Determination of the activity and nuclear decay data of 157Tb.

Terbium-157 was radiochemically extracted from an irradiated tantalum target. Since the resulting material contained a significant impurity of 158Tb, 157Tb was isotopically purified using laser resonance ionization at the RISIKO mass separator in Mainz and then implanted on an aluminum (Al) foil. The implanted 157Tb was measured by two different calibrated gamma-ray spectrometers to determine photon emission rates. After dissolving the Al foil, a high purity 157Tb solution was obtained. The corresponding activity concentration was determined with a low relative uncertainty of 0.52% through a combination of liquid scintillation counting using the TDCR method and 4π(X,e)(LS)-(X,γ)(CeBr3) coincidence counting. By combining the results from all measurement techniques, emission intensities for K X-rays and gamma-rays were derived and found to be 16.05(31)% and 0.0064(2)%, respectively. The probability for K electron capture of the first forbidden non-unique transition to the ground state was determined to be 17.16(35)%. The probabilities for the electron-capture branch to the excited level and the ground state were found to be 0.084(4)% and 99.916(4)%, respectively. A Q+ value of 60.23(18) keV was estimated based on simplified BetaShape calculations, assuming an allowed transition.

Measurements of the absolute gamma-ray emission intensities from the decay of 166Ho.

166Ho (T1/2≈ 26.8 h) is an emerging theragnostic radionuclide of interest in nuclear medicine due to its peculiar decay scheme, featuring high-energy ß- emission (≈ 1.8 MeV) coupled with the main gamma-ray emission (≈ 80.6 keV). Using the new 166Ho activity standard and the well-calibrated, high-energy resolution HPGe detector, both available at ENEA-INMRI, a new determination of several 166Ho gamma-ray emission intensities, Iγ, was performed with low uncertainty. The new Iγ values contributed to the Decay Data Evaluation Project.

Sustainable extraction and conservation of soil resources: New insights through Natural Gamma-ray Spectrometry based Proximal Sensing Method.

Soil is one the most extracted natural raw materials. The vast expanses of fertile alluvial soils of the Indo Gangetic Plains have long remained as abundant soil resource pool for brick manufacturing and construction sectors. Unmonitored continuous removal of soil is reported to cause depletion of soil reserves, loss of soil fertility and affect crop yield. Excavation and removal of soil from isolated patches of land creates low lying and elevated degraded areas which disrupts normal crop cultivation pattern. Natural gamma-ray spectrometry (NGS) can be used as a non-destructive and rapid geophysical sensing method, for identification and delineation of areas with suitable soils. During this work brick kiln areas were visited to understand soil's availability and extraction pattern. NGS measurements of samples from soil profiles were carried out to find if gamma-ray intensities varied with soil clay content. Soil texture and plasticity of the same samples were obtained following standard testing procedures. Winkler and Plasticity charts were used to assess suitability of the soils. A strong linear relationship between gamma-ray potassium (K) intensity and clay contents of soil profile samples (R2 = 0.88) was observed. NGS based devices can be used to scan soil samples rapidly and log shallow depth boreholes in grid sampling design. The gathered spectral gamma-ray data can be then used to predict and generate high resolution 3D models of soil properties, based on which resource areas of suitable soils can be delineated for long term soil extraction without affecting cultivated areas. This will help in delineating areas restricted for soil extraction, which will not only make soil mining sustainable but also address soil conservation by setting aside large cultivated fertile soil areas untouched. Adopting NGS methods will prevent unsystematic removal of fertile soil and creation of degraded lands. This will ultimately result in efficient soil resource management.

Evaluation of radioactivity concentration in farm fresh milk and concomitant dose to consumer.

In this study, activity concentrations of natural radionuclides in 28 raw milk samples collected from different dairy farms in Dhaka city of Bangladesh were measured using a high-purity germanium (HPGe) detector for the first time. The activity concentration of 226Ra, 232Th, and 40K in the investigated fresh milk samples ranged from BDL (Below detection level) to 26 ± 1.6 Bq/kg, BDL to 11.7 ± 3.3 Bq/kg and 101 ± 17 to 384 ± 32 Bq/kg, respectively. No artificial radionuclides were found in the investigated samples. Present results show inline within the range of available data in the literature. Annual committed effective doses were estimated following the consumption characteristics of raw milk by city population, values are found within the limiting range recommended by international organizations due to consumption of foodstuffs. Additionally, real-time gamma-ray dose rate in the farms/sampling locations was found in the range of 0.12 ± 0.01-0.20 ± 0.01 µSv/h by using a digital gamma survey meter (Gamma Scout) and the calculated maximum annual effective dose due to outdoor absorbed dose was found to be 0.25 mSv/y, which shows lower than the United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR) recommended limit of 2.4 mSv/y. This study indicates that the concentration of radionuclides in the farm fresh milk of Dhaka city does not pose any unwanted risk to public health, and it is safe to consume by both children and adults with the current intake level.

Absolute emission intensities of the gamma rays from the decay of 224Ra and 212Pb progenies and the half-life of the 212 Pb decay.

Absolute gamma-ray emission intensities for 36 characteristic gamma rays from the decay of 224Ra, 212Pb, and their progeny were determined by measuring sources calibrated for activity by means of primary methods based on well-defined high-purity germanium (HPGe) detectors at both NIST and NPL. Results from the two laboratories agree with recent data evaluations, except for gamma rays with low emission intensities. The decay schemes have been re-balanced based on the new results. In addition, the half-life for 212Pb was measured using several HPGe detectors, ionization chambers, and a well-type NaI(Tl) detector.

Upscaling ground-based backpack gamma-ray spectrometry to spatial resolution of UAV-based gamma-ray spectrometry for system validation.

Advances in the development of gamma-ray spectrometers have resulted in devices that are ideal for use in conjunction with the increasingly reliable systems of autonomously flying uncrewed aerial vehicles (UAVs) that have recently become available on the market. Airborne gamma-ray spectrometry (GRS) measurements have many different applications. Here, the technique is applied to a former uranium mining and processing site, which is characterized by relatively low specific activities and, hence, low count rates, requiring relatively large detectors and correspondingly big size UAVs. The future acceptance of the use of such UAV-based GRS systems for radionuclide mapping depends on their ability to measure absolute specific activities of natural radionuclides such as U-238 in near-surface soil that are consistent with the results of established and proven ground-based systems. To determine absolute specific activities on the ground, the gamma radiation data from airborne detectors must be corrected for attenuation caused by the flight altitude above ground. In recent years, mathematical procedures for altitude correction have been developed, that are specifically tailored to the working range of several tens of meters typical for UAVs. However, very limited experimental validation of these theoretical approaches is available. A very large dataset consisting of about 3000 UAV-based and 19,000 backpack-based measurements was collected at a low-grade uranium ore dump in Yangiabad, Uzbekistan. We applied different geostatistical interpolation methods to compare the data from both survey techniques by upscaling backpack data to airborne data. Compared to backpack systems, UAV-based systems have lower spatial resolution, so measurements average over larger areal units (or in geostatistical terminology: "spatial support"). Taking into account the change in spatial support, we illustrate that (1) the UAV-based measurements show good agreement with the upscaled backpack measurements and that (2) UAV surveys provide good delineation of contrasts of the relatively smooth U-238 specific activity distribution typical for former uranium mining and processing sites. We are able to show that the resolution of UAV-based systems is sufficient to map extended uranium waste facilities.

A benchmark for Monte Carlo simulations in gamma-ray spectrometry Part II: True coincidence summing correction factors.

The goal of this study is to provide a benchmark for the use of Monte Carlo simulation when applied to coincidence summing corrections. The examples are based on simple geometries: two types of germanium detectors and four kinds of sources, to mimic eight typical measurement conditions. The coincidence corrective factors are computed for four radionuclides. The exercise input files and calculation results with practical recommendations are made available for new users on a dedicated webpage.

Latent variable modeling of gamma-ray background in repeated measurements.

We propose a novel approach for background subtraction in repeated gamma-ray spectrometric measurements. This entirely data-driven method eliminates the need for Monte Carlo detector simulation. To accomplish this, we utilized the framework of Latent Variable Modeling, incorporating various matrix factorization techniques and artificial neural networks. Subsequently, we applied this method to estimate radionuclide activity through spectrum unmixing. Significant improvements in sensitivity, surpassing traditional methods, were observed for the test case scenario of aerosol filter measurements.

A novel method to estimate the dead layer of HPGe detector for Monte Carlo FEPE computation.

In this study, a novel method to determine the surface and lateral dead layers of p-type HPGe detector is proposed to compute the full energy peak efficiency (FEPE). The method employed standard radioactive point sources 241Am, 133Ba and FEPE measurement at low energies to estimate the thickness of frontal and lateral dead layers. The method is simple to apply, requires only two standard radioactive sources to estimate the optimum thickness of frontal and lateral dead layers. The proposed method is validated by measuring the efficiency of various point sources and a volume source in the energy range from 59 to 1408 keV. The measured efficiencies agree to simulation with relative deviation less than 4.0% at each energy. The proposed detector model enables to calibrate the detector for environmental radioactivity measurement without standard volume sources.

Towards a radon-in-water primary standard at LNHB.

Despite widespread radon-in-water measurements, no primary radon-in-water standards currently exist. This work aims to bridge this gap by developing a system to produce radon-in-water reference materials. The system relies on cryogenic, loss-free transfer of radon, which is standardized through defined solid angle measurements, to a radon standard in water. It allows for preparation of liquid scintillation and gamma-ray spectrometry samples with traceable radon-in-water concentrations. The system's design, functionality, and the results of pilot performance tests are described.

Natural gamma-ray spectrometry as a rapid sensing method for detecting variations in soil shrinking and cracking behaviour: An application case study.

Soils which develop desiccation cracks after drying are unsuitable for the making of earthenware. The present work was carried out to demonstrate the use of Natural Gamma-ray Spectrometry (NGS) as a rapid sensing method to detect the variation of cracking behaviour and types of clay dominant in soil using samples collected from the study region. Natural gamma-ray intensities due to potassium (K) and equivalent thorium (eTh) radioisotopes present in soil were recorded using an NGS device. Circular soil cakes of set diameter were sun-dried to find shrinking and cracking variations. Other tests included measurement of particle size distribution, Atterberg indices, basic soil physico-chemical properties, exchangeable cation contents using ICP-OES and XRD identification of clays. 6 soil varieties were identified from the distribution of data points in the binary plots of gamma-ray potassium (GR-K) and thorium (GR-eTh) counts per sec (C/s). Variation of GR-K was observed to be wider (2.14 C/s to 2.54 C/s) than GR-eTh (0.44 C/s to 0.63 C/s). The measured GR-K counts reflect changes in illite content. The soils displayed 3 categories of shrinking and cracking behaviour. The soil variety which displayed maximum mild shrinkage without fine desiccation cracks on the set surface area has the highest GR-K counts. The soil shrinking and cracking variations were not clearly defined by the classification based on the texture and plasticity chart, though the latter indicated dominant smectites. A strong linear relationship between GR-K and exchangeable K (R2 = 0.84) indicates K+ contribution mainly from illite and dominance of other clay types in outliers. Higher levels of polyvalent cations known for binding clay aggregates were observed in the non-cracking soils. Concomitant higher GR-K levels indicate that shrinking soils lacking fine desiccation cracks are associated with fluvial sediments of the recent past with parental mica. This research concludes that NGS-based portable devices can be used for rapid sensing of soils to detect variation in shrinking and cracking behaviour and dominant clay type and thus can be used for identification of soil suitable for earthenware making.

Online spectral unmixing in gamma-ray spectrometry.

We introduced in a previous paper a time-dependent full-spectrum analysis algorithm speeding up the estimation of the activity of the radionuclides present in a sample. In this paper, we present a new version of the algorithm allowing online estimation. It uses only on a buffer of few segments while keeping the time information by using a time dependent regularization, thus reducing the size of the data matrices and the length of the processing of each iteration. The algorithm is optimized and tested on both simulated and measured spectra of aerosol samples.

226Ra measurement via gamma-ray spectrometry of 222Rn progeny - quantification of radon losses from sample capsules.

Radium-226 detection in sediment samples is generally executed by means of gamma-ray spectrometry. Data evaluation relies (besides the 186.2 keV 226Ra gamma peak) on the combined analysis of major gamma peaks that are produced by the short-lived radon (222Rn) daughters 214Pb and 214Bi. Precondition for this detection approach is equilibrium decay of all members of the decay chain between 226Ra and 214Bi. In closed systems, this equilibrium is reached after about five half-lives of 222Rn (19 days). However, a closed system can only be guaranteed if the capsule which contains the sample prevents diffusive escape of radon. Such radon-tightness cannot be guaranteed for a wide range of plastic materials. Due to its polymer structure, plastic material generally tends to allow radon diffusion and hence radon loss from the sample resulting in a disturbance of the required decay equilibrium. The paper introduces an approach that allows quantifying radon loss from sample capsules by direct radon measurements using mobile radon detection equipment. The experimental findings are supported by theoretical considerations. An examined alternative approach based on the offset of the 186.2 keV data point from an efficiency function that is calculated exclusively from short-lived radon progeny peaks in the gamma-ray spectrum did not prove to be applicable due to a lack of supporting peaks in the low-energy section of the spectrum.

Measurement of Cumulative fission product yields on 235U induced by 2.8 MeV neutrons.

Off-line gamma-ray spectrometry was used to accurately measure the Cumulative fission product yields (CFPYs) of fission products in the 235U (n, f) reaction induced by 2.8 MeV neutrons. The 2.8 MeV quasi-monoenergetic neutron beam was produced by the CPNG-600 Cockcroft Walton accelerator at the China Institute of Atomic Energy （CIAE）and the gamma spectra were measured by the HPGe γ-ray Spectrometer. After fully considering and revising the sources of uncertainty, high-precision CFPYs of 4 fission products were obtained. This study has important applications in reactor design and operation and is conducive to the establishment of an evaluated nuclear database.

Influence of phosphate fertilizers on the radioactivity of agricultural soils and tobacco plants in Kenya, Tanzania, and Uganda.

Three brands of NPK fertilizers that contain variable concentrations of natural radioactivity are commonly used in tobacco plantations in Kenya, Tanzania, and Uganda. Tobacco plants are known for hyper-accumulation of natural radionuclides, particularly 238U. This study investigated if the elevated radioactivity in phosphate fertilizers could enhance radioactivity in soils and tobacco plant leaves. The 232Th, 238U, and 40K radionuclide levels in NPK-fertilized soils and tobacco leaves were measured using gamma-ray spectroscopy. The research included a one-year reference experiment with tobacco growing in plots, a ten-year semi-controlled experiment in well-managed tobacco farms, and a field survey of radioactivity in soils and tobacco leaves at three traditional tobacco fields in Migori (Kenya), Urambo (Tanzania), and Kanungu (Uganda). The findings demonstrated that soils and tobacco leaves exposed to NPK fertilizers with increased radioactivity had activity concentrations of 232Th, 238U, and 40K that were considerably higher (at all sites) than in the control samples (with no use of NPK fertilizers). As the continued application of NPK fertilizers raises concentrations of 232Th, 238U, and 40K in agricultural soils, the study assessed radiological risks for humans from exposure to agricultural soils enriched with phosphate fertilizers, and it was found to be below the exposure limit of 1 mSvy-1 suggested by the International Commission on Radiological Protection (ICRP). However, tobacco consumers, both by snuffing and smoking, may face significant radiological risks, as the snuffing and smoking resulted in effective doses that were 2.41 to 6.53 and 1.14 to 2.45 times greater than the average yearly dose that the general public receives from inhalation of natural radionuclides (United Nations Scientific Committee on Atomic Radiations estimates). Furthermore, the results indicate that the lifetime excess cancer risk for tobacco snuffers and smokers ranged from 5 × 10-5 to 24.48 × 10-3 and 2.0 × 10-5 to 9.18 × 10-3, respectively. The influence of phosphorus-derived fertilizer containing relatively high natural radioactivity, potential human radiation exposure, and radiological risk due to gamma radionuclides is estimated and discussed. The results reveal that applying phosphate fertilizers enhances natural radioactivity in soil and is subsequently influenced by soil to tobacco plant uptake. Therefore, the study recommends that countries use fertilizers with lower radionuclide content to conserve soil quality and reduce gamma-emitting radionuclides in tobacco plants.

Evaluating the intensity of the 803-keV γ ray of 210Po using a 4παß(LS)-γ(HPGe) measurement system.

The absolute intensity for the 803-keV γ ray of 210Po was evaluated by α-γ coincidence technique. A liquid sample with a known amount of 210Po embedded in scintillation fluid was measured in a coincidence-based system that comprises a Liquid Scintillator (LS) detector and a High-Purity Germanium (HPGe) detector. A photo-reflector assembly that contains the 210Po sample provides 100% efficiency for detecting the α particles. The combination between the HPGe and the LS detectors allows to reject non-coincident α-γ events while maintaining high resolution γ spectroscopy. Consequently, the faint 803-keV photopeak from 210Po could be observed in a background-free environment, and its intensity could be evaluated with good accuracy. Sample measurements were carried out over nine months to gather statistics and verify the reliability of the experimental procedure. The absolute intensity of the 803-keV line was found to be (1.22 ± 0.03) × 10-5, in excellent agreement with the adopted value in a recent data compilation and consistent with previous experimental works.

A new efficiency calibration methodology for different atmospheric filter geometries by using coaxial Ge detectors.

The study of the different pollutants present in atmospheric aerosols such as trace elements and radionuclides is essential to assess the air quality. To analyze the particulate matter (PM), atmospheric filters with different dimensions and geometries (rectangular, circular, slotted, and square filters) are usually employed. Regarding the pollutants existing in atmospheric aerosols, radionuclides are usually analyzed due to their multiple applications such as either in the environmental radiological control or as tracers of atmospheric processes. Therefore, this study aims to develop a new and general methodology to calibrate in efficiency coaxial Ge detectors to properly determine radionuclides present in the PM by gamma-ray spectrometry for several filter types. For this, granular certified reference materials (CRM) containing only natural radionuclides (238U-series, 232Th-series, and 40 K) were selected. Several granular solid CRMs were chosen allowing us to reproduce the same PM deposition geometry and to assure the homogeneity of the added CRMs. These are the main advantages in relation to the typical methods that use liquid CRMs. Furthermore, for filters whose surfaces are relatively large, they were cut in several pieces and placed one on top of the other, achieving the same geometry than the PM deposited onto the filter. Then, the experimental full-energy peak efficiencies (FEPEs) were obtained for each energy of interest (Eγ) and they were fitted versus Eγ, finding a general FEPE function for each filter type. Finally, this methodology was validated for both natural and artificial radionuclides (from 46 to 1332 keV) by using different filter types employed in proficiency test exercises, obtaining |zscore|< 2 for all cases. Supplementary Information: The online version contains supplementary material available at 10.1007/s11869-023-01336-x.

Chemical separation and measurement of platinum activation products.

A method has been developed to purify and measure platinum radioisotopes in the presence of fission products and environmental constituents. The method uses a combination of cation exchange and anion exchange chromatography and selective precipitation steps to remove other radioisotopes from the sample. The addition of stable platinum carrier allows for a gravimetric determination of the chemical yield of the procedure. Overall, the method is fast, simple, and potentially applicable for rapid turnaround of unknown samples. Using this method, multiple platinum radioisotopes were measured in two different irradiation experiments. The measured ratios of the platinum radioisotopes clearly reflect the neutron spectrum of the irradiation, suggesting that platinum radioisotopes could be valuable signatures in nuclear forensic analyses.

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.

Natural and artificial radioactive pollution in sediment and soil samples of the Bosphorus, Istanbul.

This study focused on the determination of natural (238U, 232Th, and 40K) and artificial (137Cs) radionuclide concentrations both in 55 sediment samples collected from various depths in the Bosphorus and 5 soil samples from the coastline of the Bosphorus, Istanbul, using gamma-ray spectrometry with an HPGe detector. The mean activity concentrations of natural 238U, 232Th, and 40K and anthropogenic 137Cs were determined to be 11.41 ± 0.21 Bq kg-1, 6.87 ± 0.16 Bq kg-1, 369.61 ± 3.41 Bq kg-1, and 6.54 ± 0.11 Bq kg-1, respectively, in the sediment samples. The average activity concentrations of 238U, 232Th, 40K, and 137Cs radionuclides in the soil samples were also measured to be 11.65 ± 0.18 Bq kg-1, 9.55 ± 0.15 Bq kg-1, 369.43 ± 3.09 Bq kg-1, and 4.57 ± 0.09 Bq kg-1, respectively. Radiological contour maps based on the activity concentrations of natural and artificial radionuclides in the sediment samples for the Bosphorus, Istanbul, were created. The total annual effective doses due to soil samples were calculated to be 34.58 µSv y-1.