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Abstract. Sulfate and nitrate aerosols degrade air quality, modulate radiative forcing and the hydrological cycle, and affect biogeochemical cycles, yet their global cycles are poorly understood. Here, we examined trends in 21 years of aerosol measurements made at Ragged Point, Barbados, the easternmost promontory on the island located in the eastern Caribbean Basin. Though the site has historically been used to characterize African dust transport, here we focused on changes in nitrate and non-sea-salt (nss) sulfate aerosols from 1990–2011. Nitrate aerosol concentrations averaged over the entire period were stable at 0.59 µg m−3 ± 0.04 µg m−3, except for elevated nitrate concentrations in the spring of 2010 and during the summer and fall of 2008 due to the transport of biomass burning emissions from both northern and southern Africa to our site. In contrast, from 1990 to 2000, nss-sulfate decreased 30 % at a rate of 0.023 µg m−3 yr−1, a trend which we attribute to air quality policies enacted in the United States (US) and Europe. From 2000–2011, sulfate gradually increased at a rate of 0.021 µg m−3 yr−1 to pre-1990s levels of 0.90 µg m−3. We used the Community Multiscale Air Quality (CMAQ) model simulations from the EPA's Air QUAlity TimE Series (EQUATES) to better understand the changes in nss-sulfate after 2000. The model simulations estimate that increases in anthropogenic emissions from Africa explain the increase in nss-sulfate observed in Barbados. Our results highlight the need to better constrain emissions from developing countries and to assess their impact on aerosol burdens in remote source regions. 

Abstract Iron emissions from human activities, such as oil combustion and smelting, affect the Earth's climate and marine ecosystems. These emissions are difficult to quantify accurately due to a lack of observations, particularly in remote ocean regions. In this study, we used long‐term, near‐source observations in areas with a dominance of anthropogenic iron emissions in various parts of the world to better estimate the total amount of anthropogenic iron emissions. We also used a statistical source apportionment method to identify the anthropogenic components and their sub‐sources from bulk aerosol observations in the United States. We find that the estimates of anthropogenic iron emissions are within a factor of 3 in most regions compared to previous inventory estimates. Under‐ or overestimation varied by region and depended on the number of sites, interannual variability, and the statistical filter choice. Smelting‐related iron emissions are overestimated by a factor of 1.5 in East Asia compared to previous estimates. More long‐term iron observations and the consideration of the influence of dust and wildfires could help reduce the uncertainty in anthropogenic iron emissions estimates. 

Abstract. Aerosol particles are an important part of the Earth climate system, and their concentrations are spatially and temporally heterogeneous, as well as being variable in size and composition. Particles can interact with incoming solar radiation and outgoing longwave radiation, change cloud properties, affect photochemistry, impact surface air quality, change the albedo of snow and ice, and modulate carbon dioxide uptake by the land and ocean. High particulate matter concentrations at the surface represent an important public health hazard. There are substantial data sets describing aerosol particles in the literature or in public health databases, but they have not been compiled for easy use by the climate and air quality modeling community. Here, we present a new compilation of PM2.5 and PM10 surface observations, including measurements of aerosol composition, focusing on the spatial variability across different observational stations. Climate modelers are constantly looking for multiple independent lines of evidence to verify their models, and in situ surface concentration measurements, taken at the level of human settlement, present a valuable source of information about aerosols and their human impacts complementarily to the column averages or integrals often retrieved from satellites. We demonstrate a method for comparing the data sets to outputs from global climate models that are the basis for projections of future climate and large-scale aerosol transport patterns that influence local air quality. Annual trends and seasonal cycles are discussed briefly and are included in the compilation. Overall, most of the planet or even the land fraction does not have sufficient observations of surface concentrations – and, especially, particle composition – to characterize and understand the current distribution of particles. Climate models without ammonium nitrate aerosols omit ∼ 10 % of the globally averaged surface concentration of aerosol particles in both PM2.5 and PM10 size fractions, with up to 50 % of the surface concentrations not being included in some regions. In these regions, climate model aerosol forcing projections are likely to be incorrect as they do not include important trends in short-lived climate forcers. 

Abstract The role of manganese (Mn) in ecosystem carbon (C) biogeochemical cycling is gaining increasing attention. While soil Mn is mainly derived from bedrock, atmospheric deposition could be a major source of Mn to surface soils, with implications for soil C cycling. However, quantification of the atmospheric Mn cycle, which comprises emissions from natural (desert dust, sea salts, volcanoes, primary biogenic particles, and wildfires) and anthropogenic sources (e.g., industrialization and land‐use change due to agriculture), transport, and deposition, remains uncertain. Here, we use compiled emission data sets for each identified source to model and quantify the atmospheric Mn cycle by combining an atmospheric model and in situ atmospheric concentration measurements. We estimated global emissions of atmospheric Mn in aerosols (<10 μm in aerodynamic diameter) to be 1,400 Gg Mn year⁻¹. Approximately 31% of the emissions come from anthropogenic sources. Deposition of the anthropogenic Mn shortened Mn “pseudo” turnover times in 1‐m‐thick surface soils (ranging from 1,000 to over 10,000,000 years) by 1–2 orders of magnitude in industrialized regions. Such anthropogenic Mn inputs boosted the Mn‐to‐N ratio of the atmospheric deposition in non‐desert dominated regions (between 5 × 10⁻⁵and 0.02) across industrialized areas, but that was still lower than soil Mn‐to‐N ratio by 1–3 orders of magnitude. Correlation analysis revealed a negative relationship between Mn deposition and topsoil C density across temperate and (sub)tropical forests, consisting with atmospheric Mn deposition enhancing carbon respiration as seen in in situ biogeochemical studies. 

Here, we present the data and MixSIAR code that corresponds to the manuscript “Interannual variability in the source location of North African dust transported to the Amazon.” African dust is seasonally transported to the western Tropical Atlantic Ocean (TAO) and South America (SA), including the Amazon Basin. Leading hypotheses suggest that either the Western North African potential source area (PSA) or the Central North African PSA (e.g., Bodélé Depression) is the main source of dust transported to the Amazon. However, these notions remain largely untested with geochemical data. Here, we present a more nuanced hypothesis: both PSAs contribute dust to SA with precipitation and wind patterns determining the dominant source. Our premise is based upon two years of isotopic measurements (strontium and neodymium) of African dust collected in SA integrated into a statistical model in a Bayesian framework. With this approach, we identified strong interannual variability: while the Central PSA supplied 48% in winter 2016, a region within the Western PSA, which we suggest may be located near Niger, Mali, and Algeria accounts for 54% of transport in winter 2014. We propose the variability is due to the strength of the Libyan High and differing amounts of precipitation in the Gulf of Guinea and TAO between the two years. We anticipate that our work will lead to better constraints of dust nutrient deposition and subsequent carbon sequestration in the TAO and Amazon as well as improved model predictions of dust transport. Due to the connection between dust, precipitation, and wind patterns, our work can be used to link changes in climate with past changes in the source and magnitude of dust transported to the Amazon and TAO. This data is associated with the article: Barkley, A.E., Pourmand, A., Longman, J., Sharifi, A., Prospero, J.M., Panechou, K., Bakker, N., Drake, N., Guioiseau, D., Gaston, C.J. Interannual variability in the source location of North African dust transported to the Amazon. Submitted to the Proceedings of the National Academy of Sciences ## Description of the datasets The `data/` folder contains three data sets. `ds01` contains the data collected in this study from 34 samples including the dates of collection and Sr and eNd isotopic ratios. ## Metadata of the trajectory file ds01 is a *csv* file that contain 12 columns. Column 1 presents the date in the format ‘MM:DD:YYYY’ (e.g., 01-30-2014) that sample collection was initiated. Column 2 presents the date ‘MM:DD:YYYY’ (e.g., 01-31-2014) sample collection ended. Column 3 shows the mean 87Sr/86Sr ratio (unitless) measured and Column 4 shows the 95% confidence interval (CI) for each sample run in triplicate. Column 5 shows the 143Nd/144Nd isotopic ratio reported as epsilon neodymium (unitless) and Column 6 presents the 95% CI of the mean epsilon Nd. Columns 7, 9, and 11 show the lead (Pb) isotopic ratios normalized to 204Pb with their corresponding 95% CI in Columns 8, 10, and 12. 

Abstract African dust is transported to South America (SA) every winter and spring. Hypotheses suggest that either Western or Central North Africa (e.g., Bodélé Depression) is the main source of transported dust, yet these notions remain largely untested with geochemical data. Using 2 years of isotopic measurements (strontium and neodymium) of African dust collected in SA integrated into a statistical model, we identified strong interannual variability in dust source region. Central North Africa supplied 44% of long‐range transported dust in winter 2016 while the Western region accounted for 53% of dust in winter 2014. We propose the variability is due to differences in the strength of the Libyan High and precipitation over the Gulf of Guinea and Atlantic Ocean between the 2 years. Our findings can improve constraints of dust nutrient deposition and predictions of how changes in climate impact the source and magnitude of dust transported to the Amazon. 

Abstract The equatorial North Atlantic Ocean (NAO) is a nutrient‐limited ecosystem that relies on the deposition of long‐range transported iron (Fe)‐containing aerosols to stimulate primary productivity. Using microscopy, we characterized supermicron and supercoarse mode African aerosols transported to the western NAO in boreal winter/spring. We detected three particle types including African dust, primary biological aerosol particles, and freshwater diatoms (FDs). FDs contained 4% Fe by weight due to surficial dust inclusions that may be susceptible to chemical processing and dissolution. FDs were typically larger than dust particles and comprised 38% of particles between 10 and 18 μm in diameter. The low density, high surface‐area‐to‐volume ratio, and large aspect ratios of FD particles suggest a mechanism by which they can be carried great distances aloft. These same properties likely increase the residence time of FDs in surface waters thereby increasing the time for Fe dissolution and their potential impact on marine biogeochemical cycles.