Effects of environmental factors on the monitoring of environmental radioactivity by airborne gamma-ray spectrometry.

This study describes and discusses the results of a 14 month-long campaign (April 2019 to June 2020) aimed at characterizing and quantifying the influence of environmental factors (cosmic rays, rainfall events, soil moisture and atmospheric radon) on airborne radiometric surveys, which are used for mapping the concentrations of potassium (K), uranium (U) and thorium (Th), or for monitoring the natural radioactivity in the environment. A large NaI(Tl) airborne spectrometer (4 down + 1 up detectors of 4 L) was installed at a height of 50 m on a meteorological tower to simulate an airborne hover at the Pyrenean Platform for Observation of the Atmosphere (P2OA) in Lannemezan. The continuous, high frequency acquisition of gamma-rays was accompanied by measurements of rainfall intensity, soil moisture content, atmospheric radon activity and meteorological parameters. A semi-diurnal cycle of apparent 232Th and 40K was observed and explained by atmospheric thermal tides. Both diurnal and seasonal cycles are also evident in the gamma-ray signal, mostly due to variations of soil moisture at these timescales with a maximum during summer when surface soil moisture (0-5 cm depth) is the lowest. An increase of 25% vol. of the soil moisture content, representing the range of variation between the end of summer (18% vol.) and the beginning of spring (43% vol.) leads to a decrease of gamma-rays in the K and Th window by the same amount. Conversely, these results illustrate the potential of using airborne gamma-ray spectrometry to monitor soil moisture at hectometer scales. The washout of radon-222 progeny during rainfall events influences the count of gamma-rays in the U window by adding an atmospheric component to the soil component. The amplitude of the signal increase in the U window varies with the precipitation rate and reaches 30% for an average event. By clear weather, atmospheric radon-222 volumic activity influences the count rate in the U window by about ±3.8% per Bq m-3, which translates into an influence of 148%/Bq m-3/kg Bq-1 (U). This comprehensive, multi-compartment approach is necessary to optimize and improve the processing and analysis of airborne gamma-ray spectrometry data for high sensitivity environmental studies. These results show the importance of environmental factors on the variability of gamma-ray spectrometry and the importance of taking them into account to accurately map radionuclides activities.

Temporal variations of radon concentration in the saturated soil of Alpine grassland: the role of groundwater flow.

Radon concentration has been monitored from 1995 to 1999 in the soil of the Sur-Frêtes ridge (French Alps), covered with snow from November to April. Measurements were performed at 70 cm depth, with a sampling time of 1 h, at two points: the summit of the ridge, at an altitude of 1792 m, and the bottom of the ridge, at an altitude of 1590 m. On the summit, radon concentration shows a moderate seasonal variation, with a high value from October to April (winter), and a low value from May to September (summer). At the bottom of the ridge, a large and opposite seasonal variation is observed, with a low value in winter and a high value in summer. Fluctuations of the radon concentration seem to be associated with temperature variations, an effect which is largely delusory. Indeed, these variations are actually due to water infiltration. A simplified mixing model is used to show that, at the summit of the ridge, two effects compete in the radon response: a slow infiltration response, rich in radon, with a typical time scale of days, and a fast infiltration of radon-poor rainwater. At the bottom of the ridge, similarly, two groundwater contributions compete: one slow infiltration response, similar to the response seen at the summit, and an additional slower response, with a typical time scale of about a month. This second slower response can be interpreted as the aquifer discharge in response to snow melt. This study shows that, while caution is necessary to properly interpret the various effects, the temporal variations of the radon concentration in soil can be understood reasonably well, and appear to be a sensitive tool to study the subtle interplay of near surface transfer processes of groundwater with different transit times.

Seasonal variations of natural ventilation and radon-222 exhalation in a slightly rising dead-end tunnel.

The concentration activity of radon-222 has been monitored, with some interruptions, from 1997 to 2005 in the end section of a slightly rising, dead-end, 38-m long tunnel located in the Phulchoki hill, near Kathmandu, Nepal. While a high concentration varying from 6 x 10(3) Bq m(-3) to 10 x 10(3) Bq m(-3) is observed from May to September (rainy summer season), the concentration remains at a low level of about 200 Bq m(-3) from October to March (dry winter season). This reduction of radon concentration is associated with natural ventilation of the tunnel, which, contrary to expectations for a rising tunnel, takes place mainly from October to March when the outside air temperature drops below the average tunnel temperature. This interpretation is supported by temperature measurements in the atmosphere of the tunnel, a few meters away from the entrance. The temporal variations of the diurnal amplitude of this temperature indeed follow the ventilation rate deduced from the radon measurements. In the absence of significant ventilation (summer season), the radon exhalation flux at the rock surface into the tunnel atmosphere can be inferred; it exhibits a yearly variation with additional transient reductions associated with heavy rainfall, likely to be due to water infiltration. No effect of atmospheric pressure variations on the radon concentration is observed in this tunnel. This experiment illustrates how small differences in the location and geometry of a tunnel can lead to vastly different behaviours of the radon concentration versus time. This observation has consequences for the estimation of the dose rate and the practicability of radon monitoring for tectonic purposes in underground environments.

Development of a highly sensitive radon-222 amplifier (HiSRA) for low-level atmospheric measurements.

Radon (222Rn), a radioactive gas with a half-life of 3.82 days, is continuously emanated from soil, rocks, and water by the radioactive decay of 226Ra. Radon-222 is released from the ground into the atmosphere, where it is transported mainly by turbulent diffusion or convection. For precise measurement of radon-222 atoms in the atmosphere, the detectors typically used present a small volume or surface area and are therefore not very sensitive, especially for online measurements and short sample intervals (<1 h). This article deals with the development of a Highly Sensitive Radon Amplifier (HiSRA) consisting in an enrichment system placed prior to a classic radon-222 analyzer. This system uses permeation membranes that make it possible to treat large quantities of air online (30 m3 h-1). The radon-222 concentration is increased instantaneously by at least a factor of 30 across the HiSRA system. Therefore, in this study, when coupling to an ionization chamber (AlphaGUARDTM) at the outlet of the HiSRA system, the detection limit of the overall system is multiplied by factor of 30 and induces a new LD for a radon 222 gas analyzer lower than 1 Bq m-3 for an integrating time of 10 min and 0.1 Bq m-3 for 1 h. We constructed one radon amplifier prototype that provided the preliminary results for amplification efficiency and the initial measurements presented herein.

Modelling the effect of air exchange on 222Rn and its progeny concentration in a tunnel atmosphere.

The effect of air exchange on the concentration of 222Rn and its progeny in the atmosphere of the Roselend tunnel, in the French Alps, is estimated using a box modelling scheme. In this scheme, the atmosphere is divided into a small number of well mixed zones, separated by flow restricted interfaces, characterized by their exchange rate. A four-box model, representing the three sections of the tunnel present until 2001 and an adjacent inner room, accounts for the spatial variations of the background 222Rn concentration, and for the time structure of transient bursts observed regularly in this tunnel since 1995. A delay of the order of one day, observed during some transient bursts in the inner room with respect to the end of the tunnel, is accounted for if the bursts are assumed to be mainly generated in the end section of the tunnel, and stored temporarily in the inner room via air exchange. The measured radon concentration is reproduced by this model for an air exchange rate of 1.6x10(-6) s-1 between the room and the tunnel, in a context of a global ventilation rate of 10(-5) s-1 in the tunnel. Gradual onset and decay phases, varying from burst to burst, are also suggested. The equilibrium factor of 222Rn with its progeny, measured in 2002 with values varying from 0.60+/-0.05 to 0.78+/-0.06, is interpreted with a five-box model representing the five sections of the tunnel present after 2001. This model indicates that the equilibrium factor does not provide additional constraints on the air exchange rates, but the value of the deposition rate of the unattached short-lived radon progeny can be inferred, with results varying from 0.2 to 6 h-1 in the various sections. This study illustrates the benefits of a simple modelling tool to evaluate the effect of natural ventilation on 222Rn and its progeny concentration in underground cavities, which is important for radioprotection and for a reliable characterization of signatures of hydrogeological or geodynamical processes. Conversely, this study shows that 222Rn and progeny measurements provide a non-invasive method for characterizing natural ventilation conditions in delicate underground cavities, such as painted caves.

Spatial and time variations of radon-222 concentration in the atmosphere of a dead-end horizontal tunnel.

The concentration of radon-222 has been monitored since 1995 in the atmosphere of a 2 m transverse dimension, 128 m long, dead-end horizontal tunnel located in the French Alps, at an altitude of 1600 m. Most of the time, the radon concentration is stable, with an average value ranging from 200 Bq m(-3) near the entrance to about 1000 Bq m(-3) in the most confined section, with an equilibrium factor between radon and its short-lived decay products varying from 0.61 to 0.78. However, radon bursts are repeatedly observed, with amplitudes reaching up to 36 x 10(3) Bq m(-3) and durations varying from one to several weeks, with similar spatial variations along the tunnel as the background concentration. These spatial variations are qualitatively interpreted in terms of natural ventilation. Comparing the radon background concentration with the measured radon exhalation flux at the wall yields an estimate of 8+/-2 x 10(-6) s(-1) (0.03+/-0.007 h(-1)) for the ventilation rate. The hypothesis that the bursts could be due to transient changes in ventilation can be ruled out. Thus, the bursts are the results of transient increased radon exhalation at the walls, that could be due to meteorological effects or possibly combined hydrological and mechanical forcing associated with the water level variations of the nearby Roselend reservoir lake. Such studies are of interest for radiation protection in poorly ventilated underground settings, and, ultimately, for a better understanding of radon exhalation associated with tectonic or volcanic processes.

Evaluation of the effect of a cover layer on radon exhalation from uranium mill tailings: transient radon flux analysis.

An experimental study concerning the transport of 222Rn in uranium mill tailings (UMTs) and in the cover layer was launched in 1997 with the participation of the French uranium mining company (COGEMA). Evaluation of the cover layer's effectiveness in reducing 222Rn flux emanating from UMTs was one of its objectives. In the first phase, the 222Rn flux densities were measured regularly on a UMT layer. In the second phase, the UMT was covered with a one-meter layer of compacted material consisting of crushed waste rock derived from mining activities. Radon-222 flux was then measured at the surface of this cover layer. Observations were compared with radon flux calculated using TRACI, a model for vertical water and gas flow and radon transport. The results show that the calculations bear a fair resemblance to the observations in both cases. They also show that the effectiveness of the cover layer calculated with TRACI, using the thickness and textural properties of the cover material, is very close to the measured effectiveness.

Radon-222 signatures of natural ventilation regimes in an underground quarry.

Radon-222 activity concentration has been monitored since 1999 in an underground limestone quarry located in Vincennes, near Paris, France. It is homogeneous in summer, with an average value of 1700 Bq m(-3), and varies from 730 to 1450 Bq m(-3) in winter, indicating natural ventilation with a rate ranging from 0.5 to 2.4 x 10(-6) s(-1) (0.04-0.22 day(-1)). This hypothesis is supported by measurements in the vertical access pit where, in winter, a turbulent air current produces a stable radon profile, smoothly decreasing from 700 Bq m(-3) at 20 m depth to 300 Bq m(-3) at surface. In summer, a thermal stratification is maintained in the pit, but the radon-222 concentration jumps repeatedly between 100 and 2000 Bq m(-3). These jumps are due to atmospheric pressure pumping, which induces ventilation in the quarry at a rate of about 0.1 x 10(-6) s(-1) (0.009 day(-1)). Radon-222 monitoring thus provides a dynamical characterisation of ventilation regimes, which is important for the assessment of the long-term evolution of underground systems.

Temporal signatures of advective versus diffusive radon transport at a geothermal zone in Central Nepal.

Temporal variation of radon-222 concentration was studied at the Syabru-Bensi hot springs, located on the Main Central Thrust zone in Central Nepal. This site is characterized by several carbon dioxide discharges having maximum fluxes larger than 10 kg m(-2) d(-1). Radon concentration was monitored with autonomous Barasol™ probes between January 2008 and November 2009 in two small natural cavities with high CO(2) concentration and at six locations in the soil: four points having a high flux, and two background reference points. At the reference points, dominated by radon diffusion, radon concentration was stable from January to May, with mean values of 22 ± 6.9 and 37 ± 5.5 kBq m(-3), but was affected by a large increase, of about a factor of 2 and 1.6, respectively, during the monsoon season from June to September. At the points dominated by CO(2) advection, by contrast, radon concentration showed higher mean values 39.0 ± 2.6 to 78 ± 1.4 kBq m(-3), remarkably stable throughout the year with small long-term variation, including a possible modulation of period around 6 months. A significant difference between the diffusion dominated reference points and the advection-dominated points also emerged when studying the diurnal S(1) and semi-diurnal S(2) periodic components. At the advection-dominated points, radon concentration did not exhibit S(1) or S(2) components. At the reference points, however, the S(2) component, associated with barometric tide, could be identified during the dry season, but only when the probe was installed at shallow depth. The S(1) component, associated with thermal and possibly barometric diurnal forcing, was systematically observed, especially during monsoon season. The remarkable short-term and long-term temporal stability of the radon concentration at the advection-dominated points, which suggests a strong pressure source at depth, may be an important asset to detect possible temporal variations associated with the seismic cycle.

Spatiotemporal variation of radon and carbon dioxide concentrations in an underground quarry: coupled processes of natural ventilation, barometric pumping and internal mixing.

Radon-222 and carbon dioxide concentrations have been measured during several years at several points in the atmosphere of an underground limestone quarry located at a depth of 18 m in Vincennes, near Paris, France. Both concentrations showed a seasonal cycle. Radon concentration varied from 1200 to 2000 Bq m(-3) in summer to about 800-1400 Bq m(-3) in winter, indicating winter ventilation rates varying from 0.6 to 2.5 x 10(-6) s(-1). Carbon dioxide concentration varied from 0.9 to 1.0% in summer, to about 0.1-0.3% in winter. Radon concentration can be corrected for natural ventilation using temperature measurements. The obtained model also accounts for the measured seasonal variation of carbon dioxide. After correction, radon concentrations still exhibit significant temporal variation, mostly associated with the variation of atmospheric pressure, with coupling coefficients varying from -7 to -26 Bq m(-3) hPa(-1). This variation can be accounted for using a barometric pumping model, coupled with natural ventilation in winter, and including internal mixing as well. After correction, radon concentrations exhibit residual temporal variation, poorly correlated between different points, with standard deviations varying from 3 to 6%. This study shows that temporal variation of radon concentrations in underground cavities can be understood to a satisfactory level of detail using non-linear and time-dependent modelling. It is important to understand the temporal variation of radon concentrations and the limitations in their modelling to monitor the properties of natural or artificial underground settings, and to be able to assess the existence of new processes, for example associated with the preparatory phases of volcanic eruptions or earthquakes.

Persistence of radon-222 flux during monsoon at a geothermal zone in Nepal.

The Syabru-Bensi hydrothermal zone, Langtang region (Nepal), is characterized by high radon-222 and CO(2) discharge. Seasonal variations of gas fluxes were studied on a reference transect in a newly discovered gas discharge zone. Radon-222 and CO(2) fluxes were measured with the accumulation chamber technique, coupled with the scintillation flask method for radon. In the reference transect, fluxes reach exceptional mean values, as high as 8700+/-1500 gm(-2)d(-1) for CO(2) and 3400+/-100 x 10(-3) Bq m(-2)s(-1) for radon. Gases fluxes were measured in September 2007 during the monsoon and during the dry winter season, in December 2007 to January 2008 and in December 2008 to January 2009. Contrary to expectations, radon and its carrier gas fluxes were similar during both seasons. The integrated flux along this transect was approximately the same for radon, with a small increase of 11+/-4% during the wet season, whereas it was reduced by 38+/-5% during the monsoon for CO(2). In order to account for the persistence of the high gas emissions during monsoon, watering experiments have been performed at selected radon measurement points. After watering, radon flux decreased within 5 min by a factor of 2-7 depending on the point. Subsequently, it returned to its original value, firstly, by an initial partial recovery within 3-4h, followed by a slow relaxation, lasting around 10h and possibly superimposed by diurnal variations. Monsoon, in this part of the Himalayas, proceeds generally by brutal rainfall events separated by two- or three-day lapses. Thus, the recovery ability shown in the watering experiments accounts for the observed long-term persistence of gas discharge. This persistence is an important asset for long-term monitoring, for example to study possible temporal variations associated with stress accumulation and release.