Optimization of a new liquid scintillation spectrometer for the measurement of environmental levels of 3H in water samples.

The activity concentration of 3H in water samples collected from places unaffected by nuclear activities or for human consumption can be very low. In these cases, determination procedures must achieve a Minimum Detectable Activity (MDA) low enough to ensure that 3H is accurately determined. In this paper, we present a method that uses a new Liquid Scintillation Spectrometer (LSC in what follows): the Quantulus GCT 6220. Furthermore, a new liquid scintillation cocktail, the ProSafe LT+, has been tested for 3H measurement, showing to be a good option for the determination of low levels of this radionuclide. The MDAs achieved are low enough to enable the measurement of very low levels of 3H in recent environmental water. The results obtained using a Quantulus GCT 6220 and Prosafe LT + are compared to those obtained with a Quantulus 1220 and Prosafe HC + as liquid scintillation cocktail.

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.

Accelerator Mass Spectrometry (AMS) in Radioecology.

Accelerator Mass Spectrometry (AMS) provides with an excellent sensitivity for the determination of radionuclides in the environment. In fact, conventional radiometric techniques can hardly compete with AMS in the solution of many problems involving the measurement of very low levels of radioactivity in Nature. For that reason, during the last years AMS has become a powerful tool for Radioecology studies. In this paper a review is done on the evolution of AMS applications to the measurement of environmental radioactivity and, therefore, its contribution to the understanding of radionuclide behavior in Nature. For that, the advantages of using AMS to determine key nuclides as 129I, 14C, Pu-isotopes and others in different natural compartments will be discussed. The content of the paper is illustrated with the contributions to these studies of the Spanish National Center for Accelerators (CNA) AMS systems.

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 Notch ligand DLL4 specifically marks human hematoendothelial progenitors and regulates their hematopoietic fate.

Notch signaling is essential for definitive hematopoiesis, but its role in human embryonic hematopoiesis is largely unknown. We show that in hESCs the expression of the Notch ligand DLL4 is induced during hematopoietic differentiation. We found that DLL4 is only expressed in a sub-population of bipotent hematoendothelial progenitors (HEPs) and segregates their hematopoietic versus endothelial potential. We demonstrate at the clonal level and through transcriptome analyses that DLL4(high) HEPs are enriched in endothelial potential, whereas DLL4(low/-) HEPs are committed to the hematopoietic lineage, albeit both populations still contain bipotent cells. Moreover, DLL4 stimulation enhances hematopoietic differentiation of HEPs and increases the amount of clonogenic hematopoietic progenitors. Confocal microscopy analysis of whole differentiating embryoid bodies revealed that DLL4(high) HEPs are located close to DLL4(low/-) HEPs, and at the base of clusters of CD45+ cells, resembling intra-aortic hematopoietic clusters found in mouse embryos. We propose a model for human embryonic hematopoiesis in which DLL4(low/-) cells within hemogenic endothelium receive Notch-activating signals from DLL4(high) cells, resulting in an endothelial-to-hematopoietic transition and their differentiation into CD45+ hematopoietic cells.

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.

Levels, distribution and bioavailability of transuranic elements released in the Palomares accident (Spain).

The current levels and distribution of the remaining transuranic contamination present in the terrestrial area affected by the nuclear Palomares accident have been evaluated through the determination of the Pu-isotopes and (241)Am concentrations in soils collected 35 years after the accident. In addition, after confirming that most of the contamination is present in particulate form, some bioavailability laboratory-based experiments, based on the use of single extractants, were performed as an essential step in order to study the behaviour of the Pu contamination in the soils from the affected areas.

Isolation of Pu-isotopes from environmental samples using ion chromatography for accelerator mass spectrometry and alpha spectrometry.

A radiochemical method for the isolation of plutonium-isotopes from environmental samples, based on the use of specific extraction chromatography resins for actinides (TEVA), Eichrom Industries, Inc.), has been set up in our laboratory and optimised for their posterior determination by alpha spectrometry (AS) or accelerator mass spectrometry (AMS). The proposed radiochemical method has replaced in our lab a well-established one based on the use of a relatively un-specific anion-exchange resin (AG) 1X8, Bio-rad Laboratories, Inc.), because it is clearly less time consuming, reduces the amounts and molarities of acid wastes produced, and reproducibly gives high radiochemical yields. In order to check the reliability of the proposed radiochemical method for the determination of plutonium-isotopes in different environmental matrixes, twin aliquots of a set of samples were prepared with TEVA and with AG 1X8 resins and measured by AS. Some samples prepared with TEVA resins were measured as well by AMS. As it is shown in the text, there is a comfortable agreement between AS and AMS, which adequately validates the method.

Characterization of U/Pu particles originating from the nuclear weapon accidents at Palomares, Spain, 1966 and Thule, Greenland, 1968.

Following the USAF B-52 bomber accidents at Palomares, Spain in 1966 and at Thule, Greenland in 1968, radioactive particles containing uranium (U) and plutonium (Pu) were dispersed into the environment. To improve long-term environmental impact assessments for the contaminated ecosystems, particles from the two sites have been isolated and characterized with respect to properties influencing particle weathering rates. Low (239)Pu/(235)U (0.62-0.78) and (240)Pu/(239)Pu (0.055-0.061) atom ratios in individual particles from both sites obtained by Inductively Coupled Plasma Mass Spectrometry (ICP-MS) show that the particles contain highly enriched U and weapon-grade Pu. Furthermore, results from electron microscopy with Energy Dispersive X-ray analysis (EDX) and synchrotron radiation (SR) based micrometer-scale X-ray fluorescence (micro-XRF) 2D mapping demonstrated that U and Pu coexist throughout the 1-50 microm sized particles, while surface heterogeneities were observed in EDX line scans. SR-based micrometer-scale X-ray Absorption Near Edge Structure Spectroscopy (micro-XANES) showed that the particles consisted of an oxide mixture of U (predominately UO(2) with the presence of U(3)O(8)) and Pu ((III)/(IV), (IV)/(V) or (III), (IV) and (V)). Neither metallic U or Pu nor uranyl or Pu(VI) could be observed. Characteristics such as elemental distributions, morphology and oxidation states are remarkably similar for the Palomares and Thule particles, reflecting that they originate from similar source and release scenarios. Thus, these particle characteristics are more dependent on the original material from which the particles are derived (source) and the formation of particles (release scenario) than the environmental conditions to which the particles have been exposed since the late 1960s.

On the presence of enriched amounts of 235U in hot particles from the terrestrial area affected by the Palomares accident (Spain).

The characterisation by ICP-MS of an isolated Pu-U hot particle originating from the nuclear weapons accident in Palomares (Spain) shows, for the first time, that its uranium content is highly enriched in (235)U. The enrichment has been confirmed by independent analyses of two surface soil samples collected in a heavily contaminated area close to the impact point of one of the bombs. This finding clarifies better the composition of the weapons involved in the accident and is of importance when the inventory of U and Pu in the contaminated area are to be calculated.

Altered bone morphogenetic protein signalling in the Helicobacter pylori-infected stomach.

Morphogens regulate epithelial cell fate decisions in the adult gastrointestinal tract. The authors hypothesized that influx of inflammatory cells into the lamina propria may disturb the normal expression gradients of morphogens (morphogenetic landscape) in gastrointestinal epithelia. Changes in the activity of the bone morphogenetic protein (BMP) pathway in normal and Helicobacter pylori-infected gastric mucosa were therefore examined. It is shown that BMP receptors, the activated (phosphorylated) form of the intracellular BMP signal transduction protein SMAD1, and BMP target ID2 all localize to gastric epithelial cells that are at the end of the axis of epithelial renewal in normal mucosa. Colonization of human gastric mucosa with H. pylori was associated with an increase in BMP2 expression due to influx of inflammatory cells that produce BMP2. Furthermore, whereas no BMP4 was detected in the normal antrum, focal infiltrates of BMP4-expressing cells were found in the H. pylori-infected stomach. This influx of BMP-expressing cells was associated with an increase in epithelial BMP signalling. Interestingly, a shift in activity of the BMP pathway was observed towards the precursor cell compartment (isthmus) of the gastric units. Thus, H. pylori infection results in an influx of inflammatory cells that disturb the normal activity gradient of a morphogenetic pathway with an established role in epithelial cell fate regulation. The data suggest that morphological changes in epithelial histology may result from alterations in the morphogenetic landscape secondary to changes in the cellular composition of the lamina propria.

Optimized background reduction in low-level gamma-ray spectrometry at a surface laboratory.

The background of a coaxial Ge detector placed at a surface laboratory has been reduced by means of a background reduction setup consisting of a passive shield of low-activity lead, a simple radon suppression system and an active shield with a plastic scintillation plate. In particular, we have devoted our efforts to in-depth optimization of each parameter associated with different anticoincidence setups and to their subsequent intercomparison. The overall performance of the active shield was improved by using the optimum time parameters for each setup. The final objective is to decrease the cosmic-ray background and, by this way, to reduce the detection limits of gamma-ray spectrometers at conventional laboratories, and consequently make them competitive for different measurements like (210)Pb dating.

Presence of plutonium contamination in soils from Palomares (Spain).

More than 30 years after the occurrence of an aircraft accident which involved the detonation of two nuclear weapons in the surrounding area of the village of Palomares (Spain), the affected terrestrial area has been investigated for remaining transuranic contamination. Evidence from the presence of this contamination was initially found through the analysis of the 241Am inventories in superficial soil samples collected in the region, and was confirmed through the analysis of the (239+240)Pu inventories and their associated 238Pu/(239+240)Pu activity ratios in the same samples. However, it was also observed that a considerable fraction of the remaining contamination in the area was present in particulate form, i.e. as "hot particles". The work performed in our laboratory for identification, isolation and characterisation of these "hot particles" as well as some conclusions obtained from these analyses are outlined in this paper.

Overcoming ICP-QMS instrumental limitations for (99)Tc determination in environmental solid samples using radiochemistry.

Besides its capabilities, quadrupole-based ICP-MS counting establishes several limitations on (99)Tc analysis in environmental samples. Overcoming these limitations requires the use of radiochemical methods. We have developed a new method for the detection of (99)Tc by ICP-QMS in solid environmental samples. In order to improve the limit of detection of the technique, high amounts of solid samples (> or = 100g) are used. Hence, great amounts of the interfering elements are involved in the process, and therefore special emphasis is put on achieving a good commitment between adequate matrix elements removal and a minimization of the limit of detection. The performances of the method are analyzed in terms of conveniently defined figures of merit. The developed method is applied to several fallout level samples. In this way, the real performances and especially the real limitations of this method are shown.

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.

Uranium-238 and thorium-232 series concentrations in soil, radon-222 indoor and drinking water concentrations and dose assessment in the city of Aldama, Chihuahua, Mexico.

High-resolution gamma spectrometry was used to determine the concentration of 40K, 238U and 232Th series in soil samples taken from areas surrounding the city of Aldama, in Chihuahua. Results of indoor air short-time sampling, with diffusion barrier charcoal detectors, revealed relatively high indoor radon levels, ranging from 29 to 422 Bq/m3; the radon concentrations detected exceeded 148 Bq/m3 in 76% of the homes tested. Additionally, liquid scintillation counting showed concentrations of radon in drinking water ranging from 4.3 to 42 kBq/m3. The high activity of 238U in soil found in some places may be a result of the uranium milling process performed 20 years ago in the area. High radon concentrations indoor and in water may be explained by assuming the presence of uranium-bearing rocks underneath of the city, similar to a felsic dike located near Aldama. The estimated annual effective dose of gamma radiation from the soil and radon inhalation was 3.83 mSv.

Monte Carlo simulation of the response of a germanium detector for low-level spectrometry measurements using GEANT4.

In this paper, we will expose the work performed for the adaptation and refinement of the GEANT4 simulation toolkit (originally designed for Monte Carlo simulations in High-Energy Physics) in order to simulate Ge detectors in low-level gamma spectrometry. Special emphasis will be given to show and validate our own algorithms implemented in GEANT4 code for variance reduction and data analysis, that have been used for a quicker and precise efficiency calibration at different source-detector configurations of one of the low-level germanium gamma systems available in our laboratory.

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.