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  • 1
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    Groundwater discharge impacts marine isotope budgets of Li, Mg, Ca, Sr, and Ba (2021)
    Nature Research
    Details
    Publication Date: 2022-05-26
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Mayfield, K. K., Eisenhauer, A., Santiago Ramos, D. P., Higgins, J. A., Horner, T. J., Auro, M., Magna, T., Moosdorf, N., Charette, M. A., Gonneea, M. E., Brady, C. E., Komar, N., Peucker-Ehrenbrink, B., & Paytan, A. Groundwater discharge impacts marine isotope budgets of Li, Mg, Ca, Sr, and Ba. Nature Communications, 12(1), (2021): 148-020-20248-3, doi:10.1038/s41467-020-20248-3.
    Description: Groundwater-derived solute fluxes to the ocean have long been assumed static and subordinate to riverine fluxes, if not neglected entirely, in marine isotope budgets. Here we present concentration and isotope data for Li, Mg, Ca, Sr, and Ba in coastal groundwaters to constrain the importance of groundwater discharge in mediating the magnitude and isotopic composition of terrestrially derived solute fluxes to the ocean. Data were extrapolated globally using three independent volumetric estimates of groundwater discharge to coastal waters, from which we estimate that groundwater-derived solute fluxes represent, at a minimum, 5% of riverine fluxes for Li, Mg, Ca, Sr, and Ba. The isotopic compositions of the groundwater-derived Mg, Ca, and Sr fluxes are distinct from global riverine averages, while Li and Ba fluxes are isotopically indistinguishable from rivers. These differences reflect a strong dependence on coastal lithology that should be considered a priority for parameterization in Earth-system models.
    Description: We thank A. Beck, H. Dulai, I. Santos, C. Benitez-Nelson, W. Moore, A. Martin, and H. Windom for sample access. We also thank A. Kolevica, A. Heuser, H. Pryer, J. Middleton, R. Franks, F. Lon, N. Slater, and O. Šebek for their laboratory and analytical assistance. This material is based upon research supported by the National Science Foundation Graduate Research Fellowship Program and an internship provided through the U.S. Geological Survey Graduate Research Internship Program (GRIP). This research was also supported by grants from: the German Academic Exchange Service (DAAD), Northern California chapter of the Achievement Rewards for College Scientists Foundation, International Association of GeoChemistry, Geological Society of America, Northern California Geological Society, Myers Trust, Friends of Long Marine Lab, and UC MEXUS (to K.K.M.). We acknowledge funding from EU-ITN Horizon project 643084 (to A.E. and T.M.) and NSF grant Award Number 1259440 (to A.P.). We also acknowledge funding from NSF grant award number OCE-1736949 (to T.J.H.). Any use of trade, firm or product names is for descriptive purposes only and does not imply endorsement by the U.S. Government.
    Repository Name: Woods Hole Open Access Server
    Type: Article
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    PAPER (OA)
  • 2
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    Coupling of oceanic carbon and nitrogen facilitates spatially resolved quantitative reconstruction of nitrate inventories (2018)
    Nature Research
    In:  Nature Communications, 9 (Article number 1217).
    Details
    Publication Date: 2021-03-19
    Description: Anthropogenic impacts are perturbing the global nitrogen cycle via warming effects and pollutant sources such as chemical fertilizers and burning of fossil fuels. Understanding controls on past nitrogen inventories might improve predictions for future global biogeochemical cycling. Here we show the quantitative reconstruction of deglacial bottom water nitrate concentrations from intermediate depths of the Peruvian upwelling region, using foraminiferal pore density. Deglacial nitrate concentrations correlate strongly with downcore δ13C, consistent with modern water column observations in the intermediate Pacific, facilitating the use of δ13C records as a paleo-nitrate-proxy at intermediate depths and suggesting that the carbon and nitrogen cycles were closely coupled throughout the last deglaciation in the Peruvian upwelling region. Combining the pore density and intermediate Pacific δ13C records shows an elevated nitrate inventory of 〉10% during the Last Glacial Maximum relative to the Holocene, consistent with a δ13C-based and δ15N-based 3D ocean biogeochemical model and previous box modeling studies.
    Type: Article , PeerReviewed , info:eu-repo/semantics/article
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    DOI: 10.1038/s41467-018-03647-5
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    OceanRep: Article in a Scientific Journal - peer-reviewed
  • 3
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    Ice volume and climate changes from a 6000 year sea-level record in French Polynesia (2018)
    Nature Research
    In:  Nature Communications, 9 (285).
    Details
    Publication Date: 2021-02-08
    Description: Mid- to late-Holocene sea-level records from low-latitude regions serve as an important baseline of natural variability in sea level and global ice volume prior to the Anthropocene. Here, we reconstruct a high-resolution sea-level curve encompassing the last 6000 years based on a comprehensive study of coral microatolls, which are sensitive low-tide recorders. Our curve is based on microatolls from several islands in a single region and comprises a total of 82 sea-level index points. Assuming thermosteric contributions are negligible on millennial time scales, our results constrain global ice melting to be 1.5–2.5 m (sea-level equivalent) since ~5500 years before present. The reconstructed curve includes isolated rapid events of several decimetres within a few centuries, one of which is most likely related to loss from the Antarctic ice sheet mass around 5000 years before present. In contrast, the occurrence of large and flat microatolls indicates periods of significant sea-level stability lasting up to ~300 years.
    Type: Article , PeerReviewed
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    DOI: 10.1038/s41467-017-02695-7
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    OceanRep: Article in a Scientific Journal - peer-reviewed
  • 4
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    Precise determination of delta Sr-88/86 in natural samples by double-spike MC-ICP-MS and its TIMS verification (2013)
    Royal Society of Chemistry
    In:  Journal of Analytical Atomic Spectrometry, 28 (6). p. 940.
    Details
    Publication Date: 2017-06-09
    Description: delta Sr-88/86 values of standards and a variety of natural samples were measured by MC-ICP-MS using the double-spike (DS) method and compared to results obtained by the standard-sample-bracketing (SSB) method and to DS-TIMS measurements. The external reproducibility of the SRM987 measurements carried out by DS-MC-ICP-MS was 0.021 parts per thousand (1SD), slightly better than previously published DS-TIMS and SSB-MC-ICP-MS results. The value of the IAPSO seawater standard (0.388 +/- 0.018; 2SEM) agrees with the results of the current SSB and DS-TIMS measurements and with previously published values. Using these values a variance-weighted mean for seawater was calculated (0.387 +/- 0.002, 2SEM). Compared to measurements carried out by the SSB method, natural sample measurements by the DS method are more accurate and more precise. An excellent agreement between DS-MC-ICP-MS and DS-TIMS methods was demonstrated for delta Sr-88/86 determination in natural samples over a range of similar to 0.5 parts per thousand. The DS-TIMS delta Sr-88/86 results had a smaller standard error than the DS-MC-ICP-MS measurements but required a much longer acquisition time
    Type: Article , PeerReviewed
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    DOI: 10.1039/c3ja50039j
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  • 5
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    An alternative data acquisition and evaluation strategy for improved isotope ratio precision using LA-MC-ICP-MS applied to stable and radiogenic strontium isotopes in carbonates (2008)
    Royal Society of Chemistry
    In:  Journal of Analytical Atomic Spectrometry, 23 (7). pp. 955-961.
    Details
    Publication Date: 2017-06-07
    Description: Strontium isotopes in various marine carbonates were determined using an “AXIOM” MC-ICP-MS in combination with a NewWave UP193 laser ablation unit. Using a modified measurement and data reduction strategy, an external reproducibility of 87Sr/86Sr ratios in carbonates of about 19 ppm (RSD) was achieved. For recent and sub-recent marine carbonates a mean radiogenic strontium isotope ratio 87Sr/86Sr of 0.709170 ± 0.000007 (2SE) was determined, which agrees well with the value of 0.7091741 ± 0.0000024 (2SE) reported for modern sea water (J. M. McArthur, D. Rio, F. Massari, D. Castrodi, T. R. Bailey, M. Thirlwall and S. Houghton, Palaeogeogr. Palaeoclimatol. Palaeoeco., 2006, 242(126), 2006). Compared to published laser-based methods, an improved accuracy and precision was achieved by applying a new data reduction protocol using the simultaneous responses of all isotopes measured. The latter is considered as a new principal approach for isotope ratio evaluation using LA-MC-ICP-MS. A major advantage of the presented method is the direct determination of the stable strontium isotope fractionation. Providing reproducible sample ablation, introduction into the plasma and stable plasma condition, this method excludes the efforts of a quantitative strontium recovery after ion chromatographic separation to avoid additional fractionation of the sample strontium due to chemical pre-treatment/separation (ion chromatography and solution preparation), and is therefore, together with the quicker sample preparation and spatially resolved analysis, advantageous when compared to published solution–nebulization bracketing-standard MC-ICP-MS methods for stable strontium isotope determination.
    Type: Article , PeerReviewed
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    DOI: 10.1039/B717706B
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  • 6
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    Boron isotope ratio determination in carbonates /via/ LA-MC-ICP-MS using soda-lime glass standards as reference material (2010)
    Royal Society of Chemistry
    In:  Journal of Analytical Atomic Spectrometry, 25 (12). pp. 1953-1957.
    Details
    Publication Date: 2019-09-24
    Description: A new in situ method using LA-MC-ICP-MS (193 nm excimer laser) for the determination of stable boron isotope ratios (δ11B) in carbonates was developed. Data were acquired via a standard sample standard bracketing procedure typically providing a reproducibility of 0.5‰ (SD) for samples containing 35 ppm of boron. A single ablation interval consumed about 5 µg of sample corresponding to about 0.2 ng of boron. The major finding was the similar instrumental fractionation behaviour of carbonates, soda-lime glass and sea salt with respect to boron isotopes. As no matrix induced offset was detectable between these distinct materials we propose the use of NIST glasses as internal standards for boron isotope ratio measurements via LA-MC-ICP-MS. This finding overcomes the problem of a missing matrix matched carbonate standard for in situ boron isotope studies. As a first application a set of coral samples from a culturing experiment was analysed. δ11B values range from 19.5 to 25‰ depending on the pH of the water used in the particular treatment. This is in good agreement with the results of earlier studies.
    Type: Article , PeerReviewed
    Format: text
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    DOI: 10.1039/C0JA00036A
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    OceanRep: Article in a Scientific Journal - peer-reviewed
  • 7
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    Determination of uranium isotope ratios by multi-static MIC-ICP-MS: method and implementation for precise U- and Th-series isotope measurements (2005)
    Royal Society of Chemistry
    In:  Journal of Analytical Atomic Spectrometry, 20 . pp. 395-401.
    Details
    Publication Date: 2017-05-31
    Description: In order to improve and extend the application of U- and Th-series isotope measurements a new technique for MIC-ICP-MS (multiple ion counting inductively coupled plasma mass spectrometry) was developed. This method uses either two (double MIC) or three (triple MIC) multipliers to measure in static mode in turn the U-isotopes 233U, 234U, 235U and 236U. For online internal standardization, mass bias correction and cross calibration of the multipliers a 233U/236U double spike was used. Applying this method the level of 1‰ 2σ internal precision is reached in less than 30 min, consuming less than 5 ng of total U. The multi-static MIC-ICP-MS method improves the precision by a factor of 5 for U isotope measurement compared with TIMS and by a factor of 2 compared with published ICP-MS methods. Repeated measurements of uranium CRM-145 (otherwise NBL 112A) were performed to test the reproducibility and accuracy of the method. An average 234U/238U value of (5.285 84 ± 0.000 87) × 10−5 or a δ234U value of −36.96 ± 0.16, respectively, was determined for CRM-145 in good agreement with reference data. Based on the precisely determined U isotope ratios we furthermore developed a combined multi-static U- and Th-measurement method. This approach extends this new MIC-ICP-MS technique to those U- and Th-series isotope systems having no constant isotope ratio for normalization (e.g., 230Th/232Th, 230Th/229Th) and is the key for new approaches to determining 226Ra/228Ra and 231Pa/233Pa. The applicability of the methods presented here is demonstrated by accurate dating of very young corals (10–350 y).
    Type: Article , PeerReviewed
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    DOI: 10.1039/b415958f
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  • 8
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    Separation of Mg, Ca and Fe from geological reference materials for stable isotope ratio analyses by MC-ICP-MS and double-spike TIMS (2009)
    Royal Society of Chemistry
    In:  Journal of Analytical Atomic Spectrometry, 24 . pp. 627-636.
    Details
    Publication Date: 2017-06-09
    Description: Near quantitative separation of analyte elements from the sample matrix is commonly required to obtain precise and accurate stable isotope data, especially if MC-ICP-MS is used in conjunction with the standard-sample bracketing (SSB) technique for mass bias drift correction. Here, we report a robust procedure that allows for the combined chemical separation of Mg, Ca and Fe, using ion-exchange columns that contain 1 ml AG50W-X8 (200-400 mesh) cation exchange resin. Magnesium was separated for isotope ratio analyses from many geological sample types by a single pass through this column. For Mg purification, Be, Ti, Mn, Fe and Al are selectively eluted using dilute HF and an acetone-HCl mixture. The separation of Mg from Ca-dominated carbonate samples and/or a combination of Mg, Ca and Fe separation from the same sample aliquot, is achieved by the adsorption of Ca and Fe onto the ion-exchange resin from 10 M HCl. Following purification, geological reference materials, including water, bone, carbonate and sediment samples, igneous and sedimentary rocks and a chondritic meteorite were analysed by MC-ICP-MS (Mg and Fe isotopes) and double-spike TIMS (Ca isotopes). Average external repeatabilities were +/-0.16 parts per thousand for Mg-26/Mg-24, +/-0.26 parts per thousand for Ca-44/Ca-40 and +/-0.05 parts per thousand for Fe-56/Fe-54 (2sd; n >= 5). Comparison with published data documents the accuracy of the results. For Mg isotope analyses using SSB-MC-ICP-MS, matrix-induced mass bias effects were studied using element additions. The artificial matrices left a memory in subsequent standard analyses, likely due to depositions on the cones. This observation allowed for the detection of matrix effects in unknown samples. Finally, the current status of Mg and Ca zero-delta reference materials is briefly discussed.
    Type: Article , PeerReviewed
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    DOI: 10.1039/b820154d
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    OceanRep: Article in a Scientific Journal - peer-reviewed
  • 9
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    No detectable Weddell Sea Antarctic Bottom Water export during the Last and Penultimate Glacial Maximum (2020)
    Nature Research
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    Publication Date: 2023-02-08
    Description: Weddell Sea-derived Antarctic Bottom Water (AABW) is one of the most important deep water masses in the Southern Hemisphere occupying large portions of the deep Southern Ocean (SO) today. While substantial changes in SO-overturning circulation were previously suggested, the state of Weddell Sea AABW export during glacial climates remains poorly understood. Here we report seawater-derived Nd and Pb isotope records that provide evidence for the absence of Weddell Sea-derived AABW in the Atlantic sector of the SO during the last two glacial maxima. Increasing delivery of Antarctic Pb to regions outside the Weddell Sea traced SO frontal displacements during both glacial terminations. The export of Weddell Sea-derived AABW resumed late during glacial terminations, coinciding with the last major atmospheric CO2 rise in the transition to the Holocene and the Eemian. Our new records lend strong support for a previously inferred AABW overturning stagnation event during the peak Eemian interglacial.
    Type: Article , PeerReviewed
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  • 10
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    Permian–Triassic mass extinction pulses driven by major marine carbon cycle perturbations (2020)
    Nature Research
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    Publication Date: 2023-02-08
    Description: The Permian/Triassic boundary approximately 251.9 million years ago marked the most severe environmental crisis identified in the geological record, which dictated the onwards course for the evolution of life. Magmatism from Siberian Traps is thought to have played an important role, but the causational trigger and its feedbacks are yet to be fully understood. Here we present a new boron-isotope-derived seawater pH record from fossil brachiopod shells deposited on the Tethys shelf that demonstrates a substantial decline in seawater pH coeval with the onset of the mass extinction in the latest Permian. Combined with carbon isotope data, our results are integrated in a geochemical model that resolves the carbon cycle dynamics as well as the ocean redox conditions and nitrogen isotope turnover. We find that the initial ocean acidification was intimately linked to a large pulse of carbon degassing from the Siberian sill intrusions. We unravel the consequences of the greenhouse effect on the marine environment, and show how elevated sea surface temperatures, export production and nutrient input driven by increased rates of chemical weathering gave rise to widespread deoxygenation and sporadic sulfide poisoning of the oceans in the earliest Triassic. Our findings enable us to assemble a consistent biogeochemical reconstruction of the mechanisms that resulted in the largest Phanerozoic mass extinction.
    Type: Article , PeerReviewed , info:eu-repo/semantics/article
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