A composite position independent monitor of reactor fuel irradiation using Pu, Cs, and Ba isotope ratios.

When post-irradiation materials from the nuclear fuel cycle are released to the environment, certain isotopes of actinides and fission products carry signatures of irradiation history that can potentially aid a nuclear forensic investigation into the material's provenance. In this study, combinations of Pu, Cs, and Ba isotope ratios that produce position (in the reactor core) independent monitors of irradiation history in spent light water reactor fuel are identified and explored. These position independent monitors (PIMs) are modeled for various irradiation scenarios using automated depletion codes as well as ordinary differential equation solutions to approximate nuclear physics models. Experimental validation was performed using irradiated low enriched uranium oxide fuel from a light water reactor, which was sampled at 8 axial positions from a single rod. Plutonium, barium and cesium were chemically separated and isotope ratio measurements of the separated solutions were made by quadrupole and multi-collector inductively coupled mass spectrometry (Cs and Pu, respectively) and thermal ionization mass spectrometry (Ba). The effect of axial variations in neutron fluence and energy spectrum are evident in the measured isotope ratios. Two versions of a combined Pu and Cs based PIM are developed. A linear PIM model, which can be used to solve for irradiation time is found to work well for natural U fuel with <10% 240Pu and known or short cooling times. A non-linear PIM model, which cannot be solved explicitly for irradiation time without additional information, can nonetheless still group samples by irradiation history, including high burnup LEU fuel with unknown cooling time. 137Ba/138Ba is also observed to act as a position independent monitor; it is nearly single valued across the sampled fuel rod, indicating that samples sharing an irradiation history (same irradiation time and cooling time) in a reactor despite experiencing different neutron fluxes will have a common 137Ba/138Ba ratio. Modeling of this Ba PIM shows it increases monotonically with irradiation and cooling time, and a confirmatory first order analytical solution is also presented.

Thyroid monitoring of adults and children after reactor accidents with a new dose rate measurement device.

A specialized dose rate measurement device that was designed for monitoring the thyroid dose of children and adults after reactor accidents was tested. In measurements with neck phantoms and a human patient, the device was found to be capable of measuring the required low dose rates, even within increased ambient radiation. It is suitable for the application in emergency care centers.

Evaluation of an early warning system for airborne radionuclides.

An early warning system for detection of increased levels of radioactivity in outdoor air was operative between 2004 and 2011 at the Swedish air sampling stations. The system consisted of a low resolution detector (NaI), positioned directly behind the filter and measurement of the accumulated radioactivity were performed continuously. An evaluation of the data collected during the period is presented with emphasis on natural occurring radionuclides and their influence on the detectability of anthropogenic radionuclides.

Determination of uncertainties associated to the in vivo measurement of iodine-131 in the thyroid.

Intakes of radionuclides can be estimated through in vivo measurements, and the uncertainties associated to the measured activities should be clearly stated in monitoring program reports. This study aims to evaluate the uncertainties of in vivo monitoring of iodine 131 in the thyroid. The reference values for high-energy photons are based on the IDEAS Guide. Measurements were performed at the In Vivo Monitoring Laboratory of the Institute of Radiation Protection and Dosimetry (IRD) and at the Internal Dosimetry Laboratory of the Regional Center of Nuclear Sciences (CRCN-NE). In both institutions, the experiment was performed using a NaI(Tl) 3''3″ scintillation detector and a neck-thyroid phantom. Scattering factors were calculated and compared in different counting geometries. The results show that the technique produces reproducibility equivalent to the values suggested in the IDEAS Guide and measurement uncertainties is comparable to international quality standards for this type of in vivo monitoring.

(Mis)use of (133)Ba as a calibration surrogate for (131)I in clinical activity calibrators.

Using NIST-calibrated solutions of (131)Ba and (131)I in the 5mL NIST ampoule geometry, measurements were made in three NIST-maintained Capintec activity calibrators and the NIST Vinten 671 ionization chamber to evaluate the suitability of using (133)Ba as a calibration surrogate for (131)I. For the Capintec calibrators, the (133)Ba response was a factor of about 300% higher than that of the same amount of (131)I. For the Vinten 671, the Ba-133 response was about 7% higher than that of (131)I. These results demonstrate that (133)Ba is a poor surrogate for (131)I. New calibration factors for these radionuclides in the ampoule geometry for the Vinten 671 and Capintec activity calibrators were also determined.

Size distribution of radioactive particles collected at Tokai, Japan 6 days after the nuclear accident.

Airborne radioactive particles released by the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident in 2011 were collected with a cascade low-pressure impactor at the Japan Atomic Energy Agency (JAEA) in Tokai, Japan, 114 km south of the FDNPP. Size-fractionated samples were collected twice, in the periods of March 17-April 1, 2011, and May 9-13, 2011. These size-fractionated samplings were carried out in the earliest days at a short distance from the FDNPP. Radioactivity of short-lived nuclides (several ten days of half-life) was determined as well as (134)Cs and (137)Cs. The elemental composition of size-fractionated samples was also measured. In the first collection, the activity median aerodynamic diameter (AMAD) of (129m)Te, (140)Ba, (134)Cs, (136)Cs and (137)Cs was 1.5-1.6 µm, while the diameter of (131)I was 0.45 µm. The diameters of (134)Cs and (137)Cs in the second collection were expressed as three peaks at <0.5 µm, 0.94 µm, and 7.8 µm. The (134)Cs/(137)Cs ratio of the first collection was 1.02 in total, but the ratio in the fine fractions was 0.91. A distribution map of (134)Cs/(137)Cs - (136)Cs/(137)Cs ratios was helpful in understanding the change of radioactive Cs composition. The Cs composition of size fractions <0.43 µm and the composition in the 1.1-2.1 µm range (including the AMAD of 1.5-1.6 µm) were similar to the calculated compositions of fuels in the reactors No. 1 and No. 3 at the FDNPP using the ORIGEN-II code. The Cs composition collected in May, 2011 was similar to the calculation results of reactor No. 2 fuel composition. The change of Cs composition implies that the radioactive Cs was released from the three reactors at the FDNPP via different processes.

On within sample homogeneity testing using gamma-ray spectrometry.

Several problems concerning (133)Ba activity distribution in a cylindrical source were addressed by measurements with a 47% n-type HPGe detector and by simulation. Within-sample homogeneity was tested using the count rates from normal and from pure sum peaks. The sensitivity of front versus back source measurements to deviations from uniform distribution was studied. In the case of distributions symmetric with respect to the median plane of the source quantities that can provide information on the distribution of the activity were proposed.

Rapid screening and analysis of alpha- and gamma-emitting radionuclides in liquids using a single sample preparation procedure.

A multifaceted radiochemical testing procedure has been developed to analyze a large number of liquid samples and measure a wide range of radionuclides in a short period of time. This method involves a single, unique and fast sample preparation procedure and allows sequential/concurrent determination of analytes with accuracy and precision. The same prepared sample can be selectively analyzed by gross alpha counting, gamma-ray spectroscopy, and alpha spectroscopy. This method is especially attractive in radiological emergency events where analytical data will be needed urgently as a basis for protective action. Given the simplicity and rapidity of the method, it may be suitable for field portable laboratories, which could save time and the cost associated with the transit of samples to a fixed laboratory. A 100 mL aliquot of sample was spiked with ¹³³Ba and 59Fe tracers and subjected to a chemical separation procedure using a combined BaSO4 and Fe(OH)3 co-precipitation scheme. Then, the gross alpha-particle activity of the prepared sample was measured with a low-background gas-proportional counter, followed by the analysis of its photon-emitters using a gamma-ray spectroscopy system with high-purity intrinsic Ge detectors. Gamma-ray determination of ¹³³Ba and 59Fe tracers was used to assess the chemical recoveries of BaSO4 and Fe(OH)3 fractions, respectively. Selectivity of the radionuclides for co-precipitation with either BaSO4 or Fe(OH)3 components was also investigated. Alpha mass-efficiency curves were derived using ²³°Th and ²4¹Am standards as alpha-calibration sources. Various mixtures of radionuclides, including 54Mn, 57Co, 6°Co, 85Sr, 88Y, ¹°9Cd, ¹¹³Sn, ¹³7Cs, ¹³9Ce, ²°³Hg, ²°9Po, ²²6Ra, ²²8Ra, ²³°Th, ²4¹Am, and natural uranium were used in this study. Most were quantitatively assayed with high chemical recoveries. Alpha-isotope identification and assessment of the prepared sample was achieved by alpha spectroscopy using passivated implanted planar silicon (PIPS) detectors. It has been shown that fission products could potentially be captured and analyzed by this method.

Effects of radionuclide and rainfall characteristics on field loss parameters of grass.

The decrease of foliar activity in vegetation after its initial contamination by foliar deposition is termed "field loss" (Chamberlain, 1970). This work investigated further laboratory data concerning field loss of (134)Cs, (137)Cs, (85)Sr, (133)Ba and (123m)Te deposited on grassland (Madoz-Escande et al., 2005). Treatments consisted in rainfall scenarios cumulating 14 mm per week, combining two levels of intensity (8 or 30 mm/h) and two levels of frequency/precocity (late once or early twice-a-week). The time course of field loss was monitored in the edible tissues which were sampled by mowing between the rainfalls. Data were analyzed with an offset exponential loss model which is applicable to chronic contamination and is consistent with approaches adopted in radiological assessment models. Its parameters were estimated by the maximum-likelihood method, and their accuracy was determined by nonparametric bootstrap. Radionuclide and rainfall conditions significantly affected the estimated rate (lambda(1)) and extent (A(1)) of field loss. Field loss rate (lambda(1)) and nonentrainable fraction (1-A(1)) varied by a factor 1.5-3. Cesium was very mobile but persistent. On the contrary Tellerium was found less labile, but eventually was almost completely eliminated. Strontium and Barium had intermediate behaviors. Field loss was more efficient for moderate late once-a-week rainfalls (8mm/h). Higher rainfall intensity reduced more the radionuclides losses than higher rainfall frequency/precocity. This paper reports statistically relevant effects that should be considered for more realistic assessments.

Validation of rapid methods for the determination of radiostrontium in milk.

A rapid method of (89)Sr and (90)Sr comprising ion chromatography for preconcentration and Sr extraction chromatography for separation of Sr from Ca, Ba and Y was validated with spiked milk samples. An (89)Sr/(90)Sr activity ratio of up to 12 showed the relative bias was within +/-20%. The separation time of Sr was 7h and the chemical recovery of Sr ranged from 80% to 95%. The detection limit for 500 mL milk and 90 min counting time was 0.1 Bq L(-1).

Transgenerational marking of freshwater fishes with enriched stable isotopes: a tool for fisheries management and research.

A promising new method of marking larval freshwater fishes with enriched stable isotopes by means of injecting the maternal parent with the marking agent was investigated. The (138)Ba:(137)Ba ratios in the otoliths of larval golden perch Macquaria ambigua were compared to determine the effect of injecting female broodstock with different dosages of enriched (137)Ba at various times before spawning. There was 100% mark success in the progeny of fish injected with 20 microg g(-1) of enriched (137)Ba 24 h before inducing spawning with hormones and 40 microg g(-1) administered at the same time as inducement of spawning. Injection of 40 microg g(-1) enriched (137)Ba 21 days before spawning resulted in only 81% mark success and suggests rapid elimination of barium in M. ambigua. Injection with enriched (137)Ba did not significantly affect the fertilization rate, number of fertilized eggs or hatching rate compared with long-term hatchery records. These results suggest that transgenerational marking is an effective and affordable means of mass-marking larval fishes. Thousands of larval fishes can be permanently marked with a unique artificial isotopic mark via a single injection into the maternal parent, thus avoiding the handling of individual fishes or having to deal with chemical baths. Because no single mark or tagging method is suitable for all situations, transgenerational marking with enriched stable isotopes provides another method for researchers and managers to discriminate both hatchery-reared and wild fishes.

Weather-dependent change of cesium, strontium, barium and tellurium contamination deposited as aerosols on various cultures.

Various types of plants (wheat, bean, lettuce, radish and grass) were contaminated by dry deposition of radioactive aerosols ((137)Cs, (85)Sr, (133)Ba and (123 m)Te) in order to supplement the radio-ecological data necessary for operational post-accidental codes. A few days after deposition, rainfalls were applied to these cultures to evaluate the influence of some characteristics of the rain on the contamination of the culture over time. On the other hand, for wheat and bean, the influence of the humidity condition of the foliage at the contamination time was considered. For a given plant species at a given vegetative stage, the four radionuclides were intercepted in an identical way. The interception varied from 30% for bean (young sprout) to 80% for lettuce (near maturity). The global transfer factor values were dependent on both the radionuclides and the plant species; nevertheless, a higher value was obtained for cesium, regardless of the plant and the rainfall (from 0.006 m(2)kg(fresh)(-1) for wheat-grains - contaminated at the shooting stage - or for bean-pods - contaminated at the pre-flowering stage - to 0.1m(2)kg(fresh)(-1) for a whole lettuce). The analysis of the results allowed us on the one hand, to extract parameter values of the foliar transfer directly usable in operational codes, in particular those relating to barium and tellurium, unknown until then, and on the other hand, to lay the foundations of a future, more mechanistic model, taking into account the foliar processes in a finer way.

Application of GESPECOR software for the calculation of coincidence summing effects in special cases.

In this work, coincidence summing correction factors have been measured for 133Ba, 152Eu and 88Y point sources with a 50% relative efficiency p-type detector and a 25% relative efficiency n-type detector in two close-to-detector measurement geometries. The experimental data for 133Ba and 152Eu and the results obtained with the GESPECOR software reveal a complex structure of the conventional dead layer of the p-type detector. The high value of the coincidence summing correction factor for the 511 keV peak of 88Y, in agreement with the values computed by GESPECOR, in this case cautions against the application of the semiempirical method for evaluating coincidence summing effects.

Experimental and modelling study on the uptake and desorption kinetics of 133Ba by suspended estuarine sediments from southern Spain.

Dispersion of pollutants in aquatic environments depends on their uptake by suspended solids. This work deals with the uptake kinetics of 133Ba (gamma-emitter and a good analogue of 226Ra) by suspended estuarine sediments (which can be resuspended into the water column under certain conditions). This study presents a wide set of tracing experiments, including second tracing, decantation and desorption processes. The purpose is to characterize 133Ba uptake by sediments and to investigate the use and limitations of box models in order to describe the uptake kinetics. Water and sediment samples were collected in the Huelva estuary (Spain), where environmental 226Ra concentrations have been increased by two phosphate fertilizer industries. Samples were characterized by granulometric, organic carbon content, cation exchange capacity and XRF-EP analyses. Results revealed three-step kinetics, with characteristic times of minutes, hours and days. These results enabled the selection and calibration of a suitable box model and facilitated the testing of its use as a fully predictive tool.

Preconcentration of radium isotopes from natural waters using MnO2 Resin.

We have characterized "MnO2 Resin," a new resin developed by the PG Research Foundation, for radium adsorption over wide ranges of pH, reaction times and salt concentrations. We show that the sorption of 133Ba (used as a proxy for Ra) is highly dependent on pH with the most useful range from pH 4 to 8. The surface layers of the Mn oxides apparently become more positively charged under acidic conditions (below pH 4), which prevents diffusion of positively charged alkaline earth species (e.g. Ba2+, Ra2+) into the sorption sites. Adsorption at higher pH is thought to be inhibited because of carbonate complexation. We found that the sorption characteristics for radium onto MnO2 Resin are especially favorable for low-salinity waters but the sorption is still very satisfactory for highly salted solutions (KD=2.8x10(4) in both cases) but with slower kinetics. For analytical purposes, both column and pump experiments showed high recoveries with no measurable discrimination between Ra and Ba regardless of flow rates in fresh water. Seawater tests showed that recoveries of Ra and Ba are lower than fresh water at elevated flow rates with Ra adsorption higher than Ba at flow rates above 10 ml/min.

Attenuation coefficients of soils and some building materials of Bangladesh in the energy range 276-1332 keV.

The linear and mass attenuation coefficients of different types of soil, sand, building materials and heavy beach mineral samples from the Chittagong and Cox's Bazar area of Bangladesh were measured using a high-resolution HPGe detector and the gamma-ray energies 276.1, 302.8, 356.0, 383.8, 661.6 and 1173.2 and 1332.5 keV emitted from point sources of 133Ba, 137Cs and 60Co, respectively. The linear attenuation coefficients show a linear relationship with the corresponding densities of the samples studied. The variations of the mass attenuation coefficient with gamma-ray energy were exponential in nature. The measured mass attenuation coefficient values were compared with measurements made in other countries for similar kinds of materials. The values are in good agreement with each other in most cases.

Room-temperature semiconductor detectors for in vivo monitoring of internal contamination.

In vivo monitoring of low-energy X-ray and gamma-ray emitters has always been a difficult task, primarily because of lack of accuracy and the high detection limits of classical techniques. Various types of PIN diodes (diodes with a large intrinsic zone) were tested in the Radiation Protection Department of the Studie Centrum voor Kernenergie, Centre d'étude de l'Energie Nucléaire (Mol, Belgium) in the measurement of radioactive body burden by direct methods. Current research is oriented toward the use of room-temperature diodes for the detection of low-energy photons escaping the body. In this paper, a new counting technique that involves a portable jacket containing the diodes is described. The system uses silicon diodes and is used out of shielding room in order to be near the contamination. With this method rapid analysis and long counting times are possible, stress is reduced, and medical treatment can be optimized. CdZnTe detectors were also evaluated for this measurement technique but this type of detector is better adapted for counting inside a shielding room. The improvement of the accuracy of the measurement, taking into account the effect of the ribs, is described here, as well the associated electronics necessary for this type of counting.