The sensitivity of innovative techniques for measuring low levels of radon in the environment using passive detectors.

In recent years, there has been a significant surge in interest in measuring low radon levels in the environment. These measurements are valuable, particularly for identifying radon priority areas as required by the European Council Directive 2013/59/EURATOM and for research related to climate change. Due to the limited sensitivity of existing radon detectors/monitors in addressing these challenges, substantial efforts have been devoted to developing new designs. This report compares the sensitivity of several innovative designs with that of existing passive radon monitors. These novel designs incorporate alpha track detectors, including large area low background detectors, with activated carbon fabric used as an efficient radon adsorber/radiator. Recent innovative solutions to mitigate the impact of temperature and humidity on detectors using adsorbers are also discussed. The background signal of detectors intended for use in these novel designs is examined, and their sensitivity is evaluated. The findings demonstrate that these novel designs have the potential to significantly enhance the sensitivity of long-term radon measurements, surpassing the detectors currently in widespread use by more than an order of magnitude.

Influence of humidity on activated carbon fabrics scheduled for use in high sensitivity radon detectors.

The dependence of radon adsorption on the content of adsorbed water of activated carbon fabrics of ACC-5092-10 and ACC-5092-20 was studied experimentally. Specimens with different content of adsorbed water (from zero to saturation level) were coupled with alpha-track detector and exposed to reference 222Rn concentration. Both materials demonstrated different properties: Radon adsorption in ACC-5092-10 smoothly and monotonically decreases with the increase of adsorbed water and at saturation level it is lower by a factor of 2.5 as compared to the fully dehydrated material. In ACC-5092-20 clear break point was observed at water content of about 20% where radon adsorption sharply drops by a factor of 15. ACC-5092-10 was identified as a material that keeps its high radon adsorption ability even when saturated with water. Coupled with alpha-track detector it may be used for sensitive long-term measurements 222Rn measurements even at high levels of humidity.

Methods for the experimental study of 220Rn homogeneity in calibration chambers.

This work presents two experimental methods for the evaluation of 220Rn homogeneity in calibration chambers. The first method is based on LSC of the 220Rn decay products captured in silica aerogel. The second method is based on application of solid state nuclear track detectors facing the air of the calibration chambers. The performances of the two methods are evaluated by dedicated experiments. The repeatability of the LSC-based method, estimated as relative standard deviation of the LSC measurements of ten silica aerogel samplers exposed under the same conditions is found to be 1.6%. Both methods are applied to study thoron homogeneity in the commercially available 50 L AlphaGuard emanation and calibration container, which was empty and its fan was turned on. It was found that the 220Rn distribution in this case is homogeneous within 10%. Both methods are also applied to test the thoron homogeneity in the BACCARA chamber at IRSN during a thoron calibration exercise. The results show that, at the centre of the chamber where the inputs of the sampling systems of the radon/thoron detectors were put close to each other, the thoron inhomogeneity is less than 10%. However, regions of higher thoron concentrations are clearly identified near the walls and the upper part of the chamber, with 220Rn concentrations being up to 60% higher compared to the concentration at the reference point. These results highlight the importance of the control and assessment of thoron homogeneity in thoron calibrations and in the cases when radon monitors are checked for thoron influence.

Identifying radon priority areas and dwellings with radon exceedances in Bulgaria using stored CD/DVDs.

The implementation of the 2013/59/EURATOM directive in the part related to radon exposure imposes challenges for radon measurement methodology and radon survey design. Among them is the need to have estimates (preferably direct) of the annual average radon concentrations, which can be directly compared to the recommended reference levels. On this basis, the surveys should make possible the identification of dwellings with indoor radon above the reference levels and "radon priority areas" where significant proportion of the dwellings falls in this category. The performance of the CD/DVD method for radon measurements as a tool to address these issues is presented. A recent large scale field study based on the CD/DVD method that was carried out in the suburb area of Sofia, Bulgaria is described. Part of the studied area was affected in the past by the uranium mining and milling industry. In total 462 disks (CDs and DVDs) taken from 335 private dwellings from 10 districts in the region were analyzed. The results revealed the large heterogeneity in radon distribution in the area, with the percentage of dwellings with a 222Rn level above 300 Bq m-3 ranking from about 7% to 74%. The district of Yana, for which this percent was 74, was identified as the area of highest radon priority in the region. The paper also discusses how prompt identification of dwellings with radon above the reference level by CD/DVDs can be incorporated within an integrated approach to the radon problem. Within this approach the radon hazard is identified shortly after the stakeholder's decision to test, which allows fast solution of the problem without waiting the long (and usually demotivating) one-year period needed for direct results by the commonly used prospective methods.

Unperturbed, high spatial resolution measurement of Radon-222 in soil-gas depth profile.

This work presents a method for measuring the depth distribution of 222Rn activity in soil gas. The method is based on the capacity of polycarbonates to absorb 222Rn and on the possibility of performing sensitive measurements of 222Rn absorbed by the polycarbonates via liquid scintillation counting (LSC). The method is the following: cylindrical holes are drilled along a metal rod and Makrofol® N polycarbonate foils enclosed in polyethylene envelopes are placed in each hole. The rod is driven into the soil and kept for a certain time. As long as the rod is in the soil, the polycarbonate foils are exposed to the 222Rn concentration at their depth. At the end of the exposure the rod is pulled out and the foils are transferred to liquid scintillation (LS) vials filled with liquid scintillator. The 222Rn absorbed in the foils is then measured with a LS analyzer. The rod with the polycarbonate foils acts as a passive probe which senses the 222Rn concentration at different depths beneath the ground surface. The achievable minimum detectable 222Rn activity concentration with the equipment and conditions used in this study is around 12.5 kBq/m3. It can easily be lowered below 1 kBq/m3 if larger foils and low-background LS analyzers are used. Since the method does not require air sampling the depth distribution of 222Rn in the soil is unperturbed by the sampling. The spatial distribution and the maximum measurement depth are set by the distance between the holes and the depth to which the rod can be fixed into the ground. Results from in situ applications of the method in terrains with high 222Rn in soil-gas are reported, which demonstrate the feasibility and the usefulness of the proposed approach.

A NEW GENERATION OF PASSIVE RADON MONITORS: THE FILM-BADGES FOR OCCUPATIONAL EXPOSURES.

The passive radon monitors are typically formed by a radon-diffusion chamber, enclosing a track detector or an electret. Recently, new passive Rn monitors have been developed, which are similar to the neutron film badges. These badges present unique characteristics for the assessment of the occupational exposure to radon, such as compactness, fast-time response and any desired response sensitivity. Finally, these badges make it very easy to stop and to start the measurements, as required for assessment of the occupational exposures, which operations are very difficult, if not impossible, to achieve with existing monitors. These radon badges are based on the radon sorption by solid materials, namely plastics for radon absorption and activated carbon cloths for radon adsorption. Plastics may have a rubber-like (e.g. silicone) or a glass-like morphology (e.g. polycarbonate). The most interesting materials for these applications are the glass-like solids, the properties of which are expected to be little dependent on temperature. If radon badges with a large response sensitivity are desired, then adsorptive radiators formed by thin layers of activated carbon tissues are used. The key strategy, adopted for the radon film badges, was to use radiators into which radon diffuses rapidly, in order to ensure a fast-time response for radon monitoring. All the Rn film-badges, listed above, are formed by the same very compact device and may have response sensitivities, which may differ by several orders of magnitude.

RADON-222 IN SOIL-GAS MEASUREMENTS BY COMPACT DISCS. COMPARISON TO DIFFUSION CHAMBER MEASUREMENTS.

This work presents the results from simultaneous measurements of 222Rn in soil-gas by compact discs (CDs) and diffusion chambers. The measurements were performed in three terrains with high, medium and low 222Rn-in-soil-gas concentrations. Good correlations between the CD measurements and the reference diffusion chamber measurements are observed. The results indicate that it is important to apply temperature correction in the CD measurements, in order to account for the actual temperature during the exposure of the CDs in the soil.

THE CD/DVD METHOD AS A TOOL FOR THE HEALTH PHYSICS SERVICE AND VENTILATION DIAGNOSTICS IN UNDERGROUND MINES.

The CD/DVDs used as radon (222Rn) and thoron (220Rn) detectors can provide a sufficiently sensitive and cost-efficient option for passive radiation monitoring in underground mines. This note presents results of measurements made under real environmental conditions by CD/DVDs. Comparison with conventional diffusion chambers was made and good correspondence was observed. Correlation between 222Rn and 220Rn was studied by CD/DVDs and no signs for any correlation were observed. Dedicated study in a mine gallery showed that CD/DVDs can be successfully used for the purposes of ventilation diagnostics by identifying sources of air contaminated with radon.

Diffusion lengths and partition coefficients of 131mXe and 85Kr in Makrofol N and Makrofol DE polycarbonates.

This work presents the results of an experimental study of the Makrofol® N and Makrofol® DE polycarbonate foils absorption properties of 85Kr and 131mXe. The diffusion lengths of 85Kr and 131mXe in both types of foils are determined. The partition coefficients of 85Kr from air and water and that of 131mXe from air in Makrofol® N are determined. The partition coefficients of 85Kr from water and 131mXe from air in Makrofol® DE are also determined. The parameters are determined for T = 22°C and allow for the full characterization of sorption and desorption of 85Kr and 131mXe in the foils at this temperature. The results from this study highlight the remarkable absorption ability of Makrofol® and especially of the Makrofol® N foil and show that it surpasses the Makrofol DE® foil not only as a Rn absorber, but also as Kr and Xe absorber.

COMPARATIVE STUDY OF RADON AND THORON MEASUREMENTS IN FOUR ROMANIAN SHOW CAVES.

Measurements have been carried out using four types of passive detectors in four of the most popular show caves in Romania. Three types of detectors (RSKS, RadTrak and CD) were used for radon measurements and two (Raduet and CD) for thoron measurement. Activity concentrations in air were measured in the same locations for two seasons, autumn and winter. Measured values for the different caves varied between below detection limit (5 Bq m-3) and 4024 Bq m-3 for radon and from below 10 to 583 Bq m-3 for thoron. The results indicate a very good correlation between RSKS and RadTrak detectors (r = 0.96). The most significant difference between radon concentrations measured with different types of detectors (RSKS and CD) was higher than 150%. The study suggests that the activity concentration of radon in caves, measured using track detectors, could not be influenced by the type of detector used if the microclimate factor is acknowledged.

Laboratory facility to create reference radon + thoron atmosphere under dynamic exposure conditions.

Radon (222Rn) and thoron (220Rn) levels in the environment are typically subject to significant random and systematic variations. Creation in the laboratory of reproducible and controlled exposure conditions close to that in the real environment can be useful for testing 222Rn and 220Rn detectors and for research. In this report the design and performance of a novel laboratory facility with such functionality is presented. The facility allows the exposure of detectors under controlled dynamic as well as static activity concentrations of 222Rn and 220Rn (pure and mixed) and temperature. The temperature is measured and regulated within -15 °C ÷ +60 °C by a dedicated programmable thermostat. Different reference activity concentrations in the exposure vessel are made by regulating the flow-rate of the air that flushes 222Rn/220Rn activity from the sources towards the exposure vessel. Reference atmospheres that contain 222Rn, 220Rn or a specified ratio of the two can be created. Pilot experiments that demonstrate the feasibility of the approach are presented. They include follow-up of a pre-defined temperature profile (in the range -5 °C ÷ +35 °C), test of the correspondence between planned and measured 222Rn and 220Rn activity concentrations, follow-up of a pre-defined dynamic profile of 220Rn concentrations and test of the possibility to create mixed 220Rn/222Rn atmospheres (experimentally checked for ratio of the activity concentrations from 0.27 to 4.5). The results from the experimental tests are in agreement with the values obtained by the developed theoretical model. The proposed approach can be used to plan and create stationary and dynamic reference exposure conditions that are close to the real exposure regimes in the environment.

Determination of (222)Rn absorption properties of polycarbonate foils by liquid scintillation counting. Application to (222)Rn measurements.

This work demonstrates that a Liquid Scintillation Counting (LSC) technique using a Triple to Double Coincidence Ratio counter with extending dead-time is very appropriate for the accurate measurement of (222)Rn activity absorbed in thin polycarbonate foils. It is demonstrated that using a toluene-based LS cocktail, which dissolves polycarbonates, the (222)Rn activity absorbed in thin Makrofol N foil can be determined with a relative standard uncertainty of about 0.7%. A LSC-based application of the methodology for determination of the diffusion length of (222)Rn in thin polycarbonate foils is proposed and the diffusion length of (222)Rn in Makrofol N (38.9±1.3µm) and the partition coefficient of (222)Rn in Makrofol N from air (112±12, at 20°C) and from water (272±17, at 21°C) are determined. Calibration of commercial LS spectrometers for (222)Rn measurements by LSC of thin polycarbonate foils is performed and the minimum detectable activities by this technique are estimated.

Influence of the type of CD case on the track density distribution in CDs exposed to thoron.

A novel approach for retrospective thoron (Rn-220) measurements in buildings was recently proposed. It employs CDs/DVDs as detectors, in which the alpha-tracks formed by thoron's progeny Po-212 are analyzed. Compact disks and DVDs that had been stored in their cases are suitable, because the case provides a fixed and reproducible geometry of the Po-212 source. Since the measurement and calibration procedures involve analysis of different pieces of the disk, it is important to test the homogeneity of the track density over the disk area. This report presents results of such a study, in which disks in different containers were exposed to thoron. In almost all disks, the track density was inhomogeneous, increasing significantly near the holes in the container through which thoron could enter. However, as demonstrated, in disks regularly used and randomly rotated in their containers, the track density is expected to homogenize. It is concluded that the homogeneity of the tracks should be tested in disks exposed to thoron in homes and should be estimated or compensated in calibration exposures.

A high-sensitivity method for the measurement of 222Rn based on liquid scintillation counting of polycarbonate powder.

This work describes a technique for the measurement of 222Rn by absorption in polycarbonate (PC) powder and liquid scintillation counting (LSC). The work is an improvement of the recently proposed method for 222Rn measurements by LSC of exposed PC grains. It is demonstrated that the use of PC powder as a 222Rn sampler improves 13.6 times the sampling efficiency and leads to 6.5 times smaller minimmal detectable activity concentrations (MDAC) compared with the PC grains used so far. For a 40-h exposure of 7.4-g PC powder to 222Rn in air, the MDAC with a RackBeta 1219 LS counter is 62 Bq m(-3) (assuming a 8-h sample counting time and 24-h background time). For the same conditions the estimated 222Rn MDAC with a Quantulus 1220 LS counter is 20 Bq m(-3). The proposed technique is suitable for radon in air and radon in soil-gas measurements.

Liquid scintillation counting of polycarbonates: a sensitive technique for measurement of activity concentration of some radioactive noble gases.

This work explores the application of the liquid scintillation counting of polycarbonates for measurement of the activity concentration of radioactive noble gases. Results from experimental studies of the method are presented. Potential applications in the monitoring of radioactive noble gases are discussed.

Logistic of surveys of retrospective radon concentrations by home-stored CDs/DVDs.

Recently, a method for rather precise retrospective (222)Rn measurements, based on home-stored compact disks (CDs)/DVDs, has demonstrated a promising potential for wide application. In Bulgaria, pilot surveys have been initiated based on voluntarily provided CDs/DVDs. The results showed that large-scale surveys could be efficiently organised. However, several problems were identified and are discussed in the report. The first is the relatively small proportion of participants (30-50 %) that actually provided disks. Other addressed topics include the compatibility between results of different disks from one place, the accuracy of dating CDs/DVDs and the possibility for individual a posteriori calibration of each disk. The possibility to follow year-to-year variations by disks of different age is also discussed.

Determination of the diffusion coefficient and solubility of radon in plastics.

This paper describes a method for determination of the diffusion coefficient and the solubility of radon in plastics. The method is based on the absorption and desorption of radon in plastics. Firstly, plastic specimens are exposed for controlled time to referent (222)Rn concentrations. After exposure, the activity of the specimens is followed by HPGe gamma spectrometry. Using the mathematical algorithm described in this report and the decrease of activity as a function of time, the diffusion coefficient can be determined. In addition, if the referent (222)Rn concentration during the exposure is known, the solubility of radon can be determined. The algorithm has been experimentally applied for different plastics. The results show that this approach allows the specified quantities to be determined with a rather high accuracy-depending on the quality of the counting equipment, it can be better than 10 %.

Radon mapping by retrospective measurements - an approach based on CDs/DVDs.

This article points out the ability to map retrospective (222)Rn concentrations by home stored CDs/DVDs. The method employs the high radon absorption ability of the polycarbonate material of CDs and DVDs and their track-etch properties. The principle steps for the application of the method are addressed. The possibility for individual a posteriori calibration is studied, demonstrating that better than 10% accuracy in retrospective measurements is potentially achievable. Results from retrospective measurements in three different regions are shown, demonstrating the potential of the method for large-scale radon mapping. Comparison with independently evaluated retrospective (222)Rn concentrations in places with known radon history was made and very good correspondence was observed. The experience indicates that the method can be used for large scale retrospective radon mapping and its applications can be expanded towards mapping of radon concentrations in water and soil gas.

The compact disk as radon detector--a laboratory study of the method.

The radon absorption ability and the track etch properties of the polycarbonate material of commercial compact disks make them very useful as sensitive retrospective 222Rn detectors. The basic idea is to remove, after exposure, a surface layer that is thicker than the range of the alpha particles of the 222Rn and 220Rn progenies and to count the electrochemically etched tracks at the corresponding depths (>80 microm). The effects on the response due to differences in pressure, temperature, and humidity have been studied experimentally. The effect of the growing of 210Po after long-term exposures was also estimated. The effect of all listed factors except the temperature is either absent or restricted to maximum--about 10% for the very extreme cases. The variation of the response at 83 microm depth over the temperature interval 15-25 degrees C is +/-12% around the 20 degrees C value. The dependence of the calibration factor on the etched depth beneath the surface was studied at 4 different temperatures within the range expected indoors. The results show that the depth dependence is exponential with the parameters of the exponent also being dependent on the temperature. In practice, using the track density obtained in two or more depths beneath the compact disk's front surface, an a posteriori temperature correction could be made. By this correction it is possible to substantially reduce the bias in the results due to the unknown temperature during exposure. The results imply that by using home stored compact disks long-term retrospective 222Rn measurements could be made with an uncertainty that could be potentially better than 10%. The useful range of the method starts at about 3 Bq m(-3) (for 10 y exposure time) and appears to cover practically the whole range of indoors 222Rn concentrations.

Short-lived alpha sources of energies 6.0 MeV and 7.69 MeV for calibration purposes.

An approach for preparation of short-lived alpha sources of energy 6.0 MeV and 7.69 MeV is proposed. The sources are prepared by taking a sample of 222Rn progeny on an alpha spectrometric filter. The activities (or related parameters) of 218Po, 214Pb and 214Bi at the end of sampling are precisely determined by a reference measurement with an alpha spectrometer. Further they are used as input values to calculate with a sufficient precision the number of emitted alpha particles of any energy and at any time interval of interest. Theoretical modelling and experimental results demonstrated that such sources could be prepared with a sufficient purity. There is a potential for the number of alpha particles emitted in a given time interval to be certified with an accuracy of 1-2%.