Analysis of 222Rn Surface Concentrations in the Basque Country (Spain): A Case Study of Heat Waves.

The objective of this study was to characterize radon concentrations registered in the Radiological Surveillance Network of the Basque country in relation to local meteorological parameters, and to determine its behaviour under heatwave events. For this purpose, radon measurements and meteorological parameters from June 2012 to June 2015 were analysed at two sites, Bilbao and Vitoria (northern Spain), in a region characterized by complex orography, causing large temporal and spatial variability in meteorological conditions. Yearly, seasonal, and diurnal cycle differences and similarities were investigated at both sites. The temporal evolution of radon concentration was analysed at both sites during the two heatwave periods officially identified by the State Meteorological Agency (8-11 August 2012 and 17-23 August 2012). The analysis revealed two different patterns of radon concentrations, in terms of both time and intensity, under this synoptic pattern, making it also possible to identify regional transport channels of radon concentrations between the two sites. This set of results evidences the adequate position of both stations to represent the spatial and temporal evolution of radiological variables continuously in this region.

Meteorological Approach in the Identification of Local and Remote Potential Sources of Radon: An Example in Northern Iberian Peninsula.

This paper presents a meteorological approach to identify local and remote sources driving the variability of surface daily radon concentrations. To this purpose, hourly 222Rn concentration and surface meteorological measurements, and air mass trajectories at Bilbao station (northern Iberian Peninsula) during the period 2017-2018 have been taken as reference. To investigate the potential transport pathways and potential 222Rn sources, the backward trajectory cluster analysis, trajectory sector analysis (TSA), and potential source contribution function (PSCF) are applied. On average, the diurnal 222Rn cycle shows the expected behaviour, with larger concentrations during the night and minimum concentrations during the daylight hours, with differences in the seasonal amplitudes. According to daily differences between maximum and baseline values, 222Rn daily cycles were grouped into six groups to identify meteorological conditions associated with each amplitude, and potential source areas and transport routes of 222Rn over Bilbao. The trajectory cluster and the TSA method show that the main airflow pathways are from the south, with small displacement, and the northeast, while the analysis of surface wind speed and direction indicates that the highest amplitudes of 222Rn concentrations are registered under the development of sea-land breezes. The PSCF method identified south-western and north-eastern areas highly contributing to the 222Rn concentration. These areas are confirmed by comparing with the radon flux map and the European map of uranium concentration in soil. The results have demonstrated the need in combining the analysis of local and regional/synoptic factors in explaining the origin and variability of 222Rn concentrations.

Harmonization and mapping of terrestrial gamma dose rate data in Belgium.

With several databases available, including two sets of in situ measurements of the ambient gamma dose rate and an airborne survey of K, Th, U in soil, Belgium is a favourable case for exploring the mapping methodology for terrestrial radiation. The first step is the harmonization of the different data sets, taking in situ measurements with an ion chamber as the reference. Corrections are necessary, based on the data themselves (a) to the measurements of permanent monitoring stations, (b) to the data calculated from airborne measurements of the soil activity, due in particular to the attenuation by the forest cover, and (c) to the other data calculated from the soil activity, due to the lower activity of the upper layer. After subtracting the cosmic contribution, a harmonized database of the terrestrial gamma dose rate (TGDR) based on 379 in situ measurements was built, together with a harmonized data set of 30134 TGDR values calculated from the concentrations of K, Th, U in soil deduced from the airborne survey. The two data sets are in good agreement with each other for all statistical characteristics that were examined like basic statistics, qq-plots, analysis of variance (ANOVA) or variograms, which validates the airborne-based data set by the link with in situ ion chamber measurements. ANOVA reveals the strong relation between TGDR and the soil class, which justifies the use of a soil map as the framework for developing the TGDR map. The variograms show the absence of residual spatial correlations within soil classes. The two harmonized TGDR data sets were mapped at the nodes of a kilometric grid by the moving average method within soil groups. There is a rather good agreement between the maps, confirming the equivalence between the two data sets and the validation of the airborne based one, which can obviously give more detail. After reducing the maps to a 10 km × 10 km grid, the two data sets were used to check the accuracy of the Belgian part of the European TGDR contained in the European Atlas of Natural Radiation.

Outdoor Radon as a Tool to Estimate Radon Priority Areas-A Literature Overview.

Doses from the exposure to outdoor radon are typically an order of magnitude smaller than those from indoor radon, causing a greater interest on investigation of the latter for radiation protection issues. As a consequence, assessment of radon priority areas (RPA) is mainly based on indoor radon measurements. Outdoor radon measurements might be needed to guarantee a complete estimation of radiological risk and may help to improve the estimation of RPA. Therefore, authors have analysed the available literature on outdoor radon to give an overview of outdoor radon surveys and potential correlation with indoor radon and estimation of RPA. The review has shown that outdoor radon surveys were performed at much smaller scale compared to indoor radon. Only a few outdoor radon maps were produced, with a much smaller density, covering a larger area, and therefore putting doubt on the representativeness of this data. Due to a large variety of techniques used for outdoor radon measurements and requirement to have detectors with a high sensitivity and resistance to harsh environmental conditions, a standardised measurement protocol should be derived. This is no simple endeavour since there are more applications in different scientific disciplines for outdoor radon measurements compared to indoor radon.

The assessment of local geological factors for the construction of a Geogenic Radon Potential map using regression kriging. A case study from the Euganean Hills volcanic district (Italy).

The assessment of potential radon-hazardous environments is nowadays a critical issue in planning, monitoring, and developing appropriate mitigation strategies. Although some geological structures (e.g., fault systems) and other geological factors (e.g., radionuclide content, soil organic or rock weathering) can locally affect the radon occurrence, at the basis of a good implementation of radon-safe systems, optimized modelling at territorial scale is required. The use of spatial regression models, adequately combining different types of predictors, represents an invaluable tool to identify the relationships between radon and its controlling factors as well as to construct Geogenic Radon Potential (GRP) maps of an area. In this work, two GRP maps were developed based on field measurements of soil gas radon and thoron concentrations and gamma spectrometry of soil and rock samples of the Euganean Hills (northern Italy) district. A predictive model of radon concentration in soil gas was reconstructed taking into account the relationships among the soil gas radon and seven predictors: terrestrial gamma dose radiation (TGDR), thoron (220Rn), fault density (FD), soil permeability (PERM), digital terrain model (SLOPE), moisture index (TMI), heat load index (HLI). These predictors allowed to elaborate local spatial models by using the Empirical Bayesian Regression Kriging (EBRK) in order to find the best combination and define the GRP of the Euganean Hills area. A second GRP map based on the Neznal approach (GRPNEZ) has been modelled using the TGDR and 220Rn, as predictors of radon concentration, and FD as predictor of soil permeability. Then, the two GRP maps have been compared. Results highlight that the radon potential is mainly driven by the bedrock type but the presence of fault systems and topographic features play a key role in radon migration in the subsoil and its exhalation at the soil/atmosphere boundary.

Validation of a database of mean uranium, thorium and potassium concentrations in rock samples of Portuguese geological units, generated of literature data.

The European Atlas of Natural Radiation, recently published, contains a collection of maps of Europe showing the levels of natural sources of radiation. Among the lacunae of the Atlas are maps of U, Th and K concentrations in rocks due to lack of European-wide geochemical surveys of bedrock units. The objective of this paper is to investigate the usability of scattered geochemical data of rock samples for large-scale mapping of U, Th and K concentrations in geological units. For this purpose, geochemical data were compiled from literature sources to produce a geochemical database (LIT database) that includes 2817 entries of U, Th and K concentrations measured in rock samples of geological units outcropping in Portugal. Given the methodical heterogeneity within LIT database, the influence of the geochemical analysis techniques was assessed through a three-way analysis of variance (ANOVA) using geological units, geochemical analysis techniques and loss on ignition (LOI) as categorical variables. The percentage of variation explained by geological factors was large (>35%), while the percentage of variation explained by the geochemical analysis techniques and LOI was generally lower than 5%. The geological factors were the main source of variability in the data, followed by the error component which can be assumed to represent the true spatial variability of geochemical concentrations. The pairwise comparison of the least square (LS) means computed through the ANOVA for each geochemical analysis technique indicates that LIT database can be considered consistent within itself, thus, reliable. In order to validate the usability of literature data the terrestrial gamma dose rate (TGDR) calculated from LIT database (TGDRcalc) was compared to the TGDR displayed in the Radiometric Map of Portugal (TGDRobs). The correlation between TGDRcalc and TGDRobs was highly significant (p < 0.001) and the results of a paired sample t-test and Wilcoxon median tests indicate that the differences between the arithmetic means of TGDRcalc and TGDRobs were not statistically significant (p = 0.126 and p = 0.14, respectively). Distributions of TGDRcalc and TGDRobs were seemingly equal according to the Kolmogorov-Smirnov and Anderson-Darling tests. Although, systematic discrepancies between TGDRcalc and TGDRobs were observed for sedimentary rocks, the compatibility of the RMP and LIT databases can be considered acceptable, which implies that the estimation of the contents of terrestrial radionuclides using literature data for large-scale mapping of U, Th and K contents in geological units is reasonable.

Plutonium aided reconstruction of caesium atmospheric fallout in European topsoils.

Global nuclear weapon testing and the Chernobyl accident have released large amounts of radionuclides into the environment. However, to date, the spatial patterns of these fallout sources remain poorly constrained. Fallout radionuclides (137Cs, 239Pu, 240Pu) were measured in soil samples (n = 160) collected at flat, undisturbed grasslands in Western Europe in the framework of a harmonised European soil survey. We show that both fallout sources left a specific radionuclide imprint in European soils. Accordingly, we used plutonium to quantify contributions of global versus Chernobyl fallout to 137Cs found in European soils. Spatial prediction models allowed for a first assessment of the global versus Chernobyl fallout pattern across national boundaries. Understanding the magnitude of these fallout sources is crucial not only to establish a baseline in case of future radionuclide fallout but also to define a baseline for geomorphological reconstructions of soil redistribution due to soil erosion processes.

Development of a Geogenic Radon Hazard Index-Concept, History, Experiences.

Exposure to indoor radon at home and in workplaces constitutes a serious public health risk and is the second most prevalent cause of lung cancer after tobacco smoking. Indoor radon concentration is to a large extent controlled by so-called geogenic radon, which is radon generated in the ground. While indoor radon has been mapped in many parts of Europe, this is not the case for its geogenic control, which has been surveyed exhaustively in only a few countries or regions. Since geogenic radon is an important predictor of indoor radon, knowing the local potential of geogenic radon can assist radon mitigation policy in allocating resources and tuning regulations to focus on where it needs to be prioritized. The contribution of geogenic to indoor radon can be quantified in different ways: the geogenic radon potential (GRP) and the geogenic radon hazard index (GRHI). Both are constructed from geogenic quantities, with their differences tending to be, but not always, their type of geographical support and optimality as indoor radon predictors. An important feature of the GRHI is consistency across borders between regions with different data availability and Rn survey policies, which has so far impeded the creation of a European map of geogenic radon. The GRHI can be understood as a generalization or extension of the GRP. In this paper, the concepts of GRP and GRHI are discussed and a review of previous GRHI approaches is presented, including methods of GRHI estimation and some preliminary results. A methodology to create GRHI maps that cover most of Europe appears at hand and appropriate; however, further fine tuning and validation remains on the agenda.

Intercomparison of Indoor Radon Measurements Under Field Conditions In the Framework of MetroRADON European Project.

Interlaboratory comparisons are a basic part of the regular quality controls of laboratories to warranty the adequate performance of test and measurements. The exercise presented in this article is the comparison of indoor radon gas measurements under field conditions performed with passive detectors and active monitors carried out in the Laboratory of Natural Radiation (LNR). The aim is to provide a direct comparison between different methodologies and to identify physical reasons for possible inconsistencies, particularly related to sampling and measurement techniques. The variation of radon concentration during the comparison showed a big range of values, with levels from approximately 0.5 to 30 kBq/m3. The reference values for the two exposure periods have been derived from a weighted average of participants' results applying an iterative algorithm. The indexes used to analyze the participants' results were the relative percentage difference D(%), the Zeta score ( ζ ), and the z-score ( z ). Over 80% of the results for radon in air exposure are within the interval defined by the reference value and 20% and 10% for the first and the second exposure, respectively. Most deviations were detected with the overestimating of the exposure using passive detectors due to the related degassing time of detector holder materials.

Qualitative overview of indoor radon surveys in Europe.

The revised European Directive from 2013 regarding basic safety standard oblige EU Member States to establish a national action plan regarding the exposure to radon. At the same time, International Atomic Energy Agency started technical projects in order to assist countries to establish and implement national radon action. As a consequence, in recent years, in numerous countries national radon surveys were conducted and action plans established, which were not performed before. In this paper, a qualitative overview of radon surveys performed in Europe is given with a special attention to the qualitative and conceptual description of surveys, representativeness and QA/QC (quality assurance/quality control).

Digital version of the European Atlas of natural radiation.

The European Atlas of Natural Radiation is a collection of maps displaying the levels of natural radioactivity caused by different sources. It has been developed and is being maintained by the Joint Research Centre (JRC) of the European Commission, in line with its mission, based on the Euratom Treaty: to collect, validate and report information on radioactivity levels in the environment of the EU Member States. This work describes the first version of the European Atlas of Natural Radiation, available in digital format through a web portal, as well as the methodology and results for the maps already developed. So far the digital Atlas contains: an annual cosmic-ray dose map; a map of indoor radon concentration; maps of uranium, thorium and potassium concentration in soil and in bedrock; a terrestrial gamma dose rate map; and a map of soil permeability. Through these maps, the public will be able to: familiarize itself with natural environmental radioactivity; be informed about the levels of natural radioactivity caused by different sources; have a more balanced view of the annual dose received by the European population, to which natural radioactivity is the largest contributor; and make direct comparisons between doses from natural sources of ionizing radiation and those from man-made (artificial) ones, hence, to better assess the latter. Work will continue on the European Geogenic Radon Map and on estimating the annual dose that the public may receive from natural radioactivity, by combining all the information from the different maps. More maps could be added to the Atlas, such us radon in outdoor air and in water and concentration of radionuclides in water, even if these sources usually contribute less to the total exposure.

Mapping potassium and thorium concentrations in Belgian soils.

The European Atlas of Natural Radiation developed by the Joint Research Centre (JRC) of the European Commission includes maps of potassium K and thorium Th. With several different databases available, including data (albeit not calibrated) from an airborne survey, Belgium is a favourable case for exploring the methodology of mapping for these natural radionuclides. Harmonized databases of potassium and thorium in soil were built by radiological (not airborne) and geochemical data. Using this harmonized database it was possible to calibrate the data from the airborne survey. Several methods were used to perform spatial interpolation and to smooth the data: moving average (MA) without constraint, or constrained by soil class and by geological unit. Overall, there was a reasonable agreement between the maps on a 1 × 1 km2 grid obtained with the two datasets (airborne data and harmonized soil data) with all the methods. The agreement was better when the maps are reduced to a 10 km × 10 km grid used for the European Atlas of Natural Radiation. The best agreement was observed with the MA constrained by geological unit.

Mapping uranium concentration in soil: Belgian experience towards a European map.

A map of uranium concentration in soil has been planned for the European Atlas of Natural Radiation. This Atlas is being developed by the Radioactivity Environmental Monitoring (REM) group of the Joint Research Centre (JRC) of the European Commission. The great interest in uranium compared to other terrestrial radionuclides stems from the fact that radon (222Rn) is in the decay chain of uranium (238U) and that public exposure to natural ionizing radiation is largely due to indoor radon. With several different databases available, including data (albeit not calibrated) from an airborne survey, Belgium is a favourable case for exploring the methodology of uranium mapping. A harmonized database of uranium in soil was built by merging radiological (not airborne) and geochemical data. Using this harmonized database it was possible to calibrate the data from the airborne survey. Several methods were used to perform spatial interpolation and to smooth the data: moving average without constraint, by soil class and by geological unit. When using the harmonized database, it is first necessary to evaluate the uranium concentration in areas without data or with an insufficient number of data points. Overall, there is a reasonable agreement between the maps on a 1 km × 1 km grid obtained with the two datasets (airborne U and harmonized soil U) with all the methods. The agreement is better when the maps are reduced to a 10 km × 10 km grid; the latter could be used for the European map of uranium concentration in soil.

Assessment of lithogenic radioactivity in the Euganean Hills magmatic district (NE Italy).

The Euganean Hills of North East Italy have long been recognised as an area characterized by a higher than average natural radiation background. This is due to two main reasons: a) primary lithogenic radiation due to rhyolitic and trachytic outcrops, which are "acidic alkaline" magmatic rocks potentially enriched in uranium and thorium; b) secondary sources related to a geothermal field - widely exploited for spa tourism in the area since the Roman age - producing surface release of radon-enriched fluids. Though radioactivity levels in the Euganean district have been often investigated in the past - including recent works aimed at assessing the radiation doses from radon and/or total gamma radiation - no effort has been put so far into producing a thorough assessment linking radiation protection data to geological-structural features (lithology, faults, water, organic matter content, etc.). This work represents the first part of the interdisciplinary project "Geological and geochemical control on Radon occurrence and natural radioactivity in the Euganean Hills district (North-Eastern Italy)", aimed at producing detailed results of the actual radiation levels in connection mainly with lithological parameters. A detailed sampling strategy, based on lithostratigraphy, petrology and mineralogy, has been adopted. The 151 rock samples collected were analyzed by high resolution γ-ray spectrometry with ex situ HPGe detectors. Statistical and geostatistical analyses were performed, and outlier values of U and Th - possibly associated with anomalies in the geological formation - were identified. U, Th and K concentration maps were developed using both the entire database and then again after expunging the outliers; the two were then compared. In all maps the highest values can be associated to trachyte and rhyolite lithologies, and the lowest ones to sedimentary formations. The external dose due to natural radionuclides in the soil - the so called terrestrial gamma dose rate - has been calculated using the U, Th and K distribution measured in the bedrock samples.

Calibration with MCNP of NaI detector for the determination of natural radioactivity levels in the field.

In view of assessing natural radioactivity with on-site quantitative gamma spectrometry, efficiency calibration of NaI(Tl) detectors is investigated. A calibration based on Monte Carlo simulation of detector response is proposed, to render reliable quantitative analysis practicable in field campaigns. The method is developed with reference to contact geometry, in which measurements are taken placing the NaI(Tl) probe directly against the solid source to be analyzed. The Monte Carlo code used for the simulations was MCNP. Experimental verification of the calibration goodness is obtained by comparison with appropriate standards, as reported. On-site measurements yield a quick quantitative assessment of natural radioactivity levels present ((40)K, (238)U and (232)Th). On-site gamma spectrometry can prove particularly useful insofar as it provides information on materials from which samples cannot be taken.

Log-normality of indoor radon data in the Walloon region of Belgium.

The deviations of the distribution of Belgian indoor radon data from the log-normal trend are examined. Simulated data are generated to provide a theoretical frame for understanding these deviations. It is shown that the 3-component structure of indoor radon (radon from subsoil, outdoor air and building materials) generates deviations in the low- and high-concentration tails, but this low-C trend can be almost completely compensated by the effect of measurement uncertainties and by possible small errors in background subtraction. The predicted low-C and high-C deviations are well observed in the Belgian data, when considering the global distribution of all data. The agreement with the log-normal model is improved when considering data organised in homogeneous geological groups. As the deviation from log-normality is often due to the low-C tail for which there is no interest, it is proposed to use the log-normal fit limited to the high-C half of the distribution. With this prescription, the vast majority of the geological groups of data are compatible with the log-normal model, the remaining deviations being mostly due to a few outliers, and rarely to a "fat tail". With very few exceptions, the log-normal modelling of the high-concentration part of indoor radon data is expected to give reasonable results, provided that the data are organised in homogeneous geological groups.

Homogenity of geological units with respect to the radon risk in the Walloon region of Belgium.

In the process of mapping indoor radon risk, an important step is to define geological units well-correlated with indoor radon. The present paper examines this question for the Walloon region of Belgium, using a database of more than 18,000 indoor radon measurements. With a few exceptions like the Carboniferous (to be divided into Tournaisian, Visean and Namurian-Westphalian) and the Tertiary (in which all Series may be treated together), the Series/Epoch stratigraphic level is found to be the most appropriate geological unit to classify the radon risk. A further division according to the geological massif or region is necessary to define units with a reasonable uniformity of the radon risk. In particular, Paleozoic series from Cambrian to Devonian show strong differences between different massifs. Local hot-spots are also observed in the Brabant massif. Finally, 35 geological units are defined according to their radon risk, 6 of which still present a clear weak homogeneity. In the case of 4 of these units (Jurassic, Middle Devonian of Condroz and of Fagne-Famenne, Ordovician of the Stavelot massif) homogeneity is moderate, but the data are strongly inhomogeneous for Visean in Condroz and in the Brabant massif. The 35 geological units are used in an ANOVA analysis, to evaluate the part of indoor radon variability which can be attributed to geology. The result (15.4-17.7%) agrees with the values observed in the UK.

Comparison of radioactivity data measured in PM10 aerosol samples at two elevated stations in northern Italy during the Fukushima event.

The follow-up of Fukushima radioactive plume resulting from the 11th March 2011 devastating tsunami is discussed for two Italian stations in the northern Apennines: Mt. Cimone (Modena) and Montecuccolino (Bologna). Radioactivity data collected at both stations are described, including comparison between local natural background of airborne particulate and artificial radioactivity referable to the arrival of the radioactive plume and its persistence and evolution. Analysis of back-trajectories was used to confirm the arrival of artificial radionuclides following atmospheric transport and processing. The Fukushima plume was first detected on 3rd April 2011 when high volume sampling revealed the presence of the artificial radionuclides (131)I, (137)Cs and (134)Cs. The highest activity concentrations of these nuclides were detected on 5th April 2011 at the Montecuccolino site. Fukushima radioactivity data at the two stations were usually comparable, suggesting a good vertical mixing of the plume; discrepancies were occasional and attributed to different occurrence of wet removal, typically characterized by a scattered spatial pattern. To understand the relevance to the local population of the extra dose due to the Fukushima plume, atmospheric activities of the related artificial nuclides were compared to those of the main natural radionuclides in ambient particulate, and found to be lower by over one order of magnitude. Radiation doses referable to Fukushima, maximized for a whole year occurrence at the highest activity level observed at our stations in the weeks affected by the Japanese plume, were estimated at 1.1 µSv/year.