Factors controlling 7Be and 210Pb atmospheric deposition as revealed by sampling individual rain events in the region of Geneva, Switzerland

Bulk atmospheric deposition of 7Be and 210Pb has been measured at Versoix, close to Geneva, Switzerland. Collectors were continuously deployed from November 1997 through November 1998 for periods from 1 to 22 days depending on the frequency of rain. The activities of 7Be and 210Pb integrated over the sampling interval were moderately well correlated with rainfall (r2 of 0.66 and 0.55, respectively; p < 0.001) and well correlated one with the other (r2 of 0.91; p < 0.001). The 7Be/210Pb activity ratio is close to 13.5, except for samples collected in the periods of very low precipitation which have a distinctly lower ratio. A simple model accounting for rainfall, seasonal variations and reload of the local atmosphere after a rain event explains 90% of the variance of 7Be and 210Pb deposition. Concentrations of 210Pb and Ca++ in rain were correlated with transport time of air masses over the continent as indicated by reconstruction of air mass trajectories over three days.     

Seasonal and spatial variation of atmospheric 210Pb and 7Be deposition: features of the Japan Sea side of Japan

Monthly depositional fluxes of (210)Pb and (7)Be at Tatsunokuchi, Japan which faces the Japan Sea were studied over a 12-year period from 1991 to 2002. The data were compared with the spatial variability of these fluxes at Taejon in Korea and at 11 other sites in Japan from Ishigaki of the southern islands of Okinawa to Wakkanai of the northern end of Hokkaido over a 2-year period from 2000 to 2001. The monthly depositions of both (210)Pb and (7)Be at Tatsunokuchi revealed very similar seasonal variations with a single peak; both depositions were high in winter and low in summer. This phenomenon was found to be not transient but stationary. The deposition of these nuclides was much greater on the Japan Sea side of Japan than on the Pacific Ocean side. The cause for high deposition of (210)Pb and (7)Be in winter might be explained by a combination of a series of the following processes: blowing out of air masses with a high (210)Pb concentration near the surface layer over the continent by strong winter monsoons, additional flow of cold air masses with high (7)Be concentration at high latitude, well-mixing with generation of ascending current and convection clouds over the Japan Sea, and heavy snowfalls accompanying them.     

Factors influencing ambient concentrations of (210)Pb and (7)Be over the city of Edinburgh (55.9 degrees N, 03.2 degrees W)

Concentrations of (210)Pb and (7)Be in air were continuously monitored, using a high-volume air sampler and a high-resolution gamma-ray spectrometer, during the period of July 2002 to June 2003 at the University of Edinburgh 55.9 degrees N, 03.2 degrees W. The time series of both radio-isotopes show seasonality, dependence on air-mass origin, residence time and precipitation. Surface air concentrations of (210)Pb and (7)Be ranged from 0.01 to 0.74 mBq m(-3) and 0.63-6.54 mBq m(-3), respectively. The measurements indicate that the average concentrations of both (210)Pb and (7)Be in surface air were 0.21+/-0.01 and 2.50+/-0.04 mBq m(-3), respectively; which agrees closely with the corresponding values reported for coastal air measurements in Europe.     

7Be to 210Pb concentration ratio in ground level air in Belgrade area

7Be to 210Pb concentration ratios in ground level air on two monitoring stations (MS1 and MS2) in Belgrade area were determined from 1996 to 2001. The average monthly concentrations of 7Be in ground level air were in the range of 0.6-18.3 mBq/m3 and exhibited one or two summer/early fall maxims and one minimum in winter. The maximum concentrations for 210Pb were generally observed in the fall, with the average concentrations in the range of 1.09 x 10(-4) to 30.9 x 10(-4) Bq/m3. The 7Be/210Pb ratios were in the range of 1.7-12.7 (MS1) and 1.8-11.3 (MS2), with summer maxims and late fall/winter minimums. The mean Radionuclides Loading Indices values approach zero except for 1996/1997 (MS1) and 2001 (MS2) due to higher concentrations of 7Be and 210Pb. The mean monthly concentrations of both radionuclides exhibited lognormal distributions. There is significant correlation between the 7Be/210Pb activities ratio and the air stability classes A + B + C for both monitoring stations (correlation coefficients 0.61-0.65), and no correlation with D class and E + F classes. Correlation was found between the activity of 7Be and air stability classes A + B + C (0.46-0.68), and E + F (0.38 for MS1), while for 210Pb, a moderate correlation (0.38-0.40) was found with the E + F air stability classes.     

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.     

Formation of radioactivity enriched soils in mountain areas

A field study was carried out in the Mercantour Mountains at 2200 m altitude to investigate the processes of soil enrichment in atmospheric Chernobyl (137)Cs. Soils with high (137)Cs activities have been collected in the pasture areas with frequently measured (137)Cs activity values of the order of 7000 Bq m(-2). At some single spots (about 6% of the studied area), activity in soils reached 300000 Bq m(-2), which represents 44% of the (137)Cs of the total area. Data further showed that spatial distribution of Cs depends widely on its origin: Chernobyl Cs is mainly concentrated in "enriched" soils, whereas older Cs and (241)Am fallout from nuclear weapons tests (NWTs) and natural atmospheric (210)Pb in soils is less heterogeneously distributed.In order to elucidate the processes which have led to the enrichment in Chernobyl (137)Cs in the Alps in May of 1986, we have studied the repartition of atmospheric (7)Be isotope (half-life=53.3 d) in the pasture compartments (soil, litter, grass, and snow). Snow (7)Be data give evidence that fallout enrichment is related to snow accumulation (snow drift). The transfer of beryllium occurs rapidly to the grass and litter, where the strongest pollutant accumulations were measured. However, (7)Be transport to the soil required more than 8 months.     

Lead-210 and Beryllium-7 fallout rates on the southeastern coast of Brazil

Total ²¹⁰Pb and ⁷Be fallout rates were measured on the coastal region of Niteroi, Brazil. The monthly depositional flux of ²¹⁰Pb and ⁷Be varied by a factor of 26, from 1.7 to 43.3 mBq cm⁻² year⁻¹ and ∼27, from 7.5 to 203.5 mBq cm⁻² year⁻¹, respectively. The relatively large oscillations in the depositional flux of ²¹⁰Pb at this study site were likely due to variations in air mass sources, while the ⁷Be fluctuations may be driven by a combination of weather conditions. Local geology could support the periodic high fluxes of ²¹⁰Pb from continental air masses, as shifting oceanic wind sources were affirmed by the uncorrelated ²¹⁰Pb and ⁷Be fallout activities and ⁷Be/²¹⁰Pb ratios. The ²¹⁰Pb atmospheric deposition was found to be in agreement with local sediment inventories, an important consideration in geochemical studies that estimate sedimentation processes.     

The effect of air mass origin on the ambient concentrations of Be and Pb in Islamabad, Pakistan

Concentration of radionuclides ²¹⁰Pb and ⁷Be, having half lives of 22.3 years and 53.29 days, respectively, in the surface air samples of Islamabad (33.38° N, 73.10° E and Altitude ∼536 m asl.) are measured. The non-destructive technique of gamma-spectrometry, with a high purity germanium HPGe detector, was employed for the analysis of all samples. The annual average concentrations of ²¹⁰Pb and ⁷Be in the surface air samples were determined as 0.284 ± 0.15 and 3.171 ± 1.14 mBq m⁻³, respectively. Our results have shown a seasonal variation of the concentration of ⁷Be in air samples with high values for the spring season. High concentrations for ²¹⁰Pb are obtained when air masses originate from plain areas of Pothohar region, located in the South-West, West and North West of Islamabad. Our values of concentrations show a nice agreement with the relevant reported results.     

The distribution of 210Pb in human bone and its impact on methods for the retrospective estimation of 222Rn exposure from in vivo measurements

It is possible to estimate radon exposure to man retrospectively by the in vivo measurement of the decay product (210)Pb, which accumulates in the bones. For in vivo methods, knowledge of the distribution of (210)Pb in the skeleton is needed to determine the optimal site for measurement, the skull or the knee. In this study the activity of (210)Pb in a variety of bone samples from 3 individuals have been measured in vitro using underground gamma-ray spectrometry. The individuals were unlikely to have had elevated intakes of Rn. These measurements give baseline data on the bone massic activity of (210)Pb. They show that the massic activity is similar for each of these people and there are similar massic activities of (210)Pb in the skull and the knee of the 2 individuals for which the skull was measured. Additionally for 2 of the individuals trabecular and cortical bone were separated and massic activities were found to be strongly correlated indicating that the (210)Pb is associated with the hydroxyapatite.     

Vertical distributions of 210Pb excess, 7Be and 137Cs in selected grass covered soils in Southeast Queensland, Australia

Net accumulated areal activity densities and profiles of (210)Pb(ex), (7)Be and (137)Cs in the surface 10 cm of the soil are reported for eight sites in Southeast Queensland, Australia. Areal activity densities of (210)Pb(ex) and (7)Be varied from 1,080 to 4,100 Bqm(-2) and from 176 to 778 Bqm(-2), respectively. A significant (p < 0.001) portion of the variance (R(2) > 0.99) in their vertical distributions was explained by depth in the profile using an exponential function. Around 85% of accumulated (210)Pb(ex) was present in the surface 10 cm of the soil. Beryllium-7 was mainly confined to the grass and surface 2 cm of the soil. Average penetration half-depths of 3.6 +/- 0.2 and 0.3 +/- 0.1cm were determined for (210)Pb(ex) and (7)Be, respectively. Areal activity densities of global fallout (137)Cs varied from 10 to 361 Bqm(-2). Its signal was well mixed within the surface 10 cm. Comparison of the measured (137)Cs values to the estimated input value for the region ( approximately 490 Bqm(-2)) and profiling of a 1m deep soil core suggests a vertical migration of (137)Cs over the past decades. The paleo-radon activity flux determined from the (210)Pb(ex) areal activity density (5.1 +/- 0.9 mBqm(-2) s(-1)) was not statistically different to that measured using activated charcoal cups (5.5 +/- 0.4 mBqm(-2) s(-1)), tending to suggest that Southeast Queensland is neither a net source nor a net sink of (210)Pb-bearing aerosols.     

Activities of 210Po and 210Pb in the water column at Kuala Selangor, Malaysia

Natural radionuclides, such as (210)Po and (210)Pb were measured in the water samples collected from six stations at Kuala Selangor, Malaysia. Results for (210)Po and (210)Pb in dissolved and particulate phases have showed the difference in distribution and chemical behavior. The fluctuation activities of (210)Po and (210)Pb depend on wave action, geology and degree of fresh water input occurring at study areas and probably due to different sampling dates. The distribution coefficient, K(d), values of (210)Po and (210)Pb ranged from 2.0 x 10(3)lg(-1) to 265.15 x 10(5)lg(-1), and from 3.0 x 10(3)lg(-1) to 558.16 x 10(5)lg(-1), respectively. High K(d) values of (210)Po and (210)Pb indicated that a strong adsorption of (210)Po and (210)Pb onto suspended particles, and the sinking of both nuclides on the seabed at study locations were controlled by the characteristics of suspended particles.     

Comparative trends and seasonal variation of ⁷Be, ²¹⁰Pb and ¹³⁷Cs at two altitude sites in the central part of France

The atmospheric concentrations of ¹³⁷Cs, ²¹⁰Pb, and ⁷Be were measured over a three-year period at two research stations located less than 12 km apart and at different altitudes (puy de Dôme, 1465 m a.s.l. and Opme, 660 m a.s.l., France). Seasonal trends in all radionuclides were observed at both stations, with high concentration measured during the summer and low concentrations during the winter. The ²¹⁰Pb concentrations at both stations were similar to each other. Higher concentrations of both ⁷Be and ¹³⁷Cs were measured at puy de Dôme than at Opme. These observations can be explained by the stratospheric and upper tropospheric sources of ⁷Be and the long-range transportation of ¹³⁷Cs at high altitudes. Air mass origins during sampling periods were classified into several groups by their route to the stations (marine, marine modified, continental and mediterranean). We observed that ⁷Be concentrations were constant regardless of the air mass origins, unlike ¹³⁷Cs and ²¹⁰Pb concentrations that increased when influenced by continental air masses. Higher ⁷Be concentrations were observed when air masses were arriving from the upper troposphere than from the boundary layer, the opposite was observed for ¹³⁷Cs. The temporal trend in concentrations of ⁷Be shows good agreement with previous modelling studies suggesting that there is a good understanding of its sources and the atmospheric vertical mixing of this radionuclide. The sources and mixing of ²¹⁰Pb, however, seem to be more complex than it appeared to be in previous modelling studies.     

Temporal changes of 7Be, 137Cs and 210Pb activity concentrations in surface air at Monaco and their correlation with meteorological parameters

Results of analysis of ⁷Be, ¹³⁷Cs and ²¹⁰Pb on aerosol filters carried out from 1998 to 2010 in Monaco show that a weak correlation between activity concentrations of these radionuclides in the atmosphere and meteorological parameters has been found for ⁷Be and temperature (r = 0.50), ²¹⁰Pb and temperature and humidity (r = 0.43 and 0.41, respectively), and ¹³⁷Cs and precipitation (r = 0.51). The minimum and maximum ⁷Be activity concentrations were observed during 2000 and 2009, corresponding with the maximum and minimum solar activity, respectively. The maximum ¹³⁷Cs activity concentration found in May-June 1998 was due to the accident at Algeciras in Spain. The deposition velocities of ⁷Be, ¹³⁷Cs and ²¹⁰Pb depended on the precipitation rate, and attained maximum values during dry seasons. The investigated radionuclides may be used as atmospheric tracers, especially in long-term periods.     

Relationship between variations of Be, Pb and Pb concentrations and sub-regional atmospheric transport: Simultaneous observation at distant locations

In order to investigate the applicability of ²¹²Pb as a tracer for atmospheric transport in the sub-regional scale (few hundred kilometers in horizontal direction and up to ∼1 km by height), we measured the air concentrations of the short-lived radionuclide ²¹²Pb along with the long-lived ⁷Be and ²¹⁰Pb near the ground surface. For this purpose, simultaneous observations were continued for several days at three locations: a reference point representative for standard land surface atmosphere conditions, a second location at an altitude 650 m near the reference point, and on a solitary island ∼180 km from the reference point. Measurements of radioactivity in aerosol particle samples collected at intervals of 2-3 h with a high-volume air sampler were performed by extremely low background gamma-ray spectrometry with the use of Ge detectors located at the Ogoya Underground Laboratory. Concentration of ⁷Be or ²¹⁰Pb and their variation patterns was found to be similar among the three points during the whole observation period except for moment of the passage of a cold front. The results indicate that distributions of concentrations of the long-lived nuclides were uniform in this range. On the other hand, concentration levels and the variation patterns of the short-lived ²¹²Pb differed greatly from one location to another, reflecting differences in geographical location and altitude of the observation points. Additionally, there were certain indications that observed concentration of ²¹²Pb contained two components: an autogenous component from sources nearby and a heterogenous one from faraway sources carried by atmospheric horizontal transport. Results of this study provide experimental proof that ²¹²Pb can be used as a tracer of sub-regional atmospheric transport.     

Study of 210Po and 210Pb in the riverine environments of coastal Karnataka

Activity of ²¹⁰Po and ²¹⁰Pb were measured in soil and sediment samples collected from the major rivers Kali, Sharavathi and Netravathi of Coastal Karnataka. The activity of these two radionuclides were determined by radiochemical separation of ²¹⁰Po and counting the activity using a ZnS(Ag) Alpha counter. The activity of ²¹⁰Pb was higher than that of ²¹⁰Po in the riverine environs. The ²¹⁰Po and ²¹⁰Pb content in sediment was found to increase with silt/clay and organic matter contents. However no significant correlation was found between the activity ²¹⁰Po and ²¹⁰Pb with pH in sediments. The activity of ²¹⁰Po and ²¹⁰Pb and influence of physico-chemical parameters on these radionuclides were studied and discussed in this paper.     

Determination of radionuclide levels in rainwater using ion exchange resin and γ-spectrometry

The evaluation of radioactivity accidentally released into the atmosphere involves determining the radioactivity levels of rainwater samples. Rainwater scavenges atmospheric airborne radioactivity in such a way that surface contamination can be deduced from rainfall rate and rainwater radioactivity content. For this purpose, rainwater is usually collected in large surface collectors and then measured by γ-spectrometry after such treatments as evaporation or iron hydroxide precipitation. We found that collectors can be adapted to accept large surface (diameter 47 mm) cartridges containing a strongly acidic resin (Dowex AG 88) which is able to quantitatively extract radioactivity from rainwater, even during heavy rainfall. The resin can then be measured by γ-spectrometry. The detection limit is 0.1 Bq per sample of resin (80 g) for ¹³⁷Cs. Natural ⁷Be and ²¹⁰Pb can also be measured and the activity ratio of both radionuclides is comparable with those obtained through iron hydroxide precipitation and air filter measurements. Occasionally ²²Na has also been measured above the detection limit. A comparison between the evaporation method and the resin method demonstrated that 2/3 of ⁷Be can be lost during the evaporation process. The resin method is simple and highly efficient at extracting radioactivity. Because of these great advantages, we anticipate it could replace former rainwater determination methods. Moreover, it does not necessitate the transportation of large rainwater volumes to the laboratory.     

Distribution of fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) in soils of Taiwan

Depth profiles and cumulative deposition of four fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) were determined in presumably undisturbed soils in Taiwan. Inventories of these radionuclides in different areas correlate significantly with each other (except 7Be) and with mean annual rainfall, providing a necessary condition for the development of soil erosion studies in Taiwan. However, the data show very large spatial variability between and within landscape units, reflecting the steep topographic and meteorological gradients in the island. Thus, the application of fallout radionuclides to study soil conservation in Taiwan is expected to be a demanding task; it will call for dense sampling even at undisturbed reference sites.     

Determination of strontium-90 in deer bones by liquid scintillation spectrometry after separation on Sr-specific ion exchange columns

The activity concentration of (90)Sr was determined in several deer bones from Austria. Strontium specific ion exchange columns with 4',4'(5')-di-t-butylcyclohexane-18-crown-6 from Eichrom Industries, Inc. were used for separation. The yield of the chemical procedure was quantified with AAS. Directly after column separation, the solution containing (90)Sr was mixed with the scintillation cocktail HiSafe III and measured by liquid scintillation counting. Prevention of (210)Pb contamination and reusability of the separation columns was investigated as well as the activity distribution within the bones. Results were compared with pre-Chernobyl measurements in Austria; a correlation between activity concentration of (90)Sr and site altitude was found.     

Biomonitoring of ²¹⁰Po and ²¹⁰Pb using lichens and mosses around coal-fired power plants in Western Turkey

Mosses and lichens are useful biological indicators of environmental contamination for a variety of metals and radionuclides of both natural and artificial origin. These plants lack a well-developed root system and rely largely on atmospheric deposition for nourishment. Therefore in the study, different lichens (Cladonia convoluta, Cladonia foliacea) and mosses (Homalothecium sericeum, Hypnum lacunosum, Hypnum cupressiforme, Tortella tortuosa, Didymodon acutus, Syntrichia ruralis, Syntrichia intermedia, Pterogonium graciale, Isothecium alopecuroides, Pleurochatae squarrosa) were collected around the Yata?an (Mu?la), Soma (Manisa), Seyitömer - Tunçbilek (Kütahya) coal-fired power plants and investigated for potential use as biomonitors for ²¹⁰Po and ²¹⁰Pb deposition. While the activity concentrations of ²¹⁰Po and ²¹⁰Pb in lichens are in the ranges of 151 ± 7-593 ± 21 and 97 ± 5-364 ± 13 Bq kg⁻¹, for mosses the ranges for ²¹⁰Po and ²¹⁰Pb are 124 ± 5-1125 ± 38 and 113 ± 4-490 ± 17 Bq kg⁻¹, respectively. In the study, the moss samples were observed to accumulate more ²¹⁰Po and ²¹⁰Pb compared to lichens. While the most suitable biomonitor was a moss species (H. lacunosum) for Yata?an (Mu?la), it was another moss species (S. intermedia) for Soma (Manisa) and Seyitömer - Tunçbilek (Kütahya) sites. ²¹⁰Po concentrations were found higher than ²¹⁰Pb concentrations at the all sampling stations.     

Dust is the dominant source of “heavy metals” to peat moss (Sphagnum fuscum) in the bogs of the Athabasca Bituminous Sands region of northern Alberta

Sphagnum fuscum was collected from twenty-five ombrotrophic (rain-fed) peat bogs surrounding open pit mines and upgrading facilities of Athabasca Bituminous Sands (ABS) in northern Alberta (AB) in order to assess the extent of atmospheric contamination by trace elements. As a control, this moss species was also collected at a bog near Utikuma (UTK) in an undeveloped part of AB and 264 km SW of the ABS region. For comparison, this moss was also collected in central AB, in the vicinity of the City of Edmonton which is approximately 500 km to the south of the ABS region, from the Wagner Wetland which is 22 km W of the City, from Seba Beach (ca. 90 km W) and from Elk Island National Park (ca. 45 km E). All of the moss samples were digested and trace elements concentrations determined using ICP-SMS at a commercial laboratory, with selected samples also analyzed using instrumental neutron activation analysis at the University of Alberta.The mosses from the ABS region yielded lower concentrations of Ag, As, Bi, Cd, Cu, Pb, Sb, Tl, and Zn compared to the moss from the Edmonton area. Concentrations of Ni and Mo in the mosses were comparable in these two regions, but V was more abundant in the ABS samples. Compared with the surface vegetation of eight peat cores collected in recent years from British Columbia, Ontario, Quebec and New Brunswick, the mean concentrations of Ag, As, Bi, Cd, Cu, Mo, Ni, Pb, Sb, Tl and Zn in the mosses from the ABS region are generally much lower. In fact, the concentrations of these trace elements in the samples from the ABS region are comparable to the corresponding values in forest moss from remote regions of central and northern Norway.Lithophile element concentrations (Ba, Be, Ga, Ge, Li, Sc, Th, Ti, Zr) explain most of the variation in trace metal concentrations in the moss samples. The mean concentrations of Th and Zr are greatest in the moss samples from the ABS region, reflecting dust inputs to the bogs from open pit mines, aggregate quarries, and gravel roads. Linear regressions of V, Ni, and Mo (elements enriched in bitumen) versus Sc (a conservative, lithophile element) show excellent correlations in the mosses from the ABS region, but this is true also of Ag, Pb, Sb and Tl: thus, most of the variation in the trace metal concentrations can be explained simply by the abundance of dust particles on the plants of this region. Unlike the moss samples from the ABS region and from UTK where Pb/Sc ratios resemble those of crustal rocks, the moss samples from the other regions studied yielded much greater Pb/Sc ratios implying significant anthropogenic Pb contributions at these other sites.