Meteoric 10Be in aerosol filters in the city of Seville.

Cosmogenic radionuclides in the one-million-year half-life range, like 10Be, find application fields in several Sciences. They are powerful tools in Geology and Geochronology, as they are very important tracers on the Earth, being utilized as chronometer. Meteoric 10Be (T1/2 = 1.39 × 106 y) associated to aerosols can be used as a tracer of atmospheric processes and specifically as indicators of the cosmogenic interactions in lower Stratosphere, upper Troposphere, the air exchange between both and deposition processes on the Earth surface. The applications of 10Be are even more relevant when combined with other radionuclides such as 26Al. In order to provide new data about concentration 10Be in this type of samples, the first atmospheric air filters in Spain have been analysed. Values around 104 at/m3 (atoms per cubic meter of air) for 10Be have been obtained. Due to the location and the features of the sampling site (urban area, at sea level and mid latitude), a new radiochemical procedure was designed and developed in our laboratory for the Accelerator Mass Spectrometry (AMS) measurement of 10Be in this kind of samples. The samples were measured in SARA, the 1 MV AMS system at Centro Nacional de Aceleradores (CNA).

Determination of denudation rates by the measurement of meteoric 10Be in Guadiana river sediment samples (Spain) by low-energy AMS.

The concentration of meteoric 10Be in estuarine sediment samples has been measured by Spanish Accelerator for Radionuclides Analysis (SARA) at CNA and subsequently used to assess the denudation rate in Guadiana river basin together with the sediment budget method, on both sides of the frontier between Spain and Portugal. The two methods yielded coincident results. The estimation by the 10Be method gave the denudation rate of (0.76 ±â€¯0.10) × 10-2 cm/y. After correcting for an approximate 80% attenuation of the sediment discharge into the ocean, caused by the river dams, the sediment budget method yielded the rate of (0.77 ±â€¯0.17) × 10-2 cm/y.

Natural and artificial radionuclides in a marine core. First results of 236U in North Atlantic Ocean sediments.

There are very few data available of 236U in marine sediment cores. In this study we present the results from the first oceanic depth profile of 236U in a sediment core sampled in the North Atlantic Ocean, at the PAP site (4500 m depth, Porcupine Abyssal Plain (PAP) site, 49°0' N, 16°30' W). Additionally, the sediment core was radiologically characterized through the measurement of anthropogenic 137Cs, 239Pu, 240Pu, 129I and 14C and natural 210Pb, 40K and 226Ra. The measured 236U concentrations decrease from about 90·106 at g-1 at the seafloor down to 0.5·106 at g-1 at 6 cm depth. They are several orders of magnitude lower than the reported values for soils from the Northern Hemisphere solely influenced by global fallout (i.e. from 2700·106 to 7500·106 at g-1). 236U/238U atom ratios measured are at least three orders of magnitude above the estimated level for the naturally occurring dissolved uranium. The obtained inventories are 1·1012 at m-2 for 236U, 80 Bq m-2 for 137Cs, 45 Bq m-2 for 239+240Pu and 2.6·1012 at m-2 for 129I. Atomic ratios for 236U/239Pu, 137Cs/236U and 129I/236U, obtained from the inventories are 0.036, 0.11 and 2.5 respectively. Concentration profiles show mobilization probably due to bioturbation from the abundant detritivore holothurian species living at the PAP site sea-floor. The range of 236U, 137Cs, 239+240Pu and 129I values, inventories and ratios of these anthropogenic radionuclides are more similar to the values due to fall-out than values from a contribution from the Nuclear Fuel Reprocessing Plants dispersed to the south-west of the North Atlantic Ocean. However, signs of an additional source are detected and might be associated to the nuclear wastes dumped on the Eastern North Atlantic Ocean.

Estimating the impact from Fukushima in Southern Spain by 131I and Accelerator Mass Spectrometry detection of 129I.

After the Fukushima accident, large amounts of radionuclides were discharged to the atmosphere. Some of them travelled long distances and were detected in places as far from Japan as Spain a few days after the accident. One of these radionuclides was 131I. Its isotope 129I (T1/2 = 15.7 × 106 years) was also expected to follow the same pathway. In this work, we present the results for the 129I concentration in the same atmospheric samples from Seville (Spain) where 131I activity was measured in 2011 by Baeza et al. (2012). 129I concentrations in aerosol and gaseous samples showed concentrations in the order of 104 and 105 atoms/m3, typically higher in the gaseous form with respect to the aerosol form. Also 129I in rainwater was measured, showing concentrations in the order of 108 atoms/L. The results show a very good agreement with the 131I profile, showing that, if background from other sources is not relevant, it is possible to estimate the impact of similar events years after them thanks to the sensitivity of techniques like Accelerator Mass Spectrometry.

The behaviour of ¹²9I released from nuclear fuel reprocessing factories in the North Atlantic Ocean and transport to the Arctic assessed from numerical modelling.

A quantitative evaluation of the fate of (129)I, released from the European reprocessing plants of Sellafield (UK) and La Hague (France), has been made by means of a Lagrangian dispersion model. Transport of radionuclides to the Arctic Ocean has been determined. Thus, 5.1 and 16.6 TBq of (129)I have been introduced in the Arctic from Sellafield and La Hague respectively from 1966 to 2012. These figures represent, respectively, 48% and 55% of the cumulative discharge to that time. Inventories in the North Atlantic, including shelf seas, are 4.4 and 13.8 TBq coming from Sellafield and La Hague respectively. These figures are significantly different from previous estimations based on field data. The distribution of these inventories among several shelf seas and regions has been evaluated as well. Mean ages of tracers have been finally obtained, making use of the age-averaging hypothesis. It has been found that mean ages for Sellafield releases are about 3.5 year larger than for La Hague releases.

New insights on the role of sea ice in intercepting atmospheric pollutants using (129)I.

Measurements of (129)I carried out on sea ice samples collected in the central Arctic Ocean in 2007 revealed relatively high levels in the range of 100-1400×10(7) at L(-1) that are comparable to levels measured in the surface mixed layer of the ocean at the same time. The (129)I/(127)I ratio in sea ice is much greater than that in the underlying water, indicating that the (129)I inventory in sea ice cannot be supported by direct uptake from seawater or by iodine volatilization from proximal (nearby) oceanic regimes. Instead, it is proposed that most of the (129)I inventory in the sea ice is derived from direct atmospheric transport from European nuclear fuel reprocessing plants at Sellafield and Cap La Hague. This hypothesis is supported by back trajectory simulations indicating that volume elements of air originating in the Sellafield/La Hague regions would have been present at arctic sampling stations coincident with sampling collection.

Influence of releases of (129)I and (137)Cs from European reprocessing facilities in Fucus vesiculosus and seawater from the Kattegat and Skagerrak areas.

(129)I is a very long-lived radionuclide (T1/2=15.7×10(6) years) that is present in the environment because of natural and anthropogenic sources. Compared to the pre-nuclear era, large amounts of (129)I have been released to the marine environment, especially as liquid and gaseous discharges from two European reprocessing facilities located at Sellafield (England) and La Hague (France). The marine environment, i.e., the oceans, is the major source of iodine. Brown seaweed accumulates iodine at high levels up to 1.0% of dry weigh, and therefore they are ideal bioindicators for studying levels of (129)I. In this work, (129)I concentrations have been determined in seaweed Fucus vesiculosus and seawater collected in the Kattegat and Skagerrak areas in July 2007. The resulting data were evaluated in terms of (129)I concentrations and (129)I/(137)Cs ratios. (129)I concentrations were found to be in the order of (44-575)×10(9) atoms g(-1) in seaweed and (5.4-51)×10(9) atoms g(-1) in seawater, with an enhancement in the Skagerrak area in comparison to the Kattegat area. Iodine-129 concentrations in both seaweed and seawater were used to determine the concentration factor of iodine in brown seaweed F. vesiculosus. The high levels of (129)I and (129)I/(137)Cs ratios in the Skagerrak area and their gradually decreasing trend to the Kattegat indicates that the most important contribution to the (129)I inventory in those areas comes from Sellafield and La Hague reprocessing plants.

Pre- and post-Chernobyl accident levels of 129I and 137Cs in the Southern Baltic Sea by brown seaweed Fucus vesiculosus.

(129)I is a very long-lived radionuclide (T(1/2) = 15.7 × 10(6) years) that is present in the environment both because of natural and anthropogenic sources. In this work (129)I concentration and (129)I/(127)I ratio have been determined in seaweed Fucus vesiculosus collected in the Southern Baltic Sea during 1982 and 1986 (post-Chernobyl accident). The resulting data were evaluated in terms of (129)I concentrations, (129)I/(127)I and (129)I/(137)Cs ratios. (129)I concentrations were found to be in the order of (0.82-5.89) × 10(9) atoms g(-1) in 1982 and (1.33-38.83) × 10(9) atoms g(-1) in 1986. The (129)I/(127)I ratios ranged from (22.7-87.8) × 10(-10) for seaweed collected in 1982 and from (26.1-305.5) × 10(-10) for seaweed collected in 1986. Also a linear relationship was established for (127)I concentrations in seawater and salinity in this area, enabling the estimation of concentration factors for (127)I in F. vesiculosus. The high levels of (129)I and (129)I/(127)I in the Kattegat and their gradually decreasing trend to the Baltic Sea indicates that the most important contribution to the (129)I inventory in the Baltic Sea area comes from Sellafield and La Hague reprocessing plants. With respect to Chernobyl accident, (129)I concentrations in samples collected in 1986 were not much higher than those expected in less contaminated samples from 1982. This supports the view that the contribution of the Chernobyl accident to (129)I in the Baltic region was not significant.

129I measurements on the 1MV AMS facility at the Centro Nacional de Aceleradores (CNA, Spain).

The AMS system at CNA has been the first 1MV compact AMS system designed and manufactured by HVE. In this paper we present the experimental set-up for (129)I measurements in this facility. Charge state +3 has been selected at high-energy side and an optimum stripper pressure of 6×10(-3)mbar of argon (mass thickness of about 0.15µgcm(-2)) has been reached to obtain lowest blank values ((129)I/(127)I≅3×10(-13)). The measurements of the reference materials provided by the IAEA have demonstrated the viability of this facility to make routine measurements of (129)I at environmental levels. This blank value obtained is enough for the measurement of most environmental samples and comparable with other reported backgrounds obtained in facilities working at higher energies and higher charge states.

Level and origin of 129I and 137Cs in lichen samples (Cladonia alpestris) in central Sweden.

Lichen is a symbiosis between algae and fungi. They have for decades been used as bioindicators for atmospheric deposition of heavy metals, organic compounds and radioactive elements. Especially the species Cladonia alpestris and Cladonia rangiferina are important for the food chain lichen-reindeer-man. The concentration of (129)I was determined in lichen samples (Cladonia alpestris) contaminated by fallout from atmospheric nuclear tests explosions and the Chernobyl accident. The samples were collected at Lake Rogen District (62.3°N, 12.4°E) in central Sweden in the periods 1961-1975 and 1987-1998, and analysed with accelerator mass spectrometry (AMS) at CNA (Seville) to study its distribution in different layers. Data on the (137)Cs activity measured previously were also included in this study. The (129)I concentration ranged from (0.95 ± 0.13) × 10(8) at g(-1) in 1961 in the uppermost layer to (14.2 ± 0.5) × 10(8) at g(-1) in 1987 in deepest layer. The (129)I/(137)Cs atom ratio ranged between 0.12 and 0.27 for lichen samples collected in the period 1961-1975, indicating weapons tests fallout. For lichen samples collected between 1987 and 1998 the behaviour of (137)Cs concentrations reflected Chernobyl fallout. The concentrations of the two radionuclides followed each other quite well in the profile, reflecting the same origin for both. From the point of view of the spatial distribution in the lichen, it appears that (129)I was predominantly accumulated in the lowest layer, the opposite to (137)Cs for which the highest amounts were detected systematically in the topmost layer of lichen. This vertical distribution is important for radioecology because lichen is the initial link in the food chain lichen-reindeer-man, and reindeer only graze the upper parts of lichen carpets.

Determination of 129I/127I in aerosol samples in Seville (Spain).

In this work we present results of the (129)I/(127)I ratio in aerosols of Seville, Southwest of Spain (37.4 degrees N,6 degrees W). A radiochemical method is applied to extract the iodine from the aerosols and prepare samples to be measured by accelerator mass spectrometry (AMS) at the ETH facility in Zürich. We have found the possibility of monitoring the (129)I/(127)I isotopic ratio on a two-days basis with sensitivities in the order of 10(4)-10(5) atoms (129)I/m(3), and values of 10(-8)-10(-9) for the isotopic ratio.

Iodine-129 in soils from Northern Ukraine and the retrospective dosimetry of the iodine-131 exposure after the Chernobyl accident.

Forty-eight soil profiles down to a depth of 40 cm were taken in Russia and Ukraine in 1995 and 1997, respectively, in order to investigate the feasibility of retrospective dosimetry of the 131I exposure after the Chernobyl accident via the long-lived 129I. The sampling sites covered areas almost not affected by fallout from the Chernobyl accident such as Moscow/Russia and the Zhitomir district in Ukraine as well as the highly contaminated Korosten and Narodici districts in Ukraine. 129I was analyzed by radiochemical neutron activation analysis (RNAA) and accelerator mass spectrometry (AMS). 127I was measured for some profiles by RNAA or ion chromatography (IC). The results for 127I demonstrated large differences in the capabilities of the soils to store iodine over long time spans. The depth profiles of 129I and of 137Cs showed large differences in the migration behavior between the two nuclides but also for each nuclide among the different sampling sites. Though it cannot be quantified how much 129I and 137Cs was lost out of the soil columns into deeper depths, the inventories in the columns were taken as proxies for the total inventories. For 129I, these inventories were at least three orders of magnitude higher than a pre-nuclear value of 0.084+/-0.017 mBq m(-2) derived from a soil profile taken in 1939 in Lutovinovo/Russia. From the samples from Moscow and Zhitomir, a pre-Chernobyl 129I inventory of (44+/-24) mBq m(-2) was determined, limiting the feasibility of 129I retrospective dosimetry to areas where the 129I inventories exceed 100 mBq m(-2). Higher average 129I inventories in the Korosten and Narodici districts of 130 and 848 mBq m(-2), respectively, allowed determination of the 129I fallout due to the Chernobyl accident. Based on the total 129I inventories and on literature data for the atomic ratio of 129I/131I=13.6+/-2.8 for the Chernobyl emissions and on aggregated dose coefficients for 131I, the thyroid exposure due to 131I after the Chernobyl accident was estimated for the inhabitants of four villages in the Korosten and of three villages in the Narodici districts. The limitations and uncertainties of the 129I retrospective dosimetry are discussed.

Relative influence of 129I sources in a sediment core from the Kattegat area.

The depth profiles of the (129)I concentration and the (129)I/(127)I ratio in a surface sediment core from the Kattegat area have been analyzed in order to obtain information about the different sources of (129)I in that core. Therefore, a mathematical model that relates the measured values to the available emission data from the nuclear fuel reprocessing plants and nuclear weapons tests has been applied. Results show that the reprocessing plants at La Hague and Sellafield are the main sources of (129)I in the sediment. Results about the transfer from the release points at the reprocessing plants to the sampling zone agree with other literature data. The model calculates quite fast the sedimentation of (129)I in the sampling place, probably attached to organic matter. Finally, an estimation of approximately 89 kg of (129)I released by Sellafield between 1952 and 1968 has been obtained from the model.

Wet and dry deposition of 129I in Seville (Spain) measured by accelerator mass spectrometry.

Iodine-129 (T1/2 = 1.57 x 10(7) yr) concentrations have been determined by accelerator mass spectrometry in rainwater samples taken at Seville (southwestern Spain) in 1996 and 1997. This technique allows a reduction in the detection limits for this radionuclide in comparison to radiometric counting and other mass spectrometric methods such as ICP-MS. Typical 129I concentrations range from 4.7 x 10(7) 129I atoms/l (19.2%) to 4.97 x 10(9) 129I atoms/l (5.9%), while 129I depositions are normally in the order of 10(8)-10(10) atoms/m2d. These values agree well with other results obtained for recent rainwater samples collected in Europe. Apart from these, the relationship between 129I deposition and some atmospheric factors has been analyzed, showing the importance of the precipitation rate and the concentration of suspended matter in it.

Determination of 129I in atmospheric samples by accelerator mass spectrometry.

A method for the radiochemical extraction of 129I from atmospheric charcoal filters and its measurement by accelerator mass spectrometry is presented. Either the 129I concentration or the 129I/127I atom ratio can be determined in the sample. With this method, air filters from Seville, in the Southwest of Spain (37.4 degrees N, 6 degrees W) have been analyzed. Sensitivities in the order of 10(4) atoms/m3 for 129I concentrations and 10(-10) for 129I/127I atom ratios are obtained. AMS measurements are performed with the 6 MV tandem accelerator at the ETH-Hönggerberg in Zurich.