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Over the CMIP6 historical period (1850–2014), aerosols provided the largest negative forcing compared to all other climate forcings via their ability to absorb or scatter solar radiation and alter clouds. Aerosols played an important role in counterbalancing warming by greenhouse gases (GHGs). Here we study aerosol forcing trends in the CMIP6 simulations of the NASA Goddard Institute for Space Studies (GISS) ocean-atmosphere ModelE version 2.1 (GISS-E2.1-G) using a fully coupled atmospheric composition configuration, including interactive gas-phase chemistry, and either an aerosol microphysical (MATRIX) or a mass-based aerosol (OMA) module. Simulations of the CMIP6 historical period are analyzed as well as four Shared Socioeconomic Pathway (SSP) future scenarios for 2015–2100: SSP1-2.6, SSP2-4.5, SSP3-7.0, and SSP5-8.5. The main conclusion of this study is that aerosol forcing in the GISS model has reached its turning point, switching from globally increasing to a decreasing trend in the first decade of the 21st century. This result is robust, independent of which aerosol module or SSP scenario is used. Non-linear aerosol-cloud interactions dominate as a forcing agent over aerosol-radiation interactions. Aerosols' ability to counterbalance GHG forcing on the global scale is today at a level comparable to that at the beginning of the last century. In the 1980s, the decade of largest global aerosol loads, aerosols balanced up to 80% of GHG forcing. As a consequence, global warming of the last decades, which is primarily driven by greenhouse gases, has been augmented by the effect of decreasing aerosol cooling in our model. By the end of this century, following the SSP scenarios, aerosols will only counterbalance 0%–20% of GHG forcing, depending on model and on scenario.

We examine multiple factors in the representation of satellite-retrieved atmospheric temperature diagnostics in historical simulations of climate change during the satellite era (specifically 1979–2021) using GISS ModelE contributions to the Coupled Model Intercomparison Project (Phase 6) (CMIP6). The tropospheric and stratospheric trends in these diagnostics are affected by greenhouse gases (notably carbon dioxide and ozone), coupling with the ocean, volcanic aerosols, solar activity and compositional and dynamic feedbacks. We explore the impacts of internal variability, changing forcing specifications, composition interactivity, the quality of the stratospheric circulation, vertical resolution, and possible impacts of the mis-specification of volcanic aerosol optical depths. Overall temperature trends throughout the satellite period are well captured, but discrepancies at all levels exist and have multiple distinct causes. We find that stratospheric comparisons (using Stratospheric Sounding Unit (SSU) retrievals and successor instruments) are most affected by variations in the representation of ozone depletion and feedbacks, followed by the volcanic signals. Tropospheric skill (using the Microwave Sounding Unit (MSU) retrievals) is affected by the trends in ocean heat uptake and tropospheric aerosols, but also by the representation of stratospheric processes through the impact of the Brewer-Dobson circulation on the height of the tropical tropopause. We demonstrate that no single factor is the dominant cause of the discrepancies and that almost all observations lie within the broad envelope of structural uncertainty.

Global models are widely used to simulate biomass burning aerosol (BBA). Exhaustive evaluations on model representation of aerosol distributions and properties are fundamental to assess health and climate impacts of BBA. Here we conducted a comprehensive comparison of Aerosol Comparisons between Observations and Models (AeroCom) project model simulations with satellite observations. A total of 59 runs by 18 models from three AeroCom Phase-III experiments (i.e., biomass burning emissions, CTRL16, and CTRL19) and 14 satellite products of aerosols were used in the study. Aerosol optical depth (AOD) at 550 nm was investigated during the fire season over three key fire regions reflecting different fire dynamics (i.e., deforestation-dominated Amazon, Southern Hemisphere Africa where savannas are the key source of emissions, and boreal forest burning in boreal North America). The 14 satellite products were first evaluated against AErosol RObotic NETwork (AERONET) observations, with large uncertainties found. But these uncertainties had small impacts on the model evaluation that was dominated by modeling bias. Through a comparison with Polarization and Directionality of the Earth’s Reflectances measurements with the Generalized Retrieval of Aerosol and Surface Properties algorithm (POLDER-GRASP), we found that the modeled AOD values were biased by −93 % to 152 %, with most models showing significant underestimations even for the state-of-the-art aerosol modeling techniques (i.e., CTRL19). By scaling up BBA emissions, the negative biases in modeled AOD were significantly mitigated, although it yielded only negligible improvements in the correlation between models and observations, and the spatial and temporal variations in AOD biases did not change much. For models in CTRL16 and CTRL19, the large diversity in modeled AOD was in almost equal measures caused by diversity in emissions, lifetime, and the mass extinction coefficient (MEC). We found that in the AeroCom ensemble, BBA lifetime correlated significantly with particle deposition (as expected) and in turn correlated strongly with precipitation. Additional analysis based on Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) aerosol profiles suggested that the altitude of the aerosol layer in the current models was generally too low, which also contributed to the bias in modeled lifetime. Modeled MECs exhibited significant correlations with the Ångström exponent (AE, an indicator of particle size). Comparisons with the POLDER-GRASP-observed AE suggested that the models tended to overestimate the AE (underestimated particle size), indicating a possible underestimation of MECs in models. The hygroscopic growth in most models generally agreed with observations and might not explain the overall underestimation of modeled AOD. Our results imply that current global models contain biases in important aerosol processes for BBA (e.g., emissions, removal, and optical properties) that remain to be addressed in future research.

We quantify the impacts of halogenated ozone-depleting substances (ODSs), greenhouse gases (GHGs), and short-lived ozone precursors on ozone changes between 1850 and 2014 using single-forcing perturbation simulations from several Earth system models with interactive chemistry participating in the Coupled Model Intercomparison Project Aerosol and Chemistry Model Intercomparison Project. We present the responses of ozone to individual forcings and an attribution of changes in ozone columns and vertically resolved stratospheric and tropospheric ozone to these forcings. We find that whilst substantial ODS-induced ozone loss dominates the stratospheric ozone changes since the 1970s, in agreement with previous studies, increases in tropospheric ozone due to increases in short-lived ozone precursors and methane since the 1950s make increasingly important contributions to total column ozone (TCO) changes. Increases in methane also lead to substantial extra-tropical stratospheric ozone increases. Impacts of nitrous oxide and carbon dioxide on stratospheric ozone are significant but their impacts on TCO are small overall due to several opposing factors and are also associated with large dynamical variability. The multi-model mean (MMM) results show a clear change in the stratospheric ozone trends after 2000 due to now declining ODSs, but the trends are generally not significantly positive, except in the extra-tropical upper stratosphere, due to relatively small changes in forcing over this period combined with large model uncertainty. Although the MMM ozone compares well with the observations, the inter-model differences are large primarily due to the large differences in the models' representation of ODS-induced ozone depletion.

Simulations by six Coupled Model Intercomparison Project Phase 6 (CMIP6) Earth system models indicate that the seasonal cycle of baseline tropospheric ozone at northern midlatitudes has been shifting since the mid-20th century. Beginning in ∼ 1940, the magnitude of the seasonal cycle increased by ∼10 ppb (measured from seasonal minimum to maximum), and the seasonal maximum shifted to later in the year by about 3 weeks. This shift maximized in the mid-1980s, followed by a reversal – the seasonal cycle decreased in amplitude and the maximum shifted back to earlier in the year. Similar changes are seen in measurements collected from the 1970s to the present. The timing of the seasonal cycle changes is generally concurrent with the rise and fall of anthropogenic emissions that followed industrialization and the subsequent implementation of air quality emission controls. A quantitative comparison of the temporal changes in the ozone seasonal cycle at sites in both Europe and North America with the temporal changes in ozone precursor emissions across the northern midlatitudes found a high degree of similarity between these two temporal patterns. We hypothesize that changing precursor emissions are responsible for the shift in the ozone seasonal cycle; this is supported by the absence of such seasonal shifts in southern midlatitudes where anthropogenic emissions are much smaller. We also suggest a mechanism by which changing emissions drive the changing seasonal cycle: increasing emissions of NOx allow summertime photochemical production of ozone to become more important than ozone transported from the stratosphere, and increasing volatile organic compounds (VOCs) lead to progressively greater photochemical ozone production in the summer months, thereby increasing the amplitude of the seasonal ozone cycle. Decreasing emissions of both precursor classes then reverse these changes. The quantitative parameter values that characterize the seasonal shifts provide useful benchmarks for evaluating model simulations, both against observations and between models.

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 future climate change scenarios.

We examined daily level-3 satellite retrievals of Atmospheric Infrared Sounder (AIRS) CO, Ozone Monitoring Instrument (OMI) SO2 and NO2, and Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth (AOD) over eastern China to understand how COVID-19 lockdowns affected atmospheric composition. Changes in 2020 were strongly dependent on the choice of background period since 2005 and whether trends in atmospheric composition were accounted for. Over central east China during the 23 January–8 April lockdown window, CO in 2020 was between 3 % and 12 % lower than average depending on the background period. The 2020 CO was not consistently less than expected from trends beginning between 2005 and 2016 and ending in 2019 but was 3 %–4 % lower than the background mean during the 2017–2019 period when CO changes had flattened. Similarly for AOD, 2020 was between 14 % and 30 % lower than averages beginning in 2005 and 14 %–17 % lower compared to different background means beginning in 2016. NO2 in 2020 was between 30 % and 43 % lower than the mean over different background periods and between 17 % and 33 % lower than what would be expected for trends beginning later than 2011. Relative to the 2016–2019 period when NO2 had flattened, 2020 was 30 %–33 % lower. Over southern China, 2020 NO2 was between 23 % and 27 % lower than different background means beginning in 2013, the beginning of a period of persistently lower NO2. CO over southern China was significantly higher in 2020 than what would be expected, which we suggest was partly because of an active fire season in neighboring countries. Over central east and southern China, 2020 SO2 was higher than expected, but this depended strongly on how daily regional values were calculated from individual retrievals and reflects background values approaching the retrieval detection limit. Future work over China, or other regions, needs to take into account the sensitivity of differences in 2020 to different background periods and trends in order to separate the effects of COVID-19 on air quality from previously occurring changes or from variability in other sources.

Aerosol-induced absorption of shortwave radiation can modify the climate through local atmospheric heating, which affects lapse rates, precipitation, and cloud formation. Presently, the total amount of aerosol absorption is poorly constrained, and the main absorbing aerosol species (black carbon (BC), organic aerosols (OA), and mineral dust) are diversely quantified in global climate models. As part of the third phase of the Aerosol Comparisons between Observations and Models (AeroCom) intercomparison initiative (AeroCom phase III), we here document the distribution and magnitude of aerosol absorption in current global aerosol models and quantify the sources of intermodel spread, highlighting the difficulties of attributing absorption to different species. In total, 15 models have provided total present-day absorption at 550 nm (using year 2010 emissions), 11 of which have provided absorption per absorbing species. The multi-model global annual mean total absorption aerosol optical depth (AAOD) is 0.0054 (0.0020 to 0.0098; 550 nm), with the range given as the minimum and maximum model values. This is 28 % higher compared to the 0.0042 (0.0021 to 0.0076) multi-model mean in AeroCom phase II (using year 2000 emissions), but the difference is within 1 standard deviation, which, in this study, is 0.0023 (0.0019 in Phase II). Of the summed component AAOD, 60 % (range 36 %–84 %) is estimated to be due to BC, 31 % (12 %–49 %) is due to dust, and 11 % (0 %–24 %) is due to OA; however, the components are not independent in terms of their absorbing efficiency. In models with internal mixtures of absorbing aerosols, a major challenge is the lack of a common and simple method to attribute absorption to the different absorbing species. Therefore, when possible, the models with internally mixed aerosols in the present study have performed simulations using the same method for estimating absorption due to BC, OA, and dust, namely by removing it and comparing runs with and without the absorbing species. We discuss the challenges of attributing absorption to different species; we compare burden, refractive indices, and density; and we contrast models with internal mixing to models with external mixing. The model mean BC mass absorption coefficient (MAC) value is 10.1 (3.1 to 17.7) m2 g−1 (550 nm), and the model mean BC AAOD is 0.0030 (0.0007 to 0.0077). The difference in lifetime (and burden) in the models explains as much of the BC AAOD spread as the difference in BC MAC values. The difference in the spectral dependency between the models is striking. Several models have an absorption Ångstrøm exponent (AAE) close to 1, which likely is too low given current knowledge of spectral aerosol optical properties. Most models do not account for brown carbon and underestimate the spectral dependency for OA.

Ammonia (NH3) and nitrogen oxides (NOx: nitrogen dioxide (NO2) + nitric oxide (NO)) play important roles in atmospheric chemistry. Throughout most of Africa, emissions of these gases are predominantly from soils and biomass burning. Here we use observations of tropospheric NO2 vertical column densities (VCDs) from the Ozone Monitoring Instrument (OMI) from 2005 through 2017 and atmospheric NH3 VCDs from the Infrared Atmospheric Sounding Interferometer (IASI) from 2008 through 2017 to evaluate seasonal variation of NO2 and NH3 VCDs across Africa and in seven African ecoregions. In regions where mean annual precipitation (MAP) is under 500 mm/yr we find that NO2 and NH3 VCDs are positively related to monthly precipitation, and where MAP is between 500 and 1750 mm yr-1 or higher, NO2 VCDs are negatively related to monthly precipitation. In dry ecoregions, temperature and precipitation were important predictors of NH3 and NO2 VCDs, likely related to variation in soil emissions. In mesic ecoregions, monthly NO2 VCDs were strongly related to burned area, suggesting that biomass burning drives seasonality. NH3 VCDs in mesic ecoregions were positively related to both monthly temperature and monthly CO VCDs, suggesting that a mixture of soil and biomass burning emissions influenced NH3 seasonality. In northern mesic ecoregions monthly temperature explained most of the variance in monthly NH3 VCDs, suggesting that soil sources, including animal excreta, determined NH3 seasonality. In southern mesic ecoregions, monthly CO VCDs explained more variation in NH3 VCDs than temperature, suggesting that biomass burning may have greater influence over NH3 seasonality.

Our quantitative understanding of natural tropospheric ozone concentrations is limited by the paucity of reliable measurements before the 1980s. We utilize the existing measurements to compare the long-term ozone changes that occurred within the marine boundary layer at northern and southern midlatitudes. Since 1950 ozone concentrations have increased by a factor of 2.1 ± 0.2 in the Northern Hemisphere (NH) and are presently larger than in the Southern Hemisphere (SH), where only a much smaller increase has occurred. These changes are attributed to increased ozone production driven by anthropogenic emissions of photochemical ozone precursors that increased with industrial development. The greater ozone concentrations and increases in the NH are consistent with the predominant location of anthropogenic emission sources in that hemisphere. The available measurements indicate that this interhemispheric gradient was much smaller and was likely reversed in the pre-industrial troposphere with higher concentrations in the SH. Six Earth system model (ESM) simulations indicate similar total NH increases (1.9 with a standard deviation of 0.3), but they occurred more slowly over a longer time period, and the ESMs do not find higher pre-industrial ozone in the SH. Several uncertainties in the ESMs may cause these model–measurement disagreements: the assumed natural nitrogen oxide emissions may be too large, the relatively greater fraction of ozone injected by stratosphere–troposphere exchange to the NH may be overestimated, ozone surface deposition to ocean and land surfaces may not be accurately simulated, and model treatment of emissions of biogenic hydrocarbons and their photochemistry may not be adequate.

Supervolcano eruptions have occurred throughout Earth’s history and have major environmental impacts. These impacts are mostly associated with the attenuation of visible sunlight by stratospheric sulfate aerosols, which causes cooling and deceleration of the water cycle. Supereruptions have been assumed to cause so-called volcanic winters that act as primary evolutionary factors through ecosystem disruption and famine, however, winter conditions alone may not be sufficient to cause such disruption. Here we use Earth system model simulations to show that stratospheric sulfur emissions from the Toba supereruption 74,000 years ago caused severe stratospheric ozone loss through a radiation attenuation mechanism that only moderately depends on the emission magnitude. The Toba plume strongly inhibited oxygen photolysis, suppressing ozone formation in the tropics, where exceptionally depleted ozone conditions persisted for over a year. This effect, when combined with volcanic winter in the extra-tropics, can account for the impacts of supereruptions on ecosystems and humanity.

Many nations responded to the COVID-19 pandemic by restricting travel and other activities during 2020, resulting in temporarily reduced emissions of CO2, other greenhouse gases and ozone and aerosol precursors. We present the initial results from a coordinated Intercomparison, CovidMIP, of Earth system model simulations which assess the impact on climate of these emissions reductions. Twelve models performed multiple initial-condition ensembles to produce over 300 simulations spanning both initial condition and model structural uncertainty. We find model consensus on reduced aerosol amounts (particularly over southern and eastern Asia) and associated increases in surface shortwave radiation levels. However, any impact on near-surface temperature or rainfall during 2020-2024 is extremely small and is not detectable in this initial analysis. Regional analyses on a finer scale, and closer attention to extremes (especially linked to changes in atmospheric composition and air quality) are required to test the impact of COVID- 19-related emission reductions on near-term climate.

The Scenario Model Intercomparison Project (ScenarioMIP) defines and coordinates the main set of future climate projections, based on concentration-driven simulations, within the Coupled Model Intercomparison Project phase 6 (CMIP6). This paper presents a range of its outcomes by synthesizing results from the participating global coupled Earth system models. We limit our scope to the analysis of strictly geophysical outcomes: mainly global averages and spatial patterns of change for surface air temperature and precipitation. We also compare CMIP6 projections to CMIP5 results, especially for those scenarios that were designed to provide continuity across the CMIP phases, at the same time highlighting important differences in forcing composition, as well as in results. The range of future temperature and precipitation changes by the end of the century (2081–2100) encompassing the Tier 1 experiments based on the Shared Socioeconomic Pathway (SSP) scenarios (SSP1-2.6, SSP2-4.5, SSP3-7.0 and SSP5-8.5) and SSP1-1.9 spans a larger range of outcomes compared to CMIP5, due to higher warming (by close to 1.5 °C) reached at the upper end of the 5 %–95 % envelope of the highest scenario (SSP5-8.5). This is due to both the wider range of radiative forcing that the new scenarios cover and the higher climate sensitivities in some of the new models compared to their CMIP5 predecessors. Spatial patterns of change for temperature and precipitation averaged over models and scenarios have familiar features, and an analysis of their variations confirms model structural differences to be the dominant source of uncertainty. Models also differ with respect to the size and evolution of internal variability as measured by individual models' initial condition ensemble spreads, according to a set of initial condition ensemble simulations available under SSP3-7.0. These experiments suggest a tendency for internal variability to decrease along the course of the century in this scenario, a result that will benefit from further analysis over a larger set of models. Benefits of mitigation, all else being equal in terms of societal drivers, appear clearly when comparing scenarios developed under the same SSP but to which different degrees of mitigation have been applied. It is also found that a mild overshoot in temperature of a few decades around mid-century, as represented in SSP5-3.4OS, does not affect the end outcome of temperature and precipitation changes by 2100, which return to the same levels as those reached by the gradually increasing SSP4-3.4 (not erasing the possibility, however, that other aspects of the system may not be as easily reversible). Central estimates of the time at which the ensemble means of the different scenarios reach a given warming level might be biased by the inclusion of models that have shown faster warming in the historical period than the observed. Those estimates show all scenarios reaching 1.5 °C of warming compared to the 1850–1900 baseline in the second half of the current decade, with the time span between slow and fast warming covering between 20 and 27 years from present. The warming level of 2 °C of warming is reached as early as 2039 by the ensemble mean under SSP5-8.5 but as late as the mid-2060s under SSP1-2.6. The highest warming level considered (5 °C) is reached by the ensemble mean only under SSP5-8.5 and not until the mid-2090s.d-2090s.

An intercomparison has been set up to study the representation of the atmospheric chemistry of the pre-industrial troposphere in earth system and other global tropospheric chemistry-transport models. The intercomparison employed a constrained box model and utilised tropospheric trace gas composition data for the pre-industrial times at ninety mid-latitude surface locations. Incremental additions of four organic compounds: methane, ethane, acetone and propane, were used to perturb the constrained box model and generate responses in hydroxyl radicals and tropospheric ozone at each location and with each chemical mechanism. Although the responses agreed well across the chemical mechanisms from the selected earth system and other global tropospheric chemistry-transport models, there were differences in the detailed responses between the chemical mechanisms that could be tracked down by sensitivity analysis to differences in the representation of C1–C3 chemistry. Inter-mechanism ranges in NOx compensation points were about 0.17 ± 0.12 when expressed relative to the inter-mechanism average. Monte Carlo uncertainty analysis carried out with a single chemical mechanism put the intra-mechanism range a factor of three higher at 0.50 ± 0.12. Similar differences between inter-mechanism and intra-mechanism ranges were found for hydroxyl radical depletion but were up to a factor of six wider for ozone formation from incremental additions of organic compounds. The cause of the discrepancies between the inter- and intra-mechanism ranges was found to be the large uncertainties that are present in the laboratory determinations of the rate coefficients and product channel branching ratios of some key chemical reactions involving organic peroxy radicals and hydroperoxides. Whilst these large uncertainties are present in the laboratory determinations, there will be irreducible uncertainties in the predictions from the earth system and other chemistry-transport models of methane and tropospheric ozone trends since pre-industrial times and hence their contributions to the radiative forcing of climate change. Further definitive laboratory studies of the reaction rates and product yields of the reactions of the simple organic peroxy radicals and hydroperoxides are required to resolve and reduce current uncertainties in earth system and chemistry-transport model predictions.

Near-term climate forcers (NTCFs), including aerosols and chemically reactive gases such as tropospheric ozone and methane, offer a potential way to mitigate climate change and improve air quality--so called "win-win" mitigation policies. Prior studies support improved air quality under NTCF mitigation, but with conflicting climate impacts that range from a significant reduction in the rate of global warming to only a modest impact. Here, we use state-of-the-art chemistry-climate model simulations conducted as part of the Aerosol and Chemistry Model Intercomparison Project (AerChemMIP) to quantify the 21st-century impact of NTCF reductions, using a realistic future emission scenario with a consistent air quality policy. Non-methane NTCF (NMNTCF; aerosols and ozone precursors) mitigation improves air quality, but leads to significant increases in global mean precipitation of 1.3% by mid-century and 1.4% by end-of-the-century, and corresponding surface warming of 0.23 and 0.21 K. NTCF (all-NTCF; including methane) mitigation further improves air quality, with larger reductions of up to 45% for ozone pollution, while offsetting half of the wetting by mid-century (0.7% increase) and all the wetting by end-of-the-century (non-significant 0.1% increase) and leading to surface cooling of -0.15 K by mid-century and -0.50 K by end-of-the-century. This suggests that methane mitigation offsets warming induced from reductions in NMNTCFs, while also leading to net improvements in air quality.

Socioeconomic development in low- and middle-income countries has been accompanied by increased emissions of air pollutants, such as nitrogen oxides [NOx: nitrogen dioxide (NO2) + nitric oxide (NO)], which affect human health. In sub-Saharan Africa, fossil fuel combustion has nearly doubled since 2000. At the same time, landscape biomass burning—another important NOx source—has declined in north equatorial Africa, attributed to changes in climate and anthropogenic fire management. Here, we use satellite observations of tropospheric NO2 vertical column densities (VCDs) and burned area to identify NO2 trends and drivers over Africa. Across the northern ecosystems where biomass burning occurs—home to hundreds of millions of people—mean annual tropospheric NO2 VCDs decreased by 4.5% from 2005 through 2017 during the dry season of November through February. Reductions in burned area explained the majority of variation in NO2 VCDs, though changes in fossil fuel emissions also explained some variation. Over Africa’s biomass burning regions, raising mean GDP density (USD·km−2) above its lowest levels is associated with lower NO2 VCDs during the dry season, suggesting that economic development mitigates net NO2 emissions during these highly polluted months. In contrast to the traditional notion that socioeconomic development increases air pollutant concentrations in low- and middle-income nations, our results suggest that countries in Africa’s northern biomass-burning region are following a different pathway during the fire season, resulting in potential air quality benefits. However, these benefits may be lost with increasing fossil fuel use and are absent during the rainy season.

Southern Africa produces almost a third of the Earth’s biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~ 350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~ 100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

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.

This paper quantifies the pre-industrial (1850) to present-day (2014) effective radiative forcing (ERF) of anthropogenic emissions of NOX, 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/sq.m for SO2 emissions, −0.25 ± 0.09 W/sq.m for organic carbon (OC), 0.15 ± 0.17 W/sq.m for black carbon (BC) and −0.07 ± 0.01 W/sq.m for NH3. For the combined aerosols (in the piClim-aer experiment) it is −1.01 ± 0.25 W/sq.m. 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/sq.m for methane (CH4), 0.26 ± 0.07 W/sq.m for nitrous oxide (N2O) and 0.12 ± 0.2 W/sq.m for ozone-depleting halocarbons (HC). Emissions of the ozone precursors nitrogen oxides (NOx), 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/sq.m 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.

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 (AODf, AODc), Ångström exponent (AE), dry surface scattering (SCdry), and absorption (ACdry) 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 AODc (∼ −45 % ± 25 %) than in fine AODf (∼ −15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AODc 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 AODc. 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 SCdry and ACdry, respectively. The larger underestimate of SCdry than ACdry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SCdry 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 %.

Anthropogenic aerosol emissions have increased considerably over the last century, but climate effects and quantification of the emissions are highly uncertain as one goes back in time. This uncertainty is partly due to a lack of observations in the pre-satellite era, making the observations we do have before 1990 additionally valuable. Aerosols suspended in the atmosphere scatter and absorb incoming solar radiation and thereby alter the Earth's surface energy balance. Previous studies show that Earth system models (ESMs) do not adequately represent surface energy fluxes over the historical era. We investigated global and regional aerosol effects over the time period 1961–2014 by looking at surface downwelling shortwave radiation (SDSR). We used observations from ground stations as well as multiple experiments from eight ESMs participating in the Coupled Model Intercomparison Project Version 6 (CMIP6). Our results show that this subset of models reproduces the observed transient SDSR well in Europe but poorly in China. We suggest that this may be attributed to missing emissions of sulfur dioxide in China, sulfur dioxide being a precursor to sulfate, which is a highly reflective aerosol and responsible for more reflective clouds. The emissions of sulfur dioxide used in the models do not show a temporal pattern that could explain observed SDSR evolution over China. The results from various aerosol emission perturbation experiments from DAMIP, RFMIP and AerChemMIP show that only simulations containing anthropogenic aerosol emissions show dimming, even if the dimming is underestimated. Simulated clear-sky and all-sky SDSR do not differ greatly, suggesting that cloud cover changes are not a dominant cause of the biased SDSR evolution in the simulations. Therefore we suggest that the discrepancy between modeled and observed SDSR evolution is partly caused by erroneous aerosol and aerosol precursor emission inventories. This is an important finding as it may help interpret whether ESMs reproduce the historical climate evolution for the right or wrong reason.

Poor air quality is currently responsible for large impacts on human health across the world. In addition, the air pollutants ozone (O3) and particulate matter less than 2.5 µm in diameter (PM2.5) are also radiatively active in the atmosphere and can influence Earth's climate. It is important to understand the effect of air quality and climate mitigation measures over the historical period and in different future scenarios to ascertain any impacts from air pollutants on both climate and human health. The Coupled Model Intercomparison Project Phase 6 (CMIP6) presents an opportunity to analyse the change in air pollutants simulated by the current generation of climate and Earth system models that include a representation of chemistry and aerosols (particulate matter). The shared socio-economic pathways (SSPs) used within CMIP6 encompass a wide range of trajectories in precursor emissions and climate change, allowing for an improved analysis of future changes to air pollutants. Firstly, we conduct an evaluation of the available CMIP6 models against surface observations of O3 and PM2.5. CMIP6 models consistently overestimate observed surface O3 concentrations across most regions and in most seasons by up to 16 ppb, with a large diversity in simulated values over Northern Hemisphere continental regions. Conversely, observed surface PM2.5 concentrations are consistently underestimated in CMIP6 models by up to 10 µg m−3, particularly for the Northern Hemisphere winter months, with the largest model diversity near natural emission source regions. The biases in CMIP6 models when compared to observations of O3 and PM2.5 are similar to those found in previous studies. Over the historical period (1850–2014) large increases in both surface O3 and PM2.5 are simulated by the CMIP6 models across all regions, particularly over the mid to late 20th century, when anthropogenic emissions increase markedly. Large regional historical changes are simulated for both pollutants across East and South Asia with an annual mean increase of up to 40 ppb for O3 and 12 µg m−3 for PM2.5. In future scenarios containing strong air quality and climate mitigation measures (ssp126), annual mean concentrations of air pollutants are substantially reduced across all regions by up to 15 ppb for O3 and 12 µg m−3 for PM2.5. However, for scenarios that encompass weak action on mitigating climate and reducing air pollutant emissions (ssp370), annual mean increases in both surface O3 (up 10 ppb) and PM2.5 (up to 8 µg m−3) are simulated across most regions, although, for regions like North America and Europe small reductions in PM2.5 are simulated due to the regional reduction in precursor emissions in this scenario. A comparison of simulated regional changes in both surface O3 and PM2.5 from individual CMIP6 models highlights important regional differences due to the simulated interaction of aerosols, chemistry, climate and natural emission sources within models. The projection of regional air pollutant concentrations from the latest climate and Earth system models used within CMIP6 shows that the particular future trajectory of climate and air quality mitigation measures could have important consequences for regional air quality, human health and near-term climate. Differences between individual models emphasise the importance of understanding how future Earth system feedbacks influence natural emission sources, e.g. response of biogenic emissions under climate change.

Simulations of the CMIP6 historical period 1850‐‐2014, characterized by the emergence of anthropogenic climate drivers like greenhouse gases, are presented for different configurations of the NASA Goddard Institute for Space Studies (GISS) Earth System ModelE2.1. The GISS‐E2.1 ensembles are more sensitive to forcing than their CMIP5 predecessors (GISS‐E2), but warm less during recent decades due to reduced total forcing. This forcing reduction is attributed to an increase in longwave opacity in pre‐industrial simulations, resulting in an atmosphere less sensitive to further increases in opacity that result from rising greenhouse gas concentrations. This demonstrates the importance of the base climatology to forcing and forced climate trends. Most model versions match observed temperature trends since 1979 from the ocean to the stratosphere. The choice of ocean model is important to the transient climate response, as found in CMIP5 GISS‐E2: the model that more efficiently exports heat to the deep ocean shows a smaller rise in tropospheric temperature. Model sea level rise over the historical period is traced to excessive drawdown of aquifers to meet irrigation demand with a smaller contribution from thermal expansion. This shows how fully coupled models can provide indirect observational constraints upon forcing, in this case, constraining irrigation rates with observed sea level changes. The overall agreement of GISS‐E2.1 with observed trends is familiar from evaluation of its predecessors, as is the conclusion that these trends are almost entirely anthropogenic in origin.

We assess the effective radiative forcing due to ozone‐depleting substances using models participating in the Aerosols and Chemistry and Radiative Forcing Model Intercomparison Projects (AerChemMIP, RFMIP). A large intermodel spread in this globally averaged quantity necessitates an “emergent constraint” approach whereby we link the radiative forcing to ozone declines measured and simulated during 1979–2000, excluding two volcanically perturbed periods. During this period, ozone‐depleting substances were increasing, and several merged satellite‐based climatologies document the ensuing decline of total‐column ozone. Using these analyses, we find an effective radiative forcing of −0.05 to 0.13 W m−2. Our best estimate (0.04 W m−2) is on the edge of the “likely” range given by the Fifth Assessment Report of IPCC of 0.03 to 0.33 W m−2 but is in better agreement with two other literature results.

It is important to understand how future environmental policies will impact both climate change and air pollution. Although targeting near-term climate forcers (NTCFs), defined here as aerosols, tropospheric ozone, and precursor gases, should improve air quality, NTCF reductions will also impact climate. Prior assessments of the impact of NTCF mitigation on air quality and climate have been limited. This is related to the idealized nature of some prior studies, simplified treatment of aerosols and chemically reactive gases, as well as a lack of a sufficiently large number of models to quantify model diversity and robust responses. Here, we quantify the 2015–2055 climate and air quality effects of non-methane NTCFs using nine state-of-the-art chemistry–climate model simulations conducted for the Aerosol and Chemistry Model Intercomparison Project (AerChemMIP). Simulations are driven by two future scenarios featuring similar increases in greenhouse gases (GHGs) but with “weak” (SSP3-7.0) versus “strong” (SSP3-7.0-lowNTCF) levels of air quality control measures. As SSP3-7.0 lacks climate policy and has the highest levels of NTCFs, our results (e.g., surface warming) represent an upper bound. Unsurprisingly, we find significant improvements in air quality under NTCF mitigation (strong versus weak air quality controls). Surface fine particulate matter (PM2.5) and ozone (O3) decrease by −2.2±0.32 µg m−3 and −4.6±0.88 ppb, respectively (changes quoted here are for the entire 2015–2055 time period; uncertainty represents the 95 % confidence interval), over global land surfaces, with larger reductions in some regions including south and southeast Asia. Non-methane NTCF mitigation, however, leads to additional climate change due to the removal of aerosol which causes a net warming effect, including global mean surface temperature and precipitation increases of 0.25±0.12 K and 0.03±0.012 mm d−1, respectively. Similarly, increases in extreme weather indices, including the hottest and wettest days, also occur. Regionally, the largest warming and wetting occurs over Asia, including central and north Asia (0.66±0.20 K and 0.03±0.02 mm d−1), south Asia (0.47±0.16 K and 0.17±0.09 mm d−1), and east Asia (0.46±0.20 K and 0.15±0.06 mm d−1). Relatively large warming and wetting of the Arctic also occur at 0.59±0.36 K and 0.04±0.02 mm d−1, respectively. Similar surface warming occurs in model simulations with aerosol-only mitigation, implying weak cooling due to ozone reductions. Our findings suggest that future policies that aggressively target non-methane NTCF reductions will improve air quality but will lead to additional surface warming, particularly in Asia and the Arctic. Policies that address other NTCFs including methane, as well as carbon dioxide emissions, must also be adopted to meet climate mitigation goals.

In this work, we use Coupled Model Intercomparison Project Phase 6 (CMIP6) simulations from 10 Earth system models (ESMs) and general circulation models (GCMs) to study the fast climate responses on pre-industrial climate, due to present-day aerosols. All models carried out two sets of simulations: a control experiment with all forcings set to the year 1850 and a perturbation experiment with all forcings identical to the control, except for aerosols with precursor emissions set to the year 2014. In response to the pattern of all aerosols effective radiative forcing (ERF), the fast temperature responses are characterized by cooling over the continental areas, especially in the Northern Hemisphere, with the largest cooling over East Asia and India, sulfate being the dominant aerosol surface temperature driver for present-day emissions. In the Arctic there is a warming signal for winter in the ensemble mean of fast temperature responses, but the model-to-model variability is large, and it is presumably linked to aerosol-induced circulation changes. The largest fast precipitation responses are seen in the tropical belt regions, generally characterized by a reduction over continental regions and presumably a southward shift of the tropical rain belt. This is a characteristic and robust feature among most models in this study, associated with weakening of the monsoon systems around the globe (Asia, Africa and America) in response to hemispherically asymmetric cooling from a Northern Hemisphere aerosol perturbation, forcing possibly the Intertropical Convergence Zone (ITCZ) and tropical precipitation to shift away from the cooled hemisphere despite that aerosols' effects on temperature and precipitation are only partly realized in these simulations as the sea surface temperatures are kept fixed. An interesting feature in aerosol-induced circulation changes is a characteristic dipole pattern with intensification of the Icelandic Low and an anticyclonic anomaly over southeastern Europe, inducing warm air advection towards the northern polar latitudes in winter.

Fires affect the composition of the atmosphere and Earth’s radiation balance by emitting a suite of reactive gases and particles. An interactive fire module in an Earth system model (ESM) allows us to study the natural and anthropogenic drivers, feedbacks, and interactions of open fires. To do so, we have developed pyrE, the NASA GISS (Goddard Institute for Space Studies) interactive fire emissions *module. The pyrE module is driven by environmental variables like flammability and cloud-to-ground lightning, calculated by the GISS ModelE ESM, and parameterized by anthropogenic impacts based on population density data. Fire emissions are generated from the flaming phase in pyrE (active fires). Using pyrE, we examine fire occurrence, regional fire suppression, burned area, fire emissions, and how it all affects atmospheric composition. To do so, we evaluate pyrE by comparing it to satellite-based datasets of fire count, burned area, fire emissions, and aerosol optical depth (AOD). We demonstrate pyrE’s ability to simulate the daily and seasonal cycles of open fires and resulting emissions. Our results indicate that interactive fire emissions are biased low by 32 %–42 %, depending on emitted species, compared to the GFED4s (Global Fire Emissions Database) inventory. The bias in emissions drives underestimation in column densities, which is diluted by natural and anthropogenic emissions sources and production and loss mechanisms. Regionally, the resulting AOD of a simulation with interactive fire emissions is underestimated mostly over Indonesia compared to a simulation with GFED4s emissions and to MODIS AOD. In other parts of the world pyrE’s performance in terms of AOD is marginal to a simulation with prescribed fire emissions.

Volcanic eruptions are an important climate driver. The impact of Pinatubo-sized eruptions has been observed and is well constrained. The magnitude and duration of volcanic winter effects after super-eruptions such as Toba remain disputed due to disagreement between the strong cooling predicted by models, and much milder climate perturbations according to the paleo data. Here we present a re-evaluated climate impact of a Toba-sized super-eruption based on up-to-date GISS ModelE simulations. In this study, we account for all known primary mechanisms that govern the evolution of the volcanic plume and their nonlinear interactions. The SO2 radiative effects are evaluated for the first time in coupled climate simulations with the interactive atmospheric chemistry module. We found that SO2 effects on photochemistry, dynamics, and radiative forcing are especially prominent. Due to strong absorption in ultraviolet, SO2 feedback on photochemistry partially offsets the limiting effect associated with aerosol microphysical processes. SO2 greenhouse warming soothes the radiative cooling exerted by sulfate aerosols. SO2 absorption in the shortwave and longwave causes radiative heating and lofting of the volcanic plume, and boosts the efficiency of SO2 impact on photochemistry. Our analysis shows that SO2 lifetime and magnitude of effects scale up and increase with the amount of emitted material. For a Pinatubo-sized eruption, SO2 feedbacks on chemistry and dynamics are relevant only during the initial stage of the volcanic plume evolution, while local SO2 concentrations are high. For a Toba-sized eruption, SO2 effects are as important as sulfate aerosols, and produce a less extreme volcanic winter.