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  • ddc:551.9  (32)
  • English  (32)
  • 2020-2023  (32)
  • 1955-1959
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  • English  (32)
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  • 1
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    A Triad Photoanode for Visible Light‐Driven Water Oxidation via Immobilization of Molecular Polyoxometalate on Polymeric Carbon Nitride (2022)
    Details
    Publication Date: 2022-08-04
    Description: Due to their availability, low cost, nontoxicity, and tunability, polymeric carbon nitrides (CNx) represent one of the most attractive materials classes for the development of fully sustainable photo(electro)catalytic systems for solar‐driven water splitting. However, the development of CNx‐based photoanodes for visible light‐driven water oxidation to dioxygen is rather challenging, particularly due to issues related to photoelectrode stability and effective coupling of the light absorber with water oxidation catalysts. Herein, a triadic photoanode comprising a porous TiO2 electron collector scaffold sensitized by CNx coupled to a molecular cobalt polyoxometalate (CoPOM = [Co4(H2O)2(PW9O34)2]10) catalyst is reported. Complete water oxidation to dioxygen under visible (λ 〉 420 nm) light irradiation is demonstrated, with photocurrents down to relatively low bias potentials (0.2 V vs RHE). Furthermore, polyethyleneimine (PEI), a cationic polymer is shown to act as an effective and non‐sacrificial electrostatic linker for immobilization of the anionic CoPOM onto the negatively charged surface of CNx. The optimized deposition of CoPOM using the PEI linker translates directly into improved efficiency of the transfer of photogenerated holes to water molecules and to enhanced oxygen evolution. This work thus provides important design rules for effective immobilization of POM‐based catalysts into soft‐matter photoelectrocatalytic architectures for light‐driven water oxidation.
    Description: A triadic photoanode comprised of a porous TiO2 electron collector scaffold sensitized by polymeric carbon nitride and coupled to a molecular cobalt polyoxometalate (CoPOM) catalyst exhibits visible (λ 〉 420 nm) light‐driven water oxidation to dioxygen. The beneficial role of the cationic polyethyleneimine polymer as an effective electrostatic linker for immobilization of CoPOM onto carbon nitride is highlighted.
    Description: Deutsche Forschungsgemeinschaft http://dx.doi.org/10.13039/501100001659
    Description: Vector Stiftung http://dx.doi.org/10.13039/501100013912
    Keywords: ddc:551.9
    Language: English
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  • 2
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    Analytical Artefacts Preclude Reliable Isotope Ratio Measurement of Internal Water in Coral Skeletons (2022)
    de Graaf, Stefan ; Vonhof, Hubert B. ; Reijmer, John J. G. ; [et al.]
    Details
    Publication Date: 2022-10-01
    Description: Internal water in cold‐water and tropical coral skeletons was extracted and measured for its oxygen and hydrogen isotope ratios. Water was extracted by crushing pieces of coral hard tissue in a percussion device connected to either a cavity ring‐down spectroscopy (CRDS) system or an isotope ratio mass spectrometry (IRMS) system. Despite most samples yielding sufficient water, each analytical system produces distinct isotope patterns. Experiments show that several characteristics specific to biominerals give rise to discrepancies and analytical artefacts that preclude the acquisition of reproducible isotope data. The main complication is that internal water in biogenic carbonates is distributed in an open interconnected micro‐network that readily exchanges with external water and potentially facilitates interaction with hydration water in the finely dispersed organic matrix in the coral skeleton. Furthermore, only an isotopically fractionated part of the internal water is released from the coral skeletons upon crushing. Altogether, isotope ratio measurement of internal water in corals with bulk crushing techniques does not give primary fluid isotope ratios useful for (palaeo‐)environmental or microbiological studies. As the resulting isotope patterns can show systematic behaviour per technique, isotope data may be erroneously interpreted to reflect the original calcifying fluid when using only a single technique to isotopically characterise internal fluids in coral skeletons.
    Description: Key Points: Free water trapped inside coral skeletons was extracted and isotopically analyzed on two commonly used techniques for fluid inclusion isotope analysis. Measured oxygen and hydrogen isotope ratios do not reproduce between the techniques due to several analytical artefacts. The water extracted from coral skeletons is not of primary origin.
    Description: Nederlandse Organisatie voor Wetenschappelijk Onderzoek http://dx.doi.org/10.13039/501100003246
    Description: Western Indian Ocean Marine Science Association http://dx.doi.org/10.13039/501100009106
    Keywords: ddc:551.9
    Language: English
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  • 3
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    Arctic – Atlantic Exchange of the Dissolved Micronutrients Iron, Manganese, Cobalt, Nickel, Copper and Zinc With a Focus on Fram Strait (2022)
    Details
    Publication Date: 2022-10-04
    Description: The Arctic Ocean is considered a source of micronutrients to the Nordic Seas and the North Atlantic Ocean through the gateway of Fram Strait (FS). However, there is a paucity of trace element data from across the Arctic Ocean gateways, and so it remains unclear how Arctic and North Atlantic exchange shapes micronutrient availability in the two ocean basins. In 2015 and 2016, GEOTRACES cruises sampled the Barents Sea Opening (GN04, 2015) and FS (GN05, 2016) for dissolved iron (dFe), manganese (dMn), cobalt (dCo), nickel (dNi), copper (dCu) and zinc (dZn). Together with the most recent synopsis of Arctic‐Atlantic volume fluxes, the observed trace element distributions suggest that FS is the most important gateway for Arctic‐Atlantic dissolved micronutrient exchange as a consequence of Intermediate and Deep Water transport. Combining fluxes from FS and the Barents Sea Opening with estimates for Davis Strait (GN02, 2015) suggests an annual net southward flux of 2.7 ± 2.4 Gg·a−1 dFe, 0.3 ± 0.3 Gg·a−1 dCo, 15.0 ± 12.5 Gg·a−1 dNi and 14.2 ± 6.9 Gg·a−1 dCu from the Arctic toward the North Atlantic Ocean. Arctic‐Atlantic exchange of dMn and dZn were more balanced, with a net southbound flux of 2.8 ± 4.7 Gg·a−1 dMn and a net northbound flux of 3.0 ± 7.3 Gg·a−1 dZn. Our results suggest that ongoing changes to shelf inputs and sea ice dynamics in the Arctic, especially in Siberian shelf regions, affect micronutrient availability in FS and the high latitude North Atlantic Ocean.
    Description: Plain Language Summary: Recent studies have proposed that the Arctic Ocean is a source of micronutrients such as dissolved iron (dFe), manganese (dMn), cobalt (dCo), nickel (dNi), copper (dCu) and zinc (dZn) to the North Atlantic Ocean. However, data at the Arctic Ocean gateways including Fram Strait and the Barents Sea Opening have been missing to date and so the extent of Arctic micronutrient transport toward the Atlantic Ocean remains unquantified. Here, we show that Fram Strait is the most important gateway for Arctic‐Atlantic micronutrient exchange which is a result of deep water transport at depths 〉500 m. Combined with a flux estimate for Davis Strait, this study suggests that the Arctic Ocean is a net source of dFe, dNi and dCu, and possibly also dCo, toward the North Atlantic Ocean. Arctic‐Atlantic dMn and dZn exchange seems more balanced. Properties in the East Greenland Current showed substantial similarities to observations in the upstream Central Arctic Ocean, indicating that Fram Strait may export micronutrients from Siberian riverine discharge and shelf sediments 〉3,000 km away. Increasing Arctic river discharge, permafrost thaw and coastal erosion, all consequences of ongoing climate change, may therefore alter future Arctic Ocean micronutrient transport to the North Atlantic Ocean.
    Description: Key Points: Fram Strait is the major gateway for Arctic‐Atlantic exchange of the dissolved micronutrients Fe, Mn, Co, Ni, Cu and Zn. The Arctic is a net source of dissolved Fe, Co, Ni and Cu to the Nordic Seas and toward the North Atlantic; Mn and Zn exchange are balanced. Waters of the Central Arctic Ocean, including the Transpolar Drift, are the main drivers of gross Arctic micronutrient export.
    Description: German Research Foundation
    Description: Netherlands Organization for Scientific Research
    Description: https://doi.pangaea.de/10.1594/PANGAEA.859558
    Description: https://doi.pangaea.de/10.1594/PANGAEA.871030
    Description: https://doi.pangaea.de/10.1594/PANGAEA.868396
    Description: https://doi.pangaea.de/10.1594/PANGAEA.905347
    Description: https://dataportal.nioz.nl/doi/10.25850/nioz/7b.b.jc
    Description: https://doi.pangaea.de/10.1594/PANGAEA.933431
    Description: https://www.bco-dmo.org/dataset/718440
    Description: https://doi.org/10.1594/PANGAEA.936029
    Description: https://doi.org/10.1594/PANGAEA.936027
    Description: https://doi.pangaea.de/10.1594/PANGAEA.927429
    Keywords: ddc:551.9
    Language: English
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  • 4
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    Assessing the robustness of carbonate‐associated sulfate during hydrothermal dolomitization of the Latemar platform, Italy (2021)
    Details
    Publication Date: 2022-03-30
    Description: Carbonate‐associated sulfate (CAS) is an important proxy for reconstructing marine sulfur cycling throughout Earth's history. In order to assess the impact of carbonate neomorphism on δ34SCAS data, a mineralogical‐spatial transect from early diagenetic limestone into low‐temperature hydrothermal dolostone was analyzed in the middle Triassic Latemar platform interior, northern Italy. This study addresses the yet unconstrained question whether hydrothermal dolostone preserves a marine δ34SCAS signature and, hence, might represent an archive for past seawater sulfate. In this study, δ34SCAS values were measured in low‐temperature hydrothermal dolostone and compared with data from their corresponding precursor limestone. Results shown here reveal that δ34SCAS values for dolostone and precursor limestone are indistinguishable. This points to a rock‐buffered middle Triassic marine δ34S signature not affected by hydrothermal alteration. Hence, hydrothermal dolostone represents, under favorable conditions, an archive for unraveling past marine sulfur cycling.
    Description: Deutsche Forschungsgemeinschaft http://dx.doi.org/10.13039/501100001659
    Keywords: ddc:551.9 ; ddc:552
    Language: English
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  • 5
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    Benthic Carbon Remineralization and Iron Cycling in Relation to Sea Ice Cover Along the Eastern Continental Shelf of the Antarctic Peninsula (2022)
    Details
    Publication Date: 2022-10-04
    Description: Rapid and profound climatic and environmental changes have been predicted for the Antarctic Peninsula with so far unknown impact on the biogeochemistry of the continental shelves. In this study, we investigate benthic carbon sedimentation, remineralization and iron cycling using sediment cores retrieved on a 400 mile transect with contrasting sea ice conditions along the eastern shelf of the Antarctic Peninsula. Sediments at comparable water depths of 330–450 m showed sedimentation and remineralization rates of organic carbon, ranging from 2.5 to 13 and 1.8–7.2 mmol C m−2 d−1, respectively. Both rates were positively correlated with the occurrence of marginal sea ice conditions (5%–35% ice cover) along the transect, suggesting a favorable influence of the corresponding light regime and water column stratification on algae growth and sedimentation rates. From south to north, the burial efficiency of organic carbon decreased from 58% to 27%, while bottom water temperatures increased from −1.9 to −0.1°C. Net iron reduction rates, as estimated from pore‐water profiles of dissolved iron, were significantly correlated with carbon degradation rates and contributed 0.7%–1.2% to the total organic carbon remineralization. Tightly coupled phosphate‐iron recycling was indicated by significant covariation of dissolved iron and phosphate concentrations, which almost consistently exhibited P/Fe flux ratios of 0.26. Iron efflux into bottom waters of 0.6–4.5 μmol Fe m−2 d−1 was estimated from an empirical model. Despite the deep shelf waters, a clear bentho‐pelagic coupling is indicated, shaped by the extent and duration of marginal sea ice conditions during summer, and likely to be affected by future climate change.
    Description: Plain Language Summary: The seafloor of the shallow shelf seas plays a significant role in the recycling of organic carbon and acts as a nutrient source for algae growth in the upper water layers. In Antarctic waters, the change in sea ice cover has a great impact on the growth of algae and the subsequent sinking of organic carbon to the seafloor. With global warming, profound changes in sea ice cover are expected for the Antarctic Peninsula. To better understand its imprint on the seafloor, we collected sediment samples from different locations along the eastern shelf of the Antarctic Peninsula and measured how changes in sea ice cover influence the accumulation and recycling of organic carbon. We found that moderate sea ice cover of 5%–35% increases the amount of organic carbon received by the seafloor and that the fraction that is buried in the sediments decreases from south (58%) to north (27%). We further measured that more iron, an important micro‐nutrient for algae growth, can be released from the seafloor the more organic carbon accumulates. Thus, sea ice conditions determine the organic carbon accumulation, turnover, and nutrient release at the seafloor, which are likely to be affected by future climate change.
    Description: Key Points: Antarctic shelf sediments underlying marginal sea ice cover exhibit high sedimentation and remineralization rates of organic carbon. A high degree of sedimentary Fe‐recycling is found which scales with organic carbon remineralization rates. Coupling between P and Fe recycling is observed with a constant P/Fe flux ratio of 0.26 for sediments with high Fe and P recycling rates.
    Description: Alfred Wegener Institute Helmholtz Centre for Polar and Marine Research http://dx.doi.org/10.13039/501100003207
    Description: https://doi.org/10.1594/PANGAEA.942455
    Keywords: ddc:551.9
    Language: English
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  • 6
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    Chemical Evolution of the Exceptional Arctic Stratospheric Winter 2019/2020 Compared to Previous Arctic and Antarctic Winters (2021)
    Details
    Publication Date: 2022-03-28
    Description: The winter 2019/2020 showed the lowest ozone mixing ratios ever observed in the Arctic winter stratosphere. It was the coldest Arctic stratospheric winter on record and was characterized by an unusually strong and long‐lasting polar vortex. We study the chemical evolution and ozone depletion in the winter 2019/2020 using the global Chemistry and Transport Model ATLAS. We examine whether the chemical processes in 2019/2020 are more characteristic of typical conditions in Antarctic winters or in average Arctic winters. Model runs for the winter 2019/2020 are compared to simulations of the Arctic winters 2004/2005, 2009/2010, and 2010/2011 and of the Antarctic winters 2006 and 2011, to assess differences in chemical evolution in winters with different meteorological conditions. In some respects, the winter 2019/2020 (and also the winter 2010/2011) was a hybrid between Arctic and Antarctic conditions, for example, with respect to the fraction of chlorine deactivation into HCl versus ClONO2, the amount of denitrification, and the importance of the heterogeneous HOCl + HCl reaction for chlorine activation. The pronounced ozone minimum of less than 0.2 ppm at about 450 K potential temperature that was observed in about 20% of the polar vortex area in 2019/2020 was caused by exceptionally long periods in the history of these air masses with low temperatures in sunlight. Based on a simple extrapolation of observed loss rates, only an additional 21–46 h spent below the upper temperature limit for polar stratospheric cloud formation and in sunlight would have been necessary to reduce ozone to near zero values (0.05 ppm) in these parts of the vortex.
    Description: Key Points: The Arctic stratospheric winter 2019/2020 showed the lowest ozone mixing ratios ever observed and was one of the coldest on record. Chemical evolution of the Arctic winter 2019/2020 was a hybrid between typical Arctic and typical Antarctic conditions. Only an additional 21–46 h below PSC temperatures and in sunlight would have been necessary to reduce ozone to near zero locally.
    Description: International Multidisciplinary Drifting Observatory for the Study of the Arctic Climate (MOSAiC)
    Keywords: ddc:551.5 ; ddc:551.9
    Language: English
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  • 7
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    Chemical Geodynamics Insights From a Machine Learning Approach (2022)
    Details
    Publication Date: 2022-12-07
    Description: The radiogenic isotope heterogeneity of oceanic basalts is often assessed using 2D isotope ratio diagrams. But because the underlying data are at least six dimensional (87Sr/86Sr, 143Nd/144Nd, 176Hf/177Hf, and 208,207,206Pb/204Pb), it is important to examine isotopic affinities in multi‐dimensional data space. Here, we apply t‐distributed stochastic neighbor embedding (t‐SNE), a multi‐variate statistical data analysis technique, to a recent compilation of radiogenic isotope data of mid ocean ridge (MORB) and ocean island basalts (OIB). The t‐SNE results show that the apparent overlap of MORB‐OIB data trends in 2‐3D isotope ratios diagrams does not exist in multi‐dimensional isotope data space, revealing that there is no discrete “component” that is common to most MORB‐OIB mantle sources on a global scale. Rather, MORB‐OIB sample stochastically distributed small‐scale isotopic heterogeneities. Yet, oceanic basalts with the same isotopic affinity, as identified by t‐SNE, delineate several globally distributed regional domains. In the regional geodynamic context, the isotopic affinity of MORB and OIB is caused by capturing of actively upwelling mantle by adjacent ridges, and thus melting of mantle with similar origin in on, near, and off‐ridge settings. Moreover, within a given isotopic domain, subsidiary upwellings rising from a common deep mantle root often feed OIB volcanism over large surface areas. Overall, the t‐SNE results define a fundamentally new basis for relating isotopic variations in oceanic basalts to mantle geodynamics, and may launch a 21st century era of “chemical geodynamics.”
    Description: Plain Language Summary: The isotopic heterogeneity of basalts erupted at mid ocean ridges (MORB) and ocean islands (OIB) reflects the chemical evolution of Earth's mantle. The visual inspection of various 2D isotope ratio diagrams has fueled a four decade‐long discussion whether basalt heterogeneity reflects melting of only a small number of mantle components, and in particular, whether the apparent overlap of local data trends in global 2D isotope ratio diagrams indicates that melting of a common mantle component contributes to most MORB‐OIB. Here, we use multi‐variate statistical data analysis to show that the apparent overlap of MORB‐OIB data trends in 2D isotope ratio diagrams does not exist in multi‐dimensional isotope data space. Our finding invalidates any inference made for mantle compositional evolution based on the previously proposed existence of a common mantle component, its potential nature or distribution within the mantle. Rather, global MORB‐OIB sample small‐scale isotopic heterogeneities that are distributed stochastically in the Earth's mantle. Yet, MORB‐OIB with the same isotopic affinity, as identified by our multi‐variate data analysis, delineate several globally distributed regional domains. Within the regional geodynamic context, this discovery forms a fundamentally new basis for relating isotopic variations in MORB‐OIB to mantle geodynamics.
    Description: Key Points: Multi‐variate statistical data analysis (t‐distributed stochastic neighbor embedding) identifies global Sr‐Nd‐Hf‐Pb isotopic affinities of oceanic basalts. There is no “common mantle component;” rather, global mid ocean ridge‐ocean island basalts sample stochastically distributed small‐scale isotopic heterogeneities. Globally distributed regional domains of isotopically alike oceanic lavas define a new basis for relating isotopic variations to geodynamics.
    Description: Deutsche Forschungsgemeinschaft http://dx.doi.org/10.13039/501100001659
    Description: Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung http://dx.doi.org/10.13039/501100001711
    Description: DAAD, German Academic Exchange Service
    Description: https://doi.org/10.25625/0SVW6S
    Description: https://doi.org/10.25625/BQENGN
    Keywords: ddc:551.9 ; mantle heterogeneity ; MORB ; OIB ; geodynamics ; t‐SNE ; radiogenic isotopes ; machine learning
    Language: English
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  • 8
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    Collisional mixing between inner and outer solar system planetesimals inferred from the Nedagolla iron meteorite (2021)
    Details
    Publication Date: 2022-07-28
    Description: The ungrouped iron meteorite Nedagolla is the first meteorite with bulk Mo, Ru, and Ni isotopic compositions that are intermediate between those of the noncarbonaceous (NC) and carbonaceous (CC) meteorite reservoirs. The Hf‐W chronology of Nedagolla indicates that this mixed NC–CC isotopic composition was established relatively late, more than 7 Myr after solar system formation. The mixed NC–CC isotopic composition is consistent with the chemical composition of Nedagolla, which combines signatures of metal segregation under more oxidizing conditions (relative depletions in Mo and W), characteristic for CC bodies, and more reducing conditions (high Si and Cr contents), characteristic for some NC bodies, in a single sample. These data combined suggest that Nedagolla formed as the result of collisional mixing of NC and CC core material, which partially re‐equilibrated with silicate mantle material that predominantly derives from the NC body. These mixing processes might have occurred during a hit‐and‐run collision between two differentiated bodies, which also provides a possible pathway for Nedagolla's extreme volatile element depletion. As such, Nedagolla provides the first isotopic evidence for early collisional mixing of NC and CC bodies that is expected as a result of Jupiter's growth.
    Description: Deutsche Forschungsgemeinschaft http://dx.doi.org/10.13039/501100001659
    Keywords: ddc:551.9 ; ddc:549.112
    Language: English
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  • 9
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    Determination of Cu, Zn, Ga, Ag, Cd, In, Sn and Tl in Geological Reference Materials and Chondrites by Isotope Dilution ICP-MS (2020)
    Details
    Publication Date: 2022-11-28
    Description: Mass fractions of Cu, Zn, Ga, Ag, Cd, In, Sn and Tl were determined via isotope dilution quadrupole ICP-MS in twenty-one geological reference materials (RMs) and the carbonaceous chondrites Orgueil (CI1), Murchison (CM2) and Allende (CV3). The RMs comprise basaltic/mafic (BCR-2, BE-N, BHVO-1, BHVO-2, BIR-1, BRP-1, JB-2, OKUM, W-2, WS-E), intermediate/felsic (AGV-2, G-2, JA-2, RGM-1), ultramafic (DTS-2b, MUH-1, PCC-1, UB-N) and sedimentary (MAG-1, OU-6) rocks. Pressure digestion was applied for nonbasaltic samples to ensure effective sample digestion. For basaltic RMs, hot plate digestion was found to be sufficient for a quantitative recovery of the target elements. To minimise interferences and increase ion beam intensities during isotope ratio analyses by ICP-MS, separation of the target elements was carried out from single sample aliquots using a novel anion exchange procedure. The intermediate precision (2s) estimated from two to four replicate analyses was usually 〈 4% and results are in agreement with literature data, where available. Especially for Ag and Tl, the intermediate precision was compromised, likely due to low ion beam intensities and, hence, higher background and blank contributions. For ultramafic RMs, nugget effects and incomplete digestion might compromise the intermediate precision. Results for the carbonaceous chondrites Orgueil (CI1), Murchison (CM2) and Allende (CV3) agree well with previously reported data.
    Keywords: ddc:551.9 ; isotope dilution ; chalcophile elements ; geological reference materials ; chondrites ; Q-ICP-MS
    Language: English
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  • 10
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    Detrital apatite geochemistry and thermochronology from the Oligocene/Miocene Alpine foreland record the early exhumation of the Tauern Window (2021)
    Details
    Publication Date: 2022-03-24
    Description: The early exhumation history of the Tauern Window in the European Eastern Alps and its surface expression is poorly dated and quantified, partly because thermochronological and provenance information are sparse from the Upper Austrian Northern Alpine Foreland Basin. For the first time, we combine a single‐grain double‐dating approach (Apatite Fission Track and U‐Pb dating) with trace‐element geochemistry analysis on the same apatites to reconstruct the provenance and exhumation history of the late Oligocene/early Miocene Eastern Alps. The results from 22 samples from the Chattian to Burdigalian sedimentary infill of the Upper Austrian Northern Alpine Foreland Basin were integrated with a 3D seismic‐reflection data set and published stratigraphic reports. Our highly discriminative data set indicates an increasing proportion of apatites (from 6% to 23%) with Sr/Y values 〈0.1 up‐section and an increasing amount of apatites (from 24% to 38%) containing 〉1,000 ppm light rare‐earth elements from Chattian to Burdigalian time. The number of U‐Pb ages with acceptable uncertainties increases from 40% to 59% up‐section, with mostly late Variscan/Permian ages, while an increasing number of grains (10%–27%) have Eocene or younger apatite fission track cooling ages. The changes in the apatite trace‐element geochemistry and U‐Pb data mirror increased sediment input from an ≥upper amphibolite‐facies metamorphic source of late Variscan/Permian age – probably the Ötztal‐Bundschuh nappe system – accompanied by increasing exhumation rates indicated by decreasing apatite fission track lag times. We attribute these changes to the surface response to upright folding and doming in the Penninic units of the future Tauern Window starting at 29–27 Ma. This early period of exhumation (0.3–0.6 mm/a) is triggered by early Adriatic indentation along the Giudicarie Fault System.
    Description: Science Foundation Ireland http://dx.doi.org/10.13039/501100001602
    Description: Deutsche Forschungsgemeinschaft http://dx.doi.org/10.13039/501100001659
    Keywords: ddc:551.701 ; ddc:551.9
    Language: English
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