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A Lagrangian transport model for the North Atlantic has been applied to simulate the historical releases of 137Cs, 129I and 236U from the European nuclear fuel reprocessing plants. Advection by currents, mixing and decay are included, as radionuclide interactions between water, sediments and suspended matter. The model was validated comparing predictions with measured radionuclide concentrations in water and sediments in several areas. 129I and 236U signals entering the Arctic Ocean have been compared with the input terms: the 236U signal is distorted, but the 129I signal preserves its shape. In the first moments after the releases, the sediments act as sinks for 236U, but not significantly for 129I and ultimately they become sources of 236U to the open sea. This results in a weaker correlation between input and output signals for 236U than for 129I. The same effects as for 236U have been found for 137Cs signal into the Arctic.

The Centro Nacional de Aceleradores is a user-oriented accelerator facility in Seville, Spain. Its main facilities are a 3 MV tandem accelerator, an 18 MeV proton Cyclotron, a tandetron used for AMS, a compact accelerator used for radiocarbon measurements, a 60Co irradiator and a PET/CT scanner. The technical specifications and research applications of these facilities are described. A neutron beam line associated to a charged pulsed beam in the tandem allows for time of flight measurements which determine the neutron energy. The use of an adequate stripper gas in the AMS tandetron permits to measure heavy radionuclides with very low detection levels, allowing to perform environmental studies using these radionuclides as tracers. The use of the microbeam in the tandem accelerator allows to apply the ion beam-induced current technique to investigate the spectroscopic properties and radiation hardness of different semiconductor detectors.

New data on the presence of 129I in seawater in the Southern Hemisphere measured by Accelerator Mass Spectrometry (AMS) is presented. The samples were collected in 2014 along the Namibian coast during a cruise organised by the National Marine Information and Research Centre (NatMIRC), the national laboratories of the Ministry of Fisheries and Marine Resources (MFMR) in Namibia, and the IAEA Environment Laboratories (IAEA NAEL) in Monaco. The Benguela upwelling system is known as one of the most important marine upwelling regions in the world. Strong winds induce an offshore transport of surface seawater which is substituted by cool subsurface water inshore. As this water is nutrient-rich, which leads to high primary productivity, the Benguela upwelling system has a very important role as a fishing production area. The 129I concentrations in samples were between (0.66 ± 0.14) × 107 and (1.45 ± 0.30) × 107 atoms/kg. The highest 129I concentrations were found in the offshore surface samples. Deep-sea and inshore samples contained lower 129I concentrations, possibly as an effect of the upwelling process. A comparison with previously published studies suggests that the presence of 129I in the northern Benguela upwelling system (nBUS), is mainly due to the impact of nuclear weapons global fallout, without any evident impact of nuclear fuel reprocessing.

Dealing with the 41K interference during 41Ca measurement with low energy AMS systems is challenging. The detection of 39K to correct the measured 41Ca/40Ca ratios is a powerful tool that improves precision and accuracy. However, the study of the sources of this interference can help to reduce it to its minimum. In this work, it is shown that iron is a factor enhancing the production of the 41K interference, since the (41K57Fe)− ion has the same mass as (41K19F3)−. To validate this observation, we measured 57Fe2+ together with 41M2+ (all ions with mass 41) and 39K2+ in a blank sample and an aluminum target at the 600 kV AMS system at ETH Zurich. We also show the temporal evolution of 41M/40Ca and 39K/40Ca ratios in two blank samples during a measurement on the 1 MV AMS system at CNA Seville. Even when unstable behavior for these ratios is observed for one of the blanks, the relationship between both, 41M/39K, is relatively stable over time. This supports the accuracy of the K–correction method, providing that it is applied sequence by sequence. Two programs, one for each of these compact AMS systems, were written in FORTRAN code to deal with the complexity of the data analysis due to the K-correction.

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).

The passive absorber technique is one of the most common ways to suppress the 10B interference during 10Be measurements at facilities working with beam energies above 7 MeV. At lower energies, the range straggling complicates the application of absorbers, so that other suppression techniques are normally preferred. Several experiments were conducted at the SARA (hosted at Centro Nacional de Aceleradores, Seville, Spain) and VERA (Faculty of Physics, University of Vienna, Austria) AMS facilities to demonstrate the potential of the passive absorber technique also at and below 2.4 MeV. Two different absorber setups were installed and tested. For the detection of the rare isotopes both facilities used a gas ionization chamber optimized for light ions detection based on the same design. The absorber installed at the SARA facility was a combination of SiN foils and an isobutane gas volume, whereas VERA was equipped with an absorber constituted of a stack of SiN foils. In both cases, 10Be could be clearly separated from 10B and the use of a passive absorber at the entrance of the detector gave higher transmission compared to the degrader method. Depending on the absorber design, different background contributions could be identified: Rutherford scattering of 10B on the protons contained in the SiN foils and isobutane gas was responsible of a severe background at SARA, and fragments from 9Be1H molecules surviving the stripping process resulted in events partially overlapping the 10Be gate at VERA. The measured transmissions and background levels will be presented for the tested setups, as well as the advantages and disadvantages of each absorber design.

Most of the anthropogenic radionuclide 129I released to the marine environment from the nuclear fuel reprocessing plants (NFRP) at Sellafield (England) and La Hague (France) is transported to the Arctic Ocean via the North Atlantic Current and the Norwegian Coastal Current. 129I concentrations in seawater provides a powerful and well-established radiotracer technique to provide information about the mechanisms which govern water mass transport in the Nordic Seas and the Arctic Ocean and is gaining importance when coupled with other tracers (e.g. CFC, 236U). In this work, 129I concentrations in surface and depth profiles from the Nordic Seas and the North Atlantic (NA) Ocean collected from four different cruises between 2011 and 2012 are presented. This work allowed us to i) update information on 129I concentrations in these areas, required for the accurate use of 129I as a tracer of water masses; and ii) investigate the formation of deep water currents in the eastern part of the Nordic Seas, by the analysis of 129I concentrations and temperature-salinity (T-S) diagrams from locations within the Greenland Sea Gyre. In the Nordic Seas, 129I concentrations in seawater are of the order of 109 at·kg− 1, one or two orders of magnitude higher than those measured at the NA Ocean, not so importantly affected by the releases from the NFRP. 129I concentrations of the order of 108 atoms·kg− 1 at the Ellet Line and the PAP suggest a direct contribution from the NFRP in the NA Ocean. An increase in the concentrations in the Nordic Seas between 2002 and 2012 has been detected, which agrees with the temporal evolution of the 129I liquid discharges from the NFRPs in years prior to this. Finally, 129I profile concentrations, 129I inventories and T-S diagrams suggest that deep water formation occurred in the easternmost area of the Nordic Seas during 2012.

The accelerator mass spectrometry (AMS) technique, developed 40 years ago for 14C dating, was soon used to measure other long-lived radionuclides. One of the radionuclides measured by AMS since these early years is 41Ca and for a variety of applications. Some of these applications are: the calculation of the terrestrial age of meteorites, the study of nuclear reactions of astrophysical interest, the understanding of the calcium metabolism, and the characterization of low-level nuclear waste. The main challenge in 41Ca AMS is dealing with the interference caused by its stable isobar, 41K. This interference is reduced by using calcium 2uoride (CaF2) samples and the extraction of the (CaF3)- ion. At large AMS facilities, besides, 41K ions can be discriminated from 41Ca ions using different detection techniques based on the energy loss dependence on the atomic number. The 41Ca measurement with low energy AMS systems, like the 1 MV system at the Centro Nacional de Aceleradores (CNA), is quite challenging, since this discrimination is not possible. Nevertheless, the 41K contribution can be estimated and, therefore, corrected, thanks to the sequential detection of the other stable isotope of potassium, 39K (K-correction). Although the sensitivity achieved in 41Ca AMS at low energies is 3-4 orders of magnitude lower than those achieved at larger facilities, it allows the competitive measurements for biomedical applications, and the characterization of concrete samples from nuclear reactor bioshields. Since 41Ca AMS at low energies is limited to the estimation of 41K interference, it is advisable to study the different ways toward the production of this interference. Some factors related to it have been studied in different experiments performed with the 1 MV AMS system at CNA (SARA) and the 600 kV AMS system at the ETH Laboratory of Ion Beam Physics in Zurich (TANDY). For instance, we could demonstrate that 41K can be injected also as the (41K57Fe)- molecular ion. As a cons

Most of the anthropogenic radionuclide 129I released to the marine environment from the nuclear fuel reprocessing plants (NFRP) at Sellafield (England) and La Hague (France) is transported to the Arctic Ocean via the North Atlantic Current and the Norwegian Coastal Current. 129I concentrations in seawater provides a powerful and well-established radiotracer technique to provide information about the mechanisms which govern water mass transport in the Nordic Seas and the Arctic Ocean and is gaining importance when coupled with other tracers (e.g. CFC, 236U). In this work, 129I concentrations in surface and depth profiles from the Nordic Seas and the North Atlantic (NA) Ocean collected from four different cruises between 2011 and 2012 are presented. This work allowed us to i) update information on 129I concentrations in these areas, required for the accurate use of 129I as a tracer of water masses; and ii) investigate the formation of deep water currents in the eastern part of the Nordic Seas, by the analysis of 129I concentrations and temperature-salinity (T-S) diagrams from locations within the Greenland Sea Gyre. In the Nordic Seas, 129I concentrations in seawater are of the order of 109 at·kg− 1, one or two orders of magnitude higher than those measured at the NA Ocean, not so importantly affected by the releases from the NFRP. 129I concentrations of the order of 108 atoms·kg− 1 at the Ellet Line and the PAP suggest a direct contribution from the NFRP in the NA Ocean. An increase in the concentrations in the Nordic Seas between 2002 and 2012 has been detected, which agrees with the temporal evolution of the 129I liquid discharges from the NFRPs in years prior to this. Finally, 129I profile concentrations, 129I inventories and T-S diagrams suggest that deep water formation occurred in the easternmost area of the Nordic Seas during 2012.

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.

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 ± 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 ± 0.17) × 10−2 cm/y.

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.

We present a detailed study of the performance parameters for 41Ca measurements at the 1 MV AMS system at the Centro Nacional de Aceleradores (CNA) in Seville. Mixing CaF2 with Ag, we get stable (40CaF3)− currents between 50 and 100 nA. Transmission of the 2+ state in the He stripper is 41%, while optical transmission in the HE sector is typically higher than 95%. At low energies we cannot separate 41Ca from the isobar 41K at the detector, but the interference is reduced by using (41CaF3)− ions. The remaining contribution is corrected by measurement of the other stable isotope of potassium, 39K, to estimate this interference (K-correction). After this correction, we reach a 41Ca/40Ca background level between 5 × 10−12 and 8 × 10−12, making possible measurements of 41Ca/40Ca ratios higher than 4 × 10−11. Intercomparisons with the 0.6 MV AMS system at ETH Zurich show a quite good correlation.

129I, 236U, 239Pu and 240Pu isotopes have been analyzed in the different layers of a peatbog core collected in Madagascar Island (South Hemisphere) and representing at least the last 100 years of atmospheric deposition. The determination of ultra-low levels of these isotopes has been possible by applying the Accelerator Mass Spectrometric Technique (AMS) by using the 1 MV Tandetrom AMS facility located at CNA (Seville, Spain). The elements of interest were extracted and isolated previous to the measurements by applying validated radiochemical procedures. In this contribution, the behavior along the core of the different isotopes under analysis will be discussed, evaluating in particular the magnitude of their post-depositional retention/migration. In this sense, it will be highlighted the great mobility of the 129I with a near uniform profile along the core, in opposition for example with the preservation for the Pu isotopes of the fallout bomb peak. In the case of 236U, the 236U/239Pu atomic ratios determined in a total of eight layers of the core are ranging in the interval 0.02 – 0.29 with an average value of 0.15. As far as we know, these are the first 236U results seeing the light that were obtained in deposits as peatbogs collected in the southern hemisphere.

The Centro Nacional de Aceleradores (CNA) hosts a 1 MV accelerator mass spectrometry (AMS) apparatus since September 2005. In order to improve its overall performance, several updates have been made on the existing facility during the last 10 years of operation. In this paper, two modifications conducted in 2015 will be described. To increase the transmission of the ions through the accelerator, the stripping gas on the 1 MV CNA machine was changed from Ar to He. The measured maximum transmission for almost every isotope results to be higher, especially for heavy masses: for instance, in the case of uranium in the 3+ charge state, the transmission increased from 11% with Ar gas to about 38% with He gas. The second advance consisted of the substitution of the existing gas ionization chamber with a new one provided by ETH Zurich. The ETH detector features with its miniaturized design and is optimized for low energy AMS (i.e. very low electronic noise and efficient charge collection). As the electronic noise is the most important contribution to the resolution for light ions, the total energy resolution has been reduced by 15% in the case of 10Be, allowing a better discrimination against its isobar, 10B. For the heaviest radionuclides where the quality of the spectra is determined by the charge carrier production in the gas, the resolution for 2.7 MeV uranium ions was improved by 30%, probably due to a more efficient charge collection.

Measurements of 129I carried out on sea ice samples collected in the central Arctic Ocean in 2007 revealed relatively high levels in the range of 100–1400 × 107 at L−1 that are comparable to levels measured in the surface mixed layer of the ocean at the same time. The 129I/127I ratio in sea ice is much greater than that in the underlying water, indicating that the 129I 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 129I 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.

Los radionucleidos cosmogénicos de periodo de semidesintegración grande se encuentran en la naturaleza a niveles traza, lo cual hace que su medida sea realmente difícil. El hecho de que en la técnica de espectrometría de masas convencional sea muy difícil la discriminación entre el radionúclido que se desea medir y su interferente, hacía necesario el diseño y construcción de un nuevo sistema de espectrometría de masas que cumpliera con estas expectativas. La Espectrometría de Masas con Acelerador (AMS) es una técnica para la determinación de cantidades traza de radionúclidos de periodo de semidesintegración grande, en la que un acelerador de partículas generalmente electrostático de tipo tándem se acopla a un espectrómetro de masas que contiene los elementos convencionales para el transporte y la selección de iones en función de su masa y energía, de tipo magnético y electrostático. La concentración de los radionúclidos de interés se mide mediante la identificación y recuento de los iones con técnicas de detección nuclear que se pueden usar ya que los iones viajan a energías del orden del MeV/nucleón. La concentración del radionúclido problema se puede determinar, comparando el número de cuentas que llega al detector con la corriente de iones del núcleo estable, ya que en AMS la medida es de carácter relativo. Los principales atributos de la técnica estriban en la alta sensibilidad, casi una selectividad total y un amplio rango de medida de la concentración del radionúclido. El desarrollo del AMS ha aumentado la sensibilidad de detección en varios órdenes de magnitud con respecto al espectrómetro de masas convencional. Los interferentes isobáricos y moleculares, además, pueden ser separados casi completamente. En los años 70 comenzaron a instalarse los primeros espectrómetros de masas con acelerador tipo tándem, con la finalidad principal de la medida de 14C (T1/2= 5730 a), en pequeñas muestras con aplicaciones desde datación arqueológica a estudios de cambio climát, Cosmogenic radionuclides with long half-life are located in the nature at trace levels, therefore, their measurement is really difficult. Being that the conventional Mass Spectrometry is not able to distinguish between the radionuclide and its isobar, the design and the setting up of a new system was needed. Accelerator Mass Spectrometry (AMS) is a technique adopted to measure radionuclides with a large half-life at trace levels, where a tandem electrostatic particles accelerator is coupled to a mass spectrometer, which has magnetics and electrics elements to carry and select the ions by mass and energy. Isotopes are identified and counted with nuclear detection techniques, which can be used because the ions' energy is around 1 MeV/nucleon. The concentration of the problem isotope can be determined comparing the counts which are reaching the detector with the stable ions current, because the measurement has a relative character in AMS. The main features of the technique are the high sensitivity, almost a total selectivity and a great range of measurement of the isotope concentration. The development of the AMS has increased the detection sensitivity of several orders of magnitude with respect to the conventional Mass Spectrometry. Furthermore, the isobar and molecular interference can be separated almost totally. The first tandem accelerator mass spectrometers began to be installed during the 70's with the main aim of 14C measurement (T1/2= 5730 y) in small samples, with applications in archaeological dating or climatic changes studies. It was quickly checked the great potential of such a system to the measurement of other radionuclides and other applications like Basic Nuclear Physics, Astrophysics, Material Sciences, Biomedicine, Geology, Environmental and Palaoenvironmental Sciences; therefore the use of the AMS was extended to both the light radionuclides such as 10Be (T1/2 = 1,51×106 y), 26Al (T1/2 = 7,17×105 y) and 36Cl (T1/2 = 3,01×105 a) and the heavier ones

A quantitative evaluation of the fate of 129I, 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 129I have been intro-duced 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 inven-tories 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.

SARA (Spanish Accelerator for Radionuclides Analysis) was the first multielemental AMS facility installed in Spain in 2005. Since then it has been dedicated to the routine analysis of several radionuclides, such as 10Be, 14C, 26Al, 129I and Pu isotopes. Tests have been carried out with other isotopes, such as 41Ca, 236U and 237Np, and several changes have been made to the original facility to improve performance. First, an upgraded version of the ion source SO-110 has allowed us more stable measurement conditions for volatile elements (i.e. iodine), and a better general performance. Besides, changes in the target geometry have improved the ionization efficiency and long-term stability of the source output. Moreover, different software upgrades have been introduced to meet our routine operational needs. Finally, changing the movable Faraday-cup associated electronics now allows the measurement of smaller currents (in the range of pA), which has been key for the study of 236U/238U atomic ratio in environmental samples. Apart from these modifications it has to be noted that routine radiocarbon measurements have been moved to a Micadas system (200 kV) installed at CNA in 2012. In this paper we will illustrate the evolution of the facility up to now, and our future prospects will be introduced.

The performance of the 1 MV AMS system at the CNA (Centro Nacional de Aceleradores, Seville, Spain) for 236U and 239,240Pu measurements has been extensively investigated. A very promising 236U/238U abundance sensitivity of about 3 × 10−11 has been recently achieved, and background figures for 239Pu of about 106 atoms were reported in the past. These promising results lead to the use of conventional low energy AMS systems for the analysis of 236U and 239Pu and its further application in environmental studies. First 236U results obtained on our AMS system for marine samples (sediments and water) are presented here. Results of two new IAEA reference materials (IAEA-410 and IAEA-412, marine sediments from Pacific Ocean) are reported. The obtained 236U/239Pu atom ratios, of 0.12 and 0.022, respectively, show a dependency with the contamination source (i.e. local fallout from the US tests performed at the Bikini Atoll and general fallout). The results obtained for a third IAEA reference material (IAEA-381, seawater from the Irish Sea), are also presented. In the following, the uranium and plutonium isotopic compositions obtained on a set of 5 intercomparison seawater samples from the Arctic Ocean provided by the ETH Zürich are discussed. By comparing them with the obtained results on the 600 kV AMS facility Tandy at the ETH Zürich, we demonstrate the solidity of the CNA technique for 236U/238U determinations at, at least, 7 × 10−10 level. Finally, these results are discussed in their environmental context.

129I is a very long-lived radionuclide (T1/2 = 15.7 × 106 years) that is present in the environment because of natural and anthropogenic sources. Compared to the pre-nuclear era, large amounts of 129I 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 129I. In this work, 129I 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 129I concentrations and 129I/137Cs ratios. 129I concentrations were found to be in the order of (44–575) × 109 atoms g−1 in seaweed and (5.4–51) × 109 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 129I and 129I/137Cs ratios in the Skagerrak area and their gradually decreasing trend to the Kattegat indicates that the most important contribution to the 129I inventory in those areas comes from Sellafield and La Hague reprocessing plants.

129I is a very long-lived radionuclide (T1/2 = 15.7 × 106 years) that is present in the environment both because of natural and anthropogenic sources. In this work 129I concentration and 129I/127I 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 129I concentrations, 129I/127I and 129I/137Cs ratios. 129I concentrations were found to be in the order of (0.82–5.89) × 109 atoms g−1 in 1982 and (1.33–38.83) × 109 atoms g−1 in 1986. The 129I/127I 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 127I concentrations in seawater and salinity in this area, enabling the estimation of concentration factors for 127I in F. vesiculosus. The high levels of 129I and 129I/127I in the Kattegat and their gradually decreasing trend to the Baltic Sea indicates that the most important contribution to the 129I inventory in the Baltic Sea area comes from Sellafield and La Hague reprocessing plants. With respect to Chernobyl accident, 129I 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 129I in the Baltic region was not significant.

Radioactive residues, in order to be classified as Low-Level Waste (LLW), need to fulfil certain conditions; the limitation of the maximum activity from long-lived radionuclides is one of these requirements. In order to verify compliance to this limitation, the abundance of these radionuclides in the residue must be determined. However, performing this determination through radiometric methods constitutes a laborious task. In this work, 129I concentrations, 239+240Pu activities, and 240Pu/239Pu ratios are determined in low-level radioactive residues, including resins and dry sludge, from nuclear power plants in Spain. The use of Accelerator Mass Spectrometry (AMS) enables high sensitivities to be achieved, and hence these magnitudes can be re determined with good precision. Results present a high dispersion between the 129I and 239+240Pu activities found in various aliquots of the same sample, which suggests the existence of a mixture of resins with a variety of histories in the same container. As a conclusion, it is shown that activities and isotopic ratios can provide information on the processes that occur in power plants throughout the history of the residues. Furthermore, wipes from the monitoring of surface contamination of the José Cabrera decommissioning process have been analyzed for 129I determination. The wide range of measured activities indicates an effective dispersal of 129I throughout the various locations within a nuclear power plant. Not only could these measurements be employed in the contamination monitoring of the decommissioning process, but also in the modelling of the presence of other iodine isotopes.

Large amounts of iodine-129 were, and still are, released into the environment from nuclear facilities, in particular from two reprocessing facilities located on the east coast of the North Atlantic Ocean (Sellafield and La Hague). The main transport path of the releases from the two facilities is through the North Atlantic Current (NAC) and subsequently the Norwegian Coastal Current (NCC) to the Arctic Ocean. Iceland lies on the Scotland–Greenland ridge, which separates the Atlantic and Arctic oceans. 129I data available in that area are scarce despite their importance in modeling 129I dispersion through the North Atlantic and Arctic Oceans. For this reason, we have determined the 129I/127I ratio in seawater samples by means of Accelerator Mass Spectrometry (AMS) from three locations at the Iceland and Irminger Basins at different depths (from surface to 1000 m) in order to study the transport pathways of the anthropogenic releases to the waters. The measured 129I/127I ratios, compared to the pre-anthropogenic 129I/127I value, show the strong influence of the artificial 129I discharges in the North Atlantic waters.

129I is a very long-lived radionuclide (T1/2 = 15.7 × 106 years) that is present in the environment both because of natural and anthropogenic sources. In this work 129I concentration and 129I/127I 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 129I concentrations, 129I/127I and 129I/137Cs ratios. 129I concentrations were found to be in the order of (0.82–5.89) × 109 atoms g−1 in 1982 and (1.33–38.83) × 109 atoms g−1 in 1986. The 129I/127I 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 127I concentrations in seawater and salinity in this area, enabling the estimation of concentration factors for 127I in F. vesiculosus. The high levels of 129I and 129I/127I in the Kattegat and their gradually decreasing trend to the Baltic Sea indicates that the most important contribution to the 129I inventory in the Baltic Sea area comes from Sellafield and La Hague reprocessing plants. With respect to Chernobyl accident, 129I 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 129I in the Baltic region was not significant.

Desde que el Centro Nacional de Aceleradores (CNA) abriera sus puertas en 1997, los investigadores españoles cuentan con un laboratorio de referencia para estudiar la caracterización y modificación de materiales. Uno de los proyectos que allí se desarrollan consiste en medir isótopos radiactivos, lo que con las técnicas empleadas hasta ahora no se había conseguido. Se trata de un estudio en el que coopera Enresa, empresa con la que el CNA selló un convenio de colaboración en 2008, y cuyos resultados contribuirán a mejorar la seguridad en el almacenamiento de los residuos., Since the National Accelerators Centre (NAC) opened its doors in 1997, Spanish researchers have had use of a reference centre to study the characterisation and modification of materials. One of the projects developed there has been to measure radioactive isotopes that have not been measured using the techniques employed to da te. This study involves the cooperation of Enresa, with which the NAC established a collaboration agreement in 2008, and the results of which may help to improve the safe storage of waste.

129I is a very long-lived radionuclide (T1/2 = 15.7 × 106 years) that is present in the environment both because of natural and anthropogenic sources. In this work 129I concentration and 129I/129I ratio have been determined in rainwater samples collected at Seville (south-western Spain) during the period 2005–2008. Typical 129I concentration range from (0.26–8.86)×108 atoms/L, while 129I deposition are normally in the order of 107–108 atoms/m2d. Variability in the isotopic ratio 129I/129I indicates a range of (0.17–8.71) × 10−8. Temporal evolution of the 129I deposition seem to be related with the history of the 129I gaseous releases from the European reprocessing facilities at Sellafield and La Hague. The results obtained in this work are lower than the reported in previous works for the same location during the period 1996–1999, probably due to the reduction of the total gaseous 129I releases emitted by Sellafield and La Hague. The study of the dependence of the 129I deposition with some atmospheric parameters suggests that deposition seems to be more important in wet than in dry periods and that also depends in the wind direction, being more important for winds with north to south component. The agreement between the 129I concentration and the 129I/129I ratio suggest that the gaseous 129I emitted by the reprocessing plants has enough time to equilibrate with the 127I present in the atmosphere before arriving to southern Spain, probably due to the distance between Seville and these reprocessing plants.

La Memoria que desarrollamos a continuación consta de seis capítulo, cuyo contenido se discute a continuación. En el Capítulo 2 se hace una descripción general de la técnica de AMS y una caracterización del sistema compacto de AMS del CNA (SARA, Spanish Accelerator for Radionuclides Analysis), instalación en la que se han obtenido los resultados que se presentan en esta Tesis. En el Capítulo 3 se muestra el diseño de la óptica de iones del sistema SARA, o forma en la que el haz de partículas es transportado desde la fuente de iones hasta el detector, y la puesta a punto del mismo para la detección de 129I. En este Capítulo encontramos las simulaciones realizadas para reproducir el comportamiento óptico del sistema y todos los experimentos llevados a cabo para optimizar los parámetros que hacen posible la medida de 129I en el sistema de AMS del CNA. El Capítulo 4 comienza con una reseña acerca de la presencia del yodo en la naturaleza, su distribución en los distintos compartimentos naturales y las distintas fuentes de producción de 129I, y sigue con una descripción del método radioquímico desarrollado para su extracción de muestras sólidas. Las aplicaciones medioambientales se muestran en el Capítulo 5, en el que abordaremos el problema de la medida de 129I en varios tipos de muestras ambientales, como son líquenes, algas y turbas. Concluiremos el trabajo con el Capítulo 6, en el que presentaremos un resumen de la labor realizada y de los resultados más relevantes obtenidos en este trabajo.Posteriormente al Capítulo 6 existe un Anexo en el que se pormenoriza el experimento realizado con la técnica de XRF (Fluorescencia de Rayos X) y que concluyó con la obtención de los resultados preliminares referentes al rendimiento del método radioquímico que se muestran en el Capítulo 4.De modo general, podemos decir que con la realización de este trabajo se ha conseguido un importante avance en la detección de 129I mediante AMS. Estas mejoras se han producido en tres aspectos d

La detección de radionúclidos de periodo de semidesintegración grande en muestras ambientales es interesante, entre otras razones, por la posibilidad que ofrece de trazar y comprender procesos naturales como mezclas de aguas marinas, tránsito de masas acuosas, intercambios atmosféricos verticales y horizontales, etc. Las condiciones necesarias, aunque no suficientes, para ellos son que Tn sea clar amente superior al tiempo medio de ocurrencia de la transformación ambiental problema y que el radionúclido sea conservatorio respecto a la misma. Es claro, pues, el interés que tiene el desarrollo de técnicas rigurosas y sensibles de determinación de radionúclidos en la naturaleza. La Memoria que presentamos consta de un Capítulo 2 en el que se hace una descripción general de la técnica de AMS. En el Capítulo 3 presentamos la instalación en la que se han realizado nuestras medidas: la instalación de AMS del Instituto de Física de Partículas de Zurich. El Capítulo 4 trata sobre el diseño y puesta a punto del sistema ideado para detección del 129I en esta instalación. En el Capítulo 5 se describen los métodos radioquímicos desarrollados para la separación de 129I de varios tipos de muestras naturales. Añadimos en el mismo capítulo información sobre los métodos de muestreo utilizados. Los resultados obtenidos y su interpretación se presentan en el Capítulo 6. Finalmente, las conclusiones extraídas en el trabajo se resumen en el Capítulo 7.