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Fire regimes respond to both climate and human land management practice changes, in turn modifying land cover distributions, surface albedo, carbon storage, and emissions. Much attention has recently been given to the health and climate impacts of fires, but fires are also an important source of nutrients, such as iron and phosphorus, to both land and ocean biospheres. Fires therefore create important feedbacks within the Earth system. Here we discuss recent developments showing how fires are a previously underestimated source of limiting nutrients, providing up to half the annual deposited amount of soluble iron and soluble phosphorus to southern oceans and the Amazon, respectively. Fire can therefore stimulate ocean productivity by providing long range transport of essential nutrients, released from the vegetation burned and entrained with dust from the surrounding environment, to remote regions. We considered the impact of human activity on soluble iron deposition for the past (c.1750 CE), present (c.2010 CE), and future (c.2100 CE). We find that the global carbon cycle and climate response is dominated by changes to primary productivity within the Southern Ocean (>30ºS) and that the carbon export efficiency (gram of carbon sequestered per gram of soluble iron added) for this region is 43% larger when altering fire emissions compared to altering dust emissions. Results suggest that modelling past and future changes in biogeochemical cycles should incorporate information on how fires, and the nutrients carried within their plumes, respond to changes in climate.

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.

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., Metal dissolution from atmospheric aerosol deposition plays an important role in enhancing and inhibiting phytoplankton growth and community structure. Here, the authors review the impacts of trace metal leaching from natural and anthropogenic aerosols on marine microorganisms over short and long timescales.

Atmospheric iron affects the global carbon cycle by modulating ocean biogeochemistry through the deposition of soluble iron to the ocean. Iron emitted by anthropogenic (fossil fuel) combustion is a source of soluble iron that is currently considered less important than other soluble iron sources, such as mineral dust and biomass burning. Here we show that the atmospheric burden of anthropogenic combustion iron is 8 times greater than previous estimates by incorporating recent measurements of anthropogenic magnetite into a global aerosol model. This new estimation increases the total deposition flux of soluble iron to southern oceans (30–90 °S) by 52%, with a larger contribution of anthropogenic combustion iron than dust and biomass burning sources. The direct radiative forcing of anthropogenic magnetite is estimated to be 0.021 W m−2 globally and 0.22 W m−2 over East Asia. Our results demonstrate that anthropogenic combustion iron is a larger and more complex climate forcer than previously thought, and therefore plays a key role in the Earth system., As a source of soluble iron, anthropogenic combustion iron is considered less important than natural sources. Here, the authors combine new measurements with a global aerosol model and show the atmospheric burden of anthropogenic combustion iron to be 8 times greater than previous estimates.

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.

Air pollution creates high Fe solubility in pyrogenic aerosols, raising the flux of biologically essential Fe to the oceans., 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.

The global cycle of desert dust aerosols responds strongly to climate and human perturbations, and, in turn, impacts climate and biogeochemistry. Here we focus on desert dust size distributions, how these are characterized, emitted from the surface, evolve in the atmosphere, and impact climate and biogeochemistry. Observations, theory and global model results are synthesized to highlight the evolution and impact of dust sizes. Individual particles sizes are, to a large extent, set by the soil properties and the mobilization process. The lifetime of different particle sizes controls the evolution of the size distribution as the particles move downwind, as larger particles fall out more quickly. The dust size distribution strongly controls the radiative impact of the aerosols, as well as their interactions with clouds. The size of particles controls how far downwind they travel, and thus their ability to impact biogeochemistry downwind of the source region. © 2013 The Authors.

© Author(s) 2015. CC Attribution 3.0 License. Trace element deposition from desert dust has important impacts on ocean primary productivity, the quantification of which could be useful in determining the magnitude and sign of the biogeochemical feedback on radiative forcing. However, the impact of elemental deposition to remote ocean regions is not well understood and is not currently included in global climate models. In this study, emission inventories for eight elements primarily of soil origin, Mg, P, Ca, Mn, Fe, K, Al, and Si are determined based on a global mineral data set and a soil data set. The resulting elemental fractions are used to drive the desert dust model in the Community Earth System Model (CESM) in order to simulate the elemental concentrations of atmospheric dust. Spatial variability of mineral dust elemental fractions is evident on a global scale, particularly for Ca. Simulations of global variations in the Ca / Al ratio, which typically range from around 0.1 to 5.0 in soils, are consistent with observations, suggesting that this ratio is a good signature for dust source regions. The simulated variable fractions of chemical elements are sufficiently different; estimates of deposition should include elemental variations, especially for Ca, Al and Fe. The model results have been evaluated with observations of elemental aerosol concentrations from desert regions and dust events in non-dust regions, providing insights into uncertainties in the modeling approach. The ratios between modeled and observed elemental fractions range from 0.7 to 1.6, except for Mg and Mn (3.4 and 3.5, respectively). Using the soil database improves the correspondence of the spatial heterogeneity in the modeling of several elements (Ca, Al and Fe) compared to observations. Total and soluble dust element fluxes to different ocean basins and ice sheet regions have been estimated, based on the model results. The annual inputs of soluble Mg, P, Ca, Mn, Fe and K associated with dust using the mineral data set are 0.30 Tg, 16.89 Gg, 1.32 Tg, 22.84 Gg, 0.068 Tg, and 0.15 Tg to global oceans and ice sheets.

© 2014. The Authors. Aerosol-climate interactions constitute one of the major sources of uncertainty in assessing changes in aerosol forcing in the anthropocene as well as understanding glacial-interglacial cycles. Here we focus on improving the representation of mineral dust in the Community Atmosphere Model and assessing the impacts of the improvements in terms of direct effects on the radiative balance of the atmosphere. We simulated the dust cycle using different parameterization sets for dust emission, size distribution, and optical properties. Comparing the results of these simulations with observations of concentration, deposition, and aerosol optical depth allows us to refine the representation of the dust cycle and its climate impacts. We propose a tuning method for dust parameterizations to allow the dust module to work across the wide variety of parameter settings which can be used within the Community Atmosphere Model. Our results include a better representation of the dust cycle, most notably for the improved size distribution. The estimated net top of atmosphere direct dust radiative forcing is -0.23 ± 0.14 W/m2for present day and -0.32 ± 0.20 W/m2at the Last Glacial Maximum. From our study and sensitivity tests, we also derive some general relevant findings, supporting the concept that the magnitude of the modeled dust cycle is sensitive to the observational data sets and size distribution chosen to constrain the model as well as the meteorological forcing data, even within the same modeling framework, and that the direct radiative forcing of dust is strongly sensitive to the optical properties and size distribution used.

The mineralogy of desert dust is important due to its effect on radiation, clouds and biogeochemical cycling of trace nutrients. This study presents the simulation of dust radiative forcing as a function of both mineral composition and size at the global scale, using mineral soil maps for estimating emissions. Externally mixed mineral aerosols in the bulk aerosol module in the Community Atmosphere Model version 4 (CAM4) and internally mixed mineral aerosols in the modal aerosol module in the Community Atmosphere Model version 5.1 (CAM5) embedded in the Community Earth System Model version 1.0.5 (CESM) are speciated into common mineral components in place of total dust. The simulations with mineralogy are compared to available observations of mineral atmospheric distribution and deposition along with observations of clear-sky radiative forcing efficiency. Based on these simulations, we estimate the all-sky direct radiative forcing at the top of the atmosphere as + 0.05 Wm−2 for both CAM4 and CAM5 simulations with mineralogy. We compare this to the radiative forcing from simulations of dust in release versions of CAM4 and CAM5 (+0.08 and +0.17 Wm−2) and of dust with optimized optical properties, wet scavenging and particle size distribution in CAM4 and CAM5, −0.05 and −0.17 Wm−2, respectively. The ability to correctly include the mineralogy of dust in climate models is hindered by its spatial and temporal variability as well as insufficient global in situ observations, incomplete and uncertain source mineralogies and the uncertainties associated with data retrieved from remote sensing methods.

Atmospheric aerosol deposition is an important source of nutrients and pollution to many continental and marine ecosystems. Humans have heavily perturbed the cycles of several important aerosol species, potentially affecting terrestrial and marine carbon budgets and consequently climate. The most ecologically important aerosol elements impacted by humans are nitrogen, sulfur, iron, phosphorus, and base cations. Here, we review the latest research on the modification of the atmospheric cycles of these aerosols and their resulting effects on continental and marine ecosystems. Recent studies have improved our understanding of how humans have perturbed atmospheric aerosol cycles and how they may continue to evolve in the future. Research in both aquatic and terrestrial environments has highlighted the role of atmospheric deposition as a nutrient subsidy, with effects on ecosystem productivity. These studies further emphasize the importance of local biogeochemical conditions and biota species composition to the regional responses to aerosol deposition. The size of the impact of anthropogenic aerosol deposition on the carbon cycle and the resulting climate forcing is at present not well understood. It is estimated that increases in nutrient subsidies from atmospheric deposition across all ecosystems are causing an increase in carbon dioxide uptake between 0.2 and 1.5 PgC/year. As aerosol emissions from industrial sources are reduced to improve air quality, these enhancements in carbon uptake may be reduced in the future leading to reduced carbon dioxide emission offsets. However, large uncertainties remain, not only because of limited information on how humans have modified and will modify aerosol emissions, but also because of a lack of quantitative understanding of how aerosol deposition impacts carbon cycling in many ecosystems.

This work reports on the current status of global modelling of iron (Fe) deposition fluxes and atmospheric concentrations and 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 have 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) emissions 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 (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 mineral dust and combustion aerosols together. The multi model ensemble global TFe and LFe deposition fluxes into the global ocean are calculated to be ~ 15 Tg-Fe yr−1 and ~ 0.3 Tg-Fe yr−1, respectively. 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 parametrizations of Fe-containing aerosols. The model comparison with aerosol Fe observations over oceanic regions indicate that most models overestimate surface level TFe mass concentrations near the 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 loading near and downwind from the dust source regions, with the mean normalized bias for the Northern Hemisphere (~ 14), larger than 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.