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A growing number of general circulation models are adapting interactive sulfur and aerosol schemes to improve the representation of relevant physical and chemical processes and associated feedbacks. They are motivated by investigations of climate response to major volcanic eruptions and potential solar geoengineering scenarios. However, uncertainties in these schemes are not well constrained. Stratospheric sulfate is modulated by emissions of sulfur-containing species of anthropogenic and natural origin, including volcanic activity. While the effects of volcanic eruptions have been studied in the framework of global model intercomparisons, the background conditions of the sulfur cycle have not been addressed in such a way. Here, we fill this gap by analyzing the distribution of the main sulfur species in nine global atmospheric aerosol models for a volcanically quiescent period. We use observational data to evaluate model results. Overall, models agree that the three dominant sulfur species in terms of burdens (sulfate aerosol, OCS, and SO2) make up about 98 % stratospheric sulfur and 95 % tropospheric sulfur. However, models vary considerably in the partitioning between these species. Models agree that anthropogenic emission of SO2 strongly affects the sulfate aerosol burden in the northern hemispheric troposphere, while its importance is very uncertain in other regions, where emissions are much lower. Sulfate aerosol is the main deposited species in all models, but the values deviate by a factor of 2. Additionally, the partitioning between wet and dry deposition fluxes is highly model dependent. Inter-model variability in the sulfur species is low in the tropics and increases towards the poles. Differences are largest in the dynamically active northern hemispheric extratropical region and could be attributed to the representation of the stratospheric circulation. The differences in the atmospheric sulfur budget among the models arise from the representation of both chemical and dynamical processes, whose interplay complicates the bias attribution. Several problematic points identified for individual models are related to the specifics of the chemistry schemes, model resolution, and representation of cross-tropopause transport in the extratropics. Further model intercomparison research is needed with a focus on the clarification of the reasons for biases, given the importance of this topic for the stratospheric aerosol injection studies.

This is the second of two papers in which we study the dependency of the impacts of stratospheric sulfur injections on the model and injection strategy used. Here, aerosol optical properties from simulated stratospheric aerosol injections using two aerosol models (modal scheme M7 and sectional scheme SALSA), as described in Part 1 (Laakso et al., 2022), are implemented consistently into the EC-Earth, MPI-ESM and CESM Earth system models (ESMs) to simulate the climate impacts of different injection rates ranging from 2 to 100 Tg(S) yr−1. Two sets of simulations were run with the three ESMs: (1) regression simulations, in which an abrupt change in CO2 concentration or stratospheric aerosols over pre-industrial conditions was applied to quantify global mean fast temperature-independent climate responses and quasi-linear dependence on temperature, and (2) equilibrium simulations, in which radiative forcing of aerosol injections with various magnitudes compensated for the corresponding radiative forcing of CO2 enhancement to study the dependence of precipitation on the injection magnitude. The latter also allow one to explore the regional climatic responses. Large differences in SALSA- and M7-simulated radiative forcing in Part 1 translated into large differences in the estimated surface temperature and precipitation changes in ESM simulations; for example, an injection rate of 20 Tg(S) yr−1 in CESM using M7-simulated aerosols led to only 2.2 K global mean cooling, while EC-Earth–SALSA combination produced a 5.2 K change. In equilibrium simulations, where aerosol injections were utilized to offset the radiative forcing caused by an atmospheric CO2 concentration of 500 ppm, the decrease in global mean precipitation varied among models, ranging from −0.7 % to −2.4 % compared with the pre-industrial climate. These precipitation changes can be explained by the fast precipitation response due to radiation changes caused by the stratospheric aerosols and CO2, as the global mean fast precipitation response is shown to be negatively correlated with global mean atmospheric absorption. Our study shows that estimating the impact of stratospheric aerosol injection on climate is not straightforward. This is because the simulated capability of the sulfate layer to reflect solar radiation and absorb long-wave radiation is sensitive to the injection rate as well as the aerosol model used to simulate the aerosol field. These findings emphasize the necessity for precise simulation of aerosol microphysics to accurately estimate the climate impacts of stratospheric sulfur intervention. This study also reveals gaps in our understanding and uncertainties that still exist related to these controversial techniques.

The Geoengineering Model Intercomparison Project (GeoMIP) has proposed multiple model experiments during phases 5 and 6 of the Climate Model Intercomparison Project (CMIP), with the latest set of model experiments proposed in 2015. With phase 7 of CMIP in preparation and with multiple efforts ongoing to better explore the potential space of outcomes for different solar radiation modifications (SRMs) both in terms of deployment strategies and scenarios and in terms of potential impacts, the GeoMIP community has identified the need to propose and conduct a new experiment that could serve as a bridge between past iterations and future CMIP7 experiments. Here we report the details of such a proposed experiment, named G6-1.5K-SAI, to be conducted with the current generation of scenarios and models from CMIP6 and clarify the reasoning behind many of the new choices introduced. Namely, compared to the CMIP6 GeoMIP scenario G6sulfur, we decided on (1) an intermediate emission scenario as a baseline (the Shared Socioeconomic Pathway 2-4.5), (2) a start date set in the future that includes both considerations for the likelihood of exceeding 1.5 °C above preindustrial levels and some considerations for a likely start date for an SRM implementation, and (3) a deployment strategy for stratospheric aerosol injection that does not inject in the tropical pipe in order to obtain a more latitudinally uniform aerosol distribution. We also offer more details regarding the preferred experiment length and number of ensemble members and include potential options for second-tier experiments that some modeling groups might want to run. The specifics of the proposed experiment will further allow for a more direct comparison between results obtained from CMIP6 models and those obtained from future scenarios for CMIP7.

Desert dust is an important atmospheric aerosol that affects the Earth's climate, biogeochemistry, and air quality. However, current Earth system models (ESMs) struggle to accurately capture the impact of dust on the Earth's climate and ecosystems, in part because these models lack several essential aeolian processes that couple dust with climate and land surface processes. In this study, we address this issue by implementing several new parameterizations of aeolian processes detailed in our companion paper in the Community Earth System Model version 2 (CESM2). These processes include (1) incorporating a simplified soil particle size representation to calculate the dust emission threshold friction velocity, (2) accounting for the drag partition effect of rocks and vegetation in reducing wind stress on erodible soils, (3) accounting for the intermittency of dust emissions due to unresolved turbulent wind fluctuations, and (4) correcting the spatial variability of simulated dust emissions from native to higher spatial resolutions on spatiotemporal dust variability. Our results show that the modified dust emission scheme significantly reduces the model bias against observations compared with the default scheme and improves the correlation against observations of multiple key dust variables such as dust aerosol optical depth (DAOD), surface particulate matter (PM) concentration, and deposition flux. Our scheme's dust also correlates strongly with various meteorological and land surface variables, implying higher sensitivity of dust to future climate change than other schemes' dust. These findings highlight the importance of including additional aeolian processes for improving the performance of ESM aerosol simulations and potentially enhancing model assessments of how dust impacts climate and ecosystem changes.

Water storage plays a profound role in the lives of people across the Middle East and North Africa (MENA) as it is the most water-stressed region worldwide. The lands around the Caspian and Mediterranean seas are simulated to be very sensitive to future climate warming. Available water capacity depends on hydroclimate variables such as temperature and precipitation that will depend on socioeconomic pathways and changes in climate. This work explores changes in both the mean and extreme terrestrial water storage (TWS) under an unmitigated greenhouse gas (GHG) scenario (SSP5-8.5) and stratospheric aerosol intervention (SAI) designed to offset GHG-induced warming above 1.5 ∘C and compares both with historical period simulations. Both mean TWS and extreme TWS are projected to significantly decrease under SSP5-8.5 over the domain, except for the Arabian Peninsula, particularly in the wetter lands around the Caspian and Mediterranean seas. Relative to global warming, SAI partially ameliorates the decreased mean TWS in the wet regions, while it has no significant effect on the increased TWS in drier lands. In the entire domain studied, the mean TWS is larger under SAI than pure GHG forcing, mainly due to the significant cooling and, in turn, a substantial decrease in evapotranspiration under SAI relative to SSP5-8.5. Changes in extreme water storage excursions under global warming are reduced by SAI. Extreme TWS under both future climate scenarios is larger than throughout the historical period across Iran, Iraq, and the Arabian Peninsula, but the response of the more continental eastern North Africa hyper-arid climate is different from the neighboring dry lands. In the latter case, we note a reduction in the mean TWS trend under both GHG and SAI scenarios, with extreme TWS values also showing a decline compared to historical conditions.

We implemented the Community Aerosol and Radiation Model for Atmospheres (CARMA) in both the high- and low-top model versions of the Community Earth System Model Version 2 (CESM2). CARMA is a sectional microphysical model, which we use for aerosol in both the troposphere and stratosphere. CARMA is fully coupled to chemistry, clouds, radiation, and transport routines in CESM2. This development enables the comparison of simulations with a sectional (CARMA) and a modal (MAM4) aerosol microphysical model in the same modeling framework. The new implementation of CARMA has been adopted from previous work, with some additions that align with the current CESM2 Modal Aerosol Model (MAM4) implementation. The main updates include an interactive secondary organic aerosol description in CARMA, using the volatility basis set (VBS) approach, updated wet removal, and the use of transient emissions of aerosols and trace gases. In addition, we implemented an alternative aerosol nucleation scheme in CARMA, which is also used in MAM4. Detailed comparisons of stratospheric aerosol properties after the Mount Pinatubo eruption reveal the importance of prescribing sulfur injections in a larger region rather than in a single column to better represent the observed evolution of aerosols. Both CARMA and MAM4 in CESM2 are able to represent stratospheric and tropospheric aerosol properties reasonably well when compared to observations. Several differences in the performance of the two aerosol models show, in general, an improved representation of aerosols when using the sectional aerosol model in CESM2. These include a better representation of the aerosol size distribution after the Mount Pinatubo volcanic eruption in CARMA compared to MAM4. MAM4 produces on average smaller aerosols and less removal than CARMA, which results in a larger total mass. Both CARMA and MAM4 reproduce the stratospheric aerosol optical depth (AOD) within the error bar of the observations between 2001 and 2020, except for recent larger volcanic eruptions that are overestimated by both model configurations. The CARMA background surface area density and aerosol size distribution in the stratosphere and troposphere compare well to observations, with some underestimation of the Aitken-mode size range. MAM4 shows shortcomings in reproducing coarse-mode aerosol distributions in the stratosphere and troposphere. This work outlines additional development needs for CESM2 CARMA to improve the model compared to observations in both the troposphere and stratosphere.

The Multi-Scale Infrastructure for Chemistry and Aerosols Version 0 (MUSICAv0) is a new community modeling infrastructure that enables the study of atmospheric composition and chemistry across all relevant scales. We develop a MUSICAv0 grid with Africa refinement (∼ 28 km × 28 km over Africa). We evaluate the MUSICAv0 simulation for 2017 with in situ observations and compare the model results to satellite products over Africa. A simulation from the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), a regional model that is widely used in Africa studies, is also included in the analyses as a reference. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Both models underestimate carbon monoxide (CO) compared to in situ observations and satellite CO column retrievals from the Measurements of Pollution in the Troposphere (MOPITT) satellite instrument. MUSICAv0 tends to overestimate ozone (O3), likely due to overestimated stratosphere-to-troposphere flux of ozone. Both models significantly underestimate fine particulate matter (PM2.5) at two surface sites in East Africa. The MUSICAv0 simulation agrees better with aerosol optical depth (AOD) retrievals from the Moderate Resolution Imaging Spectroradiometer (MODIS) and tropospheric nitrogen dioxide (NO2) column retrievals from the Ozone Monitoring Instrument (OMI) than WRF-Chem. MUSICAv0 has a consistently lower tropospheric formaldehyde (HCHO) column than OMI retrievals. Based on model–satellite discrepancies between MUSICAv0 and WRF-Chem and MOPITT CO, MODIS AOD, and OMI tropospheric NO2, we find that future field campaign(s) and more in situ observations in the East African region (5∘ S–5∘ N, 30–45∘ E) could substantially improve the predictive skill of atmospheric chemistry model(s). This suggested focus region exhibits the largest model–in situ observation discrepancies, as well as targets for high population density, land cover variability, and anthropogenic pollution sources.

Near-term in-plume ozone depletion was observed for about 10 d by the Aura Microwave Limb Sounder (MLS) right after the January 2022 Hunga Tonga–Hunga Ha'apai (HTHH) eruption. This work analyzes the dynamic and chemical causes of this ozone depletion. The results show that the large water injection (∼ 150 Tg) from the HTHH eruption, with ∼ 0.0013 Tg injection of ClO (or ∼ 0.0009 Tg of HCl), causes ozone loss due to strongly enhanced HOx and ClOx cycles and their interactions. Aside from the gas-phase chemistry, the heterogeneous reaction rate for HOCl + HCl → Cl2 + H2O increases to 104 cm−3 s−1 and is a major cause of chlorine activation, making this event unique compared with the springtime polar ozone depletion where HCl + ClONO2 is more important. The large water injection causes relative humidity over ice to increase to 70 %–100 %, decreases the H2SO4 / H2O binary solution weight percent to 35 % compared with the 70 % ambient value, and decreases the plume temperature by 2–6 K. These changes lead to high heterogeneous reaction rates. Plume lofting of ozone-poor air is evident during the first 2 d after the eruption, but ozone concentrations quickly recover because its chemical lifetime is short at 20 hPa. With such a large seawater injection, we expect that ∼ 5 Tg Cl was lifted into the stratosphere by the HTHH eruption in the form of NaCl, but only ∼ 0.02 % of that remained as active chlorine in the stratosphere. Lightning NOx changes are probably not the reason for the HTHH initial in-plume O3 loss.

The Middle East and North Africa (MENA) region is the dustiest region in the world, and understanding the projected changes in the dust concentrations in the region is crucial. Stratospheric aerosol injection (SAI) geoengineering aims to reduce global warming by increasing the reflection of a small amount of the incoming solar radiation to space, hence reducing the global surface temperatures. Using the output from the Geoengineering Large Ensemble Project (GLENS), we show a reduction in the dust concentration in the MENA region under both the global warming (RCP8.5) and GLENS-SAI scenarios compared to the present-day climate. This reduction in dust over the whole MENA region is stronger under the SAI scenario, except over dust hotspots and for the dry season. In other words, in the summer, with the strongest dust events, more reduction has been projected for the global warming scenario compared to the SAI scenario. The maximum reduction in the dust concentrations in the MENA region (under both global warming and SAI) is due to the weakening of the dust hotspot emissions from the sources of the Middle East. Further analysis of the differences in the surface temperature, soil water, precipitation, leaf area index and near-surface wind speed provides some insights into the underlying physical mechanisms that determine the changes in the future dust concentrations in the MENA region. Detailed correlation analysis over dust hotspots indicates that lower future dust concentrations are controlled by lower wind speed and higher precipitation in these regions under both the RCP8.5 and SAI scenarios.

The Community Earth System Model (CESM) community has been providing versatile modeling options, with simple to complex chemistry and aerosol schemes in a single model, in order to support the broad scientific community with various research interests. While different model configurations are available in CESM and these can be used for different fields of Earth system science, simulation results that are consistent across configurations are still desirable. Here we develop a new simple secondary organic aerosol (SOA) scheme in the Community Atmosphere Model (CAM) version 6.3, the atmospheric component of the CESM. The main purpose of this simplified SOA scheme is to reduce the differences in aerosol concentrations and radiative fluxes between CAM and CAM with detailed chemistry (CAM-chem) while maintaining the computational efficiency of CAM. CAM simulation results using the default CAM6 and the new SOA schemes are compared to CAM-chem results as a reference. More consistent SOA concentrations are obtained globally when using the new SOA scheme for both temporal and spatial variabilities. The new SOA scheme shows that 62 % of grid cells globally are within a factor of 2 compared to the CAM-chem SOA concentrations, which is improved from 24 % when using the default CAM6 SOA scheme. Furthermore, other carbonaceous aerosols (black carbon and primary organic aerosol) in CAM6 become closer to CAM-chem results due to more similar microphysical aging timescales influenced by SOA coating, which in turn leads to comparable wet deposition fluxes. This results in an improved global atmospheric burden and concentrations at the high latitudes of the Northern Hemisphere compared to the full chemistry version (CAM-chem). As a consequence, the radiative flux differences between CAM-chem and CAM in the Arctic region (up to 6 W m−2) are significantly reduced for both nudged and free-running simulations. We find that the CAM6 SOA scheme can still be used for radiative forcing calculation as the high biases exist both in pre-industrial and present conditions, but studies focusing on the instantaneous radiative effects would benefit from using the SOA scheme developed in this study. The new SOA scheme also has technical advantages including the use of identical SOA precursor emissions as CAM-chem from the online biogenic emissions instead of pre-calculated emissions that may introduce differences. Future parameter updates to the CAM-chem SOA scheme can be easily translated to the new CAM SOA scheme as it is derived from the CAM-chem SOA scheme.

We investigate the potential impact of stratospheric aerosol intervention (SAI) on the spatiotemporal behavior of large-scale climate teleconnection patterns represented by the North Atlantic Oscillation (NAO), Pacific Decadal Oscillation (PDO), El Niño–Southern Oscillation (ENSO) and Atlantic Multidecadal Oscillation (AMO) indices using simulations from the Community Earth System Model versions 1 and 2 (CESM1 and CESM2). The leading empirical orthogonal function of sea surface temperature (SST) anomalies indicates that greenhouse gas (GHG) forcing is accompanied by increases in variance across both the North Atlantic (i.e., AMO) and North Pacific (i.e., PDO) and a decrease over the tropical Pacific (i.e., ENSO); however, SAI effectively reverses these global-warming-imposed changes. The projected spatial patterns of SST anomaly related to ENSO show no significant change under either global warming or SAI. In contrast, the spatial anomaly pattern changes pertaining to the AMO (i.e., in the North Atlantic) and PDO (i.e., in the North Pacific) under global warming are effectively suppressed by SAI. For the AMO, the low contrast between the cold-tongue pattern and its surroundings in the North Atlantic, predicted under global warming, is restored under SAI scenarios to similar patterns as in the historical period. The frequencies of El Niño and La Niña episodes modestly increase with GHG emissions in CESM2, while SAI tends to compensate for them. All climate indices' dominant modes of inter-annual variability are projected to be preserved in both warming and SAI scenarios. However, the dominant decadal variability mode changes in the AMO, NAO, and PDO induced by global warming are not suppressed by SAI.

We quantify future changes in wildfire burned area and carbon emissions in the 21st century under four Shared Socioeconomic Pathways (SSPs) scenarios and two SSP5-8.5-based solar geoengineering scenarios with a target surface temperature defined by SSP2-4.5 – solar irradiance reduction (G6solar) and stratospheric sulfate aerosol injections (G6sulfur) – and explore the mechanisms that drive solar geoengineering impacts on fires. This study is based on fully coupled climate–chemistry simulations with simulated occurrence of fires (burned area and carbon emissions) using the Whole Atmosphere Community Climate Model version 6 (WACCM6) as the atmospheric component of the Community Earth System Model version 2 (CESM2). Globally, total wildfire burned area is projected to increase over the 21st century under scenarios without geoengineering and decrease under the two geoengineering scenarios. By the end of the century, the two geoengineering scenarios have lower burned area and fire carbon emissions than not only their base-climate scenario SSP5-8.5 but also the targeted-climate scenario SSP2-4.5. Geoengineering reduces wildfire occurrence by decreasing surface temperature and wind speed and increasing relative humidity and soil water, with the exception of boreal regions where geoengineering increases the occurrence of wildfires due to a decrease in relative humidity and soil water compared with the present day. This leads to a global reduction in burned area and fire carbon emissions by the end of the century relative to their base-climate scenario SSP5-8.5. However, geoengineering also yields reductions in precipitation compared with a warming climate, which offsets some of the fire reduction. Overall, the impacts of the different driving factors are larger on burned area than fire carbon emissions. In general, the stratospheric sulfate aerosol approach has a stronger fire-reducing effect than the solar irradiance reduction approach.

The Geoengineering Model Intercomparison Project (GeoMIP) is a coordinating framework, started in 2010, that includes a series of standardized climate model experiments aimed at understanding the physical processes and projected impacts of solar geoengineering. Numerous experiments have been conducted, and numerous more have been proposed as “test-bed” experiments, spanning a variety of geoengineering techniques aimed at modifying the planetary radiation budget: stratospheric aerosol injection, marine cloud brightening, surface albedo modification, cirrus cloud thinning, and sunshade mirrors. To date, more than 100 studies have been published that used results from GeoMIP simulations. Here we provide a critical assessment of GeoMIP and its experiments. We discuss its successes and missed opportunities, for instance in terms of which experiments elicited more interest from the scientific community and which did not, and the potential reasons why that happened. We also discuss the knowledge that GeoMIP has contributed to the field of geoengineering research and climate science as a whole: what have we learned in terms of intermodel differences, robustness of the projected outcomes for specific geoengineering methods, and future areas of model development that would be necessary in the future? We also offer multiple examples of cases where GeoMIP experiments were fundamental for international assessments of climate change. Finally, we provide a series of recommendations, regarding both future experiments and more general activities, with the goal of continuously deepening our understanding of the effects of potential geoengineering approaches and reducing uncertainties in climate outcomes, important for assessing wider impacts on societies and ecosystems. In doing so, we refine the purpose of GeoMIP and outline a series of criteria whereby GeoMIP can best serve its participants, stakeholders, and the broader science community.

The teleconnection between the quasi-biennial oscillation (QBO) and the Arctic stratospheric polar vortex, or the Holton–Tan (HT) relationship, may change in a warmer climate or one with stratospheric aerosol intervention (SAI) compared to the present-day climate (PDC). Our results from an Earth system model indicate that, under both global warming (based on RCP8.5 emission scenario) and SAI scenarios, the HT relationship weakens in early winter (November–December), although it is closer to PDC under SAI than under the RCP8.5 scenario. In contrast, the HT relationship in the middle to late winter period (January–February) does not change considerably in response to either RCP8.5 or SAI scenarios compared to PDC. While the weakening of the HT relationship under the RCP8.5 scenario is likely due to the weaker QBO wind amplitudes at the Equator, another physical mechanism must be responsible for the weaker HT relationship under SAI scenarios, since the amplitude of the QBO wind is comparable to the PDC. The strength of the polar vortex does not change under the RCP8.5 scenario compared to PDC, but it becomes stronger under SAI; we attribute the weakening of the HT relationship under SAI to a stronger polar vortex. In general, the changes in the HT relationship cannot be explained by changes to the critical line; the changes in the residual circulation (particularly due to the gravity wave contributions) are important in explaining the changes in the HT relationship under RCP8.5 and SAI scenarios.

The northern-high-latitude permafrost contains almost twice the carbon content of the atmosphere, and it is widely considered to be a non-linear and tipping element in the earth's climate system under global warming. Solar geoengineering is a means of mitigating temperature rise and reduces some of the associated climate impacts by increasing the planetary albedo; the permafrost thaw is expected to be moderated under slower temperature rise. We analyze the permafrost response as simulated by five fully coupled earth system models (ESMs) and one offline land surface model under four future scenarios; two solar geoengineering scenarios (G6solar and G6sulfur) based on the high-emission scenario (ssp585) restore the global temperature from the ssp585 levels to the moderate-mitigation scenario (ssp245) levels via solar dimming and stratospheric aerosol injection. G6solar and G6sulfur can slow the northern-high-latitude permafrost degradation but cannot restore the permafrost states from ssp585 to those under ssp245. G6solar and G6sulfur tend to produce a deeper active layer than ssp245 and expose more thawed soil organic carbon (SOC) due to robust residual high-latitude warming, especially over northern Eurasia. G6solar and G6sulfur preserve more SOC of 4.6 ± 4.6 and 3.4 ± 4.8 Pg C (coupled ESM simulations) or 16.4 ± 4.7 and 12.3 ± 7.9 Pg C (offline land surface model simulations), respectively, than ssp585 in the northern near-surface permafrost region. The turnover times of SOC decline slower under G6solar and G6sulfur than ssp585 but faster than ssp245. The permafrost carbon–climate feedback is expected to be weaker under solar geoengineering.

Abstract Simulating whole atmosphere dynamics, chemistry, and physics is computationally expensive. It can require high vertical resolution throughout the middle and upper atmosphere, as well as a comprehensive chemistry and aerosol scheme coupled to radiation physics. An unintentional outcome of the development of one of the most sophisticated and hence computationally expensive model configurations is that it often excludes a broad community of users with limited computational resources. Here, we analyze two configurations of the Community Earth System Model Version 2, Whole Atmosphere Community Climate Model Version 6 (CESM2(WACCM6)) with simplified “middle atmosphere” chemistry at nominal 1 and 2° horizontal resolutions. Using observations, a reanalysis, and direct model comparisons, we find that these configurations generally reproduce the climate, variability, and climate sensitivity of the 1° nominal horizontal resolution configuration with comprehensive chemistry. While the background stratospheric aerosol optical depth is elevated in the middle atmosphere configurations as compared to the comprehensive chemistry configuration, it is comparable among all configurations during volcanic eruptions. For any purposes other than those needing an accurate representation of tropospheric organic chemistry and secondary organic aerosols, these simplified chemistry configurations deliver reliable simulations of the whole atmosphere that require 35% and 86% fewer computational resources at nominal 1 and 2° horizontal resolution, respectively.

Extreme weather events have been demonstrated to be increasing in frequency and intensity across the globe and are anticipated to increase further with projected changes in climate. Solar climate intervention strategies, specifically stratospheric aerosol injection (SAI), have the potential to minimize some of the impacts of a changing climate while more robust reductions in greenhouse gas emissions take effect. However, to date little attention has been paid to the possible responses of extreme weather and climate events under climate intervention scenarios. We present an analysis of 16 extreme surface temperature and precipitation indices, as well as associated vegetation responses, applied to the Geoengineering Large Ensemble (GLENS). GLENS is an ensemble of simulations performed with the Community Earth System Model (CESM1) wherein SAI is simulated to offset the warming produced by a high-emission scenario throughout the 21st century, maintaining surface temperatures at 2020 levels. GLENS is generally successful at maintaining global mean temperature near 2020 levels; however, it does not completely offset some of the projected warming in northern latitudes. Some regions are also projected to cool substantially in comparison to the present day, with the greatest decreases in daytime temperatures. The differential warming–cooling also translates to fewer very hot days but more very hot nights during the summer and fewer very cold days or nights compared to the current day. Extreme precipitation patterns, for the most part, are projected to reduce in intensity in areas that are wet in the current climate and increase in intensity in dry areas. We also find that the distribution of daily precipitation becomes more consistent with more days with light rain and fewer very intense events than currently occur. In many regions there is a reduction in the persistence of long dry and wet spells compared to present day. However, asymmetry in the night and day temperatures, together with changes in cloud cover and vegetative responses, could exacerbate drying in regions that are already sensitive to drought. Overall, our results suggest that while SAI may ameliorate some of the extreme weather hazards produced by global warming, it would also present some significant differences in the distribution of climate extremes compared to the present day.

This study assesses the impacts of stratospheric aerosol intervention (SAI) and solar dimming on stratospheric ozone based on the G6 Geoengineering Model Intercomparison Project (GeoMIP) experiments, called G6sulfur and G6solar. For G6sulfur, an enhanced stratospheric sulfate aerosol burden reflects some of the incoming solar radiation back into space to cool the surface climate, while for G6solar, the reduction in the global solar constant in the model achieves the same goal. Both experiments use the high emissions scenario of SSP5-8.5 as the baseline experiment and define surface temperature from the medium emission scenario of SSP2-4.5 as the target. In total, six Earth system models (ESMs) performed these experiments, and three out of the six models include interactive stratospheric chemistry. The increase in absorbing sulfate aerosols in the stratosphere results in a heating of the lower tropical stratospheric temperatures by between 5 to 13 K for the six different ESMs, leading to changes in stratospheric transport, water vapor, and other related changes. The increase in the aerosol burden also increases aerosol surface area density, which is important for heterogeneous chemical reactions. The resulting changes in the springtime Antarctic ozone between the G6sulfur and SSP5-8.5, based on the three models with interactive chemistry, include an initial reduction in total column ozone (TCO) of 10 DU (ranging between 0–30 DU for the three models) and up to 20 DU (between 10–40 DU) by the end of the century. The relatively small reduction in TCO for the multi-model mean in the first 2 decades results from variations in the required sulfur injections in the models and differences in the complexity of the chemistry schemes. In contrast, in the Northern Hemisphere (NH) high latitudes, no significant changes can be identified due to the large natural variability in the models, with little change in TCO by the end of the century. However, all three models with interactive chemistry consistently simulate an increase in TCO in the NH mid-latitudes up to 20 DU, compared to SSP5-8.5, in addition to the 20 DU increase resulting from increasing greenhouse gases between SSP2-4.5 and SSP5-8.5. In contrast to G6sulfur, G6solar does not significantly change stratospheric temperatures compared to the baseline simulation. Solar dimming results in little change in TCO compared to SSP5-8.5. Only in the tropics does G6solar result in an increase of TCO of up to 8 DU, compared to SSP2-4.5, which may counteract the projected reduction in SSP5-8.5. This work identifies differences in the response of SAI and solar dimming on ozone for three ESMs with interactive chemistry, which are partly due to the differences and shortcomings in the complexity of aerosol microphysics, chemistry, and the description of ozone photolysis. It also identifies that solar dimming, if viewed as an analog to SAI using a predominantly scattering aerosol, would succeed in reducing tropospheric and surface temperatures, but any stratospheric changes due to the high forcing greenhouse gas scenario, including the potential harmful increase in TCO beyond historical values, would prevail.

As part of the Geoengineering Model Intercomparison Project a numerical experiment known as G6sulfur has been designed in which temperatures under a high-forcing future scenario (SSP5-8.5) are reduced to those under a medium-forcing scenario (SSP2-4.5) using the proposed geoengineering technique of stratospheric aerosol intervention (SAI). G6sulfur involves introducing sulfuric acid aerosol into the tropical stratosphere where it reflects incoming sunlight back to space, thus cooling the planet. Here, we compare the results from six Earth-system models that have performed the G6sulfur experiment and examine how SAI affects two important modes of natural variability, the northern wintertime North Atlantic Oscillation (NAO) and the Quasi-Biennial Oscillation (QBO). Although all models show that SAI is successful in reducing global mean temperature as designed, they are also consistent in showing that it forces an increasingly positive phase of the NAO as the injection rate increases over the course of the 21st century, exacerbating precipitation reductions over parts of southern Europe compared with SSP5-8.5. In contrast to the robust result for the NAO, there is less consistency for the impact on the QBO, but the results nevertheless indicate a risk that equatorial SAI could cause the QBO to stall and become locked in a phase with permanent westerly winds in the lower stratosphere.

Simulating the complex aerosol microphysical processes in a comprehensive Earth system model can be very computationally intensive; therefore many models utilize a modal approach, where aerosol size distributions are represented by observation-derived lognormal functions, and internal mixing between different aerosol species within an aerosol mode is often assumed. This approach has been shown to yield satisfactory results across a large array of applications, but there may be cases where the simplification in this approach may produce some shortcomings. In this work we show specific conditions under which the current approximations used in some modal approaches might yield incorrect answers. Using results from the Community Earth System Model v1 (CESM1) Geoengineering Large Ensemble (GLENS) project, we analyze the effects in the troposphere of a continuous increasing load of sulfate aerosols in the stratosphere, with the aim of counteracting the surface warming produced by non-mitigated increasing greenhouse gas (GHG) concentrations between 2020–2100. We show that the simulated results pertaining to the evolution of sea salt and dust aerosols in the upper troposphere are not realistic due to internal mixing assumptions in the modal aerosol treatment, which in this case reduces the size, and thus the settling velocities, of those particles and ultimately changes their mixing ratio below the tropopause. The unnatural increase of these aerosol species affects, in turn, the simulation of upper tropospheric ice formation, resulting in an increase in ice clouds that is not due to any meaningful physical mechanisms. While we show that this does not significantly affect the overall results of the simulations, we point to some areas where results should be interpreted with care in modeling simulations using similar approximations: in particular, in the evolution of upper tropospheric clouds when large amounts of sulfate are present in the stratosphere, as after a large explosive volcanic eruption or in similar stratospheric aerosol injection cases. Finally, we suggest that this can be avoided if sulfate aerosols in the coarse mode, the predominant species in these situations, are treated separately from other aerosol species in the model.

Injecting sulfur dioxide into the stratosphere with the intent to create an artificial reflective aerosol layer is one of the most studied options for solar radiation management. Previous modelling studies have shown that stratospheric sulfur injections have the potential to compensate for the greenhouse-gas-induced warming at the global scale. However, there is significant diversity in the modelled radiative forcing from stratospheric aerosols depending on the model and on which strategy is used to inject sulfur into the stratosphere. Until now, it has not been clear how the evolution of the aerosols and their resulting radiative forcing depends on the aerosol microphysical scheme used – that is, if aerosols are represented by a modal or sectional distribution. Here, we have studied different spatio-temporal injection strategies with different injection magnitudes using the aerosol–climate model ECHAM-HAMMOZ with two aerosol microphysical modules: the sectional module SALSA (Sectional Aerosol module for Large Scale Applications) and the modal module M7. We found significant differences in the model responses depending on the aerosol microphysical module used. In a case where SO2 was injected continuously in the equatorial stratosphere, simulations with SALSA produced an 88 %–154 % higher all-sky net radiative forcing than simulations with M7 for injection rates from 1 to 100 Tg (S) yr−1. These large differences are identified to be caused by two main factors. First, the competition between nucleation and condensation: while injected sulfur tends to produce new particles at the expense of gaseous sulfuric acid condensing on pre-existing particles in the SALSA module, most of the gaseous sulfuric acid partitions to particles via condensation at the expense of new particle formation in the M7 module. Thus, the effective radii of stratospheric aerosols were 10 %–52 % larger in M7 than in SALSA, depending on the injection rate and strategy. Second, the treatment of the modal size distribution in M7 limits the growth of the accumulation mode which results in a local minimum in the aerosol number size distribution between the accumulation and coarse modes. This local minimum is in the size range where the scattering of solar radiation is most efficient. We also found that different spatial-temporal injection strategies have a significant impact on the magnitude and zonal distribution of radiative forcing. Based on simulations with various injection rates using SALSA, the most efficient studied injection strategy produced a 33 %–42 % radiative forcing compared with the least efficient strategy, whereas simulations with M7 showed an even larger difference of 48 %–116 %. Differences in zonal mean radiative forcing were even larger than that. We also show that a consequent stratospheric heating and its impact on the quasi-biennial oscillation depend on both the injection strategy and the aerosol microphysical model. Overall, these results highlight the crucial impact of aerosol microphysics on the physical properties of stratospheric aerosol which, in turn, causes significant uncertainties in estimating the climate impacts of stratospheric sulfur injections.

Specified dynamics schemes are ubiquitous modeling tools for isolating the roles of dynamics and transport on chemical weather and climate. They typically constrain the circulation of a chemistry–climate model to the circulation in a reanalysis product through linear relaxation. However, recent studies suggest that these schemes create a divergence in chemical climate and the meridional circulation between models and do not accurately reproduce trends in the circulation. In this study we perform a systematic assessment of the specified dynamics scheme in the Community Earth System Model version 2, Whole Atmosphere Community Climate Model version 6 (CESM2 (WACCM6)), which proactively nudges the circulation toward the reference meteorology. Specified dynamics experiments are performed over a wide range of nudging timescales and reference meteorology frequencies, with the model's circulation nudged to its own free-running output – a clean test of the specified dynamics scheme. Errors in the circulation scale robustly and inversely with meteorology frequency and have little dependence on the nudging timescale. However, the circulation strength and errors in tracers, tracer transport, and convective mass flux scale robustly and inversely with the nudging timescale. A 12 to 24 h nudging timescale at the highest possible reference meteorology frequency minimizes errors in tracers, clouds, and the circulation, even up to the practical limit of one reference meteorology update every time step. The residual circulation and eddy mixing integrate tracer errors and accumulate them at the end of their characteristic transport pathways, leading to elevated error in the upper troposphere and lower stratosphere and in the polar stratosphere. Even in the most ideal case, there are non-negligible errors in tracers introduced by the nudging scheme. Future development of more sophisticated nudging schemes may be necessary for further progress.

In order to fight the spread of the global COVID-19 pandemic, most of the world's countries have taken control measures such as lockdowns during a few weeks to a few months. These lockdowns had significant impacts on economic and personal activities in many countries. Several studies using satellite and surface observations have reported important changes in the spatial and temporal distributions of atmospheric pollutants and greenhouse gases. Global and regional chemistry-transport model studies are being performed in order to analyze the impact of these lockdowns on the distribution of atmospheric compounds. These modeling studies aim at evaluating the impact of the regional lockdowns at the global scale. In order to provide input for the global and regional model simulations, a dataset providing adjustment factors (AFs) that can easily be applied to current global and regional emission inventories has been developed. This dataset provides, for the January–August 2020 period, gridded AFs at a 0.1×0.1 latitude–longitude degree resolution on a daily or monthly basis for the transportation (road, air and ship traffic), power generation, industry and residential sectors. The quantification of AFs is based on activity data collected from different databases and previously published studies. A range of AFs are provided at each grid point for model sensitivity studies. The emission AFs developed in this study are applied to the CAMS global inventory (CAMS-GLOB-ANT_v4.2_R1.1), and the changes in emissions of the main pollutants are discussed for different regions of the world and the first 6 months of 2020. Maximum decreases in the total emissions are found in February in eastern China, with an average reduction of 20 %–30 % in NOx, NMVOCs (non-methane volatile organic compounds) and SO2 relative to the reference emissions. In the other regions, the maximum changes occur in April, with average reductions of 20 %–30 % for NOx, NMVOCs and CO in Europe and North America and larger decreases (30 %–50 %) in South America. In India and African regions, NOx and NMVOC emissions are reduced on average by 15 %–30 %. For the other species, the maximum reductions are generally less than 15 %, except in South America, where large decreases in CO and BC (black carbon) are estimated. As discussed in the paper, reductions vary highly across regions and sectors due to the differences in the duration of the lockdowns before partial or complete recovery. The dataset providing a range of AFs (average and average ± standard deviation) is called CONFORM (COvid-19 adjustmeNt Factors fOR eMissions) (https://doi.org/10.25326/88; Doumbia et al., 2020). It is distributed by the Emissions of atmospheric Compounds and Compilation of Ancillary Data (ECCAD) database (https://eccad.aeris-data.fr/, last access: 23 August 2021).

We present here results from the Geoengineering Model Intercomparison Project (GeoMIP) simulations for the experiments G6sulfur and G6solar for six Earth system models participating in the Climate Model Intercomparison Project (CMIP) Phase 6. The aim of the experiments is to reduce the warming that results from a high-tier emission scenario (Shared Socioeconomic Pathways SSP5-8.5) to that resulting from a medium-tier emission scenario (SSP2-4.5). These simulations aim to analyze the response of climate models to a reduction in incoming surface radiation as a means to reduce global surface temperatures, and they do so either by simulating a stratospheric sulfate aerosol layer or, in a more idealized way, through a uniform reduction in the solar constant in the model. We find that over the final two decades of this century there are considerable inter-model spreads in the needed injection amounts of sulfate (29 ± 9 Tg-SO2/yr between 2081 and 2100), in the latitudinal distribution of the aerosol cloud and in the stratospheric temperature changes resulting from the added aerosol layer. Even in the simpler G6solar experiment, there is a spread in the needed solar dimming to achieve the same global temperature target (1.91 ± 0.44 %). The analyzed models already show significant differences in the response to the increasing CO2 concentrations for global mean temperatures and global mean precipitation (2.05 K ± 0.42 K and 2.28 ± 0.80 %, respectively, for SSP5-8.5 minus SSP2-4.5 averaged over 2081–2100). With aerosol injection, the differences in how the aerosols spread further change some of the underlying uncertainties, such as the global mean precipitation response (−3.79 ± 0.76 % for G6sulfur compared to −2.07 ± 0.40 % for G6solar against SSP2-4.5 between 2081 and 2100). These differences in the behavior of the aerosols also result in a larger uncertainty in the regional surface temperature response among models in the case of the G6sulfur simulations, suggesting the need to devise various, more specific experiments to single out and resolve particular sources of uncertainty. The spread in the modeled response suggests that a degree of caution is necessary when using these results for assessing specific impacts of geoengineering in various aspects of the Earth system. However, all models agree that compared to a scenario with unmitigated warming, stratospheric aerosol geoengineering has the potential to both globally and locally reduce the increase in surface temperatures.

Black carbon (BC) emissions play an important role in regional climate change in the Arctic. It is necessary to pay attention to the impact of long-range transport from regions outside the Arctic as BC emissions from local sources in the Arctic were relatively small. The task force Hemispheric Transport of Air Pollution Phase 2 (HTAP2) set up a series of simulation scenarios to investigate the response of BC in a given region to different source regions. This study investigated the responses of Arctic BC concentrations and surface temperature to 20 % anthropogenic emission reductions from six regions in 2010 within the framework of HTAP2 based on ensemble modeling results. Emission reductions from East Asia (EAS) had the most (monthly contributions: 0.2–1.5 ng m−3) significant impact on the Arctic near-surface BC concentrations, while the monthly contributions from Europe (EUR), Middle East (MDE), North America (NAM), Russia–Belarus–Ukraine (RBU), and South Asia (SAS) were 0.2–1.0, 0.001–0.01, 0.1–0.3, 0.1–0.7, and 0.0–0.2 ng m−3, respectively. The responses of the vertical profiles of the Arctic BC to the six regions were found to be different due to multiple transport pathways. Emission reductions from NAM, RBU, EUR, and EAS mainly influenced the BC concentrations in the low troposphere of the Arctic, while most of the BC in the upper troposphere of the Arctic derived from SAS. The response of the Arctic BC to emission reductions in six source regions became less significant with the increase in the latitude. The benefit of BC emission reductions in terms of slowing down surface warming in the Arctic was evaluated by using absolute regional temperature change potential (ARTP). Compared to the response of global temperature to BC emission reductions, the response of Arctic temperature was substantially more sensitive, highlighting the need for curbing global BC emissions.

In this work, the impact of Los Angeles Basin pollution transport and stratospheric intrusions on the surface ozone levels observed in the San Gabriel Mountains is investigated based on a combination of surface and lidar measurements as well as WRF-Chem (Weather Research and Forecasting with Chemistry) and WACCM (Whole Atmosphere Community Climate Model) runs. The number of days with observed surface ozone levels exceeding the National Ambient Air Quality Standards exhibit a clear seasonal pattern, with a maximum during summer, when models suggest a minimum influence of stratospheric intrusions and the largest impact from Los Angeles Basin pollution transport. Additionally, measured and modeled surface ozone and PM10 were analyzed as a function of season, time of the day, and wind direction. Measurements and models are in good qualitative agreement, with maximum surface ozone observed for southwest and west winds. For the prevailing summer wind direction, slightly south of the ozone maximum and corresponding to south-southwest winds, lower ozone levels were observed. Back trajectories suggest that this is associated with transport from the central Los Angeles Basin, where titration limits the amount of surface ozone. A quantitative comparison of the lidar profiles with WRF-Chem and WACCM models revealed good agreement near the surface, with models showing an increasing positive bias as function of altitude, reaching 75 % at 15 km above sea level. Finally, three selected case studies covering the different mechanisms affecting the near-surface ozone concentration over the San Gabriel Mountains, namely stratospheric intrusions and pollution transport, are analyzed based on surface and ozone lidar measurements, as well as co-located ceilometer measurements and models.

Secondary organic aerosol (SOA) is a dominant contributor of fine particulate matter in the atmosphere, but the complexity of SOA formation chemistry hinders the accurate representation of SOA in models. Volatility-based SOA parameterizations have been adopted in many recent chemistry modeling studies and have shown a reasonable performance compared to observations. However, assumptions made in these empirical parameterizations can lead to substantial errors when applied to future climatic conditions as they do not include the mechanistic understanding of processes but are rather fitted to laboratory studies of SOA formation. This is particularly the case for SOA derived from isoprene epoxydiols (IEPOX SOA), for which we have a higher level of understanding of the fundamental processes than is currently parameterized in most models. We predict future SOA concentrations using an explicit mechanism and compare the predictions with the empirical parameterization based on the volatility basis set (VBS) approach. We then use the Community Earth System Model 2 (CESM2.1.0) with detailed isoprene chemistry and reactive uptake processes for the middle and end of the 21st century under four Shared Socioeconomic Pathways (SSPs): SSP1–2.6, SSP2–4.5, SSP3–7.0, and SSP5–8.5. With the explicit chemical mechanism, we find that IEPOX SOA is predicted to increase on average under all future SSP scenarios but with some variability in the results depending on regions and the scenario chosen. Isoprene emissions are the main driver of IEPOX SOA changes in the future climate, but the IEPOX SOA yield from isoprene emissions also changes by up to 50 % depending on the SSP scenario, in particular due to different sulfur emissions. We conduct sensitivity simulations with and without CO2 inhibition of isoprene emissions that is highly uncertain, which results in factor of 2 differences in the predicted IEPOX SOA global burden, especially for the high-CO2 scenarios (SSP3–7.0 and SSP5–8.5). Aerosol pH also plays a critical role in the IEPOX SOA formation rate, requiring accurate calculation of aerosol pH in chemistry models. On the other hand, isoprene SOA calculated with the VBS scheme predicts a nearly constant SOA yield from isoprene emissions across all SSP scenarios; as a result, it mostly follows isoprene emissions regardless of region and scenario. This is because the VBS scheme does not consider heterogeneous chemistry; in other words, there is no dependency on aerosol properties. The discrepancy between the explicit mechanism and VBS parameterization in this study is likely to occur for other SOA components as well, which may also have dependencies that cannot be captured by VBS parameterizations. This study highlights the need for more explicit chemistry or for parameterizations that capture the dependence on key physicochemical drivers when predicting SOA concentrations for climate studies.

The connection between the dominant mode of interannual variability in the tropical troposphere, the El Niño–Southern Oscillation (ENSO), and the entry of stratospheric water vapor is analyzed in a set of model simulations archived for the Chemistry-Climate Model Initiative (CCMI) project and for Phase 6 of the Coupled Model Intercomparison Project. While the models agree on the temperature response to ENSO in the tropical troposphere and lower stratosphere, and all models and observations also agree on the zonal structure of the temperature response in the tropical tropopause layer, the only aspect of the entry water vapor response with consensus in both models and observations is that La Niña leads to moistening in winter relative to neutral ENSO. For El Niño and for other seasons, there are significant differences among the models. For example, some models find that the enhanced water vapor for La Niña in the winter of the event reverses in spring and summer, some models find that this moistening persists, and some show a nonlinear response, with both El Niño and La Niña leading to enhanced water vapor in both winter, spring, and summer. A moistening in the spring following El Niño events, the signal focused on in much previous work, is simulated by only half of the models. Focusing on Central Pacific ENSO vs. East Pacific ENSO, or temperatures in the mid-troposphere compared with temperatures near the surface, does not narrow the inter-model discrepancies. Despite this diversity in response, the temperature response near the cold point can explain the response of water vapor when each model is considered separately. While the observational record is too short to fully constrain the response to ENSO, it is clear that most models suffer from biases in the magnitude of the interannual variability of entry water vapor. This bias could be due to biased cold-point temperatures in some models, but others appear to be missing forcing processes that contribute to observed variability near the cold point.

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.

Solar geoengineering has been receiving increased attention in recent years as a potential temporary solution to offset global warming. One method of approximating global-scale solar geoengineering in climate models is via solar reduction experiments. Two generations of models in the Geoengineering Model Intercomparison Project (GeoMIP) have now simulated offsetting a quadrupling of the CO2 concentration with solar reduction. This simulation is idealized and designed to elicit large responses in the models. Here, we show that energetics, temperature, and hydrological cycle changes in this experiment are statistically indistinguishable between the two ensembles. Of the variables analyzed here, the only major differences involve highly parameterized and uncertain processes, such as cloud forcing or terrestrial net primary productivity. We conclude that despite numerous structural differences and uncertainties in models over the past two generations of models, including an increase in climate sensitivity in the latest generation of models, the models are consistent in their aggregate climate response to global solar dimming.

The potential of heterogeneous chlorine activation in the midlatitude lowermost stratosphere during summer is a matter of debate. The occurrence of heterogeneous chlorine activation through the presence of aerosol particles could cause ozone destruction. This chemical process requires low temperatures and is accelerated by an enhancement of the stratospheric water vapour and sulfate amount. In particular, the conditions present in the lowermost stratosphere during the North American Summer Monsoon season (NAM) are expected to be cold and moist enough to cause the occurrence of heterogeneous chlorine activation. Furthermore, the temperatures, the water vapour mixing ratio and the sulfate aerosol abundance are affected by future global warming and by the potential application of sulfate geoengineering. Hence, both future scenarios could promote this ozone destruction process. We investigate the likelihood of the occurrence of heterogeneous chlorine activation and its impact on ozone in the lowermost-stratospheric mixing layer between tropospheric and stratospheric air above central North America (30.6–49.6∘ N, 72.25–124.75∘ W) in summer for conditions today, at the middle and at the end of the 21st century. Therefore, the results of the Geoengineering Large Ensemble Simulations (GLENS) for the lowermost-stratospheric mixing layer between tropospheric and stratospheric air are considered together with 10-day box-model simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). In GLENS two future scenarios are simulated: the RCP8.5 global warming scenario and a geoengineering scenario, where sulfur is additionally injected into the stratosphere to keep the global mean surface temperature from changing. In the GLENS simulations, the mixing layer will warm and moisten in both future scenarios with a larger effect in the geoengineering scenario. The likelihood of chlorine activation occurring in the mixing layer is highest in the years 2040–2050 if geoengineering is applied, accounting for 3.3 %. In comparison, the likelihood of conditions today is 1.0 %. At the end of the 21st century, the likelihood of this ozone destruction process occurring decreases. We found that 0.1 % of the ozone mixing ratios in the mixing layer above central North America is destroyed for conditions today. A maximum ozone destruction of 0.3 % in the mixing layer occurs in the years 2040–2050 if geoengineering is applied. Comparing the southernmost latitude band (30–35∘ N) and the northernmost latitude band (44–49∘ N) of the considered region, we found a higher likelihood of the occurrence of heterogeneous chlorine activation in the southernmost latitude band, causing a higher impact on ozone as well. However, the ozone loss process is found to have a minor impact on the midlatitude ozone column.

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 m−2 for SO2 emissions, −0.25 ± 0.09 W m−2 for organic carbon (OC), 0.15 ± 0.17 W m−2 for black carbon (BC) and −0.07 ± 0.01 W m−2 for NH3. For the combined aerosols (in the piClim-aer experiment) it is −1.01 ± 0.25 W m−2. The multi-model means for the reactive well-mixed greenhouse gases (including any effects on ozone and aerosol chemistry) are 0.67 ± 0.17 W m−2 for methane (CH4), 0.26 ± 0.07 W m−2 for nitrous oxide (N2O) and 0.12 ± 0.2 W m−2 for ozone-depleting halocarbons (HC). Emissions of the ozone precursors nitrogen oxides (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 m−2 respectively. The differences in ERFs calculated for the different models reflect differences in the complexity of their aerosol and chemistry schemes, especially in the case of methane where tropospheric chemistry captures increased forcing from ozone production.

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.

Every year during the Asian summer monsoon season from about mid-June to early September, a stable anticyclonic circulation system forms over the Himalayas. This Asian summer monsoon (ASM) anticyclone has been shown to promote transport of air into the stratosphere from the Asian troposphere, which contains large amounts of anthropogenic pollutants. Essential details of Asian monsoon transport, such as the exact timescales of vertical transport, the role of convection in cross-tropopause exchange, and the main location and level of export from the confined anticyclone to the stratosphere are still not fully resolved. Recent airborne observations from campaigns near the ASM anticyclone edge and centre in 2016 and 2017, respectively, show a steady decrease in carbon monoxide (CO) and increase in ozone (O3) with height starting from tropospheric values of around 100 ppb CO and 30–50 ppb O3 at about 365 K potential temperature. CO mixing ratios reach stratospheric background values below ∼25 ppb at about 420 K and do not show a significant vertical gradient at higher levels, while ozone continues to increase throughout the altitude range of the aircraft measurements. Nitrous oxide (N2O) remains at or only marginally below its 2017 tropospheric mixing ratio of 333 ppb up to about 400 K, which is above the local tropopause. A decline in N2O mixing ratios that indicates a significant contribution of stratospheric air is only visible above this level. Based on our observations, we draw the following picture of vertical transport and confinement in the ASM anticyclone: rapid convective uplift transports air to near 16 km in altitude, corresponding to potential temperatures up to about 370 K. Although this main convective outflow layer extends above the level of zero radiative heating (LZRH), our observations of CO concentration show little to no evidence of convection actually penetrating the tropopause. Rather, further ascent occurs more slowly, consistent with isentropic vertical velocities of 0.7–1.5 K d−1. For the key tracers (CO, O3, and N2O) in our study, none of which are subject to microphysical processes, neither the lapse rate tropopause (LRT) around 380 K nor the cold point tropopause (CPT) around 390 K marks a strong discontinuity in their profiles. Up to about 20 to 35 K above the LRT, isolation of air inside the ASM anticyclone prevents significant in-mixing of stratospheric air (throughout this text, the term in-mixing refers specifically to mixing processes that introduce stratospheric air into the predominantly tropospheric inner anticyclone). The observed changes in CO and O3 likely result from in situ chemical processing. Above about 420 K, mixing processes become more significant and the air inside the anticyclone is exported vertically and horizontally into the surrounding stratosphere.

The realization of the difficulty of limiting global-mean temperatures to within 1.5 or 2.0 ∘C above pre-industrial levels stipulated by the 21st Conference of Parties in Paris has led to increased interest in solar radiation management (SRM) techniques. Proposed SRM schemes aim to increase planetary albedo to reflect more sunlight back to space and induce a cooling that acts to partially offset global warming. Under the auspices of the Geoengineering Model Intercomparison Project, we have performed model experiments whereby global temperature under the high-forcing SSP5-8.5 scenario is reduced to follow that of the medium-forcing SSP2-4.5 scenario. Two different mechanisms to achieve this are employed: the first via a reduction in the solar constant (experiment G6solar) and the second via modelling injections of sulfur dioxide (experiment G6sulfur) which forms sulfate aerosol in the stratosphere. Results from two state-of-the-art coupled Earth system models (UKESM1 and CESM2-WACCM6) both show an impact on the North Atlantic Oscillation (NAO) in G6sulfur but not in G6solar. Both models show a persistent positive anomaly in the NAO during the Northern Hemisphere winter season in G6sulfur, suggesting an increase in zonal flow and an increase in North Atlantic storm track activity impacting the Eurasian continent and leading to high-latitude warming over Europe and Asia. These results are broadly consistent with previous findings which show similar impacts from stratospheric volcanic aerosol on the NAO and emphasize that detailed modelling of geoengineering processes is required if accurate impacts of SRM effects are to be simulated. Differences remain between the two models in predicting regional changes over the continental USA and Africa, suggesting that more models need to perform such simulations before attempting to draw any conclusions regarding potential continental-scale climate change under SRM.

Global coupled chemistry–climate models underestimate carbon monoxide (CO) in the Northern Hemisphere, exhibiting a pervasive negative bias against measurements peaking in late winter and early spring. While this bias has been commonly attributed to underestimation of direct anthropogenic and biomass burning emissions, chemical production and loss via OH reaction from emissions of anthropogenic and biogenic volatile organic compounds (VOCs) play an important role. Here we investigate the reasons for this underestimation using aircraft measurements taken in May and June 2016 from the Korea–United States Air Quality (KORUS-AQ) experiment in South Korea and the Air Chemistry Research in Asia (ARIAs) in the North China Plain (NCP). For reference, multispectral CO retrievals (V8J) from the Measurements of Pollution in the Troposphere (MOPITT) are jointly assimilated with meteorological observations using an ensemble adjustment Kalman filter (EAKF) within the global Community Atmosphere Model with Chemistry (CAM-Chem) and the Data Assimilation Research Testbed (DART). With regard to KORUS-AQ data, CO is underestimated by 42 % in the control run and by 12 % with the MOPITT assimilation run. The inversion suggests an underestimation of anthropogenic CO sources in many regions, by up to 80 % for northern China, with large increments over the Liaoning Province and the North China Plain (NCP). Yet, an often-overlooked aspect of these inversions is that correcting the underestimation in anthropogenic CO emissions also improves the comparison with observational O3 datasets and observationally constrained box model simulations of OH and HO2. Running a CAM-Chem simulation with the updated emissions of anthropogenic CO reduces the bias by 29 % for CO, 18 % for ozone, 11 % for HO2, and 27 % for OH. Longer-lived anthropogenic VOCs whose model errors are correlated with CO are also improved, while short-lived VOCs, including formaldehyde, are difficult to constrain solely by assimilating satellite retrievals of CO. During an anticyclonic episode, better simulation of O3, with an average underestimation of 5.5 ppbv, and a reduction in the bias of surface formaldehyde and oxygenated VOCs can be achieved by separately increasing by a factor of 2 the modeled biogenic emissions for the plant functional types found in Korea. Results also suggest that controlling VOC and CO emissions, in addition to widespread NOx controls, can improve ozone pollution over East Asia.

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.

Decadal trends and interannual variations in the hydroxyl radical (OH), while poorly constrained at present, are critical for understanding the observed evolution of atmospheric methane (CH4). Through analyzing the OH fields simulated by the model ensemble of the Chemistry–Climate Model Initiative (CCMI), we find (1) the negative OH anomalies during the El Niño years mainly corresponding to the enhanced carbon monoxide (CO) emissions from biomass burning and (2) a positive OH trend during 1980–2010 dominated by the elevated primary production and the reduced loss of OH due to decreasing CO after 2000. Both two-box model inversions and variational 4D inversions suggest that ignoring the negative anomaly of OH during the El Niño years leads to a large overestimation of the increase in global CH4 emissions by up to 10 ± 3 Tg yr−1 to match the observed CH4 increase over these years. Not accounting for the increasing OH trends given by the CCMI models leads to an underestimation of the CH4 emission increase by 23 ± 9 Tg yr−1 from 1986 to 2010. The variational-inversion-estimated CH4 emissions show that the tropical regions contribute most to the uncertainties related to OH. This study highlights the significant impact of climate and chemical feedbacks related to OH on the top-down estimates of the global CH4 budget.

This study presents a multiparameter analysis of aerosol trends over the last 2 decades at regional and global scales. Regional time series have been computed for a set of nine optical, chemical-composition and mass aerosol properties by using the observations from several ground-based networks. From these regional time series the aerosol trends have been derived for the different regions of the world. Most of the properties related to aerosol loading exhibit negative trends, both at the surface and in the total atmospheric column. Significant decreases in aerosol optical depth (AOD) are found in Europe, North America, South America, North Africa and Asia, ranging from −1.2 % yr−1 to −3.1 % yr−1. An error and representativity analysis of the spatially and temporally limited observational data has been performed using model data subsets in order to investigate how much the observed trends represent the actual trends happening in the regions over the full study period from 2000 to 2014. This analysis reveals that significant uncertainty is associated with some of the regional trends due to time and space sampling deficiencies. The set of observed regional trends has then been used for the evaluation of 10 models (6 AeroCom phase III models and 4 CMIP6 models) and the CAMS reanalysis dataset and of their skills in reproducing the aerosol trends. Model performance is found to vary depending on the parameters and the regions of the world. The models tend to capture trends in AOD, the column Ångström exponent, sulfate and particulate matter well (except in North Africa), but they show larger discrepancies for coarse-mode AOD. The rather good agreement of the trends, across different aerosol parameters between models and observations, when co-locating them in time and space, implies that global model trends, including those in poorly monitored regions, are likely correct. The models can help to provide a global picture of the aerosol trends by filling the gaps in regions not covered by observations. The calculation of aerosol trends at a global scale reveals a different picture from that depicted by solely relying on ground-based observations. Using a model with complete diagnostics (NorESM2), we find a global increase in AOD of about 0.2 % yr−1 between 2000 and 2014, primarily caused by an increase in the loads of organic aerosols, sulfate and black carbon.

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.

Calculating a multi-model mean, a commonly used method for ensemble averaging, assumes model independence and equal model skill. Sharing of model components amongst families of models and research centres, conflated by growing ensemble size, means model independence cannot be assumed and is hard to quantify. We present a methodology to produce a weighted-model ensemble projection, accounting for model performance and model independence. Model weights are calculated by comparing model hindcasts to a selection of metrics chosen for their physical relevance to the process or phenomena of interest. This weighting methodology is applied to the Chemistry–Climate Model Initiative (CCMI) ensemble to investigate Antarctic ozone depletion and subsequent recovery. The weighted mean projects an ozone recovery to 1980 levels, by 2056 with a 95 % confidence interval (2052–2060), 4 years earlier than the most recent study. Perfect-model testing and out-of-sample testing validate the results and show a greater projective skill than a standard multi-model mean. Interestingly, the construction of a weighted mean also provides insight into model performance and dependence between the models. This weighting methodology is robust to both model and metric choices and therefore has potential applications throughout the climate and chemistry–climate modelling communities.

Artificial injections of sulfur dioxide (SO2) into the stratosphere show in several model studies an impact on stratospheric dynamics. The quasi-biennial oscillation (QBO) has been shown to slow down or even vanish under higher SO2 injections in the equatorial region. But the impact is only qualitatively but not quantitatively consistent across the different studies using different numerical models. The aim of this study is to understand the reasons behind the differences in the QBO response to SO2 injections between two general circulation models, the Whole Atmosphere Community Climate Model (WACCM-110L) and MAECHAM5-HAM. We show that the response of the QBO to injections with the same SO2 injection rate is very different in the two models, but similar when a similar stratospheric heating rate is induced by SO2 injections of different amounts. The reason for the different response of the QBO corresponding to the same injection rate is very different vertical advection in the two models, even in the control simulation. The stronger vertical advection in WACCM results in a higher aerosol burden and stronger heating of the aerosols and, consequently, in a vanishing QBO at lower injection rate than in simulations with MAECHAM5-HAM. The vertical velocity increases slightly in MAECHAM5-HAM when increasing the horizontal resolution. This study highlights the crucial role of dynamical processes and helps to understand the large uncertainties in the response of different models to artificial SO2 injections in climate engineering studies.

A new set of stratospheric aerosol geoengineering (SAG) model experiments has been performed with Community Earth System Model version 2 (CESM2) with the Whole Atmosphere Community Climate Model (WACCM6) that are based on the Coupled Model Intercomparison Project phase 6 (CMIP6) overshoot scenario (SSP5-34-OS) as a baseline scenario to limit global warming to 1.5 or 2.0 ∘C above 1850–1900 conditions. The overshoot scenario allows us to applying a peak-shaving scenario that reduces the needed duration and amount of SAG application compared to a high forcing scenario. In addition, a feedback algorithm identifies the needed amount of sulfur dioxide injections in the stratosphere at four pre-defined latitudes, 30∘ N, 15∘ N, 15∘ S, and 30∘ S, to reach three surface temperature targets: global mean temperature, and interhemispheric and pole-to-Equator temperature gradients. These targets further help to reduce side effects, including overcooling in the tropics, warming of high latitudes, and large shifts in precipitation patterns. These experiments are therefore relevant for investigating the impacts on society and ecosystems. Comparisons to SAG simulations based on a high emission pathway baseline scenario (SSP5-85) are also performed to investigate the dependency of impacts using different injection amounts to offset surface warming by SAG. We find that changes from present-day conditions around 2020 in some variables depend strongly on the defined temperature target (1.5 ∘C vs. 2.0 ∘C). These include surface air temperature and related impacts, the Atlantic Meridional Overturning Circulation, which impacts ocean net primary productivity, and changes in ice sheet surface mass balance, which impacts sea level rise. Others, including global precipitation changes and the recovery of the Antarctic ozone hole, depend strongly on the amount of SAG application. Furthermore, land net primary productivity as well as ocean acidification depend mostly on the global atmospheric CO2 concentration and therefore the baseline scenario. Multi-model comparisons of experiments that include strong mitigation and carbon dioxide removal with some SAG application are proposed to assess the robustness of impacts on societies and ecosystems.

To mitigate the projected global warming in the 21st century, it is well-recognized that society needs to cut CO2 emissions and other short-lived warming agents aggressively. However, to stabilize the climate at a warming level closer to the present day, such as the “well below 2 ∘C” aspiration in the Paris Agreement, a net-zero carbon emission by 2050 is still insufficient. The recent IPCC special report calls for a massive scheme to extract CO2 directly from the atmosphere, in addition to decarbonization, to reach negative net emissions at the mid-century mark. Another ambitious proposal is solar-radiation-based geoengineering schemes, including injecting sulfur gas into the stratosphere. Despite being in public debate for years, these two leading geoengineering schemes have not been directly compared under a consistent analytical framework using global climate models. Here we present the first explicit analysis of the hydroclimate impacts of these two geoengineering approaches using two recently available large-ensemble (>10 members) model experiments conducted by a family of state-of-the-art Earth system models. The CO2-based mitigation simulation is designed to include both emission cuts and carbon capture. The solar-radiation-based mitigation simulation is designed to inject sulfur gas strategically at specified altitudes and latitudes and run a feedback control algorithm to avoid common problems previously identified such as the overcooling of the tropics and large-scale precipitation shifts. Our analysis focuses on the projected aridity conditions over the Americas in the 21st century in detailed terms of the potential mitigation benefits, the temporal evolution, the spatial distribution (within North and South America), the relative efficiency, and the physical mechanisms. We show that sulfur injection, in contrast to previous notions of leading to excessive terrestrial drying (in terms of precipitation reduction) while offsetting the global mean greenhouse gas (GHG) warming, will instead mitigate the projected drying tendency under RCP8.5. The surface energy balance change induced by sulfur injection, in addition to the well-known response in temperature and precipitation, plays a crucial role in determining the overall terrestrial hydroclimate response. However, when normalized by the same amount of avoided global warming in these simulations, sulfur injection is less effective in curbing the worsening trend of regional land aridity in the Americas under RCP8.5 when compared with carbon capture. Temporally, the climate benefit of sulfur injection will emerge more quickly, even when both schemes are hypothetically started in the same year of 2020. Spatially, both schemes are effective in curbing the drying trend over North America. However, for South America, the sulfur injection scheme is particularly more effective for the sub-Amazon region (southern Brazil), while the carbon capture scheme is more effective for the Amazon region. We conclude that despite the apparent limitations (such as an inability to address ocean acidification) and potential side effects (such as changes to the ozone layer), innovative means of sulfur injection should continue to be explored as a potential low-cost option in the climate solution toolbox, complementing other mitigation approaches such as emission cuts and carbon capture (Cao et al., 2017). Our results demonstrate the urgent need for multi-model comparison studies and detailed regional assessments in other parts of the world.

The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of non-refractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 µg sm−3). Lower concentrations (∼0.1–0.3 µg sm−3) are observed in the northern middle and high latitudes and very low concentrations ( µg sm−3) in the southern middle and high latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction and underestimate the secondary fraction. Measured OA in the remote free troposphere is highly oxygenated, with organic aerosol to organic carbon (OA ∕ OC) ratios of ∼2.2–2.8, and is 30 %–60 % more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model–measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA and a stronger production of secondary OA in global models needed to provide better agreement with observations.

The hydroxyl radical (OH) plays critical roles within the troposphere, such as determining the lifetime of methane (CH4), yet is challenging to model due to its fast cycling and dependence on a multitude of sources and sinks. As a result, the reasons for variations in OH and the resulting methane lifetime (τCH4), both between models and in time, are difficult to diagnose. We apply a neural network (NN) approach to address this issue within a group of models that participated in the Chemistry-Climate Model Initiative (CCMI). Analysis of the historical specified dynamics simulations performed for CCMI indicates that the primary drivers of τCH4 differences among 10 models are the flux of UV light to the troposphere (indicated by the photolysis frequency JO1D), the mixing ratio of tropospheric ozone (O3), the abundance of nitrogen oxides (NOx≡NO+NO2), and details of the various chemical mechanisms that drive OH. Water vapour, carbon monoxide (CO), the ratio of NO:NOx, and formaldehyde (HCHO) explain moderate differences in τCH4, while isoprene, methane, the photolysis frequency of NO2 by visible light (JNO2), overhead ozone column, and temperature account for little to no model variation in τCH4. We also apply the NNs to analysis of temporal trends in OH from 1980 to 2015. All models that participated in the specified dynamics historical simulation for CCMI demonstrate a decline in τCH4 during the analysed timeframe. The significant contributors to this trend, in order of importance, are tropospheric O3, JO1D, NOx, and H2O, with CO also causing substantial interannual variability in OH burden. Finally, the identified trends in τCH4 are compared to calculated trends in the tropospheric mean OH concentration from previous work, based on analysis of observations. The comparison reveals a robust result for the effect of rising water vapour on OH and τCH4, imparting an increasing and decreasing trend of about 0.5 % decade−1, respectively. The responses due to NOx, ozone column, and temperature are also in reasonably good agreement between the two studies.

Abstract The Community Earth System Model version 2 (CESM2) includes three main atmospheric configurations: the Community Atmosphere Model version 6 (CAM6) with simplified chemistry and a simplified organic aerosol (OA) scheme, CAM6 with comprehensive tropospheric and stratospheric chemistry representation (CAM6‐chem), and the Whole Atmosphere Community Climate Model version 6 (WACCM6). Both, CAM6‐chem and WACCM6 include a more comprehensive secondary organic aerosols (SOA) approach using the Volatility Basis Set (VBS) scheme and prognostic stratospheric aerosols. This paper describes the different OA schemes available in the different atmospheric configurations of CESM2 and discusses differences in aerosol burden and resulting climate forcings. Derived OA burden and trends differ due to differences in OA formation using the different approaches. Regional differences in Aerosol Optical Depth with larger values using the comprehensive approach occur over SOA source regions. Stronger increasing SOA trends between 1960 and 2015 in WACCM6 compared to CAM6 are due to increasing biogenic emissions aligned with increasing surface temperatures. Using the comprehensive SOA approach further leads to improved comparisons to aircraft observations and SOA formation of ≈143 Tg/yr. We further use WACCM6 to identify source contributions of OA from biogenic, fossil fuel, and biomass burning emissions, to quantify SOA amounts and trends from these sources. Increasing SOA trends between 1960 and 2015 are the result of increasing biogenic emissions aligned with increasing surface temperatures. Biogenic emissions are at least two thirds of the total SOA burden. In addition, SOA source contributions from fossil fuel emissions become more important, with largest values over Southeast Asia. The estimated total anthropogenic forcing of OA in WACCM6 for 1995–2010 conditions is −0.43 W/m2, mostly from the aerosol direct effect.

The modeling study presented here aims to estimate how uncertainties in global hydroxyl radical (OH) distributions, variability, and trends may contribute to resolving discrepancies between simulated and observed methane (CH4) changes since 2000. A multi-model ensemble of 14 OH fields was analyzed and aggregated into 64 scenarios to force the offline atmospheric chemistry transport model LMDz (Laboratoire de Meteorologie Dynamique) with a standard CH4 emission scenario over the period 2000–2016. The multi-model simulated global volume-weighted tropospheric mean OH concentration ([OH]) averaged over 2000–2010 ranges between 8.7×105 and 12.8×105 molec cm−3. The inter-model differences in tropospheric OH burden and vertical distributions are mainly determined by the differences in the nitrogen oxide (NO) distributions, while the spatial discrepancies between OH fields are mostly due to differences in natural emissions and volatile organic compound (VOC) chemistry. From 2000 to 2010, most simulated OH fields show an increase of 0.1–0.3×105 molec cm−3 in the tropospheric mean [OH], with year-to-year variations much smaller than during the historical period 1960–2000. Once ingested into the LMDz model, these OH changes translated into a 5 to 15 ppbv reduction in the CH4 mixing ratio in 2010, which represents 7 %–20 % of the model-simulated CH4 increase due to surface emissions. Between 2010 and 2016, the ensemble of simulations showed that OH changes could lead to a CH4 mixing ratio uncertainty of >±30 ppbv. Over the full 2000–2016 time period, using a common state-of-the-art but nonoptimized emission scenario, the impact of [OH] changes tested here can explain up to 54 % of the gap between model simulations and observations. This result emphasizes the importance of better representing OH abundance and variations in CH4 forward simulations and emission optimizations performed by atmospheric inversions.

Fluxes of halogenated volatile organic compounds (VOCs) over the Southern Ocean remain poorly understood, and few atmospheric measurements exist to constrain modeled emissions of these compounds. We present observations of CHBr3, CH2Br2, CH3I, CHClBr2, CHBrCl2, and CH3Br during the O2∕N2 Ratio and CO2 Airborne Southern Ocean (ORCAS) study and the second Atmospheric Tomography mission (ATom-2) in January and February of 2016 and 2017. Good model–measurement correlations were obtained between these observations and simulations from the Community Earth System Model (CESM) atmospheric component with chemistry (CAM-Chem) for CHBr3, CH2Br2, CH3I, and CHClBr2 but all showed significant differences in model : measurement ratios. The model : measurement comparison for CH3Br was satisfactory and for CHBrCl2 the low levels present precluded us from making a complete assessment. Thereafter, we demonstrate two novel approaches to estimate halogenated VOC fluxes; the first approach takes advantage of the robust relationships that were found between airborne observations of O2 and CHBr3, CH2Br2, and CHClBr2. We use these linear regressions with O2 and modeled O2 distributions to infer a biological flux of halogenated VOCs. The second approach uses the Stochastic Time-Inverted Lagrangian Transport (STILT) particle dispersion model to explore the relationships between observed mixing ratios and the product of the upstream surface influence of sea ice, chl a, absorption due to detritus, and downward shortwave radiation at the surface, which in turn relate to various regional hypothesized sources of halogenated VOCs such as marine phytoplankton, phytoplankton in sea-ice brines, and decomposing organic matter in surface seawater. These relationships can help evaluate the likelihood of particular halogenated VOC sources and in the case of statistically significant correlations, such as was found for CH3I, may be used to derive an estimated flux field. Our results are consistent with a biogenic regional source of CHBr3 and both nonbiological and biological sources of CH3I over these regions.

Local finite-amplitude wave activity (LWA) measures the waviness of the local flow. In this work we relate the anticyclonic part of LWA, AWA (anticyclonic wave activity), to surface ozone in summertime over the US on interannual to decadal timescales. Interannual covariance between AWA diagnosed from the European Centre for Medium-Range Weather Forecast Era-Interim reanalysis and ozone measured at EPA Clean Air Status and Trends Network (CASTNET) stations is analyzed using maximum covariance analysis (MCA). The first two modes in the MCA analysis explain 84 % of the covariance between the AWA and MDA8 (maximum daily 8 h average ozone), explaining 29 % and 14 % of the MDA8 ozone variance, respectively. Over most of the US we find a significant relationship between ozone at most locations and AWA over the analysis domain (24–53∘ N and 130–65∘ W) using a linear regression model. This relationship is diagnosed (i) using reanalysis meteorology and measured ozone from CASTNET, or (ii) using meteorology and ozone simulated by the Community Atmospheric Model version 4 with chemistry (CAM4-chem) within the Community Earth System Model (CESM1). Using the linear regression model we find that meteorological biases in AWA in CAM4-chem, as compared to the reanalysis meteorology, induce ozone changes between −4 and +8 ppb in CAM4-chem. Future changes (ca. 2100) in AWA are diagnosed in different climate change simulations in CAM4-chem, simulations which differ in their initial conditions and in one case differ in their reactive species emissions. All future simulations have enhanced AWA over the US, with the maximum enhancement in the southwest. As diagnosed using the linear regression model, the future change in AWA is predicted to cause a corresponding change in ozone ranging between −6 and 6 ppb. The location of this change depends on subtle features of the change in AWA. In a number of locations this change is consistent with the magnitude and the sign of the overall simulated future ozone change.