Opal Biogenic silica POC Ballast Dust Lithogenic material a b s t r a c tThe concentration and the major phase composition (particulate organic matter, CaCO 3 , 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 sizefractionated (1-51 mm, 4 51 mm) 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 mg/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 mg/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 mg/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 CaCO 3 in large (4 51 mm) particles in the upper 2000 m, but not deeper than 2000 m, and no correlations between POC and CaCO 3 at any depth in small ( o51 mm) 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.
Vertical distributions of iron (Fe) concentrations and isotopes were determined in the total dissolvable and dissolved pools in the water column at three coastal stations located along the Peruvian margin, in the core of the Oxygen Minimum Zone (OMZ). The shallowest station 121 (161 m total water depth) was characterized by lithogenic input from the continental plateau, yielding concentrations as high as 456 nM in the total dissolvable pool. At the 2 other stations (stations 122 and 123), Fe concentrations of dissolved and total dissolvable pools exhibited maxima in both surface and deep layers. Fe isotopic composition (d 56 Fe) showed a fractionation toward lighter values for both physical pools throughout the water column for all stations with minimum values observed for the surface layer (between À0.64 and À0.97& at 10-20 m depth) and deep layer (between À0.03 and À1.25& at 160-300 m depth). An Fe isotope budget was established to determine the isotopic composition of the particulate pool. We observed a range of d 56 Fe values for particulate Fe from +0.02 to À0.87&, with lightest values obtained at water depth above 50 m. Such light values in the both particulate and dissolved pools suggest sources other than atmospheric dust deposition in the surface ocean, including lateral transport of isotopically light Fe. Samples collected at station 122 closest to the sediment show the lightest isotope composition in the dissolved and the particulate pools (À1.25 and À0.53& respectively) and high Fe(II) concentrations (14.2 ± 2.1 nM) consistent with a major reductive benthic Fe sources that is transferred to the ocean water column. A simple isotopic model is proposed to link the extent of Fe(II) oxidation and the Fe isotope composition of both particulate and dissolved Fe pools. This study demonstrates that Fe isotopic composition in OMZ regions is not only affected by the relative contribution of reductive and non-reductive shelf sediment input but also by seawater-column processes during the transport and oxidation of Fe from the source region to open seawater.
Groundwater-derived solute fluxes to the ocean have long been assumed static and subordinate to riverine fluxes, if not neglected entirely, in marine isotope budgets. Here we present concentration and isotope data for Li, Mg, Ca, Sr, and Ba in coastal groundwaters to constrain the importance of groundwater discharge in mediating the magnitude and isotopic composition of terrestrially derived solute fluxes to the ocean. Data were extrapolated globally using three independent volumetric estimates of groundwater discharge to coastal waters, from which we estimate that groundwater-derived solute fluxes represent, at a minimum, 5% of riverine fluxes for Li, Mg, Ca, Sr, and Ba. The isotopic compositions of the groundwater-derived Mg, Ca, and Sr fluxes are distinct from global riverine averages, while Li and Ba fluxes are isotopically indistinguishable from rivers. These differences reflect a strong dependence on coastal lithology that should be considered a priority for parameterization in Earth-system models.
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