Gamma spectrometric measurements to determine the isotopic composition and total uranium mass in UO2 pellets (D = 7.5 mm; H = 3.5 mm, rho = 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.
Recycling and conventional reuse of lead materials and structures originating from controlled areas in nuclear facilities rely on historical knowledge and well selected characterization procedures. At the SCK•CEN, one of these procedures involves performing high-resolution gamma-ray spectrometry measurements on several cylindrical shaped test samples (50 mm diameter and approximately 5 mm thickness), obtained during the lead melting campaigns. The high density (11.3 g/cm³) of these samples is a challenge for radionuclide analysis by gamma-ray spectrometry since no such calibration sources nor reference materials are available. We used the efficiency transfer procedure, relying on regular standard sources available in our laboratory, to set up calibrations for this specific counting geometry. The method proves to be fit for purpose.
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.
Inversion of in situ borehole gamma spectrometry data is a faster and relatively less laborious method for calculating the vertical distribution of radioactivity in soil than conventional soil sampling method. However, the efficiency calculation of a detector for such measurements is a challenging task due to spatial and temporal variation of the soil properties and other measurement parameters. In this study, the sensitivity of different soil characteristics and measurement parameters on simulated efficiencies for a 662 keV photon peak were investigated. In addition, a Bayesian data inversion with a Gaussian process model was used to calculate the activity concentration of 137Cs and its uncertainty considering the sources of uncertainty identified during the sensitivity analysis, including soil density, borehole radius, and the uncertainty in detector position in the borehole. Several soil samples were also collected from the borehole and surrounding area, and 137Cs activity concentration was measured to compare with the inversion results. The calculated 137Cs activity concentrations agree well with those obtained from soil samples. Therefore, it can be concluded that the vertical radioactivity distribution can be calculated using the probabilistic method using in situ gamma spectrometric measurements.
The efficiency transfer procedure from a geometry where a volume source was placed directly on the endcap of a germanium detector to three different distant geometries was carried out using the EFFTRAN code. One of these distant geometries included absorbers consisting of poly(methyl methacrylate). The efficiency transfer to this geometry therefore had to be realized as a two-stage transfer, since a direct efficiency transfer is not possible using EFFTRAN in such a case. Efficiency transfer to all three distant geometries yielded results which can be considered as fit-for-purpose in e.g. most of the applications of gamma ray spectrometry.
A reliable detector model is needed for Monte Carlo efficiency calibration. A LaBr3(Ce) detector model was optimized and verified using different radioactive sources (241Am, 133Ba, 137Cs, 60Co and 152Eu) and geometries (point, extended and surface). PENELOPE and MCNP were used for Monte Carlo simulations. A good agreement was observed between simulated and experimental full energy peak efficiencies (FEPE) as their mean relative difference was 2.84% ± 1.93% and 2.79% ± 1.99% for PENELOPE and MCNP simulation, respectively. The differences between simulated FEPEs of two Monte Carlo codes were negligible except for low energies (< 100 keV).
The minimum detectable activity (MDA) for gamma spectrometric measurements was studied as a function of filling height for two detectors having different background characteristics and for two sample matrices: a water sample with a low content of natural radionuclides, and zircon sand, with high activities of uranium and thorium. The zircon sand is also a material in which the self-attenuation of low-energy gamma photons will be high. The results show that for the water sample it is always favourable to completely fill the sample container. However, due to the inherent content of naturally occurring radionuclides in the zircon sand the MDA may not necessarily improve with the filling height, since an increased amount of sample will increase the background in the spectrum as well.
This article presents yearly mean concentrations of cosmogenic radionuclides 7Be and 22Na occurring in dry and wet depositions (fallout) and aerosols. Time dependencies negatively correlated with the yearly mean number of sunspots. Activity concentrations of 7Be and 22Na in aerosols in the surface air had a correlation of near-unity. 7Be in aerosols exhibited a smoother time dependence than 22Na, implying that the production of 22Na is more sensitive to the solar activity than the production of 7Be. The effect of the measured doses on the general population through internal and external exposure to radiation from cosmogenic radionuclides was small.
True coincidence summing correction factors for 133 Ba, 152 Eu and 125 Sb were determined experimentally for a small volume source and compared with correction factors obtained with three softwares (EFFTRAN-X, GESPECOR and VGSL). The radionuclides investigated have a relatively challenging decay scheme and their spectra are known to suffer from losses due to summation (γ–γ, γ–X and X–X) when measured at close distances on a HPGe detector sensitive to low energy photons. This study shows that the softwares were in good agreement with each other and the experimental data and the calculated activity was consistent with the activity in the volume source.
An internal consistency test of the calculation of coincidence-summing correction factors FC for volume sources is presented. The test is based on exact equations relating the values of FC calculated for three ideal measurement configurations. The test is applied to a number of 33 sets of FC values sent by 21 teams. Most sets passed the test, but not the results obtained using the quasi-point source approximation; in the latter case the test qualitatively indicated the magnitude of the bias of FC.
In situ gamma spectrometry is a widely applied analysis technique for the determination of radioactivity levels in soil. Compared to traditional laboratory analysis of soil samples, in situ techniques offer a quick and low-cost way of obtaining accurate results from on-site measurements. However, although the technique is well-known, the dependence of in situ gamma spectrometry on complex and time-consuming calibration procedures as well as in-depth knowledge of the geometric distribution of the source in the ground deters many potential users from employing it in their routine work. Aiming to alleviate this issue, a software tool named InSiCal (In Situ gamma spectrometry Calculator) has been developed to make in situ gamma spectrometry more accessible to both experts and non-experts in the field. This is done by simplifying and streamlining both calibration and activity calculation through a simple and intuitive graphical user interface. Testing in real field conditions show that InSiCal is capable of yielding results which are in very good agreement with soil sample analyses, and that the results may be obtained using different detector types (HPGe, NaI, LaBr and CZT). Overall, InSiCal, provides results which are comparable in accuracy to laboratory measurements, indicating that it fulfills its purpose successfully.
The isotopic composition of uranium was measured using high resolution gamma spectrometry. Two acid solutions and two samples in the form of UO2 pellets were measured. The measurements were done in close geometries, i.e. directly on the endcap of the high purity germanium detector (HPGe). Applying no corrections for count losses due to true coincidence summing (TCS) resulted in up to about 40% deviation in the abundance of 235U from the results obtained with mass spectrometry. However, after correction for TCS, excellent agreement was achieved between the results obtained using two different measurement methods, or a certified value. Moreover, after corrections, the fitted relative response curves correlated excellently with simulated responses, for the different geometries, of the HPGe detector.
The gamma spectrometry of environmental samples poses a series of specific problems for the practitioner. The determination of full energy peak efficiencies is, in the case of environmental samples, one of the greatest challenges. In this paper, the calibration of two HPGe detectors for environmental samples in Marinelli beakers was performed using the newly developed MEFFTRAN software. The results obtained with MEFFTRAN were compared to the experimental efficiencies measured using the calibration sample produced at the Laboratory for Radiation and Environment Protection, Institute for Nuclear Sciences Vinca, Belgrade, in order to confirm the validity of the calculation. It is shown that calculated and experimental efficiencies are in good agreement with the discrepancies from -3.9% to +1.5%. The results were also validated by measuring secondary reference materials provided by the IAEA within several interlaboratory proficiency tests. The activity concentration of the radionuclides in the secondary reference materials was determined using the efficiency obtained by MEFFTRAN and compared with the target value given by the IAEA. All the results in materials provided by the IAEA were acceptable except one, proving that MEFFTRAN produces satisfactory results.
We present a numerical fitting method for transmission data that outputs an equivalent sample composition. This output is used as input to a generalised efficiency transfer model based on the EFFTRAN software integrated in a LIMS. The procedural concept allows choosing between efficiency transfer with a predefined sample composition or with an experimentally determined composition based on a transmission measurement. The method can be used for simultaneous quantification of low-energy gamma emitters like (210)Pb, (241)Am, (234)Th in typical environmental samples.
The aim of this study was to check for equivalence of computer codes that are capable of performing calculations of true coincidence summing (TCS) correction factors. All calculations were performed for a set of well-defined detector parameters, sample parameters and decay scheme data. The studied geometry was a point source of (133)Ba positioned directly on the detector window of a low-energy (n-type) detector. Good agreement was established between the TCS correction factors computed by the different codes.
A laboratory exercise for calculation of true coincidence summing correction factors as well as calculating the effect of deviations between sample and standard source (filling height) was developed. This laboratory exercise was held in a masters course in nuclear chemistry the first time during fall 2013. The aim of the exercise was to high-light the importance of correcting for biases due to different systematic effects in gamma spectrometric measurements.
Four calculation codes were implemented on experimental data to calculate corrections of common systematic effects within high resolution gamma spectrometry. The detector parameters were sparsely optimized to imitate the usage that can be expected from personnel with limited experience. The transfer of the efficiency from the calibration geometry (60 ml, density 1.0 g/cm 3 ) to 200 ml geometry (density 1.5 g/cm 3 ) failed with all codes, which was discouraging. However, a majority of the other corrected activities deviated with less than 10 % from the reference activity values, even for density corrections or when corrections had been calculated for new source-detector-geometries. Smaller deviations, around 5 % or less, were achieved when corrections were done within the calibrated geometry. This shows a robustness of the calculation codes even if the in-data is not perfectly optimized.
Determination of full energy peak efficiency is one of the most important tasks that have to be performed before gamma spectrometry of environmental samples. Many methods, including measurement of specific reference materials, Monte Carlo simulations, efficiency transfer and semi empirical calculations, were developed in order to complete this task.Monte Carlo simulation, based on GEANT4 simulation package and EFFTRAN efficiency transfer software are applied for the efficiency calibration of three detectors, readily used in the Environment and Radiation Protection Laboratory of Institute for Nuclear Sciences Vinca, for measurement of environmental samples. Efficiencies were calculated for water, soil and aerosol samples. The aim of this paper is to perform efficiency calculations for HPGe detectors using both GEANT4 simulation and EFFTRAN efficiency transfer software and to compare obtained results with the experimental results. This comparison should show how the two methods agree with experimentally obtained efficiencies of our measurement system and in which part of the spectrum do the discrepancies appear. The detailed knowledge of accuracy and precision of both methods should enable us to choose an appropriate method for each situation that is presented in our and other laboratories on a daily basis. (C) 2014 Elsevier B.V. All rights reserved.
Resumen del poster presentado a la 3rd International Conference on Radioecology and Environmental Radioactivity celebrada en Barcelona (Espana) del 7 al 12 de septiembre de 2014.
The half-life of 176Lu was determined by measuring the 176Lu activity in metallic lutetium foils. Three different HPGe-detectors located 225 m underground were employed for the study. Measurements using the sum-peak method were performed and resulted in an average massic activity of (52.61±0.36) Bq g−1. The foils were of natural isotopic abundance so using the massic activity and the value of the natural isotopic abundance of (2.59±0.01)%, a half-life of (3.722±0.029)×1010a could be calculated.