In situgamma spectrometry using a portable HPGe detector. Radiological characterisation and environmental surveillance around an operating nuclear power plant. Possibilities and limits.

The in situtechnique for measuring radionuclides in the soil using a portable Ge detector is a highly versatile tool for both the radiological characterisation and for the monitoring of operating nuclear power plants. The main disadvantage of this technique is related to the lack of knowledge of the geometry of the source whose activity concentration is to be determined. However, its greatest advantage is the high spatial representability of the samples and the reduced time and resource consumption compared to gamma spectrometry laboratory measurements. In this study, the possibilities and limits offered byin situgamma spectrometry with a high-resolution gamma portable detector in two common uses are shown. First, the radiological background characterisation and its relationship with the geology of an area of 2700 km2are assessed. Second, its potential for monitoring man-made activity concentration in soils located around an operating nuclear power plant in Spain for surveillance purposes is evaluated. Finally, high-accuracy radiation maps were prepared from the measurements that were carried out. These radiation maps are essential tools to know the radioactive background of an area, especially useful to assess artificial radioactive deposits produced after a nuclear accident or incident.

Study of radionuclides and heavy metal migration through soil profiles (0-60 cm) at points near the targets of NATO strikes in 1995: environmental monitoring and assessment.

The activity concentrations of natural and artificial radionuclides (40K, 232Th, 226Ra, 238U, 137Cs) and concentrations of six heavy metals of interest (Cd, Cr, Cu, Ni, Pb and Zn) were investigated in 18 soil samples through soil depths (0-10, 10-20, 20-30, 30-40.40-50, 50-60 cm) at the three selected sites in the Hadzici. Since at this area ammunition with depleted uranium had been used during the NATO strikes in 1995, this study was conducted with the aim to assess the radiological and environmental health hazards. Radioactivity was determined by gamma spectrometry using HPGe and LEGE detectors and content of heavy metals by using a flame atomic absorption spectrometry. The correlation with distribution of the radionuclides and their activity concentrations through depths was found only at the site 1 for 40K, 232Th and 226Ra, where minimum/maximum activity concentrations for 40K were 814.42 Bq/kg/1039.48 Bq/kg, for 232Th 53.98 Bq/kg/74.12 Bq/kg and for 226Ra 50.32 Bq/kg/65.73 Bq/kg. Vertical distribution of 137Cs along 3 site profiles was used for distinction of cultivated and uncultivated soil. Using the activity ratio of 238U/226Ra and 235U/238U, the presence of depleted uranium (DU) was established at the site 3. Obtained Igeo values for determined heavy metals showed that all of three sites were unpolluted to moderately polluted. Pb content in all three sites showed correlation with concentration decreasing with increasing soil depth.

Natural radioactivity assessment and geophysical interpretation of parts of Igarra area, Southern Nigeria.

To evaluate the concentration of natural radionuclides and to carry out geophysical interpretation of part of Igarra area, Southern Nigeria, an integrated geophysical approach was adopted involving radiometric, gravity, and magnetic methods. The RS-230 Super-Spec spectrometer, G-512 Lacoste and Romberg gravimeter, and the GSM-19v7.0 Overhauser instrument were used for the radiometric, gravity, and magnetic data acquisitions, respectively, along a specified traverse within the area. The datasets were processed using Oasis Montaj, Grav-Master, and Ms-Excel software. Gravity results show that the mean free air and Bouguer anomalies in the area are - 67.42 and - 84.22 mGal, while magnetic survey indicates that the mean corrected magnetic field intensity in this area is 32218.49 nT. Radiometric survey results show that the mean radioactivity concentrations of thorium ([Formula: see text], uranium ([Formula: see text]), and potassium ([Formula: see text]) are 31.81 Bq/kg, 26.48 Bq/kg, and 167.33 Bq/kg, respectively. Further analysis also revealed that the mean radioactivity equivalent of the area is 84.86 Bq/kg; absorbed dose rate is 72.74nGy/h, while the mean external hazard index is 0.30. A novel model equation for estimating absorbed dose rate from radioactivity equivalent was also obtained and validated. The gravity and magnetic survey results indicate the presence of low-density and high magnetic basement rocks underlying this area, while radiometric results reveal that radiations in this area did not exceed acceptable standards of 370 Bq/kg for radioactivity equivalent, 84 nGy/h for absorbed dose rate, and unity which corresponds to 370 Bq/kg for external hazard index as recommended by the United Nations Scientific Committee on the Effects of Atomic Radiation and the International Atomic Energy Agency.

Method development for rapid quantification of Rn-222 in surface water and groundwater.

Understanding the risks of a developing unconventional hydrocarbons industry, including shale gas, to the chemical quality of surface water and groundwater involves firstly establishing baseline compositions against which any future changes can be assessed. Contaminants of geogenic origin are of particular interest and radon has been identified as one potential contaminant from shale sources. Robust measurement and monitoring of radon in water at environmental concentrations is essential for ensuring protection of water sources and maintaining public confidence. Traditional techniques for Rn-222 determination in water, such as inference by gamma spectrometry and direct alpha counting, are impractical for direct field measurement, and the relatively short half-life of Rn-222 (~ 3.82 days) means that longer analytical protocols from field to the laboratory may result in greater uncertainty for Rn-222 activity. Therefore, a rapid and low-cost method would be beneficial. We have developed and refined a laboratory procedure for Rn-222 monitoring using liquid scintillation counting (LSC). The accuracy of Rn-222 activities obtained via this procedure was evaluated by the analysis of almost 200 water samples collected from streams and boreholes as part of a detailed baseline investigation in the Vale of Pickering, Yorkshire, one potential location for future shale gas exploration. LSC was preferred for measurement of Rn-222 and had comparable accuracy to gamma spectrometry and direct alpha counting. The methodology provided a rapid, portable and low-maintenance option relative to the two established techniques and is shown to be a favourable choice for the measurement of radon in surface water and groundwater at environmental concentrations.

A study of the radiological baseline conditions around the planned Sinop (Turkey) nuclear power plant using the mapping method.

This study makes a first attempt at a detailed estimation of the background radioactivity level and its distribution at the Sinop nuclear power plant site. The activity concentration levels of 226Ra, 232Th, 40K and 137Cs radionuclides in soil samples collected from 88 locations around Sinop Province, Turkey, in November 2016, were measured using gamma spectrometry. The distributions of radionuclide levels obtained from the results were evaluated using a geostatistical method, and the estimated radiation levels were determined using the ordinary kriging (OK) method, which is the best linear unbiased estimator (BLUE) for unmeasured points. Estimates of distribution results were evaluated using cross-validation diagrams, and it was shown that the OK method could predict radiological distributions for appropriate criteria. Finally, using the kriging parameters, distributions of radiation levels for the entire work area were mapped at a spatial resolution of 100 × 100 m2. These maps show that the natural radionuclides (226Ra, 232Th and 40K) are distributed at higher levels to the southeast of Sinop than in the other regions, and the activity of an artificial radionuclide (137Cs) is high in the interior and northern sections.

Environmental risk assessment of radioactivity and heavy metals in soil of Toplica region, South Serbia.

Activity levels of natural and artificial radionuclides and content of ten heavy metals (As, Cd, Co, Cr, Cu, Mn, Ni, Pb, Zn and Hg) were investigated in 41 soil samples collected from Toplica region located in the south part of Serbia. Radioactivity was determined by gamma spectrometry using HPGe detector. The obtained mean activity concentrations ± standard deviations of radionuclides 226Ra, 232Th, 40K and 137Cs were 29.9 ± 9.4, 36.6 ± 11.5, 492 ± 181 and 13.4 ± 18.7 Bq kg-1, respectively. According to Shapiro-Wilk normality test, activity concentrations of 226Ra and 232Th were consistent with normal distribution. External exposure from radioactivity was estimated through dose and radiation risk assessments. Concentrations of heavy metals were measured by using ICP-OES, and their health risks were then determined. Enrichment by heavy metals and pollution level in soils were evaluated using the enrichment factor, the geoaccumulation index (Igeo), pollution index and pollution load index. Based on GIS approach, the spatial distribution maps of radionuclides and heavy metal contents were made. Spearman correlation coefficient was used for correlation analysis between radionuclide activity concentrations and heavy metal contents.

Spectral windows analysis method for monitoring anthropogenic radionuclides in real-time environmental gamma-ray scintillation spectrometry.

This paper proposes an analysis methodology based on the spectral windows technique aimed for environmental real-time gamma-ray spectra obtained with scintillation detectors. The method permits us to monitor activity concentrations of selected isotopes, such as anthropogenic radionuclides like 137Cs and 131I, by removing the Compton scattering plus other external contributions and resolving peak overlapping within any window. Activity concentrations are presented for 137Cs, 131I, 214Bi, and 214Pb when applying the method to a monitor using a LaBr3(Ce) detector. The method avoids false-positive and false-negative results of anthropogenic radionuclides in the presence of radiation from natural origins by obtaining activity concentrations that correspond to those obtained by a Gaussian fitting commercial software.

Assessment of dry and wet atmospheric deposits of radioactive aerosols: application to Fukushima radiocaesium fallout.

The Fukushima Dai-ichi nuclear accident led to massive atmospheric deposition of radioactive substances onto the land surfaces. The spatial distribution of deposits has been estimated by Japanese authorities for gamma-emitting radionuclides through either airborne monitoring surveys (since April 2011) or in situ gamma-ray spectrometry of bare soil areas (since summer 2011). We demonstrate that significant differences exist between the two surveys for radiocaesium isotopes and that these differences can be related to dry deposits through the use of physically based relationships involving aerosol deposition velocities. The methodology, which has been applied to cesium-134 and cesium-137 deposits within 80-km of the nuclear site, provides reasonable spatial estimations of dry and wet deposits that are discussed and compared to atmospheric numerical simulations from the Japanese Atomic Energy Agency and the French Institute of Radioprotection and Nuclear Safety. As a complementary approach to numerical simulations, this field-based analysis has the possibility to contribute information that can be applied to the understanding and assessment of dose impacts to human populations and the environment around Fukushima.

Low-level gamma ray counting on environmental samples.

One of the major demands in gamma spectrometry of environmental samples is the accurate determination of activity concentration of present radionuclides (naturally occurring and those of artificial origin), due to the fact they are commonly of relatively low content. Thus, all these measurements have in common that the detection limit, in the spectral region of interest should be as low as possible. For this reason, the construction of a good passive, as well as active shield requires a detailed knowledge of the origin of the background events in the absence of an environmental sample. In addition, an analysis of the impact on detection limits due to the presence of the sample itself is also important. Also, the knowledge of the statistical basics for low-level counting is helpful to enable the best choice of detector characteristics (relative efficiency, peak to Compton ratio, resolution), measuring time, and required level of precaution against the different background contributions. In this paper, the background spectra of several gamma spectroscopy systems (with passive and active veto shields) are analyzed and discussed, regarding their capabilities for measurements of environmental samples. Furthermore, various environmental samples are analyzed by low-level gamma spectrometry, including the sample measurements in the presence of an active veto shield against cosmic-ray muons. The disturbance of radioactive equilibrium between members of radioactive series in the samples is commented on, together with the possibility of use of certain gamma lines (including their interference and the corresponding intensities) for radionuclide activities determination.

Radioactivity determination in depth distribution of stone samples of Kalaburagi District, Karnataka, India.

The activity concentrations of 238U, 232Th and 40K were found using high-resolution gamma-ray spectrometry on depth profile samples collected from the Kalaburagi districts. This study aims to ascertain the radioactivity Changes concerning the depth profile. With values of 51.64 ± 0.50 Bq kg-1 for 238U, 58.77 ± 0.23 for 232Th and 313.92 ± 3.57 for 40K, respectively, the depth profile samples of Jayanagar in the Kalaburagi region exhibit significant activity concentrations among the measured values. Moreover, estimates of the K/Th and K/U ratios have been made, based on surface-level collected samples, which may have values that differ from the samples under study.

A tomographic spatial-unfolding method for Compton gamma imaging measurements.

An advanced spatial-unfolding technique capable of reconstructing the activity distribution within an exclusion zone from Compton gamma imager measurements taken outside of it is introduced. Although the method is generally applicable to extended sources, we demonstrate it here on a calibrated Cs-137 point source through Monte Carlo simulation studies as well as with measurements made using a Silicon Compton Telescope for Safety and Security (SCoTSS) gamma imager. For synthetic data the method accurately reconstructs the total activity contained within the mapped zone of interest, even when the size of the basis elements used to reconstruct the activity distribution is larger than the source itself. For experimental data, the method reliably located the source but underestimated its activity by up to 17%. This is accurate enough for real-world security applications. The underestimation is likely due to effects not yet included in the simulated response of the detector. The method has widespread applicability in the radiological/nuclear safety and security field, particularly for scenarios in which a threat material or contaminated area lies within a no-entry or no-fly zone.

Gamma-spectrometry measurements of filtration media from an Advanced Gas-cooled Reactor.

Filtration media used to quantify particulate and gaseous releases have been collected from Hartlepool Power Station in the United Kingdom and measured using high-sensitivity gamma-spectrometry systems. Radionuclides that are relevant to the monitoring regime of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) have been detected. Results are reported and compared to detections recorded on the International Monitoring System (IMS). Time series activity plots have been produced and results interpreted with respect to known plant activities. The reported results improve the understanding of trace-level radionuclide emissions from Advanced Gas-cooled Reactors (AGRs) and aid interpretation of IMS measurements. This work is being performed as part of the Xenon Environmental Nuclide Analysis at Hartlepool (XENAH) collaboration between the Atomic Weapons Establishment (AWE, UK), EDF Energy (UK), Pacific Northwest National Laboratory (PNNL, US) and the Swedish Defence Agency (FOI, Sweden).

Effect of drying temperature on the quantitative analysis of 131I in algal samples by γ-spectrometry.

131I has been extensively utilized in nuclear medicine, resulting in its widespread detection in coastal algal samples due to its discharge. Therefore, it is essential to monitor 131I in the coastal algal samples. γ-spectrometry is an expeditious method for measuring 131I, but this method requires the pretreatment of the algal sample. The effect on 131I in the algal sample during the oven-drying treatment is unclear. In this study, the Laminaria japonica Areschoug and Sargassum vachellianum Greville were collected at two locations and analyzed for 131I using γ-spectrometry. Additionally, the content of iodine was measured using an Inductively Coupled Plasma-Mass Spectrometer (ICP-MS) to clarify the effect of 131I loss during drying treatment at different temperatures. The results demonstrated that the dried Laminaria and Sargassum samples had calculated 131I activity concentration relative standard deviations (RSDs) of 6.34 % and 16.31 %, respectively, while the fresh samples exhibited RSDs of 11.70 % and 15.57 %. Additionally, the iodine content RSDs in the dried samples were 9.19 % for Laminaria and 10.34 % for Sargassum. Significantly, discrepancies in 131I activity concentration between the fresh and dried Laminaria and Sargassum were 5.4 % and 10.3 %. These findings indicate that the temperature factor in drying has no effect on 131I loss in Laminaria and Sargassum in the range of 70 °C-110 °C.

Measurement of radon exhalation rate and radiation doses in fly ash samples.

Coal based thermal power plants contribute about ~ 72% of the power generation in India. Indian coal is of bituminous type, having a high ash content with 55-60% ash. Due to considerable environmental importance the collected fly ash has become a subject of worldwide interest in recent years. In the present study radon exhalation rate and the activity concentration of 226Ra, 232Th and 40K radionuclides in fly ash samples from Kasimpur Thermal Power Plant, Aligarh, Uttar Pradesh, India have been measured by 'Sealed Can technique' using LR-115 type II detectors and a low-level NaI (Tl)- based gamma-ray spectrometer, respectively. Radon exhalation rate has been found to vary from 57.1 ± 5.3 to 119.4 ± 7.7 mBq m-2 h-1 with an average value of 87.3 ± 5.8 mBq m-2 h-1. Activity concentration of 226Ra ranged from 20.0 ± 8.5 to 30.0 ± 9.7 Bq kg-1 with an average value 23.4 ± 9.0 Bq kg-1, 232Th ranged from 17.0 ± 9.9 to 69.0 ± 13.8 Bq kg-1 with an average value of 46.5 ± 12.1 Bq kg-1 and 40K ranged from 130.0 ± 7.2 to 332.0 ± 11.1 Bq kg-1 with an average value of 177.0 ± 8.1 Bq kg-1.

Integration of beta counting system with ORION-DSP coupled to NaI(Tl) detector-a comparative study with an HPGe detector.

The integration of the ORION digital signal processing-based MCA system coupled with a 3″ × 3″ NaI(Tl) detector assembly with a GM detector for counting beta (ß) has eliminated the need for a standalone ß-γ method in which U3O8 is determined by gross ß and gross γ counting. Uraniferous and mixed U-Th samples were taken up for study and compared with the results obtained from Canberra p-type coaxial high resolution gamma ray spectrometry detector. In uraniferous samples, U3O8 values obtained are within ±10%, whereas in the case of mixed U-Th samples, U3O8 values are within ±15%. Regression graphs drawn between the outcomes from the two analytical systems indicate R2 > 0.95 for Ra(eU3O8) and ThO2. In uraniferous samples, the R2 value for U3O8 was found to be > 0.99, but in mixed U-Th samples, it is 0.92. The closeness of agreement between the results obtained from two methods at various concentrations over the analytical range shows that the integrated system is suitable for the quantitative determination of eU3O8, U3O8, Ra(eU3O8), ThO2 and K in geological rock samples.

Proximal gamma-ray spectroscopy to predict soil properties using windows and full-spectrum analysis methods.

Fine-scale spatial information on soil properties is needed to successfully implement precision agriculture. Proximal gamma-ray spectroscopy has recently emerged as a promising tool to collect fine-scale soil information. The objective of this study was to evaluate a proximal gamma-ray spectrometer to predict several soil properties using energy-windows and full-spectrum analysis methods in two differently managed sandy loam fields: conventional and organic. In the conventional field, both methods predicted clay, pH and total nitrogen with a good accuracy (R2 ≥ 0.56) in the top 0-15 cm soil depth, whereas in the organic field, only clay content was predicted with such accuracy. The highest prediction accuracy was found for total nitrogen (R2 = 0.75) in the conventional field in the energy-windows method. Predictions were better in the top 0-15 cm soil depths than in the 15-30 cm soil depths for individual and combined fields. This implies that gamma-ray spectroscopy can generally benefit soil characterisation for annual crops where the condition of the seedbed is important. Small differences in soil structure (conventional vs. organic) cannot be determined. As for the methodology, we conclude that the energy-windows method can establish relations between radionuclide data and soil properties as accurate as the full-spectrum analysis method.

Gamma spectrometric measurement of uranium isotopic composition and mass in sintered UO2 pellets using the efficiency transfer method.

Gamma spectrometric measurements to determine the isotopic composition and total uranium mass in UO2 pellets (D = 7.5 mm; H = 3.5 mm, ρ = 10 g/cm3) were carried out. The required efficiency curve was obtained by applying the efficiency transfer method from a calibration standard (D = 65 mm; H = 20 mm) of a slightly acidified water solution. The average isotopic composition of ten UO2 pellets was consistent with values of natural uranium given by IUPAC. The average relative bias for the 235U/238U amount ratio was -0.73% using the 1001 keV gamma line for 238U and 0.50% using the 63 keV gamma line (186 keV was always used for 235U). For the total uranium mass, the mean deviation as compared to mass determinations using a balance was 5.5% using the 1001 keV gamma line for 238U and 4.3% using the 63 keV gamma line.

Characterization of a 4παß(LS)-γ(HPGe) prototype system for low-background measurements.

A ground-level prototype system for low-background measurements was developed and tested. The system consists of a high-purity germanium (HPGe) detector used for detecting γ rays and coupled to a liquid scintillator (LS) used for detecting α and ß particles. Both detectors are surrounded by shielding materials and anti-cosmic detectors ("veto") used to suppress background events. The energy and timestamp of detected α, ß and γ emissions are recorded event-by-event and analyzed offline. By requiring timing coincidence between the HPGe and LS detectors, background events originating from outside the volume of the measured sample can be effectively rejected. The system performance was evaluated using liquid samples containing known activities of an α emitter (241Am) or a ß emitter (60Co) whose decays are accompanied by γ rays. The LS detector was found to provide a solid angle of almost 4π for α and ß particles. Compared to the traditional γ-singles mode, operating the system in coincidence mode (i.e., α-γ or ß-γ) reduced the background counts by a factor of ∼100. Consequently, the minimal detectable activity for 241Am and 60Co was improved by a factor of 9, being 4 mBq and 1 mBq for an 11-d measurement, respectively. Furthermore, by applying a spectrometric cut in the LS spectrum that corresponds to α emission from 241Am, a background reduction factor of ∼2400 (compared to γ-singles mode) was achieved. Beyond low-background measurements, this prototype exhibits additional compelling features, such as the ability to focus on certain decay channels and study their properties. This concept for a measurement system may be of interest to laboratories that monitor environmental radioactivity, studies involving environmental measurements and/or trace-level radioactivity.

Unmanned stationary online monitoring system based on buoy for marine gamma radioactivity.

Research on unmanned online monitoring equipment for marine radioactivity surrounding nuclear power plants is of great significance. In this work, a small radioactivity monitoring system based on buoy was designed and manufactured for the emergency situation of nuclear accidents. The core of the radioactivity monitoring system is the underwater gamma spectrometer. The spectrometer can respond to gamma rays from 60 keV to 3 MeV, and can identify the nuclides whose characteristic rays belong to this energy range. The detection efficiency curve was calculated through Monte Carlo simulation and verified in a standard liquid source. A data acquisition processor was also designed to coordinate the detectors in the system and wirelessly transmit online monitoring data. Three experiments were carried out in the seawater around the Tianwan Nuclear Power Plant in Lianyungang, China using this online marine radioactivity monitoring system based on buoys. The stability and radioactivity monitoring capabilities of the system have been verified.

2D inversion of in situ gamma-ray spectrometric measurements of 137Cs for site characterization.

Environmental contamination by radioactive materials can be characterized by in situ gamma surface measurements. During such measurements, the field of view of a gamma detector can be tens of meters wide, resulting in a count rate that integrates the signal over a large measurement support volume/area. The contribution of a specific point to the signal depends on various parameters, such as the height of the detector above the ground surface, the gamma energy and the detector properties, etc. To improve the spatial resolution of the activity concentration, contributions of a radionuclide from nearby areas to the count rate of a single measurement should be disentangled. The experiments described in this paper, deployed 2D inversion of in situ gamma spectrometric measurements using a non-negative least squares-based Tikhonov regularization method. Data were acquired using a portable LaBr3 gamma detector. The detector response as a function of the distance of the radioactive source, required for the inversion process, was simulated using the Monte Carlo N-Particle (MCNP) transport code. The uncertainty on activity concentration was calculated using the Monte Carlo error propagation method. The 2D inversion methodology was first satisfactorily assessed for 133Ba and 137Cs source activity distributions using reference pads. Secondly, this method was applied on a 137Cs contaminated site, making use of above-ground in-situ gamma spectrometry measurements, conducted on a regular grid. The inversion process results were compared with the results from in-situ borehole measurements and laboratory analyses of soil samples. The calculated 137Cs activity concentration levels were compared against the activity concentration value for exemption or clearance of materials which can be applied by default to any amount and any type of solid material. Using the 2D inversion and the Monte Carlo error propagation method, a high spatial resolution classification of the site, in terms of exceeding the exemption limit, could be made. The 137Cs activity concentrations obtained using the inversion process agreed well with the results from the in-situ borehole measurements and those from the soil samples, showing that the 2D inversion is a convenient approach to deconvolute the contribution of radioactive sources from nearby areas within a detector's field of view, and increases the resolution of spatial contamination mapping.