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).

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.

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.

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.

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.

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.

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.

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.

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.

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.

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.

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.

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.

The presence of some artificial and natural radionuclides in a Eucalyptus forest in the south of Spain.

Long-lived artificial radionuclides (137Cs, 90Sr) were studied in a Eucalyptus plantation located in the south-west of Spain. Radionuclide concentrations were determined in different types of samples corresponding to specific forest components (soil, trees, herbs and litter). Depth profile distributions were obtained in two selected core soils. Two layers were separately measured in three other cores. The concentration factor, defined as the ratio between the mean activity concentration in a component and the mean activity concentration in the soil, was calculated for each component. The biomass of different components was estimated in order to evaluate the total density concentration (Bq/ha) of the artificial radionuclides (137Cs, 90Sr) in the Eucalyptus plantation. The transfer of the radionuclides between the different forest components can be inferred from the results. Additionally, other naturally occurring radionuclides (40K, 226Ra, 228Ra, 228Ac) were determined for comparison. Transport of radionuclides from forest to a nearby pulp mill is also discussed.

Radioactive discharges from an alkaline pulp mill located in the south of Spain.

Artificial and natural radionuclides present in environmental samples (Eucalyptus wood and bark) can be transferred in an alkaline pulp mill and concentrated in the recycling process. Some part of the radionuclides can be released into the environment associated with the discharges from such a factory. An alkaline pulp mill located in the South of Spain was extensively sampled during 1993 and different radionuclides analysed in the collected samples. Thus the concentrations and fluxes of natural (40K, 226Ra, 228Ra and 228Th) and artificial (137Cs and 90Sr) radionuclides associated with the samples collected along the pulp production process are presented. It is shown that radium and thorium radionuclides behave similarly to strontium and calcium and, consequently, concentrate within the Ca-cycle. Furthermore, 40K and 137Cs are concentrated during the Na-cycle. Finally, the results obtained by the authors are compared with the levels found in similar factories, though situated in the North of Europe, by other researchers.

Factor of merit and minimum detectable activity for 90Sr determinations by gas-flow proportional counting or Cherenkov counting.

The determination of 90Sr in environmental samples can be done by using a gas-flow proportional counter (beta-counting) or a liquid-scintillation spectrometer (Cherenkov counting). In this work, we present the factor of merit (FOM) and the minimum detectable activity (MDA) for both the counters. Quantitative relationships are proposed for FOM and MDA determination.

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 226Ra and 224Ra in drinking waters by liquid scintillation counting.

A method for the determination of Ra-isotopes in water samples has been developed. Ra is coprecipitated with Ba as sulphate. The precipitate is then dissolved with EDTA and counted with a liquid scintillation system after mixing with a scintillation cocktail. The study of the temporal evolution of the separated activity gives the isotopic composition of the sample, i.e. the 224Ra and 226Ra contribution to the total activity. The method has been applied to some Spanish drinking waters.