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  • Wiley  (11)
  • GSA (Geological Society of America)  (3)
  • 2020-2024  (14)
  • 1
    Publication Date: 2023-02-08
    Description: Key Points Calibration of XRF core scanning data highlights the need for careful examination of sediment properties such as porosity/water Grain size and water content in the sediment trigger systematic artifacts in the signal intensity of light elements (e.g. Si and Al) Known terrigenous flux proxies (e.g Ti/Ca, Fe/Ca) are influenced by sea level variations X‐ray fluorescence (XRF) core scanning of marine and lake sediments has been extensively used to study changes in past environmental and climatic processes over a range of timescales. The interpretation of XRF‐derived element ratios in paleoclimatic and paleoceanographic studies primarily considers differences in the relative abundances of particular elements. Here we present new XRF core scanning data from two long sediment cores in the Andaman Sea in the northern Indian Ocean and show that sea level related processes influence terrigenous inputs based proxies such as Ti/Ca, Fe/Ca, and elemental concentrations of the transition metals (e.g. Mn). Zr/Rb ratios are mainly a function of changes in median grain size of lithogenic particles and often covary with changes in Ca concentrations that reflect changes in biogenic calcium carbonate production. This suggests that a common process (i.e. sea level) influences both records. The interpretation of lighter element data (e.g. Si and Al) based on low XRF counts is complicated as variations in mean grain size and water content result in systematic artifacts and signal intensities not related to the Al or Si content of the sediments. This highlights the need for calibration of XRF core scanning data based on discrete sample analyses and careful examination of sediment properties such as porosity/water content for reliably disentangling environmental signals from other physical properties. In the case of the Andaman Sea, reliable extraction of a monsoon signal will require accounting for the sea level influence on the XRF data.
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  • 2
    Publication Date: 2023-02-08
    Description: Increased carbon sequestration in the ocean subsurface is commonly assumed to have been one of the main causes responsible for lower glacial atmospheric CO2 concentrations. Remineralized carbon must have been stored away from the atmosphere for thousands of years, yet the water mass structure accommodating such increased carbon storage continues to be debated. Here, we present new sediment-derived bottom-water neodymium isotope records that allow fingerprinting of water masses and provide a more complete picture of the Atlantic Meridional Overturning Circulation geometry during the Last Glacial Maximum. These results suggest that the vertical and meridional structure of the Atlantic water mass distribution only experienced minor changes since the last ice age. In particular, we find no compelling evidence supporting glacial southern-sourced water substantially expanding to shallower depths and farther into the Northern Hemisphere than today, which had been previously inferred from stable carbon isotope (δ13C) reconstructions. We argue that depleted δ13C values observed in the deep Northwest Atlantic do not necessarily indicate the presence of southern-sourced water. Instead, these values may represent a northern-sourced water mass with lower than modern preformed δ13C values that were further modified downstream by increased sequestration of remineralized carbon, facilitated by a more sluggish glacial deep circulation, corroborating previous evidence.
    Type: Article , PeerReviewed
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  • 3
    Publication Date: 2024-01-11
    Description: Beryllium isotopes have emerged as a quantitative tracer of continental weathering, but accurate and precise determination of the cosmogenic 10 Be and stable 9 Be in seawater is challenging, because seawater contains high concentrations of matrix elements but extremely low concentrations of 9 Be and 10 Be. In this study, we develop a new, time‐efficient procedure for the simultaneous preconcentration of 9 Be and 10 Be from (coastal) seawater based on the iron co‐precipitation method. The concentrations of 9 Be, 10 Be, and the resulting 10 Be/ 9 Be ratio for Changjiang Estuary water derived from the new procedure agree well with those obtained from the conventional procedure requiring separate preconcentration for 9 Be and 10 Be determinations. By avoiding the separate preconcentration, our newly developed procedure contributes toward more time‐efficient handling of samples, less sample cross‐contamination, and a more reliable 10 Be/ 9 Be ratio. Prior to this, we validated the iron co‐precipitation method using artificial seawater and natural water samples from the Amazon Estuary regarding: (1) the “matrix effect” for Be analysis, (2) its extraction efficiency for pg g −1 levels Be in the presence and absence of organic matter, and (3) the data comparability with another preconcentration method. We calculated that for the determination of 9 Be and 10 Be in most open ocean seawater with typical 10 Be concentrations of 〉 500 atoms g −1 , good precisions (〈 5%) can be achieved using less than 3 liters of seawater compared to more than 20 liters routinely used previously. Even for coastal seawater with extremely low 10 Be concentration (e.g., 100 atoms g −1 ), we estimate a maximum amount of 10 liters to be adequate.
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  • 4
    Publication Date: 2024-02-07
    Description: Ratios of (un)reactive iron species, authigenic molybdenum contents (Moauth), and molybdenum isotope compositions (δ98Moauth) in sedimentary rocks are geochemical proxies that are widely used to reconstruct past marine redox states, which have been calibrated in modern marine settings covering oxic to euxinic conditions. However, syn- and postdepositional processes can result in alterations and ambiguities of proxy-derived redox signals that can challenge the validity of paleoreconstructions. We present new data from modern organic-rich sediments of two oxygen minimum zone settings in the Gulf of California and the Peruvian margin. The results show that Mo is fully immobilized shortly after deposition by reaction with hydrogen sulfide (H2S) produced during organoclastic sulfate reduction. Thus, any H2S produced deeper in the sediment (e.g., by sulfate reduction coupled to anaerobic methane oxidation) leaves the initially deposited Mo concentrations and δ98Mo signatures unaltered, which supports the robustness of Mo-based redox proxies. In contrast, the Fe speciation data reveal continued pyritization due to constant exposure of Fe minerals to H2S. Importantly, both Fe bound to oxides and carbonates (highly reactive Fe) and also poorly reactive Fe (e.g., sheet silicates) undergo pyritization during early diagenesis. This process generates Fe-based proxy signatures that falsely imply ferruginous or euxinic conditions.
    Type: Article , PeerReviewed
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  • 5
    Publication Date: 2024-02-07
    Description: The correlation between concentrations of dissolved barium (dBa) and silicon (dSi) in the modern ocean supports the use of Ba as a paleoceanographic proxy. However, the mechanisms behind their linkage and the exact processes controlling oceanic Ba cycling remain enigmatic. To discern the extent to which this association arises from biogeochemical processes versus physical mixing, we examine the behavior of Ba and Si at the Congo River-dominated Southeast Atlantic margin where active biological processes and large boundary inputs override the large-scale ocean circulation. Here we present the first combined measurements of dissolved stable Ba (δ138Ba) and Si (δ30Si) isotopes as well as Ba and Si fluxes estimated based on 228Ra from the Congo River mouth to the northern Angola Basin. In the surface waters, river-borne particle desorption or dissolution and shelf inputs lead to non-conservative additions of both dBa and dSi to the Congo-shelf-zone, with the Ba flux increasing more strongly than that of Si across the shelf. In the epipelagic and mesopelagic layers, Ba and Si are decoupled likely due to different depths of in situ barite precipitation and biogenic silica production. In the deep waters of the northern Angola Basin, we observe large enrichment of dBa, likely originating from high benthic inputs from the Congo deep-sea fan sediments. Our results reveal different mechanisms controlling the biogeochemical cycling of Ba and Si and highlight a strong margin influence on marine Ba cycling. Their close association across the global ocean must therefore mainly be a consequence of the large-scale ocean circulation. Key Points Stronger enrichment of dissolved barium (dBa) than silicon (dSi) observed in the shelf-zone of the Congo plume Diatom silica production has negligible effect on dissolved Ba isotopic compositions in large river plumes Strong dBa enrichment (up to 24 nM) in the deep water of the northern Angola Basin likely originates from high benthic inputs
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  • 6
    Publication Date: 2024-02-07
    Description: Stable barium isotopes are a potential proxy for riverine inputs into the ocean that reflect monsoon variability and climate change. However, dissolved Ba isotope (δ138BaDBa) geochemistry in river estuaries, a dynamic land to ocean transition zone, has rarely been systematically examined to date. Here, we show that significant Ba isotope fractionation occurs at near-zero salinities in the Yangtze and Pearl River Estuary, whereas conservative mixing dominates δ138BaDBa distributions beyond low salinities, which are well predicted by an ion exchange model. Elevated δ138BaDBa in the river endmember results from preferential removal of light Ba isotopes by adsorption to fluvial particles. Subsequently, δ138BaDBa rapidly drops to minimum signatures at increased salinities indicating particle desorption of isotopically light Ba. Nevertheless, the apparently conservative δ138BaDBa-salinity relationship beyond the low-salinity minimum in both estuaries provides a modern calibration for using Ba isotopes as a proxy for paleosalinity and river water inputs into the ocean.
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  • 7
    Publication Date: 2024-02-07
    Description: Limited constraints on the variability of the deep-water production in the Labrador Sea complicate reconstructions of the strength of the Atlantic Meridional Overturning Circulation (AMOC) during the Late Quaternary. Large volumes of detrital carbonates were repeatedly deposited in the Labrador Sea during the last 32 kyr, potentially affecting radiogenic Nd isotope signatures. To investigate this the Nd isotope compositions of deep and intermediate waters were extracted from the authigenic Fe-Mn oxyhydroxide fraction, foraminiferal coatings, the residual silicates and leachates of dolostone grains. We provide a first order estimation of Nd release via dissolution of detrital carbonates and its contribution to the authigenic ԑNd signatures in the Labrador Sea. During the Last Glacial Maximum the Nd isotope signatures in the Labrador Sea would allow active water mass mixing with more radiogenic ɛNd values (-12.6 and -14) prevailing in its eastern part whereas less radiogenic values (ɛNd ∼ -18.4) were found on the western Labrador slope. The deposition of detrital carbonates during Heinrich stadials (2,1) was accompanied by negative detrital and authigenic Nd isotope excursions (ɛNd ∼ -31) that were likely controlled by dissolution of dolostone or dolostone associated mineral inclusions. This highly unradiogenic signal dominated the authigenic phases and individual water masses in the Labrador Sea, serving as potential source of highly unradiogenic Nd to the North Atlantic region, while exported southward. The Holocene authigenic ɛNd signatures of the coatings and leachates significantly differed from those of the detrital silicates, approaching modern bottom water mass signatures during the Late Holocene. Key Points - Estimation of Nd release via dissolution of detrital carbonates and its contribution to the authigenic ԑNd signatures in the Labrador Sea - Dissolution of detrital dolostones in the water column during Heinrich stadials at least partially controlled ɛNd signatures - During the LGM generally more radiogenic signatures possibly indicate active water mass advection and mixing in the Labrador Sea
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  • 8
    Publication Date: 2024-02-07
    Description: The development of stable barium (Ba) isotope measurements provides a novel tool to investigate the geochemical cycling of Ba in the ocean and its sediments. In sediment pore waters, gradients of dissolved Ba concentrations result from various diagenetic processes. The distribution and fractionation of Ba isotopes in the pore waters are expected to further improve our understanding of these early diagenetic control mechanisms. Here, we present pore water profiles of dissolved stable Ba isotopic signatures (δ138Bapw) from shallow water sediments covering the entire Pearl River Estuary (PRE) in Southern China. We find pronounced depth-dependent Ba isotope variations generally showing a shift from heavy to light δ138Bapw signatures from the sediment surface down to 15 cm depth. These gradients are well reproduced by a diffusion-reaction model, which generates an apparent fractionation factor (138ε) of −0.60 ± 0.10‰ pointing to preferential removal of low-mass Ba isotopes from the pore water during solution-solid phase interactions. Consequently, the combined diagenetic processes induce the highest δ138Bapw values of +0.5 to +0.7‰ in the pore waters of the topmost sediment layer. Although the detrital fraction dominates the Ba content in the PRE surface sediments, the determined gradients of pore water Ba isotopes, together with concentration variations of Ba and other redox-sensitive elements such as manganese (Mn), show that non-detrital excess Ba carriers including Mn oxides and authigenic barite clearly affect the post-depositional Ba dynamics. Stable Ba isotopes are thus a potentially powerful tracer of Ba geochemistry during early sediment diagenesis in estuarine depositional environments. Key Points We present a data set of dissolved stable Ba isotopic compositions in surface sediment pore waters of a large river estuary Pore water Ba isotope values generally decrease with increasing sediment depth, reflecting post-depositional Ba isotope fractionation A diffusion-reaction model predicts the distribution and fractionation of stable Ba isotopes in the sediment pore waters well
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  • 9
    Publication Date: 2024-02-07
    Description: Reactive iron (Fe) oxides in marine sediments may represent a source of bioavailable Fe to the ocean via reductive dissolution and sedimentary Fe release or can promote organic carbon preservation and long-term burial. Furthermore, enrichments of reactive Fe (sum of Fe oxides, carbonates and sulfides normalized to total Fe) in ancient sediments are utilized as a paleo-proxy for anoxic conditions. Considering the general importance of reactive Fe oxides in marine biogeochemistry, it is important to quantify their terrestrial sources and fate at the land-ocean interface. We applied sequential Fe extractions to sediments from the Amazon shelf to investigate the transformation of river-derived Fe oxides during early diagenesis. We found that ∼22 % of the Amazon River-derived Fe oxides are converted to Fe-containing clay minerals in Amazon shelf sediments. The incorporation of reactive Fe into authigenic clay minerals (commonly referred to as reverse weathering) is substantiated by the relationship between Fe oxide loss and potassium (K) uptake from sedimentary pore waters, which is in agreement with the previously reported Fe/K stoichiometry of authigenic clay minerals. Mass balance calculations suggest that widely applied sequential extractions do not separate Fe-rich authigenic clay minerals from reactive Fe oxides and carbonates. We conclude that the balance between terrestrial supply of reactive Fe and reverse weathering in continental margin sediments has to be taken into account in the interpretation of sedimentary Fe speciation data. Key Points - Reactive Fe is transferred from river-derived Fe oxides into Fe-containing silicate minerals during early diagenesis - Standard sequential extraction schemes do not separate Fe oxides and carbonates from authigenic silicate minerals in Amazon shelf sediments - Terrigenous supply of reactive Fe and reverse weathering need to be considered in the interpretation of sedimentary Fe speciation
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  • 10
    Publication Date: 2024-02-07
    Description: The development of the South Asian monsoon (SAM) and Himalaya‐Tibetan Plateau uplift were closely intertwined with some studies suggesting that uplift initiated the monsoon whereas others link tectonics with monsoon‐controlled exhumation. Silicate weathering controls atmospheric CO2 on geological timescales resulting in a large potential for monsoon strength and the Himalayan orogeny to influence global climate but detailed records of SAM‐induced weathering on million year (Myr) timescales are lacking. Here, we present radiogenic Sr, Nd, and Pb isotope compositions of clay minerals produced by silicate weathering and transported to the central Bay of Bengal. The radiogenic isotope data exhibit a relatively small range and demonstrate a remarkably consistent mixture of sources dominated by Himalayan rocks and the Indo‐Burman ranges, which consist of sediments derived from the Himalayas. This suggests that the spatial pattern of regional weathering, which today is highest in the regions of strongest monsoon rains, has persisted in a similar form for the last 27 Myrs. A pronounced increase in primary clay mineral abundance (from 9% to 22%) coincident with global cooling 13.9 Myrs ago points to a shift in the weathering regime given that the clay provenance did not change dramatically. Relatively weaker chemical weathering intensity during the mid and late Miocene cooling suggests increased aridity and changes in the large scale atmospheric circulation in the SAM domain. The establishment of the dry winter monsoon season during the mid and late Miocene may have caused this shift in the weathering regime and can reconcile much of the contrasting evidence for SAM initiation.
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