AMS of the Minor Plutonium Isotopes.

VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure 239Pu, 240Pu, 241Pu, 242Pu and 244Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of 244Pu/239Pu = (5.7 ± 1.0) × 10-5 based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the 242Pu/240Pu ratio as an estimate of the initial 241Pu/239Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method.

Uncertainty budget for a whole body counter in the scan geometry and computer simulation of the calibration phantoms.

At the Austrian Research Centers Seibersdorf (ARCS), a whole body counter (WBC) in the scan geometry is used to perform routine measurements for the determination of radioactive intake of workers. The calibration of the WBC is made using bottle phantoms with a homogeneous activity distribution. The same calibration procedures have been simulated using Monte Carlo N-Particle (MCNP) code and FLUKA and the results of the full energy peak efficiencies for eight energies and five phantoms have been compared with the experimental results. The deviation between experiment and simulation results is within 10%. Furthermore, uncertainty budget evaluations have been performed to find out which parameters make substantial contributions to these differences. Therefore, statistical errors of the Monte Carlo simulation, uncertainties in the cross section tables and differences due to geometrical considerations have been taken into account. Comparisons between these results and the one with inhomogeneous distribution, for which the activity is concentrated only in certain parts of the body (such as head, lung, arms and legs), have been performed. The maximum deviation of 43% from the homogeneous case has been found when the activity is concentrated on the arms.

Determination of plutonium in environmental samples by AMS and alpha spectrometry.

Environmental samples from nuclear weapons test sites at the atolls of Mururoa and Fangataufa (French Polynesia, south Pacific) have been analyzed for their content of plutonium isotopes by applying the independent techniques of decay counting (Alpha Spectrometry) and accelerator mass spectrometry (AMS). Here, we propose the combination of both techniques which results in a maximum of information on the isotopic signature of Pu in environmental samples. Plutonium was chemically separated from the bulk material by anion exchange. (242)Pu was used as an internal standard for both AMS and alpha spectrometry. The samples for alpha spectrometry were prepared by micro-precipitation with NdF(3). After alpha spectrometry, the samples were reprocessed for AMS. Pu was co-precipitated with Fe(OH)(3) and finally, solid samples were prepared. At the VERA (Vienna Environmental Research Accelerator) facility, the various Pu isotopes were separated by their isotopic masses and quantified by the AMS technique. A good agreement of the results obtained from the AMS measurements was found with those obtained from Alpha Spectrometry. Overall, the data agree on average within 10% of each other. Isotope ratios for (238)Pu, (239)Pu and (240)Pu can be extracted from our investigations. Alpha spectrometry delivers data for the (238)Pu and the combination of ((239+240))Pu concentrations in those samples. In addition, the AMS technique provides information on the individual concentrations of (240)Pu and (239)Pu.

Investigation of food contamination since the Chernobyl fallout in Austria.

In a large-scale investigation the decrease of the activity concentration of 137Cs in foodstuffs after the widespread Chernobyl fallout was determined. At different times after the deposition in 1986 more than 1000 samples of various foodstuffs in Austria were taken and investigated with regard to their activity concentration. The investigation showed that in the first year after deposition, the activity concentration decreased to about 6-10% (milk, fruit), and 3-6%, respectively (grain, potatoes, vegetables) of the values in the fallout maximum. The calculated effective half-lives are significantly shorter than observed after nuclear weapon test series and result in a smaller long-term exposure than estimated before. The effective ingestion dose in the 50 years following of a one-time nuclear fallout amounts to about 1.3 times of the first year ingestion dose. In 2002, the ingestion dose in Austria amounts to 2.24 microSv (adult), or 0.88 microSv (5-year infant) respectively, which is less than 0.5% of the ingestion dose of the first year and amounts to 0.7% of the ingestion dose from natural radionuclides.

Certified Reference Material IAEA-446 for radionuclides in Baltic Sea seaweed.

A Certified Reference Material (CRM) for radionuclides in seaweed (Fucus vesiculosus) from the Baltic Sea (IAEA-446) is described and the results of the certification process are presented. The (40)K, (137)Cs, (234)U and (239+240)Pu radionuclides were certified for this material, and information values for 12 other radionuclides ((90)Sr, (99)Tc, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (230)Th, (232)Th, (235)U, (238)U, (239)Pu and (240)Pu) are presented. The CRM can be used for Quality Assurance/Quality Control of analysis of radionuclides in seaweed and other biota samples, as well as for development and validation of analytical methods, and for training purposes.

Determination of U, Pu and Am isotopes in Irish Sea sediment by a combination of AMS and radiometric methods.

Samples from a marine sediment core from the Irish Sea (54.416 N, 3.563 W) were analyzed for the isotopic composition of uranium, plutonium and americium by a combination of radiometric methods and AMS. The radiochemical procedure consisted of a Pu separation step by anion exchange, subsequent U separation by extraction chromatography using UTEVA® and finally Am separation with TRU® Resin. Additionally to radiometric determination of these isotopes by alpha spectrometry, the separated samples were also used for the determination of (236)U/(238)U and plutonium isotope ratios by Accelerator Mass Spectrometry (AMS) at the VERA facility.