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  1. Reversible scavenging, the oceanographic process by which dissolved metals exchange onto and off sinking particles and are thereby transported to deeper depths, has been well established for the metal thorium for decades. Reversible scavenging both deepens the elemental distribution of adsorptive elements and shortens their oceanic residence times in the ocean compared to nonadsorptive metals, and scavenging ultimately removes elements from the ocean via sedimentation. Thus, it is important to understand which metals undergo reversible scavenging and under what conditions. Recently, reversible scavenging has been invoked in global biogeochemical models of a range of metals including lead, iron, copper, and zinc to fit modeled data to observations of oceanic dissolved metal distributions. Nonetheless, the effects of reversible scavenging remain difficult to visualize in ocean sections of dissolved metals and to distinguish from other processes such as biological regeneration. Here, we show that particle-rich “veils” descending from high-productivity zones in the equatorial and North Pacific provide idealized illustrations of reversible scavenging of dissolved lead (Pb). A meridional section of dissolved Pb isotope ratios across the central Pacific shows that where particle concentrations are sufficiently high, such as within particle veils, vertical transport of anthropogenic surface–dissolved Pb isotope ratios toward the deep ocean is manifested as columnar isotope anomalies. Modeling of this effect shows that reversible scavenging within particle-rich waters allows anthropogenic Pb isotope ratios from the surface to penetrate ancient deep waters on timescales sufficiently rapid to overcome horizontal mixing of deep water Pb isotope ratios along abyssal isopycnals. 
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  2. Abstract

    The cycling of marine particulate matter is critical for sequestering carbon in the deep ocean and in marine sediments. Biogenic minerals such as calcium carbonate (CaCO3) and opal add density to more buoyant organic material, facilitating particle sinking and export. Here, we compile and analyze a global data set of particulate organic carbon (POC), particulate inorganic carbon (PIC, or CaCO3), and biogenic silica (bSi, or opal) concentrations collected using large volume pumps (LVPs). We analyze the distribution of all three biogenic phases in the small (1–53 μm) and large (>53 μm) size classes. Over the entire water column 76% of POC exists in the small size fraction. Similarly, the small size class contains 82% of PIC, indicating the importance of small‐sized coccolithophores to the PIC budget of the ocean. In contrast, 50% of bSi exists in the large size fraction, reflecting the larger size of diatoms and radiolarians compared with coccolithophores. We use PIC:POC and bSi:POC ratios in the upper ocean to document a consistent signal of shallow mineral dissolution, likely linked to biologically mediated processes. Sediment trap PIC:POC and bSi:POC are elevated with respect to LVP samples and increase strongly with depth, indicating the concentration of mineral phases and/or a deficit of POC in large sinking particles. We suggest that future sampling campaigns pair LVPs with sediment traps to capture the full particulate field, especially the large aggregates that contribute to mineral‐rich deep ocean fluxes, and may be missed by LVPs.

     
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  3. Abstract

    Understanding particle cycling processes in the ocean is critical for predicting the response of the biological carbon pump to external perturbations. Here, measurements of particulate organic carbon (POC) concentration in two size fractions (1–51 and >51 μm) from GEOTRACES Pacific meridional transect GP15 are combined with a POC cycling model to estimate rates of POC production, (dis)aggregation, sinking, remineralization, and vertical transport mediated by migrating zooplankton, in the euphotic zone (EZ) and upper mesopelagic zone (UMZ) of distinct environments. We find coherent variations in POC cycling parameters and fluxes throughout the transect. Thus, the settling speed of POC in the >51 μm fraction increased with depth in the UMZ, presumably due to higher particle densities at depth. The settling flux of total POC (>1 μm) out of the EZ was positively correlated with primary production integrated over the EZ; the highest export occurred in the subarctic gyre while the lowest occurred in the subtropical gyres. The ratio of POC settling flux to integrated primary production was low (<5%) along GP15, which suggests an efficient recycling of POC in the EZ in all trophic regimes. Specific rates of POC remineralization did not show clear variations with temperature or dissolved oxygen concentration, that is, POC recycling was apparently controlled by other factors such as microbial colonization and substrate lability. Particle cohesiveness, as approximated by the second‐order rate constant for particle aggregation, was negatively correlated with trophic regime: particles appeared more cohesive in low‐productivity regions than in high‐productivity regions.

     
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  4. Particle cycling rates in marine systems are difficult to measure directly, but of great interest in understanding how carbon and other elements are distributed throughout the ocean. Here, rates of particle production, aggregation, disaggregation, sinking, remineralization, and transport mediated by zooplankton diel vertical migration were estimated from size-fractionated measurements of particulate organic carbon (POC) concentration collected during the NASA EXport Processes in the Ocean from RemoTe Sensing (EXPORTS) cruise at Station P in summer 2018. POC data were combined with a particle cycling model using an inverse method. Our estimates of the total POC settling flux throughout the water column are consistent with those derived from thorium-234 disequilibrium and sediment traps. A budget for POC in two size fractions, small (1–51 µm) and large (> 51 µm), was produced for both the euphotic zone (0–100 m) and the upper mesopelagic zone (100–500 m). We estimated that POC export at the base of the euphotic zone was 2.2 ± 0.8 mmol m−2 d−1, and that both small and large particles contributed considerably to the total export flux along the water column. The model results indicated that throughout the upper 500 m, remineralization leads to a larger loss of small POC than does aggregation, whereas disaggregation results in a larger loss of large POC than does remineralization. Of the processes explicitly represented in the model, zooplankton diel vertical migration is a larger source of large POC to the upper mesopelagic zone than the convergence of large POC due to particle sinking. Positive model residuals reveal an even larger unidentified source of large POC in the upper mesopelagic zone. Overall, our posterior estimates of particle cycling rate constants do not deviate much from values reported in the literature, i.e., size-fractionated POC concentration data collected at Station P are largely consistent with prior estimates given their uncertainties. Our budget estimates should provide a useful framework for the interpretation of process-specific observations obtained by various research groups in EXPORTS. Applying our inverse method to other systems could provide insight into how different biogeochemical processes affect the cycling of POC in the upper water column. 
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  5. Particulate inorganic carbon (PIC) plays a major role in the ocean carbon cycle impacting pH, dissolved inorganic carbon, and alkalinity, as well as particulate organic carbon (POC) export and transfer efficiency to the deep sea. Remote sensing retrievals of PIC in surface waters span two decades, yet knowledge of PIC concentration variability in the water column is temporally and spatially limited due to a reliance on ship sampling. To overcome the space–time gap in observations, we have developed optical sensors for PIC concentration and flux that exploit the high mineral birefringence of CaCO 3 minerals, and thus enable real-time data when deployed operationally from ship CTDs and ARGO-style Carbon Flux Explorer floats. For PIC concentrations, we describe a fast (10 Hz) digital low-power (∼0.5 W) sensor that utilizes cross-polarized transmitted light to detect the photon yield from suspended birefringent particles in the water column. This sensor has been CTD-deployed to depths as great as 6,000 m and cross-calibrated against particulates sampled by large volume in situ filtration and CTD/rosettes. We report data from the September–November 2018 GEOTRACES GP15 meridional transect from the Aleutian Islands to Tahiti along 152°W where we validated two prototype sensors deployed on separate CTD systems surface to bottom at 39 stations, many of which were taken in nearly particle-free waters. We compare sensor results with major particle phase composition (particularly PIC and particulate aluminum) from simultaneously collected size-fractionated particulate samples collected by large volume in situ filtration. We also report results from the June 2017 California Current Ecosystem-Long Term Ecological Research (CCE-LTER) process study in California coastal waters where high PIC levels were found. We demonstrate that the PIC concentration sensor can detect PIC concentration variability from 0.01 to >1 μM in the water column (except in nepheloid layers) and outline engineering needs and progress on its integration with the Carbon Flux Explorer, an autonomous float. 
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  6. The downward flux of sinking particles is a prominent Hg removal and redistribution process in the ocean; however, it is not well-constrained. Using data from three U.S. GEOTRACES cruises including the Pacific, Atlantic, and Arctic Oceans, we examined the mercury partitioning coefficient, K d , in the water column. The data suggest that the K d varies widely over three ocean basins. We also investigated the effect of particle concentration and composition on K d by comparing the concentration of small-sized (1–51 μm) suspended particulate mass (SPM) as well as its compositional fractions in six different phases to the partitioning coefficient. We observed an inverse relationship between K d and suspended particulate mass, as has been observed for other metals and known as the “particle concentration effect,” that explains much of the variation in K d . Particulate organic matter (POM) and calcium carbonate (CaCO 3 ) dominated the Hg partitioning in all three ocean basins while Fe and Mn could make a difference in some places where their concentrations are elevated, such as in hydrothermal plumes. Finally, our estimated Hg residence time has a strong negative correlation with average log bulk K d , indicating that K d has significant effect on Hg residence time. 
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  8. Abstract

    We compile full ocean‐depth size‐fractionated (1–51 and >51 μm) particle concentration and composition of suspended particulate matter from three recent U.S. GEOTRACES cruises, and exploit detailed information of particle characteristics measured to give insights into controls on sinking velocity and mass flux. Our model integrates the concept of fractal scaling into Stokes' Law by incorporating one of two porosity‐size power law relationships that result in fractal dimensions of 1.4 and 2.1. The medians of pump‐derived total (>1 μm) mass flux in the upper 100 m of gyre stations are 285.1, 609.2, and 99.3 mg/m2/d in the North Atlantic, Eastern Tropical South Pacific, and Western Arctic Ocean cruises, respectively. In this data set, variations in particle concentration were generally more important than sinking velocity in controlling variations in mass flux. We examine different terms in a Stokes' Law model to explore how variations in particle and water column characteristics from these three cruises affect mass flux. The decomposition of different aspects of the Stokes' relationship sheds light on the lowest total mass flux of the three cruises in the Western Arctic, which could be explained by the Arctic having the lowest particle concentrations as well as the lowest sinking velocities due to having the smallest particle sizes and the most viscous water. This work shows the importance of both particle characteristics and size distribution for mass fluxes, and similar methods can be applied to existing and future size‐fractionated filtered particulate measurements to improve our understanding of the biological pump elsewhere.

     
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  9. Abstract

    We present full water depth sections of size‐fractionated (1–51 μm; >51 μm) concentrations of suspended particulate matter and major particle phase composition (particulate organic matter [POM], including its carbon isotopic composition [POC‐δ13C] and C:N ratio, calcium carbonate [CaCO3], opal, lithogenic particles, and iron and manganese [oxyhydr]oxides) from the U.S. GEOTRACES Arctic Cruise (GN01) in the western Arctic in 2015. Whereas biogenic particles (POM and opal) dominate the upper 1,000 m, lithogenic particles are the most abundant particle type at depth. Minor phases such as manganese (Mn) oxides are higher in GN01 than in any other U.S. GEOTRACES cruises so far. Extremely depleted POC‐δ13C, as low as ~ −32‰, is ubiquitous at the surface of the western Arctic Ocean as a result of different growth rates of phytoplankton. Moderate penetration of depleted POC‐δ13C to depth indicates active sinking of large particles in the central basin. Lateral transport from the Chukchi shelf is also of significance in the western Arctic, as is evident from increases in biogenic silica to POC ratios and Mn oxide concentrations in the halocline, as well as lithogenic element contents in the deep waters. Our study supports previous suggestions of the near absence of CaCO3in the Arctic Basin. This study presents the first data set of concentration and composition of suspended particles in the western Arctic Ocean and sheds new light on the vertical and lateral processes that govern particle distribution in this enclosed ocean basin.

     
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