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PreprintThorium speciation in seawater( 2005-07) Santschi, Peter H. ; Murray, James W. ; Baskaran, Mark ; Benitez-Nelson, Claudia R. ; Guo, L. D. ; Hung, C.-C. ; Lamborg, Carl H. ; Moran, S. Bradley ; Passow, Uta ; Roy-Barman, MatthieuSince the 1960’s, thorium isotopes occupy a special place in the oceanographer’s toolbox as tracers for determining rates and mechanisms of oceanic scavenging, particle dynamics, and carbon fluxes. Due to their unique and constant production rates from soluble parent nuclides of uranium and radium, their disequilibrium can be used to calculate rates and time scales of sinking particles. In addition, by ratio-ing particulate 234Th (as well, in principle, other Thnuclides) to carbon (and other elements), and linking this ratio to the parent-daughter disequilibrium in the water column, it is possible to calculate fluxes of carbon and other elements. Most of these applications are possible with little knowledge of the dissolved chemical properties of thorium, other than its oxidation state (IV) and tendency to strongly sorb to surfaces, i.e., its “particle- or surface-activity”. However, the use of any tracer is hindered by a lack of knowledge of its chemical properties. Recent observations in the variability of carbon to 234Th ratios in different particle types, as well as of associations of Th(IV) with various marine organic biomolecules has led to the need for a review of current knowledge and what future endeavors should be taken to understand the marine chemistry of thorium.
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ArticleGEOTRACES intercalibration of 230Th, 232Th, 231Pa, and prospects for 10Be(Association for the Sciences of Limnology and Oceanography, 2012-04) Anderson, Robert F. ; Fleisher, Martin Q. ; Robinson, Laura F. ; Edwards, R. Lawrence ; Hoff, John A. ; Moran, S. Bradley ; Rutgers van der Loeff, Michiel M. ; Thomas, Alexander L. ; Roy-Barman, Matthieu ; Francois, RogerNineteen labs representing nine nations participated in the GEOTRACES intercalibration initiative that determined concentrations of 232Th, 230Th, 231Pa, or 10Be in seawater, suspended particles or sediments. Results generally demonstrated good agreement among labs that analyzed marine sediments. Two sets of seawater samples, aliquots of particulate material filtered in situ, and/or aliquots of biogenic sediments were distributed to participating labs. Internal consistency among participating labs improved substantially between the first and second set of seawater samples. Contamination was a serious problem for 232Th. Standard Niskin bottles introduced no detectable contamination, whereas sample containers, reagents, and labware were implicated as sources of contamination. No detectable differences in concentrations of dissolved 232Th, 230Th, or 231Pa were observed among samples of seawater filtered through Nuclepore, Supor, or QMA (quartz) filters with pore diameters ranging between 0.4 and 1.0 μm. Isotope yield monitors equilibrate with dissolved Th in seawater on a time scale of much less than 1 day. Samples of filtered seawater acidified to a pH between 1.7 and 1.8 experienced no detectable loss of dissolved Th or Pa during storage for up to 3 years. The Bermuda Atlantic Time Series station will serve as a GEOTRACES baseline station for future intercalibration of 232Th and 230Th concentrations in seawater. Efforts to improve blanks and standard calibration are ongoing, as is the development of methods to determine concentrations of particulate nuclides, tests of different filtration methods, and an increasing awareness of the need to define protocols for reporting uncertainties.
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PreprintWhat did we learn about ocean particle dynamics in the GEOSECS–JGOFS era?( 2014-12-30) Jeandel, Catherine ; Rutgers van der Loeff, Michiel M. ; Lam, Phoebe J. ; Roy-Barman, Matthieu ; Sherrell, Robert M. ; Kretschmer, Sven ; German, Christopher R. ; Dehairs, FrankParticles determine the residence time of many dissolved elements in seawater. Although a substantial number of field studies were conducted in the framework of major oceanographic programs as GEOSECS and JGOFS, knowledge about particle dynamics is still scarce. Moreover, the particulate trace metal behavior remains largely unknown. The GEOSECS sampling strategy during the 1970’s focused on large sections across oceanic basins, where particles were collected by membrane filtration after Niskin bottle sampling, biasing the sampling towards the small particle pool. Late in this period, the first in situ pumps allowing large volume sampling were also developed. During the 1990’s, JGOFS focused on the quantification of the “exported carbon flux” and its seasonal variability in representative biogeochemical provinces of the ocean, mostly using sediment trap deployments. Although scarce and discrete in time and space, these pioneering studies allowed an understanding of the basic fate of marine particles. This understanding improved considerably, especially when the analysis of oceanic tracers such as natural radionuclides allowed the first quantification of processes such as dissolved-particle exchange and particle settling velocities. Because the GEOTRACES program emphasizes the importance of collecting, characterizing and 39 analyzing marine particles, this paper reflects our present understanding of the sources, fate and sinks of oceanic particles at the early stages of the program.
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ArticleGlobal ocean sediment composition and burial flux in the deep sea(American Geophysical Union, 2021-03-21) Hayes, Christopher T. ; Costa, Kassandra M. ; Anderson, Robert F. ; Calvo, Eva ; Chase, Zanna ; Demina, Ludmila L. ; Dutay, Jean-Claude ; German, Christopher R. ; Heimbürger, Lars-Eric ; Jaccard, Samuel L. ; Jacobel, Allison W. ; Kohfeld, Karen E. ; Kravchishina, Marina ; Lippold, Jörg ; Mekik, Figen ; Missiaen, Lise ; Pavia, Frank ; Paytan, Adina ; Pedrosa-Pamies, Rut ; Petrova, Mariia V. ; Rahman, Shaily ; Robinson, Laura F. ; Roy-Barman, Matthieu ; Sanchez-Vidal, Anna ; Shiller, Alan M. ; Tagliabue, Alessandro ; Tessin, Allyson C. ; van Hulten, Marco ; Zhang, JingQuantitative knowledge about the burial of sedimentary components at the seafloor has wide-ranging implications in ocean science, from global climate to continental weathering. The use of 230Th-normalized fluxes reduces uncertainties that many prior studies faced by accounting for the effects of sediment redistribution by bottom currents and minimizing the impact of age model uncertainty. Here we employ a recently compiled global data set of 230Th-normalized fluxes with an updated database of seafloor surface sediment composition to derive atlases of the deep-sea burial flux of calcium carbonate, biogenic opal, total organic carbon (TOC), nonbiogenic material, iron, mercury, and excess barium (Baxs). The spatial patterns of major component burial are mainly consistent with prior work, but the new quantitative estimates allow evaluations of deep-sea budgets. Our integrated deep-sea burial fluxes are 136 Tg C/yr CaCO3, 153 Tg Si/yr opal, 20Tg C/yr TOC, 220 Mg Hg/yr, and 2.6 Tg Baxs/yr. This opal flux is roughly a factor of 2 increase over previous estimates, with important implications for the global Si cycle. Sedimentary Fe fluxes reflect a mixture of sources including lithogenic material, hydrothermal inputs and authigenic phases. The fluxes of some commonly used paleo-productivity proxies (TOC, biogenic opal, and Baxs) are not well-correlated geographically with satellite-based productivity estimates. Our new compilation of sedimentary fluxes provides detailed regional and global information, which will help refine the understanding of sediment preservation.
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PreprintTh-234 sorption and export models in the water column : a review( 2005-10-10) Savoye, Nicolas ; Benitez-Nelson, Claudia R. ; Burd, Adrian B. ; Cochran, J. Kirk ; Charette, Matthew A. ; Buesseler, Ken O. ; Jackson, George A. ; Roy-Barman, Matthieu ; Schmidt, Sabine ; Elskens, MarcOver the past few decades, the radioisotope pair of 238U/234Th has been widely and increasingly used to describe particle dynamics and particle export fluxes in a variety of aquatic systems. The present paper is one of five review articles dedicated to 234Th. It is focused on the models associated with 234Th whereas the companion papers (same issue) are focused on present and future methodologies and techniques (Rutgers van der Loeff et al.), C/234Th ratios (Buesseler et al.), 234Th speciation (Santschi et al.) and present and future applications of 234Th (Waples et al.). In this paper, we review current 234Th scavenging models and discuss the relative importance of the non steady state and physical terms associated with the most commonly used model to estimate 234Th flux. Based on this discussion we recommend that for future work the use of models should be accompanied by a discussion of the effect that model and data uncertainty have on the model results. We also suggest that future field work incorporate repeat occupations of sample sites on time scales of 1-4 weeks in order to evaluate steady state versus non steady state estimates of 234Th export, especially during high flux events (> ca. 800 dpm m-2 d-1). Finally, knowledge of the physical oceanography of the study area is essential, particularly in ocean margins and in areas of established upwelling (e.g. Equatorial Pacific). These suggestions will greatly enhance the application of 234Th as a tracer of particle dynamics and flux in more complicated regimes.
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Article230 Th normalization: new insights on an essential tool for quantifying sedimentary fluxes in the modern and quaternary ocean(John Wiley & Sons, 2020-01-27) Costa, Kassandra M. ; Hayes, Christopher T. ; Anderson, Robert F. ; Pavia, Frank ; Bausch, Alexandra ; Deng, Feifei ; Dutay, Jean-Claude ; Geibert, Walter ; Heinze, Christoph ; Henderson, Gideon M. ; Hillaire‐Marcel, Claude ; Hoffmann, Sharon S. ; Jaccard, Samuel L. ; Jacobel, Allison W. ; Kienast, Stephanie S. ; Kipp, Lauren ; Lerner, Paul ; Lippold, Jörg ; Lund, David C. ; Marcantonio, Franco ; McGee, David ; McManus, Jerry F. ; Mekik, Figen ; Middleton, Jennifer L. ; Missiaen, Lise ; Not, Christelle ; Pichat, Sylvain ; Robinson, Laura F. ; Rowland, George H. ; Roy-Barman, Matthieu ; Tagliabue, Alessandro ; Torfstein, Adi ; Winckler, Gisela ; Zhou, Yuxin230Th normalization is a valuable paleoceanographic tool for reconstructing high‐resolution sediment fluxes during the late Pleistocene (last ~500,000 years). As its application has expanded to ever more diverse marine environments, the nuances of 230Th systematics, with regard to particle type, particle size, lateral advective/diffusive redistribution, and other processes, have emerged. We synthesized over 1000 sedimentary records of 230Th from across the global ocean at two time slices, the late Holocene (0–5,000 years ago, or 0–5 ka) and the Last Glacial Maximum (18.5–23.5 ka), and investigated the spatial structure of 230Th‐normalized mass fluxes. On a global scale, sedimentary mass fluxes were significantly higher during the Last Glacial Maximum (1.79–2.17 g/cm2kyr, 95% confidence) relative to the Holocene (1.48–1.68 g/cm2kyr, 95% confidence). We then examined the potential confounding influences of boundary scavenging, nepheloid layers, hydrothermal scavenging, size‐dependent sediment fractionation, and carbonate dissolution on the efficacy of 230Th as a constant flux proxy. Anomalous 230Th behavior is sometimes observed proximal to hydrothermal ridges and in continental margins where high particle fluxes and steep continental slopes can lead to the combined effects of boundary scavenging and nepheloid interference. Notwithstanding these limitations, we found that 230Th normalization is a robust tool for determining sediment mass accumulation rates in the majority of pelagic marine settings (>1,000 m water depth).
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ArticleThe transpolar drift as a source of riverine and shelf-derived trace elements to the central Arctic Ocean(American Geophysical Union, 2020-04-08) Charette, Matthew A. ; Kipp, Lauren ; Jensen, Laramie T. ; Dabrowski, Jessica S. ; Whitmore, Laura M. ; Fitzsimmons, Jessica N. ; Williford, Tatiana ; Ulfsbo, Adam ; Jones, Elizabeth M. ; Bundy, Randelle M. ; Vivancos, Sebastian M. ; Pahnke, Katharina ; John, Seth G. ; Xiang, Yang ; Hatta, Mariko ; Petrova, Mariia V. ; Heimbürger, Lars-Eric ; Bauch, Dorothea ; Newton, Robert ; Pasqualini, Angelica ; Agather, Alison ; Amon, Rainer M. W. ; Anderson, Robert F. ; Andersson, Per S. ; Benner, Ronald ; Bowman, Katlin ; Edwards, R. Lawrence ; Gdaniec, Sandra ; Gerringa, Loes J. A. ; González, Aridane G. ; Granskog, Mats A. ; Haley, Brian ; Hammerschmidt, Chad R. ; Hansell, Dennis A. ; Henderson, Paul B. ; Kadko, David C. ; Kaiser, Karl ; Laan, Patrick ; Lam, Phoebe J. ; Lamborg, Carl H. ; Levier, Martin ; Li, Xianglei ; Margolin, Andrew R. ; Measures, Christopher I. ; Middag, Rob ; Millero, Frank J. ; Moore, Willard S. ; Paffrath, Ronja ; Planquette, Helene ; Rabe, Benjamin ; Reader, Heather ; Rember, Robert ; Rijkenberg, Micha J. A. ; Roy-Barman, Matthieu ; van der Loeff, Michiel Rutgers ; Saito, Mak A. ; Schauer, Ursula ; Schlosser, Peter ; Sherrell, Robert M. ; Shiller, Alan M. ; Slagter, Hans ; Sonke, Jeroen E. ; Stedmon, Colin ; Woosley, Ryan J. ; Valk, Ole ; van Ooijen, Jan ; Zhang, RuifengA major surface circulation feature of the Arctic Ocean is the Transpolar Drift (TPD), a current that transports river‐influenced shelf water from the Laptev and East Siberian Seas toward the center of the basin and Fram Strait. In 2015, the international GEOTRACES program included a high‐resolution pan‐Arctic survey of carbon, nutrients, and a suite of trace elements and isotopes (TEIs). The cruises bisected the TPD at two locations in the central basin, which were defined by maxima in meteoric water and dissolved organic carbon concentrations that spanned 600 km horizontally and ~25–50 m vertically. Dissolved TEIs such as Fe, Co, Ni, Cu, Hg, Nd, and Th, which are generally particle‐reactive but can be complexed by organic matter, were observed at concentrations much higher than expected for the open ocean setting. Other trace element concentrations such as Al, V, Ga, and Pb were lower than expected due to scavenging over the productive East Siberian and Laptev shelf seas. Using a combination of radionuclide tracers and ice drift modeling, the transport rate for the core of the TPD was estimated at 0.9 ± 0.4 Sv (106 m3 s−1). This rate was used to derive the mass flux for TEIs that were enriched in the TPD, revealing the importance of lateral transport in supplying materials beneath the ice to the central Arctic Ocean and potentially to the North Atlantic Ocean via Fram Strait. Continued intensification of the Arctic hydrologic cycle and permafrost degradation will likely lead to an increase in the flux of TEIs into the Arctic Ocean.