46 results on '"Steier, Peter"'
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2. Reconstructing the chronology of the natural and anthropogenic uranium isotopic signals in a marine sediment core from Beppu Bay, Japan.
- Author
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Takahashi H, Sakaguchi A, Hain K, Wiederin A, Kuwae M, Steier P, Takaku Y, Yamasaki S, and Sueki K
- Abstract
The long-lived U isotopes,
233 U and236 U, have been used increasingly in recent years as marine circulation tracers and for identifying sources of uranium contamination in the environment. The sedimentation histories of these two U isotopes in combination with natural238 U were reconstructed for an anoxic sediment core collected from Beppu Bay, Japan, in the western North Pacific Ocean showing good time resolution (less than 2.6 y/sample). The233 U/236 U atom ratio showed a prominent peak of (3.20 ± 0.30) × 10-2 around 1957 which can be attributed to the input from atmospheric nuclear weapons tests including thermonuclear tests conducting in the Equatorial Pacific. The integrated233 U/236 U ratio of (1.64 ± 0.08) × 10-2 for the sediment was found to be in relatively good agreement with the representative ratio published for global fallout (∼1.4 × 10-2 ). A prominent increase in the authigenic ratio of233 U/238 Ua,s in the leached fraction (1.39 ± 0.11 × 10-11 ) and the bulk digestion (1.36 ± 0.10 × 10-11 ) was also observed around 1957. This reflects the input supply of233 U to the seawater which is known to have a relatively constant238 U content. The authigenic236 U/238 Ua,s ratio (0.18 ± 0.02 × 10-9 ) obtained for 1921 increased from the early 1950's to a maximum of (6.59 ± 0.60) × 10-9 around 1962. The variation in this ratio represents well the introduction history of U into the surface environment without site-specific U contamination and the time profile is also consistent with the137 Cs signature. This work thus provides a benchmark for the long-term use of the isotopic U composition as an input parameter for seawater circulation tracers and as a chronological marker for anoxic sediments and sedimentary rocks. Especially the233 U/236 U ratio may serve as a key-marker for the new geological age Anthropocene., Competing Interests: The authors declare no conflict of interest., (© 2023 The Author(s).)- Published
- 2023
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3. Tracing Atlantic water transit time in the subarctic and Arctic Atlantic using 99 Tc- 233 U- 236 U.
- Author
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Lin G, Qiao J, Steier P, Danielsen M, Guðnason K, Joensen HP, and Stedmon CA
- Subjects
- Water, Seawater, Arctic Regions, Denmark, Atlantic Ocean, Water Pollutants, Radioactive analysis
- Abstract
The pathway and transport time of Atlantic water passing northern Europe can be traced via anthropogenic radioisotopes released from reprocessing of spent nuclear fuels at Sellafield (SF) and La Hague (LH). These reprocessing derived radioisotopes, with extremely low natural background, are source specific and unique fingerprints for Atlantic water. This study explores a new approach using
99 Tc-233 U-236 U tracer to estimate the transit time of Atlantic water in the coast of Greenland. We isolate the reprocessing plants (RP) signal of236 U (236 URP ) by incorporating233 U measurements and combine this with99 Tc which solely originates from RP, to estimate the transit time of Atlantic water circulating from Sellafield to the coast of Greenland-Iceland-Faroe Islands. Both being conservative radioisotopes, the temporal variation of99 Tc/236 URP ratio in Atlantic water is only influenced by their historic discharges from RP, thus99 Tc/236 URP can potentially be a robust tracer to track the transport of Atlantic water in the North Atlantic-Arctic region. Based on our observation data of99 Tc-233 U-236 U in seawater and the proposed99 Tc/236 URP tracer approach, Atlantic water transit times were estimated to be 16-22, 25 and 25 years in the coast of Greenland, Iceland and Faroe Island, respectively. Our estimates from northeast Greenland coastal waters agree with earlier results (17-22 years). Therefore, this work provides an independent approach to estimate Atlantic water transit time with which to compare estimates from ocean modelling and other radiotracer approaches., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 The Authors. Published by Elsevier B.V. All rights reserved.)- Published
- 2022
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4. Understanding source terms of anthropogenic uranium in the Arctic Ocean - First 236 U and 233 U dataset in Barents Sea sediments.
- Author
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Qiao J, Heldal HE, and Steier P
- Subjects
- Arctic Regions, Atlantic Ocean, Geologic Sediments, Oceans and Seas, Radiation Monitoring, Uranium analysis, Water Pollutants, Radioactive analysis
- Abstract
This work reports the first dataset of
236 U and233 U in sediment cores taken from the Barents Sea, with the aim to better understand the source terms of anthropogenic uranium in the Arctic region. Concentrations of236 U and233 U along with137 Cs, and233 U/236 U atomic ratio were measured in six sediment profiles. The cumulative areal inventories of236 U and233 U obtained in this work are (3.50-12.7) × 1011 atom/m2 and (4.92-21.2) × 109 atom/m2 , with averages values of (8.08 ± 2.93) × 1011 atom/m2 and (1.08 ± 0.56) × 1010 atom/m2 , respectively. The total quantities of236 U and233 U deposited in the Barents Sea bottom sediments were estimated to be 507 ± 184 g and 7 ± 3 g, respectively, which are negligible compared to the total direct deposition of236 U (6000 g) and233 U (40-90 g) from global fallout in the Barents Sea. The integrated atomic ratios of233 U/236 U ranging in (0.98-1.57) × 10-2 reflect the predominant global fallout signal of236 U in the Barents Sea sediments and the highest reactor-236 U contribution accounts for 30 ± 14 % among the six sediment cores. The reactor-236 U input in the Barents Sea sediments is most likely transported from the European reprocessing plants rather than related to any local radioactive contamination. These results provide better understanding on the source term of anthropogenic236 U in the Barents Sea, prompt the oceanic tracer application of236 U for studying the dynamics of the Atlantic-Arctic Ocean and associated climate changes. The236 U-233 U benchmarked age-depth profiles seem to match reasonably well with the reported input function history of radioactive contamination in the Barents Sea, indicating the high potential of anthropogenic236 U-233 U pair as a useful tool for sediment dating., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 The Authors. Published by Elsevier B.V. All rights reserved.)- Published
- 2022
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5. Deciphering sources of U contamination using isotope ratio signatures in the Loire River sediments: Exploring the relevance of 233 U/ 236 U and stable Pb isotope ratios.
- Author
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Morereau A, Jaegler H, Hain K, Steier P, Golser R, Beaumais A, Lepage H, Eyrolle F, Grosbois C, Cazala C, and Gourgiotis A
- Subjects
- Environmental Monitoring, Isotopes analysis, Lead, Geologic Sediments, Uranium
- Abstract
A broad range of contaminants has been recorded in sediments of the Loire River over the last century. Among a variety of anthropogenic activities of this nuclearized watershed, extraction of uranium and associated activities during more than 50 years as well as operation of several nuclear power plants led to industrial discharges, which could persist for decades in sedimentary archives of the Loire River. Highlighting and identifying the origin of radionuclides that transited during the last decades and were recorded in the sediments is challenging due to i) the low concentrations which are often close or below the detection limits of routine environmental surveys and ii) the mixing of different sources. The determination of the sources of anthropogenic radioactivity was performed using multi-isotopic fingerprints (
236 U/238 U,206 Pb/207 Pb and208 Pb/207 Pb) and the newly developed233 U/236 U tracer. For the first time233 U/236 U data in a well-dated river sediment core in the French river Loire are reported here. Results highlight potential sources of contamination among which a clear signature of anthropogenic inputs related to two accidents of a former NUGG NPP that occurred in 1969 and 1980. The233 U and236 U isotopes were measured by recent high performance analytical methods due to their ultra-trace levels in the samples and show a negligible radiological impact on health and on the environment. The determination of mining activities by the use of stable Pb isotopes is still challenging probably owing to the limited dissemination of the Pb-bearing material marked by the U-ore signature downstream to the former U mines., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022. Published by Elsevier Ltd.)- Published
- 2022
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6. Correction: Novel 90 Sr analysis of environmental samples by Ion-Laser InterAction Mass Spectrometry.
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Honda M, Martschini M, Marchhart O, Priller A, Steier P, Golser R, Sato TK, Kazuaki T, and Sakaguchi A
- Abstract
Correction for 'Novel
90 Sr analysis of environmental samples by Ion-Laser InterAction Mass Spectrometry' by Maki Honda et al. , Anal. Methods , 2022, 14 , 2732-2738, https://doi.org/10.1039/D2AY00604A.- Published
- 2022
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7. Novel 90 Sr analysis of environmental samples by Ion-Laser InterAction Mass Spectrometry.
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Honda M, Martschini M, Marchhart O, Priller A, Steier P, Golser R, Sato TK, Kazuaki T, and Sakaguch A
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- Animals, Lasers, Mass Spectrometry methods, Soil, Strontium Radioisotopes analysis
- Abstract
The sensitive analysis of
90 Sr with accelerator mass spectrometry (AMS) was developed to advance environmental radiology. One advantage of AMS is the ability to analyze environmental samples with90 Sr/88 Sr atomic ratios of 10-14 in following a simple chemical separation. Three different IAEA samples with known90 Sr concentrations (moss-soil, animal bone, Syrian soil: 1 g each) were analyzed to assess the validity of the chemical separation and the AMS measurement. The90 Sr measurements were conducted on the AMS system VERA combined with the Ion Laser InterAction Mass Spectrometry (ILIAMS) setup at the University of Vienna, which has excellent isobaric separation performance. The isobaric interference of90 Zr in the90 Sr AMS was first largely removed by chemical separation. The separation factor of Zr in two-step column chromatography with Sr resin and anion exchange resin was 106 . The90 Zr remaining in the sample was effectively suppressed by ILIAMS. This procedure achieved a limit of detection <0.1 mBq in the90 Sr AMS, which is lower than typical β-ray detection. The agreement between AMS measurements and nominal values for the90 Sr concentrations of IAEA samples indicated that the new highly-sensitive90 Sr analysis in the environmental samples with AMS is reliable.- Published
- 2022
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8. Anthropogenic 236 U and 233 U in the Baltic Sea: Distributions, source terms, and budgets.
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Lin M, Qiao J, Hou X, Steier P, Golser R, Schmidt M, Dellwig O, Hansson M, Bäck Ö, Vartti VP, Stedmon C, She J, Murawski J, Aldahan A, and Schmied SAK
- Subjects
- Baltic States, Computer Simulation, Ecosystem, Seawater, Water Pollutants, Radioactive analysis
- Abstract
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 (
236 U and233 U) 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 of236 U and233 U in the Baltic Sea (2018-2019) and the first long-term hindcast simulation for reprocessing-derived236 U dispersion in the North-Baltic Sea (1971-2018). Using233 U/236 U fingerprints, we distinguish236 U from the nuclear weapon testing and civil nuclear industries, which have comparable contributions (142 ± 13 and 174 ± 40 g) to the236 U inventory in modern Baltic seawater. Budget calculations for236 U inputs since the 1950s indicate that, the major236 U 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 of236 U 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 aged236 U signals, and the previously unknown236 U 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 of236 U-129 I dual-tracer in investigating water-mass mixing and estimating water age in the Baltic Sea, and this work provides fundamental knowledge for future236 U tracer studies in the Baltic Sea., (Copyright © 2021 The Authors. Published by Elsevier Ltd.. All rights reserved.)- Published
- 2022
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9. Deciphering anthropogenic uranium sources in the equatorial northwest Pacific margin.
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Qiao J, Ransby D, and Steier P
- Subjects
- Pacific Ocean, Philippines, Plutonium analysis, Radiation Monitoring, Radioactive Fallout analysis, Uranium, Water Pollutants, Radioactive analysis
- Abstract
This work reports the first high-resolution deposition records of anthropogenic uranium (
236 U and233 U) in a sediment core taken at the continental slope of the Philippine Sea off Mindanao Island in the equatorial northwest Pacific Ocean. Two notable peaks were observed in both profiles of236 U and233 U concentrations, with a narrower peak in 1951-1957 corresponding to close-in Pacific Proving Grounds (PPG) signal, and a broader peak in 1960s-1980s corresponding to the global fallout from nuclear weapons testing.236 U and233 U areal cumulative inventories in the studied sediment core are (2.79 ± 0.20) ∙ 1012 atom ∙ m- 2 and (3.12 ± 0.41) ∙ 1010 atom ∙ m- 2 , respectively, about 20-30% of reported233 U and236 U inventories from the direct global fallout deposition. The overall233 U/236 U atomic ratios obtained in this work vary within (0.3-3.5) ∙ 10- 2 , with an integrated233 U/236 U atomic ratio of (1.12 ± 0.17) ∙ 10-2 . The contribution from global fallout and close-in PPG fallout to236 U in the sediment core is estimated to be about 69% and 31%, respectively. We believe the main driving process for anthropogenic uranium deposition in the Philippine sediment is continuous scavenging of dissolved236 U from the surface seawater by sinking particles., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 The Authors. Published by Elsevier B.V. All rights reserved.)- Published
- 2022
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10. Revisiting the Middle and Upper Palaeolithic archaeology of Gruta do Caldeirão (Tomar, Portugal).
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Zilhão J, Angelucci DE, Arnold LJ, d'Errico F, Dayet L, Demuro M, Deschamps M, Fewlass H, Gomes L, Linscott B, Matias H, Pike AWG, Steier P, Talamo S, and Wild EM
- Subjects
- Animals, Fossils, Humans, Portugal, Spain, Archaeology methods, Geologic Sediments analysis, Radiometric Dating methods
- Abstract
Gruta do Caldeirão features a c. 6 m-thick archaeological stratification capped by Holocene layers ABC-D and Ea, which overlie layer Eb, a deposit of Magdalenian age that underwent significant disturbance, intrusion, and component mixing caused by funerary use of the cave during the Early Neolithic. Here, we provide an updated overview of the stratigraphy and archaeological content of the underlying Pleistocene succession, whose chronology we refine using radiocarbon and single-grain optically stimulated luminescence dating. We find a high degree of stratigraphic integrity. Dating anomalies exist in association with the succession's two major discontinuities: between layer Eb and Upper Solutrean layer Fa, and between Early Upper Palaeolithic layer K and Middle Palaeolithic layer L. Mostly, the anomalies consist of older-than-expected radiocarbon ages and can be explained by bioturbation and palimpsest-forming sedimentation hiatuses. Combined with palaeoenvironmental inferences derived from magnetic susceptibility analyses, the dating shows that sedimentation rates varied in tandem with the oscillations in global climate revealed by the Greenland oxygen isotope record. A steep increase in sedimentation rate is observed through the Last Glacial Maximum, resulting in a c. 1.5 m-thick accumulation containing conspicuous remains of occupation by people of the Solutrean technocomplex, whose traditional subdivision is corroborated: the index fossils appear in the expected stratigraphic order; the diagnostics of the Protosolutrean and the Lower Solutrean predate 24,000 years ago; and the constraints on the Upper Solutrean place it after Greenland Interstadial 2.2. (23,220-23,340 years ago). Human usage of the site during the Early Upper and the Middle Palaeolithic is episodic and low-intensity: stone tools are few, and the faunal remains relate to carnivore activity. The Middle Palaeolithic is found to persist beyond 39,000 years ago, at least three millennia longer than in the Franco-Cantabrian region. This conclusion is upheld by Bayesian modelling and stands even if the radiocarbon ages for the Middle Palaeolithic levels are removed from consideration (on account of observed inversions and the method's potential for underestimation when used close to its limit of applicability). A number of localities in Spain and Portugal reveal a similar persistence pattern. The key evidence comes from high-resolution fluviatile contexts spared by the site formation issues that our study of Caldeirão brings to light-palimpsest formation, post-depositional disturbance, and erosion. These processes. are ubiquitous in the cave and rock-shelter sites of Iberia, reflecting the impact on karst archives of the variation in climate and environments that occurred through the Upper Pleistocene, and especially at two key points in time: between 37,000 and 42,000 years ago, and after the Last Glacial Maximum. Such empirical difficulties go a long way towards explaining the controversies surrounding the associated cultural transitions: from the Middle to the Upper Palaeolithic, and from the Solutrean to the Magdalenian. Alongside potential dating error caused by incomplete decontamination, proper consideration of sample association issues is required if we are ever to fully understand what happened with the human settlement of Iberia during these critical intervals, and especially so with regards to the fate of Iberia's last Neandertal populations., Competing Interests: The authors have declared that no competing interests exist.
- Published
- 2021
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11. 70-Year Anthropogenic Uranium Imprints of Nuclear Activities in Baltic Sea Sediments.
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Lin M, Qiao J, Hou X, Dellwig O, Steier P, Hain K, Golser R, and Zhu L
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- Baltic States, Geologic Sediments, Humans, Oceans and Seas, Uranium analysis, Water Pollutants, Radioactive analysis
- Abstract
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
236 U and233 U 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 novel233 U/236 U signature, we distinguished and quantified236 U 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 of233 U (7-15 kg) from the atmospheric nuclear weapon testing and pinpointed the233 U peak signal in the mid-to-late 1950s as a potential time marker for the onset of the Anthropocene Epoch. This work also provides fundamental236 U data on Chernobyl accident and early discharges from civil nuclear facilities, prompting worldwide233 U-236 U 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.- Published
- 2021
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12. On the Quality Control for the Determination of Ultratrace-Level 236 U and 233 U in Environmental Samples by Accelerator Mass Spectrometry.
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Lin M, Qiao J, Hou X, Golser R, Hain K, and Steier P
- Abstract
Our recent attempt to determine ultratrace-level
236 U and233 U in small-volume seawater samples was challenged by high and unstable procedure blanks in our environmental radioactivity laboratory, which used to be a spent fuel research facility. Through intercomparison experiments with different laboratories and background checks on the chemical reagents and laboratory dust, the resuspended U-bearing dust was identified as the dominating source of the236 U and233 U contamination. With the implementation of background control (especially dust control) measures, the procedure blanks and detection limits of236 U and233 U for the radiochemical separation procedure have been significantly improved by three orders of magnitudes. With well-controlled blanks, the analytical precision for236 U and233 U predominantly relies on the AMS counting statistics. Background check and dust control are strongly recommended before the analyses of environmental-level long-lived radionuclides (such as236 U and233 U) that are conducted in the former or active nuclear facilities, even if clearance of radioactivity relevant for radioprotection was achieved.- Published
- 2021
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13. An unknown source of reactor radionuclides in the Baltic Sea revealed by multi-isotope fingerprints.
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Qiao J, Zhang H, Steier P, Hain K, Hou X, Vartti VP, Henderson GM, Eriksson M, Aldahan A, Possnert G, and Golser R
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- Baltic States, Humans, Radioactive Fallout analysis, Sweden, Radioisotopes analysis, Seawater analysis, Uranium analysis, Water Pollutants, Radioactive analysis
- Abstract
We present an application of multi-isotopic fingerprints (i.e.,
236 U/238 U,233 U/236 U,236 U/129 I and129 I/127 I) for the discovery of previously unrecognized sources of anthropogenic radioactivity. Our data indicate a source of reactor236 U in the Baltic Sea in addition to inputs from the two European reprocessing plants and global fallout. This additional reactor236 U may come from unreported discharges from Swedish nuclear research facilities as supported by high236 U levels in sediment nearby Studsvik, or from accidental leakages of spent nuclear fuel disposed on the Baltic seafloor, either reported or unreported. Such leakages would indicate problems with the radiological safety of seafloor disposal, and may be accompanied by releases of other radionuclides. The results demonstrate the high sensitivity of multi-isotopic tracer systems, especially the233 U/236 U signature, to distinguish environmental emissions of unrevealed radioactive releases for nuclear safeguards, emergency preparedness and environmental tracer studies.- Published
- 2021
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14. First dataset of 236 U and 233 U around the Greenland coast: A 5-year snapshot (2012-2016).
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Qiao J, Hain K, and Steier P
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- Arctic Regions, Greenland, Seawater, Radiation Monitoring, Uranium analysis, Water Pollutants, Radioactive analysis
- Abstract
We report the first combined dataset of
236 U and233 U in the Greenland marine environment during the period of 2012-2016. Results are discussed in terms of time evolution and spatial distribution of236 U concentration, and atomic ratios of236 U/238 U and233 U/236 U.236 U concentrations along the Greenland coast are distributed within a relatively narrow range of (0.7-12.9) × 107 atom/L, corresponding to236 U/238 U atomic ratios of (1.1-15.5) × 10-9 . The233 U/236 U atomic ratios obtained vary from 0.12 × 10-2 to 1.16 × 10-2 , with the majority distributed in the range of (0.2-0.7) × 10-2 . We applied233 U/236 U and236 U/238 U atomic ratios in a binary mixing model to identify possible236 U source terms. The results indicate that anthropogenic236 U and233 U in Greenland surface seawater originated from the direct global fallout (DGF) and the Sellafield and La Hague reprocessing plants (RP) is diluted by a third endmember, mostly likely natural ocean water (NOW), containing marginal236 U and233 U. A preliminary estimation of the source terms of236 U using233 U/236 U atomic ratios indicate that, for both eastern and western Greenland seawater, contributions from global fallout (GF) constitute about 30% of236 U. The dominating source for236 U, i.e. 70 %, is associated to reactor236 U including discharges from RP and local reactor input in the Arctic Ocean., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)- Published
- 2020
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15. Radiocarbon analysis of carbonaceous aerosols in Bratislava, Slovakia.
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Kontuľ I, Kaizer J, Ješkovský M, Steier P, and Povinec PP
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- Aerosols, Biomass, Carbon, Environmental Monitoring, Fossil Fuels, Particulate Matter, Seasons, Slovakia, Air Pollutants, Radioactive analysis, Radiation Monitoring
- Abstract
Aerosols dispersed in the atmosphere represent important factors influencing not only the environment, but also human health. Carbonaceous aerosols are one of the main components of total atmospheric aerosols, and their sources are of great interest. Radiocarbon analysis provides an excellent way to determine the fraction of fossil and non-fossil aerosols in the atmosphere. Over the period of one year (June 2017-June 2018), we sampled atmospheric aerosols with size greater than 0.3 μm in Bratislava, Slovakia and used the exposed quartz filters for radiocarbon analysis of the elemental carbon (EC) aerosol fraction. The results show that on average the fossil fuel combustion is the dominant source of EC aerosol particles in Bratislava. In summer months, they represent more than half (65-80%) of the total EC aerosols. The relative amount of EC particles derived from biomass burning was 20-35% in summer, which increased to 40-55% in winter months. The dominance of fossil fraction is caused by high degree of industrialization and urbanization of the city. The increase of biomass fraction in winter is probably caused by domestic wood burning in areas surrounding the Bratislava city., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)
- Published
- 2020
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16. Pushing Limits of ICP-MS/MS for the Determination of Ultralow 236 U/ 238 U Isotope Ratios.
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Jaegler H, Gourgiotis A, Steier P, Golser R, Diez O, and Cazala C
- Abstract
Determination of uranium isotope ratios is of great expedience for assessing its origin in environmental samples. In particular, the
236 U/238 U isotope ratio provides a powerful tool to discriminate between the different sources of uranium (uranium ore, geochemical background, and uranium from anthropogenic activities). However, in the environment, this ratio is typically below 10-8 . This low abundance of236 U and the presence in large excess of major isotopes (mainly238 U and235 U) complicates the accurate detection of236 U signal by mass spectrometry and thus highly sensitive analytical instruments providing high abundance sensitivity are required. This work pushes the limits of triple quadrupole-based ICP-MS technology for accurate detection of236 U/238 U isotope ratios down to 10-10 , which is so far mainly achievable by AMS. Coupled with an efficient desolvating module, N2 O was used as the reaction gas in the collision reaction cell of the ICP-MS/MS. This configuration allows a significant decrease of the uranium polyatomic interferences (235 UH+ ions) and an accurate determination of low236 U/238 U isotope ratios. This new methodology was successfully validated through measurements of certified reference material from 10-7 to 10-9 and then through comparisons with AMS measurement results for ratios down to 10-10 . This is the first time that236 U/238 U isotope ratios as low as 10-10 were determined by ICP-MS/MS. The possibility of measuring low236 U/238 U isotope ratios can offer a large variety of geochemical applications in particular for the determination of uranium sources in the environment.- Published
- 2020
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17. Radionuclides in surface waters around the damaged Fukushima Daiichi NPP one month after the accident: Evidence of significant tritium release into the environment.
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Querfeld R, Pasi AE, Shozugawa K, Vockenhuber C, Synal HA, Steier P, and Steinhauser G
- Abstract
Following the Fukushima nuclear accident (2011), radionuclides mostly of volatile elements (e.g.,
131 I,134,137 Cs,132 Te) have been investigated frequently for their presence in the atmosphere, pedosphere, biosphere, and the Pacific Ocean. Smaller releases of radionuclides with intermediate volatility, (e.g.,90 Sr), have been reported for soil. However, few reports have been published which targeted the contamination of surface (fresh) waters in Japan soon after the accident. In the present study, 10 surface water samples (collected on April 10, 2011) have been screened for their radionuclide content (3 H,90 Sr,129 I,134 Cs, and137 Cs), revealing partly unusually high contamination levels. Especially high tritium levels (184 ± 2 Bq·L-1 ; the highest levels ever reported in scientific literature after Fukushima) were found in a puddle water sample from close to the Fukushima Daiichi nuclear power plant. The ratios between paddy/puddle water from one location only a few meters apart vary around 1% for134 Cs, 12% for129 I (131 I), and around 40% for both3 H and90 Sr. This illustrates the adsorption of radiocesium on natural minerals and radioiodine on organic substances (in the rice paddy), whereas the concentration differences of3 H and90 Sr between the two waters are mainly dilution driven., (Copyright © 2019 Elsevier B.V. All rights reserved.)- Published
- 2019
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18. Radiocarbon re-dating of contact-era Iroquoian history in northeastern North America.
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Manning SW, Birch J, Conger MA, Dee MW, Griggs C, Hadden CS, Hogg AG, Ramsey CB, Sanft S, Steier P, and Wild EM
- Abstract
A time frame for late Iroquoian prehistory is firmly established on the basis of the presence/absence of European trade goods and other archeological indicators. However, independent dating evidence is lacking. We use 86 radiocarbon measurements to test and (re)define existing chronological understanding. Warminster, often associated with Cahiagué visited by S. de Champlain in 1615-1616 CE, yields a compatible radiocarbon-based age. However, a well-known late prehistoric site sequence in southern Ontario, Draper-Spang-Mantle, usually dated ~1450-1550, yields much later radiocarbon-based dates of ~1530-1615. The revised time frame dramatically rewrites 16th-century contact-era history in this region. Key processes of violent conflict, community coalescence, and the introduction of European goods all happened much later and more rapidly than previously assumed. Our results suggest the need to reconsider current understandings of contact-era dynamics across northeastern North America.
- Published
- 2018
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19. Limits on Supernova-Associated ^{60}Fe/^{26}Al Nucleosynthesis Ratios from Accelerator Mass Spectrometry Measurements of Deep-Sea Sediments.
- Author
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Feige J, Wallner A, Altmeyer R, Fifield LK, Golser R, Merchel S, Rugel G, Steier P, Tims SG, and Winkler SR
- Abstract
We searched for the presence of ^{26}Al in deep-sea sediments as a signature of supernova influx. Our data show an exponential dependence of ^{26}Al with the sample age that is fully compatible with radioactive decay of terrigenic ^{26}Al. The same set of samples demonstrated a clear supernova ^{60}Fe signal between 1.7 and 3.2 Myr ago. Combining our ^{26}Al data with the recently reported ^{60}Fe data results in a lower limit of 0.18_{-0.08}^{+0.15} for the local interstellar ^{60}Fe/^{26}Al isotope ratio. It compares to most of the ratios deduced from nucleosynthesis models and is within the range of the observed average galactic ^{60}Fe/^{26}Al flux ratio of (0.15±0.05).
- Published
- 2018
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20. The increase of soil organic carbon as proposed by the "4/1000 initiative" is strongly limited by the status of soil development - A case study along a substrate age gradient in Central Europe.
- Author
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Schiefer J, Lair GJ, Lüthgens C, Wild EM, Steier P, and Blum WEH
- Abstract
During COP 21 in Paris 2015, several states and organizations agreed on the "4/1000" initiative for food security and climate. This initiative aims to increase world's soil organic carbon (SOC) stocks by 4‰ annually. The influence of soil development status on SOC dynamics is very important but usually not considered in studies. We analyse SOC accumulation under forest, grassland and cropping systems along a soil age gradient (10-17,000years) to show the influence of soil development status on SOC increase. SOC stocks (0-40cm) and accumulation rates along a chronosequence in alluvial soils of the Danube River in the Marchfeld (eastern Austria) were analysed. The analysed Fluvisols and Chernozems have been used as forest, grassland and cropland for decades or hundreds of years. The results showed that there is a fast build-up of OC stocks (0-40cm) in young soils with accumulation of ~1.3tha
-1 a-1 OC in the first 100years and ~0.5tha-1 a-1 OC between 100 and 350years almost independent of land use. Chernozems with a sediment deposition age older than 5.000years have an accumulation rate<0.01tOCha-1 a-1 (0-40cm). Radiocarbon dating showed that the topsoil (0-10cm) consists mainly of ">modern" and "modern" carbon indicating a fast carbon cycling. Carbon in subsoil is less exposed to decomposition and OC can be stored at long-time scales in the subsoil (14 C age of 3670±35 BP). In view of the '4/1000' initiative, soils with constant carbon input (forest & grassland) fulfil the intended 4‰ growth rate of SOC stocks only in the first 60years of soil development. We proclaim that under the present climate in Central Europe, the increase of SOC stocks in soil is strongly affected by the state of soil development., (Copyright © 2018 Elsevier B.V. All rights reserved.)- Published
- 2018
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21. Precise dating of the Middle-to-Upper Paleolithic transition in Murcia (Spain) supports late Neandertal persistence in Iberia.
- Author
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Zilhão J, Anesin D, Aubry T, Badal E, Cabanes D, Kehl M, Klasen N, Lucena A, Martín-Lerma I, Martínez S, Matias H, Susini D, Steier P, Wild EM, Angelucci DE, Villaverde V, and Zapata J
- Abstract
The late persistence in Southern Iberia of a Neandertal-associated Middle Paleolithic is supported by the archeological stratigraphy and the radiocarbon and luminescence dating of three newly excavated localities in the Mula basin of Murcia (Spain). At Cueva Antón, Mousterian layer I-k can be no more than 37,100 years-old. At La Boja, the basal Aurignacian can be no less than 36,500 years-old. The regional Middle-to-Upper Paleolithic transition process is thereby bounded to the first half of the 37th millennium Before Present, in agreement with evidence from Andalusia, Gibraltar and Portugal. This chronology represents a lag of minimally 3000 years with the rest of Europe, where that transition and the associated process of Neandertal/modern human admixture took place between 40,000 and 42,000 years ago. The lag implies the presence of an effective barrier to migration and diffusion across the Ebro river depression, which, based on available paleoenvironmental indicators, would at that time have represented a major biogeographical divide. In addition, (a) the Phlegraean Fields caldera explosion, which occurred 39,850 years ago, would have stalled the Neandertal/modern human admixture front because of the population sink it generated in Central and Eastern Europe, and (b) the long period of ameliorated climate that came soon after (Greenland Interstadial 8, during which forests underwent a marked expansion in Iberian regions south of 40°N) would have enhanced the "Ebro Frontier" effect. These findings have two broader paleoanthropological implications: firstly, that, below the Ebro, the archeological record made prior to 37,000 years ago must be attributed, in all its aspects and components, to the Neandertals (or their ancestors); secondly, that modern human emergence is best seen as an uneven, punctuated process during which long-lasting barriers to gene flow and cultural diffusion could have existed across rather short distances, with attendant consequences for ancient genetics and models of human population history.
- Published
- 2017
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22. 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).
- Author
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Quinto F, Blechschmidt I, Garcia Perez C, Geckeis H, Geyer F, Golser R, Huber F, Lagos M, Lanyon B, Plaschke M, Steier P, and Schäfer T
- Abstract
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
233 U,237 Np,242 Pu, and243 Am 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 for237 Np,242 Pu, and243 Am 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 representing241 Am and244 Pu employed in a previous tracer test demonstrated the analytical capability of AMS for in situ studies lasting more than a decade.- Published
- 2017
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23. Anthropogenic 236 U in Danish Seawater: Global Fallout versus Reprocessing Discharge.
- Author
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Qiao J, Steier P, Nielsen S, Hou X, Roos P, and Golser R
- Subjects
- Atlantic Ocean, Baltic States, Denmark, Iodine Radioisotopes, North Sea, Oceans and Seas, Water Pollutants, Radioactive, Seawater, Uranium analysis
- Abstract
This work focuses on the occurrence of
236 U in seawater along Danish coasts, which is the sole water-exchange region between the North Sea-Atlantic Ocean and the Baltic Sea. Seawater collected in 2013 and 2014 were analyzed for236 U (as well as238 U and137 Cs). Our results indicate that236 U concentrations in Danish seawater are distributed within a relatively narrow range of (3.6-8.2) × 107 atom/L and, to a certain extent, independent of salinity.236 U/238 U atomic ratios in Danish seawater are more than 4 times higher than the estimated global fallout value of 1× 10-9 . The levels of236 U/238 U atomic ratios obtained are comparable to those reported for the open North Sea and much higher than several other open oceans worldwide. This indicates that besides the global fallout input, the discharges from the two major European nuclear reprocessing plants are dominating sources of236 U in Danish seawater. However, unexpectedly high236 U/238 U ratios as well as high236 U concentrations were observed at low-salinity locations of the Baltic Sea. While this feature might be interpreted as a clue for another significant236 U input in the Baltic Sea, it may also be caused by the complexity of water currents or slow turnover rate.- Published
- 2017
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24. Plutonium Isotopes ( 239-241 Pu) Dissolved in Pacific Ocean Waters Detected by Accelerator Mass Spectrometry: No Effects of the Fukushima Accident Observed.
- Author
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Hain K, Faestermann T, Fimiani L, Golser R, Gómez-Guzmán JM, Korschinek G, Kortmann F, Lierse von Gostomski C, Ludwig P, Steier P, Tazoe H, and Yamada M
- Subjects
- Isotopes, Mass Spectrometry, Pacific Ocean, Radiation Monitoring, Radioactive Fallout, Water Pollutants, Radioactive, Fukushima Nuclear Accident, Plutonium
- Abstract
The concentration of plutonium (Pu) and the isotopic ratios of
240 Pu to239 Pu and241 Pu to239 Pu were determined by accelerator mass spectrometry (AMS) in Pacific Ocean water samples (20 L each) collected in late 2012. The isotopic Pu ratios are important indicators of different contamination sources and were used to identify a possible release of Pu into the ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. In particular,241 Pu is a well-suited indicator for a recent entry of Pu because241 Pu from fallout of nuclear weapon testings has already significantly decayed. A total of 10 ocean water samples were prepared at the Radiochemie München of the TUM and analyzed at the Vienna Environmental Research Laboratory (VERA). Several samples showed a slightly elevated240 Pu/239 Pu ratio of up to 0.22 ± 0.02 compared to global fallout (240 Pu/239 Pu = 0.180 ± 0.007), whereas all measured241 Pu-to-239 Pu ratios were consistent with nuclear weapon fallout (241 Pu/239 Pu < 2.4 × 10-3 ), which means that no impact from the Fukushima accident was detected. From the average241 Pu-to-239 Pu ratio of 8-2 +3 ×10-4 at a sampling station located at a distance of 39.6 km to FDNPP, the 1-σ upper limit for the FDNPP contribution to the239 Pu inventory in the water column was estimated to be 0.2%. Pu, with the signature of weapon-grade Pu was found in a single sample collected around 770 km off the west coast of the United States.- Published
- 2017
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25. Sphagnum-dominated bog systems are highly effective yet variable sources of bio-available iron to marine waters.
- Author
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Krachler R, Krachler RF, Wallner G, Steier P, El Abiead Y, Wiesinger H, Jirsa F, and Keppler BK
- Subjects
- Chlorella, Ecosystem, Haptophyta, Phytoplankton, Scotland, Seawater chemistry, Environmental Monitoring, Iron metabolism, Sphagnopsida physiology, Wetlands
- Abstract
Iron is a micronutrient of particular interest as low levels of iron limit primary production of phytoplankton and carbon fluxes in extended regions of the world's oceans. Sphagnum-peatland runoff is extraordinarily rich in dissolved humic-bound iron. Given that several of the world's largest wetlands are Sphagnum-dominated peatlands, this ecosystem type may serve as one of the major sources of iron to the ocean. Here, we studied five near-coastal creeks in North Scotland using freshwater/seawater mixing experiments of natural creek water and synthetic seawater based on a (59)Fe radiotracer technique combined with isotopic characterization of dissolved organic carbon by Accelerator Mass Spectrometry. Three of the creeks meander through healthy Sphagnum-dominated peat bogs and the two others through modified peatlands which have been subject to artificial drainage for centuries. The results revealed that, at the time of sampling (August 16-24, 2014), the creeks that run through modified peatlands delivered 11-15μg iron per liter creek water to seawater, whereas the creeks that run through intact peatlands delivered 350-470μg iron per liter creek water to seawater. To find out whether this humic-bound iron is bio-available to marine algae, we performed algal growth tests using the unicellular flagellated marine prymnesiophyte Diacronema lutheri and the unicellular marine green alga Chlorella salina, respectively. In both cases, the riverine humic material provided a highly bio-available source of iron to the marine algae. These results add a new item to the list of ecosystem services of Sphagnum-peatlands., (Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.)
- Published
- 2016
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26. Uranium from German Nuclear Power Projects of the 1940s--A Nuclear Forensic Investigation.
- Author
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Mayer K, Wallenius M, Lützenkirchen K, Horta J, Nicholl A, Rasmussen G, van Belle P, Varga Z, Buda R, Erdmann N, Kratz JV, Trautmann N, Fifield LK, Tims SG, Fröhlich MB, and Steier P
- Abstract
Here we present a nuclear forensic study of uranium from German nuclear projects which used different geometries of metallic uranium fuel. Through measurement of the (230)Th/(234)U ratio, we could determine that the material had been produced in the period from 1940 to 1943. To determine the geographical origin of the uranium, the rare-earth-element content and the (87)Sr/(86)Sr ratio were measured. The results provide evidence that the uranium was mined in the Czech Republic. Trace amounts of (236)U and (239)Pu were detected at the level of their natural abundance, which indicates that the uranium fuel was not exposed to any major neutron fluence., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)
- Published
- 2015
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27. Method for (236)U Determination in Seawater Using Flow Injection Extraction Chromatography and Accelerator Mass Spectrometry.
- Author
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Qiao J, Hou X, Steier P, Nielsen S, and Golser R
- Abstract
An automated analytical method implemented in a flow injection (FI) system was developed for rapid determination of (236)U in 10 L seawater samples. (238)U was used as a chemical yield tracer for the whole procedure, in which extraction chromatography (UTEVA) was exploited to purify uranium, after an effective iron hydroxide coprecipitation. Accelerator mass spectrometry (AMS) was applied for quantifying the (236)U/(238)U ratio, and inductively coupled plasma mass spectrometry (ICPMS) was used to determine the absolute concentration of (238)U; thus, the concentration of (236)U can be calculated. The key experimental parameters affecting the analytical effectiveness were investigated and optimized in order to achieve high chemical yields and simple and rapid analysis as well as low procedure background. Besides, the operational conditions for the target preparation prior to the AMS measurement were optimized, on the basis of studying the coprecipitation behavior of uranium with iron hydroxide. The analytical results indicate that the developed method is simple and robust, providing satisfactory chemical yields (80-100%) and high analysis speed (4 h/sample), which could be an appealing alternative to conventional manual methods for (236)U determination in its tracer application.
- Published
- 2015
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28. 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.
- Author
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Quinto F, Golser R, Lagos M, Plaschke M, Schäfer T, Steier P, and Geckeis H
- Abstract
(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.
- Published
- 2015
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29. Airborne Plutonium and non-natural Uranium from the Fukushima DNPP found at 120 km distance a few days after reactor hydrogen explosions.
- Author
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Shinonaga T, Steier P, Lagos M, and Ohkura T
- Subjects
- Adult, Aerosols analysis, Cesium Radioisotopes analysis, Humans, Japan, Radiation Monitoring, Radiometry, Wind, Air Pollutants, Radioactive analysis, Explosions, Fukushima Nuclear Accident, Hydrogen analysis, Nuclear Power Plants, Plutonium analysis, Uranium analysis
- Abstract
Plutonium (Pu) and non-natural uranium (U) originating from the Fukushima Daiichi Nuclear Power Plant (FDNPP) were identified in the atmosphere at 120 km distance from the FDNPP analyzing the ratio of number of atoms, following written as n(isotope)/n(isotope), of Pu and U. The n((240)Pu)/n((239)Pu), n((241)Pu)/n((239)Pu), n((234)U)/n((238)U), n((235)U)/n((238)U) and n((236)U)/n((238)U) in aerosol samples collected before and after the FDNPP incident were analyzed by accelerator mass spectrometry (AMS) and inductively coupled plasma mass spectrometry (ICPMS). The activity concentrations of (137)Cs and (134)Cs in the same samples were also analyzed by gamma spectrometry before the destructive analysis. Comparing the time series of analytical data on Pu and U obtained in this study with previously reported data on Pu, U, and radioactive Cs, we concluded that Pu and non-natural U from the FDNPP were transported in the atmosphere directly over a 120 km distance by aerosol and wind within a few days after the reactor hydrogen explosions. Effective dose of Pu were calculated using the data of Pu: (130 ± 21) nBq/m(3), obtained in this study. We found that the airborne Pu contributes only negligibly to the total dose at the time of the incident. However the analytical results show that the amount of Pu and non-natural U certainly increased in the environment after the incident.
- Published
- 2014
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30. Isotopic compositions of (236)U and Pu isotopes in "black substances" collected from roadsides in Fukushima prefecture: fallout from the Fukushima Dai-ichi nuclear power plant accident.
- Author
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Sakaguchi A, Steier P, Takahashi Y, and Yamamoto M
- Subjects
- Cesium Radioisotopes analysis, Chemical Fractionation, Geography, Japan, Nuclear Power Plants, Soil chemistry, Volatilization, Air Pollutants, Radioactive analysis, Dust analysis, Fukushima Nuclear Accident, Plutonium analysis, Radiation Monitoring methods, Radioactive Fallout analysis, Uranium analysis
- Abstract
Black-colored road dusts were collected in high-radiation areas in Fukushima Prefecture. Measurement of (236)U and Pu isotopes and (134,137)Cs in samples was performed to confirm whether refractory elements, such as U and Pu, from the fuel core were discharged and to ascertain the extent of fractionation between volatile and refractory elements. The concentrations of (134,137)Cs in all samples were exceptionally high, ranging from 0.43 to 17.7 MBq/kg, respectively. (239+240)Pu was detected at low levels, ranging from 0.15 to 1.14 Bq/kg, and with high (238)Pu/(239+240)Pu activity ratios of 1.64-2.64. (236)U was successfully determined in the range of (0.28 to 6.74) × 10(-4) Bq/kg. The observed activity ratios for (236)U/(239+240)Pu were in reasonable agreement with those calculated for the fuel core inventories, indicating that trace amounts of U from the fuel cores were released together with Pu isotopes but without large fractionation. The quantities of U and (239+240)Pu emitted to the atmosphere were estimated as 3.9 × 10(6) Bq (150 g) and 2.3 × 10(9) Bq (580 mg), respectively. With regard to U, this is the first report to give a quantitative estimation of the amount discharged. Appreciable fractionation between volatile and refractory radionuclides associated with the dispersal/deposition processes with distance from the Fukushima Dai-ichi Nuclear Power Plant was found.
- Published
- 2014
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31. A review on 129I analysis in air.
- Author
-
Jabbar T, Wallner G, and Steier P
- Subjects
- Air Pollutants, Radioactive analysis, Environmental Monitoring, Iodine Radioisotopes analysis
- Abstract
A review of literature focused on (129)I determination in air is provided. (129)I analysis in the environment represents a vital tool for tracing transport mechanisms, distribution pathways, safety assessment and its application as environmental tracer. To achieve that, specific chemical extraction methods and high sensitivity analytical techniques have been developed. This paper is intended to give an overview about the sample collection, extraction and distribution of (129)I in the air. Sensitivity of available measurement techniques for the determination of (129)I is compared. The article also provides the summary of current worldwide distribution of (129)I in air and respective radiation exposure of man., (Copyright © 2013 Elsevier Ltd. All rights reserved.)
- Published
- 2013
- Full Text
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32. Sequential injection method for rapid and simultaneous determination of 236U, 237Np, and Pu isotopes in seawater.
- Author
-
Qiao J, Hou X, Steier P, and Golser R
- Abstract
An automated analytical method implemented in a novel dual-column tandem sequential injection (SI) system was developed for simultaneous determination of (236)U, (237)Np, (239)Pu, and (240)Pu in seawater samples. A combination of TEVA and UTEVA extraction chromatography was exploited to separate and purify target analytes, whereupon plutonium and neptunium were simultaneously isolated and purified on TEVA, while uranium was collected on UTEVA. The separation behavior of U, Np, and Pu on TEVA-UTEVA columns was investigated in detail in order to achieve high chemical yields and complete purification for the radionuclides of interest. (242)Pu was used as a chemical yield tracer for both plutonium and neptunium. (238)U was quantified in the sample before the separation for deducing the (236)U concentration from the measured (236)U/(238)U atomic ratio in the separated uranium target using accelerator mass spectrometry. Plutonium isotopes and (237)Np were measured using inductively coupled plasma mass spectrometry after separation. The analytical results indicate that the developed method is robust and efficient, providing satisfactory chemical yields (70-100%) of target analytes and relatively short analytical time (8 h/sample).
- Published
- 2013
- Full Text
- View/download PDF
33. Investigation of the isotopic ratio 129I/I in petrified wood.
- Author
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Jabbar T, Steier P, Wallner G, Cichocki O, and Sterba JH
- Subjects
- Austria, Uranium analysis, Fossils, Iodine analysis, Iodine Radioisotopes analysis, Wood chemistry
- Abstract
In fossil specimens, measurements of the natural isotopic ratio (129)I/I may provide a method to estimate the age of sample. The motivation for measuring the isotopic composition ((129)I/I) of petrified wood samples collected from Austria was to check this feasibility. Alkaline fusion together with anion exchange was used to extract iodine from the sample. Typical sample size for this study was 10-90 g. An atomic ratio as low as 10(-14) was determined using accelerator mass spectrometry (AMS). Uranium concentrations measured by instrumental neutron activation analysis (INAA) and α-spectrometry were found to be less than 3 mg kg(-1), therefore the contribution from fissiogenic (129)I was small and an estimation of ages was based on the decrease of the initial ratio (due to decay of the cosmogenic (129)I in a closed system) after subtraction of the fissiogenic (129)I. The value of the prenuclear ratio is crucial for the use of the (129)I system for dating purposes in the terrestrial environment. From the preanthropogenic (initial) ratio of 1.5 × 10(-12) of the hydrosphere and the results of the present study for the samples from Altenburg (1.05 × 10(-12)) and Fuerwald (6.16 × 10(-13)), respective ages of 8 ± 2.2 and 20.2 ± 2.2 million years were derived. Since samples were collected from a stratum deposited in the Upper Oligocene/Ergerien period (~25-30 million years ago), it can be concluded that these isotopic ratios do not show ages but an elapsed time since fossil wood was isolated from mineral rich water. Paleontological investigation shows that samples from Altenburg had mixed characteristics of old and modern Tertiary plants, thus an origin from a younger stratum re-sedimented with Oligocene cannot be excluded. However, the sample from Drasenhofen reflects that the (129)I/I system might not always be suitable for the dating of petrified wood sample due to fixation of anthropogenic (129)I into surface fractures., (Copyright © 2013 Elsevier Ltd. All rights reserved.)
- Published
- 2013
- Full Text
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34. Measurements of ²³⁶U in ancient and modern peat samples and implications for postdepositional migration of fallout radionuclides.
- Author
-
Quinto F, Hrnecek E, Krachler M, Shotyk W, Steier P, and Winkler SR
- Subjects
- Radioactive Pollutants analysis, Soil, Uranium analysis
- Abstract
(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.
- Published
- 2013
- Full Text
- View/download PDF
35. Iodine-129 in seawater offshore Fukushima: distribution, inorganic speciation, sources, and budget.
- Author
-
Hou X, Povinec PP, Zhang L, Shi K, Biddulph D, Chang CC, Fan Y, Golser R, Hou Y, Ješkovský M, Jull AJ, Liu Q, Luo M, Steier P, and Zhou W
- Subjects
- Fukushima Nuclear Accident, Iodine Radioisotopes, Japan, Nuclear Power Plants, Iodine analysis, Radiation Monitoring, Seawater chemistry
- Abstract
The Fukushima nuclear accident in March 2011 has released a large amount of radioactive pollutants to the environment. Of the pollutants, iodine-129 is a long-lived radionuclide and will remain in the environment for millions of years. This work first report levels and inorganic speciation of (129)I in seawater depth profiles collected offshore Fukushima in June 2011. Significantly elevated (129)I concentrations in surface water were observed with the highest (129)I/(127)I atomic ratio of 2.2 × 10(-9) in the surface seawater 40 km offshore Fukushima. Iodide was found as the dominant species of (129)I, while stable (127)I was mainly in iodate form, reflecting the fact that the major source of (129)I is the direct liquid discharges from the Fukushima NPP. The amount of (129)I directly discharged from the Fukushima Dai-ichi nuclear power plant to the sea was estimated to be 2.35 GBq, and about 1.09 GBq of (129)I released to the atmosphere from the accident was deposited in the sea offshore Fukushima. A total release of 8.06 GBq (or 1.2 kg) of (129)I from the Fukushima accident was estimated. These Fukushima-derived (129)I data provide necessary information for the investigation of water circulation and geochemical cycle of iodine in the northwestern Pacific Ocean in the future.
- Published
- 2013
- Full Text
- View/download PDF
36. Determination of (239)Pu, (240)Pu, (241)Pu and (242)Pu at femtogram and attogram levels - evidence for the migration of fallout plutonium in an ombrotrophic peat bog profile.
- Author
-
Quinto F, Hrnecek E, Krachler M, Shotyk W, Steier P, and Winkler SR
- Subjects
- Americium analysis, Cesium Radioisotopes analysis, Germany, Mass Spectrometry methods, Plutonium analysis, Radiation Monitoring methods, Radioactive Fallout analysis, Soil analysis, Soil Pollutants, Radioactive analysis, Wetlands
- Abstract
The isotopic composition of plutonium ((239)Pu, (240)Pu, (241)Pu and (242)Pu) was investigated in a ∼0.5 m long peat core from an ombrotrophic bog (Black Forest, Germany) using clean room procedures and accelerator mass spectrometry (AMS). This sophisticated analytical approach was ultimately needed to detect reliably the Pu concentrations present in the peat samples at femtogram (fg) and attogram (ag) levels. The mean (240)Pu/(239)Pu isotopic ratio of 0.19 ± 0.02 (N = 32) in the peat layers, representing approximately the last 80 years, was in good agreement with the accepted value of 0.18 for the global fallout in the Northern Hemisphere. This finding is largely supported by the corresponding and rather constant (241)Pu/(239)Pu (0.0012 ± 0.0005) and (242)Pu/(239)Pu (0.004 ± 0.001) ratios. Since the Pu isotopic composition characteristic of the global fallout was also identified in peat samples pre-dating the period of atmospheric atom bomb testing (AD 1956-AD 1980), migration of Pu within the peat profile is clearly indicated. These results highlight, for the first time, the mobility of Pu in a peat bog with implications for the migration of Pu in other acidic, organic rich environments such as forest soils and other wetland types. These findings constitute a direct observation of the behaviour of Pu at fg and ag levels in the environment. The AMS measurements of Pu concentrations (referring to a corresponding activity of (240+239)Pu from 0.07 mBq g(-1) to 5 mBq g(-1)) essentially confirm our a priori estimates based on existing (241)Am and (137)Cs data in the investigated peat core and agree well with the global fallout levels from the literature. Exclusively employing the Pu isotope ratios established for the peat samples, the date of the Pu irradiation (AD 1956, correctable to AD 1964) was calculated and subsequently compared to the (210)Pb age of the peat layers; this comparison provided an additional hint that global fallout derived Pu is not fixed in the peat column, but has migrated downwards along the peat profile to layers preceding the nuclear age.
- Published
- 2013
- Full Text
- View/download PDF
37. Bomb fall-out 236 U as a global oceanic tracer using an annually resolved coral core.
- Author
-
Winkler SR, Steier P, and Carilli J
- Abstract
Anthropogenic
236 U ( t½ =23.4 My) is an emerging isotopic ocean tracer with interesting oceanographic properties, but only with recent advances in accelerator mass spectrometry techniques is it now possible to detect the levels from global fall-out of nuclear weapons testing across the water column. To make full use of this tracer, an assessment of its input into the ocean over the past decades is required. We captured the bomb-pulse of236 U in an annually resolved coral core record from the Caribbean Sea. We thereby establish a concept which gives236 U great advantage - the presence of reliable, well-resolved chronological archives. This allows studies of not only the present distribution pattern, but gives access to the temporal evolution of236 U in ocean waters over the past decades.- Published
- 2012
- Full Text
- View/download PDF
38. Retrospective measurements of airborne 129iodine in Austria.
- Author
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Jabbar T, Wallner G, Steier P, Katzlberger C, and Kandler N
- Subjects
- Air Pollutants, Radioactive toxicity, Austria epidemiology, Humans, Iodine toxicity, Iodine Radioisotopes analysis, Iodine Radioisotopes toxicity, Mass Spectrometry, Radiation Dosage, Radiation Monitoring, Retrospective Studies, Risk Factors, Seasons, Thyroid Neoplasms epidemiology, Air Pollutants, Radioactive analysis, Environmental Exposure, Iodine analysis, Thyroid Neoplasms chemically induced
- Abstract
The knowledge about the distribution of anthropogenic (129)I is crucial for a successful establishment of transport mechanisms, fate and behaviour in the environment. In present study, the historical record of dry deposition of (129)I in Austria over four decades back to the 1960s is reconstructed. The (129)I/(127)I isotopic ratio of the order of 10(-9)-10(-7) in airborne particles revealed a prominent anthropogenic (129)I signature. The time profile of airborne (129)I follows directly the pattern of the gaseous emissions from European reprocessing plants. Furthermore, temporal variations of (129)I were traced monthly over two years. The potential risks of internal exposure to (129)I are associated with both inhalation and ingestion. Since dose via inhalation was found insignificant, the thyroid equivalent dose from the internal exposure of (129)I using a value of 10(-8) for the isotopic ratio (129)I/(127)I in the thyroid and ICRP reference man was calculated. The corresponding thyroid cancer risk factor of 10(-11) for an adult from life-time exposure is one order of magnitude higher than for a 1-year old child. Due to low radiation toxicity of (129)I the annual dose is 8 × 10(4) times lower than the dose limit of the National Research Council, USA which is 0.04 mSv y(-1) to whole body or any organ for a combined beta and photon emitting radionuclide., (Copyright © 2012 Elsevier Ltd. All rights reserved.)
- Published
- 2012
- Full Text
- View/download PDF
39. Iodine isotopes (127I and 129I) in aerosols at high altitude Alp stations.
- Author
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Jabbar T, Steier P, Wallner G, Priller A, Kandler N, and Kaiser A
- Subjects
- Anion Exchange Resins, Austria, Germany, Mass Spectrometry, Aerosols chemistry, Air Pollutants analysis, Altitude, Iodine Isotopes analysis, Iodine Radioisotopes analysis
- Abstract
Concentrations of gases and particulate matter have been proven to be affected by meteorological and geographical variables from urban locations to high mountain clean air sites. Following our previous research in Vienna, we summarize here new findings about concentration levels of iodine isotopes in aerosols collected at two Alpine meteorological stations, Sonnblick (Austria) and Zugspitze (Germany) during 2001. The present study mainly focuses on the effect of altitude on the anthropogenic concentration of (129)I and on the isotopic ratio (129)I/(127)I. Iodine was separated from matrix elements by using either an anion exchange method or solvent extraction, and was analyzed by ICP-MS and AMS. Over the altitude change from Vienna to Zugspitze and Sonnblick (202 m to 2962 m and 3106 m above sea level), stable iodine level decreased from an average of 0.94 ng m(-3) to 0.52 ng m(-3) and 0.62 ng m(-3), respectively. Similarly, (129)I concentrations at both Alpine stations were about 1 order of magnitude lower (10(4) atoms m(-3)) than values obtained for Vienna (10(5) atoms m(-3)) and reveal a strong vertical concentration gradient of (129)I. A high degree of variability is observed, which is due to wide variation in the origin of air masses. Furthermore, air trajectory analysis demonstrates the importance of large scale air transport mostly from southeast Europe for influencing Sonnblick whereas influence from northwest Europe is strong at Zugspitze. In contrast to (129)I, a higher concentration of (7)Be was found at higher altitude stations compared to Vienna which probably results from its production in the upper atmosphere.
- Published
- 2012
- Full Text
- View/download PDF
40. Uranium-236 as a new oceanic tracer: A first depth profile in the Japan Sea and comparison with caesium-137.
- Author
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Sakaguchi A, Kadokura A, Steier P, Takahashi Y, Shizuma K, Hoshi M, Nakakuki T, and Yamamoto M
- Abstract
We present a feasibility study for using
236 U as an oceanic circulation tracer based on depth profiles of236 U and137 Cs in the Japan/East Sea. The concentration of the predominantly anthropogenic236 U, 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 of137 Cs for the same water samples, but with a slightly lower ratio of137 Cs/236 U below 2000 m. The cumulative inventory of dissolved236 U 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 of236 U. Our results suggest that236 U behaves as a conservative nuclide in seawater, with potential advantages over other tracers of oceanic circulation.- Published
- 2012
- Full Text
- View/download PDF
41. The age of olfactory bulb neurons in humans.
- Author
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Bergmann O, Liebl J, Bernard S, Alkass K, Yeung MS, Steier P, Kutschera W, Johnson L, Landén M, Druid H, Spalding KL, and Frisén J
- Subjects
- Cell Movement physiology, Humans, Neurons physiology, Olfactory Bulb physiology, Neurogenesis physiology, Neurons cytology, Olfactory Bulb cytology, Smell physiology
- Abstract
Continuous turnover of neurons in the olfactory bulb is implicated in several key aspects of olfaction. There is a dramatic decline postnatally in the number of migratory neuroblasts en route to the olfactory bulb in humans, and it has been unclear to what extent the small number of neuroblasts at later stages contributes new neurons to the olfactory bulb. We have assessed the age of olfactory bulb neurons in humans by measuring the levels of nuclear bomb test-derived (14)C in genomic DNA. We report that (14)C concentrations correspond to the atmospheric levels at the time of birth of the individuals, establishing that there is very limited, if any, postnatal neurogenesis in the human olfactory bulb. This identifies a fundamental difference in the plasticity of the human brain compared to other mammals., (Copyright © 2012 Elsevier Inc. All rights reserved.)
- Published
- 2012
- Full Text
- View/download PDF
42. Light induced suppression of sulfur in a cesium sputter ion source.
- Author
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Martschini M, Rohlén J, Andersson P, Golser R, Hanstorp D, Lindahl AO, Priller A, Steier P, and Forstner O
- Abstract
New techniques for suppression of atomic isobars in negative ion beams are of great interest for accelerator mass spectrometry (AMS). Especially small and medium-sized facilities can significantly extend their measurement capabilities to new interesting isotopes with a technique independent of terminal voltage. In a new approach, the effect of continuous wave laser light directed towards the cathode surface in a cesium sputter ion source of the Middleton type was studied. The laser light induced a significant change in oxygen, sulfur and chlorine negative ion production from a AgCl target. Approximately 100 mW of laser light reduced the sulfur to chlorine ratio by one order of magnitude. The effect was found to depend on laser power and ion source parameters but not on the laser wavelength. The time constant of the effect varied from a few seconds up to several minutes. Experiments were first performed at the ion beam facility GUNILLA at University of Gothenburg with macroscopic amounts of sulfur. The results were then reproduced at the VERA AMS facility with chemically cleaned AgCl targets containing ∼1 ppm sulfur. The physical explanation behind the effect is still unclear. Nevertheless, the technique has been successfully applied during a regular AMS measurement of
36 Cl.- Published
- 2012
- Full Text
- View/download PDF
43. Dynamics of human adipose lipid turnover in health and metabolic disease.
- Author
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Arner P, Bernard S, Salehpour M, Possnert G, Liebl J, Steier P, Buchholz BA, Eriksson M, Arner E, Hauner H, Skurk T, Rydén M, Frayn KN, and Spalding KL
- Subjects
- Adipocytes chemistry, Adipocytes metabolism, Adipose Tissue cytology, Adolescent, Adult, Aged, Aged, 80 and over, Carbon Radioisotopes analysis, Cell Size, Cellular Senescence, Child, Child, Preschool, Cohort Studies, DNA chemistry, Dyslipidemias metabolism, Dyslipidemias pathology, Humans, Hyperlipidemia, Familial Combined genetics, Hyperlipidemia, Familial Combined metabolism, Hyperlipidemia, Familial Combined pathology, Lipolysis, Middle Aged, Nuclear Weapons, Obesity metabolism, Subcutaneous Fat metabolism, Time Factors, Triglycerides analysis, Triglycerides metabolism, Young Adult, Adipose Tissue metabolism, Health, Lipid Metabolism, Metabolic Diseases metabolism
- Abstract
Adipose tissue mass is determined by the storage and removal of triglycerides in adipocytes. Little is known, however, about adipose lipid turnover in humans in health and pathology. To study this in vivo, here we determined lipid age by measuring (14)C derived from above ground nuclear bomb tests in adipocyte lipids. We report that during the average ten-year lifespan of human adipocytes, triglycerides are renewed six times. Lipid age is independent of adipocyte size, is very stable across a wide range of adult ages and does not differ between genders. Adipocyte lipid turnover, however, is strongly related to conditions with disturbed lipid metabolism. In obesity, triglyceride removal rate (lipolysis followed by oxidation) is decreased and the amount of triglycerides stored each year is increased. In contrast, both lipid removal and storage rates are decreased in non-obese patients diagnosed with the most common hereditary form of dyslipidaemia, familial combined hyperlipidaemia. Lipid removal rate is positively correlated with the capacity of adipocytes to break down triglycerides, as assessed through lipolysis, and is inversely related to insulin resistance. Our data support a mechanism in which adipocyte lipid storage and removal have different roles in health and pathology. High storage but low triglyceride removal promotes fat tissue accumulation and obesity. Reduction of both triglyceride storage and removal decreases lipid shunting through adipose tissue and thus promotes dyslipidaemia. We identify adipocyte lipid turnover as a novel target for prevention and treatment of metabolic disease.
- Published
- 2011
- Full Text
- View/download PDF
44. Pego do Diabo (Loures, Portugal): dating the emergence of anatomical modernity in westernmost Eurasia.
- Author
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Zilhão J, Davis SJ, Duarte C, Soares AM, Steier P, and Wild E
- Subjects
- Animals, Humans, Portugal, Anatomy, Anthropology, Fossils
- Abstract
Background: Neandertals and the Middle Paleolithic persisted in the Iberian Peninsula south of the Ebro drainage system for several millennia beyond their assimilation/replacement elsewhere in Europe. As only modern humans are associated with the later stages of the Aurignacian, the duration of this persistence pattern can be assessed via the dating of diagnostic occurrences of such stages., Methodology/principal Findings: Using AMS radiocarbon and advanced pretreatment techniques, we dated a set of stratigraphically associated faunal samples from an Aurignacian III-IV context excavated at the Portuguese cave site of Pego do Diabo. Our results establish a secure terminus ante quem of ca. 34,500 calendar years ago for the assimilation/replacement process in westernmost Eurasia. Combined with the chronology of the regional Late Mousterian and with less precise dating evidence for the Aurignacian II, they place the denouement of that process in the 37th millennium before present., Conclusions/significance: These findings have implications for the understanding of the emergence of anatomical modernity in the Old World as a whole, support explanations of the archaic features of the Lagar Velho child's anatomy that invoke evolutionarily significant Neandertal/modern admixture at the time of contact, and counter suggestions that Neandertals could have survived in southwest Iberia until as late as the Last Glacial Maximum.
- Published
- 2010
- Full Text
- View/download PDF
45. Chronology for the Aegean Late Bronze Age 1700-1400 B.C.
- Author
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Manning SW, Ramsey CB, Kutschera W, Higham T, Kromer B, Steier P, and Wild EM
- Subjects
- Bayes Theorem, Carbon Radioisotopes, Chronology as Topic, Greece, Ancient, History, Ancient, Plants, Seeds, Trees growth & development, Volcanic Eruptions, Archaeology, Civilization history
- Abstract
Radiocarbon (carbon-14) data from the Aegean Bronze Age 1700-1400 B.C. show that the Santorini (Thera) eruption must have occurred in the late 17th century B.C. By using carbon-14 dates from the surrounding region, cultural phases, and Bayesian statistical analysis, we established a chronology for the initial Aegean Late Bronze Age cultural phases (Late Minoan IA, IB, and II). This chronology contrasts with conventional archaeological dates and cultural synthesis: stretching out the Late Minoan IA, IB, and II phases by approximately 100 years and requiring reassessment of standard interpretations of associations between the Egyptian and Near Eastern historical dates and phases and those in the Aegean and Cyprus in the mid-second millennium B.C.
- Published
- 2006
- Full Text
- View/download PDF
46. Direct dating of Early Upper Palaeolithic human remains from Mladec.
- Author
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Wild EM, Teschler-Nicola M, Kutschera W, Steier P, Trinkaus E, and Wanek W
- Subjects
- Czech Republic, Female, History, Ancient, Humans, Male, Mandible anatomy & histology, Time Factors, Fossils, Skull anatomy & histology
- Abstract
The human fossil assemblage from the Mladec Caves in Moravia (Czech Republic) has been considered to derive from a middle or later phase of the Central European Aurignacian period on the basis of archaeological remains (a few stone artefacts and organic items such as bone points, awls, perforated teeth), despite questions of association between the human fossils and the archaeological materials and concerning the chronological implications of the limited archaeological remains. The morphological variability in the human assemblage, the presence of apparently archaic features in some specimens, and the assumed early date of the remains have made this fossil assemblage pivotal in assessments of modern human emergence within Europe. We present here the first successful direct accelerator mass spectrometry radiocarbon dating of five representative human fossils from the site. We selected sample materials from teeth and from one bone for 14C dating. The four tooth samples yielded uncalibrated ages of approximately 31,000 14C years before present, and the bone sample (an ulna) provided an uncertain more-recent age. These data are sufficient to confirm that the Mladec human assemblage is the oldest cranial, dental and postcranial assemblage of early modern humans in Europe and is therefore central to discussions of modern human emergence in the northwestern Old World and the fate of the Neanderthals.
- Published
- 2005
- Full Text
- View/download PDF
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