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In this work, we apply the GFDL Earth System Model (GFDL‐ESM4.1) to explore the climate responses to a stratospheric aerosol injection (SAI) scenario that aims to restrict global warming to 2.0°C above pre‐industrial levels (1850–1900) under the CMIP6 overshoot scenario (SSP5‐34‐OS). Simulations of this SAI scenario with the CESM Whole Atmosphere Community Climate Model (CESM2‐WACCM6) showed nearly unchanged interhemispheric and pole‐to‐Equator surface temperature gradients relative to present‐day conditions around 2020, and reduced global impacts, such as heatwaves, sea ice melting, and shifting precipitation patterns (Tilmes et al., 2020, https://doi.org/10.5194/esd‐11‐579‐2020). However, model structural uncertainties can lead to varying climate projections under the same forcing. Implementing identical stratospheric aerosol radiative properties in GFDL‐ESM4.1, which has a much lower Effective Climate Sensitivity compared to CESM2‐WACCM6, resulted in a decrease in global‐mean surface temperature by more than 1.5°C and a corresponding reduction in precipitation responses. Two major reasons contribute to the different temperature response between the two models: first, GFDL‐ESM4.1 has less warming in the SSP534‐OS scenario; second, GFDL‐ESM4.1 has shown more pronounced cooling in response to the same stratospheric AOD perturbation. Notably, the Southern Hemisphere experiences substantial cooling compared to the Northern Hemisphere, accompanied by a northward shift of the Intertropical Convergence Zone (ITCZ). Furthermore, our analysis reveals that spatially heterogeneous forcing within the SAI scenario results in diverse climate feedback parameters in the GFDL‐ESM4.1 model, through varying surface warming/cooling patterns. This research highlights the importance of considering model structural uncertainties and forcing spatial patterns for a comprehensive evaluation of future scenarios and geoengineering strategies. Plain Language Summary Solar radiation modification (SRM) has been explored as a way to mitigate global warming due to ongoing greenhouse gas emissions, but the full consequences remain highly uncertain. One SRM approach, which involves injecting small scattering particles into the upper atmosphere to reduce incoming sunlight, was previously tested using the CESM2‐WACCM6 climate model to limit global warming to 2.0°C above the pre‐industrial level. Applying the stratospheric aerosol radiative properties in the GFDL‐ESM4.1 model, we found a more than 1.5°C decrease in Earth's surface temperature and a reduction in rainfall, compared to CESM2‐WACCM6. In particular, the Southern Hemisphere experienced greater cooling compared to the Northern Hemisphere, leading to a northward shift in the tropical rainfall zone. Our findings also showed that spatially uneven particle injection results in varied climate responses within the same model. These results underscore the importance of considering the different characteristics of climate models and the spatial patterns of implementation when evaluating the potential impacts of SRM strategies. Key Points The stratospheric aerosol injection (SAI) strategy used in CESM2‐WACCM6 to target a warming of 2.0°C leads to a global surface overcooling in GFDL‐ESM4.1 The SAI applied on the SSP5‐34‐OS scenario also results in a decrease in global precipitation and a northward shift of ITCZ in GFDL‐ESM4.1 Strong spatially heterogeneous forcing leads to varying climate feedback parameters within the GFDL‐ESM4.1

Anthropogenic aerosols exert a cooling influence that offsets part of the greenhouse gas warming. Due to their short tropospheric lifetime of only several days, the aerosol forcing responds quickly to emissions. Here, we present and discuss the evolution of the aerosol forcing since 2000. There are multiple lines of evidence that allow us to robustly conclude that the anthropogenic aerosol effective radiative forcing (ERF) – both aerosol–radiation interactions (ERFari) and aerosol–cloud interactions (ERFaci) – has become less negative globally, i.e. the trend in aerosol effective radiative forcing changed sign from negative to positive. Bottom-up inventories show that anthropogenic primary aerosol and aerosol precursor emissions declined in most regions of the world; observations related to aerosol burden show declining trends, in particular of the fine-mode particles that make up most of the anthropogenic aerosols; satellite retrievals of cloud droplet numbers show trends in regions with aerosol declines that are consistent with these in sign, as do observations of top-of-atmosphere radiation. Climate model results, including a revised set that is constrained by observations of the ocean heat content evolution show a consistent sign and magnitude for a positive forcing relative to the year 2000 due to reduced aerosol effects. This reduction leads to an acceleration of the forcing of climate change, i.e. an increase in forcing by 0.1 to 0.3 W m−2, up to 12 % of the total climate forcing in 2019 compared to 1750 according to the Intergovernmental Panel on Climate Change (IPCC).

The hydroxyl radical (OH) sets the oxidative capacity of the atmosphere and, thus, profoundly affects the removal rate of pollutants and reactive greenhouse gases. While observationally derived constraints exist for global annual mean present-day OH abundances and interannual variability, OH estimates for past and future periods rely primarily on global atmospheric chemistry models. These models disagree ± 30% in mean OH and in its changes from the preindustrial to late 21st century, even when forced with identical anthropogenic emissions. A simple steady-state relationship that accounts for ozone photolysis frequencies, water vapor, and the ratio of reactive nitrogen to carbon emissions explains temporal variability within most models, but not intermodel differences. Here, we show that departure from the expected relationship reflects the treatment of reactive oxidized nitrogen species (NO y ) and the fraction of emitted carbon that reacts within each chemical mechanism, which remain poorly known due to a lack of observational data. Our findings imply a need for additional observational constraints on NO y partitioning and lifetime, especially in the remote free troposphere, as well as the fate of carbon-containing reaction intermediates to test models, thereby reducing uncertainties in projections of OH and, hence, lifetimes of pollutants and greenhouse gases.

We present estimates of changes in the direct aerosol effects (DRE) and its anthropogenic component (DRF) from 2001 to 2015 using the GFDL chemistry–climate model AM3 driven by CMIP6 historical emissions. AM3 is evaluated against observed changes in the clear-sky shortwave direct aerosol effect (DREswclr) derived from the Clouds and the Earth's Radiant Energy System (CERES) over polluted regions. From 2001 to 2015, observations suggest that DREclrsw increases (i.e., less radiation is scattered to space by aerosols) over western Europe (0.7–1 W m−2 decade−1) and the eastern US (0.9–1.4 W m−2 decade−1), decreases over India (−1 to −1.6 W m−2 decade−1), and does not change significantly over eastern China. AM3 captures these observed regional changes in DREclrsw well in the US and western Europe, where they are dominated by the decline of sulfate aerosols, but not in Asia, where the model overestimates the decrease of DREclrsw. Over India, the model bias can be partly attributed to a decrease of the dust optical depth, which is not captured by our model and offsets some of the increase of anthropogenic aerosols. Over China, we find that the decline of SO2 emissions after 2007 is not represented in the CMIP6 emission inventory. Accounting for this decline, using the Modular Emission Inventory for China, and for the heterogeneous oxidation of SO2 significantly reduces the model bias. For both India and China, our simulations indicate that nitrate and black carbon contribute more to changes in DREclrsw than in the US and Europe. Indeed, our model suggests that black carbon (+0.12 W m−2) dominates the relatively weak change in DRF from 2001 to 2015 (+0.03 W m−2). Over this period, the changes in the forcing from nitrate and sulfate are both small and of the same magnitude (−0.03 W m−2 each). This is in sharp contrast to the forcing from 1850 to 2001 in which forcings by sulfate and black carbon largely cancel each other out, with minor contributions from nitrate. The differences between these time periods can be well understood from changes in emissions alone for black carbon but not for nitrate and sulfate; this reflects non-linear changes in the photochemical production of nitrate and sulfate associated with changes in both the magnitude and spatial distribution of anthropogenic emissions.

Changes in atmospheric methane abundance have implications for both chemistry and climate as methane is both a strong greenhouse gas and an important precursor for tropospheric ozone. A better understanding of the drivers of trends and variability in methane abundance over the recent past is therefore critical for building confidence in projections of future methane levels. In this work, the representation of methane in the atmospheric chemistry model AM4.1 is improved by optimizing total methane emissions (to an annual mean of 580±34 Tg yr−1) to match surface observations over 1980–2017. The simulations with optimized global emissions are in general able to capture the observed trend, variability, seasonal cycle, and latitudinal gradient of methane. Simulations with different emission adjustments suggest that increases in methane emissions (mainly from agriculture, energy, and waste sectors) balanced by increases in methane sinks (mainly due to increases in OH levels) lead to methane stabilization (with an imbalance of 5 Tg yr−1) during 1999–2006 and that increases in methane emissions (mainly from agriculture, energy, and waste sectors) combined with little change in sinks (despite small decreases in OH levels) during 2007–2012 lead to renewed growth in methane (with an imbalance of 14 Tg yr−1 for 2007–2017). Compared to 1999–2006, both methane emissions and sinks are greater (by 31 and 22 Tg yr−1, respectively) during 2007–2017. Our tagged tracer analysis indicates that anthropogenic sources (such as agriculture, energy, and waste sectors) are more likely major contributors to the renewed growth in methane after 2006. A sharp increase in wetland emissions (a likely scenario) with a concomitant sharp decrease in anthropogenic emissions (a less likely scenario), would be required starting in 2006 to drive the methane growth by wetland tracer. Simulations with varying OH levels indicate that a 1 % change in OH levels could lead to an annual mean difference of ∼4 Tg yr−1 in the optimized emissions and a 0.08-year difference in the estimated tropospheric methane lifetime. Continued increases in methane emissions along with decreases in tropospheric OH concentrations during 2008–2015 prolong methane's lifetime and therefore amplify the response of methane concentrations to emission changes. Uncertainties still exist in the partitioning of emissions among individual sources and regions.

The evolution of tropospheric ozone from 1850 to 2100 has been studied using data from Phase 6 of the Coupled Model Intercomparison Project (CMIP6). We evaluate long-term changes using coupled atmosphere–ocean chemistry–climate models, focusing on the CMIP Historical and ScenarioMIP ssp370 experiments, for which detailed tropospheric-ozone diagnostics were archived. The model ensemble has been evaluated against a suite of surface, sonde and satellite observations of the past several decades and found to reproduce well the salient spatial, seasonal and decadal variability and trends. The multi-model mean tropospheric-ozone burden increases from 247 ± 36 Tg in 1850 to a mean value of 356 ± 31 Tg for the period 2005–2014, an increase of 44 %. Modelled present-day values agree well with previous determinations (ACCENT: 336 ± 27 Tg; Atmospheric Chemistry and Climate Model Intercomparison Project, ACCMIP: 337 ± 23 Tg; Tropospheric Ozone Assessment Report, TOAR: 340 ± 34 Tg). In the ssp370 experiments, the ozone burden increases to 416 ± 35 Tg by 2100. The ozone budget has been examined over the same period using lumped ozone production (PO3) and loss (LO3) diagnostics. Both ozone production and chemical loss terms increase steadily over the period 1850 to 2100, with net chemical production (PO3-LO3) reaching a maximum around the year 2000. The residual term, which contains contributions from stratosphere–troposphere transport reaches a minimum around the same time before recovering in the 21st century, while dry deposition increases steadily over the period 1850–2100. Differences between the model residual terms are explained in terms of variation in tropopause height and stratospheric ozone burden.

We analyse historical (1850–2014) atmospheric hydroxyl (OH) and methane lifetime data from Coupled Model Intercomparison Project Phase 6 (CMIP6)/Aerosols and Chemistry Model Intercomparison Project (AerChemMIP) simulations. Tropospheric OH changed little from 1850 up to around 1980, then increased by around 9 % up to 2014, with an associated reduction in methane lifetime. The model-derived OH trends from 1980 to 2005 are broadly consistent with trends estimated by several studies that infer OH from inversions of methyl chloroform and associated measurements; most inversion studies indicate decreases in OH since 2005. However, the model results fall within observational uncertainty ranges. The upward trend in modelled OH since 1980 was mainly driven by changes in anthropogenic near-term climate forcer emissions (increases in anthropogenic nitrogen oxides and decreases in CO). Increases in halocarbon emissions since 1950 have made a small contribution to the increase in OH, whilst increases in aerosol-related emissions have slightly reduced OH. Halocarbon emissions have dramatically reduced the stratospheric methane lifetime by about 15 %–40 %; most previous studies assumed a fixed stratospheric lifetime. Whilst the main driver of atmospheric methane increases since 1850 is emissions of methane itself, increased ozone precursor emissions have significantly modulated (in general reduced) methane trends. Halocarbon and aerosol emissions are found to have relatively small contributions to methane trends. These experiments do not isolate the effects of climate change on OH and methane evolution; however, we calculate residual terms that are due to the combined effects of climate change and non-linear interactions between drivers. These residual terms indicate that non-linear interactions are important and differ between the two methodologies we use for quantifying OH and methane drivers. All these factors need to be considered in order to fully explain OH and methane trends since 1850; these factors will also be important for future trends.

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.

Mitigation of greenhouse gas emissions often reduces co-emitted air pollutants, with advantages for human health. Avoided mortality from air pollution, a co-benefit of CO 2 abatement, is estimated under global climate change mitigation scenarios to be in the range of US$50–US$380 per tonne of CO 2 . This exceeds the projected mitigation costs for 2030 and 2050, and is within the lower range of costs expected in 2100. Actions to reduce greenhouse gas (GHG) emissions often reduce co-emitted air pollutants, bringing co-benefits for air quality and human health. Past studies 1 , 2 , 3 , 4 , 5 , 6 typically evaluated near-term and local co-benefits, neglecting the long-range transport of air pollutants 7 , 8 , 9 , long-term demographic changes, and the influence of climate change on air quality 10 , 11 , 12 . Here we simulate the co-benefits of global GHG reductions on air quality and human health using a global atmospheric model and consistent future scenarios, via two mechanisms: reducing co-emitted air pollutants, and slowing climate change and its effect on air quality. We use new relationships between chronic mortality and exposure to fine particulate matter 13 and ozone 14 , global modelling methods 15 and new future scenarios 16 . Relative to a reference scenario, global GHG mitigation avoids 0.5±0.2, 1.3±0.5 and 2.2±0.8 million premature deaths in 2030, 2050 and 2100. Global average marginal co-benefits of avoided mortality are US$50–380 per tonne of CO 2 , which exceed previous estimates, exceed marginal abatement costs in 2030 and 2050, and are within the low range of costs in 2100. East Asian co-benefits are 10–70 times the marginal cost in 2030. Air quality and health co-benefits, especially as they are mainly local and near-term, provide strong additional motivation for transitioning to a low-carbon future.

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.