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ArticleRadium isotopes as submarine groundwater discharge (SGD) tracers: review and recommendations(Elsevier, 2021-05-14) Garcia-Orellana, Jordi ; Rodellas, Valenti ; Tamborski, Joseph ; Diego-Feliu, Marc ; van Beek, Pieter ; Weinstein, Yishai ; Charette, Matthew A. ; Alorda-Kleinglass, Aaron ; Michael, Holly A. ; Stieglitz, Thomas ; Scholten, Jan C.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.
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ArticleSr-90 and Sr-89 in seawater off Japan as a consequence of the Fukushima Dai-ichi nuclear accident(Copernicus Publications on behalf of the European Geosciences Union, 2013-06-03) Casacuberta, Nuria ; Masqué, Pere ; Garcia-Orellana, Jordi ; Garcia-Tenorio, R. ; Buesseler, Ken O.The impact of the earthquake and tsunami on the east coast of Japan on 11 March 2011 caused a loss of power at the Fukushima Dai-ichi nuclear power plant (NPP) that resulted in one of the most important releases of artificial radioactivity into the environment. Although several works were devoted to evaluating the atmospheric dispersion of radionuclides, the impact of the discharges to the ocean has been less investigated. Here we evaluate the distribution of Fukushima-derived 90Sr (n = 57) and 89Sr (n = 19) throughout waters 30–600 km offshore in June 2011. Concentrations of 90Sr and 89Sr in both surface waters and shallow profiles ranged from 0.8 ± 0.2 to 85 ± 3 Bq m−3 and from 19 ± 6 to 265 ± 74 Bq m−3, respectively. Because of its short half-life, all measured 89Sr was due to the accident, while the 90Sr concentrations can be compared to the background levels in the Pacific Ocean of about 1.2 Bq m−3. Fukushima-derived radiostrontium was mainly detected north of Kuroshio Current, as this was acting as a southern boundary for transport. The highest activities were associated with near-shore eddies, and larger inventories were found in the closest stations to Fukushima NPP. The data evidence a major influence of direct liquid discharges of radiostrontium compared to the atmospheric deposition. Existing 137Cs data reported from the same samples allowed us to establish a 90Sr / 137Cs ratio of 0.0256 ± 0.0006 in seawater off Fukushima, being significantly different than that of the global atmospheric fallout (i.e., 0.63) and may be used in future studies to track waters coming from the east coast of Japan. Liquid discharges of 90Sr to the ocean were estimated, resulting in an inventory of 53 ± 1 TBq of 90Sr in the inshore study area in June 2011 and total releases of 90Sr ranging from 90 to 900 TBq, depending upon the reported estimates of 137Cs releases that are considered.
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PreprintDistribution of Pb-210 and Po-210 in the arctic water column during the 2007 sea-ice minimum: Particle export in the ice-covered basins.(Elsevier, 2018-10-22) Roca-Martí, Montserrat ; Puigcorbé, Viena ; Friedrich, Jana ; Rutgers van der Loeff, Michiel ; Rabe, Benjamin ; Korhonen, Meri ; Cámara Mor, Patricia ; Garcia-Orellana, Jordi ; Masqué, Pere210Pb and 210Po are naturally occurring radionuclides that are commonly used as a proxy for particle and carbon export. In this study, the distribution of the 210Po/210Pb pair was investigated in the water column of the Barents, Kara and Laptev Seas and the Nansen, Amundsen and Makarov Basins in order to understand the particle dynamics in the Arctic Ocean during the 2007 sea-ice minimum (August-September). Minimum activities of total 210Pb and 210Po were found in the upper and lower haloclines (approx. 60-130 m), which are partly attributed to particle scavenging over the shelves, boundary current transport and subsequent advection of the water with low 210Pb and 210Po activities into the central Arctic. Widespread and substantial (>50%) deficits of 210Po with respect to 210Pb were detected from surface waters to 200 m on the shelves, but also in the basins. This was particularly important in the Makarov Basin where, despite very low chlorophyll-a levels, estimates of annual new primary production were three times higher than in the Eurasian Basin. In the Nansen, Amundsen and Makarov 32 Basins, estimates of annual new primary production correlated with the deficits of 210Po in the upper 200 m of the water column, suggesting that in situ production and subsequent export of biogenic material were the mechanisms that controlled the removal of 210Po in the central Arctic. Unlike 210Po, 234Th deficits measured during the same expedition were found to be very small and not significant below 25 m in the basins (Cai et al., 2010), which indicates, given the shorter half-life of 234Th, that particle export fluxes in the central Arctic would have been higher before July-August in 2007 than later in the season.
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ArticleGuidelines and limits for the quantification of ra isotopes and related radionuclides with the radium delayed coincidence counter (RaDeCC)(American Geophysical Union, 2020-03-27) Diego-Feliu, Marc ; Rodellas, Valenti ; Alorda-Kleinglass, Aaron ; Tamborski, Joseph ; van Beek, Pieter ; Heins, L. ; Bruach, Joan Manuel ; Arnold, Ralph ; Garcia-Orellana, JordiThe 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.
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ArticleQuantifying Po-210/Pb-210 disequilibrium in seawater: a comparison of two precipitation methods with differing results(Frontiers Media, 2021-06-22) Roca-Martí, Montserrat ; Puigcorbé, Viena ; Castrillejo, Maxi ; Casacuberta, Nuria ; Garcia-Orellana, Jordi ; Cochran, J. Kirk ; Masqué, PereThe disequilibrium between lead-210 (210Pb) and polonium-210 (210Po) is increasingly used in oceanography to quantify particulate organic carbon (POC) export from the upper ocean. This proxy is based on the deficits of 210Po typically observed in the upper water column due to the preferential removal of 210Po relative to 210Pb by sinking particles. Yet, a number of studies have reported unexpected large 210Po deficits in the deep ocean indicating scavenging of 210Po despite its radioactive mean life of ∼ 200 days. Two precipitation methods, Fe(OH)3 and Co-APDC, are typically used to concentrate Pb and Po from seawater samples, and deep 210Po deficits raise the question whether this feature is biogeochemically consistent or there is a methodological issue. Here, we present a compilation of 210Pb and 210Po studies that suggests that 210Po deficits at depths >300 m are more often observed in studies where Fe(OH)3 is used to precipitate Pb and Po from seawater, than in those using Co-APDC (in 68 versus 33% of the profiles analyzed for each method, respectively). In order to test whether 210Po/210Pb disequilibrium can be partly related to a methodological artifact, we directly compared the total activities of 210Pb and 210Po in four duplicate ocean depth-profiles determined by using Fe(OH)3 and Co-APDC on unfiltered seawater samples. While both methods produced the same 210Pb activities, results from the Co-APDC method showed equilibrium between 210Pb and 210Po below 100 m, whereas the Fe(OH)3 method resulted in activities of 210Po significantly lower than 210Pb throughout the entire water column. These results show that 210Po deficits in deep waters, but also in the upper ocean, may be greater when calculated using a commonly used Fe(OH)3 protocol. This finding has potential implications for the use of the 210Po/210Pb pair as a tracer of particle export in the oceans because 210Po (and thus POC) fluxes calculated using Fe(OH)3 on unfiltered seawater samples may be overestimated. Recommendations for future research are provided based on the possible reasons for the discrepancy in 210Po activities between both analytical methods.
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ArticleRadium mass balance sensitivity analysis for submarine groundwater discharge estimation in semi-enclosed basins: the case study of Long Island Sound(Frontiers Media, 2020-07-17) Tamborski, Joseph ; Cochran, J. Kirk ; Bokuniewicz, Henry J. ; Heilbrun, Christina ; Garcia-Orellana, Jordi ; Rodellas, Valenti ; Wilson, RobertEstimation of submarine groundwater discharge (SGD) to semi-enclosed basins by Ra isotope mass balance is herein assessed. We evaluate 224Ra, 226Ra, and 228Ra distributions in surface and bottom waters of Long Island Sound (CT-NY, United States) collected during spring 2009 and summer 2010. Surface water and bottom water Ra activities display an apparent seasonality, with greater activities during the summer. Long-lived Ra isotope mass balances are highly sensitive to boundary fluxes (water flux and Ra activity). Variation (50%) in the 224Ra, 226Ra, and 228Ra offshore seawater activity results in a 63–74% change in the basin-wide 226Ra SGD flux and a 58–60% change in the 228Ra SGD flux, but only a 4–9% change in the 224Ra SGD flux. This highlights the need to accurately constrain long-lived Ra activities in the inflowing and outflowing water, as well as water fluxes across boundaries. Short-lived Ra isotope mass balances are sensitive to internal Ra fluxes, including desorption from resuspended particles and inputs from sediment diffusion and bioturbation. A 50% increase in the sediment diffusive flux of 224Ra, 226Ra, and 228Ra results in a ∼30% decrease in the 224Ra SGD flux, but only a ∼6–10% decrease in the 226Ra and 228Ra SGD flux. When boundary mixing is uncertain, 224Ra is the preferred tracer of SGD if sediment contributions are adequately constrained. When boundary mixing is well-constrained, 226Ra and 228Ra are the preferred tracers of SGD, as sediment contributions become less important. A three-dimensional numerical model is used to constrain boundary mixing in Long Island Sound (LIS), with mean SGD fluxes of 1.2 ± 0.9 × 1013 L y–1 during spring 2009 and 3.3 ± 0.7 × 1013 L y–1 during summer 2010. The SGD flux to LIS during summer 2010 was one order of magnitude greater than the freshwater inflow from the Connecticut River. The maximum marine SGD-driven N flux is 14 ± 11 × 108 mol N y–1 and rivals the N load of the Connecticut River.
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ArticleCoastal ocean and shelf-sea biogeochemical cycling of trace elements and isotopes : lessons learned from GEOTRACES(The Royal Society, 2016-10-17) Charette, Matthew A. ; Lam, Phoebe J. ; Lohan, Maeve C. ; Kwon, Eun Young ; Hatje, Vanessa ; Jeandel, Catherine ; Shiller, Alan M. ; Cutter, Gregory A. ; Thomas, Alex ; Boyd, Philip ; Homoky, William B. ; Milne, Angela ; Thomas, Helmuth ; Andersson, Per S. ; Porcelli, Don ; Tanaka, Takahiro ; Geibert, Walter ; Dehairs, Frank ; Garcia-Orellana, JordiContinental shelves and shelf seas play a central role in the global carbon cycle. However, their importance with respect to trace element and isotope (TEI) inputs to ocean basins is less well understood. Here, we present major findings on shelf TEI biogeochemistry from the GEOTRACES programme as well as a proof of concept for a new method to estimate shelf TEI fluxes. The case studies focus on advances in our understanding of TEI cycling in the Arctic, transformations within a major river estuary (Amazon), shelf sediment micronutrient fluxes and basin-scale estimates of submarine groundwater discharge. The proposed shelf flux tracer is 228-radium (T1/2 = 5.75 yr), which is continuously supplied to the shelf from coastal aquifers, sediment porewater exchange and rivers. Model-derived shelf 228Ra fluxes are combined with TEI/ 228Ra ratios to quantify ocean TEI fluxes from the western North Atlantic margin. The results from this new approach agree well with previous estimates for shelf Co, Fe, Mn and Zn inputs and exceed published estimates of atmospheric deposition by factors of approximately 3–23. Lastly, recommendations are made for additional GEOTRACES process studies and coastal margin-focused section cruises that will help refine the model and provide better insight on the mechanisms driving shelf-derived TEI fluxes to the ocean.
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ArticleThe GEOTRACES Intermediate Data Product 2017(Elsevier, 2018-06-01) Schlitzer, Reiner ; Anderson, Robert F. ; Dodas, Elena Masferrer ; Lohan, Maeve C. ; Geibert, Walter ; Tagliabue, Alessandro ; Bowie, Andrew R. ; Jeandel, Catherine ; Maldonado, Maria T. ; Landing, William M. ; Cockwell, Donna ; Abadie, Cyril ; Abouchami, Wafa ; Achterberg, Eric P. ; Agather, Alison ; Aguliar-Islas, Ana ; van Aken, Hendrik M. ; Andersen, Morten ; Archer, Corey ; Auro, Maureen E. ; Baar, Hein J. W. de ; Baars, Oliver ; Baker, Alex R. ; Bakker, Karel ; Basak, Chandranath ; Baskaran, Mark ; Bates, Nicholas R. ; Bauch, Dorothea ; van Beek, Pieter ; Behrens, Melanie K. ; Black, Erin E. ; Bluhm, Katrin ; Bopp, Laurent ; Bouman, Heather ; Bowman, Katlin ; Bown, Johann ; Boyd, Philip ; Boye, Marie ; Boyle, Edward A. ; Branellec, Pierre ; Bridgestock, Luke ; Brissebrat, Guillaume ; Browning, Thomas A. ; Bruland, Kenneth W. ; Brumsack, Hans-Jürgen ; Brzezinski, Mark A. ; Buck, Clifton S. ; Buck, Kristen N. ; Buesseler, Ken O. ; Bull, Abby ; Butler, Edward ; Cai, Pinghe ; Cámara Mor, Patricia ; Cardinal, Damien ; Carlson, Craig ; Carrasco, Gonzalo ; Casacuberta, Nuria ; Casciotti, Karen L. ; Castrillejo, Maxi ; Chamizo, Elena ; Chance, Rosie ; Charette, Matthew A. ; Chaves, Joaquin E. ; Cheng, Hai ; Chever, Fanny ; Christl, Marcus ; Church, Thomas M. ; Closset, Ivia ; Colman, Albert S. ; Conway, Tim M. ; Cossa, Daniel ; Croot, Peter L. ; Cullen, Jay T. ; Cutter, Gregory A. ; Daniels, Chris ; Dehairs, Frank ; Deng, Feifei ; Dieu, Huong Thi ; Duggan, Brian ; Dulaquais, Gabriel ; Dumousseaud, Cynthia ; Echegoyen-Sanz, Yolanda ; Edwards, R. Lawrence ; Ellwood, Michael J. ; Fahrbach, Eberhard ; Fitzsimmons, Jessica N. ; Flegal, A. Russell ; Fleisher, Martin Q. ; van de Flierdt, Tina ; Frank, Martin ; Friedrich, Jana ; Fripiat, Francois ; Fröllje, Henning ; Galer, Stephen J. G. ; Gamo, Toshitaka ; Ganeshram, Raja S. ; Garcia-Orellana, Jordi ; Garcia Solsona, Ester ; Gault-Ringold, Melanie ; George, Ejin ; Gerringa, Loes J. A. ; Gilbert, Melissa ; Godoy, Jose Marcus ; Goldstein, Steven L. ; Gonzalez, Santiago ; Grissom, Karen ; Hammerschmidt, Chad R. ; Hartman, Alison ; Hassler, Christel ; Hathorne, Ed C. ; Hatta, Mariko ; Hawco, Nicholas J. ; Hayes, Christopher T. ; Heimbürger, Lars-Eric ; Helgoe, Josh ; Heller, Maija Iris ; Henderson, Gideon M. ; Henderson, Paul B. ; van Heuven, Steven ; Ho, Peng ; Horner, Tristan J. ; Hsieh, Yu-Te ; Huang, Kuo-Fang ; Humphreys, Matthew P. ; Isshiki, Kenji ; Jacquot, Jeremy E. ; Janssen, David J. ; Jenkins, William J. ; John, Seth ; Jones, Elizabeth M. ; Jones, Janice L. ; Kadko, David ; Kayser, Rick ; Kenna, Timothy C. ; Khondoker, Roulin ; Kim, Taejin ; Kipp, Lauren ; Klar, Jessica K. ; Klunder, Maarten ; Kretschmer, Sven ; Kumamoto, Yuichiro ; Laan, Patrick ; Labatut, Marie ; Lacan, Francois ; Lam, Phoebe J. ; Lambelet, Myriam ; Lamborg, Carl H. ; le Moigne, Frederique ; Le Roy, Emilie ; Lechtenfeld, Oliver J. ; Lee, Jong-Mi ; Lherminier, Pascale ; Little, Susan ; López-Lora, Mercedes ; Lu, Yanbin ; Masque, Pere ; Mawji, Edward ; McClain, Charles R. ; Measures, Christopher I. ; Mehic, Sanjin ; Menzel Barraqueta, Jan-Lukas ; Merwe, Pier van der ; Middag, Rob ; Mieruch, Sebastian ; Milne, Angela ; Minami, Tomoharu ; Moffett, James W. ; Moncoiffe, Gwenaelle ; Moore, Willard S. ; Morris, Paul J. ; Morton, Peter L. ; Nakaguchi, Yuzuru ; Nakayama, Noriko ; Niedermiller, John ; Nishioka, Jun ; Nishiuchi, Akira ; Noble, Abigail E. ; Obata, Hajime ; Ober, Sven ; Ohnemus, Daniel C. ; van Ooijen, Jan ; O'Sullivan, Jeanette ; Owens, Stephanie A. ; Pahnke, Katharina ; Paul, Maxence ; Pavia, Frank ; Pena, Leopoldo D. ; Peters, Brian ; Planchon, Frederic ; Planquette, Helene ; Pradoux, Catherine ; Puigcorbé, Viena ; Quay, Paul D. ; Queroue, Fabien ; Radic, Amandine ; Rauschenberg, Sara ; Rehkämper, Mark ; Rember, Robert ; Remenyi, Tomas A. ; Resing, Joseph A. ; Rickli, Joerg ; Rigaud, Sylvain ; Rijkenberg, Micha J. A. ; Rintoul, Stephen R. ; Robinson, Laura F. ; Roca-Martí, Montserrat ; Rodellas, Valenti ; Roeske, Tobias ; Rolison, John M. ; Rosenberg, Mark ; Roshan, Saeed ; Rutgers van der Loeff, Michiel M. ; Ryabenko, Evgenia ; Saito, Mak A. ; Salt, Lesley ; Sanial, Virginie ; Sarthou, Geraldine ; Schallenberg, Christina ; Schauer, Ursula ; Scher, Howie ; Schlosser, Christian ; Schnetger, Bernhard ; Scott, Peter M. ; Sedwick, Peter N. ; Semiletov, Igor P. ; Shelley, Rachel U. ; Sherrell, Robert M. ; Shiller, Alan M. ; Sigman, Daniel M. ; Singh, Sunil Kumar ; Slagter, Hans ; Slater, Emma ; Smethie, William M. ; Snaith, Helen ; Sohrin, Yoshiki ; Sohst, Bettina M. ; Sonke, Jeroen E. ; Speich, Sabrina ; Steinfeldt, Reiner ; Stewart, Gillian ; Stichel, Torben ; Stirling, Claudine H. ; Stutsman, Johnny ; Swarr, Gretchen J. ; Swift, James H. ; Thomas, Alexander ; Thorne, Kay ; Till, Claire P. ; Till, Ralph ; Townsend, Ashley T. ; Townsend, Emily ; Tuerena, Robyn ; Twining, Benjamin S. ; Vance, Derek ; Velazquez, Sue ; Venchiarutti, Celia ; Villa-Alfageme, Maria ; Vivancos, Sebastian M. ; Voelker, Antje H. L. ; Wake, Bronwyn ; Warner, Mark J. ; Watson, Ros ; van Weerlee, Evaline ; Weigand, M. Alexandra ; Weinstein, Yishai ; Weiss, Dominik ; Wisotzki, Andreas ; Woodward, E. Malcolm S. ; Wu, Jingfeng ; Wu, Yingzhe ; Wuttig, Kathrin ; Wyatt, Neil ; Xiang, Yang ; Xie, Ruifang C. ; Xue, Zichen ; Yoshikawa, Hisayuki ; Zhang, Jing ; Zhang, Pu ; Zhao, Ye ; Zheng, Linjie ; Zheng, Xin-Yuan ; Zieringer, Moritz ; Zimmer, Louise A. ; Ziveri, Patrizia ; Zunino, Patricia ; Zurbrick, CherylThe GEOTRACES Intermediate Data Product 2017 (IDP2017) is the second publicly available data product of the international GEOTRACES programme, and contains data measured and quality controlled before the end of 2016. The IDP2017 includes data from the Atlantic, Pacific, Arctic, Southern and Indian oceans, with about twice the data volume of the previous IDP2014. For the first time, the IDP2017 contains data for a large suite of biogeochemical parameters as well as aerosol and rain data characterising atmospheric trace element and isotope (TEI) sources. The TEI data in the IDP2017 are quality controlled by careful assessment of intercalibration results and multi-laboratory data comparisons at crossover stations. The IDP2017 consists of two parts: (1) a compilation of digital data for more than 450 TEIs as well as standard hydrographic parameters, and (2) the eGEOTRACES Electronic Atlas providing an on-line atlas that includes more than 590 section plots and 130 animated 3D scenes. The digital data are provided in several formats, including ASCII, Excel spreadsheet, netCDF, and Ocean Data View collection. Users can download the full data packages or make their own custom selections with a new on-line data extraction service. In addition to the actual data values, the IDP2017 also contains data quality flags and 1-σ data error values where available. Quality flags and error values are useful for data filtering and for statistical analysis. Metadata about data originators, analytical methods and original publications related to the data are linked in an easily accessible way. The eGEOTRACES Electronic Atlas is the visual representation of the IDP2017 as section plots and rotating 3D scenes. The basin-wide 3D scenes combine data from many cruises and provide quick overviews of large-scale tracer distributions. These 3D scenes provide geographical and bathymetric context that is crucial for the interpretation and assessment of tracer plumes near ocean margins or along ridges. The IDP2017 is the result of a truly international effort involving 326 researchers from 25 countries. This publication provides the critical reference for unpublished data, as well as for studies that make use of a large cross-section of data from the IDP2017. This article is part of a special issue entitled: Conway GEOTRACES - edited by Tim M. Conway, Tristan Horner, Yves Plancherel, and Aridane G. González.