60Fe and 244Pu deposited on Earth constrain the r-process yields of recent nearby supernovae.

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 (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.

60Fe deposition during the late Pleistocene and the Holocene echoes past supernova activity.

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.

Plutonium and other radionuclides persist across marine-to-terrestrial ecotopes in the Montebello Islands sixty years after nuclear tests.

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.

Measurement of fallout radionuclides, (239)(,240)Pu and (137)Cs, in soil and creek sediment: Sydney Basin, Australia.

Soil and sediment samples from the Sydney basin were measured to ascertain fallout radionuclide activity concentrations and atom ratios. Caesium-137 ((137)Cs) was measured using gamma spectroscopy, and plutonium isotopes ((239)Pu and (240)Pu) were quantified using accelerator mass spectrometry (AMS). Fallout radionuclide activity concentrations were variable ranging from 0.6 to 26.1 Bq/kg for (137)Cs and 0.02-0.52 Bq/kg for (239+240)Pu. Radionuclides in creek sediment samples were an order of magnitude lower than in soils. (137)Cs and (239+240)Pu activity concentration in soils were well correlated (r(2) = 0.80) although some deviation was observed in samples collected at higher elevations. Soil ratios of (137)Cs/(239+240)Pu (decay corrected to 1/1/2014) ranged from 11.5 to 52.1 (average = 37.0 ± 12.4) and showed more variability than previous studies. (240)Pu/(239)Pu atom ratios ranged from 0.117 to 0.165 with an average of 0.146 (±0.013) and an error weighted mean of 0.138 (±0.001). These ratios are lower than a previously reported ratio for Sydney, and lower than the global average. However, these ratios are similar to those reported for other sites within Australia that are located away from former weapons testing sites and indicate that atom ratio measurements from other parts of the world are unlikely to be applicable to the Australian context.

Accumulation of plutonium in mammalian wildlife tissues following dispersal by accidental-release tests.

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.

Plutonium in wildlife and soils at the Maralinga legacy site: persistence over decadal time scales.

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.

Design of a compact electron cyclotron resonance ion source for medium charge state light ions.

At the Australian Nuclear Science and Technology Organization we are developing a new isotope ratio mass spectrometer based on the measurement of multiple charge state ions. We have carried out a review of our existing ECR ion source and identified a number of design flaws. For the new instrument, we are producing a new ECR source and have refined the design, in particular by using 3D simulations to improve the magnetic confinement field and by a combination of simulations and experiments to improve the design of the microwave coupling.

Performance of an electron cyclotron resonance ion source designed for isotope ratio mass spectrometry.

We have designed, built, and tested an electron cyclotron resonance ion source suited to the needs of an experimental program examining new methods of isotope ratio mass spectrometry using multiply charged ions. Contaminant levels have been reduced to low levels. Sample absorption and desorption effects are under investigation and preliminary results are presented.

Ultra-low-level determination of (236)U in IAEA marine reference materials by ICPMS and AMS.

The development of analytical procedures for the measurement of ultra-low levels of (236)U in marine samples using high-resolution inductively coupled plasma mass spectrometry (HR-ICPMS) and accelerator mass spectrometry (AMS) techniques are discussed and results are presented for IAEA reference materials-marine sediments (IAEA-135, 306, 384 and 385), marine biota (IAEA-134 and 414) and seawater (IAEA-381), collected in areas affected by nuclear reprocessing plants and nuclear weapons tests. The obtained minimum detection limit of the (236)U/(238)U atom ratio was 1x10(-8) for AMS and 1x10(-6) for HR-ICPMS.