and long-lived fallout isotopes (¹³¹I, ¹³⁴Cs and ¹³⁷Cs) were found in environmental samples collected in Northwest Germany (rain water, river sediment, soil, grass and cow milk) from March to May 2011, following the radioactivity releases after the nuclear accident in Fukushima, Japan. The measured concentrations are consistent with reported concentrations in air, amount of rainfall and expected values applying simple radioecological models. The [¹³⁴Cs]/[¹³⁷Cs] ratio reported for air (about 1) allows for discrimination between “recent” and “old” ¹³⁷Cs. Expected ¹³⁶Cs values fell below the detection limits of the instrumentation, despite large sample masses and long counting times.     

Thermal neutron fluence from ultra low-level γ-ray spectrometry of spoons activated during the JCO criticality accident at Tokai-mura in 1999

During the JCO-accident in Tokai-mura in 1999, the surrounding village was irradiated by an uncontrolled neutron flux. At some locations in that village, the thermal neutron flux was determined retrospectively by measurement of the very low activity of ⁵¹Cr and ⁶⁰Co in stainless-steel spoons using γ-ray spectrometry in underground laboratories. Activities determined in the HADES underground facility are presented here, together with calibrations performed using a well-defined thermal neutron flux to directly estimate the fluence of thermal neutrons independent of most assumptions. The results show measurable ⁵¹Cr in three samples and ⁶⁰Co in four samples taken from locations at distances of up to 430 m from the accident location despite the elapse of 4 half-lives of ⁵¹Cr before measurement. Effects of air transport of the samples were considered and shown to be negligible.     

Temporal variation of Be concentrations in atmosphere for 8 y from 2000 at Yamagata,Japan: solar influence on the Be time series

We have been continuously observing the daily ⁷Be concentrations in surface air at Yamagata, Japan (38.25° N, 140.35° E) since 2000. The yearly profile of the ⁷Be concentration indicates the variation in galactic cosmic rays owing to solar modulation. Over 8 y, the ⁷Be concentration, cosmic neutrons, and number of sunspots varied by 37.4%, 12.2%, and 92.8%, respectively. The influence of precipitation on the ⁷Be variability was approximately 5%. Hence, the yearly ⁷Be concentration was mainly varied by the solar modulation of the ⁷Be production rates. Based on the production rates found in an EXPACS simulation, the observed variability indicates ⁷Be transport from high latitudes. The daily ⁷Be concentrations have two significant periodic components of 19 d and 36 d. The 36-d component implies a relationship between the sun's rotation and the vertical transport of air masses under quiet solar activity.     

Lead-210 and Beryllium-7 fallout rates on the southeastern coast of Brazil

Total ²¹⁰Pb and ⁷Be fallout rates were measured on the coastal region of Niteroi, Brazil. The monthly depositional flux of ²¹⁰Pb and ⁷Be varied by a factor of 26, from 1.7 to 43.3 mBq cm⁻² year⁻¹ and ∼27, from 7.5 to 203.5 mBq cm⁻² year⁻¹, respectively. The relatively large oscillations in the depositional flux of ²¹⁰Pb at this study site were likely due to variations in air mass sources, while the ⁷Be fluctuations may be driven by a combination of weather conditions. Local geology could support the periodic high fluxes of ²¹⁰Pb from continental air masses, as shifting oceanic wind sources were affirmed by the uncorrelated ²¹⁰Pb and ⁷Be fallout activities and ⁷Be/²¹⁰Pb ratios. The ²¹⁰Pb atmospheric deposition was found to be in agreement with local sediment inventories, an important consideration in geochemical studies that estimate sedimentation processes.     

Laboratory studies of the diffusive transport of Cs and Co through potential waste repository soils

Tests using reconstituted samples have been performed to assess the diffusive transport of ¹³⁷Cs and ⁶⁰Co through natural regolith materials from a region in South Australia being considered for a radioactive waste repository. A double diffusion cell apparatus made of polycarbonate resin was developed to estimate the effective diffusion (D_e) and sorption coefficients (K_d) that allowed large withdrawals from the source and collector cells and has enabled tests with low concentrations of radioactivity. An alternative to porous stainless steel filter plates has also been used to reduce uncertainty in test interpretation. Analysis of the transient data used a staged method of the Laplace transform to take into consideration the volume of the samples withdrawn from the apparatus during testing. At test completion samples were cut into slices and analysed for radionuclide concentration. Data obtained from the sliced samples confirmed that both numerical and experimental data produced acceptable mass balance. The D_e values obtained in this study were of the order of 10⁻⁶ cm² s⁻¹ for both species, higher than previously published data. The K_d values from the diffusion and batch sorption tests were in reasonable agreement for ¹³⁷Cs, but an order of magnitude different for ⁶⁰Co. The sorption of the latter radionuclide was strongly pH dependent, and this dependency during diffusion tests would benefit from further investigation.     

Aspects on the analysis of 210Po

There has been little development regarding analysis of polonium (Po) in environmental samples since the 1960ies. This is due to the straightforward spontaneous deposition of this element on silver (Ag), nickel (Ni) or copper (Cu) without any radiochemical separation. For many years, no radiochemical yield determinant was used and it was generally supposed that the yield was 100% after two depositions. Counting was often done using ZnS scintillation counter coupled to a photomultiplier tube. However, the use of the yield determinants ²⁰⁸Po and ²⁰⁹Po and the development of alpha spectrometry showed that the yield was lower. Furthermore, the tendency of Po to volatilize at low temperatures constrains the sample preparation techniques; dry-ashing cannot be used. But during the wet-ashing procedure, there are still some losses.The aim of this study was to evaluate the Po losses during wet-ashing by the use of a double-tracer technique. We have found that the losses were about 30% when open glass beakers were used and about 17% when the samples were digested in microwave oven. When long-necked bottles (Kjeldahl flasks) were used, a loss of about 20% was registered.It has also been observed that ²¹⁰Pb to some extent is plating out together with its daughter nuclide Po during the electrochemical deposition. This will result in a systematic error since an unknown amount of supported ²¹⁰Po will be produced from the ²¹⁰Pb decay depending on the fraction of ²¹⁰Pb being deposited on the disc and the waiting time between deposition and measurement of the sample. A further consequence of this is that in the assessment of the ²¹⁰Pb content in the sample, very often the remaining liquid is stored after deposition for build-up of ²¹⁰Po. Since some ²¹⁰Pb is lost on the disc, the result for ²¹⁰Pb will be too low. Both these systematic errors give rise to a too high ²¹⁰Po/²¹⁰Pb ratio. The fraction of ²¹⁰Pb which is plating out has been assessed in this study for different matrices and is about 50-90%. During the measurement by solid state Si-detectors, some Po is evaporated in the vacuum conditions contaminating the detectors. Experiments have here been done by heating the discs after deposition which indicate that less Po is evaporated from Ag than from Ni. The losses from Ag are less than that from the other metals probably due to a deeper penetration into the surface of Po. We conclude that in most aspects, Ag is better to use than the other plating metals.