Gamma spectrometry analysis of radioiodine in charcoal from high volume aerosol samples.

Following accidental releases, gamma spectrometry of impregnated charcoal filters is used to measure gaseous 131I contamination, but is subject to sampling inhomogeneity. In this study two germanium detectors are calibrated using a charcoal multi-gamma standard. Activities in samples spiked with a matrix of 131I aliquots are compared based on measurement, spike known activity, and monte-carlo simulation, and used to test a simple mixing method. Measurement efficiency, and removal of 11% inhomogeneity effect by mixing, was successfully reproduced in GESPECOR calculations.

An automated programme for the optimisation of HPGe detector parameters using an evolutionary algorithm with GESPECOR.

We describe the development of an automated, user-friendly programme which, making use of the GESPECOR gamma spectrometry software to conduct Monte Carlo simulations, yields an optimised model of a HPGe detector by applying suitable optimisation algorithms without requiring any further user intervention. The programme is capable of simultaneously employing multiple experimental FEP efficiency curves for the parameter optimisation process. Application of the optimisation process to a HPGe detector demonstrates that accurate, robust models can be achieved using this approach.

Small field detector correction factors kQclin,Qmsr (fclin,fmsr) for silicon-diode and diamond detectors with circular 6 MV fields derived using both empirical and numerical methods.

PURPOSE: The use of radiotherapy fields smaller than 3 cm in diameter has resulted in the need for accurate detector correction factors for small field dosimetry. However, published factors do not always agree and errors introduced by biased reference detectors, inaccurate Monte Carlo models, or experimental errors can be difficult to distinguish. The aim of this study was to provide a robust set of detector-correction factors for a range of detectors using numerical, empirical, and semiempirical techniques under the same conditions and to examine the consistency of these factors between techniques. METHODS: Empirical detector correction factors were derived based on small field output factor measurements for circular field sizes from 3.1 to 0.3 cm in diameter performed with a 6 MV beam. A PTW 60019 microDiamond detector was used as the reference dosimeter. Numerical detector correction factors for the same fields were derived based on calculations from a geant4 Monte Carlo model of the detectors and the Linac treatment head. Semiempirical detector correction factors were derived from the empirical output factors and the numerical dose-to-water calculations. RESULTS: The PTW 60019 microDiamond was found to over-respond at small field sizes resulting in a bias in the empirical detector correction factors. The over-response was similar in magnitude to that of the unshielded diode. Good agreement was generally found between semiempirical and numerical detector correction factors except for the PTW 60016 Diode P, where the numerical values showed a greater over-response than the semiempirical values by a factor of 3.7% for a 1.1 cm diameter field and higher for smaller fields. CONCLUSIONS: Detector correction factors based solely on empirical measurement or numerical calculation are subject to potential bias. A semiempirical approach, combining both empirical and numerical data, provided the most reliable results.

Tracking of airborne radionuclides from the damaged Fukushima Dai-ichi nuclear reactors by European networks.

Radioactive emissions into the atmosphere from the damaged reactors of the Fukushima Dai-ichi nuclear power plant (NPP) started on March 12th, 2011. Among the various radionuclides released, iodine-131 ((131)I) and cesium isotopes ((137)Cs and (134)Cs) were transported across the Pacific toward the North American continent and reached Europe despite dispersion and washout along the route of the contaminated air masses. In Europe, the first signs of the releases were detected 7 days later while the first peak of activity level was observed between March 28th and March 30th. Time variations over a 20-day period and spatial variations across more than 150 sampling locations in Europe made it possible to characterize the contaminated air masses. After the Chernobyl accident, only a few measurements of the gaseous (131)I fraction were conducted compared to the number of measurements for the particulate fraction. Several studies had already pointed out the importance of the gaseous (131)I and the large underestimation of the total (131)I airborne activity level, and subsequent calculations of inhalation dose, if neglected. The measurements made across Europe following the releases from the Fukushima NPP reactors have provided a significant amount of new data on the ratio of the gaseous (131)I fraction to total (131)I, both on a spatial scale and its temporal variation. It can be pointed out that during the Fukushima event, the (134)Cs to (137)Cs ratio proved to be different from that observed after the Chernobyl accident. The data set provided in this paper is the most comprehensive survey of the main relevant airborne radionuclides from the Fukushima reactors, measured across Europe. A rough estimate of the total (131)I inventory that has passed over Europe during this period was <1% of the released amount. According to the measurements, airborne activity levels remain of no concern for public health in Europe.

Modelling the biological half-life and seasonality of ¹4C in Fucus vesiculosus from the east coast of Ireland: implications for the estimation of future trends.

Radiocarbon levels were recorded in Fucus vesiculosus samples collected on a monthly basis over a three-year period at a site on the east coast of Ireland. The resulting data was analysed using a numerical model which estimates the transit times from the Sellafield plant to the sampling location, and the mean availability time of ¹4C in seaweed. With the inclusion of a model parameter allowing for seasonal variability in uptake by the Fucus, good correlation was observed between the predicted and measured concentrations. Future temporal trends of ¹4C Fucus concentrations along the eastern Irish coastline were modelled with the application of three possible prospective discharge scenarios, predicting ¹4C Fucus concentrations to reduce to ambient background levels within 2.5-years of discharges being set to zero. Such projections may prove helpful in assessing the consequences of discharge management and policy making in the context of the OSPAR convention.

Modelling the reworking effects of bioturbation on the incorporation of radionuclides into the sediment column: implications for the fate of particle-reactive radionuclides in Irish Sea sediments.

A microcosm laboratory experiment was conducted to determine the impact of biological reworking by the ragworm Nereis diversicolor on the redistribution of particle-bound radionuclides deposited at the sediment-water interface. Over the course of the 40-day experiment, as much as 35% of a (137)Cs-labelled particulate tracer deposited on the sediment surface was redistributed to depths of up to 11 cm by the polychaete. Three different reworking models were employed to model the profiles and quantify the biodiffusion and biotransport coefficients: a gallery-diffuser model, a continuous sub-surface egestion model and a biodiffusion model. Although the biodiffusion coefficients obtained for each model were quite similar, the continuous sub-surface egestion model provided the best fit to the data. The average biodiffusion coefficient, at 1.8 +/- 0.9 cm(2) y(-1), is in good agreement with the values quoted by other workers on the bioturbation effects of this polychaete species. The corresponding value for the biotransport coefficient was found to be 0.9 +/- 0.4 cm y(-1). The effects of non-local mixing were incorporated in a model to describe the temporal evolution of measured (99)Tc and (60)Co radionuclide sediment profiles in the eastern Irish Sea, influenced by radioactive waste discharged from the Sellafield reprocessing plant. Reworking conditions in the sediment column were simulated by considering an upper mixed layer, an exponentially decreasing diffusion coefficient, and appropriate biotransport coefficients to account for non-local mixing. The diffusion coefficients calculated from the (99)Tc and (60)Co cores were in the range 2-14 cm(2) y(-1), which are consistent with the values found by other workers in the same marine area, while the biotransport coefficients were similar to those obtained for a variety of macrobenthic organisms in controlled laboratories and field studies.

(239)Pu, (240)Pu, and (241)Am determination in hot particles by low level gamma-spectrometry.

A nondestructive method based on low-energy, high-resolution photon spectrometry is presented which allows accurate determination of (239)Pu, (240)Pu, and (241)Am (as a daughter of (241)Pu) activities in radioactive particles containing relatively high levels of plutonium isotopes. The proposed method requires only one measurement for the establishment of an absolute efficiency curve. Since the density and composition of the radioactive particles of interest may vary, a self-absorption correction is required for the accurate determination of isotopic activities and ratios. This correction is carried out for each individual particle using the convenient gamma-ray emissions of (241)Am.

In-vitro analysis of the dissolution kinetics and systemic availability of plutonium ingested in the form of 'hot' particles from the Semipalatinsk NTS.

In-vitro leaching of radioactive 'hot' particles isolated from soils sampled at the Semipalatinsk Nuclear Test Site has been carried out in order to evaluate the fraction of plutonium activity released into simulated human stomach and small intestine fluids during digestion. Characterisation of the particles (10-100 Bq(239,240)Pu) and investigation of their dissolution kinetics in simulated fluids has been accomplished using a combination of high-resolution alpha-spectrometry, gamma-spectrometry and liquid scintillation counting. The results of these analyses indicate that plutonium transfer across the human gut following the ingestion of 'hot' particles can be up to two orders of magnitude lower than that expected for plutonium in a more soluble form, and show that for areas affected by local fallout, use of published ingestion dose coefficients, together with bulk radionuclide concentrations in soil, may lead to a considerable overestimation of systemic uptake via the ingestion pathway.

Americium, plutonium and uranium contamination and speciation in well waters, streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site, Kazakhstan.

New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel'kem 1 and Tel'kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that (241)Am, (239,240)Pu and (238)U concentrations in well waters within the study area are in the range 0.04-87mBq dm(-3), 0.7-99mBq dm(-3), and 74-213mBq dm(-3), respectively, and for (241)Am and (239,240)Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01mBq dm(-3), 0.08mBq dm(-3) and 0.32mBq dm(-3) for (241)Am, (239,240)Pu and (238)U, respectively. The (235)U/(238)U isotopic ratio in almost all well and stream waters is slightly elevated above the 'best estimate' value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53-85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11-42microSv (mean 21microSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel'kem explosions.

Trends in the spatial and temporal distribution of 129I and 99Tc in coastal waters surrounding Ireland using Fucus vesiculosus as a bio-indicator.

Spatial and temporal trends in (129)I and (99)Tc concentrations around the Irish coastline have been evaluated using Fucus vesiculosus as a bio-indicator. (129)I concentrations in a recent set of seawater samples have also been recorded and reveal an identical spatial pattern. Concentrations of (129)I in Fucus from the northeast coast of Ireland proved to be at least two orders of magnitude higher than concentrations in Fucus from the west coast. The (129)I content of Fucus increased significantly between 1985 and 2003, in line with increases in discharges of (129)I from the Sellafield nuclear reprocessing plant. Similar trends were observed in the case of (99)Tc. (129)I/(99)Tc ratios in Irish seawater were deduced from the Fucus data, and compared to ratios in discharges from Sellafield and from the French reprocessing plant at Cap de la Hague. Levels of (129)I and (99)Tc in Fucus from the west coast were found to be enhanced with respect to levels in seaweeds from other regions in the Northern Hemisphere unaffected by discharges from nuclear installations such as those referred to.

Source-term characterisation and solid speciation of plutonium at the Semipalatinsk NTS, Kazakhstan.

New data on the concentrations of key fission/activation products and transuranium nuclides in samples of soil and water from the Semipalatinsk Nuclear Test Site are presented and interpreted. Sampling was carried out at Ground Zero, Lake Balapan, the Tel'kem craters and reference locations within the test site boundary well removed from localised sources. Radionuclide ratios have been used to characterise the source term(s) at each of these sites. The geochemical partitioning of plutonium has also been examined and it is shown that the bulk of the plutonium contamination at most of the sites examined is in a highly refractory, non-labile form.

Uranium-thorium disequilibrium in north-east Atlantic waters.

In this paper we report and compare the concentrations of 234Th and 238U measured in surface and subsurface waters collected in the course of a sampling campaign in the north east Atlantic in June-July 1998. Dissolved 234Th concentrations in surface waters ranged from 5 to 20 Bq m(-3), showing a large deficiency relative to 238U concentrations (typically 42 Bq m-3). This disequilibrium is indicative of active 234Th scavenging from surface waters. Observed 234Th/238U activity ratios, together with corresponding 234Th particulate concentrations, were used to calculate mean residence times for 234Th with respect to scavenging onto particles (tau(diss)) and subsequent removal from surface waters (tau(part)). Residence times in the range 5-30 days were determined for tau(diss) and 4-18 days for tau(part) (n=14). In addition, ultrafiltration experiments at six stations in the course of the same expedition revealed that in north-east Atlantic surface waters a significant fraction (46+/-17%; n=6) of the thorium in the (operationally-defined) dissolved phase (<0.45 microm) is in colloidal form. These observations are consistent with the 'colloidal pumping' model in which it is assumed that 234Th is rapidly absorbed by colloidal particles, which then aggregate, albeit at a slower rate, into larger filterable particles. In essence, colloids act as intermediaries in the transition from the fully dissolved to the filter-retained (>0.45 microm) phase. Thus, the time (tau(c)) for fully dissolved 234Th to appear in the filter-retained fraction is dependent on the rate of colloidal aggregation. Here, we determined tau(c) values in the range 3-17 days.

Measurement of the residual radioactivity induced in the front foil of a target assembly in a modern medical cyclotron.

The levels of residual radioactivity induced in Havar foils at the entrance of a high-pressure 18O-enriched water target used for the production of 18F- in a medical cyclotron with 16 MeV protons have been determined using high-resolution gamma-ray spectrometry. Whole body and skin dose rates arising from exposure to these foils during their periodic replacement have been estimated. The results indicate that irradiated foils do not represent a significant radiological hazard for the cyclotron operating staff and that no waste disposal difficulties should be encountered after an appropriate 'cooling' period of 2 years.

Oxidation-state distribution of plutonium in surface and subsurface waters at Thule, northwest Greenland.

The speciation of plutonium in Arctic waters sampled on the northwest Greenland shelf in August 1997 is discussed in this paper. Specifically, we report the results of analyses carried out on seawater sampled (a) close to the Thule air base where, in 1968, a US military aircraft carrying four nuclear weapons crashed on sea ice, releasing kilogram quantities of plutonium to the snow pack and underlying seabed sediments, and (b) at a reference station (Upernavik) located approximately 400 km to the south. The data show that most of the plutonium in the dissolved phase at Thule is in the form of Pu(V, VI) (mean: 68+/-6%; n = 6), with little if any distinction apparent between surface and bottom waters. Further, the oxidation state distribution at stations close to the accident site is similar to that measured at Upernavik, remote from this site. It is also similar to the distribution observed in shelf waters at mid-latitudes, suggesting that the underlying processes controlling plutonium speciation are insensitive to temperature over the range 0-25 degrees C. Measurements using tangential-flow ultrafiltration indicate that virtually all of the plutonium (including the fraction in a reduced chemical form) is present as fully dissolved species. Most of this plutonium would seem to be of weapons fallout origin, as the mean 238Pu/239,240Pu activity ratio in the water column (dissolved phase) at Thule (0.06+/-0.02; n = 10) is similar to the global fallout ratio at this latitude (approximately 0.04). Thus, there is little evidence of weapons-grade plutonium in the water column at Thule at the present time.

Vertical and horizontal fluxes of plutonium and americium in the western Mediterranean and the Strait of Gibraltar.

New data on the vertical distributions of plutonium and americium in the waters of the western Mediterranean and the Strait of Gibraltar are examined in terms of the processes governing their delivery to, transport in and removal from the water column within the basin. Residence times for plutonium and americium in surface waters of approximately 15 and approximately 3 years, respectively, are deduced, and it is shown that by the mid 1990s only approximately 35% of the 239,240Pu and approximately 5% of the 241Am deposited as weapons fallout still resided in the water column. Present 239,240Pu inventories in the water column and the underlying sediments are estimated to be approximately 25 TBq and approximately 40 TBq, respectively, which reconcile well with the time-integrated fallout deposition in this zone, taken to be approximately 69 TBq. The data show that there are significant net outward fluxes of plutonium and americium from the basin through the Strait of Gibraltar at the present time. These appear to be compensated by net inward fluxes of similar magnitude through the Strait of Sicily. Thus, the time-integrated fallout deposition in the western basin can be accounted for satisfactorily in terms of present water column and sediment inventories. Enhanced scavenging on the continental shelves, as evidenced by the appreciably higher transuranic concentrations in shelf sediments, supports this contention.

Determination of the 243 Cm/244 Cm ratio alpha spectrometry and spectral deconvolution in environmental samples exposed to discharges from the nuclear fuel cycle.

The presence of curium nuclides in irradiated nuclear fuel is well known, as is their occurrence in environmental materials exposed to liquid waste discharges from reprocessing plants and to fallout following the Chernobyl accident. Knowledge of the 242 Cm/244 Cm and 243 Cm/244 Cm atom ratios can be a useful tool for characterizing a source-term and assessing the burn-up history of nuclear fuel. Here, a practical technique, based on high-resolution alpha spectrometry and spectral deconvolution, is described by which the 243, 244 Cm multiplet can be resolved at the low activities typical of most environmental samples. The resulting 243 Cm/244 Cm ratio is then used to correct for any interference by 243 Cm in the 242 Cm window. The technique has been applied to the determination of the 243 Cm/244 Cm ratio in samples of seabed sediment collected near the Sellafield outfall, riverine sediment sampled downstream of the Mayak reprocessing plant and soil and lichen from within the Chernobyl exclusion zone. Near Sellafield, the 243 Cm/244 Cm ratio was found to be < 2%, while near Mayak and Chernobyl it was considerably higher, being approximately 6-8%.

Perturbation in the 240Pu/239Pu global fallout ratio in local sediments following the nuclear accidents at Thule (Greenland) and Palomares (Spain).

It is well established that the main source of the plutonium found in marine sediments throughout the Northern Hemisphere is global stratospheric fallout, characterized by a typical 240Pu/239Pu atom ratio of approximately 0.18. Measurement of perturbations in this ratio at various sites which had been subjected to close-in fallout, mainly from surface-based testing (e.g. Bikini Atoll, Nevada test site, Mururoa Atoll), has confirmed the feasibility of using this ratio to distinguish plutonium from different fallout sources. In the present study, the 240Pu/239Pu ratio has been examined in samples of sediment (and soil) collected at Thule (Greenland) and Palomares (Spain), where accidents involving the release and dispersion of plutonium from fractured nuclear weapons occurred in 1968 and 1966, respectively. The 240Pu/239Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution, and confirmed in the case of the most active samples by high-resolution X-ray spectrometry. Only samples which displayed plutonium heterogeneities, i.e. hot particles or concentrations well in excess (at least two orders of magnitude) of those expected from global fallout, were selected for analysis. The analytical results showed that at Thule the mean 240Pu/239Pu atom ratio was 0.033 +/- 0.004 (n = 4), while at Palomares the equivalent ratio appeared to be significantly higher at 0.056 +/- 0.003 (n = 4). Both ratios are indicative of low burn-up plutonium and are consistent with those reported for weapons-grade plutonium. It is noteworthy that the mean 238Pu/239Pu activity ratio in the Thule samples, at 0.0150 +/- 0.0017 (n = 4), was also lower than that measured in the Palomares samples, namely, 0.0275 +/- 0.0012 (n = 4). The 241Pu/239Pu ratios were similarly different. Finally, the data show, in contrast to Palomares, that not all of the samples from the Thule accident site were contaminated with plutonium of identical isotopic composition.