Since the 1956 completion of nuclear testing at the Montebello Islands, Western Australia, this remote uninhabited island group has been relatively undisturbed (no major remediations) and currently ...functions as high-value marine and terrestrial habitat within the Montebello/Barrow Islands Marine Conservation Reserves. The former weapons testing sites, therefore, provide a unique opportunity for assessing the fate and behaviour of Anthropocene radionuclides subjected to natural processes across a range of shallow-marine to island-terrestrial ecological units (ecotopes). We collected soil, sediment and biota samples and analysed their radionuclide content using gamma and alpha spectrometry, photostimulated luminescence autoradiography and accelerator mass spectrometry.
We found the activity levels of the fission and neutron-activation products have decreased by ~hundred-fold near the ground zero locations. However, Pu concentrations remain elevated, some of which are high relative to most other Australian and international sites (up to 25,050 Bq kg−1 of 239+240+241Pu). Across ecotopes, Pu ranked from highest to lowest in the following order: island soils > dunes > foredunes > marine sediments > and beach intertidal zone. Low values of Pu and other radionuclides were detected in all local wildlife tested including endangered species. Activity concentrations ranked (highest to lowest) terrestrial arthropods > terrestrial mammal and reptile bones > algae > oyster flesh > whole crab > sea turtle bone > stingray and teleost fish livers > sea cucumber flesh > sea turtle skin > teleost fish muscle. The three detonations (one from within a ship and two from 30 m towers) resulted in differing contaminant forms, with the ship detonation producing the highest activity concentrations and finer more inhalable particulate forms. The three sites are distinct in their 240/239Pu and 241/239Pu atom ratios, including the Pu transported by natural process or within migratory living organisms.
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•1950s nuclear tests have left a legacy of long-lived radionuclides.•Today, the sites have high value as marine and terrestrial habitats.•Pu is persistent, but in variable amounts across marine-to-terrestrial ecotopes.•The dominant Pu in all marine and terrestrial wildlife was locally-sourced.•Pu remains a long-term exposure concern to human visitors and wildlife.
Nuclides synthesized in massive stars are ejected into space via stellar winds and supernova explosions. The solar system (SS) moves through the interstellar medium and collects these nucleosynthesis ...products. One such product is 60Fe, a radionuclide with a half-life of 2.6 My that is predominantly produced in massive stars and ejected in supernova explosions. Extraterrestrial 60Fe has been found on Earth, suggesting close-by supernova explosions ∼2 to 3 and ∼6 Ma. Here, we report on the detection of a continuous interstellar 60Fe influx on Earth over the past ∼33,000 y. This time period coincides with passage of our SS through such interstellar clouds, which have a significantly larger particle density compared to the local average interstellar medium embedding our SS for the past few million years. The interstellar 60Fe was extracted from five deep-sea sediment samples and accelerator mass spectrometry was used for single-atom counting. The low number of 19 detected atoms indicates a continued but low influx of interstellar 60Fe. The measured 60Fe time profile over the 33 ky, obtained with a time resolution of about ±9 ky, does not seem to reflect any large changes in the interstellar particle density during Earth’s passage through local interstellar clouds, which could be expected if the local cloud represented an isolated remnant of the most recent supernova ejecta that traversed the Earth ∼2 to 3 Ma. The identified 60Fe influx may signal a late echo of some million-year-old supernovae with the 60Fe-bearing dust particles still permeating the interstellar medium.
The mobility of plutonium (Pu) in soils, and its uptake into a range of wildlife, were examined using recent and ∼25 year old data from the Taranaki area of the former Maralinga weapons test site, ...Australia. Since its initial deposition in the early 1960s, the dispersed Pu has been incorporated into the soil profile and food chain through natural processes, allowing for the study of Pu sequestration and dynamics in relatively undisturbed semi-arid conditions.
The data indicate downward mobility of Pu in soil at rates of ∼0.2–0.3 cm per year for the most mobile fraction. As a result, while all of the Pu was initially deposited on the ground surface, approximately 93% and 62% remained in the top 0–2 cm depth after 25- and 50-years respectively. No large-scale lateral spreading of the Taranaki plume was observed. Pu activity concentrations in 0–1 cm soils with biotic crusts were not elevated when compared with nearby bare soils, although a small number of individual data suggest retention of Pu-containing particles may be occurring in some biotic crusts.
Soil-to-animal transfer, as measured by concentration ratios (CRwo-soil), was 4.1E−04 (Geometric Mean (GM)) in mammals, which aligns well with those from similar species and conditions (such as the Nevada Test Site, US), but are lower than the GM of the international mammal data reported in the Wildlife Transfer Database (WTD). These lower values are likely due to the presence of a low-soluble, particulate form of the Pu in Maralinga soils. Arthropod concentration ratios (3.1E−03 GM), were similar to those from Rocky Flats, US, while values for reptiles (2.0E−02 GM) were higher than the WTD GM value which was dominated by data from Chernobyl. Comparison of uptake data spanning approximately 30 years indicates no decrease over time for mammals, and a potential increase for reptiles. The results confirm the persistence of bioavailable Pu after more than 50 years since deposition, and also the presence of larger-sized particles which currently affect CRwo-soil calculations, and which may serve as an ongoing source of bioavailable Pu as they are subjected to weathering into the future.
•Plutonium in soils and wildlife was studied at Maralinga, Australia.•Downward mobility of Pu in soil is occurring at ∼0.2–0.3 cm per year.•Soil-to-animal transfer has persisted at about the same rates over the last 30 yrs.•Soil-to-animal transfer is lower for mammals compared with reference values.•Concentration ratio calculations are influenced by low-solubility Pu particles.
Natural plutonium from supernovaeThe rapid neutron capture process (r-process) produces many of the heavy chemical elements, but the astrophysical settings where it occurs remain unclear. Leading ...candidates are neutron star mergers and some types of supernovae. Wallner et al. analyzed the plutonium content of a deep-sea crust sample, identifying a few dozen atoms of the r-process isotope plutonium- 244 that were delivered to Earth within the past few million years. There was a simultaneous signal of iron-60, which is known to be produced in supernovae. Comparing the ratios of these isotopes constrains the relative contributions of supernovae and neutron star mergers to r-process nucleosynthesis.Science, this issue p. 742Half of the chemical elements heavier than iron are produced by the rapid neutron capture process (r-process). The sites and yields of this process are disputed, with candidates including some types of supernovae (SNe) and mergers of neutron stars. We search for two isotopic signatures in a sample of Pacific Ocean crust—iron-60 (60Fe) (half-life, 2.6 million years), which is predominantly produced in massive stars and ejected in supernova explosions, and plutonium-244 (244Pu) (half-life, 80.6 million years), which is produced solely in r-process events. We detect two distinct influxes of 60Fe to Earth in the last 10 million years and accompanying lower quantities of 244Pu. The 244Pu/60Fe influx ratios are similar for both events. The 244Pu influx is lower than expected if SNe dominate r-process nucleosynthesis, which implies some contribution from other sources.
Actinides AMS on the VEGA accelerator Hotchkis, M.A.C.; Child, D.P.; Froehlich, M.B. ...
Nuclear instruments & methods in physics research. Section B, Beam interactions with materials and atoms,
01/2019, Letnik:
438
Journal Article
Recenzirano
The VEGA 1MV accelerator at ANSTO is designed to be a highly versatile AMS instrument. In this paper we focus on describing those aspects of the system that are designed to optimise its performance ...for actinides isotopic analysis, in particular the implementation of fast isotope cycling and multiple isotope detection methods to enable isotope detection across a wide range of rates and currents. Charge state yields are reported in the energy range from 0.3 to 1.0 MeV with helium gas stripping, showing that the highest yield for the 3+ charge state occurs around 1 MeV and exceeds 40%. Accuracy and precision for uranium isotope ratios are shown to approach 1% over a wide range of concentrations and isotope ratios. The ionisation efficiency for plutonium is shown to exceed 3%, leading to overall detection efficiency over 1%. In the absence of background, this leads to sub-attogram detection limits for several Pu isotopes including 244Pu.
We examined the distribution of plutonium (Pu) in the tissues of mammalian wildlife inhabiting the relatively undisturbed, semi-arid former Taranaki weapons test site, Maralinga, Australia. The ...accumulation of absorbed Pu was highest in the skeleton (83% ± 6%), followed by muscle (10% ± 9%), liver (6% ± 6%), kidneys (0.6% ± 0.4%), and blood (0.2%). Pu activity concentrations in lung tissues were elevated relative to the body average. Foetal transfer was higher in the wildlife data than in previous laboratory studies. The amount of Pu in the gastrointestinal tract was highly elevated relative to that absorbed within the body, potentially increasing transfer of Pu to wildlife and human consumers that may ingest gastrointestinal tract organs. The Pu distribution in the Maralinga mammalian wildlife generally aligns with previous studies related to environmental exposure (e.g. Pu in humans from worldwide fallout), but contrasts with the partitioning models that have traditionally been used for human worker-protection purposes (approximately equal deposition in bone and liver) which appear to under-predict the skeletal accumulation in environmental exposure conditions.
•Accumulation of absorbed Pu in the skeleton was highest among wildlife mammalian tissues.•The lungs and the gastrointestinal tract had relatively high Pu activity concentrations.•Results differ from traditional Pu partitioning models used for humans.
Half of the chemical elements heavier than iron are produced by the rapid neutron capture process (r-process). The sites and yields of this process are disputed, with candidates including some types ...of supernovae (SNe) and mergers of neutron stars. We search for two isotopic signatures in a sample of Pacific Ocean crust-iron-60 (
Fe) (half-life, 2.6 million years), which is predominantly produced in massive stars and ejected in supernova explosions, and plutonium-244 (
Pu) (half-life, 80.6 million years), which is produced solely in r-process events. We detect two distinct influxes of
Fe to Earth in the last 10 million years and accompanying lower quantities of
Pu. The
Pu/
Fe influx ratios are similar for both events. The
Pu influx is lower than expected if SNe dominate r-process nucleosynthesis, which implies some contribution from other sources.
The British government performed a number of nuclear weapon tests on Australian territory from 1952 through to 1963 with the cooperation of the Australian government. Nine fission bombs were ...detonated in South Australia at Emu Junction and Maralinga, and a further three fission weapons were detonated in the Monte Bello Islands off the coast of Western Australia. A number of soil samples were collected by the Australian Radiation Laboratories in 1972 and 1978 during field surveys at these nuclear weapon test sites. They were analysed by gamma spectrometry and, for a select few samples, by alpha spectrometry to measure the remaining activities of fission products, activation products and weapon materials. We have remeasured a number of these Montebello Islands and Emu Junction soil samples using the ANTARES AMS facility, ANSTO. These samples were analysed for plutonium and uranium isotopic ratios and isotopic concentrations. Very low 240Pu/239Pu ratios were measured at both sites (∼0.05 for Alpha Island and ∼0.02 for Emu Field), substantially below global fallout averages. Well correlated but widely varying 236U and plutonium concentrations were measured across both sites, but 233U did not correlate with these other isotopes and instead showed correlation with distance from ground zero, indicating in situ production in the soils.
Nuclides synthesized in massive stars are ejected into space via stellar winds and supernova explosions. The solar system (SS) moves through the interstellar medium and collects these nucleosynthesis ...products. One such product is
Fe, a radionuclide with a half-life of 2.6 My that is predominantly produced in massive stars and ejected in supernova explosions. Extraterrestrial
Fe has been found on Earth, suggesting close-by supernova explosions ∼2 to 3 and ∼6 Ma. Here, we report on the detection of a continuous interstellar
Fe influx on Earth over the past ∼33,000 y. This time period coincides with passage of our SS through such interstellar clouds, which have a significantly larger particle density compared to the local average interstellar medium embedding our SS for the past few million years. The interstellar
Fe was extracted from five deep-sea sediment samples and accelerator mass spectrometry was used for single-atom counting. The low number of 19 detected atoms indicates a continued but low influx of interstellar
Fe. The measured
Fe time profile over the 33 ky, obtained with a time resolution of about ±9 ky, does not seem to reflect any large changes in the interstellar particle density during Earth's passage through local interstellar clouds, which could be expected if the local cloud represented an isolated remnant of the most recent supernova ejecta that traversed the Earth ∼2 to 3 Ma. The identified
Fe influx may signal a late echo of some million-year-old supernovae with the
Fe-bearing dust particles still permeating the interstellar medium.
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