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.

Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes. Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50 % decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2∕3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1. Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AOD_f, AOD_c), Ångström exponent (AE), dry surface scattering (SC_dry), and absorption (AC_dry) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21 % ± 20 % (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from −37 % (MODIS-Terra) to −16 % (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R>0.75), suggesting that the models are capable of capturing spatio-temporal variations in AOD. We find a much larger underestimate in coarse AOD_c (∼ −45 % ± 25 %) than in fine AOD_f (∼ −15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AOD_c bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AOD_c. Column AEs are underestimated by about 10 % ± 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. +140 % if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment. Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of −35 % ± 25 % and −20 % ± 18 % for SC_dry and AC_dry, respectively. The larger underestimate of SC_dry than AC_dry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SC_dry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models. Considerable inter-model diversity in the simulated optical properties is often found in regions that are, unfortunately, not or only sparsely covered by ground-based observations. This includes, for instance, the Sahara, Amazonia, central Australia, and the South Pacific. This highlights the need for a better site coverage in the observations, which would enable us to better assess the models, but also the performance of satellite products in these regions. Using fine-mode AOD as a proxy for present-day aerosol forcing estimates, our results suggest that models underestimate aerosol forcing by ca. −15 %, however, with a considerably large interquartile range, suggesting a spread between −35 % and +10 %.

This paper quantifies the pre-industrial (1850) to present-day (2014) effective radiative forcing (ERF) of anthropogenic emissions of NO_X, volatile organic compounds (VOCs; including CO), SO₂, NH₃, black carbon, organic carbon, and concentrations of methane, N₂O and ozone-depleting halocarbons, using CMIP6 models. Concentration and emission changes of reactive species can cause multiple changes in the composition of radiatively active species: tropospheric ozone, stratospheric ozone, stratospheric water vapour, secondary inorganic and organic aerosol, and methane. Where possible we break down the ERFs from each emitted species into the contributions from the composition changes. The ERFs are calculated for each of the models that participated in the AerChemMIP experiments as part of the CMIP6 project, where the relevant model output was available. The 1850 to 2014 multi-model mean ERFs (± standard deviations) are −1.03 ± 0.37 W m⁻² for SO₂ emissions, −0.25 ± 0.09 W m⁻² for organic carbon (OC), 0.15 ± 0.17 W m⁻² for black carbon (BC) and −0.07 ± 0.01 W m⁻² for NH₃. For the combined aerosols (in the piClim-aer experiment) it is −1.01 ± 0.25 W m⁻². The multi-model means for the reactive well-mixed greenhouse gases (including any effects on ozone and aerosol chemistry) are 0.67 ± 0.17 W m⁻² for methane (CH₄), 0.26 ± 0.07 W m⁻² for nitrous oxide (N₂O) and 0.12 ± 0.2 W m⁻² for ozone-depleting halocarbons (HC). Emissions of the ozone precursors nitrogen oxides (NO_x), volatile organic compounds and both together (O₃) lead to ERFs of 0.14 ± 0.13, 0.09 ± 0.14 and 0.20 ± 0.07 W m⁻² respectively. The differences in ERFs calculated for the different models reflect differences in the complexity of their aerosol and chemistry schemes, especially in the case of methane where tropospheric chemistry captures increased forcing from ozone production.

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.

Stratospheric ozone and water vapour are key components of the Earth system, and past and future changes to both have important impacts on global and regional climate. Here, we evaluate long-term changes in these species from the pre-industrial period (1850) to the end of the 21st century in Coupled Model Intercomparison Project phase 6 (CMIP6) models under a range of future emissions scenarios. There is good agreement between the CMIP multi-model mean and observations for total column ozone (TCO), although there is substantial variation between the individual CMIP6 models. For the CMIP6 multi-model mean, global mean TCO has increased from ∼ 300 DU in 1850 to ∼ 305 DU in 1960, before rapidly declining in the 1970s and 1980s following the use and emission of halogenated ozone-depleting substances (ODSs). TCO is projected to return to 1960s values by the middle of the 21st century under the SSP2-4.5, SSP3-7.0, SSP4-3.4, SSP4-6.0, and SSP5-8.5 scenarios, and under the SSP3-7.0 and SSP5-8.5 scenarios TCO values are projected to be ∼ 10 DU higher than the 1960s values by 2100. However, under the SSP1-1.9 and SSP1-1.6 scenarios, TCO is not projected to return to the 1960s values despite reductions in halogenated ODSs due to decreases in tropospheric ozone mixing ratios. This global pattern is similar to regional patterns, except in the tropics where TCO under most scenarios is not projected to return to 1960s values, either through reductions in tropospheric ozone under SSP1-1.9 and SSP1-2.6, or through reductions in lower stratospheric ozone resulting from an acceleration of the Brewer–Dobson circulation under other Shared Socioeconomic Pathways (SSPs). In contrast to TCO, there is poorer agreement between the CMIP6 multi-model mean and observed lower stratospheric water vapour mixing ratios, with the CMIP6 multi-model mean underestimating observed water vapour mixing ratios by ∼ 0.5 ppmv at 70 hPa. CMIP6 multi-model mean stratospheric water vapour mixing ratios in the tropical lower stratosphere have increased by ∼ 0.5 ppmv from the pre-industrial to the present-day period and are projected to increase further by the end of the 21st century. The largest increases (∼ 2 ppmv) are simulated under the future scenarios with the highest assumed forcing pathway (e.g. SSP5-8.5). Tropical lower stratospheric water vapour, and to a lesser extent TCO, shows large variations following explosive volcanic eruptions.

Feedbacks play a fundamental role in determining the magnitude of the response of the climate system to external forcing, such as from anthropogenic emissions. The latest generation of Earth system models includes aerosol and chemistry components that interact with each other and with the biosphere. These interactions introduce a complex web of feedbacks that is important to understand and quantify. This paper addresses multiple pathways for aerosol and chemical feedbacks in Earth system models. These focus on changes in natural emissions (dust, sea salt, dimethyl sulfide, biogenic volatile organic compounds (BVOCs) and lightning) and changes in reaction rates for methane and ozone chemistry. The feedback terms are then given by the sensitivity of a pathway to climate change multiplied by the radiative effect of the change. We find that the overall climate feedback through chemistry and aerosols is negative in the sixth Coupled Model Intercomparison Project (CMIP6) Earth system models due to increased negative forcing from aerosols in a climate with warmer surface temperatures following a quadrupling of CO₂ concentrations. This is principally due to increased emissions of sea salt and BVOCs which are sensitive to climate change and cause strong negative radiative forcings. Increased chemical loss of ozone and methane also contributes to a negative feedback. However, overall methane lifetime is expected to increase in a warmer climate due to increased BVOCs. Increased emissions of methane from wetlands would also offset some of the negative feedbacks. The CMIP6 experimental design did not allow the methane lifetime or methane emission changes to affect climate, so we found a robust negative contribution from interactive aerosols and chemistry to climate sensitivity in CMIP6 Earth system models.