Seasonal 7Be and 137Cs activities in surface air before and after the Chernobyl event

Seasonal fluctuations of cosmogenic (7)Be (T(1/2)=53.4 days) and anthropogenic (137)Cs (T(1/2)=30 years) activities in surface air (aerosols) have been extracted from a long data record (1972-2000) at high latitude (56 degrees N-68 degrees N, Sweden). Normalization to weekly average values was used to control long-term trends so that cyclical trends could be investigated. Enhanced (7)Be activity was observed in spring and summer seasons and likely relates to the seasonal thinning of the tropopause. Variations in the (137)Cs activity record seem to reflect how the isotope was injected in the atmosphere (stratospheric from bomb tests and tropospheric from the Chernobyl accident) and subsequent transport mechanisms. Accordingly, until 1986, the surface air (137)Cs activity was strongly related to nuclear weapons test fallout and exhibits temporal fluctuations resembling the (7)Be. Conversely, since 1986 the Chernobyl-produced (137)Cs dominates the long-term record that shows annual cycles that are strongly controlled by atmospheric boundary layer conditions. Additionally, short-term data within the post-Chernobyl period suggest subtle intrusion of air masses rich in (137)Cs that may occur throughout the year, and differences resulting from spatial occurrence at these latitudes. This is an important observation that may have to do with year-to-year variation and calls for caution when interpreting short-term data records.     

Measurements of short-lived cosmic-ray-produced radionuclides in rainwater

Cosmic-ray-produced (CP) nuclides with half-lives shorter than 21h were measured in rainwater by ultra-low-background gamma spectrometry at Ogoya Underground Laboratory. As levels of CP nuclides are extremely low and their half-lives are very short, quick sampling methods for a large volume of rainwater and rapid chemical separations by ion exchange method were developed. The nuclides measured were short-lived (24)Na, (28)Mg, (38)S, (38)Cl, (39)Cl, as well as nuclides with longer half-lives (7)Be and (22)Na. The number of atoms of CP nuclides in rainwater were evaluated to range from 30 to 1500L(-1) for (24)Na (n=16, mean; 520 [6.7mBqL(-1)]), 80 to 600L(-1) for (28)Mg (n=13, mean; 260 [2.4mBqL(-1)]), 400 to 1900L(-1) for (39)Cl (n=6, mean; 1200 [250mBqL(-1)]), 1x10(6) to 4x10(7)L(-1) for (7)Be (n=16, mean; 7x10(6) [1.05BqL(-1)]) and 2x10(3) to 1x10(5)L(-1) for (22)Na (n=9, mean; 2x10(4) [0.2mBqL(-1)]).     

Vertical distribution and inventories of 137Cs in the Syrian soils of the eastern Mediterranean region

Vertical distribution and inventories of (137)Cs have been determined using radiocesium distributions in presumably undistributed soil profiles, collected from 36 sites distributed all over Syria (eastern Mediterranean region). Vertical distributions of (137)Cs in the collected profiles were found to be strongly correlated with soil type and five groups were identified. Based on these profiles, total (137)Cs inventory (bomb test and Chernobyl) varied between 320 Bq m(-2) and 9,647 Bq m(-2). Geographical mapping of (137)Cs inventories showed that the highest values were found in the coastal, middle and north-east regions of Syria indicating that Chernobyl atmospheric contribution to the total (137)Cs deposition in the region is predominant. In contrast, the lowest values were found in the south-east region (Syrian Badia), where a relatively uniform distribution was observed, which may only be attributed to the past global nuclear bomb test. The measured inventories were also compared with a mathematical model for estimating bomb derived (137)Cs reference inventories.     

Estimating the date corresponding to the horizon of the first detection of 137Cs and 239+240Pu in sediment cores

The anthropogenic bomb fallout nuclides 137Cs and plutonium isotopes (240Pu, 239Pu) are important chronometers for the determination of recent sediment accumulation rates using sediment cores collected from various water bodies. One of the crucial time horizons used to date sediment core profiles corresponds to the date of first detection of these nuclides. Although atmospheric nuclear testing began during the mid-1940s, the year corresponding to a nuclide's first detection when measured in 2006 depends on a number of factors including fallout history, radioactive half-life, gamma/alpha detection limits, geographic latitude and the accumulated thickness of the sediment section. This paper reports estimations of the year of first detection in sediment profiles of fallout 137Cs and Pu measured by gamma and alpha spectrometry, respectively. We find that for the latitude 30-40 degrees south of the equator the year of first detection for 137Cs is 1955. The date is earlier in the northern hemisphere due to higher fallout rates. Due to better measurement sensitivity first detection of Pu is generally earlier than 137Cs by 1-2 years.     

Depositional records of plutonium and (137)Cs released from Nagasaki atomic bomb in sediment of Nishiyama reservoir at Nagasaki

In a sediment core of Nishiyama reservoir at Nagasaki city, depth profiles of (240)Pu/(239)Pu isotopic ratio, (239+240)Pu and (137)Cs activities were determined. Sediments containing plutonium and (137)Cs, which were deposited immediately after a detonation of Nagasaki atomic bomb, were identified in the core. Observed below the sediments were macroscopic charcoals, providing evidence for initial deposit of the fallout of the Nagasaki atomic bomb. This is the first entire depositional records of plutonium and (137)Cs released from the Nagasaki atomic bomb together with those from atmospheric nuclear tests.     

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.     

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.     

A 10-year study of the 137Cs distribution in soil and a comparison of Cs soil inventory with precipitation-determined deposition

During a 10-year period, 1988-1998, surface soil samples have been collected at Blentarp in southern Sweden and analysed for 137Cs from the Chernobyl accident and from the nuclear weapons tests. The distance between the sampling plots on the different sampling occasions has been no more than 3 m. The results show that the depth distribution of 137Cs is very similar for each of the sampling occasions, indicating that the caesium migration at this site is very small. The total activity measured in the soil cores is in agreement with the calculated activity of 137Cs deposited at the site after nuclear weapons tests and the Chernobyl accident, based on air activity concentration and the amount of precipitation. The calculated deposition of 137Cs originating from the bomb tests amounts to 1.41 kBq m-2 for the period 1962-1986, which is in agreement with the activity of nuclear weapons fallout measured in the soil samples (1.60 kBq m-2 as a mean value of the first four years of sampling). The calculated activity of 137Cs of Chernobyl origin was 0.79 kBq m-2, which agrees well with the value of 0.79 kBq m-2 measured in the soil samples in 1988.     

Effects of collector types in sampling of atmospheric depositional fluxes

The bulk gross alpha, gross beta and ⁷Be depositional fluxes were measured in Málaga (36.7°N, 4.5°W), a coastal Mediterranean station in the south of Spain for one whole year. In order to quantify the local variation of deposition rates, we have analysed the monthly results from two deposition collectors: a “pot “collector with a continuous water-covered surface and a “funnel” collector. In general, the alpha and beta depositional fluxes from the funnel collector were approximately two times lower than the pot collector. Whereas for the cosmogenic ⁷Be, the depositional flux of ⁷Be from funnel collector was also approximately two times lower than the pot collector. A good correlation of the depositional flux of ⁷Be has been obtained from both collectors.     

226Ra, 40K and 7Be activity concentrations in plants in the environment of Kaiga,India

Leaves, stem and bark samples from several plant species were collected from tropical forest of Kaiga, in the west coast of India where two nuclear power reactors of 220 MW each have just been commissioned and another two are under construction, and analysed for their (226)Ra, (40)K and (7)Be concentrations. The activities of (226)Ra and (40)K in plants were found to vary in the range BDL-13.2 and 12.0-797.3 Bq kg(-1), respectively. Plants show significant (7)Be activity in leaves, the activity varies in 72.5-1,060.8 Bq kg(-1). Stem and bark of plants show higher levels of (226)Ra and (40)K when compared to leaves. Soil-to-plant transfer factor for (226)Ra and (40)K were found to vary in the range BDL-0.37 and 0.09-5.61, respectively for different plants. The concentration of (226)Ra and (40)K in leaves depends on the age of the leaves.     

Contributing to shipping container security: can passive sensors bring a solution?

Illicit trafficking of fissionable material in container cargoes is recognized as a potential weakness in Nuclear Security. Triggered by the attacks of 11 September 2001, measures were undertaken to enhance maritime security in extension to the Safety Of Life At Sea Convention and in line with the US Container Security Initiatives. Effective detection techniques are needed that allow the inspector to intercept illicit trafficking of nuclear weapons components or components of other nuclear explosive devices. Many security measures focus on active interrogation of the container content by X-ray scan, which might be extended with the newly developed tagged neutron inspection system. Both active interrogation techniques can, with the current huge volume of container traffic, only be applied to a limited number of selected containers. The question arises whether a passive detection technique can offer an alternative solution. This study investigates if containers equipped with a small passive detector will register during transport the neutron irradiation by fissionable material such as plutonium in a measurable way. In practice, 4/5 of the containers are about 1/8 filled with hydrogenous material and undergo a typical 2 months route. For this reference case, it was found that the most compatible passive detector would be an activation foil of iridium. Monte-Carlo simulations showed that for the reference case the activity of a 250 μm thin foil with 6 cm² cross-section would register 1.2 Bq when it is irradiated by a significant quantity of Reactor-Grade PuO₂. However this activity drops with almost two orders of magnitude for other fillings and other isotopic compositions and forms of the Pu-source. The procedure of selecting the target material for Pu detection is detailed with the theoretical methods, in order to be useful for other applications. Moreover the value of such additional passive sensors for securing maritime container transport is situated within the global framework of the First, Second and Third Line of Defense against illicit trafficking.     

127I and 129I/127I isotopic ratio in marine alga Fucus virsoides from the North Adriatic Sea

The only stable iodine isotope is 127I and the natural 129I/127I ratio in the biosphere has increased from 10(-15)-10(-14) to 10(-10)-10(-9), mainly due to emissions from nuclear fuel reprocessing plants. In Europe they are located at La Hague (France) and Sellafield (England), where the ratio of 129I/127I is up to 10(-4). The marine environment, i.e. the oceans, is the major source of iodine with average concentrations of around 60 mirogL(-1) iodine in seawater. Brown algae accumulate iodine at high levels of up to 1.0% of dry weight, and therefore they are an ideal bioindicator for studying the levels of 127I and 129I in the marine environment. A radiochemical neutron activation analysis (RNAA) method, developed at our laboratory, was used for 129I determination in the brown alga Fucus virsoides (Donati) J. Agardh, and the same technique of RNAA was used for total 127I determination. The samples were collected along the coast of the Gulf of Trieste and the West coast of Istria in the North Adriatic Sea in the period from 2005 to 2006. Values of the 129I/127I ratio up to 10(-9) were found, which is in agreement with the present average global distribution of 129I. The levels of stable iodine found were in the range from 235 to 506 microg g(-1) and the levels of 129I from 1.7 to 7.3 x 10(-3)Bq kg(-1) (2.6-10.9 x 10(-7) microg g(-1)), on a dry matter basis.     

Level and origin of iodine-129 in the Baltic Sea

Environmental samples, such as seawater, seaweed, lake water, lake sediment and grass collected from the Baltic Sea area were analyzed for 129I and 127I by radiochemical neutron activation analysis. In 2000, the concentration of 129I in the seawater from Borholm and M?en in the Baltic Sea has reached 6.0 x 10(-13) and 16 x 10(-13) g/l, respectively, these are more than two orders of magnitude higher than the global fallout level. The highest value of 270 x 10(-13) g/l being found in the seawater from the Kattegat. By comparison of the level of 129I in the lake water and precipitation in this region, it is estimated that more than 95% of 129I in the Baltic Sea originates from reprocessing emissions, especially from the French nuclear fuel reprocessing plant at La Hague. More than 30% of 129I in the south Baltic and 93% in the Kattegat directly originates from the marine discharges of the European reprocessing plants.     

The transfer of 239/240Pu to cow milk

In summer 1993 we measured the transfer of (239/240)Pu to milk from herbage from a pasture located 5 km from the Chernobyl nuclear power plant. In one treatment cows were allowed to graze freely on the pasture. In a second treatment, cows were fed herbage collected from the pasture in stalls. The milk transfer coefficient; F(m) did not vary significantly between treatments and the mean value of 7.5x10(-6)d l(-1) was higher than previously reported values. Despite many values of F(m) for Pu in the literature we identified few relevant original data sets. Transfer coefficient values for Pu are only appropriate when used in conjunction with a specified time period or an appropriate model which allows for the biological half-life. We recommend for screening purposes an F(m) value of 1x10(-5)d l(-1) for Pu, with an order of magnitude lower value being appropriate for cows which are only exposed for one grazing season.     

Concentration measurements of 7Be at ground level air at Palermo, Italy-comparison with solar activity over a period of 21 years

Air activity concentrations of (7)Be in Palermo determined for the period January 1995-December 2002 by gamma-ray spectrometric analysis of particulate samples collected on paper filter by a high-volume sampler (approximately 900 m(3) h(-1)) are reported. The temporal behaviour of (7)Be concentration presents the same characteristics already observed in the measurements carried out over the previous 13-year (1982-1994) investigated period. The mean value of 5.06 mBq m(-3) obtained from the analysis of the 4636 particulate samples collected from 1982 to 2002 can be considered a representative value of (7)Be air concentration at ground level in our geographical zone. The comparison of long-term variation in the (7)Be concentrations with the cyclic solar activity-extended to the whole period of 21 years-confirms the inverse correlation between the two quantities.     

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.     

Classification of hot particles from the Chernobyl accident and nuclear weapons detonations by non-destructive methods.

Both after the Chernobyl accident and nuclear weapon detonations, agglomerates of radioactive material, so-called hot particles, were released or formed which show a behaviour in the environment quite different from the activity released in gaseous or aerosol form. The differences in their characteristic properties, in the radionuclide composition and the uranium and actinide contents are described in detail for these particles. While nuclear bomb hot particles (both from fission and fusion bombs) incorporate well detectable trace amounts of 60Co and 152Eu, these radionuclides are absent in Chernobyl hot particles. In contrast, Chernobyl hot particles contain 125Sb and 144Ce which are absent in atomic bomb HPs. Obvious differences are also observable between fusion and fission bombs' hot particles (significant differences in 152Eu/l55Eu, 154Eu/155Eu and 238Pu/239Pu ratios) which facilitate the identification of HPs of unknown provensence. The ratio of 239Pu/240Pu in Chernobyl hot particles could be determined by a non-destructive method at 1:1.5. A non-destructive method to determine the content of non-radioactive elements by Kalpha-emission measurements was developed by which inactive Zr, Nb, Fe and Ni could be verified in the particles.     

Precipitation scavenging of 7Be and 137Cs radionuclides in air

Atmospheric depositional fluxes of the naturally occurring 7Be of cosmogenic origin and 137Cs from fallout of the Chernobyl accident were measured over a 6-year period (January 1987-December 1992) at Thessaloniki, Greece (40 degrees 38'N, 22 degrees 58'E). Total precipitation accumulation during 1987-1992 varied between 33.7 cm and 65.2 cm, reflecting a relatively dry (precipitation-free) climate. The activity concentrations of 7Be and 137Cs in rainwater depended on the precipitation rate, being higher for low precipitation rates and lesser for high precipitation rates. 137Cs was removed by rain and snow more efficiently than 7Be. Snowfall was more efficient than rainfall in removing the radionuclides from the atmosphere. The annual bulk depositional fluxes of 7Be varied between 477 and 1133 Bq m(-2) y(-1) and this variability was attributed to the amount of precipitation and the variations of the atmospheric concentrations of 7Be. The annual bulk depositional fluxes of 137Cs showed a significant decrease over time from 1987 to 1992, resulting in a removal half-life of 1.33 years. The presence of 137Cs in air, and therefore in rainwater and snow, long after the Chernobyl accident (26 April 1986) was mainly due to the resuspension process. The normalized depositional fluxes of both radionuclides showed maximal values during the spring season where the maximum amount of precipitation occurred. The relatively high positive correlation between 7Be and 137Cs normalized depositional fluxes indicates that the scavenging process of local precipitation controlled the fluxes of both radionuclides. The dry depositional flux of 7Be was less than 9.37% of total (wet and dry) depositional flux. The fraction of dry-to-total depositional flux of 137Cs was much higher than that of 7Be, due to the resuspended soil.     

Transuranium radionuclide pollution in the waters of the La Maddalena National Marine Park

Following the grounding and subsequent explosion, in October 2003, of a nuclear submarine in the waters of the La Maddalena National Marine Park, fears arose of possible radioactive leakages. However, isotopic analyses on algae showed that the gamma-ray emitting artificial radionuclides that one might expect to leak from a damaged nuclear reactor (such as U-235, I-131, Cs-137) were absent, and that U-238/U-234 activities were in equilibrium with values typical of sea water; this excluded any direct anthropogenic contamination as a result of the accident. We used alpha autoradiographic techniques to detect possible traces of transuranium radionuclides; 160 samples of algae, granites, sea urchins, gastropods, limpets, cuttlefish and jellyfish were collected from the area, as well as from other Mediterranean coastlines and the Baltic Sea. All samples were autoradiographed, and selected samples further analysed by alpha spectrometry. There were no alpha track concentrations above background levels in our control Mediterranean specimens. In the samples from the La Maddalena and Baltic areas two different track distributions were observed: --those homogeneously distributed over the surfaces examined; --groups (10 to over 500) of radially distributed alpha tracks (forming "star" bursts, or "hot spots") emanating from point sources. By comparing radionuclide activities measured by alpha spectroscopy with alpha track densities, we extrapolated Pu activities for all samples. About 74% of algae had Pu activities of less than 1 Bq/kg and 0.25 Bq/kg, 16% had accumulated Pu to levels between 1 and 2 Bq/kg, and a very few specimens had concentrations between 2 and 6 Bq/kg. Plots showed that alpha tracks and stars concentrate around the northern and eastern margins of the Rada (Basin) di Santo Stefano, sites facing the nuclear submarine base on the eastern shore of the island of Santo Stefano. What is the source of these nuclides: last century's atmospheric nuclear testing, Chernobyl or a local source? Their concentrated, extremely localised occurrence seems difficult to explain in terms of left-over worldwide nuclear pollution. A local source seems more plausible.     

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.