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  • 1
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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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  • 2
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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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  • 3
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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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  • 4
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    No detectable Weddell Sea Antarctic Bottom Water export during the Last and Penultimate Glacial Maximum (2020)
    Nature Research
    Details
    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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  • 5
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    Permian–Triassic mass extinction pulses driven by major marine carbon cycle perturbations (2020)
    Nature Research
    Details
    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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  • 6
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    Determination of radiogenic and stable strontium isotope ratios (87Sr/86Sr; δ88/86Sr) by thermal ionization mass spectrometry applying an 87Sr/84Sr double spike (2009)
    Royal Society of Chemistry
    In:  Journal of Analytical Atomic Spectrometry, 24 (9). pp. 1267-1271.
    Details
    Publication Date: 2021-07-05
    Description: Recent findings of natural strontium isotope fractionation have opened up a new field of research in non-traditional stable isotope geochemistry. While previous studies were based on data obtained by MC-ICP-MS we here present a novel approach combining thermal ionization mass spectrometry (TIMS) with the use of an 87Sr/84Sr double spike (DS). Our results for the IAPSO sea water and JCp-1 coral standards, respectively, are in accord with previously published data. The strontium isotope composition of the IAPSO sea water standard was determined as δ88/86Sr = 0.386(5)‰ (δ values relative to the SRM987), 87Sr/86Sr* = 0.709312(9) n = 10 and a corresponding conventionally normalized 87Sr/86Sr = 0.709168(7) (all uncertainties 2SEM). For the JCp-1 coral standard we obtained δ88/86Sr = 0.197(8)‰, 87Sr/86Sr* = 0.709237(2) and 87Sr/86Sr = 0.709164(5) n = 3. We show that by applying this DS-TIMS method the precision is improved by at least a factor of 2–3 when compared to MC-ICP-MS.
    Type: Article , PeerReviewed
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    DOI: 10.1039/b906292k
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  • 7
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    A simplified procedure for the determination of stable chlorine isotope ratios (δ37Cl) using LA-MC-ICP-MS (2008)
    Royal Society of Chemistry
    In:  Journal of Analytical Atomic Spectrometry, 23 (5). pp. 769-772.
    Details
    Publication Date: 2019-09-23
    Description: Stable chlorine isotopes (37Cl, 35Cl) are considered as important tracers of geochemical processes, especially in subduction zone systems. However, high-quality chlorine isotope data are scarcely available. Here we present a comparatively simple procedure for the precise and accurate determination of stable chlorine isotope ratios (δ37Cl) using LA-MC-ICP-MS. Chlorine was extracted from solid samples by pyrohydrolysis. After quantitative precipitation as AgCl the dried precipitates where analysed in a sample-standard bracketing approach using a weak laser ablation (0.3 J/cm2) for sample evaporation. Atlantic Ocean sea salt and the sea water standard IAPSO were used as SMOC (standard mean ocean chloride) for normalisation (δ37Cl = 0 ‰). The precision and accuracy of the presented method was validated analysing the reference materials JB-1a and JB-2. The chlorine isotope ratios of these standards were determined as δ37ClJB-1a = (−0.99 ± 0.06) ‰ and δ37ClJB-2 = (−0.60 ± 0.03) ‰ (errors 2SE), respectively, in accordance with published data. Applying the presented method a total amount of less than 1 μg of chlorine was consumed during a typical measurement including 10 ablation periods on the sample.
    Type: Article , PeerReviewed
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    DOI: 10.1039/b718597a
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  • 8
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    No freshwater-filled glacial Arctic Ocean (2022)
    Nature Research
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    Publication Date: 2024-02-07
    Type: Article , PeerReviewed
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  • 9
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    Groundwater discharge impacts marine isotope budgets of Li, Mg, Ca, Sr, and Ba (2021)
    Nature Research
    Details
    Publication Date: 2024-02-07
    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.
    Type: Article , PeerReviewed
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  • 10
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    Modern and sub-fossil corals suggest reduced temperature variability in the eastern pole of the Indian Ocean Dipole during the medieval climate anomaly (2021)
    Nature Research
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    Publication Date: 2024-02-07
    Description: We present two 40 year records of monthly coral Sr/Ca ratios from the eastern pole of the Indian Ocean Dipole. A modern coral covers the period from 1968 to 2007. A sub-fossil coral derives from the medieval climate anomaly (MCA) and spans 1100–1140 ad. The modern coral records SST variability in the eastern pole of the Indian Ocean Dipole. A strong correlation is also found between coral Sr/Ca and the IOD index. The correlation with ENSO is asymmetric: the coral shows a moderate correlation with El Niño and a weak correlation with La Niña. The modern coral shows large interannual variability. Extreme IOD events cause cooling 〉 3 °C (1994, 1997) or ~ 2 °C (2006). In total, the modern coral indicates 32 warm/cool events, with 16 cool and 16 warm events. The MCA coral shows 24 warm/cool events, with 14 cool and 10 warm events. Only one cool event could be comparable to the positive Indian Ocean Dipole in 2006. The seasonal cycle of the MCA coral is reduced (〈 50% of to the modern) and the skewness of the Sr/Ca data is lower. This suggests a deeper thermocline in the eastern Indian Ocean associated with a La Niña-like mean state in the Indo-Pacific during the MCA.
    Type: Article , PeerReviewed
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