Comparing levoglucosan and mannosan ratios in sediments and corresponding aerosols from recent Australian fires.

The monosaccharide anhydrides levoglucosan, mannosan, and galactosan are known as 'fire sugars' as they are powerful proxies used to trace fire events. Despite their increasing use, their application is not completely understood, especially in the context of tracing past fire events using sediment samples. There are many uncertainties about fire sugar formation, partitioning, transport, complexation, and stability along all stages of the source-to-sink pathway. While these uncertainties exist, the efficacy of fire sugars as fire tracers remains limited. This study compared high-resolution fire sugar fluxes in freshwater sediment cores to known fire records in Tasmania, Australia. Past fire events correlated with fire sugar flux increases down-core, with the magnitude of the flux inversely proportional to the distance of the fires from the study site. For the first time, fire sugar ratios (levoglucosan/mannosan, L/M) in aerosols were compared with those in sediments from the same time-period. The L/M ratio in surface sediments (1.42-2.58) were significantly lower than in corresponding aerosols (5.08-15.62). We propose two hypotheses that may explain the lower average L/M of sediments. Firstly, the degradation rate of levoglucosan is higher than mannosan in the water column, sediment-water interface, and/or sediment. Secondly, the L/M ratio of non-atmospheric emissions during fires may be lower than that of atmospheric emissions from the same fire. Due to the uncertainties about transport partitioning (atmospheric versus non-atmospheric emissions) and fire sugar degradation along all stages of the source-to-sink pathway, we advise caution when inferring vegetation type (e.g. softwood, hardwood, or grasses) based purely on fire sugar ratios in sediments (e.g. L/M ratio). Future investigations are required to increase the efficacy of fire sugars as a complimentary, or standalone, fire tracer in sediments.

Accelerator mass spectrometry measurements of 233U in groundwater, soil and vegetation at a legacy radioactive waste site.

Low-level radioactive wastes were disposed at the Little Forest Legacy Site (LFLS) near Sydney, Australia between 1960 and 1968. According to the disposal records, 233U contributes a significant portion of the inventory of actinide activity buried in the LFLS trenches. Although the presence of 233U in environmental samples from LFLS has been previously inferred from alpha-spectrometry measurements, it has been difficult to quantify because the 233U and 234U α-peaks are superimposed. Therefore, the amounts of 233U in groundwaters, soils and vegetation from the vicinity of the LFLS were measured using accelerator mass spectrometry (AMS). The AMS results show the presence of 233U in numerous environmental samples, particularly those obtained within, and in the immediate vicinity of, the trenched area. There is evidence for dispersion of 233U in groundwater (possibly mobilised by co-disposed organic liquids), and the data also suggest other sources of 233U contamination in addition to the trench wastes. These may include leakages and spills from waste drums as well as waste burnings, which also occurred at the site. The AMS results confirm the historic information regarding disposal of 233U in the LFLS trenches. The AMS technique has been valuable to ascertain the distribution and environmental behaviour of 233U at the LFLS and the results demonstrate the applicability of AMS for evaluating contamination of 233U at other radioactive waste sites.

A record of fallout 239Pu and 240Pu at World Heritage Bathurst Harbour, Tasmania, Australia.

This study presents the first measurements of anthropogenic plutonium (239Pu and 240Pu) concentrations and atom ratios (240Pu/239Pu) for Tasmania, in sediment collected from Bathurst Harbour, in the Tasmanian Wilderness World Heritage Area, Australia. The weighted mean 240Pu/239Pu atom ratio measured at this site was 0.172 ± 0.007 which is consistent with published data from mainland Australia and global and Southern Hemisphere averages. The 240Pu/239Pu atom ratios ranged between 0.11 and 0.21 with the earliest recorded 240Pu/239Pu atom ratios being the lowest, suggesting an influence of low atom ratio fallout from nuclear testing in Australia. Post-moratorium fallout 240Pu/239Pu atom ratios were consistent with other records. Lead-210 (210Pb) sediment chronologies indicate sediment accumulation rates have increased since the early part of the 19th century at this location.

Radionuclides in sea turtles at the Montebello Islands former nuclear test sites: Current and historical dose rates for adults and embryos.

Radionuclides from 1950s weapons testing at the Montebello Islands, Western Australia, may impact sea turtle embryos incubating within eggs laid in contaminated sands or be taken up into adult body tissues where they can contribute to radiation dose over a turtles' 60+ year lifespan. We measured plutonium in all local samples including turtle skin, bones, hatchlings, eggshells, sea sediments, diet items and beach sands. The amount of Pu in developing embryos/hatchling samples was orders of magnitude lower than that in the surrounding sands. These contaminated sands caused most dose to eggs (external dose from 137Cs, 152Eu), while most of the dose to adults was from internalised radionuclides (98%). While current dose rates are relatively low, local dose rates were high for about ten years following the 1950s detonations and may have resulted in lethality or health impacts to a generation of turtles that likely carry biomarkers today.

Challenges associated with the behaviour of radioactive particles in the environment.

A series of different nuclear sources associated with the nuclear weapon and fuel cycles have contributed to the release of radioactive particles to the environment. Following nuclear weapon tests, safety tests, conventional destruction of weapons, reactor explosions and fires, a major fraction of released refractory radionuclides such as uranium (U) and plutonium (Pu) were present as entities ranging from sub microns to fragments. Furthermore, radioactive particles and colloids have been released from reprocessing facilities and civil reactors, from radioactive waste dumped at sea, and from NORM sites. Thus, whenever refractory radionuclides are released to the environment following nuclear events, radioactive particles should be expected. Results from many years of research have shown that particle characteristics such as elemental composition depend on the source, while characteristics such as particle size distribution, structure, and oxidation state influencing ecosystem transfer depend also on the release scenarios. When radioactive particles are deposited in the environment, weathering processes occur and associated radionuclides are subsequently mobilized, changing the apparent Kd. Thus, particles retained in soils or sediments are unevenly distributed, and dissolution of radionuclides from particles may be partial. For areas affected by particle contamination, the inventories can therefore be underestimated, and impact and risk assessments may suffer from unacceptable large uncertainties if radioactive particles are ignored. To integrate radioactive particles into environmental impact assessments, key challenges include the linking of particle characteristics to specific sources, to ecosystem transfer, and to uptake and retention in biological systems. To elucidate these issues, the EC-funded COMET and RATE projects and the IAEA Coordinated Research Program on particles have revisited selected contaminated sites and archive samples. This COMET position paper summarizes new knowledge on key sources that have contributed to particle releases, including particle characteristics based on advanced techniques, with emphasis on particle weathering processes as well as on heterogeneities in biological samples to evaluate potential uptake and retention of radioactive particles.

Measurement of (233)U/(234)U ratios in contaminated groundwater using alpha spectrometry.

The uranium isotope (233)U is not usually observed in alpha spectra from environmental samples due to its low natural and fallout abundance. It may be present in samples from sites in the vicinity of nuclear operations such as reactors or fuel reprocessing facilities, radioactive waste disposal sites or sites affected by clandestine nuclear operations. On an alpha spectrum, the two most abundant alpha emissions of (233)U (4.784 MeV, 13.2%; and 4.824 MeV, 84.3%) will overlap with the (234)U doublet peak (4.722 MeV, 28.4%; and 4.775 MeV, 71.4%), if present, resulting in a combined (233+234)U multiplet. A technique for quantifying both (233)U and (234)U from alpha spectra was investigated. A series of groundwater samples were measured both by accelerator mass spectrometry (AMS) to determine (233)U/(234)U atom and activity ratios and by alpha spectrometry in order to establish a reliable (233)U estimation technique using alpha spectra. The Genie™ 2000 Alpha Analysis and Interactive Peak Fitting (IPF) software packages were used and it was found that IPF with identification of three peaks ((234)U minor, combined (234)U major and (233)U minor, and (233)U major) followed by interference correction on the combined peak and a weighted average activity calculation gave satisfactory agreement with the AMS data across the (233)U/(234)U activity ratio range (0.1-20) and (233)U activity range (2-300 mBq) investigated. Correlation between the AMS (233)U and alpha spectrometry (233)U was r(2) = 0.996 (n = 10).