Retrospective determination of fallout radionuclides and 236U/238U, 233U/236U and 240Pu/239Pu atom ratios on air filters from Vienna and Salzburg, Austria.

137Cs and 241Pu (via 241Am) concentrations were measured γ-spectrometrically on air filters from the early 1960s (mainly from 1964-66) from Vienna, Austria, and an alpine station in Salzburg, Austria. Accelerator mass spectrometry (AMS) was used to determine 240Pu/239Pu, 236U/238U and 233U/236U atom ratios as well as 236U, 239Pu and 240Pu atom concentrations. The maximum 236U/238U atom ratio of these unique undisturbed global fallout samples was (1.19 ± 0.31) × 10-5 in spring 1964. The 233U/236U atom ratios were found within (0.15-0.49) × 10-2 and indicate that the weapons tests of the early 1960s can be excluded as 233U source. The 236U/239Pu atom ratios were calculated in the range of 0.22-0.48.

Anthropogenic 236U and 233U in the Baltic Sea: Distributions, source terms, and budgets.

The Baltic Sea receives substantial amounts of hazardous substances and nutrients, which accumulate for decades and persistently impair the Baltic ecosystems. With long half-lives and high solubility, anthropogenic uranium isotopes (236U and 233U) are ideal tracers to depict the ocean dynamics in the Baltic Sea and the associated impacts on the fates of contaminants. However, their applications in the Baltic Sea are hampered by the inadequate source-term information. This study reports the first three-dimensional distributions of 236U and 233U in the Baltic Sea (2018-2019) and the first long-term hindcast simulation for reprocessing-derived 236U dispersion in the North-Baltic Sea (1971-2018). Using 233U/236U fingerprints, we distinguish 236U from the nuclear weapon testing and civil nuclear industries, which have comparable contributions (142 ± 13 and 174 ± 40 g) to the 236U inventory in modern Baltic seawater. Budget calculations for 236U inputs since the 1950s indicate that, the major 236U sources in the Baltic Sea are the atmospheric fallouts (∼1.35 kg) and discharges from nuclear reprocessing plants (> 211 g), and there is a continuous sink of 236U to the anoxic sediments (589 ± 43 g). Our findings also indicate that the limited water renewal endows the Baltic Sea a strong "memory effect" retaining aged 236U signals, and the previously unknown 236U in the Baltic Sea is likely attributed to the retention of the mid-1990s' discharges from the nuclear reprocessing plants. Our preliminary results demonstrate the power of 236U-129I dual-tracer in investigating water-mass mixing and estimating water age in the Baltic Sea, and this work provides fundamental knowledge for future 236U tracer studies in the Baltic Sea.

70-Year Anthropogenic Uranium Imprints of Nuclear Activities in Baltic Sea Sediments.

A strongly stratified water structure and a densely populated catchment make the Baltic Sea one of the most polluted seas. Understanding its circulation pattern and time scale is essential to predict the dynamics of hypoxia, eutrophication, and pollutants. Anthropogenic 236U and 233U have been demonstrated as excellent transient tracers in oceanic studies, but unclear input history and inadequate long-term monitoring records limit their application in the Baltic Sea. From two dated Baltic sediment cores, we obtained high-resolution records of anthropogenic uranium imprints originating from three major human nuclear activities throughout the Atomic Era. Using the novel 233U/236U signature, we distinguished and quantified 236U inputs from global fallout (45.4-52.1%), Chernobyl accident (0.3-1.8%), and discharges from civil nuclear industries (46.1-54.3%) to the Baltic Sea. We estimated the total release of 233U (7-15 kg) from the atmospheric nuclear weapon testing and pinpointed the 233U peak signal in the mid-to-late 1950s as a potential time marker for the onset of the Anthropocene Epoch. This work also provides fundamental 236U data on Chernobyl accident and early discharges from civil nuclear facilities, prompting worldwide 233U-236U tracer studies. We anticipate our data to be used in a broader application in model-observation interdisciplinary research on water circulation and pollutant dynamics in the Baltic Sea.

First study on 236U in the Northeast Pacific Ocean using a new target preparation procedure for AMS measurements.

We succeeded in obtaining the depth profile of 236U for a sampling station in the Northeast Pacific Ocean using only one litre of seawater sample from each depth. For this purpose, a new procedure was developed that allowed for the preparation of accelerator mass spectrometry targets for trace uranium using only 100 µg of iron carrier material. The 236U concentrations in water samples from the Northeast Pacific Ocean showed large variations from (9.26 ± 0.42) × 106 atoms/kg at 60 m depth to (0.08 ± 0.02) × 106 atoms/kg at a depth of 3000 m. The high 236U concentrations in surface water reflect the input of 236U by global and local fallout from nuclear weapons tests. The low 236U concentrations in seawater from 1500 m and below are an indicator for the low vertical diffusion of surface water to deeper layers in the North Pacific Ocean. The total inventory of 236U on the water column was (8.35 ± 0.23) × 1012 atoms/m2, which is lower compared to those of other ocean regions solely affected by global fallout on comparable latitudes. This study represents the first dataset for 236U in the Pacific Ocean and shows the possibility of downsizing sample volumes which may help in future applications of 236U as tracer for large ocean areas.

Uranium-236 as a new oceanic tracer: A first depth profile in the Japan Sea and comparison with caesium-137.

We present a feasibility study for using 236U as an oceanic circulation tracer based on depth profiles of 236U and 137Cs in the Japan/East Sea. The concentration of the predominantly anthropogenic 236U, measured with Accelerator Mass Spectrometry (AMS), decreased from (13±3)×106 atom/kg in surface water to (1.6±0.3)×106 atom/kg close to the sea floor (2800 m). The profile has a smooth trend with depth and concentration values are generally proportional to that of 137Cs for the same water samples, but with a slightly lower ratio of 137Cs/236U below 2000 m. The cumulative inventory of dissolved 236U in the water column was estimated to be (13.7±0.9)×1012 atom/m2, which is similar to the global-fallout level (17.8×1012 atom/m2) in Japan. Additional analyses of suspended solids (SS) and bottom sediments yielded negligible amounts of 236U. Our results suggest that 236U behaves as a conservative nuclide in seawater, with potential advantages over other tracers of oceanic circulation.