Multi-group approximation, scattering and calibration coefficients, uncertainty estimates and detection limits of a NaI(Tl)-based gamma spectrometry set-up for low-level activity analysis

This paper describes a quantitative radioactivity analysis method especially suitable for environmental samples with low-level activity. The method, consisting of a multi-group approximation based on total absorption and Compton spectra of gamma rays, is coherently formalized and a computer algorithm thereof designed to analyze low-level activity NaI(Tl) gamma ray spectra of environmental samples. Milk powder from 1988 was used as the example case. Included is a special analysis on the uncertainty estimation. Gamma sensitiveness is defined and numerically evaluated. The results reproduced the calibration data well, attesting to the reliability of the method. The special analysis shows that the uncertainty of the assessed activity is tied to that of the calibration activity data. More than 77% of measured 1461-keV photons of ⁴⁰K were counted in the range of clearly lower energies. Pile-up of single line photons (¹³⁷Cs) looks negligible compared to that of a two-line cascade (¹³⁴Cs). The detection limit varies with radionuclide and spectrum region and is related to the gamma sensitiveness of the detection system. The best detection limit always lies in a spectrum region holding a line of the radionuclide and the highest sensitiveness. The most radioactive milk powder sample showed a activity concentration of 21 ± 1 Bq g⁻¹for ¹³⁷Cs, 323 ± 13 Bq g⁻¹ for ⁴⁰K and no ¹³⁴Cs.     

A follow up of the decrease of non exchangeable organically bound tritium levels in the surroundings of a nuclear research center

In the past decades limited amounts of tritium were handled on the CEA site of Bruyères le Châtel with authorised atmospheric releases. A small fraction of the tritium released entered into environmental samples under three forms: (i) as part of free water (TFWT - Tissue Free Water Tritium), or associated with organic matter in two ways; either (ii) bound to the oxygen and nitrogen atoms of the material as exchangeable organically bound tritium (E-OBT), or (iii) bound to carbon atoms as non exchangeable organically bound tritium (NE-OBT). The first two components provide only a picture of atmospheric tritium concentrations at the sampling time as they are in equilibrium with atmospheric moisture and soil humidity. Unlike these exchangeable forms, however, NE-OBT is tightly bound to the organic matter and provides an integrated record of atmospheric tritium during the growing phase of the vegetation. We mapped NE-OBT in tree leaf samples in an area of about 25 × 30 km² around the centre of the CEA site and compared the results with those obtained during a previous sampling exercise in 1989. At this time, the activity levels were almost ten times higher than those observed presently in a similar area almost 20 years later which is consistent with the decrease of atmospheric releases issued from the centre. As the activity levels are now close to environmental background specific attention was also paid to the analytical procedure to ensure reliable low level NE-OBT detection.     

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.     

CO2 dispersion around two PWR nuclear power plants in Brazil

Atmospheric air samples were taken within 3 km from power plants encompassing five different distances and wind directions. Samples were taken between 2002 and 2005 aiming to evaluate the environmental ¹⁴C enrichment due to the operation of Brazilian nuclear power plants. The sampling system consisted of a pump connected to a trapping column filled with a 3 M NaOH solution. The trapped CO₂ was analyzed for ¹⁴C by using a single stage accelerator mass spectrometry (SSAMS).     

Determination of radionuclide levels in rainwater using ion exchange resin and γ-spectrometry

The evaluation of radioactivity accidentally released into the atmosphere involves determining the radioactivity levels of rainwater samples. Rainwater scavenges atmospheric airborne radioactivity in such a way that surface contamination can be deduced from rainfall rate and rainwater radioactivity content. For this purpose, rainwater is usually collected in large surface collectors and then measured by γ-spectrometry after such treatments as evaporation or iron hydroxide precipitation. We found that collectors can be adapted to accept large surface (diameter 47 mm) cartridges containing a strongly acidic resin (Dowex AG 88) which is able to quantitatively extract radioactivity from rainwater, even during heavy rainfall. The resin can then be measured by γ-spectrometry. The detection limit is 0.1 Bq per sample of resin (80 g) for ¹³⁷Cs. Natural ⁷Be and ²¹⁰Pb can also be measured and the activity ratio of both radionuclides is comparable with those obtained through iron hydroxide precipitation and air filter measurements. Occasionally ²²Na has also been measured above the detection limit. A comparison between the evaporation method and the resin method demonstrated that 2/3 of ⁷Be can be lost during the evaporation process. The resin method is simple and highly efficient at extracting radioactivity. Because of these great advantages, we anticipate it could replace former rainwater determination methods. Moreover, it does not necessitate the transportation of large rainwater volumes to the laboratory.     

Variation of radiation level and radionuclide enrichment in high background area

Significantly high radiation level and radionuclide concentration along Quilon beach area of coastal Kerala have been reported by several investigators. Detailed gamma radiation level survey was carried out using a portable scintillometer. Detailed studies on radionuclides concentration in different environmental matrices of high background areas were undertaken in the coastal areas of Karunagapalli, Kayankulam, Chavara, Neendakara and Kollam to study the distribution and enrichment of the radionuclides in the region. The absorbed gamma dose rates in air in high background area are in the range 43-17,400 nGyh⁻¹. Gamma radiation level is found to be maximum at a distance of 20 m from the sea waterline in all beaches. The soil samples collected from different locations were analysed for primordial radionuclides by gamma spectrometry. The activity of primordial radionuclides was determined for the different size fractions of soil to study the enrichment pattern. The highest activity of ²³²Th and ²²⁶Ra was found to be enriched in 125-63 μ size fraction. The preferential accumulation of ⁴⁰K was found in <63 μ fraction. The minimum ²³²Th activity was 30.2 Bq kg⁻¹, found in 1000-500 μ particle size fraction at Kollam and maximum activity of 3250.4 Bq kg⁻¹ was observed in grains of size 125-63 μ at Neendakara. The lowest ²²⁶Ra activity observed was 33.9 Bq kg⁻¹ at Neendakara in grains of size 1000-500 μ and the highest activity observed was 482.6 Bq kg⁻¹ in grains of size 125-63 μ in Neendakara. The highest ⁴⁰K activity found was 1923 Bq kg⁻¹ in grains of size <63 μ for a sample collected from Neendakara. A good correlation was observed between computed dose and measured dose in air. The correlation between ²³²Th and ²²⁶Ra was also moderately high. The results of these investigations are presented and discussed in this paper.     

Study of the comparative dynamics of the incorporation of tissue free-water tritium (TFWT) in bulrushes (Typha latifolia) and carp (Cyprinus carpio) in the Almaraz nuclear power plant cooling reservoir

The Almaraz nuclear power plant (Spain) uses the water of Arrocampo reservoir for cooling, and consequently raises the radioactive levels of the aquatic ecosystem of this reservoir. From July 2002 to June 2005, monthly samples of surface water, bulrushes (Typha latifolia) and carp (Cyprinus carpio) were collected from this reservoir. They were analyzed to determine the temporal evolution of the levels of ³H in surface water and of its transfer from the surface water to free-water in the tissues (TFWT) of the aforementioned two organisms. The tritium levels in the surface water oscillate with a biannual period, with their values in the study period ranging between 53 and 433 Bq/L. The incorporation of tritium to bulrushes and carp was fairly similar, the respective mean concentration factors being 0.74 and 0.8 (unitless, as Bq/L tissue water per Bq/L reservoir water). The temporal evolution of the levels fairly closely followed that observed for the surface water tritium, although detailed analysis showed the dominant periodicity for the bulrushes to be annual. This difference reflects the influence on the incorporation of tritium to bulrushes of diverse environmental and metabolic factors, especially evapotranspiration and the seasonal growth of this plant.     

Tritium profiles in snowpacks

The release of tritiated water (HTO) to the atmosphere during the winter can contribute significantly to snow contamination and to water-soil-plant contamination after the spring thaw. The dose significance of such a release depends on the persistence of tritiated water in the snowpack, which is primarily controlled by the HTO diffusion process in snow and the rate of re-emission into the atmosphere from the snowpack surface. Monitoring data collected after an acute winter release at Chalk River Laboratories and data obtained in winter over a chronically contaminated area were analyzed to estimate the diffusion coefficient of HTO in the snowpack. Under conditions of cold and dry snow, the diffusion coefficient lay in the range 1-2 × 10⁻¹⁰ m² s⁻¹, an order of magnitude lower than diffusion in water but an order of magnitude higher than self-diffusion in ice. These results confirm the theoretical predictions (Bales, 1991). Values up to six times higher were found for warmer periods and just before spring melt, when other processes contribute to profile evolution. The low diffusion rate of tritium in cold, dry snow means that tritium remains in the snowpack throughout the winter, to be released during spring thaw to potentially contaminate surface water, soil and crops.     

Experimental investigation and modelling of tritium washout by precipitation in the area of the nuclear power plant of Paks, Hungary

Tritium occurs in nature in trace amounts, but its concentration is changing due to natural and artificial sources. Studies focusing on natural tritium have to take into account the effect of artificial sources. Also, the impact of tritium is an important issue in environmental protection, e.g. in connection with the emissions from nuclear power plants. The present work focuses on the rain washout of tritium emitted from the Paks nuclear power plant in Hungary. Rainwater collectors were placed around the plant and after a period of precipitation, rainwater was collected and analysed for tritium content. Samples were analysed using low-level liquid scintillation counting, with some also subject to the more accurate ³He ingrowth method. The results clearly show the trace of the tritium plume emitted from the plant; however, values are only about one order of magnitude higher than environmental background levels. A washout model was devised to estimate the distribution of tritium around the plant. The model gives slightly higher concentrations than those measured in the field, but in general the agreement is satisfactory. The modelled values demonstrate that the effect of the plant on rainwater tritium levels is negligible over a distance of some kilometres.     

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.     

Pre-concentration of naturally occurring radionuclides and the determination of (212)Pb from fresh waters

A novel technique has been developed for determining the ²¹²Pb activity of fresh waters. This is of interest to environmental monitoring programmes that utilise gross α-activity methods to screen for anthropogenic radionuclides. The contribution from ²¹²Pb varies, and is difficult to experimentally measure due to its relatively short half-life (t_½ = 10.6 h) and low environmental activity (<0.1 Bq l⁻¹). The use of a three-stage technique that encompasses a unique form of pre-concentration, separation and analysis by liquid scintillation counting allows a lower detection limit of 0.006 Bq l⁻¹ with a chemical yield of 92.5 ± 5.6%. The measurement can be obtained within 7 h of sample collection, and is calculated using the radioactive decay of ²¹²Bi. Other naturally occurring radionuclides may also be extracted using the pre-concentration stage of the technique, with efficiencies above 90% at a range of pH values.     

Suitable gamma energy for gamma-spectrometric determination of U in surface soil samples of a high rainfall area in India

The paper presents a systematic study on suitability of various gamma lines for monitoring of ²³⁸U activity in soil samples around a uranium mineralized zone of Kylleng Pyndengsohiong Mawthabah (Domiasiat), Meghalaya in India. The area lies in a plateau region which recieves the highest average annual rainfall (12,000 mm) in the world. The geochemical behaviour of the uranium and its daughter products at such wet climatic conditions imposes restrictions to assess ²³⁸U through gamma lines of radon decay products. Soil samples were collected from nine locations around the uranium mineralization zone for analysis. The ratio of the concentration of uranium obtained from gamma energies of radium daughter products to the 63.29 keV of ²³⁴Th was found to vary from 1.01 to 2.07, which indicates a pronounced disequilibrium between uranium and radium daughters. The results obtained from various gamma energies were validated from the data generated by Instrumental Neutron Activation Analysis (INAA) technique. The ²³⁸U activities from the two analytical methods show a well fitted regression line with correlation coefficient 0.99 which validates the reliability of 63.29 keV energy for estimation of uranium in such conditions.     

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.     

The effect of air mass origin on the ambient concentrations of Be and Pb in Islamabad, Pakistan

Concentration of radionuclides ²¹⁰Pb and ⁷Be, having half lives of 22.3 years and 53.29 days, respectively, in the surface air samples of Islamabad (33.38° N, 73.10° E and Altitude ∼536 m asl.) are measured. The non-destructive technique of gamma-spectrometry, with a high purity germanium HPGe detector, was employed for the analysis of all samples. The annual average concentrations of ²¹⁰Pb and ⁷Be in the surface air samples were determined as 0.284 ± 0.15 and 3.171 ± 1.14 mBq m⁻³, respectively. Our results have shown a seasonal variation of the concentration of ⁷Be in air samples with high values for the spring season. High concentrations for ²¹⁰Pb are obtained when air masses originate from plain areas of Pothohar region, located in the South-West, West and North West of Islamabad. Our values of concentrations show a nice agreement with the relevant reported results.     

Determination of organically bound tritium background level in biological samples from a wide area in the south-west of France

In this paper, the authors describe a sensitive method for low-level non-exchangeable OBT determination. This methodology combines suitable sample treatment, a combustion apparatus for large-sized samples and low-background liquid scintillation spectrometry, along with precautions that substantially reduce the risks of sample contamination. Great care must be taken in the measurement of non-exchangeable OBT at environmental levels. Many authors have discussed the opportunities for cross-contamination between samples and contamination by exchange with the laboratory atmosphere. The authors also describe an application of the methodology to a large-scale sampling and measurement campaign, aimed at the determination of the environmental non-exchangeable OBT background level in tree leaves and ferns collected on the site and in the vicinity of a research centre located in the south-west of France, not far from Bordeaux. This study constitutes a "zero level" for the non-exchangeable OBT activity, as, to our knowledge, there is no tritium source within or in the surroundings of the sampled area capable of producing non-exchangeable OBT activities above the natural levels. Our analyses showed that non-exchangeable OBT activities in the collected samples were very low, ranging from below the detection limit (ca 0.7 Bq kg(-1) of dry material) to ca 2 Bq kg(-1) of dry material. These values are similar to the natural tritium background measured in water samples. No discrepancies can be shown between fern samples and oak tree leaf samples or between samples collected inside and outside the research site.     

Recent atmospheric lead deposition recorded in an ombrotrophic peat bog of Great Hinggan Mountains, Northeast China, from Pb and Cs dating

Radioactive markers are useful in dating lead deposition patterns from industrialization in peat archive. Peat cores were collected in an ombrotrophic peat bog in the Great Hinggan Mountains in Northeast China in September 2008 and dated using ²¹⁰Pb and ¹³⁷Cs radiometric techniques. The mosses in both cores were examined systematically for dry bulk density, water and ash content. Lead also was measured using atomic emission spectroscopy with inductively coupled plasma (ICP-AES). Both patterned peat profiles were preserved well without evident anthropogenic disturbance. Unsupported ²¹⁰Pb and ¹³⁷Cs decreased with the depth in both of the two sample cores. The ²¹⁰Pb chronologies were established using the constant rate of supply model (CRS) and are in good agreement with the ¹³⁷Cs time marker. Recent atmospheric ²¹⁰Pb flux in Great Hinggan Mountains peat bog was estimated to be 337 Bq m⁻² y⁻¹, which is consistent with published data for the region. Lead deposition rate in this region was also derived from these two peat cores and ranged from 24.6 to 55.8 mg m⁻² y⁻¹ with a range of Pb concentration of 14-262 μg g⁻¹. The Pb deposition patterns were consistent with increasing industrialization over the last 135-170 y, with a peak of production and coal burning in the last 50 y in Northeast China. This work presents a first estimation of atmospheric Pb deposition rate in peatlands in China and suggests an increasing trend of environmental pollution due to anthropogenic contaminants in the atmosphere. More attention should be paid to current local pollution problems, and society should take actions to seek a balance between economic development and environmental protection.     

Radioactivity in environmental samples: Calibration standards measurement methods,quality assurance,and data analysis

The numerous environmental radioactivity measurements made by and for the U.S. Environmental Protection Agency (U.S. EPA) include measurements on samples of water, urine, food, milk, and air filters. Calibration standards are listed which are available in the form of water solutions and soils for a wide range of radionuclides. Method validation procedures for U.S. EPA approval include protocol development and single-laboratory and multiple-laboratory evaluation for precision and accuracy. Interlaboratory comparison studies are conducted for both cross-check and performance evaluation samples and involve 295 federal, state, and local laboratories. For water samples, 80%–90% of the participating laboratories are within the control limits for most of the radionuclides measured; however, some problem areas exist, especially for radium-228 and strontium-89 and -90. For milk and food samples, more than 90% of the laboratories are within control limits for cobalt-60 and cesium-137 but some problems exist for the measurement of strontium-90, iodine-131, and potassium-40. For tritium, 91% of the laboratories are within the control limit for water samples and 87% are within the control limits for the urine samples. The laboratory performance for air filter samples shows some problems for gross beta, strontium-90 and cesium-137 measurements.     

Microdistribution of Am in structures of submerged macrophyte Elodea canadensis growing in the Yenisei River

A submerged macrophyte of the Yenisei River, Elodea canadensis, was used to study the microdistribution of the artificial radionuclide ²⁴¹Am among different components of the plant. The total amount of ²⁴¹Am added to the experimental system was 1850 ± 31 Bq/L. The total amount of ²⁴¹Am accumulated by the plants was 182 Bq per sample, or 758,333 ± 385 Bq/kg dry mass. It has been found that the major portion of ²⁴¹Am accumulated by E. canadensis, up to 85%, was bound to solid components of the cells. It is observed that the microdistribution of ²⁴¹Am within different components of the submerged plant E. canadensis was not uniform. ²⁴¹Am distribution vary depending on the age of the leaf blades, the state of the cells and morphological features of the plant stem.     

Chronic risk assessment of exposure to volatile organic compounds in the atmosphere near the largest Mediterranean industrial site

This study focuses on characterising the risk of exposure to volatile organic compounds (VOCs) by means of inhalation in people living in the vicinity of the largest chemical production site in the Mediterranean area. Eighty-six VOCs were initially selected for this study based on their adverse environmental and health effects. The monitoring campaign was conducted for 276 days in three different locations around the chemical site. The analytical method used for the characterisation was based on European standard method EN-14662-2, which consists of the active sampling of air for 24 h in charcoal tubes, followed by extraction with carbon disulphide and GC-MS analysis. Forty-four VOCs with toxicological data available concerning their carcinogenic and non-carcinogenic health effects were quantified during the monitoring campaign. None of the quantified VOCs showed average concentrations exceeding their chronic reference concentrations and, therefore, no non-carcinogenic health effects are expected as a result of this exposure. However, the global average cancer risk due to VOC exposure in the area (3.3 × 10^− 4) was found to be above the values recommended by the WHO and USEPA.The influence of the analytical method was also evaluated by comparing cancer risk estimates using a thermal desorption (TD) method based on method EN-14662-1. The results of the 24-h samples for the solvent extraction method were compared with the average of 12 daily samples of 2-h for the TD method for 24 sampling days. Although the global estimated lifetime cancer risk was statistically comparable for both methods, some differences were found in individual VOC risks.To our knowledge, this is the first study that estimates the carcinogenic and non-carcinogenic risks posed by the inhalation of VOCs in people living near a chemical site of this size, and compares the estimated cancer risk obtained using two different standard analytical methods.     

Natural radioactivity levels in topsoil from the Pearl River Delta Zone, Guangdong, China

Concentrations of the natural radionuclides ²³⁸U, ²²⁶Ra, ²³²Th and ⁴⁰K have been measured by γ-ray spectrometry in 796 topsoil samples from the Pearl River Delta Zone (PRDZ) of Guangdong, China. The mean concentrations for ²³⁸U, ²²⁶Ra, ²³²Th and ⁴⁰K were found to be 140 ± 37 Bq kg⁻¹, 134 ± 41 Bq kg⁻¹, 187 ± 80 Bq kg⁻¹ and 680 ± 203 Bq kg⁻¹ dry mass, respectively. These values were all higher than the mean values in soil for China and the world. Outdoor air-absorbed dose rates, calculated from activity concentrations of ²²⁶Ra, ²³²Th and ⁴⁰K, ranged from 86 to 237 nGy h⁻¹, with a mean value of 165 ± 46 nGy h⁻¹. The corresponding annual outdoor effective dose rate per person was estimated to be between 0.11 and 0.29 mSv y⁻¹, with a mean value of 0.20 ± 0.06 mSv y⁻¹, which was also higher than the world mean value of 0.07 mSv y⁻¹. The radium equivalent activity (Ra_eq) and the external hazard index (I_r) resulted from the natural radionuclides in soil, were also calculated and found to vary from 230 to 676 Bq kg⁻¹ and from 0.6 to 1.8, respectively. The Ra_eq and the I_r in all the investigated regions were up to 75% higher than the set limits of 370 Bq kg⁻¹ and 1.0, respectively.