Determination of fresh nuclear fallout.
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The external dose attributable to fallout from worldwide atmospheric nuclear testing, which represents about 40% of the total effective dose received before 2000, is dominated by specific fission products such as 95Zr, 104Ba, 106Ru, 103Ru, and 144Ce, which are far less well-documented than 90Sr and 137Cs. The depositions of these nuclides over France were calculated on the basis of activity measurements in air and rainwater samples collected from 1961 to 1977. These depositions were then compared to the same radionuclides activities measured in grass during that period. This study shows that the transfer and deposition processes occur in a very similar manner for all the studied radionuclides. Depositions calculated in this study, consistent in most cases with UNSCEAR estimates, constitute a good basis for the external dose assessment of nuclear weapon test fallout over Western Europe.
A sharp increase in the ratio of strontium-89 to strontium-90 in rain was observed at Fayetteville, Arkansas, after the French nuclear detonations of February and April 1960. Experimental data obtained suggest the possibility that part of the debris from atom bombs detonated in the tropical region may enter the stratosphere.
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We examined the concentration, size distribution, redox state and isotopic composition of plutonium (Pu) in groundwater at the 100K-Area at the U.S. Department of Energy's (DOE) Hanford Site. Total concentrations of Pu isotopes were extremely low (10(-4) to 10(-6) pCi/kg, approximately 10(4) to 10(6) atoms/kg) but measurable for the first time in the 100K-Area wells using mass spectrometric analyses that are much more sensitive than alpha spectroscopy methods used previously. Size fractionation data from two wells suggest that 7-29% of the Pu is associated with colloids, operationally defined here as particles between 1 kDa-0.2 microm in size. These colloids were collected using a 1 kDa cross-flow ultrafiltration (CFF) system developed specifically for groundwater actinide studies to include careful controls both in the field and during processing to ensure in situ geochemical conditions are maintained and size separations can be well characterized. Pu in this colloidal fraction was exclusively in the more reduced Pu(III/IV) form, consistent with the higher affinity of Pu in the lower oxidation states for particle surfaces. While the overall concentrations of Pu were low, the Pu isotopic composition suggests at least two local sources of groundwater Pu, namely, local Hanford reactor operations at the 100K-Area and spent nuclear fuel from the N-reactor, which was stored in concrete pools at this site. Differences between this site and the Savannah River Site (SRS) are noted, since groundwater Pu at the F-Area seepage basin at SRS has been found using these same methods, to be characterized by lower colloidal abundances and higher oxidation states. This difference is not directly attributable to groundwater redox potential or geochemical conditions, but rather the physical-chemical difference in Pu sources, which at SRS appear to be dominated downstream from the seepage basins by decay of 244Cm, resulting in more oxidized forms of 240Pu. There is no clear evidence for colloid facilitated transport of Pu in groundwater at the Hanford Site, since downstream wells have both an order of magnitude lower concentrations of Pu and a lower fractional colloidal distribution.
A method by inductively coupled plasma mass spectrometry (ICP-MS) was developed which allows the measurement of (236)U at concentration ranges down to 3 x 10(-14)g g(-1) and extremely low (236)U/(238)U isotope ratios in soil samples of 10(-7). By using the high-efficiency solution introduction system APEX in connection with a sector-field ICP-MS a sensitivity of more than 5,000 counts fg(-1) uranium was achieved. The use of an aerosol desolvating unit reduced the formation rate of uranium hydride ions UH(+)/U(+) down to a level of 10(-6). An abundance sensitivity of 3 x 10(-7) was observed for (236)U/(238)U isotope ratio measurements at mass resolution 4000. The detection limit for (236)U and the lowest detectable (236)U/(238)U isotope ratio were improved by more than two orders of magnitude compared with corresponding values by alpha spectrometry. Determination of uranium in soil samples collected in the vicinity of Chernobyl nuclear power plant (NPP) resulted in that the (236)U/(238)U isotope ratio is a much more sensitive and accurate marker for environmental contamination by spent uranium in comparison to the (235)U/(238)U isotope ratio. The ICP-MS technique allowed for the first time detection of irradiated uranium in soil samples even at distances more than 200 km to the north of Chernobyl NPP (Mogilev region). The concentration of (236)U in the upper 0-10 cm soil layers varied from 2 x 10(-9)g g(-1) within radioactive spots close to the Chernobyl NPP to 3 x 10(-13)g g(-1) on a sampling site located by >200 km from Chernobyl.
Here I describe a collective model to predict the long term behaviour of 90Sr in river catchments. The model is applied to 11 Italian rivers contaminated by 90Sr due to nuclear explosions in the atmosphere over past decades. The uncertainty at the 68% confidence level of the model, when used as a generic tool for evaluating the concentration of the radionuclide in water, is a factor 1.8 around the predicted values. The reliability of the model output is due to the mutual compensation effects of different phenomena occurring in the catchments that lead to 'collective' behaviours which are scantily variable and uncertain despite the large range of catchment characteristics. The model is based on the assumption that the time behaviour of the 90Sr (Bq s-1) transported by water, following a single pulse of radionuclide deposition, is the sum of some exponential components. In the present paper the components were supposed characterised by the following decay constants: lambda 1 = 2.3 x 10(-7) s-1, lambda 2 = 4.2 x 10(-9) S-1 and lambda 3 = 4.2 x 10(-10) S-1. The average value of 90Sr transfer coefficient from the catchment to the river, that, in the case of a pulse deposition, is approximately equal to the ratio between the radionuclide concentration in water and the deposition, is estimated to be 0.2 m-1.
Underwater gamma-ray spectrometry is an effective alternative or complement to traditional sampling and laboratory analyses for applications such as contamination assessment in emergency situations, long-term monitoring of radioactive releases or investigation of sunken radioactive objects. This technique was recently used in a seabed contamination study undertaken at the South Pacific nuclear weapons test sites of the Mururoa and Fangataufa atolls in order to guide and focus sediment core sampling in the areas with highest gamma-emitting radionuclide levels. 60Co inventories estimated on the basis of the underwater gamma-ray spectrometry survey were in good agreement with results previously obtained by traditional sediment sampling and laboratory analysis.
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Iodine-131 in milk and in rain water in Nagoya, Japan, (a location 8,000 km from Chernobyl) was monitored between May and July 1986. The 131I concentration in rain water ranged from 43.1 Bq L-1 on 4 May to 15 mBq L-1 on 12 July, and that in milk ranged from 21.8 Bq L-1 on 19 May to 11 mBq L-1 on 14 July. Iodine-131 concentrations in milk were estimated to be 4 to 6 times greater than those in rain water during the first few weeks after the accident. Both concentrations decreased with approximately the same effective half-life of 5.9 +/- 0.3 d for rain water and 5.0 +/- 0.2 d for milk. The 131I concentration in milk sold in markets varied from dairy to dairy and ranged from 0.07 to 0.2 times that in fresh milk. The maximum thyroidal dose equivalents estimated for an adult man and for a baby were far lower than the population annual dose equivalent to the thyroid from natural radiation.
Brown coal unusually rich in uranium is burnt in a coal-fired power plant that lies inside the confines of a small industrial town named Ajka, Hungary, and has been operational since 1943. The 238U (226Ra) activity discharged to the atmosphere per unit electrical energy produced was about 330-400 GBq (GW y)(-1), which is 66-80 times more than that was estimated by UNSCEAR (1988) as a characteristic value for old type coal-fired power plants [5 GBq (GW y)(-1)]. The objective of this study was the experimentally established assessment of the artificial increment in the dose from external exposure to gamma rays of terrestrial radionuclides outdoors. Soil samples were collected in and near Ajka from 81 locations. The samples were investigated by Ge(Li) gamma spectrometry. Considerably elevated concentrations of uranium and its progeny have been measured in most of the samples that were collected near to the plant. Concentrations of 238U and 226Ra in the top (0-5 cm depth) layer of undisturbed soil at public areas inside town were 4.7 times higher, on average, than those in the uncontaminated deeper layers. Dose rate in air (air kerma) from external exposure to terrestrial gamma rays outdoors at a height of 1 m and effective doses were estimated from the measured activity concentrations using some relevant literature data. The estimated artificial increment in the dose rate in air was, on average, 32.8, 10.3, and 102.1 nGy h(-1) at public areas, vegetable gardens, and backyards, respectively. The mean artificial increment in the annual per caput effective dose from external exposure to terrestrial radionuclides outdoors is 21.8 microSv y(-1). The collective dose commitment per unit energy generated from outdoor exposure to the deposited uranium progeny is about 8.0-9.1 person Sv (GW y)(-1), which is 67-76 times more than that evaluated by UNSCEAR (1988) for a typical "old" coal-fired power plant [0.12 person Sv (GW y)(-1)]. Ajka is a suitable place for studying the dosimetric consequences of the utilization of coal for energy production experimentally.
The present situation of radioactive contamination at the village of Dolon and nearby villages such as Mostik, Cheremushka and Budene was investigated to serve as an aid to resolve dose discrepancy between model calculations and TL measurements made for external gamma-ray dose in air in Dolon. The paper was focused on the reevaluation of the accumulated levels and distribution of long-lived radionuclides 137Cs and Pu isotopes in soil using long core samples up to a depth of 30 and 100 cm. The inventories of 137Cs and 239,240Pu found were in the wide range of 140-10,310 and 140-14,320 Bq/m2, respectively. Most of the Pu in soil was tightly incorporated into various sizes of fused particles. Both 137Cs and 239,240Pu in soil were accumulated in the smaller soil size fraction of <125 microm, and the presence of hot particles, probably due to Pu, was clearly observed by star-like patterns from alpha-tracks. The obtained data will be helpful for evaluating the current and future radiation risks to the people living around there.
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