Exerpts from the history of alpha recoils

Any confined air volume holding radon (²²²Rn) gas bears a memory of past radon concentrations due to ²¹⁰Pb (T_1/2 = 22 y) and its progenies entrapped in all solid objects in the volume. The efforts of quantifying past radon exposures by means of the left-behind long-lived radon progenies started in 1987 with this author’s unsuccessful trials of removing ²¹⁴Po from radon exposed glass objects. In this contribution the history and different techniques of assessing radon exposure to man in retrospect will be overviewed. The main focus will be on the implantation of alpha recoils into glass surfaces, but also potential traps in radon dwellings will be discussed. It is concluded that for a successful retrospective application, three crucial imperatives must be met, i.e. firstly, the object must persistently store a certain fraction of the created ²¹⁰Pb atoms, secondly, be resistant over decades towards disturbances from the outside and thirdly, all ²¹⁰Pb atoms analysed must originate from airborne radon only.For large-scale radon epidemiological studies, non-destructive and inexpensive measurement techniques are essential. Large-scale studies cannot be based on objects rarely found in dwellings or not available for measurements     

Seasonal variations of aerosol residence time in the lower atmospheric boundary layer

During a one year period, from Jan. 2002 up to Dec. 2002, approximately 130 air samples were analyzed to determine the atmospheric air activity concentrations of short- and long-lived (222Rn) decay products 214Pb and 210Pb. The samples were taken by using a single-filter technique and gamma-spectrometry was applied to determine the activity concentrations. A seasonal fluctuation in the concentration of 214Pb and 210Pb in surface air was observed. The activity concentrations of both radionuclides were observed to be relatively higher during the winter/autumn season than in spring/summer season. The mean activity concentration of 214Pb and 210Pb within the whole year was found to be 1.4+/-0.27 Bq m(-3) and 1.2+/-0.15 mBq m(-3), respectively. Different 210Pb:214Pb activity ratios during the year varied between 1.78 x 10(-4) and 1.6 x 10(-3) with a mean value of 8.9 x 10(-4) +/- 7.6 x 10(-5). From the ratio between the activity concentrations of the radon decay products 214Pb and 210Pb a mean residence time (MRT) of aerosol particles in the atmosphere of about 10.5+/-0.91 d could be estimated. The seasonal variation pattern shows relatively higher values of MRT in spring/summer season than in winter/autumn season. The MRT data together with relative humidity (RH), air temperature (T) and wind speed (WS), were used for a comprehensive regression analysis of its seasonal variation in the atmospheric air.     

The sources and fate of 210Po in the urban air: A review

The origin of ²¹⁰Po activity and its fluctuations in the air are discussed in this paper. In the case of atmospheric aerosol samples, a comparison of the ²¹⁰Po/²¹⁰Pb and ²¹⁰Bi/²¹⁰Pb activity ratios makes it possible not only to determine aerosol residence times but also to appraise the contribution of the unsupported ²¹⁰Po coming from other sources than ²²²Rn decay, such as human industrial activities, especially coal combustion. A simple mathematical method makes it possible to observe the seasonal fluctuations of the anthropogenic excess of ²¹⁰Po in the urban air. The average doses of ²¹⁰Po intake with food (including drinking water) and inhalation of urban aerosols are usually lower than those from ²¹⁰Po intake by cigarette smokers and negligible in comparison to total natural radiation exposure.     

Po-210 and Pb-210 as atmospheric tracers and global atmospheric Pb-210 fallout: a review

Over the past ∼5 decades, the distribution of ²²²Rn and its progenies (mainly ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Po) have provided a wealth of information as tracers to quantify several atmospheric processes that include: i) source tracking and transport time scales of air masses; ii) the stability and vertical movement of air masses iii) removal rate constants and residence times of aerosols; iv) chemical behavior of analog species; and v) washout ratios and deposition velocities of aerosols. Most of these applications require that the sources and sink terms of these nuclides are well characterized.Utility of ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Po as atmospheric tracers requires that data on the ²²²Rn emanation rates is well documented. Due to low concentrations of ²²⁶Ra in surface waters, the ²²²Rn emanation rates from the continent is about two orders of magnitude higher than that of the ocean. This has led to distinctly higher ²¹⁰Pb concentrations in continental air masses compared to oceanic air masses. The highly varying concentrations of ²¹⁰Pb in air as well the depositional fluxes have yielded insight on the sources and transit times of aerosols. In an ideal enclosed air mass (closed system with respect to these nuclides), the residence times of aerosols obtained from the activity ratios of ²¹⁰Pb/²²²Rn, ²¹⁰Bi/²¹⁰Pb, and ²¹⁰Po/²¹⁰Pb are expected to agree with each other, but a large number of studies have indicated discordance between the residence times obtained from these three pairs. Recent results from the distribution of these nuclides in size-fractionated aerosols appear to yield consistent residence time in smaller-size aerosols, possibly suggesting that larger size aerosols are derived from resuspended dust. The residence times calculated from the ²¹⁰Pb/²²²Rn, ²¹⁰Bi/²¹⁰Pb, and ²¹⁰Po/²¹⁰Pb activity ratios published from 1970’s are compared to those data obtained in size-fractionated aerosols in this decade and possible reasons for the discordance is discussed with some key recommendations for future studies.The existing global atmospheric inventory data of ²¹⁰Pb is re-evaluated and a ‘global curve’ for the depositional fluxes of ²¹⁰Pb is established. A current global budget for atmospheric ²¹⁰Po and ²¹⁰Pb is also established. The relative importance of dry fallout of ²¹⁰Po and ²¹⁰Pb at different latitudes is evaluated. The global values for the deposition velocities of aerosols using ²¹⁰Po and ²¹⁰Pb are synthesized.     

Activity concentrations of 226Ra, 228Ra, 210Pb, 40K and 7Be and their temporal variations in surface air

Activity concentrations of the long-lived natural radionuclides ²²⁶Ra, ²²⁸Ra, ²¹⁰Pb, ⁴⁰K and of ⁷Be in surface air were measured twice monthly at a semi-rural location 10 km north of Munich (FRG) for at least three years. For the time interval 1983–1985, all values were found to be distributed log-normally, with geometric means (in μBq m⁻³) of 1·2 for ²²⁶Ra, 0·5 for ²²⁸Ra, 580 for ²¹⁰Pb, 12 for ⁴⁰K and 3500 for ⁷Be. Reflecting their common origin, the activity concentrations of ²²⁶Ra and ⁴⁰K are correlated with surface air dust concentrations (geometric mean 59 μg m⁻³). Seasonal variations of ²¹⁰Pb and ⁷Be air activity concentrations are established for the time interval 1978–1985.The contribution of local soil activity to the air activity concentrations of these radionuclides and of natural uranium is discussed. Resuspension factors are found to be of the order of 10⁻⁹m⁻¹.     

Detection of 210Po on filter papers 16 years after use for the collection of short-lived radon progeny in a room

Radon gas was allowed to accumulate in its radium source and then injected into a 36 m(3) test room, resulting in an initial radon concentration of 15 kBq m(-3). Filter papers were used to collect the short-lived radon progeny and thus to measure the Potential Alpha Energy Concentration (PAEC) in-situ in the year 1984 at different times and conditions according to the experimental design. The radon progeny collected on the filter papers were studied as a function of aerosol particle concentration ranging from 10(2)-10(5) particles cm(-3) in three different experiments. The highest aerosol particle concentration was generated by indoor cigarette smoking. Those filters were stored after the experiment, and were used after 16 years to study the activity of the radon long-lived alpha emitter progeny, (210)Po (T(1/2)=138 days). This isotope is separated from the short-lived progeny by (210)Pb beta emitter with 22.3 years half-life. After 16 years' storage of these filters, each filter paper was sandwiched and wrapped between two CR-39 nuclear track detectors, to put the detectors in contact with the surfaces of different filters, for 337 days. Correlation between the PAEC measured using filter papers in the year 1984 and the activity of long-lived alpha emitter (210)Po on the same filter papers measured in the year 2000 were studied. The results of the (210)Po activity showed a very good correlation of 0.92 with the PAEC 16 years ago. The results also depict that the PAEC and (210)Po activity in indoor air increased with the increase of aerosol particle concentration, which shows the attachment of short-lived radon progeny with the aerosol particles. The experiment proves that indoor cigarette smoking is a major source of aerosol particles carrying radon progeny and, thus, indoor cigarette smoking is an additional source of internal radiation hazard to the occupants whether smoker or non-smoker.     

Radon transport through a cool-season grass

²²²Rn released by mature tall fescue (Festuca arundinacea Schreb.) growing on uranium mill wastes in a controlled environment was a direct function of leaf area and essentially unrelated to the quantity of water transpired by the plants. The quantity of ²²²Rn released by the grass blades at maturity was approximately 0·01 Bq m⁻² s⁻¹ (0·3 pCi m⁻² s⁻¹). We suggest that the radioactive gas is transported from the rooting medium to leaves by mass flow in liquid water, but from leaves to the atmosphere by a path generally independent of water, i.e., primarily through the leaf cuticle and epicuticular wax.     

Spatial and temporal distribution of lead-210 in the surface layers of the atmosphere

The levels of ²¹⁰Pb in surface air from about sixty locations and in rainwater from about forty locations, around the globe, are summarised in this report. The spatial, annual and long-term variations in the levels of ²¹⁰Pb are discussed. The concentrations vary as a function of the continentality of the locations and at many stations there is a seasonal variation. There is no significant long-term variation in activity levels, possibly indicating the absence of a major anthropogenic source of this nuclide. The activity ratio of ²²²Rn/²¹⁰Pb is around 6000 in India and varies seasonally depending on air mass source.     

Dynamic simulation of radon daughter concentrations in apartments using solar rockbed heat storage

In solar rockbed storage systems, heat is transferred during the day from the collector to a bed of pebbles, and released at night to warm the living space. When the rocks used for storage contain significant concentrations of uranium, ²²²Rn and its daughters may be released to the living area. A microcomputer model was used to simulate variations in air filtration rate and source strength through several days of operation. Source strengths were estimated from theoretical considerations and literature data. Resulting ²²²Rn and daughter concentrations were computed by solving system equations by fourth-order Runge-Kutta integration. During the day, when the living space is isolated from the radon source, interior ²²²Rn concentrations approach those of the outdoors. A nighttime steady-state concentration is approached about 6 h after heat discharge begins. Due to the dynamic nature of the simulation, equilibrium between ²²²Rn and its daughters is not reached. Time-weighted average nighttime exposures (6 p.m.–8 a.m.) for 10 simulation runs varied from 0.001 to 0.018 working level (WL). Comparison with one set of measurement data showed the model to overpredict concentrations but to approximate the ²²²Rn buildup rate well. Combinations of source strength, infiltration rate, and exterior radon concentration which would lead to exposures exceeding 0.02 WL were calculated.     

Contribution of (222)Rn-bearing water to indoor radon and indoor air quality assessment in hot spring hotels of Guangdong, China

This study investigates the contribution of radon (²²²Rn)-bearing water to indoor ²²²Rn in thermal baths. The ²²²Rn concentrations in air were monitored in the bathroom and the bedroom. Particulate matter (PM, both PM₁₀ and PM_2.5) and carbon dioxide (CO₂) were also monitored with portable analyzers. The bathrooms were supplied with hot spring water containing 66-260 kBq m⁻³ of ²²²Rn. The results show that the spray of hot spring water from the bath spouts is the dominant mechanism by which ²²²Rn is released into the air of the bathroom, and then it diffuses into the bedroom. Average ²²²Rn level was 110-410% higher in the bedrooms and 510-1200% higher in the bathrooms compared to the corresponding average levels when there was no use of hot spring water. The indoor ²²²Rn levels were influenced by the ²²²Rn concentrations in the hot spring water and the bathing times. The average ²²²Rn transfer coefficients from water to air were 6.2 × 10⁻⁴-4.1 × 10⁻³. The 24-h average levels of CO₂ and PM₁₀ in the hotel rooms were 89% and 22% higher than the present Indoor Air Quality (IAQ) standard of China. The main particle pollutant in the hotel rooms was PM_2.5. Radon and PM₁₀ levels in some hotel rooms were at much higher concentrations than guideline levels, and thus the potential health risks to tourists and especially to the hotel workers should be of great concern, and measures should be taken to lower inhalation exposure to these air pollutants.     

Possible effect of solar tides on radon signals

Large temporal variations of radon (²²²Rn) are often encountered in air in the geologic environment, at time scales from diurnal to annual. Interpretations as to the nature of these variations, unique to ²²²Rn, often invoke either above surface atmospheric variations, or the influence of subtle active geodynamic processes. So far the eventual geophysical drivers of the variation of ²²²Rn as well as its specific qualities enabling this temporal variation are not known. New insight on the temporal variation of ²²²Rn is gained by experimental simulation in confined air. Two short laboratory experiments, and one external experiment lasting over 3 years, were performed inside closed canisters and using natural and commercial ²²²Rn sources. Internal and external gamma and alpha detectors recorded variations of the radiation, up to around 20% of the equilibrium level. Radon signals of different time scale occurred with: a) periodic annual and semi-annual signals; b) non-periodic multi-day signals; c) periodic daily signals. Similar, related, inversely-related and dissimilar temporal patterns were manifested in the measured time series of the different sensors. Diurnal periodicity was dominated by the solar tide components S1, S2 and S3, exhibiting unlike relative amplitudes and different phases at the different sensors. A compound association occurs among the amplitudes and phases of the diurnal and seasonal periodicities of the daily ²²²Rn signal, linking the periodic phenomena to the rotation of earth around its axis and around the sun. ²²²Rn variation patterns in the frequency-time domain cannot be driven by the corresponding atmospheric variation patterns. These results, obtained under static and isolated conditions, are in disagreement with the expected radioactive equilibrium and its spatially uniform expression within and around the experimental volume. The external influence which drives the daily signals evolving from ²²²Rn inside the canister is non-atmospheric and seemed to be from a remote source and traversed a 5-cm thick lead shield. The similarities with observations on ²²²Rn signals from upper crustal levels imply that such an external influence, possibly as a component of solar irradiance, drives the ²²²Rn signals to a depth of at least 100 m. New combined prospects for the research are indicated in terms of the radioactive behavior of ²²²Rn in air and in terms of an above surface geophysical driver for this behavior.     

Size distributions and growth of natural and chernobylderived submicron aerosols in Tennessee

The median aerodynamic diameters of aerosol-associated SO₄²⁻, ²¹⁰Pb, ⁷Be, and Chernobyl-derived fission products in Tennessee were examined using high-volume cascade impactors. Regardless of season, the ‘steady-state’ size distributions of SO₄²⁻ shifted to larger sizes than found for either ²¹⁰Pb or ⁷Be, and for ⁷Be sizes showed a weaker seasonal dependency than for either SO₄²⁻ or ²¹⁰Pb. It is suggested that the size differences are the result of the different spatial distributions of these species in the atmosphere during aerosol formation and growth. The mean growth rate of aerosols between ≈0·2 μm and ≈0·4 μm was estimated to be ≈0·03 μm d⁻¹ from a comparison of the median diameter of ²¹⁰Pb when it is first produced from ²¹⁴Po decay with the median diameter after a mean atmospheric residence time of 7 d.Measurements of the size distributions of radioactive aerosols released during the nuclear reactor accident at Chernobyl were made in May and June 1986, and provided rare information on growth rates of aerosols released to the atmosphere over a short time period. A linear growth rate of ≈0·013 μm d⁻¹ was observed in the lower troposphere after the median diameter had reached ≈0·4 μm. Chernobyl-derived ^134,137Cs was less soluble than ⁷Be, suggesting the presence of an aerosol core derived from reactor constituents. An analysis of time intervals and trends in both concentrations and isotopic ratios, when compared to Soviet data on the time course of radioactive releases from the damaged reactor, suggested that the large releases which occurred in early May were an important component of the globally transported ¹³⁷Cs.     

The distribution of radon in tunnels with different geological characteristics in China

In China, as the economy is developing and the population is expanding, some underground buildings have been used as supermarkets, restaurants and entertainment places. Tunnels in mountains are one type of underground building, and the radon (²²²Rn) level in tunnels is an important issue. Radon levels in different type tunnels appear to differ, and relatively higher levels of ²²²Rn are associated with particular types of bedrock. The ²²²Rn levels in tunnels in five different geological characteristics were analyzed. Those built in granite had the highest ²²²Rn levels with a geometric mean (GM) of 280 Bq m⁻³, while those built in limestone (GM: 100 Bq m⁻³) and andesitic porphyry (GM: 96 Bq m⁻³) were lower. The sequence of ²²²Rn concentrations was: granite > tuff > quartz sandstone > limestone > andesitic porphyry, and the ²²²Rn in granite was statistically significantly higher than in limestone and andesitic porphyry. Tunnels built in granite, tuff, quartz sandstone, limestone tended to have higher ²²²Rn concentrations in summer than in winter, while the reverse tendency was true in andesitic porphyry tunnels. Only the difference in limestone was statistically significant.     

Nationwide indoor 222Rn and 220Rn map for India: a review

Considering the role of radon in epidemiology, an attempt was made to make a nation-wide map of indoor ²²²Rn and ²²⁰Rn for India. More than 5000 measurements have been carried out in 1500 dwellings across the country comprising urban and nonurban locations. The solid state nuclear track detectors based twin cup ²²²Rn/²²⁰Rn discrimination dosimeters were deployed for the measurement of indoor ²²²Rn, ²²⁰Rn and their progeny levels. The geometric means of estimated annual inhalation dose rate due to indoor ²²²Rn, ²²⁰Rn and their progeny in the dwellings was 0.94 mSvy⁻¹ (geometric standard deviation 2.5). It was observed that the major contribution to the indoor inhalation dose was due to indoor ²²²Rn and its progeny. However, the contribution due to indoor ²²⁰Rn and its progeny was not trivial as it was found to be about 20% of the total indoor inhalation dose rates. The indoor ²²²Rn levels in dwellings was significantly different depending on the nature of walls and floorings.     

Extraction of fallout 210Pb from soils and its distribution in soil profiles

Natural fallout ²¹⁰Pb may be extracted from soils with hot, dilute nitric acid without extracting significant quantities of ²¹⁰Pb produced by decay of radon in the soil. This method was used to determine the distribution of fallout ²¹⁰Pb in the profiles of nine New Zealand soils. The measured levels were similar to equilibrium cumulative depositions calculated from deposition records. The results indicate that these soils have quantitatively retained fallout ²¹⁰Pb, with 75–100% of it being concentrated in the top 10 cm of soil. This permanent retention of fallout lead by soils suggests that accumulation of lead in the upper soil layer is likely in areas of aerosol lead pollution.     

The temporal variations of (7)Be, (210)Pb and (210)Po in air in England

We have conducted measurements of naturally occurring radionuclides (7)Be, (210)Pb and (210)Po in air at ground level at Chilton, Oxfordshire, England. The sampling and analysis regime for the latter two isotopes has been optimised to minimise uncertainties in measurement due to decay of (210)Po and in-growth of (210)Pb during the sampling and analysis period. Analysis times were reduced by using Cerenkov counting to assay the (210)Bi daughter of (210)Pb. Monthly data collected over a four-year period are presented and discussed. (7)Be activity concentrations appear to peak in spring. (210)Pb activity concentrations also follow a seasonal trend reflecting different (222)Rn emanation rates from soil during winter and summer. Data for (210)Po show no such trend.     

Seasonal variations of 222Rn concentrations in the air of a tunnel located in Nagano city

The seasonal variation of 222Rn concentrations in the air of tunnels constructed during World War II at Nagano City has been investigated. The determination of 222Rn concentrations in tunnel air was performed using a solid-state nuclear track detector technique. The monthly radon concentrations changed smoothly, decreasing towards winter and increasing towards summer, and it was found that the concentrations strongly correlate with the temperature difference between the inside and the outside of the tunnel. In the innermost areas of the tunnel, the maximum concentration was observed in July, its value being about 6500 Bq m (-3). The concentrations of radon in the tunnel air decrease exponentially towards the openings of the tunnel, which indicates that the radon concentration in the tunnel is basically governed by diffusion and mixing of radon gas with air. These observations lead to the conclusion that the seasonal variation of the radon concentration in the tunnel air is mainly caused by a convection current due to a stack effect induced by the temperature difference between the tunnel air and the outside air.     

Seasonal variations of Rn concentrations in the air of a tunnel located in Nagano city

The seasonal variation of 222Rn concentrations in the air of tunnels constructed during World War II at Nagano City has been investigated. The determination of 222Rn concentrations in tunnel air was performed using a solid-state nuclear track detector technique. The monthly radon concentrations changed smoothly, decreasing towards winter and increasing towards summer, and it was found that the concentrations strongly correlate with the temperature difference between the inside and the outside of the tunnel. In the innermost areas of the tunnel, the maximum concentration was observed in July, its value being about 6500 Bq m (-3). The concentrations of radon in the tunnel air decrease exponentially towards the openings of the tunnel, which indicates that the radon concentration in the tunnel is basically governed by diffusion and mixing of radon gas with air. These observations lead to the conclusion that the seasonal variation of the radon concentration in the tunnel air is mainly caused by a convection current due to a stack effect induced by the temperature difference between the tunnel air and the outside air.     

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

This article points out the ability to map retrospective ²²²Rn 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 ²²²Rn 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.     

Development and calibration of a portable radon sampling system for groundwater Rn activity concentration measurements

The assembling of a system for field sampling and activity concentration measurement of radon dissolved in groundwater is described. Special attention is given in presenting the calibration procedure to obtain the radon activity concentration in groundwater from the raw counting rate registered in a portable scintillation detector and in establishing the precision of the activity concentration measurements. A field procedure was established and the system tested during one year of monthly observations of ²²²Rn activity concentration in groundwater drawn from two wells drilled on metamorphic rocks exposed at Eastern São Paulo State, Brazil. The observed mean ²²²Rn activity concentrations are 374 Bq/dm³ in one well and about 1275 Bq/dm³ in the other one. In both wells the ²²²Rn activity concentrations showed a seasonal variation similar to variations previously reported in the literature for the same region.