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Abstract Most oceanic lead (Pb) is from anthropogenic emissions into the atmosphere deposited into surface waters, mostly during the past two centuries. The space‐ and time‐dependent emission patterns of anthropogenic Pb (and its isotope ratios) constitute a global geochemical experiment providing information on advective, mixing, chemical, and particle flux processes redistributing Pb within the ocean. Pb shares aspects of its behavior with other elements, for example, atmospheric input, dust solubilization, biological uptake, and reversible exchange between dissolved and adsorbed Pb on sinking particles. The evolving distributions allow us to see signals hidden in steady‐state tracer distributions. The global anthropogenic Pb emission experiment serves as a tool to understand oceanic trace element dynamics. We obtained a high‐resolution (5° station spacing) depth transect of dissolved Pb concentrations and Pb isotopes from Alaska (55°N) to just north of Tahiti (20°S) near 152°W longitude. The sections reveal distinct sources of Pb (American, Australian, and Chinese), transport of Australian style Pb to the water mass formation region of Sub‐Antarctic Mode Water which is advected northward, columnar Pb isotope contours due to reversible particle exchange on sinking particles from high‐productivity particle veils, and a gradient of high northern deep water [Pb] to low southern deep water [Pb] that is created by reversible exchange release of Pb from sinking particles carrying predominantly northern hemisphere Pb.²⁰⁸Pb/²⁰⁶Pb versus²⁰⁶Pb/²⁰⁷Pb isotope relationships show that most oceanic Pb in the North Pacific is from Chinese and American sources, whereas Pb in the South Pacific is from Australian and American sources. 

Industrial activities have increased the supply of iron to the ocean, but the magnitude of anthropogenic input and its ecological consequences are not well-constrained by observations. Across four expeditions to the North Pacific transition zone, we document a repeated supply of isotopically light iron from an atmospheric source in spring, reflecting an estimated 39 ± 9 % anthropogenic contribution to the surface ocean iron budget. Expression of iron-stress genes in metatranscriptomes, and evidence for colimitation of ecosystem productivity by iron and nitrogen, indicates that enhanced iron supply should spur spring phytoplankton blooms, accelerating the seasonal drawdown of nitrate delivered by winter mixing. This effect is consistent with regional trends in satellite ocean color, which show a shorter, more intense spring bloom period, followed by an earlier arrival of oligotrophic conditions in summer. Continued iron emissions may contribute to poleward shifts in transitional marine ecosystems, compounding the anticipated impacts from ocean warming and stratification. 

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. 

Abstract. Over the past decade, the GEOTRACES and wider trace metalgeochemical community has made substantial contributions towardsconstraining the marine cobalt (Co) cycle and its major biogeochemicalprocesses. However, few Co speciation studies have been conducted in theNorth and equatorial Pacific Ocean, a vast portion of the world's oceans byvolume and an important end-member of deep thermohaline circulation.Dissolved Co (dCo) samples, including total dissolved and labile Co, weremeasured at-sea during the GEOTRACES Pacific Meridional Transect (GP15) expedition along the 152∘ W longitudinal from 56∘ N to20∘ S. Along this transect, upper-ocean dCo (σ0<26) was linearly correlated with dissolved phosphate (slope = 82±3, µmol : mol) due to phytoplankton uptake and remineralization.As depth increased, dCo concentrations became increasingly decoupled fromphosphate concentrations due to co-scavenging with manganese oxide particlesin the mesopelagic. The transect revealed an organically bound coastalsource of dCo to the Alaskan Stream associated with low-salinity waters. Anintermediate-depth hydrothermal flux of dCo was observed off the Hawaiiancoast at the Loihi Seamount, and the elevated dCo was correlated withpotential xs3He at and above the vent site; however, the Loihi Seamountlikely did not represent a major source of Co to the Pacific basin. Elevatedconcentrations of dCo within oxygen minimum zones (OMZs) in the equatorialNorth and South Pacific were consistent with the suppression of oxidativescavenging, and we estimate that future deoxygenation could increase the OMZdCo inventory by 18 % to 36 % over the next century. In Pacific Deep Water(PDW), a fraction of elevated ligand-bound dCo appeared protected fromscavenging by the high biogenic particle flux in the North Pacific basin.This finding is counter to previous expectations of low dCo concentrationsin the deep Pacific due to scavenging over thermohaline circulation.Compared to a Co global biogeochemical model, the observed transectdisplayed more extreme inventories and fluxes of dCo than predicted by themodel, suggesting a highly dynamic Pacific Co cycle. 

Abstract Despite the Pacific being the location of the earliest seawater Cd studies, the processes which control Cd distributions in this region remain incompletely understood, largely due to the sparsity of data. Here, we present dissolved Cd and δ¹¹⁴Cd data from the US GEOTRACES GP15 meridional transect along 152°W from the Alaskan margin to the equatorial Pacific. Our examination of this region's surface ocean Cd isotope systematics is consistent with previous observations, showing a stark disparity between northern Cd‐rich high‐nutrient low‐chlorophyll waters and Cd‐depleted waters of the subtropical and equatorial Pacific. Away from the margin, an open system model ably describes data in Cd‐depleted surface waters, but atmospheric inputs of isotopically light Cd likely play an important role in setting surface Cd isotope ratios (δ¹¹⁴Cd) at the lowest Cd concentrations. Below the surface, Southern Ocean processes and water mass mixing are the dominant control on Pacific Cd and δ¹¹⁴Cd distributions. Cd‐depleted Antarctic Intermediate Water has a far‐reaching effect on North Pacific intermediate waters as far as 47°N, contrasting with northern‐sourced Cd signatures in North Pacific Intermediate Water. Finally, we show that the previously identified negative Cd* signal at depth in the North Pacific is associated with the PO₄maximum and is thus a consequence of an integrated regeneration signal of Cd and PO₄at a slightly lower Cd:P ratio than the deep ocean ratio (0.35 mmol mol⁻¹), rather than being related to in situ removal processes in low‐oxygen waters. 

Abstract Atmospheric deposition represents a major input for micronutrient trace elements (TEs) to the surface ocean and is often quantified indirectly through measurements of aerosol TE concentrations. Sea spray aerosol (SSA) dominates aerosol mass concentration over much of the global ocean, but few studies have assessed its contribution to aerosol TE loading, which could result in overestimates of “new” TE inputs. Low‐mineral aerosol concentrations measured during the U.S. GEOTRACES Pacific Meridional Transect (GP15; 152°W, 56°N to 20°S), along with concurrent towfish sampling of surface seawater, provided an opportunity to investigate this aspect of TE biogeochemical cycling. Central Pacific Ocean surface seawater Al, V, Mn, Fe, Co, Ni, Cu, Zn, and Pb concentrations were combined with aerosol Na data to calculate a “recycled” SSA contribution to aerosol TE loading. Only vanadium was calculated to have a SSA contribution averaging >1% along the transect (mean of 1.5%). We derive scaling factors from previous studies on TE enrichments in the sea surface microlayer and in freshly produced SSA to assess the broader potential for SSA contributions to aerosol TE loading. Maximum applied scaling factors suggest that SSA could contribute significantly to the aerosol loading of some elements (notably V, Cu, and Pb), while for others (e.g., Fe and Al), SSA contributions largely remained <1%. Our study highlights that a lack of focused measurements of TEs in SSA limits our ability to quantify this component of marine aerosol loading and the associated potential for overestimating new TE inputs from atmospheric deposition. 

Abstract The surface waters of the Arctic Ocean include an important inventory of freshwater from rivers, sea ice melt, and glacial meltwaters. While some freshwaters are mixed directly into the surface ocean, cryospheric reservoirs, such as snow, sea ice, and melt ponds act as incubators for trace metals, as well as potential sources to the surface ocean upon melting. The availability and reactivity of these metals depends on their speciation, which may vary across each pool or undergo transformation upon mixing. We present here baseline measurements of colloidal (∼0.003–0.200 μm) iron (Fe), zinc (Zn), nickel (Ni), copper (Cu), cadmium (Cd), and manganese (Mn) in snow, sea ice, melt ponds, and the underlying seawater. We consider both the total concentration of colloidal metals ([cMe]) in each cryospheric reservoir and the contribution of cMe to the overall dissolved metal phase (%cMe). Notably, snow contained higher (cMe) as well as higher %cMe relative to seawater for metals such as Fe and Zn across most stations. Stations close to the North Pole had relatively high aerosol deposition, imparting high (cFe) and (cZn), as well as high %cFe, %cZn, %cMn, and %cCd (>80%). In contrast, surface seawater concentrations of Cd, Cu, Mn, and Ni were dominated by the soluble phase (<0.003 μm), suggesting little impact of cMe from the melting cryosphere, or rapid aggregation/disaggregation dynamics within surface waters leading to the loss of cMe. This has important implications for how trace metal biogeochemistry speciation and thus fluxes may change in a future ice‐free Arctic Ocean.