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  • Thorium  (2)
  • trace metals  (2)
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  • 1
    Publication Date: 2017-12-14
    Description: © The Author(s), 2016. This is the author's version of the work and is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Deep Sea Research Part I: Oceanographic Research Papers 113 (2016): 57-79, doi:10.1016/j.dsr.2016.03.008.
    Description: Thorium is a highly particle-reactive element that possesses different measurable radio-isotopes in seawater, with well-constrained production rates and very distinct half-lives. As a result, Th has emerged as a key tracer for the cycling of marine particles and of their chemical constituents, including particulate organic carbon. Here two different versions of a model of Th and particle cycling in the ocean are tested using an unprecedented data set from station GT11-22 of the U.S. GEOTRACES North Atlantic Section: (i) 21 228;230;234Th activities of dissolved and particulate fractions, (ii) 228Ra activities, (iii) 234;238U activities estimated from salinity data and an assumed 234U/238U ratio, and (iv) particle concentrations, below a depth of 125 m. The two model versions assume a single class of particles but rely on different assumptions about the rate parameters for sorption reactions and particle processes: a first version (V1) assumes vertically uniform parameters (a popular description), whereas the second (V2) does not. Both versions are tested by fitting to the GT11-22 data using generalized nonlinear least squares and by analyzing residuals normalized to the data errors. We find that model V2 displays a significantly better fit to the data than model V1. Thus, the mere allowance of vertical variations in the rate parameters can lead to a significantly better fit to the data, without the need to modify the structure or add any new processes to the model. To understand how the better fit is achieved we consider two parameters, K = k1=(k-1 + β-1) and K/P, where k1 is the adsorption rate constant, k-1 the desorption rate constant, β-1 the remineralization rate constant, and P the particle concentration. We find that the rate constant ratio K is large (≥0.2) in the upper 1000 m and decreases to a nearly uniform value of ca. 0.12 below 2000 m, implying that the specific rate at which Th attaches to particles relative to that at which it is released from particles is higher in the upper ocean than in the deep ocean. In contrast, K/P increases with depth below 500 m. The parameters K and K/P display significant positive and negative monotonic relationship with P, respectively, which is collectively consistent with a particle concentration effect.
    Description: We acknowledge the U.S. National Science Foundation for providing funding for this study (grant OCE-1232578) and for U.S. GEOTRACES North Atlantic section ship time, sampling, and data analysis.
    Description: 2017-03-31
    Keywords: GEOTRACES ; North Atlantic ; Thorium ; Particles ; Reversible Exchange ; Model ; Inverse Method
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 2
    Publication Date: 2019-06-10
    Description: Author Posting. © American Geophysical Union, 2019. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Global Biogeochemical Cycles 33(1), (2019): 15-36, doi:10.1029/2018GB005985.
    Description: Better constraints on the magnitude of particulate export and the residence times of trace elements are required to understand marine food web dynamics, track the transport of anthropogenic trace metals in the ocean, and improve global climate models. While prior studies have been successful in constructing basin‐scale budgets of elements like carbon in the upper ocean, the cycling of particulate trace metals is poorly understood. The 238U‐234Th method is used here with data from the GP‐16 GEOTRACES transect to investigate the upper ocean processes controlling the particulate export of cadmium, cobalt, and manganese in the southeastern Pacific. Patterns in the flux data indicated that particulate cadmium and cobalt behave similarly to particulate phosphorus and organic carbon, with the highest export in the productive coastal region and decreasing flux with depth due to remineralization. The export of manganese was influenced by redox conditions at the low oxygen coastal stations and by precipitation and/or scavenging elsewhere. Residence times with respect to export (total inventory divided by particulate flux) for phosphorus, cadmium, cobalt, and manganese in the upper 100 and 200 m were determined to be on the order of months to years. These GEOTRACES‐based synthesis efforts, combining a host of concentration and tracer data with unprecedented resolution, will help to close the oceanic budgets of trace metals.
    Description: This work was supported by the National Science Foundation (OCE‐1232669 and OCE‐1518110), and Erin Black was also funded by a NASA Earth and Space Science Graduate Fellowship (NNX13AP31H). The authors would like to thank the captain, crew, and scientists aboard the R/V Thomas G. Thompson. A special thanks to two anonymous reviewers and Virginie Sanial for providing the additional 228Ra‐based estimates for Cd. All original data have been made available in either the supporting information or through BCO‐DMO (see Website and Database References).
    Description: 2019-06-10
    Keywords: thorium ; export ; trace metals ; residence time
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 3
    Publication Date: 2018-01-10
    Description: © The Author(s), 2017. This is the author's version of the work. It is posted here under a nonexclusive, irrevocable, paid-up, worldwide license granted to WHOI. It is made available for personal use, not for redistribution. The definitive version was published in Deep Sea Research Part I: Oceanographic Research Papers 125 (2017): 106-128, doi:10.1016/j.dsr.2017.05.003.
    Description: The high particle reactivity of thorium has resulted in its widespread use in tracing processes impacting marine particles and their chemical constituents. The use of thorium isotopes as tracers of particle dynamics, however, largely relies on our understanding of how the element scavenges onto particles. Here, we estimate apparent rate constants of Th adsorption (k1), Th desorption (k−1), bulk particle degradation (β-1), and bulk particle sinking speed (w) along the water column at 11 open-ocean stations occupied during the GEOTRACES North Atlantic Section (GA03). First, we provide evidence that the budgets of Th isotopes and particles at these stations appear to be generally dominated by radioactive production and decay sorption reactions, particle degradation, and particle sinking. Rate parameters are then estimated by fitting a Th and particle cycling model to data of dissolved and particulate 228,230,234Th, 228Ra, particle concentrations, and 234,238U estimates based on salinity, using a nonlinear programming technique. We find that the adsorption rate constant (k1) generally decreases with depth across the section: broadly, the time scale 1/k1 averages 1.0 yr in the upper 1000 m and (1.4–1.5) yr below. A positive relationship between k1 and particle concentration (P) is found, i.e., , k1 ∝ Pb where b ≥ 1, consistent with the notion that k1 increases with the number of surface sites available for adsorption. The rate constant ratio, K = k1/(k-1 + β-1), which measures the collective influence of rate parameters on Th scavenging, averages 0.2 for most stations and most depths. We clarify the conditions under which K/P is equivalent to the distribution coefficient, KD, test that the conditions are met at the stations, and find that decreases with P, in line with a particle concentration effect (dKD/dP 〈 0). In contrast to the influence of colloids as envisioned by the Brownian pumping hypothesis, we provide evidence that the particle concentration effect arises from the joint effect of P on the rate constants for thorium attachment to, and detachment from, particles.
    Description: We acknowledge the U.S. National Science Foundation for providing funding for this study (grant OCE-1232578) and for U.S. GEOTRACES North Atlantic section ship time, sampling, and data analysis. The U.S. NSF also supported the generation of 230Th data (OCE-0927064 to LDEO, OCE-O092860 to WHOI, and OCE-0927754 to UMN) and 228,234Th data (OCE-0925158 to WHOI).
    Keywords: GEOTRACES ; Thorium ; Particle Concentration Effect ; Single-particle class model ; Inverse method
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 4
    Publication Date: 2019-05-22
    Description: Author Posting. © American Geophysical Union, 2019. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Global Biogeochemical Cycles 32(12), (2019): 1738-1758, doi:10.1029/2018GB005994.
    Description: Sinking particles strongly regulate the distribution of reactive chemical substances in the ocean, including particulate organic carbon and other elements (e.g., P, Cd, Mn, Cu, Co, Fe, Al, and 232Th). Yet, the sinking fluxes of trace elements have not been well described in the global ocean. The U.S. GEOTRACES campaign in the North Atlantic (GA03) offers the first data set in which the sinking flux of carbon and trace elements can be derived using four different radionuclide pairs (238U:234Th ;210Pb:210Po; 228Ra:228Th; and 234U:230Th) at stations co‐located with sediment trap fluxes for comparison. Particulate organic carbon, particulate P, and particulate Cd fluxes all decrease sharply with depth below the euphotic zone. Particulate Mn, Cu, and Co flux profiles display mixed behavior, some cases reflecting biotic remineralization, and other cases showing increased flux with depth. The latter may be related to either lateral input of lithogenic material or increased scavenging onto particles. Lastly, particulate Fe fluxes resemble fluxes of Al and 232Th, which all have increasing flux with depth, indicating a dominance of lithogenic flux at depth by resuspended sediment transported laterally to the study site. In comparing flux estimates derived using different isotope pairs, differences result from different timescales of integration and particle size fractionation effects. The range in flux estimates produced by different methods provides a robust constraint on the true removal fluxes, taking into consideration the independent uncertainties associated with each method. These estimates will be valuable targets for biogeochemical modeling and may also offer insight into particle sinking processes.
    Description: This study grew out of a synthesis workshop at the Lamont‐Doherty Earth Observatory of Columbia University in August 2016. This workshop was sponsored by the U.S. GEOTRACES Project Office (NSF 1536294) and the Ocean Carbon and Biogeochemistry (OCP) Project Office (NSF 1558412 and NASA NNX17AB17G). The U.S. National Science Foundation supported all of the analytical work on GA03. Kuanbo Zhou measured 228Th in the large size class particles (NSF 0925158 to WHOI). NSF 1061128 to Stony Brook University supported the BaRFlux project, for which Chistina Heilbrun is acknowledged for laboratory and field work. The lead author acknowledges support from a start‐up grant from the University of Southern Mississippi. Two anonymous reviewers are thanked for their constructive comments. All GEOTRACES GA03 data used in this study are accessible through the Biological and Chemical Oceanography Data Management Office (http://data.bco‐dmo.org/jg/dir/BCO/GEOTRACES/NorthAtlanticTransect/), and derived parameters are reported in the supporting information.
    Description: 2019-05-22
    Keywords: biological carbon pump ; trace metals ; North Atlantic ; export ; GEOTRACES
    Repository Name: Woods Hole Open Access Server
    Type: Article
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