Aerosol trace metal leaching and impacts on marine microorganisms

Metal dissolution from atmospheric aerosol deposition to the oceans is important in enhancing and inhibiting phytoplankton growth rates and modifying plankton community structure, thus impacting marine biogeochemistry. Here we review the current state of knowledge on the causes and effects of the leaching of multiple trace metals from natural and anthropogenic aerosols. Aerosol deposition is considered both on short timescales over which phytoplankton respond directly to aerosol metal inputs, as well as longer timescales over which biogeochemical cycles are affected by aerosols

Pyrogenic iron: The missing link to high iron solubility in aerosols

Atmospheric deposition is a source of potentially bioavailable iron (Fe) and thus can partially control biological productivity in large parts of the ocean. However, the explanation of observed high aerosol Fe solubility compared to that in soil particles is still controversial, as several hypotheses have been proposed to explain this observation. Here, a statistical analysis of aerosol Fe solubility estimated from four models and observations compiled from multiple field campaigns suggests that pyrogenic aerosols are the main sources of aerosols with high Fe solubility at low concentration. Additionally, we find that field data over the Southern Ocean display a much wider range in aerosol Fe solubility compared to the models, which indicate an underestimation of labile Fe concentrations by a factor of 15. These findings suggest that pyrogenic Fe-containing aerosols are important sources of atmospheric bioavailable Fe to the open ocean and crucial for predicting anthropogenic perturbations to marine productivity

Impact of Changes to the Atmospheric Soluble Iron Deposition Flux on Ocean Biogeochemical Cycles in the Anthropocene

Iron can be a growth‐limiting nutrient for phytoplankton, modifying rates of net primary production, nitrogen fixation, and carbon export ‐ highlighting the importance of new iron inputs from the atmosphere. The bioavailable iron fraction depends on the emission source and the dissolution during transport. The impacts of anthropogenic combustion and land use change on emissions from industrial, domestic, shipping, desert, and wildfire sources suggest that Northern Hemisphere soluble iron deposition has likely been enhanced between 2% and 68% over the Industrial Era. If policy and climate follow the intermediate Representative Concentration Pathway 4.5 trajectory, then results suggest that Southern Ocean (>30°S) soluble iron deposition would be enhanced between 63% and 95% by 2100. Marine net primary productivity and carbon export within the open ocean are most sensitive to changes in soluble iron deposition in the Southern Hemisphere; this is predominantly driven by fire rather than dust iron sources. Changes in iron deposition cause large perturbations to the marine nitrogen cycle, up to 70% increase in denitrification and 15% increase in nitrogen fixation, but only modestly impacts the carbon cycle and atmospheric CO2 concentrations (1–3 ppm). Regionally, primary productivity increases due to increased iron deposition are often compensated by offsetting decreases downstream corresponding to equivalent changes in the rate of phytoplankton macronutrient uptake, particularly in the equatorial Pacific. These effects are weaker in the Southern Ocean, suggesting that changes in iron deposition in this region dominates the global carbon cycle and climate response

Atmospheric processing of iron in mineral and combustion aerosols: development of an intermediate-complexity mechanism suitable for Earth system models

Atmospheric processing of iron in dust and combustion aerosols is simulated using an intermediate-complexity soluble iron mechanism designed for Earth system models. The solubilization mechanism includes both a dependence on aerosol water pH and in-cloud oxalic acid. The simulations of size-resolved total, soluble and fractional iron solubility indicate that this mechanism captures many but not all of the features seen from cruise observations of labile iron. The primary objective was to determine the extent to which our solubility scheme could adequately match observations of fractional iron solubility. We define a semi-quantitative metric as the model mean at points with observations divided by the observational mean (MMO). The model is in reasonable agreement with observations of fractional iron solubility with an MMO of 0.86. Several sensitivity studies are performed to ascertain the degree of complexity needed to match observations; including the oxalic acid enhancement is necessary, while different parameterizations for calculating model oxalate concentrations are less important. The percent change in soluble iron deposition between the reference case (REF) and the simulation with acidic processing alone is 63.8%, which is consistent with previous studies. Upon deposition to global oceans, global mean combustion iron solubility to total fractional iron solubility is 8.2%; however, the contribution of fractional iron solubility from combustion sources to ocean basins below 15°S is approximately 50%. We conclude that, in many remote ocean regions, sources of iron from combustion and dust aerosols are equally important. Our estimates of changes in deposition of soluble iron to the ocean since preindustrial climate conditions suggest roughly a doubling due to a combination of higher dust and combustion iron emissions along with more efficient atmospheric processing.We would like to acknowledge the support of DOE DE-SC0006735 and NSF 1049033. Carlos Pérez García-Pando acknowledges long-term support from the AXA Research Fund through the AXA Chair on Sand and Dust Storms, as well as the support received through the Ramón y Cajal program (grant RYC-2015-18690) of the Spanish Ministry of Economy and Competitiveness.Peer Reviewe

Data from: Recent (1980-to-2015) trends and variability in daily-to-interannual soluble iron deposition from dust, fire, and anthropogenic sources

Thumbnail image credit: NASA Earth Observatory images by Joshua Stevens, using GEOS data from the Global Modeling and Assimilation Office at NASA GSFC, https://gmao.gsfc.nasa.gov/.The iron cycle is a key component of the Earth system. Yet how variable the atmospheric flux of soluble (bioaccessible) iron into oceans is, and how this variability is modulated by human activity and a changing climate, is not well-known. Quantifying soluble iron daily-to-interannual deposition variability from all major iron sources, not only dust, will advance quantification of changes in marine biogeochemistry in response to the continuing human perturbation to the Earth System. The data in this repository relates to Hamilton et al. (2020) which characterized Satellite Era (1980-to-2015) daily-to-interannual modelled soluble iron emission and deposition variability from both pyrogenic (fires and anthropogenic combustion) and dust sources. Multi-model monthly mean soluble iron and dust deposition data is provided, as presented in the main manuscript. Also provided is daily deposition data for CAM6. A new transient monthly varying (1980 to 2015) anthropogenic (sum of combustion and metal smelting) iron emission data set was developed for this study, that data set is also included here.DSH, LL, and NMM would like to acknowledge support from DE-SC000679, DE-SC0016362, and Cornell Atkinson Center for Sustainability funding. JFK acknowledges support from National Science Foundation (NSF) grants 1552519 and 1856389. HM was supported by the Ministry of Education, Culture, Sports, Science, and Technology and the Japan Society for the Promotion of Science (MEXT/JSPS) KAKENHI Grant Numbers JP17H04709 and JP19H05699, by the MEXT Arctic Challenge for Sustainability (ArCS) and ArCS-II projects, and by the Environment Research and Technology Development Fund (2–1703 and 2-2003) of the Environmental Restoration and Conservation Agency

Climate-driven oscillation of phosphorus and iron limitation in the North Pacific Subtropical Gyre

The supply of nutrients is a fundamental regulator of ocean productivity and carbon sequestration. Nutrient sources, sinks, residence times, and elemental ratios vary over broad scales, including those resulting from climate-driven changes in upper water column stratification, advection, and the deposition of atmospheric dust. These changes can alter the proximate elemental control of ecosystem productivity with cascading ecological effects and impacts on carbon sequestration. Here, we report multidecadal observations revealing that the ecosystem in the eastern region of the North Pacific Subtropical Gyre (NPSG) oscillates on subdecadal scales between inorganic phosphorus (Pi) sufficiency and limitation, when Pi concentration in surface waters decreases below 50–60 nmol?kg?1. In situ observations and model simulations suggest that sea-level pressure changes over the northwest Pacific may induce basin-scale variations in the atmospheric transport and deposition of Asian dust-associated iron (Fe), causing the eastern portion of the NPSG ecosystem to shift between states of Fe and Pi limitation. Our results highlight the critical need to include both atmospheric and ocean circulation variability when modeling the response of open ocean pelagic ecosystems under future climate change scenarios

Annual mean soluble iron deposition and ocean BGC response for each case in Hamilton et al. (2020)

Iron can be a growth‐limiting nutrient for phytoplankton, modifying rates of net primary production, nitrogen fixation, and carbon export, highlighting the importance of new iron inputs from the atmosphere. The bioavailable iron fraction depends on the emission source and the dissolution during transport. The impacts of anthropogenic combustion and land use change on emissions from industrial, domestic, shipping, desert, and wildfire sources suggest that Northern Hemisphere soluble iron deposition has likely been enhanced between 2 to 68% over the Industrial Era. If policy and climate follow the intermediate Representative Concentration Pathway 4.5 trajectory then results suggest that Southern Ocean (>30°S) soluble iron deposition would be enhanced between 63 to 95% by 2100. Marine net primary productivity and carbon export within the open ocean are most sensitive to changes in soluble iron deposition in the Southern Hemisphere; this is predominantly driven by fire rather than dust iron sources. Changes in iron deposition cause large perturbations to the marine nitrogen cycle, up to 70% increase in denitrification and 15% increase in nitrogen fixation, but only modestly impacts the carbon cycle and atmospheric CO2 concentrations (1‐3 ppm). Regionally, primary productivity increases due to increased iron deposition are often compensated by offsetting decreases downstream corresponding to equivalent changes in the rate of phytoplankton macronutrient uptake, particularly in the equatorial Pacific. These effects are weaker in the Southern Ocean, suggesting that changes in iron deposition in this region dominates the global carbon cycle and climate response.This work was supported by Department of Energy (DOE) and National Science Foundation (NSF) grants for atmospheric deposition impacts on ocean biogeochemistry (DE-Sc0016362; NSF 1049033; CCF-1522054). DSH was also supported by the Atkinson Center for a Sustainable Future. JKM was also supported by DOE grant DE-SC0016539. AA would like to thank the Helmholtz Foundation, its ATMO programme and its impulse and integration fund. TCB and SDR thank the NSF grant (1049033) for its support. This material is based upon work supported by the National Center for Atmospheric Research, which is a major facility sponsored by the National Science Foundation under Cooperative Agreement No. 1852977

Reviews and syntheses: the GESAMP atmospheric iron deposition model intercomparison study

Abstract. This work reports on the current status of the global modeling of iron (Fe) deposition fluxes and atmospheric concentrations and the analyses of the differences between models, as well as between models and observations. A total of four global 3-D chemistry transport (CTMs) and general circulation (GCMs) models participated in this intercomparison, in the framework of the United Nations Joint Group of Experts on the Scientific Aspects of Marine Environmental Protection (GESAMP) Working Group 38, “The Atmospheric Input of Chemicals to the Ocean”. The global total Fe (TFe) emission strength in the models is equal to ∼72 Tg Fe yr−1 (38–134 Tg Fe yr−1) from mineral dust sources and around 2.1 Tg Fe yr−1 (1.8–2.7 Tg Fe yr−1) from combustion processes (the sum of anthropogenic combustion/biomass burning and wildfires). The mean global labile Fe (LFe) source strength in the models, considering both the primary emissions and the atmospheric processing, is calculated to be 0.7 (±0.3) Tg Fe yr−1, accounting for both mineral dust and combustion aerosols. The mean global deposition fluxes into the global ocean are estimated to be in the range of 10–30 and 0.2–0.4 Tg Fe yr−1 for TFe and LFe, respectively, which roughly corresponds to a respective 15 and 0.3 Tg Fe yr−1 for the multi-model ensemble model mean. The model intercomparison analysis indicates that the representation of the atmospheric Fe cycle varies among models, in terms of both the magnitude of natural and combustion Fe emissions as well as the complexity of atmospheric processing parameterizations of Fe-containing aerosols. The model comparison with aerosol Fe observations over oceanic regions indicates that most models overestimate surface level TFe mass concentrations near dust source regions and tend to underestimate the low concentrations observed in remote ocean regions. All models are able to simulate the tendency of higher Fe concentrations near and downwind from the dust source regions, with the mean normalized bias for the Northern Hemisphere (∼14), larger than that of the Southern Hemisphere (∼2.4) for the ensemble model mean. This model intercomparison and model–observation comparison study reveals two critical issues in LFe simulations that require further exploration: (1) the Fe-containing aerosol size distribution and (2) the relative contribution of dust and combustion sources of Fe to labile Fe in atmospheric aerosols over the remote oceanic regions

Pyrogenic iron: The missing link to high iron solubility in aerosols.

Atmospheric deposition is a source of potentially bioavailable iron (Fe) and thus can partially control biological productivity in large parts of the ocean. However, the explanation of observed high aerosol Fe solubility compared to that in soil particles is still controversial, as several hypotheses have been proposed to explain this observation. Here, a statistical analysis of aerosol Fe solubility estimated from four models and observations compiled from multiple field campaigns suggests that pyrogenic aerosols are the main sources of aerosols with high Fe solubility at low concentration. Additionally, we find that field data over the Southern Ocean display a much wider range in aerosol Fe solubility compared to the models, which indicate an underestimation of labile Fe concentrations by a factor of 15. These findings suggest that pyrogenic Fe-containing aerosols are important sources of atmospheric bioavailable Fe to the open ocean and crucial for predicting anthropogenic perturbations to marine productivity