Atmospheric Dry and Wet Deposition of Total Phosphorus to the Great Lakes.

Quantifying atmospheric loadings of total phosphorus (TP) to freshwater environments is essential to improve understanding of its fate and transport, and to mitigate the effects of excessive levels in freshwater ecosystems. To date, atmospheric deposition of TP in the U.S. is poorly characterized due to the lack of long-term deposition observations. Here, we integrate several historical datasets to develop an estimate of dry and wet deposition to the Great Lakes region. For dry deposition, we use TP concentrations in fine particulate matter (PM2.5) samples from fourteen land-based IMPROVE sites (2013-2020) upwind of the Great Lakes to provide new fine particle phosphorus dry deposition estimates. For wet deposition, we use TP concentrations in wet-only precipitation samples collected at eleven land-based sites (2001-2009) in the Great Lakes region. For both wet and dry deposition, a seasonal cycle is evident with higher concentrations in warmer and wetter months when compared to colder months. Additionally, there is an increasing gradient from north to south in wet deposition, likely driven by both higher precipitation and increased emissions near southern sites. Despite different sampling time periods, these updated observations can provide further constraints on the TP loadings to each of the five Great Lakes. We estimate annual deposition of TP to Lakes Superior, Michigan, Huron, Erie and Ontario at 526, 702, 495, 212, and 185 MTA per year, which is lower than prior estimates for Lakes Superior, Erie and Ontario, comparable for Lake Huron, and about two times greater for Lake Michigan. When considering only the contribution of fine particulate PM to the dry deposition, wet deposition dominated over dry at all lakes except for Lake Huron. However, prior global estimates suggest greater contributions from larger particles (PM10 and PM100), yet observations to validate these estimates over the Great Lakes are not available. Our findings indicate that dry deposition of a range of particle sizes are needed to constrain the total atmospheric deposition of TP over the Great Lakes.

Phases in fine volcanic ash.

Volcanic ash emissions impact atmospheric processes, depositional ecosystems, human health, and global climate. These effects are sensitive to the size and composition of the ash; however, datasets describing the constituent phases over size ranges relevant for atmospheric transport and widely distributed impacts are practically nonexistent. Here, we present results of X-ray diffraction measurements on size-separated fractions of 40 ash samples from VEI 2-6 eruptions. We characterize changes in phase fractions with grainsize, tectonic setting, and whole-rock SiO2. For grainsizes < 45 µm, average fractions of crystalline silica and surface salts increased while glass and iron oxides decreased with respect to the bulk sample. Samples from arc and intraplate settings are distinguished by feldspar and clinopyroxene fractions (determined by different crystallization sequences) which, together with glass, comprise 80-100% of most samples. We provide a dataset to approximate glass-free proportions of major crystalline phases; however, glass fractions are highly variable. To tackle this, we describe regressions between glass and major crystal phase fractions that help constrain the major phase proportions in volcanic ash with limited a priori information. Using our dataset, we find that pore-free ash density is well-estimated as a function of the clinopyroxene + Fe-oxide fraction, with median values of 2.67 ± 0.01 and 2.85 ± 0.03 g/cm3 for intraplate and arc samples, respectively. Finally, we discuss effects including atmospheric transport and alteration on modal composition and contextualize our proximal airfall ash samples with volcanic ash cloud properties. Our study helps constrain the atmospheric and environmental budget of the phases in fine volcanic ash and their effect on ash density, integral to refine our understanding of the impact of explosive volcanism on the Earth system from single eruptions to global modeling.

Photocatalytic chlorine atom production on mineral dust-sea spray aerosols over the North Atlantic.

Active chlorine in the atmosphere is poorly constrained and so is its role in the oxidation of the potent greenhouse gas methane, causing uncertainty in global methane budgets. We propose a photocatalytic mechanism for chlorine atom production that occurs when Sahara dust mixes with sea spray aerosol. The mechanism is validated by implementation in a global atmospheric model and thereby explaining the episodic, seasonal, and location-dependent 13C depletion in CO in air samples from Barbados [J.E. Mak, G. Kra, T. Sandomenico, P. Bergamaschi, J. Geophys. Res. Atmos. 108 (2003)], which remained unexplained for decades. The production of Cl can also explain the anomaly in the CO:ethane ratio found at Cape Verde [K. A. Read et al., J. Geophys. Res. Atmos. 114 (2009)], in addition to explaining the observation of elevated HOCl [M. J. Lawler et al., Atmos. Chem. Phys. 11, 7617-7628 (2011)]. Our model finds that 3.8 Tg(Cl) y-1 is produced over the North Atlantic, making it the dominant source of chlorine in the region; globally, chlorine production increases by 41%. The shift in the methane sink budget due to the increased role of Cl means that isotope-constrained top-down models fail to allocate 12 Tg y-1 (2% of total methane emissions) to 13C-depleted biological sources such as agriculture and wetlands. Since 2014, an increase in North African dust emissions has increased the 13C isotope of atmospheric CH4, thereby partially masking a much greater decline in this isotope, which has implications for the interpretation of the drivers behind the recent increase of methane in the atmosphere.

Global environmental implications of atmospheric methane removal through chlorine-mediated chemistry-climate interactions.

Atmospheric methane is both a potent greenhouse gas and photochemically active, with approximately equal anthropogenic and natural sources. The addition of chlorine to the atmosphere has been proposed to mitigate global warming through methane reduction by increasing its chemical loss. However, the potential environmental impacts of such climate mitigation remain unexplored. Here, sensitivity studies are conducted to evaluate the possible effects of increasing reactive chlorine emissions on the methane budget, atmospheric composition and radiative forcing. Because of non-linear chemistry, in order to achieve a reduction in methane burden (instead of an increase), the chlorine atom burden needs to be a minimum of three times the estimated present-day burden. If the methane removal target is set to 20%, 45%, or 70% less global methane by 2050 compared to the levels in the Representative Concentration Pathway 8.5 scenario (RCP8.5), our modeling results suggest that additional chlorine fluxes of 630, 1250, and 1880 Tg Cl/year, respectively, are needed. The results show that increasing chlorine emissions also induces significant changes in other important climate forcers. Remarkably, the tropospheric ozone decrease is large enough that the magnitude of radiative forcing decrease is similar to that of methane. Adding 630, 1250, and 1880 Tg Cl/year to the RCP8.5 scenario, chosen to have the most consistent current-day trends of methane, will decrease the surface temperature by 0.2, 0.4, and 0.6 °C by 2050, respectively. The quantity and method in which the chlorine is added, its interactions with climate pathways, and the potential environmental impacts on air quality and ocean acidity, must be carefully considered before any action is taken.

Stratospheric impacts on dust transport and air pollution in West Africa and the Eastern Mediterranean.

Saharan dust intrusions strongly impact Atlantic and Mediterranean coastal regions. Today, most operational dust forecasts extend only 2-5 days. Here we show that on timescales of weeks to months, North African dust emission and transport are impacted by sudden stratospheric warmings (SSWs), which establish a negative North Atlantic Oscillation-like surface signal. Chemical transport models show a large-scale dipolar dust response to SSWs, with the burden in the Eastern Mediterranean enhanced up to 30% and a corresponding reduction in West Africa. Observations of inhalable particulate (PM10) concentrations and aerosol optical depth confirm this dipole. On average, a single SSW causes 680-2460 additional premature deaths in the Eastern Mediterranean and prevents 1180-2040 premature deaths in West Africa from exposure to dust-source fine particulate (PM2.5). Currently, SSWs are predictable 1-2 weeks in advance. Altogether, the stratosphere represents an important source of subseasonal predictability for air quality over West Africa and the Eastern Mediterranean.

Improved Parameterization for the Size Distribution of Emitted Dust Aerosols Reduces Model Underestimation of Super Coarse Dust.

Aircraft measurement campaigns have revealed that super coarse dust (diameter >10 µm) surprisingly accounts for approximately a quarter of aerosols by mass in the atmosphere. However, most global aerosol models either underestimate or do not include super coarse dust abundance. To address this problem, we use brittle fragmentation theory to develop a parameterization for the emitted dust size distribution that includes emission of super coarse dust. We implement this parameterization in the Community Earth System Model (CESM) and find that it brings the model in good agreement with aircraft measurements of super coarse dust close to dust source regions. However, the CESM still underestimates super coarse dust in dust outflow regions. Thus, we conclude that the model underestimation of super coarse atmospheric dust is in part due to the underestimation of super coarse dust emission and likely in part due to errors in deposition processes.

Earth, Wind, Fire, and Pollution: Aerosol Nutrient Sources and Impacts on Ocean Biogeochemistry.

A key Earth system science question is the role of atmospheric deposition in supplying vital nutrients to the phytoplankton that form the base of marine food webs. Industrial and vehicular pollution, wildfires, volcanoes, biogenic debris, and desert dust all carry nutrients within their plumes throughout the globe. In remote ocean ecosystems, aerosol deposition represents an essential new source of nutrients for primary production. The large spatiotemporal variability in aerosols from myriad sources combined with the differential responses of marine biota to changing fluxes makes it crucially important to understand where, when, and how much nutrients from the atmosphere enter marine ecosystems. This review brings together existing literature, experimental evidence of impacts, and new atmospheric nutrient observations that can be compared with atmospheric and ocean biogeochemistry modeling. We evaluate the contribution and spatiotemporal variability of nutrient-bearing aerosols from desert dust, wildfire, volcanic, and anthropogenic sources, including the organic component, deposition fluxes, and oceanic impacts.

Changing atmospheric acidity as a modulator of nutrient deposition and ocean biogeochemistry.

Anthropogenic emissions to the atmosphere have increased the flux of nutrients, especially nitrogen, to the ocean, but they have also altered the acidity of aerosol, cloud water, and precipitation over much of the marine atmosphere. For nitrogen, acidity-driven changes in chemical speciation result in altered partitioning between the gas and particulate phases that subsequently affect long-range transport. Other important nutrients, notably iron and phosphorus, are affected, because their soluble fractions increase upon exposure to acidic environments during atmospheric transport. These changes affect the magnitude, distribution, and deposition mode of individual nutrients supplied to the ocean, the extent to which nutrient deposition interacts with the sea surface microlayer during its passage into bulk seawater, and the relative abundances of soluble nutrients in atmospheric deposition. Atmospheric acidity change therefore affects ecosystem composition, in addition to overall marine productivity, and these effects will continue to evolve with changing anthropogenic emissions in the future.

Constraining the atmospheric limb of the plastic cycle.

Plastic pollution is one of the most pressing environmental and social issues of the 21st century. Recent work has highlighted the atmosphere's role in transporting microplastics to remote locations [S. Allen et al., Nat. Geosci. 12, 339 (2019) and J. Brahney, M. Hallerud, E. Heim, M. Hahnenberger, S. Sukumaran, Science 368, 1257-1260 (2020)]. Here, we use in situ observations of microplastic deposition combined with an atmospheric transport model and optimal estimation techniques to test hypotheses of the most likely sources of atmospheric plastic. Results suggest that atmospheric microplastics in the western United States are primarily derived from secondary re-emission sources including roads (84%), the ocean (11%), and agricultural soil dust (5%). Using our best estimate of plastic sources and modeled transport pathways, most continents were net importers of plastics from the marine environment, underscoring the cumulative role of legacy pollution in the atmospheric burden of plastic. This effort uses high-resolution spatial and temporal deposition data along with several hypothesized emission sources to constrain atmospheric plastic. Akin to global biogeochemical cycles, plastics now spiral around the globe with distinct atmospheric, oceanic, cryospheric, and terrestrial residence times. Though advancements have been made in the manufacture of biodegradable polymers, our data suggest that extant nonbiodegradable polymers will continue to cycle through the earth's systems. Due to limited observations and understanding of the source processes, there remain large uncertainties in the transport, deposition, and source attribution of microplastics. Thus, we prioritize future research directions for understanding the plastic cycle.

Improved representation of the global dust cycle using observational constraints on dust properties and abundance.

Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, atmospheric models struggle to accurately represent its spatial and temporal distribution. These model errors are partially caused by fundamental difficulties in simulating dust emission in coarse-resolution models and in accurately representing dust microphysical properties. Here we mitigate these problems by developing a new methodology that yields an improved representation of the global dust cycle. We present an analytical framework that uses inverse modeling to integrate an ensemble of global model simulations with observational constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth. We then compare the inverse model results against independent measurements of dust surface concentration and deposition flux and find that errors are reduced by approximately a factor of two relative to current model simulations of the Northern Hemisphere dust cycle. The inverse model results show smaller improvements in the less dusty Southern Hemisphere, most likely because both the model simulations and the observational constraints used in the inverse model are less accurate. On a global basis, we find that the emission flux of dust with geometric diameter up to 20 µm (PM20) is approximately 5,000 Tg/year, which is greater than most models account for. This larger PM20 dust flux is needed to match observational constraints showing a large atmospheric loading of coarse dust. We obtain gridded data sets of dust emission, vertically integrated loading, dust aerosol optical depth, (surface) concentration, and wet and dry deposition fluxes that are resolved by season and particle size. As our results indicate that this data set is more accurate than current model simulations and the MERRA-2 dust reanalysis product, it can be used to improve quantifications of dust impacts on the Earth system.

Rooting carbon dioxide removal research in the social sciences.

Reports from a variety of bodies have highlighted the role that carbon dioxide removal (CDR) technologies and practices must play in order to try to avoid the worst effects of anthropogenic climate change. Research into the feasibility of these technologies is primarily undertaken by scholars in the natural sciences, yet, as we argue in this commentary, there is great value in collaboration between these scholars and their colleagues in the social sciences. Spurred by this belief, in 2019, a university and a non-profit organization organized and hosted a workshop in Washington, DC, intended to bring natural and physical scientists, technology developers, policy professionals and social scientists together to explore how to better integrate social science knowledge into the field of CDR research. The workshop sought to build interdisciplinary collaborations across CDR topics, draft new social science research questions and integrate and exchange disciplinary-specific terminology. But a snowstorm kept many social scientists who had organized the conference from making the trip in person. The workshop went on without them and organizers did the best they could to include the team remotely, but in the age before daily video calls, remote participation was not as successful as organizers had hoped. And thus, a workshop that was supposed to focus on social science integration moved on, without many of the social scientists who organized the event. The social scientists in the room were supposed to form the dominant voice but with so many stuck in a snow storm, the balance of expertise shifted, as it often does when social scientists collaborate with natural and physical scientists. The outcomes of that workshop, lessons learned and opportunities missed, form the basis of this commentary, and they collectively indicate the barriers to integrating the natural, physical and social sciences on CDR. As the need for rapid, effective and successful CDR has only increased since that time, we argue that CDR researchers from across the spectrum must come together in ways that simultaneously address the technical, social, political, economic and cultural elements of CDR development, commercialization, adoption and diffusion if the academy is to have a material impact on climate change in the increasingly limited window we have to address it.

African biomass burning is a substantial source of phosphorus deposition to the Amazon, Tropical Atlantic Ocean, and Southern Ocean.

The deposition of phosphorus (P) from African dust is believed to play an important role in bolstering primary productivity in the Amazon Basin and Tropical Atlantic Ocean (TAO), leading to sequestration of carbon dioxide. However, there are few measurements of African dust in South America that can robustly test this hypothesis and even fewer measurements of soluble P, which is readily available for stimulating primary production in the ocean. To test this hypothesis, we measured total and soluble P in long-range transported aerosols collected in Cayenne, French Guiana, a TAO coastal site located at the northeastern edge of the Amazon. Our measurements confirm that in boreal spring when African dust transport is greatest, dust supplies the majority of P, of which 5% is soluble. In boreal fall, when dust transport is at an annual minimum, we measured unexpectedly high concentrations of soluble P, which we show is associated with the transport of biomass burning (BB) from southern Africa. Integrating our results into a chemical transport model, we show that African BB supplies up to half of the P deposited annually to the Amazon from transported African aerosol. This observational study links P-rich BB aerosols from Africa to enhanced P deposition in the Amazon. Contrary to current thought, we also show that African BB is a more important source of soluble P than dust to the TAO and oceans in the Southern Hemisphere and may be more important for marine productivity, particularly in boreal summer and fall.

Tracing and constraining anthropogenic aerosol iron fluxes to the North Atlantic Ocean using iron isotopes.

Atmospheric dust is an important source of the micronutrient Fe to the oceans. Although relatively insoluble mineral Fe is assumed to be the most important component of dust, a relatively small yet highly soluble anthropogenic component may also be significant. However, quantifying the importance of anthropogenic Fe to the global oceans requires a tracer which can be used to identify and constrain anthropogenic aerosols in situ. Here, we present Fe isotope (δ56Fe) data from North Atlantic aerosol samples from the GEOTRACES GA03 section. While soluble aerosol samples collected near the Sahara have near-crustal δ56Fe, soluble aerosols from near North America and Europe instead have remarkably fractionated δ56Fe values (as light as -1.6‰). Here, we use these observations to fingerprint anthropogenic combustion sources, and to refine aerosol deposition modeling. We show that soluble anthropogenic aerosol Fe flux to the global surface oceans is highly likely to be underestimated, even in the dusty North Atlantic.

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 (P i ) sufficiency and limitation, when P i 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 P i 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.

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.

Evaluation of global simulations of aerosol particle and cloud condensation nuclei number, with implications for cloud droplet formation.

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011-2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of -24% and -35% for particles with dry diameters > 50 and > 120nm, as well as -36% and -34% for CCN at supersaturations of 0.2% and 1.0%, respectively. However, they seem to behave differently for particles activating at very low supersaturations (< 0.1 %) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN0.2) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120 nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40% during winter and 20% in summer. In contrast to the large spread in simulated aerosol particle and CCN number concentrations, the CDNC derived from simulated CCN spectra is less diverse and in better agreement with CDNC estimates consistently derived from the observations (average NMB -13% and -22% for updraft velocities 0.3 and 0.6 ms-1, respectively). In addition, simulated CDNC is in slightly better agreement with observationally derived values at lower than at higher updraft velocities (index of agreement 0.64 vs. 0.65). The reduced spread of CDNC compared to that of CCN is attributed to the sublinear response of CDNC to aerosol particle number variations and the negative correlation between the sensitivities of CDNC to aerosol particle number concentration (∂N d/∂N a) and to updraft velocity (∂N d/∂w). Overall, we find that while CCN is controlled by both aerosol particle number and composition, CDNC is sensitive to CCN at low and moderate CCN concentrations and to the updraft velocity when CCN levels are high. Discrepancies are found in sensitivities ∂N d/∂N a and ∂N d/∂w; models may be predisposed to be too "aerosol sensitive" or "aerosol insensitive" in aerosol-cloud-climate interaction studies, even if they may capture average droplet numbers well. This is a subtle but profound finding that only the sensitivities can clearly reveal and may explain inter-model biases on the aerosol indirect effect.

Black carbon radiative effects highly sensitive to emitted particle size when resolving mixing-state diversity.

Post-industrial increases in atmospheric black carbon (BC) have a large but uncertain warming contribution to Earth's climate. Particle size and mixing state determine the solar absorption efficiency of BC and also strongly influence how effectively BC is removed, but they have large uncertainties. Here we use a multiple-mixing-state global aerosol microphysics model and show that the sensitivity (range) of present-day BC direct radiative effect, due to current uncertainties in emission size distributions, is amplified 5-7 times (0.18-0.42 W m-2) when the diversity in BC mixing state is sufficiently resolved. This amplification is caused by the lifetime, core absorption, and absorption enhancement effects of BC, whose variability is underestimated by 45-70% in a single-mixing-state model representation. We demonstrate that reducing uncertainties in emission size distributions and how they change in the future, while also resolving modeled BC mixing state diversity, is now essential when evaluating BC radiative effects and the effectiveness of BC mitigation on future temperature changes.

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.

Anthropogenic combustion iron as a complex climate forcer.

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.