Francesca Quinto

Abundance of live 244Pu in deep-sea reservoirs on Earth points to rarity of actinide nucleosynthesis

Half of the heavy elements including all actinides are produced in r-process nucleosynthesis, whose sites and history remain a mystery. If continuously produced, the Interstellar Medium is expected to build-up a quasi-steady state of abundances of short-lived nuclides (with half-lives ≤100 My), including actinides produced in r-process nucleosynthesis. Their existence in today’s interstellar medium would serve as a radioactive clock and would establish that their production was recent. In particular 244Pu, a radioactive actinide nuclide (half-life=81 My), can place strong constraints on recent r-process frequency and production yield. Here we report the detection of live interstellar 244Pu, archived in Earth’s deep-sea floor during the last 25 My, at abundances lower than expected from continuous production in the Galaxy by about 2 orders of magnitude. This large discrepancy may signal a rarity of actinide r-process nucleosynthesis sites, compatible with neutron-star mergers or with a small subset of actinide-producing supernovae.A. Wallner, 2, ∗ T. Faestermann, J. Feige, C. Feldstein, K. Knie, 5 G. Korschinek, W. Kutschera, A. Ofan, M. Paul, F. Quinto, † G. Rugel, ‡ and P. Steier Department of Nuclear Physics, Research School of Physics and Engineering, The Australian National University, Canberra, Australia VERA Laboratory, Faculty of Physics, University of Vienna, Währinger Strasse 17, A-1090, Austria Technische Universität München, D-85747 Garching, Germany Racah Institute of Physics, Hebrew University, Jerusalem, Israel GSI Helmholtzzentrum für Schwerionenforschung GmbH, Planckstr. 1, 64291 Darmstadt, Germany

The first use of 236U in the general environment and near a shutdown nuclear power plant

We present a first effort to investigate (236)U in the environment near a shutdown nuclear power plant far away from highly contaminated sites, by using accelerator mass spectrometry. The detection limit of about 1pg (236)U allowed us to identify a minimal increase of the (236)U/(238)U isotopic ratio correlated to a peak of (137)Cs in river sediments downstream of the nuclear power plant, and to detect anthropogenic (236)U also upstream, where it is probably not related to the power plant but to global fallout. The (236)U content shoved variations of the (236)U/(238)U isotopic ratio in relation to the chemical-physical characteristics of the sediments. This demonstrates the potential of (236)U as an environmental tracer, and as an indicator for releases from nuclear facilities.

Measurements of 236U in Ancient and Modern Peat Samples and Implications for Postdepositional Migration of Fallout Radionuclides

(236)U was analyzed in an ombrotrophic peat core representing the last 80 years of atmospheric deposition and a minerotrophic peat sample from the last interglacial period. The determination of (236)U at levels of 10(7) atoms/g was possible by using ultraclean laboratory procedures and accelerator mass spectrometry. The vertical profile of the (236)U/(238)U isotopic ratio along the ombrotrophic peat core represents the first observation of the (236)U bomb peak in a terrestrial environment. A constant level of anthropogenic (236)U with an average (236)U/(238)U isotopic ratio of (1.24 ± 0.08) × 10(-6) in the top layers of the core was observed. Comparing the abundances of the global fallout derived (236)U and (239)Pu along the peat core, the post depositional migration of plutonium clearly exceeds that of uranium. However, the cumulative (236)U/(239)Pu ratio of 0.62 ± 0.31 is in agreement with previous studies on the global fallout uranium and plutonium. In the interglacial peat samples a (236)U/(238)U isotopic ratio of (3.3 ± 0.7) × 10(-12) was detected; although this measurement is an upper limit, it constitutes a significant step forward in the experimental determination of the natural (236)U abundance and represents a true background sample for the ombrotrophic peat core.

Accelerator mass spectrometry of actinides in ground- and seawater: An innovative method allowing for the simultaneous analysis of U, Np, Pu, Am, and Cm isotopes below ppq levels

(236)U, (237)Np, and Pu isotopes and (243)Am were determined in ground- and seawater samples at levels below ppq (fg/g) with a maximum sample size of 250 g. Such high sensitivity was possible by using accelerator mass spectrometry (AMS) at the Vienna Environmental Research Accelerator (VERA) with extreme selectivity and recently improved efficiency and a significantly simplified separation chemistry. The use of nonisotopic tracers was investigated in order to allow for the determination of (237)Np and (243)Am, for which isotopic tracers either are rarely available or suffer from various isobaric mass interferences. In the present study, actinides were concentrated from the sample matrix via iron hydroxide coprecipitation and measured sequentially without previous chemical separation from each other. The analytical method was validated by the analysis of the Reference Material IAEA 443 and was applied to groundwater samples from the Colloid Formation and Migration (CFM) project at the deep underground rock laboratory of the Grimsel Test Site (GTS) and to natural water samples affected solely by global fallout. While the precision of the presented analytical method is somewhat limited by the use of nonisotopic spikes, the sensitivity allows for the determination of ∼10(5) atoms in a sample. This provides, e.g., the capability to study the long-term release and retention of actinide tracers in field experiments as well as the transport of actinides in a variety of environmental systems by tracing contamination from global fallout.

OPTIMIZATION OF 236U AMS AT CIRCE

Actinide isotopes are present in environmental samples at ultra-trace levels (236U concentration is quoted to be on the order of pg/kg or fg/kg). Their detection requires the resolution of mass spectrometry (MS) techniques, but only accelerator mass spectrometry (AMS) has the sensitivity required. In order to perform the isotopic ratio measurements of actinides, such as 236U/238U, an upgrade of the Center for Isotopic Research on Cultural and Environmental Heritage accelerator (CIRCE) in Caserta, Italy, has been performed. The system was originally equipped for radiocarbon AMS measurements. The main difficulty of AMS measurement of 236U is the intense neighboring beam of 238U. Although most of the 238U ions are suppressed by means of magnetic and electrostatic elements, a small fraction of this intense beam can interfere with the rare isotopes. This paper reports the preliminary results of the 236U/238U isotopic ratio measurement limit <5.6 x 10^(-11)), aimed also to better understand the origin of background ions. For this purpose, a large 16-strip silicon detector providing spatial resolution has been used. In addition, calculations to assess the performance of the system obtained by adding a high-resolution time of flight-energy (TOF-E) detector are discussed.

137Cs, 60Co and 40K uptake by lettuce plants in two distributions of soil contamination.

(137)Cs and (60)Co, two of the radionuclides more representative of discharges from nuclear facilities, are of interest for radiological protections because of their great mobility in biosphere and affinity with biological systems. The aim of the present work is the investigation of the possible influence of the vertical distribution of (137)Cs and (60)Co in soil upon their uptake by lettuce as function of plants growth. An experiment ad hoc has been carried out in field conditions. The results show that (i) the transfer of (137)Cs and (60)Co from soil to lettuce is independent by their distribution in soil, (ii) the soil-plant transfer factors of (137)Cs and (60)Co show a similar trend vs. growth stage, (iii) the (40)K transfer factor trend is different from those of anthropogenic radionuclides, and (iv) (137)Cs and (60)Co specific activities are about 1Bq/kg, in the mature vegetable with soil activity from 9 to 21kBq/m(2).

Multiactinide Analysis with Accelerator Mass Spectrometry for Ultratrace Determination in Small Samples: Application to an in Situ Radionuclide Tracer Test within the Colloid Formation and Migration Experiment at the Grimsel Test Site (Switzerland)

The multiactinide analysis with accelerator mass spectrometry (AMS) was applied to samples collected from the run 13-05 of the Colloid Formation and Migration (CFM) experiment at the Grimsel Test Site (GTS). In this in situ radionuclide tracer test, the environmental behavior of 233U, 237Np, 242Pu, and 243Am was investigated in a water conductive shear zone under conditions relevant for a nuclear waste repository in crystalline rock. The concentration of the actinides in the GTS groundwater was determined with AMS over 6 orders of magnitude from ∼15 pg/g down to ∼25 ag/g. Levels above 10 fg/g were investigated with both sector field inductively coupled plasma mass spectrometry (SF-ICPMS) and AMS. Agreement within a relative uncertainty of 50% was found for 237Np, 242Pu, and 243Am concentrations determined with the two analytical methods. With the extreme sensitivity of AMS, the long-term release and retention of the actinides was investigated over 8 months in the tailing of the breakthrough curve of run 13-05 as well as in samples collected up to 22 months after. Furthermore, the evidence of masses 241 and 244 u in the CFM samples most probably representing 241Am and 244Pu employed in a previous tracer test demonstrated the analytical capability of AMS for in situ studies lasting more than a decade.