Abstract. 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 2 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 a geometric diameter up to 20 µm (PM20) is approximately 5000 Tg yr−1, 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 datasets 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 dataset 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.

Abstract. The large uncertainty in the mineral dust direct radiative effect (DRE) hinders projections of future climate change due to anthropogenic activity. Resolving modeled dust mineral speciation allows for spatially and temporally varying refractive indices consistent with dust aerosol composition. Here, for the first time, we quantify the range in dust DRE at the top of the atmosphere (TOA) due to current uncertainties in the surface soil mineralogical content using a dust mineral-resolving climate model. We propagate observed uncertainties in soil mineral abundances from two soil mineralogy atlases along with the optical properties of each mineral into the DRE and compare the resultant range with other sources of uncertainty across six climate models. The shortwave DRE responds region-specifically to the dust burden depending on the mineral speciation and underlying shortwave surface albedo: positively when the regionally averaged annual surface albedo is larger than 0.28 and negatively otherwise. Among all minerals examined, the shortwave TOA DRE and single scattering albedo at the 0.44–0.63 µm band are most sensitive to the fractional contribution of iron oxides to the total dust composition. The global net (shortwave plus longwave) TOA DRE is estimated to be within −0.23 to +0.35 W m−2. Approximately 97 % of this range relates to uncertainty in the soil abundance of iron oxides. Representing iron oxide with solely hematite optical properties leads to an overestimation of shortwave DRE by +0.10 W m−2 at the TOA, as goethite is not as absorbing as hematite in the shortwave spectrum range. Our study highlights the importance of iron oxides to the shortwave DRE: they have a disproportionally large impact on climate considering their small atmospheric mineral mass fractional burden (∼2 %). An improved description of iron oxides, such as those planned in the Earth Surface Mineral Dust Source Investigation (EMIT), is thus essential for more accurate estimates of the dust DRE.

Abstract. Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, the relative contributions of the world's major source regions to the global dust cycle remain poorly constrained. This problem hinders accounting for the potentially large impact of regional differences in dust properties on clouds, the Earth's energy balance, and terrestrial and marine biogeochemical cycles. Here, we constrain the contribution of each of the world's main dust source regions to the global dust cycle. We use an analytical framework that integrates an ensemble of global aerosol model simulations with observationally informed constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth (DAOD). We obtain a dataset that constrains the relative contribution of nine major source regions to size-resolved dust emission, atmospheric loading, DAOD, concentration, and deposition flux. We find that the 22–29 Tg (1 standard error range) global loading of dust with a geometric diameter up to 20 µm is partitioned as follows: North African source regions contribute ∼ 50 % (11–15 Tg), Asian source regions contribute ∼ 40 % (8–13 Tg), and North American and Southern Hemisphere regions contribute ∼ 10 % (1.8–3.2 Tg). These results suggest that current models on average overestimate the contribution of North African sources to atmospheric dust loading at ∼ 65 %, while underestimating the contribution of Asian dust at ∼ 30 %. Our results further show that each source region's dust loading peaks in local spring and summer, which is partially driven by increased dust lifetime in those seasons. We also quantify the dust deposition flux to the Amazon rainforest to be ∼ 10 Tg yr−1, which is a factor of 2–3 less than inferred from satellite data by previous work that likely overestimated dust deposition by underestimating the dust mass extinction efficiency. The data obtained in this paper can be used to obtain improved constraints on dust impacts on clouds, climate, biogeochemical cycles, and other parts of the Earth system.

Abstract. Herein, we present a description of the Mechanism of Intermediate complexity for Modelling Iron (MIMI v1.0). This iron processing module was developed for use within Earth system models and has been updated within a modal aerosol framework from the original implementation in a bulk aerosol model. MIMI simulates the emission and atmospheric processing of two main sources of iron in aerosol prior to deposition: mineral dust and combustion processes. Atmospheric dissolution of insoluble to soluble iron is parameterized by an acidic interstitial aerosol reaction and a separate in-cloud aerosol reaction scheme based on observations of enhanced aerosol iron solubility in the presence of oxalate. Updates include a more comprehensive treatment of combustion iron emissions, improvements to the iron dissolution scheme, and an improved physical dust mobilization scheme. An extensive dataset consisting predominantly of cruise-based observations was compiled to compare to the model. The annual mean modelled concentration of surface-level total iron compared well with observations but less so in the soluble fraction (iron solubility) for which observations are much more variable in space and time. Comparing model and observational data is sensitive to the definition of the average as well as the temporal and spatial range over which it is calculated. Through statistical analysis and examples, we show that a median or log-normal distribution is preferred when comparing with soluble iron observations. The iron solubility calculated at each model time step versus that calculated based on a ratio of the monthly mean values, which is routinely presented in aerosol studies and used in ocean biogeochemistry models, is on average globally one-third (34 %) higher. We redefined ocean deposition regions based on dominant iron emission sources and found that the daily variability in soluble iron simulated by MIMI was larger than that of previous model simulations. MIMI simulated a general increase in soluble iron deposition to Southern Hemisphere oceans by a factor of 2 to 4 compared with the previous version, which has implications for our understanding of the ocean biogeochemistry of these predominantly iron-limited ocean regions.

Abstract. Recent studies have shown that surface ozone (O3) concentrations over central eastern China (CEC) have increased significantly during the past decade. We quantified the effects of changes in meteorological conditions and O3 precursor emissions on surface O3 levels over CEC between July 2003 and July 2015 using the GEOS-Chem model. The simulated monthly mean maximum daily 8 h average O3 concentration (MDA8 O3) in July increased by approximately 13.6 %, from 65.5±7.9 ppbv (2003) to 74.4±8.7 ppbv (2015), comparable to the observed results. The change in meteorology led to an increase in MDA8 O3 of 5.8±3.9 ppbv over the central part of CEC, in contrast to a decrease of about -0.8±3.5 ppbv over the eastern part of the region. In comparison, the MDA8 O3 over the central and eastern parts of CEC increased by 3.5±1.4 and 5.6±1.8 ppbv due to the increased emissions. The increase in averaged O3 in the CEC region resulting from the emission increase (4.0±1.9 ppbv) was higher than that caused by meteorological changes (3.1±4.9 ppbv) relative to the 2003 standard simulation, while the regions with larger O3 increases showed a higher sensitivity to meteorological conditions than to emission changes. Sensitivity tests indicate that increased levels of anthropogenic non-methane volatile organic compounds (NMVOCs) dominate the O3 increase over the eastern part of CEC, and anthropogenic nitrogen oxides (NOx) mainly increase MDA8 O3 over the central and western parts and decrease O3 in a few urban areas in the eastern part. Budget analysis showed that net photochemical production and meteorological conditions (transport in particular) are two important factors that influence O3 levels over the CEC. The results of this study suggest a need to further assess the effectiveness of control strategies for O3 pollution in the context of regional meteorology and anthropogenic emission changes.