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Paleo-proxy data indicate that a “Green Sahara” thrived in northern Africa during the early- to mid-Holocene (MH; 11 000 to 5000 years before present), characterized by more vegetation cover and reduced dust emissions. Utilizing a state-of-the-art atmospheric chemical transport model, TM5-MP, we assessed the changes in biogenic volatile organic compound (BVOC) emissions, dust emissions and secondary organic aerosol (SOA) concentrations in northern Africa during this period relative to the pre-industrial (PI) period. Our simulations show that dust emissions reduced from 280.6 Tg a−1 in the PI to 26.8 Tg a−1 in the MH, agreeing with indications from eight marine sediment records in the Atlantic Ocean. The northward expansion in northern Africa resulted in an increase in annual emissions of isoprene and monoterpenes during the MH, around 4.3 and 3.5 times higher than that in the PI period, respectively, causing a 1.9-times increase in the SOA surface concentration. Concurrently, enhanced BVOC emissions consumed more hydroxyl radical (OH), resulting in less sulfate formation. This effect counteracted the enhanced SOA surface concentration, altogether leading to a 17 % increase in the cloud condensation nuclei at 0.2 % super saturation over northern Africa. Our simulations provide consistent emission datasets of BVOCs, dust and the SOA formation aligned with the northward shift of vegetation during the “Green Sahara” period, which could serve as a benchmark for MH aerosol input in future Earth system model simulation experiments.

The Radiative Forcing Model Intercomparison Project (RFMIP) allows estimates of effective radiative forcing (ERF) in the Coupled Model Intercomparison Project phase six (CMIP6). We analyze the RFMIP output, including the new experiments from models that use the same parameterization for anthropogenic aerosols (RFMIP-SpAer), to characterize and better understand model differences in aerosol ERF. We find little changes in the aerosol ERF for 1970–2014 in the CMIP6 multi-model mean, which implies greenhouse gases primarily explain the positive trend in the total anthropogenic ERF. Cloud-mediated effects dominate the present-day aerosol ERF in most models. The results highlight a regional increase in marine cloudiness due to aerosols, despite suppressed cloud lifetime effects in that RFMIP-SpAer experiment. Negative cloud-mediated effects mask positive direct effects in many models, which arise from strong anthropogenic aerosol absorption. The findings suggest opportunities to better constrain simulated ERF by revisiting the optical properties and long-range transport of aerosols. Key Points: - Coupled Model Intercomparison Project phase six (CMIP6) averaged trend in aerosol effective radiative forcing (ERF) is small for 1970–2014 and weakly positive for 2000–2014 - Positive direct aerosol radiative effects in CMIP6 models are associated with strong aerosol absorption - Diverse and often strong cloud-mediated effects primarily determine the magnitude of aerosol ERF in CMIP6

Atmospheric iron (Fe) deposition to the open ocean affects net primary productivity, nitrogen fixation, and carbon uptake. We investigate changes in soluble Fe (SFe) deposition from the pre-industrial period to the late 21st century using the EC-Earth3-Iron Earth System model. EC-Earth3-Iron considers various sources of Fe, including dust, fossil fuel combustion, and biomass burning, and features comprehensive atmospheric chemistry, representing atmospheric oxalate, sulfate, and Fe cycles. We show that anthropogenic activity has changed the magnitude and spatial distribution of SFe deposition by increasing combustion Fe emissions and atmospheric acidity and oxalate levels. We report that SFe deposition has doubled since the early industrial era, using the Coupled Model Intercomparison Project Phase 6 emission inventory. We highlight acidity as the main solubilization pathway for dust-Fe and oxalate-promoted processing for the solubilization of combustion-Fe. We project a global SFe deposition increase of 40% by the late 21st century relative to present day under Shared Socioeconomic Pathway (SSP) 3–7.0, which assumes weak climate change mitigation policies. Conversely, SSPs with stronger mitigation pathways (1–2.6 and 2–4.5) result in 35% and 10% global decreases, respectively. Despite these differences, SFe deposition increases over the equatorial Pacific and decreases in the Southern Ocean (SO) for all SSPs. We further observe that deposition over the equatorial Pacific and SO are highly sensitive to future changes in dust emissions from Australia and South America, as well as from North Africa. Future studies should focus on the potential impact of climate- and human-induced changes in dust and wildfires combined., This work was funded by the European Research Council under the Horizon 2020 research and innovation programme through the ERC Consolidator Grant FRAGMENT (grant agreement no. 773051), the AXA Research Fund through the AXA Chair on Sand and Dust Storms at BSC, the Spanish Ministerio de Economía y Competitividad through the NUTRIENT project (CGL2017-88911-R), the European Union's Horizon 2020 research and innovation programme under grant agreement no 821205 (FORCeS), and ESA through the DOMOS project (ESA AO/1-10546/20/I-NB). We acknowledge the EMIT project, which is supported by the National Aeronautics and Space Administration Earth Venture Instrument program, under the Earth Science Division of the Science Mission Directorate. RLM received additional support from the NASA Modeling, Analysis and Prediction Program (NNG14HH42I). We also acknowledge the resources obtained on the Marenostrum4 supercomputer at BSC, granted through the PRACE project eFRAGMENT2 and RES project AECT-2020-3-0020, along with the technical support provided by BSC and the Computational Earth Sciences team of the BSC Earth Sciences Department., Peer Reviewed, Postprint (published version)

The Earth system model EC-Earth3 for contributions to CMIP6 is documented here, with its flexible coupling framework, major model configurations, a methodology for ensuring the simulations are comparable across different high-performance computing (HPC) systems, and with the physical performance of base configurations over the historical period. The variety of possible configurations and sub-models reflects the broad interests in the EC-Earth community. EC-Earth3 key performance metrics demonstrate physical behavior and biases well within the frame known from recent CMIP models. With improved physical and dynamic features, new Earth system model (ESM) components, community tools, and largely improved physical performance compared to the CMIP5 version, EC-Earth3 represents a clear step forward for the only European community ESM. We demonstrate here that EC-Earth3 is suited for a range of tasks in CMIP6 and beyond.

This work presents an analysis of the effect of climate change on surface ozone discussing the related penalties and benefits around the globe from the global modelling perspective based on simulations with five CMIP6 (Coupled Model Intercomparison Project Phase 6) Earth System Models. As part of AerChemMIP (Aerosol Chemistry Model Intercomparison Project) all models conducted simulation experiments considering future climate (ssp370SST) and present-day climate (ssp370pdSST) under the same future emissions trajectory (SSP3-7.0). A multi-model global average climate change benefit on surface ozone of -0.96 ± 0.07 ppbv °C-1 is calculated which is mainly linked to the dominating role of enhanced ozone destruction with higher water vapour abundances under a warmer climate. Over regions remote from pollution sources, there is a robust decline in mean surface ozone concentration on an annual basis as well as for boreal winter and summer varying spatially from -0.2 to -2 ppbv °C-1, with strongest decline over tropical oceanic regions. The implication is that over regions remote from pollution sources (except over the Arctic) there is a consistent climate change benefit for baseline ozone due to global warming. However, ozone increases over regions close to anthropogenic pollution sources or close to enhanced natural biogenic volatile organic compounds emission sources with a rate ranging regionally from 0.2 to 2 ppbv C-1, implying a regional surface ozone penalty due to global warming. Overall, the future climate change enhances the efficiency of precursor emissions to generate surface ozone in polluted regions and thus the magnitude of this effect depends on the regional emission changes considered in this study within the SSP3_7.0 scenario. The comparison of the climate change impact effect on surface ozone versus the combined effect of climate and emission changes indicates the dominant role of precursor emission changes in projecting surface ozone concentrations under

Understanding how multiphase processes affect the iron-containing aerosol cycle is key to predicting ocean biogeochemistry changes and hence the feedback effects on climate. For this work, the EC-Earth Earth system model in its climate–chemistry configuration is used to simulate the global atmospheric oxalate (OXL), sulfate (SO), and iron (Fe) cycles after incorporating a comprehensive representation of the multiphase chemistry in cloud droplets and aerosol water. The model considers a detailed gas-phase chemistry scheme, all major aerosol components, and the partitioning of gases in aerosol and atmospheric water phases. The dissolution of Fe-containing aerosols accounts kinetically for the solution's acidity, oxalic acid, and irradiation. Aerosol acidity is explicitly calculated in the model, both for accumulation and coarse modes, accounting for thermodynamic processes involving inorganic and crustal species from sea salt and dust. Simulations for present-day conditions (2000–2014) have been carried out with both EC-Earth and the atmospheric composition component of the model in standalone mode driven by meteorological fields from ECMWF's ERA-Interim reanalysis. The calculated global budgets are presented and the links between the (1) aqueous-phase processes, (2) aerosol dissolution, and (3) atmospheric composition are demonstrated and quantified. The model results are supported by comparison to available observations. We obtain an average global OXL net chemical production of 12.615 ± 0.064 Tg yr−1 in EC-Earth, with glyoxal being by far the most important precursor of oxalic acid. In comparison to the ERA-Interim simulation, differences in atmospheric dynamics and the simulated weaker oxidizing capacity in EC-Earth overall result in a ∼ 30 % lower OXL source. On the other hand, the more explicit representation of the aqueous-phase chemistry in EC-Earth compared to the previous versions of the model leads to an overall ∼ 20 % higher sulfate production, but this is, Stelios Myriokefalitakis, Evangelos Gerasopoulos, and Maria Kanakidou acknowledge support by the project “PANhellenic infrastructure for Atmospheric Composition and climatE change” (MIS 5021516) implemented under the Action “Reinforcement of the Research and Innovation Infrastructure”, which is funded by the Operational Programme “Competitiveness, Entrepreneurship and Innovation” (NSRF 2014–2020) and cofinanced by Greece and the European Union (European Regional Development Fund). This work was supported by computational time granted from the National Infrastructures for Research and Technology S.A. (GRNET S.A.) in the National HPC facility – ARIS – under project ID 010003 (ANION). Elisa Bergas-Massó, María Gonçalves-Ageitos, and Carlos Pérez García-Pando gratefully acknowledge the computer resources at Marenostrum4 granted through the PRACE project eFRAGMENT3 and the RES project AECT-2020-3-0020, as well as the technical support provided by the Barcelona Supercomputing Center (BSC) and the CES team of the Earth Sciences Department. Their work was supported by the ERC Consolidator Grant FRAGMENT (grant agreement no. 773051) and the AXA Chair on Sand and Dust Storms at BSC funded by the AXA Research Fund, both of which are led by Carlos Pérez García-Pando, who also acknowledges the Ramon y Cajal program (grant no. RYC-2015-18690) of the Spanish Ministry of Science, Innovation and Universities and the ICREA program. The research leading to these results has also received funding from the Spanish Ministerio de Economía y Competitividad as part of the NUTRIENT project (CGL2017-88911-R) and the H2020 GA 821205 project FORCeS. Support for this research was provided to Akinori Ito by the JSPS KAKENHI (grant no. 20H04329) and the Integrated Research Program for Advancing Climate Models (TOUGOU) (grant no. JPMXD0717935715) from the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan. Twan van Noije, Philippe Le Sager, Maria Kanakidou, and Stelios Myr, Peer Reviewed, Postprint (published version)

Understanding how multiphase processes affect the iron-containing aerosol cycle is key to predicting ocean biogeochemistry changes and hence the feedback effects on climate. For this work, the EC-Earth Earth system model in its climate-chemistry configuration is used to simulate the global atmospheric oxalate (OXL), sulfate (SO42-), and iron (Fe) cycles after incorporating a comprehensive representation of the multiphase chemistry in cloud droplets and aerosol water. The model considers a detailed gas-phase chemistry scheme, all major aerosol components, and the partitioning of gases in aerosol and atmospheric water phases. The dissolution of Fe-containing aerosols accounts kinetically for the solution's acidity, oxalic acid, and irradiation. Aerosol acidity is explicitly calculated in the model, both for accumulation and coarse modes, accounting for thermodynamic processes involving inorganic and crustal species from sea salt and dust. Simulations for present-day conditions (2000-2014) have been carried out with both EC-Earth and the atmospheric composition component of the model in standalone mode driven by meteorological fields from ECMWF's ERA-Interim reanalysis. The calculated global budgets are presented and the links between the (1) aqueous-phase processes, (2) aerosol dissolution, and (3) atmospheric composition are demonstrated and quantified. The model results are supported by comparison to available observations. We obtain an average global OXL net chemical production of 12.615 ± 0.064 Tg yr-1 in EC-Earth, with glyoxal being by far the most important precursor of oxalic acid. In comparison to the ERA-Interim simulation, differences in atmospheric dynamics and the simulated weaker oxidizing capacity in EC-Earth overall result in a ∼ 30 % lower OXL source. On the other hand, the more explicit representation of the aqueous-phase chemistry in EC-Earth compared to the previous versions of the model leads to an overall ∼ 20 % higher sulfate production, but this