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  • 11
    Publication Date: 2022-11-10
    Description: © The Author(s), 2022. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in van Beek, P., François, R., Honda, M., Charette, M., Reyss, J.-L., Ganeshram, R., Monnin, C., & Honjo, S. Fractionation of 226Ra and Ba in the upper North Pacific Ocean. Frontiers in Marine Science, 9, (2022): 859117, https://doi.org/10.3389/fmars.2022.859117.
    Description: Investigations conducted during the GEOSECS program concluded that radium-226 (T1/2 = 1602 y) and barium are tightly correlated in waters above 2500 m in the Atlantic, Pacific and Antarctic Oceans, with a fairly uniform 226Ra/Ba ratio of 2.3 ± 0.2 dpm µmol-1 (4.6 nmol 226Ra/mol Ba). Here, we report new 226Ra and Ba data obtained at three different stations in the Pacific Ocean: stations K1 and K3 in the North-West Pacific and station old Hale Aloha, off Hawaii Island. The relationship between 226Ra and Ba found at these stations is broadly consistent with that reported during the GEOSECS program. At the three investigated stations, however, we find that the 226Ra/Ba ratios are significantly lower in the upper 500 m of the water column than at greater depths, a pattern that was overlooked during the GEOSECS program, either because of the precision of the measurements or because of the relatively low sampling resolution in the upper 500 m. Although not always apparent in individual GEOSECS profiles, this trend was noted before from the non-zero intercept of the linear regression when plotting the global data set of Ba versus 226Ra seawater concentration and was attributed, at least in part, to the predominance of surface input from rivers for Ba versus bottom input from sediments for 226Ra. Similarly, low 226Ra/Ba ratios in the upper 500 m have been reported in other oceanic basins (e.g. Atlantic Ocean). Parallel to the low 226Ra/Ba ratios in seawater, higher 226Ra/Ba ratios were found in suspended particles collected in the upper 500 m. This suggests that fractionation between the two elements may contribute to the lower 226Ra/Ba ratios found in the upper 500 m, with 226Ra being preferentially removed from surface water, possibly as a result of mass fractionation during celestite formation by acantharians and/or barite precipitation, since both chemical elements have similar ionic radius and the same configuration of valence electrons. This finding has implications for dating of marine carbonates by 226Ra, which requires a constant initial 226Ra/Ba ratio incorporated in the shells and for using 226Ra as an abyssal circulation and mixing tracer.
    Description: This work was supported by a Lavoisier fellowship attributed by the French Ministry of Foreign Affairs to PB in year 2002 and by the Woods Hole Oceanographic Institution (WHOI). This work was completed at the University of Edinburgh in 2003, while PB was a postdoctoral fellow there, with a Marie Curie fellowship from the European Union. The European Union is thus also thanked. MC acknowledges support from the National Science Foundation, Chemical Oceanography program.
    Keywords: Radium ; Barium ; Seawater ; Ratio ; Fractionation ; Dating ; Ocean circulation ; Suspended particles
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 12
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2020. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research-Oceans 125(4), (2020): e2019JC015544, doi:10.1029/2019JC015544.
    Description: The Radium Delayed Coincidence Counter (RaDeCC) is one of the most extensively used equipment for measuring 223Ra and 224Ra activities in water and sediment samples. Samples are placed in a closed He‐circulation system that carries the Rn produced by the decay of Ra to a scintillation cell. Each alpha decay recorded in the cell is routed to an electronic delayed coincidence system which enables the discrimination of 223Ra and 224Ra. In this study, the measurement and quantification methods using the RaDeCC system are assessed through analyses of registered data in different RaDeCC systems worldwide and a set of simulations. Results of this work indicate that the equations used to correct for 223Ra and 224Ra cross‐talk interferences are only valid for a given range of activities and ratios between isotopes. Above certain limits that are specified in this study, these corrections may significantly overestimate the quantification of 223Ra and 224Ra activities (up to ~40% and 30%, respectively), as well as the quantification of their parents 227Ac and 228Th. High activities of 226Ra may also produce an overestimation of 224Ra activities due to the buildup of 222Rn, especially when long measurements with low activities of 224Ra are performed. An improved method to quantify 226Ra activities from the buildup of 222Rn with the RaDeCC system is also developed in this study. Wethus provide a new set of guidelines for the appropriate quantification of 223Ra, 224Ra, 227Ac, 228Th, and 226Ra with the RaDeCC system.
    Description: The authors acknowledge the support from the Generalitat de Catalunya autonomous government through its funding schema to excellence research groups (grants 2017 SGR 1588 and 2014 SGR 1356) and the support from Spanish Government (projects CGL2013‐48869‐C2‐1‐R/2‐R and CGL2016‐77122‐C2‐1‐576 R/2‐R). We would like to thank all the people who contributed to this work sharing the data of their RaDeCC systems, including J. Scholten, C. Claude, M.A. Charette, J.K. Cochran, and R. Neuholz. We want to express our gratitude to our colleagues from the Laboratori de Radioactivitat Ambiental (Universitat Autònoma de Barcelona) and Dr. W. Geibert (AWI) for improving the quality of this work. A. Alorda‐Kleinglass acknowledges financial support from ICTA “Unit of Excellence” (MinECo, MDM2015‐0552‐17‐1)PhD fellowship, BES‐2017‐080740. Dr. V. Rodellas acknowledges financial support from the Beatriu de Pinós postdoctoral program of the Generalitat de Catalunya autonomous government (2017‐BP‐00334). P. van Beek thanks the support from ANR (MED‐SGD project, ANR‐15‐CE01‐0004). M. Diego‐Feliu acknowledges the economic support from the FI‐2017 fellowships of the Generalitat de Catalunya autonomous government (2017FI_B_00365). Compliance with AGU's DataPolicy: All the https://data.mendeley.com/datasets/jtct7mt8zr/2 codes and spreadsheets used in this article are provided online (supplementary material).
    Description: 2020-09-27
    Keywords: RaDeCC ; Ra isotopes ; quantification ; U/Th series ; submarine groundwater discharge
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 13
    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 Rodellas, V., Stieglitz, T. C., Tamborski, J. J., van Beek, P., Andrisoa, A., & Cook, P. G. Conceptual uncertainties in groundwater and porewater fluxes estimated by radon and radium mass balances. Limnology and Oceanography, (2021), https://doi.org/10.1002/lno.11678.
    Description: Radium isotopes and radon are routinely used as tracers to quantify groundwater and porewater fluxes into coastal and freshwater systems. However, uncertainties associated with the determination of the tracer flux are often poorly addressed and often neglect all the potential errors associated with the conceptualization of the system (i.e., conceptual uncertainties). In this study, we assess the magnitude of some of the key uncertainties related to the determination of the radium and radon inputs supplied by groundwater and porewater fluxes into a waterbody (La Palme Lagoon, France). This uncertainty assessment is addressed through a single model ensemble approach, where a tracer mass balance is run multiple times with variable sets of assumptions and approaches for the key parameters determined through a sensitivity test. In particular, conceptual uncertainties linked to tracer concentration, diffusive fluxes, radon evasion to the atmosphere, and change of tracer inventory over time were considered. The magnitude of porewater fluxes is further constrained using a comparison of independent methods: (1) 224Ra and (2) 222Rn mass balances in overlying waters, (3) a model of 222Rn deficit in sediments, and (4) a fluid‐salt numerical transport model. We demonstrate that conceptual uncertainties are commonly a major source of uncertainty on the estimation of groundwater or porewater fluxes and they need to be taken into account when using tracer mass balances. In the absence of a general framework for assessing these uncertainties, this study provides a practical approach to evaluate key uncertainties associated to radon and radium mass balances.
    Description: This research is a contribution to the ANR @RAction chair (ANR‐14‐ACHN‐0007‐01—T Stieglitz) and Labex OT‐Med (ANR‐11‐LABEX‐0061, part of the “Investissements d'Avenir” program through the A*MIDEX project ANR‐11‐IDEX‐0001‐02) funded by the French National Research Agency (ANR). This project has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska‐Curie grant 748896. V. Rodellas acknowledges financial support from the Beatriu de Pinós postdoctoral programme of the Catalan Government (2017‐BP‐00334). P. van Beek acknowledges financial support from the ANR (MED‐SGD project, ANR‐15‐CE01‐0004). We thank S. Thomas (Labex OT‐Med) for constructive comments and M. Diego‐Feliu for his help on statistical analysis. This study contributes to the work carried out by the MERS research group 2017‐SGR‐1588.
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 14
    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Garcia-Orellana, J., Rodellas, V., Tamborski, J., Diego-Feliu, M., van Beek, P., Weinstein, Y., Charette, M., Alorda-Kleinglass, A., Michael, H. A., Stieglitz, T., & Scholten, J. Radium isotopes as submarine groundwater discharge (SGD) tracers: review and recommendations. Earth-Science Reviews, 220, (2021): 103681, https://doi.org/10.1016/j.earscirev.2021.103681.
    Description: Submarine groundwater discharge (SGD) is now recognized as an important process of the hydrological cycle worldwide and plays a major role as a conveyor of dissolved compounds to the ocean. Naturally occurring radium isotopes (223Ra, 224Ra, 226Ra and 228Ra) are widely employed geochemical tracers in marine environments. Whilst Ra isotopes were initially predominantly applied to study open ocean processes and fluxes across the continental margins, their most common application in the marine environment has undoubtedly become the identification and quantification of SGD. This review focuses on the application of Ra isotopes as tracers of SGD and associated inputs of water and solutes to the coastal ocean. In addition, we review i) the processes controlling Ra enrichment and depletion in coastal groundwater and seawater; ii) the systematics applied to estimate SGD using Ra isotopes and iii) we summarize additional applications of Ra isotopes in groundwater and marine studies. We also provide some considerations that will help refine SGD estimates and identify the critical knowledge gaps and research needs related to the current use of Ra isotopes as SGD tracers.
    Description: J.Garcia-Orellana acknowledges the financial support of the Spanish Ministry of Science, Innovation and Universities, through the “Maria de Maeztu” programme for Units of Excellence (CEX2019-000940-M), the Generalitat de Catalunya (MERS; 2017 SGR – 1588) and the project OPAL (PID2019-110311RB-C21). V. Rodellas acknowledges financial support from the Beatriu de Pinós postdoctoral program of the Generalitat de Catalunya (2017-BP-00334 and 2019-BP-00241). M. Charette received support from the U.S. National Science Foundation (OCE-1736277). J. Scholten acknowledges the support through the SEAMOUNT BONUS project (art. 185), which is funded jointly by the EU and the Federal Ministry of Education and Research of Germany (BMBF, grant no. 03F0771B). P. van Beek and T. Stieglitz acknowledge support from the French ANR project MED-SGD (ANR-15-01CE-0004) and chair @RAction MED-LOC (ANR-14-ACHN-0007-01). A. Alorda-Kleinglass acknowledges financial support from ICTA “Unit of Excellence” (MinECo, MDM2015-0552-17-1) and PhD fellowship, BES-2017-080740. H. Michael acknowledges support from the U.S. National Science Foundation (EAR-1759879). M. Diego-Feliu acknowledges the financial support from the FI-2017 fellowships of the Generalitat de Catalunya (2017-FIB-00365). Fig. 3, Fig. 4, Fig. 7, Fig. 12 were designed by Gemma Solà (www.gemmasola.com).
    Repository Name: Woods Hole Open Access Server
    Type: Article
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