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%).     

Effect of pH on the sorption of uranium in soils

This work was undertaken to study the influence of soil type and chemical composition on uranium sorption ratios (SR in 1 kg-1) in order to reduce the uncertainty associated with this parameter in risk assessment models. Thirteen soil samples were collected from three different locations in France under different geological conditions. Clay content varied from 7.0 to 50.0%, pH ranged from 5.5 to 8.8 and organic matter content from 1.0 to 4.6%. Soils were incubated at room temperature in polyethylene packets for 28 days in the presence of 1 mg U kg-1 soil. Sorption ratio values varied from 0.9 to 3198 for all soils with no significant effect of soil texture or of organic matter. However, soil pH was highly linearly correlated with (log SR) as a probable consequence of the existence of different uranium complexes as a function of soil pH. The sorption behaviour differences between UO2(2+) and UO2(2+)-carbonate complexes are so great that any other effect of soil properties on U sorption is hidden. Thus, soil pH should be the focus variable for reduction of the uncertainty associated with the soil Kd value used in environmental risk assessments, even for reducing the uncertainty in site-specific Kd values.     

Calibration of a portable HPGe detector using MCNP code for the determination of 137Cs in soils

In situ gamma spectrometry provides a fast method to determine (137)Cs inventories in soils. To improve the accuracy of the estimates, one can use not only the information on the photopeak count rates but also on the peak to forward-scatter ratios. Before applying this procedure to field measurements, a calibration including several experimental simulations must be carried out in the laboratory. In this paper it is shown that Monte Carlo methods are a valuable tool to minimize the number of experimental measurements needed for the calibration.     

An airborne gamma-ray spectrometry survey of nuclear sites in Belgium

As part of a wider study to define the existing background levels in Belgium an airborne gamma-ray survey was conducted in two areas associated with nuclear sites. In the Mol area, the survey zone included areas surrounding the SCK-CEN nuclear research centre, and its associated neighbourhood which includes radioactive waste stores, fuel manufacture and fabrication facilities and an international accelerator laboratory. In the vicinity of Fleurus, the survey included the IRE complex with radiochemical laboratories, irradiation facilities and stores, and isotope production accelerators. The survey was conducted using a twin engined helicopter equipped with a combined scintillation and semiconductor spectrometer. The system was installed and tested in the UK, and then transferred to Belgium for operations. The complete survey was conducted successfully within 1 week. The results provide a comprehensive record of the radiation environment of the nuclear sites at time of survey, and show a range of signals associated with the types of activity present in each area. They confirm that radiation fields are largely confined to the operational sites, and provide a traceable record against which future changes could be assessed. The demonstration of efficient deployment between two European countries, coupled with rapid mapping of many different radiometric signals around these sites confirms the utility of the airborne gamma spectrometry approach for accurate definition of enhanced radiation fields. This has important implications for emergency response.     

Some observations on the geochemistry and isotopic composition of uranium in relation to the reprocessing of nuclear fuels

In order to determine whether or not uranium depleted in ²³⁵U and derived from the British Nuclear Fuels Ltd (BNFL) nuclear fuel reprocessingg plant at Sellafield, Cumbria, UK can be detected in environmental samples, we have investigated the isotopic composition of uranium in ammonium carbonate leachates from marine and terrestial samples from near Sellafield. Some show a depletion in ²³⁵U and the presence of ²³⁶U which unequivocally identifies the presence of uranium derived from BNFL. The ²³⁴U/²³⁸U activity ratio and total uranium content of samples are not significantly different from those of natural uranium abundances. The highest concentrations of uranium are found in anaerobic organic-rich silts and the lowest in sandy silts and coarse-grained sands.     

Assessment of natural and anthropogenic radioactivity levels in rocks and soils in the environs of Swieradow Zdroj in Sudetes, Poland, by in situ gamma-ray spectrometry

The natural radioactivity of 40K, 208Ti, 212Pb, 214Pb, 228Ac, and the fallout of 137Cs in typical rocks and soils of Swieradów Zdrój area (Sudetes Mountains, Poland) were measured in situ using a portable gamma-ray spectrometry workstation. The measurement points were chosen for different regional lithology: within hornfelses of the Szklarska Poreba schist-belt, quartz rocks, gneisses of the Swieradów Zdrój unit, leucogranites, leptinites, mica schists of the Stara Kamienica belt, and finally the zones of the southern and northern contacts of the Stara Kamienica schist-belt with leucogranites and gneisses of the Lesna unit, respectively. 40K activity varied in the range from about 320 Bq kg(-1) (quartz) to 1200 Bq kg(-1) (gneisses). The activity concentrations associated with 228Ac (232Th series) varied in the range from 25 Bq kg(-1) (quartz) to 62 Bq kg(-1) (leucogranites), whereas activity concentration of 226Ra varied in the range from about 31 Bq kg(-1) (hornfelses) to 122 Bq kg(-1) (leucogranites). Relatively low deposits of 137Cs were noted in the investigated area, where the activity concentrations ranged from 4001 (hornfelses) Bq m(-2) to less than 154 Bq m(-2) (leucogranites).     

Sorption-desorption tests to assess the risk derived from metal contamination in mineral and organic soils

We obtained the sorption isotherms of Cd, Cu, Pb and Zn from seven soils with contrasting properties, including mineral and organic soils. The distribution coefficients (Kd) were determined from batch tests in a solution that simulated the soil solution cationic composition. The Kd values of the target metals varied greatly depending on soil type and initial metal concentration. Sorption isotherms were fitted to Freundlich and Langmuir models, and derived parameters were correlated to soil properties through the construction of a correlation matrix and application of Principal Component Analysis. The batch Kd showed a satisfactory agreement with the Kd obtained from field-contaminated soils. The sorption tests were complemented with the estimation of the reversibility of metal sorption by the application of an extraction test. The extraction yields, which did not relate to the initial metal concentration, depended on the metal-soil combination, and showed no correlation to batch Kd values. The risk derived from a contamination event was estimated through the quantification of a Retention Factor, defined as the ratio of the Kd versus the extraction yield. Results showed that this was an excellent index to highlight which metal and soil represent the most vulnerable scenarios after a contamination event.     

Classification of soil samples according to their geographic origin using gamma-ray spectrometry and principal component analysis

A principal component analysis (PCA) was used for classification of soil samples from different locations in Serbia and Montenegro. Based on activities of radionuclides ((226)Ra, (238)U, (235)U, (40)K, (134)Cs, (137)Cs, (232)Th and (7)Be) detected by gamma-ray spectrometry, the classification of soils according to their geographical origin was performed. Application of PCA to our experimental data resulted in satisfactory classification rate (86.0% correctly classified samples). The obtained results indicate that gamma-ray spectrometry in conjunction with PCA is a viable tool for soil classification.     

Fractionation of natural radionuclides in soils from a uranium mineralized area in the south-west of Spain

A new version of a classical method was applied to study the distribution of natural radionuclides (238U, 230Th, and 226Ra) in the soil fractions obtained by a sequential extraction procedure. The potential significance of the fractions obtained with this method was tested on two very similar soils but with very different contents of the three radionuclides, collected in the proximity of a disused uranium mine located in the Extremadura region in the south-west of Spain. The results confirmed that, if only non-residual fractions are considered, the sequential method applied shows a characteristic speciation pattern of these natural radionuclides in this soil matrix, i.e., the distribution of each of the three radionuclides was very similar for the two soil samples.     

In situ gamma-ray spectrometry in forests: determination of kerma rate in air from 137Cs

Continental margins are important areas to be considered when studying the distributions and depositions of pollutants, both conventional and radioactive. Coastal sediments accumulate most of those contaminants which can be introduced following atmospheric and/or fluvial pathways. Moreover, their residence times within the water column are usually shortened due to their affinity to associate with the downward falling particulate matter, more abundant at shallower depths. In this paper the distribution profiles and inventories of plutonium, americium and cesium are detailed, providing useful information about recent sedimentation phenomena such as sediment mixing, slumping processes and bioturbation. Unsupported 210Pb data are used as reliable indicators of enhanced/reduced deposition events. Also, the calculated inventories have enabled the estimation of the radiological contribution of the Spanish Mediterranean margin to the total radioactivity deposited onto the Mediterranean sea floor.     

Determination of thorium, uranium and potassium elemental concentrations in surface soils in Cyprus

A comprehensive study was conducted to determine thorium, uranium and potassium elemental concentrations in surface soils throughout the accessible area of Cyprus using high-resolution gamma-ray spectrometry. A total of 115 soil samples was collected from all over the bedrock surface of the island based on the different lithological units of the study area. The soil samples were air-dried, sieved through a fine mesh, sealed in 1000-ml plastic Marinelli beakers, and measured in the laboratory in terms of their gamma radioactivity for a counting time of 18 h each. From the measured gamma-ray spectra, elemental concentrations were determined for thorium (range from 2.5 x 10(-3) to 9.8 microg g(-1)), uranium (from 8.1 x 10(-4) to 3.2 microg g(-1)) and potassium (from 1.3 x 10(-4) to 1.9%). The arithmetic mean values (A.M. +/- S.D.) calculated from all samples are: (1.2+/-1.7 microg g(-1)), (0.6+/-0.7) microg g(-1), and (0.4+/-0.3%), for thorium, uranium and potassium, respectively, which are by a factor of three-six lower than the world average values of 7.4 microg g(-1) (Th), 2.8 microg g(-1) (U) and 1.3% (K) derived from all data available worldwide. The best-fitting relation between the concentrations of Th and K versus U and also of K versus Th, is essentially of linear type with a correlation coefficient of 0.93, 0.84 and 0.90, respectively. The Th/U, K/U and K/Th ratios (slopes) extracted are equal to 2.0, 2.8 x 10(3) and 1.4 x 10(3), respectively.     

Characterization of Pu concentration and its isotopic composition in soils of Gansu in northwestern China

The total ^239+240Pu activities and ²⁴⁰Pu/²³⁹Pu atom ratios in surface soil samples (0–5 cm) in the Kumtag Desert in western Gansu Province, and in a soil core sample in Lanzhou were investigated using a sector-field ICP-MS. In the surface soil samples, ^239+240Pu activities in fine particles (<150 μm) were 1.3–2.1 times of those in coarse particles (150 μm–1 mm) which ranged from 0.005 to 0.157 mBq/g. Atom ratios of ²⁴⁰Pu/²³⁹Pu in the surface soils ranged from 0.168 to 0.192 with a mean of 0.182 ± 0.008. The mean ratio was similar to the typical global fallout value although the Kumtag Desert was believed to have received close-in fallout derived from Chinese nuclear weapons tests mainly conducted in the 1970s. Furthermore, the mean ²⁴⁰Pu/²³⁹Pu atom ratio observed in the soil core sample in Lanzhou was similar to the typical global fallout value. In the soil core sample, ^239+240Pu activities in the various layers ranged from 0.012 to 0.23 mBq/g, and the inventory of ^239+240Pu (32.4 Bq/m², 0–23 cm) was slightly lower than that expected from global fallout (42 Bq/m²) at the same latitude. Rapid downward migration of Pu isotopes was observed in Lanzhou soil core sample layers. The contribution of the 10-cm deep top layers of surface soils to total inventory was only 17%, while the contribution of deeper layers (10–23 cm) was as high as 83%. The ^239+240Pu activity levels and ²⁴⁰Pu/²³⁹Pu atom ratios in soils in Gansu Province, China are similar to those in atmospheric deposition samples collected in the spring in recent years in Japan.     

Arbuscular mycorrhizas contribute to phytostabilization of uranium in uranium mining tailings

Uranium (U) tailings pose environmental risks and call for proper remediation. In this paper medic and ryegrass plants were used as host plants to examine whether inoculation with an AM fungus, Glomus intraradices, would help phytostabilization of U tailings. The need of amending with uncontaminated soil for supporting plant survival was also examined by mixing soil with U tailing at different mixing ratios. Soil amendment increased plant growth and P uptake. Ryegrass produced a more extensive root system and a greater biomass than medic plants at all mixing ratios. Medic roots were extensively colonized by G. intraradices whereas ryegrass were more sparsely colonized. Plant growth was not improved by mycorrhizas, which, however, improved P nutrition of medic plants. Medic plants contained higher U concentrations and showed higher specific U uptake efficiency compared to ryegrass. In the presence of U tailing, most U had been retained in plant roots, and this distribution pattern was further enhanced by mycorrhizal colonization. The results suggest a role for AM fungi in phytostabilization of U tailings.     

Use of pooled samples to assess human exposure to parabens,benzophenone-3 and triclosan in Queensland,Australia

Parabens, benzophenone-3 and triclosan are common ingredients used as preservatives, ultraviolet radiation filters and antimicrobial agents, respectively. Human exposure occurs through consumption of processed food and use of cosmetics and consumer products. The aim of this study was to provide a preliminary characterisation of exposure to selected personal care product chemicals in the general Australian population. De-identified urine specimens stratified by age and sex were obtained from a community-based pathology laboratory and pooled (n = 24 pools of 100). Concentrations of free and total (sum of free plus conjugated) species of methyl, ethyl, propyl and butyl paraben, benzophenone-3 and triclosan were quantified using isotope dilution tandem mass spectrometry; with geometric means 232, 33.5, 60.6, 4.32, 61.5 and 87.7 ng/mL, respectively. Age was inversely associated with paraben concentration, and females had concentrations approximately two times higher than males. Total paraben and benzophenone-3 concentrations are significantly higher than reported worldwide, and the average triclosan concentration was more than one order of magnitude higher than in many other populations. This study provides the first data on exposure of the general Australian population to a range of common personal care product chemical ingredients, which appears to be prevalent and warrants further investigation.     

The radioactivity measurements in soils and fertilizers using gamma spectrometry technique

Because of their mineral content, soils are naturally radioactive and one of the sources of radioactivity other than those of natural origin is mainly due to the extensive use of fertilizers. The main aim of this paper is to evaluate the fluxes of natural radionuclides in local production of phosphate fertilizers to determine the content of radioactivity in several commercial fertilizers produced in Algeria and to estimate their radiological impact in a cultivated soil even for the long-term exposure due to their application.For these purposes, virgin and fertilized soils were collected from outlying Setif region in Algeria and from phosphate fertilizers used in this area.Gamma spectrometry was exploited to determine activity concentration due to naturally occurring ²²⁶Ra, ²³²Th and ⁴⁰K in five types of samples (two different sorts of fertilizers, virgin and fertilized soils and well water used for irrigation) taken from Setif’s areas.The results show that these radionuclides were present in an average concentration of 134.7 ± 24.1, 131.8 ± 16.7, 11644 ± 550 Bq/kg for the first fertilizer NPK and 190.3 ± 30, 117.2 ± 10.3, 5312 ± 249 Bq/kg for the second fertilizer (NPKs). For the virgin and the fertilized soils, the corresponding values were respectively 47.01 ± 7.3, 33 ± 7, 329.4 ± 19.7 Bq/kg and 53.2 ± 10.6, 50.0 ± 7, 311.4 ± 18.7 Bq/kg. For well water, the values were 1.93 and 0.12 Bq/kg; however the third value was below the Minimum Detectable Activity (MDA).The radium equivalent activity (Raeq) and the representative level index I_γr for all samples were also calculated. The data were discussed and compared with those given in the literature.     

Method design and validation for the determination of uranium levels in human urine using high-resolution alpha spectrometry

Quantification of uranium in human urine is a valuable technique for assessing occupational and public exposure to uranium. A reliable method has been developed and validated in the ARPANSA Radiochemistry Laboratory by means of standard radiochemical separation and purification techniques and measurement using high-resolution alpha spectrometry. This method can be used to evaluate the levels of naturally occurring 234U, 235U and 238U in urine. Method design and validation is the process of defining an analytical requirement, and then confirming that the method under consideration has performance capabilities consistent with what the application requires. The method was designed to measure levels down to 2 mBq/day of total uranium, corresponding to approximately 1/100th of the annual committed effective dose of 20 mSv. Validation tests were developed to assess selectivity, accuracy, recovery and quantification of uncertainty. The radiochemical recovery of this method was measured using (232)U tracer. The typical minimum detectable concentration for total uranium for 24-h urine samples is approximately 0.6 mBq/day or 0.019 microg/day.     

Comparative study of natural radioactivity levels in soil samples from the Upper Siwaliks and Punjab,India using gamma-ray spectrometry

Natural radioactive materials under certain conditions can reach hazardous radiological levels. So, it becomes necessary to study the natural radioactivity levels in soil to assess the dose for the population in order to know the health risks and to have a baseline for future changes in the environmental radioactivity due to human activities. The natural radionuclide (²²⁶Ra, ²³²Th, and ⁴⁰K) contents in soil were determined for 26 locations around the Upper Siwaliks of Kala Amb, Nahan and Morni Hills, Northern India, using high-resolution gamma-ray spectrometric analysis. It was observed that the concentration of natural radionuclides viz., ²²⁶Ra, ²³²Th and ⁴⁰K, in the soil varies from 28.3 ± 0.5 to 81.0 ± 1.7 Bq kg⁻¹, 61.2 ± 1.3 to 140.3 ± 2.6 Bq kg⁻¹ and 363.4 ± 4.9 to 1002.2 ± 11.2 Bq kg⁻¹ respectively. The total absorbed dose rate calculated from activity concentration of ²²⁶Ra, ²³²Th and ⁴⁰K ranged from 71.1 to 162.0 nGy h⁻¹. The radium equivalent (R_eq) and the external hazard index (H_ex), which resulted from the natural radionuclides in soil, were also calculated and found to vary from 149.4 to 351.8 Bq kg⁻¹and from 0.40 to 0.95 respectively. These values in Upper Siwaliks area were compared with that from the adjoining areas of Punjab. The radium equivalent activities in all the soil samples were lower than the limit (370 Bq kg⁻¹) set in the Organization for Economic Cooperation and Development (OECD) report and the dose equivalent was within the safe limit of 1 mSv y⁻¹.     

Thermal neutron fluence from ultra low-level gamma-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 gamma-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 430m 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.     

Determination of total content and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes by ICP-QMS

The aim of this work was to determine the concentrations and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes. An analytical method was developed with a plutonium and uranium separation procedure based on extraction chromatography (using 2 mL TEVA and UTEVA columns) and detection with a quadrupole ICP-MS applying an ultra-sonic nebulizer coupled with a membrane desolvation system. Starting from blank swipes, the background equivalent concentration (BEC) was 8 fg for ²³⁹Pu and 1 ng ²³⁸U. The method was successfully applied to certified reference materials as well as to round robin samples obtained in the framework of the inter-laboratory exercise program, promoted by the Brazilian–Argentine Agency for Accounting and Control of Nuclear Materials (ABACC), together with the US Department of Energy (USDOE). After the introduction of an additional ion-exchange separation step, the methodology was applied to the IAEA-384 sediment reference sample with precise and accurate total plutonium and uranium, ²⁴⁰Pu/²³⁹Pu, ²⁴¹Pu/²³⁹Pu, ²³⁴U/²³⁸U and ²³⁵U/²³⁸U atomic ratio results.     

Discrimination of source reactor type by multivariate statistical analysis of uranium and plutonium isotopic concentrations in unknown irradiated nuclear fuel material

The problem of identifying the provenance of unknown nuclear material in the environment by multivariate statistical analysis of its uranium and/or plutonium isotopic composition is considered. Such material can be introduced into the environment as a result of nuclear accidents, inadvertent processing losses, illegal dumping of waste, or deliberate trafficking in nuclear materials. Various combinations of reactor type and fuel composition were analyzed using Principal Components Analysis (PCA) and Partial Least Squares Discriminant Analysis (PLSDA) of the concentrations of nine U and Pu isotopes in fuel as a function of burnup. Real-world variation in the concentrations of (234)U and (236)U in the fresh (unirradiated) fuel was incorporated. The U and Pu were also analyzed separately, with results that suggest that, even after reprocessing or environmental fractionation, Pu isotopes can be used to determine both the source reactor type and the initial fuel composition with good discrimination.