The importance of wind-blown mineral dust for cloud droplet formation is studied by considering (i) the adsorption of water on the surface of insoluble particles, (ii) particle coating by soluble material (atmospheric aging) which augments cloud condensation nuclei (CCN) activity, and (iii) the effect of dust on inorganic aerosol concentrations through thermodynamic interactions with mineral cations. The ECHAM5/MESSy Atmospheric Chemistry (EMAC) model is used to simulate the composition of global atmospheric aerosol, while the ISORROPIA-II thermodynamic equilibrium model treats the interactions of K⁺-Ca²⁺-Mg²⁺-NH₄⁺-Na⁺-SO₄²⁻-NO₃⁻-Cl⁻-H₂O aerosol with gas-phase inorganic constituents. Dust is considered a mixture of inert material with reactive minerals and its emissions are calculated online by taking into account the soil particle size distribution and chemical composition of different deserts worldwide. The impact of dust on droplet formation is treated through the unified dust activation parameterization that considers the inherent hydrophilicity from adsorption and acquired hygroscopicity from soluble salts during aging. Our simulations suggest that the presence of dust increases cloud droplet number concentration (CDNC) over major deserts (e.g., up to 20 % over the Sahara and the Taklimakan desert) and decreases CDNC over polluted areas (e.g., up to 10 % over southern Europe and 20 % over northeastern Asia). This leads to a global net decrease in CDNC by 11 %. The adsorption activation of insoluble aerosols and the mineral dust chemistry are shown to be equally important for the cloud droplet formation over the main deserts; for example, these effects increase CDNC by 20 % over the Sahara. Remote from deserts the application of adsorption theory is critically important since the increased water uptake by the large aged dust particles (i.e., due to the added hydrophilicity by the soluble coating) reduce the maximum supersaturation and thus cloud droplet formation from the relatively smaller anthropogenic particles (e.g., CDNC decreases by 10 % over southern Europe and 20 % over northeastern Asia by applying adsorption theory). The global average CDNC decreases by 10 % by considering adsorption activation, while changes are negligible when accounting for the mineral dust chemistry. Sensitivity simulations indicate that CDNC is also sensitive to the mineral dust mass and inherent hydrophilicity, and not to the chemical composition of the emitted dust.

Aerosols influence the Earth's energy balance directly by modifying the radiation transfer and indirectly by altering the cloud microphysics. Anthropogenic aerosol emissions dropped considerably when the global COVID-19 pandemic resulted in severe restraints on mobility, production, and public life in spring 2020. We assess the effects of these reduced emissions on direct and indirect aerosol radiative forcing over Europe, excluding contributions from contrails. We simulate the atmospheric composition with the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model in a baseline (business-as-usual) and a reduced emission scenario. The model results are compared to aircraft observations from the BLUESKY aircraft campaign performed in May–June 2020 over Europe. The model agrees well with most of the observations, except for sulfur dioxide, particulate sulfate, and nitrate in the upper troposphere, likely due to a biased representation of stratospheric aerosol chemistry and missing information about volcanic eruptions. The comparison with a baseline scenario shows that the largest relative differences for tracers and aerosols are found in the upper troposphere, around the aircraft cruise altitude, due to the reduced aircraft emissions, while the largest absolute changes are present at the surface. We also find an increase in all-sky shortwave radiation of 0.21 ± 0.05 W m⁻² at the surface in Europe for May 2020, solely attributable to the direct aerosol effect, which is dominated by decreased aerosol scattering of sunlight, followed by reduced aerosol absorption caused by lower concentrations of inorganic and black carbon aerosols in the troposphere. A further increase in shortwave radiation from aerosol indirect effects was found to be much smaller than its variability. Impacts on ice crystal concentrations, cloud droplet number concentrations, and effective crystal radii are found to be negligible.

Aromatics contribute a significant fraction to organic compounds in the troposphere and are mainly emitted by anthropogenic activities and biomass burning. Their oxidation in lab experiments is known to lead to the formation of ozone and aerosol precursors. However, their overall impact on tropospheric composition is uncertain as it depends on transport, multiphase chemistry, and removal processes of the oxidation intermediates. Representation of aromatics in global atmospheric models has been either neglected or highly simplified. Here, we present an assessment of their impact on gas-phase chemistry, using the general circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry). We employ a comprehensive kinetic model to represent the oxidation of the following monocyclic aromatics: benzene, toluene, xylenes, phenol, styrene, ethylbenzene, trimethylbenzenes, benzaldehyde, and lumped higher aromatics that contain more than nine C atoms. Significant regional changes are identified for several species. For instance, glyoxal increases by 130 % in Europe and 260 % in East Asia, respectively. Large increases in HCHO are also predicted in these regions. In general, the influence of aromatics is particularly evident in areas with high concentrations of NO_x, with increases up to 12 % in O₃ and 17 % in OH. On a global scale, the estimated net changes of trace gas levels are minor when aromatic compounds are included in our model. For instance, the tropospheric burden of CO increases by about 6 %, while the burdens of OH, O₃, and NO_x (NO+NO₂) decrease between 3 % and 9 %. The global mean changes are small, partially because of compensating effects between high- and low-NO_x regions. The largest change is predicted for the important aerosol precursor glyoxal, which increases globally by 36 %. In contrast to other studies, the net change in tropospheric ozone is predicted to be negative, −3 % globally. This change is larger in the Northern Hemisphere where global models usually show positive biases. We find that the reaction with phenoxy radicals is a significant loss for ozone, on the order of 200–300 Tg yr⁻¹, which is similar to the estimated ozone loss due to bromine chemistry. Although the net global impact of aromatics is limited, our results indicate that aromatics can strongly influence tropospheric chemistry on a regional scale, most significantly in East Asia. An analysis of the main model uncertainties related to oxidation and emissions suggests that the impact of aromatics may even be significantly larger.

A comprehensive ice nucleation parameterization has been implemented in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations (ICNCs). The parameterization of Barahona and Nenes (2009, hereafter BN09) allows for the treatment of ice nucleation taking into account the competition for water vapour between homogeneous and heterogeneous nucleation in cirrus clouds. Furthermore, the influence of chemically heterogeneous, polydisperse aerosols is considered by applying one of the multiple ice nucleating particle parameterizations which are included in BN09 to compute the heterogeneously formed ice crystals. BN09 has been modified in order to consider the pre-existing ice crystal effect and implemented to operate both in the cirrus and in the mixed-phase regimes. Compared to the standard EMAC parameterizations, BN09 produces fewer ice crystals in the upper troposphere but higher ICNCs in the middle troposphere, especially in the Northern Hemisphere where ice nucleating mineral dust particles are relatively abundant. Overall, ICNCs agree well with the observations, especially in cold cirrus clouds (at temperatures below 205 K), although they are underestimated between 200 and 220 K. As BN09 takes into account processes which were previously neglected by the standard version of the model, it is recommended for future EMAC simulations.

The interactions between aeolian dust and anthropogenic air pollution, notably chemical ageing of mineral dust and coagulation of dust and pollution particles, modify the atmospheric aerosol composition and burden. Since the aerosol particles can act as cloud condensation nuclei, this affects the radiative transfer not only directly via aerosol–radiation interactions, but also indirectly through cloud adjustments. We study both radiative effects using the global ECHAM/MESSy atmospheric chemistry-climate model (EMAC) which combines the Modular Earth Submodel System (MESSy) with the European Centre/Hamburg (ECHAM) climate model. Our simulations show that dust–pollution–cloud interactions reduce the condensed water path and hence the reflection of solar radiation. The associated climate warming outweighs the cooling that the dust–pollution interactions exert through the direct radiative effect. In total, this results in a net warming by dust–pollution interactions which moderates the negative global anthropogenic aerosol forcing at the top of the atmosphere by (0.2 ± 0.1) W m⁻².

Long-term exposure to ambient ozone (O₃) is associated with excess respiratory mortality. Pollution emissions, demographic, and climate changes are expected to drive future ozone-related mortality. Here, we assess global mortality attributable to ozone according to an Intergovernmental Panel on Climate Change (IPCC) Shared Socioeconomic Pathway (SSP) scenario applied in Coupled Model Intercomparison Project Phase 6 (CMIP6) models, projecting a temperature increase of about 3.6 °C by the end of the century. We estimated ozone-related mortality on a global scale up to 2090 following the Global Burden of Disease (GBD) 2019 approach, using bias-corrected simulations from three CMIP6 Earth System Models (ESMs) under the SSP3-7.0 emissions scenario. Based on the three ESMs simulations, global ozone-related mortality by 2090 will amount to 2.79 M [95% CI 0.97 M–5.23 M] to 3.12 M [95% CI 1.11 M–5.75 M] per year, approximately ninefold that of the 327 K [95% CI 103 K–652 K] deaths per year in 2000. Climate change alone may lead to an increase of ozone-related mortality in 2090 between 42 K [95% CI −37 K–122 K] and 217 K [95% CI 68 K–367 K] per year. Population growth and ageing are associated with an increase in global ozone-related mortality by a factor of 5.34, while the increase by ozone trends alone ranges between factors of 1.48 and 1.7. Ambient ozone pollution under the high-emissions SSP3-7.0 scenario is projected to become a significant human health risk factor. Yet, optimizing living conditions and healthcare standards worldwide to the optimal ones today (application of minimum baseline mortality rates) will help mitigate the adverse consequences associated with population growth and ageing, and ozone increases caused by pollution emissions and climate change.