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Funding: SL, AB and HP report financial support was provided by Natural Environment Research Council. Anthropogenic activities have significantly enhanced atmospheric metal inputs to the ocean, which has potentially important consequences for marine ecosystems. This study assesses the potential of Zn and Cu isotope compositions to distinguish between natural and anthropogenic atmospheric inputs of these metals to the surface ocean. To this end, the isotopic compositions of Zn and Cu in aerosols collected from the eastern tropical Atlantic Ocean on the GEOTRACES GA06 cruise are examined. Enrichment factors and fractional solubility measurements indicate the presence of a significant anthropogenic component in the aerosols collected furthest from the North African dust plume for both Zn and Cu. The mean δ65CuNIST SRM 976 for the fully digested aerosols is +0.07 ± 0.39 ‰ (n = 9, 2 SD), which is indistinguishable from the lithogenic value, and implies that Cu isotopes are not an effective tracer of aerosol sources in this region. The mean δ66ZnJMC-Lyon value for the aerosols that underwent a total digestion is +0.17 ± 0.22 ‰ (n = 11, 2 SD). The aerosols leached with ammonium acetate have similar Zn isotope compositions, with a mean of +0.15 ± 0.16 ‰ (n = 7, 2 SD). The aerosols were collected in a region with prevalent mineral dust but, despite this, exhibit isotopically lighter Zn than lithogenic Zn with δ66Zn ≈ +0.3 ‰. When coupled with the previously published Pb isotope data, the aerosols exhibit coupled Zn-Pb isotope systematics that are indicative of mixing between mineral dust (δ66Zn = +0.28 ‰ and 206Pb/207Pb = 1.205) and anthropogenic emissions (δ66Zn = −0.22 ‰ and 206Pb/207Pb = 1.129). This demonstrates the potential of Zn isotopes to trace atmospheric Zn inputs from anthropogenic sources to the surface ocean. Publisher PDF

Funding: This work was funded by a Royal Society International Collaboration Award (No. IC160088) to G. M. Henderson. The Irrawaddy (Ayeyarwaddy) and Salween (Thanlwin) globally rank among the largest rivers for supplying dissolved and particulate material to the ocean. Along with the Sittaung and Kaladan rivers they have societal importance to Myanmar in terms water sources and food production. Despite their importance for global biogeochemical cycles and the ~50 million people who live in their catchments, the chemistry of these rivers is poorly known. This study presents a comprehensive survey of dissolved (

Funding: The ISSS-08 program was supported by the Knut and Alice Wallenberg Foundation, the Far Eastern Branch of the Russian Academy of Sciences and the Swedish Research Council (VR contract 621–e2004-4283). Tracing riverine freshwater transport pathways within the Arctic Ocean is key to understanding changes in Arctic Ocean freshwater inventories. Dissolved Ba concentrations have been used in this capacity but are compromised by non-conservative processes. To assess the potential for Ba isotopes to provide insights into the impact of such processes on Arctic Ocean dissolved Ba inventories, Ba concentration and isotope data for surface seawater samples from the Siberian Shelf and Bering Sea/Strait are presented. These samples capture the mixing of riverine freshwater discharged by the rivers Yenisey, Lena and Ob, with Atlantic and Pacific derived seawater, which are traced by relationships between salinity, Ba concentration and δ138/134Ba. The δ138/134Ba of net river inputs, following modification by estuarine processes, are constrained to be 0.31 ± 0.04‰, 0.20 ± 0.06‰ and 0.23 ± 0.04‰, for the rivers Yenisey, Lena and Ob respectively. These values are used to estimate an average δ138/134Ba for Eurasian river freshwater input to the Arctic Ocean of 0.23 ± 0.04‰. The Ba concentration and δ138/134Ba of Lena River freshwater transported across the Laptev Sea are modified by non-conservative processes. These non-conservative processes do not result in distinctive modification of dissolved Ba concentration-δ138/134Ba mixing relationships between Eurasian riverine freshwater and Arctic seawater, which unfortunately limits the potential of Ba isotopes to improve tracing riverine freshwater sources in the central Arctic Ocean basins using dissolved Ba inventories. More generally the results of this study help advance understanding of Ba isotope cycling in the environment and their development as an emerging tracer of marine processes. Postprint

Funding: Luke Bridgestock was supported by a Leverhulme Trust Early Career Fellowship (ECF-2019-049) for part of this research. The collection of Johor River estuary samples was supported by funding from the Singapore National Research Foundation (NRF), Prime Minister's Office, under the Marine Science Research and Development Programme (Project MSRDP-03) and the Royal Society's Commonwealth Science Grant (CSC\R1\170048). The IAEA is grateful for the support provided to its Environment Laboratories by the Government of the Principality of Monaco. Barium (Ba) isotope variations offer the potential to trace environmental processes, including long-term changes in river discharge and marine export production. Riverine inputs are an important source of dissolved Ba to the ocean, which we estimate to be ~10 to 20 Gmol yr−1. A large fraction (~20 to 75%) of this net riverine dissolved Ba flux to the ocean is derived from estuarine processes, in particular the release of exchangeable Ba from riverine suspended particles due to exchange with major cations in seawater. Despite the importance of this process for controlling the input of dissolved Ba to the ocean, its impact on the δ138/134Ba of net riverine dissolved Ba fluxes remains unknown. To address this observational gap, Ba concentration and isotope data from across the estuarine mixing zones of the Amazon (Brazil), Fly (Papua New Guinea) and Johor (Malaysia) Rivers are presented. Desorption from suspended riverine particles releases Ba with δ138/134Ba 0.2 to 0.3‰ lower than corresponding river dissolved loads, modifying the isotope composition of net riverine dissolved Ba fluxes that reach the ocean. This offset likely represents an isotope fractionation accompanying the adsorption of Ba by particulate phases within river catchments, which can explain the systematic enrichment of heavier Ba isotopes in river dissolved loads relative to weathering lithologies. River dissolved loads are also systematically offset to higher δ138/134Ba than the main oceanic Ba sink: burial of BaSO4 in marine sediment. This represents an apparent imbalance in the modern marine Ba isotope budget. Our results suggest that accounting for modification of the δ138/134Ba of net riverine Ba fluxes to the ocean by estuarine processes is likely to play a key role towards balancing the modern marine Ba isotope budget. Postprint