Calibration of HPGe detectors using certified reference materials of natural origin

The feasibility of using certified reference materials for the full energy efficiency calibration of p-type coaxial high-purity germanium detectors for the determination of radioactivity in environmental samples is discussed. The main sources of uncertainty are studied and the contributions to the total uncertainty budget for the most intense gamma lines are presented. The correction factors due to self-absorption and true coincidence summing effects are discussed in detail. The calibration procedure is validated for natural and artificial radionuclide determination in different matrices through an internal cross-validation and through the participation in a world-wide open proficiency test

Radiological characterization of granitoid outcrops and dimension stones of the Variscan Corsica-Sardinia Batholith

This study focuses on the radiological characterization of granitoid outcrops and dimension stones using in situ gamma-ray spectrometry. Extensive measurements were performed on 210 granitoid outcrops of the Corsica-Sardinia Batholith. The large statistical sample allowed us to improve the analysis by considering a log-normal distribution of radioelements and propagating the uncertainties using Monte Carlo method. The activity concentrations of 40K, 226Ra (238U) and 232Th in C-SB area were 1,177 −304 +408 , 60 −23 +36 and 69 −25 +38 Bq/kg (at 1σ uncertainty). The median abundance of K, U and Th on the Variscan C-SB was higher than the average values of the upper continental crust and was comparable with Variscan belt. This corresponds to an outdoor absorbed dose rate of 124 −26 +33 nGy/h at 1σ uncertainty which is 3σ higher than the population-weighted average absorbed dose rate (60 nGy/h). Seven commercial granites (Rosa Beta, Ghiandone, Giallo San Giacomo, Rosa Cinzia, Grigio Malaga, Bianco Sardo and Grigio Perla) were investigated to characterize their radiological hazard through 147 measurements taken in 73 extractive quarries. All of the commercial granites were categorized as A2 material based on their activity concentration indices, excluding (at the 3σ level) any restriction on their utilization as superficial materials. Rosa Beta, Grigio Malaga, Grigio Perla and Bianco Sardo can also be used as bulk materials as they can be included in the A1 category. In the case of Ghiandone, Giallo San Giacomo and Rosa Cinzia, we are confident of an A1 classification only at the 1σ level

Advanced gamma-ray spectrometry for environmental radioactivity monitoring

The environmental radioactivity monitoring programs start in the late 1950s of the 20th century following the global fallout from testing of nuclear weapons in the atmosphere, becoming a cause of concern regarding health effects. Later, the necessity of world industrialization for new energy sources led to develop national plans on electricity production from nuclear technology, initializing in this context world wide exploration for fuel minerals: uranium exploration gained a particular attention in late 1940's in USA, Canada and former USSR and in 1951 in Australia with respective national plans. Nowadays there are about 440 nuclear power plants for electricity generation with about 70 more NPP under construction giving rise to the nuclear emergency preparedness of a large number of states (like Radioactivity Environmental Monitoring (REM) data bank and EUropean Radiological Data Exchange Platform (EURDEP). Furthermore, a lot of applications in the field of geosciences are related to the environmental radioactivity measurements going from geological mapping, mineral exploration, geochemical database construction to heat -flow studies. Gamma-ray spectroscopy technique is widely used when dealing with environmental radioactivity monitoring programs. The purpose of this work is to investigate the potentialities that such a technique offers in monitoring radioactivity concentration through three different interventions in laboratory, in-situ and airborne measurements. An advanced handling of gamma-ray spectrometry method is realized by improving the performances of instruments and realizing and testing dedicated equipments able to deal with practical problems of radioactivity monitoring. For each of these gamma-ray spectrometry methods are faced also the problems of calibration, designing of monitoring plans and data analyzing and processing. In the first chapter I give a general description for the common radionuclides present in the environment having a particular interest for monitoring programs. Three categories of environmental radionuclides classified according to their origin as cosmogenic, primordial and man-made are discussed. The cosmic rays continuously produce radionulides and also direct radiation, principally high energetic muons. Cosmogenic radionuclides are originated from the interaction of cosmic rays with stable nuclides present in the Earth’s atmosphere. Primordial radionuclides are associated with the phenomenon of nucleosynthesis of the stars and are present in the Earth’s crust. Man-made radionuclides commonly present in natural environments are principally derived from radioactive fallout from atmospheric nuclear weapons testing and peaceful applications of nuclear technology like nuclear power plants for electricity generation and the associated nuclear fuel cycle facilities. A relevant contribution, generally with local implication comes from the so called non-nuclear industries which are responsible for technologically enhancement of natural radioelements producing huge amounts of naturally occurring radioactive materials (NORM/TENORM). In the second chapter is described a homemade approach to the solution of the problem rising in monitoring situations in which a high number of samples is to be measured through gamma-ray spectrometry with HPGe detectors. Indeed, in such cases the costs sustaining the manpower involved in such programs becomes relevant to the laboratory budget and sometimes becomes a limitation of their capacities. Manufacturers like ORTEC® and CANBERRA produce gamma-ray spectrometers supported by special automatic sample changers which can process some tens of samples without any human attendance. However, more improvements can be done to such systems in shielding design and detection efficiency. We developed a fully automated gamma-ray spectrometer system using two coupled HPGe detectors, which is a well known method used to increase the detection efficiency. An alternative approach on shielding design and sample changer automation was realized. The utilization of two coupled HPGe detectors permits to achieve good statistical accuracies in shorter time, which contributes in drastically reducing costs and man power involved. A detailed description of the characterization of absolute full-energy peak efficiency of such instrument is reported here. Finally, the gamma-ray spectrometry system, called MCA_Rad, was used to characterize the natural radioactivity concentration of bed-rocks in Tuscany Region, Italy. More than 800 samples are measured and reported here together with the potential radioactivity concentration map of bed rocks in Tuscany Region. In the third chapter is described the application of portable scintillation gamma -ray spectrometers for in-situ monitoring programs focusing on the problems of calibration and spectrum analysis method. In-situ γ-ray spectrometry with sodium iodide scintillators is a well developed and consolidated method for radioactive survey. Conventionally, a series of self-constructed calibration pads prevalently enriched with one of the radioelements is used to calibrate this portable instrument. This method was further developed by introducing the stripping (or window analysis) described in International Atomic Energy Agency (IAEA) guidelines as a standard methods for natural radioelement exploration and mapping. We realized a portable instrument using scintillation gamma-ray spectrometers with sodium iodide detector. An alternative calibration method using instead well-characterized natural sites, which show a prevalent concentration of one of the radioelements, is developed. This procedure supported by further development of the full spectrum analysis (FSA) method implemented in the non-negative least square (NNLS) constrain was applied for the first time in the calibration and in the spectrum analysis. This new approach permits to avoid artifacts and non physical results in the FSA analysis related with the χ2 minimization process. It also reduces the statistical uncertainty, by minimizing time and costs, and allows to easily analyze more radioisotopes other than the natural ones. Indeed, as an example of the potentialities of such a method 137Cs isotopes has been implemented in the analysis. Finally, this method has been tested by acquiring gamma Ombrone -ray spectra using a 10.16 cm×10.16 cm sodium iodide detector in 80 different sites in the basin, in Tuscany. The results from the FSA method with NNLS constrain have been compared with the laboratory measurements by using HPGe detectors on soil samples collected. In the forth chapter is discussed the self-construction of an airborne gamma-ray spectrometer, AGRS_16.0L. Airborne gamma-ray spectrometry (AGRS) method is widely considered as an important tool for mapping environmental radioactivity both for geosciences studies and for purposes of radiological emergency response in potentially contaminated sites. Indeed, they have been used in several countries since the second half of the twentieth century, like USA and Canada, Australia, Russia, Checz Republic, and Switzerland. We applied the calibration method described in the previous chapter using well -characterized natural sites and implemented for the first time in radiometric data analysis FSA analysis method with NNLS constrain. This method permits to decrease the statistical uncertainty and consequently reduce the minimum acquisition time (which depend also on AGRS system and on the flight parameters), by increasing in this way the spatial resolution. Finally, the AGRS_16.0L was used for radioelement mapping survey over Elba Island. It is well known that the natural radioactivity is strictly connected to the geological structure of the bedrocks and this information has been taken into account for the analysis and maps construction. A multivariate analysis approach was considered in the geostatistical interpolation of radiometric data, by putting them in relation with the geology though the Collocated Cokriging (CCoK) interpolator. Finally, the potential radioelement maps of potassium, uranium and thorium are constructed for Elba Island

A century of oil and gas exploration in Albania: assessment of Naturally Occurring Radioactive Materials (NORMs)

Because potential Naturally Occurring Radioactive Materials (NORMs) generated from oil and gas extractions in Albania have been disposed without regulatory criteria in many decades, an extensive survey in one of the most productive regions (Vlora-Elbasan) has been performed. Among 52 gamma-ray spectrometry measurements of soil, oil-sand, sludge, produced water and crude oil samples, we discover that relatively low activity concentrations of 226Ra, 228Ra, 228Th and 40K, which are 23 +/- 2 Bq/kg, 23 +/- 2 Bq/kg, 24 +/- 3 Bq/kg and 549 +/- 12 Bq/kg, respectively, come from oil-sand produced by hydrocarbon extraction from molasses formations. The mineralogical characterization together with the 228Ra/40K and 226Ra/40K ratios of these Neogene deposits confirm the geological and geodynamic model that predicts a dismantling of Mesozoic source rocks. The average activity concentrations (+/- standard deviations) of the radium isotopes (226Ra, 228Ra) and of the 228Th and 40K radionuclides in soil samples are determined to be 20 +/- 5 Bq/kg, 25 +/- 10 Bq/kg, 25 +/- 9 Bq/kg and 326 +/- 83 Bq/kg, respectively. Based on these arguments, the future radiological assessment of other fields in the region can be strategically planned focusing on the oil-sands from molasses sediments. No disequilibrium in the 228Ra decay segment has been observed in soil, sludge and oil-sand samples within the standard uncertainties. After a detailed radiological characterization of the four main oilfields, we can conclude that the outdoor absorbed dose rate never exceeds the worldwide population weighted average absorbed dose rate in outdoor air from terrestrial gamma radiation.Comment: 21 pages, 5 figures, 2 tables, Chemosphere 201

Expected geoneutrino signal at JUNO

Constraints on the Earth's composition and on its radiogenic energy budget come from the detection of geoneutrinos. The KamLAND and Borexino experiments recently reported the geoneutrino flux, which reflects the amount and distribution of U and Th inside the Earth. The KamLAND and Borexino experiments recently reported the geoneutrino flux, which reflects the amount and distribution of U and Th inside the Earth. The JUNO neutrino experiment, designed as a 20 kton liquid scintillator detector, will be built in an underground laboratory in South China about 53 km from the Yangjiang and Taishan nuclear power plants. Given the large detector mass and the intense reactor antineutrino flux, JUNO aims to collect high statistics antineutrino signals from reactors but also to address the challenge of discriminating the geoneutrino signal from the reactor background.The predicted geoneutrino signal at JUNO is 39.7 $^{+6.5}_{-5.2}$ TNU, based on the existing reference Earth model, with the dominant source of uncertainty coming from the modeling of the compositional variability in the local upper crust that surrounds (out to $\sim$ 500 km) the detector. A special focus is dedicated to the 6{\deg} x 4{\deg} Local Crust surrounding the detector which is estimated to contribute for the 44% of the signal. On the base of a worldwide reference model for reactor antineutrinos, the ratio between reactor antineutrino and geoneutrino signals in the geoneutrino energy window is estimated to be 0.7 considering reactors operating in year 2013 and reaches a value of 8.9 by adding the contribution of the future nuclear power plants. In order to extract useful information about the mantle's composition, a refinement of the abundance and distribution of U and Th in the Local Crust is required, with particular attention to the geochemical characterization of the accessible upper crust.Comment: Slight changes and improvements in the text,22 pages, 4 Figures, 3 Tables. Prog. in Earth and Planet. Sci. (2015

first intercomparison among laboratories involved in cost action tu1301 norm4building determination of natural radionuclides in ceramics

Abstract This work describes the outcomes of the COST Action-TU1301 "NORM4Building" intercomparison on the determination of natural radioactivity in ceramics. Twenty-two laboratories involved in the intercomparison are evaluated for their performance using robust statistics. The reference values of 226 Ra ( 214 Bi and 214 Pb) are determined to be 122 ± 11 Bq kg −1 and 124 ± 14 Bq kg −1 , respectively and in secular equilibrium in the uranium chain while the reference values of 232 Th ( 228 Ac) is determined to be 61 ± 6 Bq kg −1 and that of 40 K was determined to be 955 ± 40 Bq kg −1 . Although the aim of the exercise was to determine the activity concentration of 226 Ra, 232 Th and 40 K and evaluation of the "Activity Concentration Index", laboratories were asked to report complete characterization of natural radionuclides. The results of this exercise pointed out a good performance among laboratories since the percentage of the acceptable results were above 90% for the radionuclides of interest. Based on these results, considering the systematic rejection of the results reported from a few laboratories we emphasize the need for quality control procedures

Determination of activity concentration of 210 Po in mussels ( Mytilus galloprovincialis ) from Butrinti Lagoon, Albanian Ionian coast

This study reports the activity concentration of 210Po in mussels (Mytilus galloprovincialis) from Butrinti Lagoon. The concentrations of 210Po in mussels collected in spring are found to be approximately twice higher than those collected in autumn, respectively 389.5 ± 16.9 and 227.4 ± 5.0 Bq kg−1 (d.w.). Hypothesis on factors affecting 210Po concentration in mussels are raised based on available studies. The annual effective ingestion dose due to 210Po intake was found to be comparable to other studies and varying from 74.2 ± 3.4 to 36.5 ± 1.0 µSv y−1

First characterisation of natural radioactivity in building materials manufactured in Albania

This study focuses on the radiological characterisation of building materials manufactured in Albania by using a high-resolution gamma-ray spectrometer. The average activity concentrations of (40)K, (226)Ra and (232)Th were, respectively, 644.1±64.2, 33.4 ± 6.4 and 42.2 ± 7.6 Bq kg(-1) in the clay brick samples and 179.7 ± 48.9, 55.0 ± 5.8 and 17.0 ± 3.3 Bq kg(-1) in the cement samples. The calculated activity concentration index (ACI), varied from 0.48±0.02 to 0.63±0.04 in the clay brick samples and from 0.29±0.03 to 0.37±0.02 in the cement samples. Based on the ACI, all of the clay brick and cement samples were categorised as A1 materials. The authors can exclude (at 3σ level) any restriction of their use as bulk materials

Reference worldwide model for antineutrinos from reactors

Antineutrinos produced at nuclear reactors constitute a severe source of background for the detection of geoneutrinos, which bring to the Earth's surface information about natural radioactivity in the whole planet. In this framework we provide a reference worldwide model for antineutrinos from reactors, in view of reactors operational records yearly published by the International Atomic Energy Agency (IAEA). We evaluate the expected signal from commercial reactors for ongoing (KamLAND and Borexino), planned (SNO+) and proposed (Juno, RENO-50, LENA and Hanohano) experimental sites. Uncertainties related to reactor antineutrino production, propagation and detection processes are estimated using a Monte Carlo based approach, which provides an overall site dependent uncertainty on the signal in the geoneutrino energy window on the order of 3%. We also implement the off-equilibrium correction to the reference reactor spectra associated with the long-lived isotopes and we estimate a 2.4% increase of the unoscillated event rate in the geoneutrino energy window due to the storage of spent nuclear fuels in the cooling pools. We predict that the research reactors contribute to less than 0.2% to the commercial reactor signal in the investigated 14 sites. We perform a multitemporal analysis of the expected reactor signal over a time lapse of 10 years using reactor operational records collected in a comprehensive database published at www.fe.infn.it/antineutrino.Comment: Slight changes and improvements in the text, added references. 17 pages, 6 figures, 8 tables; Physical Review D 201

A γ-Spectroscopy System for Atmospheric Radon Detection

Radon isotopes and their decay products cause most of the natural radioactivity in atmosphere at ground level (Jacobi, 1964; Altshuler et al., 1964; UNSCEAR, 1988, 1993; Porstendorfer, 1994; Kathren, 1998). 222Rn (Radon) and 220Rn (Thoron) enter the atmosphere from the Earths surface, where they are produced via radioactive decay of the precursors 238U and 232Th respectively. The major contribution to the natural radioactivity dose is from the inhalation of the daughters of this gas. They are attached to very fine particles (Bergamini et al., 1973; Porstendorfer, 1994; Mohammed et al., 2000) and deposit on the surface of the different parts of the respiratory system with a probability dependent on aerosol particle sizes (ICRP, 1994). The dynamics of the gas could be similar to that of the atmospheric particulate and the daily change in concentration can be correlated to it. The γ-rays produced by the Radon daughters come both from the earth surface and from the radon contained in the air. For a detector placed in a fixed position, the first contribution remains constant over the time while the second follows the change in gas concentration in air. In order to determine the two contributions a system composed by three sodium iodide detectors has been designed and installed on a tower at the LNL (Laboratori Nazionali di Legnaro). The aim of this project is to understand the behavior of γ emissions from ground surface at different altitudes and also to study the correlation between the atmospheric conditions, like the altitude of the atmosphere inversion layer, and the radon concentration in air. http://www.fe.infn.it/u/mantovani/CV/Proceedings/Bezzon_11b.pd