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  • Opal  (2)
  • Thorium  (2)
  • trace metals
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  • 1
    Publication Date: 2022-05-25
    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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  • 2
    Publication Date: 2022-05-25
    Description: © The Author(s), 2015. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Deep Sea Research Part II: Topical Studies in Oceanography 116 (2015): 303-320, doi:10.1016/j.dsr2.2014.11.020.
    Description: The concentration and the major phase composition (particulate organic matter, CaCO3, opal, lithogenic matter, and iron and manganese oxyhydroxides) of marine particles is thought to determine the scavenging removal of particle-reactive TEIs. Particles are also the vector for transferring carbon from the atmosphere to the deep ocean via the biological carbon pump, and their composition may determine the efficiency and strength of this transfer. Here, we present the first full ocean depth section of size-fractionated (1–51 µm, 〉51 µm) suspended particulate matter (SPM) concentration and major phase composition from the US GEOTRACES North Atlantic Zonal Transect between Woods Hole, MA and Lisbon, Portugal conducted in 2010 and 2011. Several major particle features are notable in the section: intense benthic nepheloid layers were observed in the western North American margin with concentrations of SPM of up to 1648 µg/L, two to three orders of magnitude higher than surrounding waters, that were dominated by lithogenic material. A more moderate benthic nepheloid layer was also observed in the eastern Mauritanian margin (44 µg/L) that had a lower lithogenic content and, notably, significant concentrations of iron and manganese oxyhydroxides (2.5% each). An intermediate nepheloid layer reaching 102 µg/L, an order of magnitude above surrounding waters, was observed associated with the Mediterranean Outflow. Finally, there was a factor of two enhancement in SPM at the TAG hydrothermal plume due almost entirely to the addition of iron oxyhydroxides from the hydrothermal vent. We observe correlations between POC and CaCO3 in large (〉51 µm) particles in the upper 2000 m, but not deeper than 2000 m, and no correlations between POC and CaCO3 at any depth in small (〈51 µm) particles. There were also no correlations between POC and lithogenic material in large particles. Overall, there were very large uncertainties associated with all regression coefficients for mineral ballast (“carrying coefficients”), suggesting that mineral ballast was not a strong predictor for POC in this section.
    Description: US and International GEOTRACES Offices (NSF OCE-0850963 and OCE-1129603)
    Keywords: Particles ; SPM ; CaCO3 ; Opal ; Biogenic silica ; POC ; Ballast ; Dust ; Lithogenic material
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 3
    Publication Date: 2022-05-26
    Description: Author Posting. © Elsevier B.V., 2007. This is the author's version of the work. It is posted here by permission of Elsevier B.V. for personal use, not for redistribution. The definitive version was published in Deep Sea Research Part II: Topical Studies in Oceanography 54 (2007): 601-638, doi:10.1016/j.dsr2.2007.01.013.
    Description: This paper investigates ballasting and remineralization controls of carbon sedimentation in the twilight zone (100-1000 m) of the Southern Ocean. Size-fractionated (〈1 μm, 1-51 μm, 〉51 μm) suspended particulate matter was collected by large volume in-situ filtration from the upper 1000 m in the Subantarctic (55°S, 172°W) and Antarctic (66°S, 172°W) zones of the Southern Ocean during the Southern Ocean Iron Experiment (SOFeX) in January-February 2002. Particles were analyzed for major chemical constituents (POC, P, biogenic Si, CaCO3), and digital and SEM image analyses of particles were used to aid in the interpretation of the chemical profiles. Twilight zone waters at 66°S in the Antarctic had a steeper decrease in POC with depth than at 55°S in the Subantarctic, with lower POC concentrations in all size fractions at 66°S than at 55°S, despite up to an order of magnitude higher POC in surface waters at 66°S. The decay length scale of 〉51 μm POC was significantly shorter in the upper twilight zone at 66°S (δe=26 m) compared to 55°S (δe=81 m). Particles in the carbonate-producing 55°S did not have higher excess densities than particles from the diatom-dominated 66°S, indicating that there was no direct ballast effect that accounted for deeper POC penetration at 55°S. An indirect ballast effect due to differences in particle packaging and porosities cannot be ruled out, however, as aggregate porosities were high (~97%) and variable. Image analyses point to the importance of particle loss rates from zooplankton grazing and remineralization as determining factors for the difference in twilight zone POC concentrations at 55°S and 66°S, with stronger and more focused shallow remineralization at 66°S. At 66°S, an abundance of large (several mm long) fecal pellets from the surface to 150 m, and almost total removal of large aggregates by 200 m, reflected the actions of a single or few zooplankton species capable of grazing diatoms in the euphotic zone, coupled with a more diverse particle feeding zooplankton community immediately below. Surface waters with high biomass levels and high proportion of biomass in the large size fraction were associated with low particle loading at depth, with all indications implying conditions of low export. The 66°S region exhibits this “High Biomass, Low Export” (HBLE) condition, with very high 〉51 μm POC concentrations at the surface (~2.1 μM POC), but low concentrations below 200 m (〈0.07 μM POC). The 66°S region remained HBLE after iron fertilization. Iron addition at 55°S caused a ten fold increase in 〉51 μm biomass concentrations in the euphotic zone, bringing surface POC concentrations to levels found at 66°S (~3.8 μM), and a concurrent decrease in POC concentrations below 200 m. The 55°S region, which began with moderate levels of biomass and stronger particle export, transitioned to being HBLE after iron fertilization. We propose that iron addition to already HBLE waters will not cause mass sedimentation events. The stability of an iron-induced HBLE condition is unknown. Better understanding of biological pump processes in non-HBLE Subantarctic waters is needed.
    Description: This work was supported by the DOE Office of Science, Biological and Environmental Research Program. Shiptime for SOFeX was funded by NSF.
    Keywords: Ballast ; Remineralization ; POC ; Twilight Zone ; Mesopelagic ; Southern Ocean ; MULVFS ; Opal ; Carbonate ; Phosphorus
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 4
    Publication Date: 2022-05-26
    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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