Rock deformation vs. radon emission: some constraints from shear stress-controlled experiments.

Numerous field and laboratory studies have been conducted to investigate the relationship between radon variation and seismic events, as well as the complex link between radon emission and rock deformation mechanisms. However, a clear understanding of this correspondence and systematic observations of these phenomena are still lacking, and recent experimental studies have yet to yield conclusive results. In this study, we investigate the possible relationships between radon migration dynamics and rock deformation at the micro-scale through laboratory experiments using the SHIVA apparatus under shear stress-controlled conditions and simultaneous high-resolution radon measurements. We studied the behaviour of three different lithologies to show that radon emission varies in response to rock deformation and this variation is highly dependent on the mineralogy and microstructure. This study represents the first attempt to define radon gas as an indicator of transient and rapid rock deformation at the micro-scale.

The Analysis of 222Rn and 220Rn Natural Radioactivity for Local Hazard Estimation: The Case Study of Cerveteri (Central Italy).

Radon (222Rn) is the second most common cause of lung cancer after smoking. As radon poses a significant risk to human health, radon-affected areas should be identified to ensure people's awareness of risk and remediation. The primary goal of this research was to investigate the local natural radioactivity (in soils, groundwater, and indoors) because of the presence of tuff outcrops (from middle-lower Pleistocene volcanic activity) that naturally produce radioactive gas radon at Cerveteri (Rome, Central Italy). The results of the radon survey highlighted moderate (>16,000 Bq/m3) but localized anomalies in soils in correspondence with a funerary site pertaining to the Etruscan Necropolis of Cerveteri, which extends over a volcanic rock plateau. Indoor radon measurements were performed at several tuff-made dwellings, and the results showed medium-low (<200 Bq/m3) values of indoor radon except for some cases exceeding the reference level (>300 Bq/m3) recommended by the 2013/59 Euratom Directive. Although no clinical data exist regarding the health effects of thoron (220Rn) on humans, the study of 220Rn average activity concentration in the soil gas survey reveals new insights for the interpretation of radon sources that can affect dwellings, even taking into account the considerable difference in the half-lives of 222Rn and 220Rn.

Active Monitoring of Residential Radon in Rome: A Pilot Study.

We present an overview of the potential of active monitoring techniques to investigate the many factors affecting the concentration of radon in houses. We conducted two experiments measuring radon concentration in 25 apartments in Rome and suburban areas for two weeks and in three apartments in the historic center for several months. The reference levels of 300 and 100 Bq/m3 are overcome in 17% and 60% of the cases, respectively, and these percentages rise to 20% and 76% for average overnight radon (more relevant for residents' exposure). Active detectors allowed us to identify seasonal radon fluctuations, dependent on indoor-to-outdoor temperature, and how radon travels from the ground to upper floors. High levels of radon are not limited to the lowest floors when the use of heating and ventilation produces massive convection of air. Lifestyle habits also reflect in the different values of gas concentration measured on different floors of the same building or in distinct rooms of the same apartment, which cannot be ascribed to the characteristics of the premises. However, the finding that high residential radon levels tend to concentrate in the historic center proves the influence of factors such as building age, construction materials, and geogenic radon.

Multi-level continuous monitoring of indoor radon activity.

We present the results of an experiment taking place inside the geophysical museum of Rocca di Papa (Rome, Italy), where the high radon levels detected might pose a risk to the health of workers and of the public audience. As a first step towards the mitigation of potential exposure risk, four active sensors were installed at different floors of the building, in order to continuously monitor not only radon exhalation from the soil but also its transport from the ground up to elevated floors. Collecting more than three years of data of radon concentration enables us to identify fluctuations over both short and seasonal scales and to elucidate the relation between radon variations and changes of internal temperature and relative humidity. The analysis of such dataset reveals how the healthiness of indoor environments in terms of radon concentration is controlled by a number of factors, including the environmental conditions and the use of heating and ventilation systems. Finally, the continuous radon monitoring at different levels of the building provides a unique chance to trace the vertical radon diffusion, allowing to make a first-order estimate of upward radon velocity.

Radon Hazard in Central Italy: Comparison among Areas with Different Geogenic Radon Potential.

Radon (222Rn) is a natural radioactive gas formed in rocks and soil by the decay of its parent nuclide (238-Uranium). The rate at which radon migrates to the surface, be it along faults or directly emanated from shallow soil, represents the Geogenic Radon Potential (GRP) of an area. Considering that the GRP is often linked to indoor radon risk levels, we have conducted multi-disciplinary research to: (i) define local GRPs and investigate their relationship with associated indoor Rn levels; (ii) evaluate inhaled radiation dosages and the associated risk to the inhabitants; and (iii) define radon priority areas (RPAs) as required by the Directive 2013/59/Euratom. In the framework of the EU-funded LIFE-Respire project, a large amount of data (radionuclide content, soil gas samples, terrestrial gamma, indoor radon) was collected from three municipalities located in different volcanic districts of the Lazio region (central Italy) that are characterised by low to high GRP. Results highlight the positive correlation between the radionuclide content of the outcropping rocks, the soil Rn concentrations and the presence of high indoor Rn values in areas with medium to high GRP. Data confirm that the Cimini-Vicani area has inhalation dosages that are higher than the reference value of 10 mSv/y.

Carrier and dilution effects of CO2 on thoron emissions from a zeolitized tuff exposed to subvolcanic temperatures.

Radon (222Rn) and thoron (220Rn) are two isotopes belonging to the noble gas radon (sensu lato) that is frequently employed for the geochemical surveillance of active volcanoes. Temperature gradients operating at subvolcanic conditions may induce chemical and structural modifications in rock-forming minerals and their related 222Rn-220Rn emissions. Additionally, CO2 fluxes may also contribute enormously to the transport of radionuclides through the microcracks and pores of subvolcanic rocks. In view of these articulated phenomena, we have experimentally quantified the changes of 220Rn signal caused by dehydration of a zeolitized tuff exposed to variable CO2 fluxes. Results indicate that, at low CO2 fluxes, water molecules and hydroxyl groups adsorbed on the glassy surface of macro- and micropores are physically removed by an intermolecular proton transfer mechanism, leading to an increase of the 220Rn signal. By contrast, at high CO2 fluxes, 220Rn emissions dramatically decrease because of the strong dilution capacity of CO2 that overprints the advective effect of carrier fluids. We conclude that the sign and magnitude of radon (sensu lato) changes observed in volcanic settings depend on the flux rate of carrier fluids and the rival effects between advective transport and radionuclide dilution.

Deep versus shallow sources of CO2 and Rn from a multi-parametric approach: the case of the Nisyros caldera (Aegean Arc, Greece).

Estimating the quantity of CO2 diffusively emitted from the Earth's surface has important implications for volcanic surveillance and global atmospheric CO2 budgets. However, the identification and quantification of non-hydrothermal contributions to CO2 release can be ambiguous. Here, we describe a multi-parametric approach employed at the Nisyros caldera, Aegean Arc, Greece, to assess the relative influence of deep and shallow gases released from the soil. In April 2019, we measured diffuse soil surface CO2 fluxes, together with their carbon isotope compositions, and at a depth of 80 cm, the CO2 concentration, soil temperature, and the activities of radon and thoron. The contributions of deep CO2 and biogenic CO2 fluxes were distinguished on the basis of their carbon isotope compositions. A Principal Component Analysis (PCA), performed on the measured parameters, effectively discriminates between a deep- and a shallow degassing component. The total CO2 output estimated from a relatively small testing area was two times higher with respect to that observed in a previous survey (October 2018). The difference is ascribed to variation in the soil biogenic CO2 production, that was high in April 2019 (a wet period) and low or absent in October 2018 (a dry period). Accounting for seasonal biogenic activity is therefore critical in monitoring and quantifying CO2 emissions in volcanic areas, because they can partially- or completely overwhelm the volcanic-hydrothermal signal.

Transient to stationary radon (220Rn) emissions from a phonolitic rock exposed to subvolcanic temperatures.

Rock substrates beneath active volcanoes are frequently subjected to temperature changes caused by the input of new magma from the depth and/or the intrusion of magma bodies of variable thickness within the subvolcanic rocks. The primary effect of the influx of hot magma is the heating of surrounding host rocks with the consequent modification of their physical and chemical properties. To assess mobilization in subvolcanic thermal regimes, we have performed radon (220Rn) thermal experiments on a phonolitic lava exposed to temperatures in the range of 100-900°C. Results from these experiments indicate that transient Rn signals are not unequivocally related to substrate deformation caused by tectonic stresses, but rather to the temperature-dependent diffusion of radionuclides through the structural discontinuities of rocks which serve as preferential pathways for gas release. Intense heating/cooling cycles are accompanied by rapid expansion and contraction of minerals. Rapid thermal cycling produced both inter- and intra-crystal microfracturing, as well as the formation of macroscopic faults. The increased number of diffusion paths dramatically intensified Rn migration, leading to much higher emissions than temperature-dependent transient changes. This geochemical behaviour is analogous to positive anomalies recorded on active volcanoes where dyke injections produce thermal stress and deformation in the host rocks. An increased Rn signal far away from the location of a magmatic intrusion is also consistent with microfracturing of subsurface rocks over long distances via thermal stress propagation and the opening of new pathways.

Implementing soil radon detectors for long term continuous monitoring.

The employment of different instruments for radon continuous measurements within the Italian Radon mOnitoring Network (IRON), mostly INGV, Algade AER and Airthings Corentium instruments, requires a uniform characterization and calibration protocol for the results to be comparable in a rigorous way. A 56 L stainless steel radon chamber with a sensitivity of 0.95 ±â€¯0.01 Bq m-3 per pulse h-1 has been used and validation of Algade AER, Airthings Corentium and Durridge RAD7 radon monitors equipped with solid-state detectors operated at different absolute humidity values has been performed, extending their operative range. Robustness to atmospheric electromagnetic phenomena of INGV and Algade AER instruments has been investigated and, for the former instrument, improved.

Integrating radon and thoron flux data with gamma radiation mapping in radon-prone areas. The case of volcanic outcrops in a highly-urbanized city (Roma, Italy).

An integration of laboratory radon and thoron exhalation data with gamma radiation mapping is applied to assess the geogenic radon and the exposure of people to natural radiation in a highly-urbanized city (Roma, Italy). The study area is a protected territory where ignimbrites from Colli Albani volcano and alluvial sediments largely crop out. A map of total gamma radiation, a gamma transect across Caffarella valley and 9 vertical gamma profiles have been carried out, showing that the main control of gamma levels is, of course, the lithological nature, without neglecting the simultaneous effect of other parameters such as slope morphology, erosion/weathering processes, occurrence of sinkholes or underground tunnels. The surveys allowed to distinguish the medians of ignimbrites (from 816 ±â€¯16 cps to 936 ±â€¯19 cps) from that of alluvial materials (611 ±â€¯14) cps), but showed also that alluvial sediments with anomalously high radioactivity (769 ±â€¯14 cps) can be locally recognized, providing valuable information on the interaction between sedimentation and erosion in fluvial valleys. Total gamma activity was converted into absorbed gamma dose rate ranging from 0.33 to 0.38 µSv/hr. Outdoor Annual Effective Dose Equivalents were also estimated between 0.58 and 0.67 mSv y-1. Laboratory radon and thoron exhalation rates of collected material are positively correlated with gamma radiation. Volcanic and alluvial sediments are well-discriminated. The correlation between the two variables is evident, but not robust because of the variable concentration of 40 K, which is not contributing to radon and thoron exhalation rates. Anomalous data of soil samples located at the foot of a slope can be interpreted as due to reworking and accumulation processes. Similar gamma radiation data documents analogous concentration of radon and thoron parent-nuclides, but coexisting different radon and thoron exhalation rates provides an additional information on different grain size distributions which can be considered as a proxy for soil gas permeability. The integration of gamma mapping and radon and thoron exhalation measurements is a very useful tool to assess people exposure to natural radiation, in terms of dose rates and potential indoor radon. Gamma mapping, which provides data on the radiation source (the bedrock) is fast and not expensive. It allows to obtain very detailed pictures of a study area, but it needs to be combined with laboratory determination of radon and thoron release in order to definitely and correctly interpret variations of gamma signal. Furthermore, laboratory determination of soil radon exhalation gives information on the release of radon and is a good proxy for soil gas permeability. It has the great advantage over in-situ measurements of gas flow not to be influenced by seasonal pedoclimatic parameters and is affected by lower analytical uncertainties. These data are thus reproducible and precise and can be used to estimate potential radon hazard, which is the main source of exposure and thus the most important parameter for human protection from environmental radioactivity.

Using a multi-method approach based on soil radon deficit, resistivity, and induced polarization measurements to monitor non-aqueous phase liquid contamination in two study areas in Italy and India.

Geochemical and geophysical surveys employing radon deficit, resistivity, and induced polarization (IP) measurements were undertaken on soil contaminated with non-aqueous phase liquids (NAPLs) in two different sites in India and in Italy. Radon deficit, validated through the comparison with average soil radon in reference unpolluted areas, shows the extension of contamination in the upper part of the unsaturated aquifers. In site 1 (Italy), the spill is not recent. A residual film of kerosene covers soil grains, inhibiting their chargeability and reducing electrical resistivity difference with background unpolluted areas. No correlation between the two parameters is observed. Soil volatile organic compounds (VOCs) concentration is not linked with radon deficit, supporting the old age of the spillage. NAPL pollution in sites 2a and 2b (India) is more recent and probably still active, as demonstrated by higher values of electrical resistivity. A good correlation with IP values suggests that NAPL is still distributed as droplets or as a continuous phase in the pores, strengthening the scenario of a fresh spill or leakage. Residual fraction of gasoline in the pore space of sites 2a and 2b is respectively 1.5 and 11.8 kg per cubic meter of terrain. This estimation is referred to the shallower portion of the unsaturated aquifer. Electrical resistivity is still very high indicating that the gasoline has not been strongly degraded yet. Temperature and soil water content influence differently radon deficit in the three areas, reducing soil radon concentration and partly masking the deficit in sites 2a and 2b.

Soil radon survey to assess NAPL contamination from an ancient spill. Do kerosene vapors affect radon partition ?

A soil radon-deficit survey was carried out in a site polluted with kerosene (Rome, Italy) in winter 2016 to assess the contamination due to the NAPL residual component in the vadose zone and to investigate the role of the vapor plume. Radon is indeed more soluble in the residual NAPL than in air or water, but laboratory experiments demonstrated that it is also preferentially partitioned in the NAPL vapors that transport it and may influence soil radon distribution patterns. Specific experimental configurations were designed and applied to a 31-station grid to test this hypothesis; two RAD7 radon monitors were placed in-series and connected to the top of a hollow probe driven up to 80-cm depth; the first instrument was directly attached to the probe and received humid soil gas, which was counted and then conveyed to the second monitor through a desiccant (drierite) cylinder capturing moisture and eventually the NAPL volatile component plus the radon dissolved in vapors. The values from the two instruments were cross-calibrated through specifically designed laboratory experiments and compared. The results are in agreement within the error range, so the presence of significant NAPL vapors, eventually absorbed by drierite, was ruled out. This is in agreement with low concentrations of soil VOCs. Accordingly, the radon-deficit is ascribed to the residual NAPL in the soil pores, as shown very well also by the obtained maps. Preferential areas of radon-deficit were recognised, as in previous surveys. An average estimate of 21 L (17 Kg) of residual NAPL per cubic meter of terrain is provided on the basis of original calculations, developed from published equations. A comparison with direct determination of total hydrocarbon concentration (23 kg per cubic meter of terrain) is provided.

Laboratory simulation of recent NAPL spills to investigate radon partition among NAPL vapours and soil air.

Soil radon is employed to trace residual NAPL (Non-Aqueous Phase Liquid) contamination because it is very soluble in these substances and is strongly depleted over polluted volumes of the subsoil. The solubility of radon into NAPL vapors, generally poorly considered, is investigated here, either as growth of radon exhalation from a material contaminated with increasing volumes of kerosene, or as radon partition between liquid kerosene, water and total air, considered ad the sum of kerosene vapors plus air.