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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.

The Montreal Protocol and its amendments (MPA) have been a huge success in preserving the stratospheric ozone layer from being destroyed by unabated chlorofluorocarbon (CFC) emissions. The phaseout of CFCs has not only prevented serious impacts on our health and climate, but also avoided strong alterations of atmospheric circulation patterns. With the Earth system model SOCOLv4, we study the dynamical and climatic impacts of a scenario with unabated CFC emissions by 2100, disentangling radiative and chemical (ozone-mediated) effects of CFCs. In the stratosphere, chemical effects of CFCs (i.e., the resulting ozone loss) are the main drivers of circulation changes, weakening wintertime polar vortices and speeding up the Brewer–Dobson circulation. These dynamical impacts during wintertime are due to low-latitude ozone depletion and the resulting reduction in the Equator-to-pole temperature gradient. Westerly winds in the lower stratosphere strengthen, which is for the Southern Hemisphere (SH) similar to the effects of the Antarctic ozone hole over the second half of the 20th century. Furthermore, the winter and spring stratospheric wind variability increases in the SH, whereas it decreases in summer and fall. This seasonal variation in wind speed in the stratosphere has substantial implications for the major modes of variability in the tropospheric circulation in the scenario without the MPA (No-MPA). We find coherent changes in the troposphere, such as patterns that are reminiscent of negative Southern and Northern Annular modes (SAM and NAM) and North Atlantic Oscillation (NAO) anomalies during seasons with a weakened vortex (winter and spring); the opposite occurs during seasons with strengthened westerlies in the lower stratosphere and troposphere (summer). In the troposphere, radiative heating by CFCs prevails throughout the year, shifting the SAM into a positive phase and canceling out the ozone-induced effects on the NAO, whereas the North Pacific sector shows an increase in the meridional sea-level pressure gradient as both CFC heating and ozone-induced effects reinforce each other there. Furthermore, global warming is amplified by 1.7 K with regionally up to a 12 K increase over eastern Canada and the western Arctic. Our study sheds light on the adverse effects of a non-adherence to the MPA on the global atmospheric circulation, uncovering the roles of the underlying physical mechanisms. In so doing, our study emphasizes the importance of the MPA for Earth's climate to avoid regional amplifications of negative climate impacts.

In the Arctic stratosphere, the combination of chemical ozone depletion by halogenated ozone-depleting substances (hODSs) and dynamic fluctuations can lead to severe ozone minima. These Arctic ozone minima are of great societal concern due to their health and climate impacts. Owing to the success of the Montreal Protocol, hODSs in the stratosphere are gradually declining, resulting in a recovery of the ozone layer. On the other hand, continued greenhouse gas (GHG) emissions cool the stratosphere, possibly enhancing the formation of polar stratospheric clouds (PSCs) and, thus, enabling more efficient chemical ozone destruction. Other processes, such as the acceleration of the Brewer–Dobson circulation, also affect stratospheric temperatures, further complicating the picture. Therefore, it is currently unclear whether major Arctic ozone minima will still occur at the end of the 21st century despite decreasing hODSs. We have examined this question for different emission pathways using simulations conducted within the Chemistry-Climate Model Initiative (CCMI-1 and CCMI-2022) and found large differences in the models' ability to simulate the magnitude of ozone minima in the present-day climate. Models with a generally too-cold polar stratosphere (cold bias) produce pronounced ozone minima under present-day climate conditions because they simulate more PSCs and, thus, high concentrations of active chlorine species (ClOx). These models predict the largest decrease in ozone minima in the future. Conversely, models with a warm polar stratosphere (warm bias) have the smallest sensitivity of ozone minima to future changes in hODS and GHG concentrations. As a result, the scatter among models in terms of the magnitude of Arctic spring ozone minima will decrease in the future. Overall, these results suggest that Arctic ozone minima will become weaker over the next decades, largely due to the decline in hODS abundances. We note that none of the models analysed here project a notable increase of ozone minima in the future. Stratospheric cooling caused by increasing GHG concentrations is expected to play a secondary role as its effect in the Arctic stratosphere is weakened by opposing radiative and dynamical mechanisms.

It is now recognized and confirmed that the ozone layer shields the biosphere from dangerous solar UV radiation and is also important for the global atmosphere and climate. The observed massive ozone depletion forced the introduction of limitations on the production of halogen-containing ozone-depleting substances (hODSs) by the Montreal Protocol and its amendments and adjustments (MPA). Previous research has demonstrated the success of the Montreal Protocol and increased public awareness of its necessity. In this study, we evaluate the benefits of the Montreal Protocol on climate and ozone evolution using the Earth system model (ESM) SOCOLv4.0 (modeling tools for studies of SOlar Climate Ozone Links) which includes dynamic modules for the ocean, sea ice, interactive ozone, and stratospheric aerosol. Here, we analyze the results of the numerical experiments performed with and without limitations on the ozone-depleting substance (ODS) emissions. In the experiments, we have used CMIP6 (Coupled Model Intercomparison Project) SSP2-4.5 and SSP5-8.5 (Shared Socioeconomic Pathway) scenarios for future forcing behavior. We confirm previous results regarding catastrophic ozone layer depletion and substantial climate warming in the case without MPA limitations. We show that the climate effects of MPA consist of additional global-mean warming by up to 2.5 K in 2100 caused by the direct radiative effect of the hODSs, which is comparable to large climate warming obtained with the SSP5-8.5 scenario. For the first time, we reveal the dramatic effects of MPA on chemical species and cloud cover. The response of surface temperature, precipitation, and sea-ice fields was demonstrated for the first time with the model that has interactive tropospheric and stratospheric chemistry. We have found some differences in the climate response compared to the model with prescribed ozone, which should be further addressed. Our research updates and complements previous modeling studies on the quantifying of MPA benefits for the terrestrial atmosphere and climate.

This study evaluates the future evolution of atmospheric ozone simulated with the Earth system model (ESM) SOCOLv4. Simulations have been performed based on two potential shared socioeconomic pathways (SSPs): the middle-of-the-road (SSP2-4.5) and fossil-fueled (SSP5-8.5) scenarios. The future changes in ozone, as well as in chemical drivers (NOx and CO) and temperature, were estimated between 2015 and 2099 and for several intermediate subperiods (i.e., 2015–2039, 2040–2069, and 2070–2099) via dynamic linear modeling. In both scenarios, the model projects a decline in tropospheric ozone in the future that starts in the 2030s in SSP2-4.5 and after the 2060s in SSP5-8.5 due to a decrease in concentrations of NOx and CO. The results also suggest a very likely ozone increase in the mesosphere and the upper and middle stratosphere, as well as in the lower stratosphere at high latitudes. Under SSP5-8.5, the ozone increase in the stratosphere is higher because of stronger cooling (>1 K per decade) induced by greenhouse gases (GHGs), which slows the catalytic ozone destruction cycles. In contrast, in the tropical lower stratosphere, ozone concentrations decrease in both experiments and increase over the middle and high latitudes of both hemispheres due to the speeding up of the Brewer–Dobson circulation, which is stronger in SSP5-8.5. No evidence was found of a decline in ozone levels in the lower stratosphere at mid-latitudes. In both future scenarios, the total column ozone is expected to be distinctly higher than present in middle to high latitudes and might be lower in the tropics, which causes a decrease in the mid-latitudes and an increase in the tropics in the surface level of ultraviolet radiation. The results of SOCOLv4 suggest that the stratospheric-ozone evolution throughout the 21st century is strongly governed not only by a decline in halogen concentration but also by future GHG forcing. In addition, the tropospheric-ozone column changes, which are mainly due to the changes in anthropogenic emissions of ozone precursors, also have a strong impact on the total column. Therefore, even though the anthropogenic halogen-loading problem has been brought under control to date, the sign of future ozone column changes, globally and regionally, is still unclear and largely depends on diverse future human activities. The results of this work are, thus, relevant for developing future strategies for socioeconomic pathways.

A previous model intercomparison of the Tambora aerosol cloud has highlighted substantial differences among simulated volcanic aerosol properties in the pre-industrial stratosphere and has led to questions about the applicability of global aerosol models for large-magnitude explosive eruptions prior to the observational period. Here, we compare the evolution of the stratospheric aerosol cloud following the well-observed June 1991 Mt. Pinatubo eruption simulated with six interactive stratospheric aerosol microphysics models to a range of observational data sets. Our primary focus is on the uncertainties regarding initial SO2 emission following the Pinatubo eruption, as prescribed in the Historical Eruptions SO2 Emission Assessment experiments (HErSEA), in the framework of the Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP). Six global models with interactive aerosol microphysics took part in this study: ECHAM6-SALSA, EMAC, ECHAM5-HAM, SOCOL-AERv2, ULAQ-CCM, and UM-UKCA. Model simulations are performed by varying the SO2 injection amount (ranging between 5 and 10 Tg S) and the altitude of injection (between 18–25 km). The comparisons show that all models consistently demonstrate faster reduction from the peak in sulfate mass burden in the tropical stratosphere. Most models also show a stronger transport towards the extratropics in the Northern Hemisphere, at the expense of the observed tropical confinement, suggesting a much weaker subtropical barrier in all the models, which results in a shorter e-folding time compared to the observations. Furthermore, simulations in which more than 5 Tg S in the form of SO2 is injected show an initial overestimation of the sulfate burden in the tropics and, in some models, in the Northern Hemisphere and a large surface area density a few months after the eruption compared to the values measured in the tropics and the in situ measurements over Laramie. This draws attention to the importance of including processes such as the ash injection for the removal of the initial SO2 and aerosol lofting through local heating.

There is evidence that the ozone layer has begun to recover owing to the ban on the production of halogenated ozone-depleting substances (hODS) accomplished by the Montreal Protocol and its amendments and adjustments (MPA). However, recent studies, while reporting an increase in tropospheric ozone from the anthropogenic NOx and CH4 and confirming the ozone recovery in the upper stratosphere from the effects of hODS, also indicate a continuing decline in the lower tropical and mid-latitudinal stratospheric ozone. While these are indications derived from observations, they are not reproduced by current global chemistry–climate models (CCMs), which show positive or near-zero trends for ozone in the lower stratosphere. This makes it difficult to robustly establish ozone evolution and has sparked debate about the ability of contemporary CCMs to simulate future ozone trends. We applied the new Earth system model (ESM) SOCOLv4 (SOlar Climate Ozone Links, version 4) to calculate long-term ozone trends between 1985–2018 and compare them with trends derived from the BAyeSian Integrated and Consolidated (BASIC) ozone composite and MERRA-2, ERA-5, and MSRv2 reanalyses. We designed the model experiment with a six-member ensemble to account for the uncertainty of the natural variability. The trend analysis is performed separately for the ozone depletion (1985–1997) and ozone recovery (1998–2018) phases of the ozone evolution. Within the 1998–2018 period, SOCOLv4 shows statistically significant positive ozone trends in the mesosphere, upper and middle stratosphere, and a steady increase in the tropospheric ozone. The SOCOLv4 results also suggest slightly negative trends in the extra-polar lower stratosphere, yet they barely agree with the BASIC ozone composite in terms of magnitude and statistical significance. However, in some realizations of the SOCOLv4 experiment, the pattern of ozone trends in the lower stratosphere resembles much of what is observed, suggesting that SOCOLv4 may be able to reproduce the observed trends in this region. Thus, the model results reveal marginally significant negative ozone changes in parts of the low-latitude lower stratosphere, which agrees in general with the negative tendencies extracted from the satellite data composite. Despite the slightly smaller significance and magnitude of the simulated ensemble mean, we confirm that modern CCMs such as SOCOLv4 are generally capable of simulating the observed ozone changes, justifying their use to project the future evolution of the ozone layer.

Energetic particle precipitation leads to ionization in the Earth's atmosphere, initiating the formation of active chemical species which destroy ozone and have the potential to impact atmospheric composition and dynamics down to the troposphere. We report on one exceptionally strong high-energy electron precipitation event detected by balloon measurements in geomagnetic midlatitudes on 14 December 2009, with ionization rates locally comparable to strong solar proton events. This electron precipitation was possibly caused by wave–particle interactions in the slot region between the inner and outer radiation belts, connected with still poorly understood natural phenomena in the magnetosphere. Satellite observations of odd nitrogen and nitric acid are consistent with widespread electron precipitation into magnetic midlatitudes. Simulations with a 3D chemistry–climate model indicate the almost complete destruction of ozone in the upper mesosphere over the region where high-energy electron precipitation occurred. Such an extraordinary type of energetic particle precipitation can have major implications for the atmosphere, and their frequency and strength should be carefully studied.

The short-living cosmogenic isotope 7Be, which is produced by cosmic rays in the atmosphere, is often used as a tracer for atmospheric dynamics, with precise and high-resolution measurements covering the recent decades. The long-living isotope 10Be, as measured in polar ice cores with an annual resolution, is a proxy for long-term cosmic-ray variability, whose signal can, however, be distorted by atmospheric transport and deposition that need to be properly modeled to be accounted for. While transport of 7Be can be modeled with high accuracy using the known meteorological fields, atmospheric transport of 10Be was typically modeled using case-study-specific simulations or simplified box models based on parameterizations. Thus, there is a need for a realistic model able to simulate atmospheric transport and deposition of beryllium with a focus on polar regions and (inter)annual timescales that is potentially able to operate in a self-consistent mode without the prescribed meteorology. Since measurements of 10Be are extremely laborious and hence scarce, it is difficult to compare model results directly with measurement data. On the other hand, the two beryllium isotopes are believed to have similar transport and deposition properties, being different only in production and lifetime, and thus the results of 7Be transport can be generally applied to 10Be. Here we present a new model, called CCM SOCOL-AERv2-BE, to trace isotopes of 7Be and 10Be in the atmosphere based on the chemistry–climate model (CCM) SOCOL (SOlar Climate Ozone Links), which has been improved by including modules for the production, deposition, and transport of 7Be and 10Be. Production of the isotopes was modeled for both galactic and solar cosmic rays by applying the CRAC (Cosmic Ray Atmospheric Cascade) model. Transport of 7Be was modeled without additional gravitational settling due to the submicron size of the background aerosol particles. An interactive deposition scheme was applied including both wet and dry deposition. Modeling was performed using a full nudging to the meteorological fields for the period of 2002–2008 with a spin-up period of 1996–2001. The modeled concentrations of 7Be in near-ground air were compared with the measured ones at a weekly time resolution in four nearly antipodal high-latitude locations: two in the Northern (Finland and Canada) and two in the Southern (Chile and the Kerguelen Islands) Hemisphere. The model results agree with the measurements in the absolute level within error bars, implying that the production, decay, and lateral deposition are correctly reproduced. The model also correctly reproduces the temporal variability of 7Be concentrations on annual and sub-annual scales, including the presence and absence of the annual cycle in the Northern and Southern Hemisphere, respectively. We also modeled the production and transport of 7Be for a major solar energetic particle event (SPE) on 20 January 2005, which appears insufficient to produce a measurable signal but may serve as a reference event for historically known extreme SPEs. Thus, a new full 3D time-dependent model, based on CCM SOCOL, of 7Be and 10Be atmospheric production, transport, and deposition has been developed. Comparison with real data on the 7Be concentration in the near-ground air validates the model and its accuracy.

In this paper, we present a new version of the chemistry–climate model SOCOL-AERv2 supplemented by an iodine chemistry module. We perform three 20-year ensemble experiments to assess the validity of the modeled iodine and to quantify the effects of iodine on ozone. The iodine distributions obtained with SOCOL-AERv2-I agree well with AMAX-DOAS observations and with CAM-chem model simulations. For the present-day atmosphere, the model suggests that the iodine-induced chemistry leads to a 3 %–4 % reduction in the ozone column, which is greatest at high latitudes. The model indicates the strongest influence of iodine in the lower stratosphere with 30 ppbv less ozone at low latitudes and up to 100 ppbv less at high latitudes. In the troposphere, the account of the iodine chemistry reduces the tropospheric ozone concentration by 5 %–10 % depending on geographical location. In the lower troposphere, 75 % of the modeled ozone reduction originates from inorganic sources of iodine, 25 % from organic sources of iodine. At 50 hPa, the results show that the impacts of iodine from both sources are comparable. Finally, we determine the sensitivity of ozone to iodine by applying a 2-fold increase in iodine emissions, as it might be representative for iodine by the end of this century. This reduces the ozone column globally by an additional 1.5 %–2.5 %. Our results demonstrate the sensitivity of atmospheric ozone to iodine chemistry for present and future conditions, but uncertainties remain high due to the paucity of observational data of iodine species.

This paper features the new atmosphere–ocean–aerosol–chemistry–climate model, SOlar Climate Ozone Links (SOCOL) v4.0, and its validation. The new model was built by interactively coupling the Max Planck Institute Earth System Model version 1.2 (MPI-ESM1.2) (T63, L47) with the chemistry (99 species) and size-resolving (40 bins) sulfate aerosol microphysics modules from the aerosol–chemistry–climate model, SOCOL-AERv2. We evaluate its performance against reanalysis products and observations of atmospheric circulation, temperature, and trace gas distribution, with a focus on stratospheric processes. We show that SOCOLv4.0 captures the low- and midlatitude stratospheric ozone well in terms of the climatological state, variability and evolution. The model provides an accurate representation of climate change, showing a global surface warming trend consistent with observations as well as realistic cooling in the stratosphere caused by greenhouse gas emissions, although, as in previous model versions, a too-fast residual circulation and exaggerated mixing in the surf zone are still present. The stratospheric sulfur budget for moderate volcanic activity is well represented by the model, albeit with slightly underestimated aerosol lifetime after major eruptions. The presence of the interactive ocean and a successful representation of recent climate and ozone layer trends make SOCOLv4.0 ideal for studies devoted to future ozone evolution and effects of greenhouse gases and ozone-destroying substances, as well as the evaluation of potential solar geoengineering measures through sulfur injections. Potential further model improvements could be to increase the vertical resolution, which is expected to allow better meridional transport in the stratosphere, as well as to update the photolysis calculation module and budget of mesospheric odd nitrogen. In summary, this paper demonstrates that SOCOLv4.0 is well suited for applications related to the stratospheric ozone and sulfate aerosol evolution, including its participation in ongoing and future model intercomparison projects.

As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), several climate modeling centers performed a coordinated pre-study experiment with interactive stratospheric aerosol models simulating the volcanic aerosol cloud from an eruption resembling the 1815 Mt. Tambora eruption (VolMIP-Tambora ISA ensemble). The pre-study provided the ancillary ability to assess intermodel diversity in the radiative forcing for a large stratospheric-injecting equatorial eruption when the volcanic aerosol cloud is simulated interactively. An initial analysis of the VolMIP-Tambora ISA ensemble showed large disparities between models in the stratospheric global mean aerosol optical depth (AOD). In this study, we now show that stratospheric global mean AOD differences among the participating models are primarily due to differences in aerosol size, which we track here by effective radius. We identify specific physical and chemical processes that are missing in some models and/or parameterized differently between models, which are together causing the differences in effective radius. In particular, our analysis indicates that interactively tracking hydroxyl radical (OH) chemistry following a large volcanic injection of sulfur dioxide (SO2) is an important factor in allowing for the timescale for sulfate formation to be properly simulated. In addition, depending on the timescale of sulfate formation, there can be a large difference in effective radius and subsequently AOD that results from whether the SO2 is injected in a single model grid cell near the location of the volcanic eruption, or whether it is injected as a longitudinally averaged band around the Earth.

Water vapor (H2O) is the source of reactive hydrogen radicals in the middle atmosphere, whereas carbon monoxide (CO), being formed by CO2 photolysis, is suitable as a dynamical tracer. In the mesosphere, both H2O and CO are sensitive to solar irradiance (SI) variability because of their destruction/production by solar radiation. This enables us to analyze the solar signal in both models and observed data. Here, we evaluate the mesospheric H2O and CO response to solar irradiance variability using the Chemistry-Climate Model Initiative (CCMI-1) simulations and satellite observations. We analyzed the results of four CCMI models (CMAM, EMAC-L90MA, SOCOLv3, and CESM1-WACCM 3.5) operated in CCMI reference simulation REF-C1SD in specified dynamics mode, covering the period from 1984–2017. Multiple linear regression analyses show a pronounced and statistically robust response of H2O and CO to solar irradiance variability and to the annual and semiannual cycles. For periods with available satellite data, we compared the simulated solar signal against satellite observations, namely the GOZCARDS composite for 1992–2017 for H2O and Aura/MLS measurements for 2005–2017 for CO. The model results generally agree with observations and reproduce an expected negative and positive correlation for H2O and CO, respectively, with solar irradiance. However, the magnitude of the response and patterns of the solar signal varies among the considered models, indicating differences in the applied chemical reaction and dynamical schemes, including the representation of photolyzes. We suggest that there is no dominating thermospheric influence of solar irradiance in CO, as reported in previous studies, because the response to solar variability is comparable with observations in both low-top and high-top models. We stress the importance of this work for improving our understanding of the current ability and limitations of state-of-the-art models to simulate a solar signal in the chemistry and dynamics of the middle atmosphere.

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.

The top-of-atmosphere (TOA) outgoing longwave flux over the 9.6 µm ozone band is a fundamental quantity for understanding chemistry–climate coupling. However, observed TOA fluxes are hard to estimate as they exhibit considerable variability in space and time that depend on the distributions of clouds, ozone (O3), water vapor (H2O), air temperature (Ta), and surface temperature (Ts). Benchmarking present-day fluxes and quantifying the relative influence of their drivers is the first step for estimating climate feedbacks from ozone radiative forcing and predicting radiative forcing evolution. To that end, we constructed observational instantaneous radiative kernels (IRKs) under clear-sky conditions, representing the sensitivities of the TOA flux in the 9.6 µm ozone band to the vertical distribution of geophysical variables, including O3, H2O, Ta, and Ts based upon the Aura Tropospheric Emission Spectrometer (TES) measurements. Applying these kernels to present-day simulations from the Chemistry-Climate Model Initiative (CCMI) project as compared to a 2006 reanalysis assimilating satellite observations, we show that the models have large differences in TOA flux, attributable to different geophysical variables. In particular, model simulations continue to diverge from observations in the tropics, as reported in previous studies of the Atmospheric Chemistry Climate Model Intercomparison Project (ACCMIP) simulations. The principal culprits are tropical middle and upper tropospheric ozone followed by tropical lower tropospheric H2O. Five models out of the eight studied here have TOA flux biases exceeding 100 mW m−2 attributable to tropospheric ozone bias. Another set of five models have flux biases over 50 mW m−2 due to H2O. On the other hand, Ta radiative bias is negligible in all models (no more than 30 mW m−2). We found that the atmospheric component (AM3) of the Geophysical Fluid Dynamics Laboratory (GFDL) general circulation model and Canadian Middle Atmosphere Model (CMAM) have the lowest TOA flux biases globally but are a result of cancellation of opposite biases due to different processes. Overall, the multi-model ensemble mean bias is -133±98 mW m−2, indicating that they are too atmospherically opaque due to trapping too much radiation in the atmosphere by overestimated tropical tropospheric O3 and H2O. Having too much O3 and H2O in the troposphere would have different impacts on the sensitivity of TOA flux to O3 and these competing effects add more uncertainties on the ozone radiative forcing. We find that the inter-model TOA outgoing longwave radiation (OLR) difference is well anti-correlated with their ozone band flux bias. This suggests that there is significant radiative compensation in the calculation of model outgoing longwave radiation.

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.

We perform the first multi-model intercomparison of the impact of nudged meteorology on the stratospheric residual circulation using hindcast simulations from the Chemistry–Climate Model Initiative (CCMI). We examine simulations over the period 1980–2009 from seven models in which the meteorological fields are nudged towards a reanalysis dataset and compare these with their equivalent free-running simulations and the reanalyses themselves. We show that for the current implementations, nudging meteorology does not constrain the mean strength of the stratospheric residual circulation and that the inter-model spread is similar, or even larger, than in the free-running simulations. The nudged models generally show slightly stronger upwelling in the tropical lower stratosphere compared to the free-running versions and exhibit marked differences compared to the directly estimated residual circulation from the reanalysis dataset they are nudged towards. Downward control calculations applied to the nudged simulations reveal substantial differences between the climatological lower-stratospheric tropical upward mass flux (TUMF) computed from the modelled wave forcing and that calculated directly from the residual circulation. This explicitly shows that nudging decouples the wave forcing and the residual circulation so that the divergence of the angular momentum flux due to the mean motion is not balanced by eddy motions, as would typically be expected in the time mean. Overall, nudging meteorological fields leads to increased inter-model spread for most of the measures of the mean climatological stratospheric residual circulation assessed in this study. In contrast, the nudged simulations show a high degree of consistency in the inter-annual variability in the TUMF in the lower stratosphere, which is primarily related to the contribution to variability from the resolved wave forcing. The more consistent inter-annual variability in TUMF in the nudged models also compares more closely with the variability found in the reanalyses, particularly in boreal winter. We apply a multiple linear regression (MLR) model to separate the drivers of inter-annual and long-term variations in the simulated TUMF; this explains up to ∼75 % of the variance in TUMF in the nudged simulations. The MLR model reveals a statistically significant positive trend in TUMF for most models over the period 1980–2009. The TUMF trend magnitude is generally larger in the nudged models compared to their free-running counterparts, but the intermodel range of trends doubles from around a factor of 2 to a factor of 4 due to nudging. Furthermore, the nudged models generally do not match the TUMF trends in the reanalysis they are nudged towards for trends over different periods in the interval 1980–2009. Hence, we conclude that nudging does not strongly constrain long-term trends simulated by the chemistry–climate model (CCM) in the residual circulation. Our findings show that while nudged simulations may, by construction, produce accurate temperatures and realistic representations of fast horizontal transport, this is not typically the case for the slower zonal mean vertical transport in the stratosphere. Consequently, caution is required when using nudged simulations to interpret the behaviour of stratospheric tracers that are affected by the residual circulation.

SOCOL-AERv1 was developed as an aerosol–chemistry–climate model to study the stratospheric sulfur cycle and its influence on climate and the ozone layer. It includes a sectional aerosol model that tracks the sulfate particle size distribution in 40 size bins, between 0.39 nm and 3.2 µm. Sheng et al. (2015) showed that SOCOL-AERv1 successfully matched observable quantities related to stratospheric aerosol. In the meantime, SOCOL-AER has undergone significant improvements and more observational datasets have become available. In producing SOCOL-AERv2 we have implemented several updates to the model: adding interactive deposition schemes, improving the sulfate mass and particle number conservation, and expanding the tropospheric chemistry scheme. We compare the two versions of the model with background stratospheric sulfate aerosol observations, stratospheric aerosol evolution after Pinatubo, and ground-based sulfur deposition networks. SOCOL-AERv2 shows similar levels of agreement as SOCOL-AERv1 with satellite-measured extinctions and in situ optical particle counter (OPC) balloon flights. The volcanically quiescent total stratospheric aerosol burden simulated in SOCOL-AERv2 has increased from 109 Gg of sulfur (S) to 160 Gg S, matching the newly available satellite estimate of 165 Gg S. However, SOCOL-AERv2 simulates too high cross-tropopause transport of tropospheric SO2 and/or sulfate aerosol, leading to an overestimation of lower stratospheric aerosol. Due to the current lack of upper tropospheric SO2 measurements and the neglect of organic aerosol in the model, the lower stratospheric bias of SOCOL-AERv2 was not further improved. Model performance under volcanically perturbed conditions has also undergone some changes, resulting in a slightly shorter volcanic aerosol lifetime after the Pinatubo eruption. With the improved deposition schemes of SOCOL-AERv2, simulated sulfur wet deposition fluxes are within a factor of 2 of measured deposition fluxes at 78 % of the measurement stations globally, an agreement which is on par with previous model intercomparison studies. Because of these improvements, SOCOL-AERv2 will be better suited to studying changes in atmospheric sulfur deposition due to variations in climate and emissions.

We have derived values of the ultraviolet index (UVI) at solar noon using the Tropospheric Ultraviolet Model (TUV) driven by ozone, temperature and aerosol fields from climate simulations of the first phase of the Chemistry-Climate Model Initiative (CCMI-1). Since clouds remain one of the largest uncertainties in climate projections, we simulated only the clear-sky UVI. We compared the modelled UVI climatologies against present-day climatological values of UVI derived from both satellite data (the OMI-Aura OMUVBd product) and ground-based measurements (from the NDACC network). Depending on the region, relative differences between the UVI obtained from CCMI/TUV calculations and the ground-based measurements ranged between −5.9 % and 10.6 %. We then calculated the UVI evolution throughout the 21st century for the four Representative Concentration Pathways (RCPs 2.6, 4.5, 6.0 and 8.5). Compared to 1960s values, we found an average increase in the UVI in 2100 (of 2 %–4 %) in the tropical belt (30∘ N–30∘ S). For the mid-latitudes, we observed a 1.8 % to 3.4 % increase in the Southern Hemisphere for RCPs 2.6, 4.5 and 6.0 and found a 2.3 % decrease in RCP 8.5. Higher increases in UVI are projected in the Northern Hemisphere except for RCP 8.5. At high latitudes, ozone recovery is well identified and induces a complete return of mean UVI levels to 1960 values for RCP 8.5 in the Southern Hemisphere. In the Northern Hemisphere, UVI levels in 2100 are higher by 0.5 % to 5.5 % for RCPs 2.6, 4.5 and 6.0 and they are lower by 7.9 % for RCP 8.5. We analysed the impacts of greenhouse gases (GHGs) and ozone-depleting substances (ODSs) on UVI from 1960 by comparing CCMI sensitivity simulations (1960–2100) with fixed GHGs or ODSs at their respective 1960 levels. As expected with ODS fixed at their 1960 levels, there is no large decrease in ozone levels and consequently no sudden increase in UVI levels. With fixed GHG, we observed a delayed return of ozone to 1960 values, with a corresponding pattern of change observed on UVI, and looking at the UVI difference between 2090s values and 1960s values, we found an 8 % increase in the tropical belt during the summer of each hemisphere. Finally we show that, while in the Southern Hemisphere the UVI is mainly driven by total ozone column, in the Northern Hemisphere both total ozone column and aerosol optical depth drive UVI levels, with aerosol optical depth having twice as much influence on the UVI as total ozone column does.

Energetic particle precipitation (EPP) affects the chemistry of the polar middle atmosphere by producing reactive nitrogen (NOy) and hydrogen (HOx) species, which then catalytically destroy ozone. Recently, there have been major advances in constraining these particle impacts through a parametrization of NOy based on high-quality observations. Here we investigate the effects of low (auroral) and middle (radiation belt) energy range electrons, separately and in combination, on reactive nitrogen and hydrogen species as well as on ozone during Southern Hemisphere winters from 2002 to 2010 using the SOCOL3-MPIOM chemistry-climate model. Our results show that, in the absence of solar proton events, low-energy electrons produce the majority of NOy in the polar mesosphere and stratosphere. In the polar vortex, NOy subsides and affects ozone at lower altitudes, down to 10 hPa. Comparing a year with high electron precipitation with a quiescent period, we found large ozone depletion in the mesosphere; as the anomaly propagates downward, 15 % less ozone is found in the stratosphere during winter, which is confirmed by satellite observations. Only with both low- and middle-energy electrons does our model reproduce the observed stratospheric ozone anomaly.

Climate models consistently predict an acceleration of the Brewer–Dobson circulation (BDC) due to climate change in the 21st century. However, the strength of this acceleration varies considerably among individual models, which constitutes a notable source of uncertainty for future climate projections. To shed more light upon the magnitude of this uncertainty and on its causes, we analyse the stratospheric mean age of air (AoA) of 10 climate projection simulations from the Chemistry-Climate Model Initiative phase 1 (CCMI-I), covering the period between 1960 and 2100. In agreement with previous multi-model studies, we find a large model spread in the magnitude of the AoA trend over the simulation period. Differences between future and past AoA are found to be predominantly due to differences in mixing (reduced aging by mixing and recirculation) rather than differences in residual mean transport. We furthermore analyse the mixing efficiency, a measure of the relative strength of mixing for given residual mean transport, which was previously hypothesised to be a model constant. Here, the mixing efficiency is found to vary not only across models, but also over time in all models. Changes in mixing efficiency are shown to be closely related to changes in AoA and quantified to roughly contribute 10 % to the long-term AoA decrease over the 21st century. Additionally, mixing efficiency variations are shown to considerably enhance model spread in AoA changes. To understand these mixing efficiency variations, we also present a consistent dynamical framework based on diffusive closure, which highlights the role of basic state potential vorticity gradients in controlling mixing efficiency and therefore aging by mixing.

Previous multi-model intercomparisons have shown that chemistry–climate models exhibit significant biases in tropospheric ozone compared with observations. We investigate annual-mean tropospheric column ozone in 15 models participating in the SPARC–IGAC (Stratosphere–troposphere Processes And their Role in Climate–International Global Atmospheric Chemistry) Chemistry-Climate Model Initiative (CCMI). These models exhibit a positive bias, on average, of up to 40 %–50 % in the Northern Hemisphere compared with observations derived from the Ozone Monitoring Instrument and Microwave Limb Sounder (OMI/MLS), and a negative bias of up to ∼ 30 % in the Southern Hemisphere. SOCOLv3.0 (version 3 of the Solar-Climate Ozone Links CCM), which participated in CCMI, simulates global-mean tropospheric ozone columns of 40.2 DU – approximately 33 % larger than the CCMI multi-model mean. Here we introduce an updated version of SOCOLv3.0, SOCOLv3.1, which includes an improved treatment of ozone sink processes, and results in a reduction in the tropospheric column ozone bias of up to 8 DU, mostly due to the inclusion of N2O5 hydrolysis on tropospheric aerosols. As a result of these developments, tropospheric column ozone amounts simulated by SOCOLv3.1 are comparable with several other CCMI models. We apply Gaussian process emulation and sensitivity analysis to understand the remaining ozone bias in SOCOLv3.1. This shows that ozone precursors (nitrogen oxides (NOx), carbon monoxide, methane and other volatile organic compounds, VOCs) are responsible for more than 90 % of the variance in tropospheric ozone. However, it may not be the emissions inventories themselves that result in the bias, but how the emissions are handled in SOCOLv3.1, and we discuss this in the wider context of the other CCMI models. Given that the emissions data set to be used for phase 6 of the Coupled Model Intercomparison Project includes approximately 20 % more NOx than the data set used for CCMI, further work is urgently needed to address the challenges of simulating sub-grid processes of importance to tropospheric ozone in the current generation of chemistry–climate models.

The impact of changes in incoming solar irradiance on stratospheric ozone abundances should be included in climate simulations to aid in capturing the atmospheric response to solar cycle variability. This study presents the first systematic comparison of the representation of the 11-year solar cycle ozone response (SOR) in chemistry–climate models (CCMs) and in pre-calculated ozone databases specified in climate models that do not include chemistry, with a special focus on comparing the recommended protocols for the Coupled Model Intercomparison Project Phase 5 and Phase 6 (CMIP5 and CMIP6). We analyse the SOR in eight CCMs from the Chemistry–Climate Model Initiative (CCMI-1) and compare these with results from three ozone databases for climate models: the Bodeker Scientific ozone database, the SPARC/Atmospheric Chemistry and Climate (AC&C) ozone database for CMIP5 and the SPARC/CCMI ozone database for CMIP6. The peak amplitude of the annual mean SOR in the tropical upper stratosphere (1–5 hPa) decreases by more than a factor of 2, from around 5 to 2 %, between the CMIP5 and CMIP6 ozone databases. This substantial decrease can be traced to the CMIP5 ozone database being constructed from a regression model fit to satellite and ozonesonde measurements, while the CMIP6 database is constructed from CCM simulations. The SOR in the CMIP6 ozone database therefore implicitly resembles the SOR in the CCMI-1 models. The structure in latitude of the SOR in the CMIP6 ozone database and CCMI-1 models is considerably smoother than in the CMIP5 database, which shows unrealistic sharp gradients in the SOR across the middle latitudes owing to the paucity of long-term ozone measurements in polar regions. The SORs in the CMIP6 ozone database and the CCMI-1 models show a seasonal dependence with enhanced meridional gradients at mid- to high latitudes in the winter hemisphere. The CMIP5 ozone database does not account for seasonal variations in the SOR, which is unrealistic. Sensitivity experiments with a global atmospheric model without chemistry (ECHAM6.3) are performed to assess the atmospheric impacts of changes in the representation of the SOR and solar spectral irradiance (SSI) forcing between CMIP5 and CMIP6. The larger amplitude of the SOR in the CMIP5 ozone database compared to CMIP6 causes a likely overestimation of the modelled tropical stratospheric temperature response between 11-year solar cycle minimum and maximum by up to 0.55 K, or around 80 % of the total amplitude. This effect is substantially larger than the change in temperature response due to differences in SSI forcing between CMIP5 and CMIP6. The results emphasize the importance of adequately representing the SOR in global models to capture the impact of the 11-year solar cycle on the atmosphere. Since a number of limitations in the representation of the SOR in the CMIP5 ozone database have been identified, we recommend that CMIP6 models without chemistry use the CMIP6 ozone database and the CMIP6 SSI dataset to better capture the climate impacts of solar variability. The SOR coefficients from the CMIP6 ozone database are published with this paper.

Major mid-winter stratospheric sudden warmings (SSWs) are the largest instance of wintertime variability in the Arctic stratosphere. Because SSWs are able to cause significant surface weather anomalies on intra-seasonal timescales, several previous studies have focused on their potential future change, as might be induced by anthropogenic forcings. However, a wide range of results have been reported, from a future increase in the frequency of SSWs to an actual decrease. Several factors might explain these contradictory results, notably the use of different metrics for the identification of SSWs and the impact of large climatological biases in single-model studies. To bring some clarity, we here revisit the question of future SSW changes, using an identical set of metrics applied consistently across 12 different models participating in the Chemistry–Climate Model Initiative. Our analysis reveals that no statistically significant change in the frequency of SSWs will occur over the 21st century, irrespective of the metric used for the identification of the event. Changes in other SSW characteristics – such as their duration, deceleration of the polar night jet, and the tropospheric forcing – are also assessed: again, we find no evidence of future changes over the 21st century.

We evaluate how the coupled aerosol–chemistry–climate model SOCOL-AERv1.0 represents the influence of the 1991 eruption of Mt. Pinatubo on stratospheric aerosol properties and atmospheric state. The aerosol module is coupled to the radiative and chemical modules and includes comprehensive sulfur chemistry and microphysics, in which the particle size distribution is represented by 40 size bins with radii spanning from 0.39 nm to 3.2 µm. SOCOL-AER simulations are compared with satellite and in situ measurements of aerosol parameters, temperature reanalyses, and ozone observations. In addition to the reference model configuration, we performed series of sensitivity experiments looking at different processes affecting the aerosol layer. An accurate sedimentation scheme is found to be essential to prevent particles from diffusing too rapidly to high and low altitudes. The aerosol radiative feedback and the use of a nudged quasi-biennial oscillation help to keep aerosol in the tropics and significantly affect the evolution of the stratospheric aerosol burden, which improves the agreement with observed aerosol mass distributions. The inclusion of van der Waals forces in the particle coagulation scheme suggests improvements in particle effective radius, although other parameters (such as aerosol longevity) deteriorate. Modification of the Pinatubo sulfur emission rate also improves some aerosol parameters, while it worsens others compared to observations. Observations themselves are highly uncertain and render it difficult to conclusively judge the necessity of further model reconfiguration. The model revealed problems in reproducing aerosol sizes above 25 km and also in capturing certain features of the ozone response. Besides this, our results show that SOCOL-AER is capable of predicting the most important global-scale atmospheric effects following volcanic eruptions, which is also a prerequisite for an improved understanding of solar geoengineering effects from sulfur injections to the stratosphere.

>We analyse simulations performed for the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion caused by anthropogenic stratospheric chlorine and bromine. We consider a total of 155 simulations from 20 models, including a range of sensitivity studies which examine the impact of climate change on ozone recovery. For the control simulations (unconstrained by nudging towards analysed meteorology) there is a large spread (±20 DU in the global average) in the predictions of the absolute ozone column. Therefore, the model results need to be adjusted for biases against historical data. Also, the interannual variability in the model results need to be smoothed in order to provide a reasonably narrow estimate of the range of ozone return dates. Consistent with previous studies, but here for a Representative Concentration Pathway (RCP) of 6.0, these new CCMI simulations project that global total column ozone will return to 1980 values in 2049 (with a 1σ uncertainty of 2043–2055). At Southern Hemisphere mid-latitudes column ozone is projected to return to 1980 values in 2045 (2039–2050), and at Northern Hemisphere mid-latitudes in 2032 (2020–2044). In the polar regions, the return dates are 2060 (2055–2066) in the Antarctic in October and 2034 (2025–2043) in the Arctic in March. The earlier return dates in the Northern Hemisphere reflect the larger sensitivity to dynamical changes. Our estimates of return dates are later than those presented in the 2014 Ozone Assessment by approximately 5–17 years, depending on the region, with the previous best estimates often falling outside of our uncertainty range. In the tropics only around half the models predict a return of ozone to 1980 values, around 2040, while the other half do not reach the 1980 value. All models show a negative trend in tropical total column ozone towards the end of the 21st century. The CCMI models generally agree in their simulation of the time evolution of stratospheric chlorine and bromine, which are the main drivers of ozone loss and recovery. However, there are a few outliers which show that the multi-model mean results for ozone recovery are not as tightly constrained as possible. Throughout the stratosphere the spread of ozone return dates to 1980 values between models tends to correlate with the spread of the return of inorganic chlorine to 1980 values. In the upper stratosphere, greenhouse gas-induced cooling speeds up the return by about 10–20 years. In the lower stratosphere, and for the column, there is a more direct link in the timing of the return dates of ozone and chlorine, especially for the large Antarctic depletion. Comparisons of total column ozone between the models is affected by different predictions of the evolution of tropospheric ozone within the same scenario, presumably due to differing treatment of tropospheric chemistry. Therefore, for many scenarios, clear conclusions can only be drawn for stratospheric ozone columns rather than the total column. As noted by previous studies, the timing of ozone recovery is affected by the evolution of N2O and CH4. However, quantifying the effect in the simulations analysed here is limited by the few realisations available for these experiments compared to internal model variability. The large increase in N2O given in RCP 6.0 extends the ozone return globally by ∼ 15 years relative to N2O fixed at 1960 abundances, mainly because it allows tropical column ozone to be depleted. The effect in extratropical latitudes is much smaller. The large increase in CH4 given in the RCP 8.5 scenario compared to RCP 6.0 also lengthens ozone return by ∼ 15 years, again mainly through its impact in the tropics. Overall, our estimates of ozone return dates are uncertain due to both uncertainties in future scenarios, in particular those of greenhouse gases, and uncertainties in models. The scenario uncertainty is small in the short term but increases with time, and becomes large by the end of the century. There are still some model–model differences related to well-known processes which affect ozone recovery. Efforts need to continue to ensure that models used for assessment purposes accurately represent stratospheric chemistry and the prescribed scenarios of ozone-depleting substances, and only those models are used to calculate return dates. For future assessments of single forcing or combined effects of CO2, CH4, and N2O on the stratospheric column ozone return dates, this work suggests that it is more important to have multi-member (at least three) ensembles for each scenario from every established participating model, rather than a large number of individual models.

Understanding and modeling the large-scale transport of trace gases and aerosols is important for interpreting past (and projecting future) changes in atmospheric composition. Here we show that there are large differences in the global-scale atmospheric transport properties among the models participating in the IGAC SPARC Chemistry–Climate Model Initiative (CCMI). Specifically, we find up to 40 % differences in the transport timescales connecting the Northern Hemisphere (NH) midlatitude surface to the Arctic and to Southern Hemisphere high latitudes, where the mean age ranges between 1.7 and 2.6 years. We show that these differences are related to large differences in vertical transport among the simulations, in particular to differences in parameterized convection over the oceans. While stronger convection over NH midlatitudes is associated with slower transport to the Arctic, stronger convection in the tropics and subtropics is associated with faster interhemispheric transport. We also show that the differences among simulations constrained with fields derived from the same reanalysis products are as large as (and in some cases larger than) the differences among free-running simulations, most likely due to larger differences in parameterized convection. Our results indicate that care must be taken when using simulations constrained with analyzed winds to interpret the influence of meteorology on tropospheric composition.

The stratospheric age of air (AoA) is a useful measure of the overall capabilities of a general circulation model (GCM) to simulate stratospheric transport. Previous studies have reported a large spread in the simulation of AoA by GCMs and coupled chemistry–climate models (CCMs). Compared to observational estimates, simulated AoA is mostly too low. Here we attempt to untangle the processes that lead to the AoA differences between the models and between models and observations. AoA is influenced by both mean transport by the residual circulation and two-way mixing; we quantify the effects of these processes using data from the CCM inter-comparison projects CCMVal-2 (Chemistry–Climate Model Validation Activity 2) and CCMI-1 (Chemistry–Climate Model Initiative, phase 1). Transport along the residual circulation is measured by the residual circulation transit time (RCTT). We interpret the difference between AoA and RCTT as additional aging by mixing. Aging by mixing thus includes mixing on both the resolved and subgrid scale. We find that the spread in AoA between the models is primarily caused by differences in the effects of mixing and only to some extent by differences in residual circulation strength. These effects are quantified by the mixing efficiency, a measure of the relative increase in AoA by mixing. The mixing efficiency varies strongly between the models from 0.24 to 1.02. We show that the mixing efficiency is not only controlled by horizontal mixing, but by vertical mixing and vertical diffusion as well. Possible causes for the differences in the models' mixing efficiencies are discussed. Differences in subgrid-scale mixing (including differences in advection schemes and model resolutions) likely contribute to the differences in mixing efficiency. However, differences in the relative contribution of resolved versus parameterized wave forcing do not appear to be related to differences in mixing efficiency or AoA.

Continued anthropogenic greenhouse gas (GHG) emissions are expected to cause further global warming throughout the 21st century. Understanding the role of natural forcings and their influence on global warming is thus of great interest. Here we investigate the impact of a recently proposed 21st century grand solar minimum on atmospheric chemistry and climate using the SOCOL3-MPIOM chemistry–climate model with an interactive ocean element. We examine five model simulations for the period 2000–2199, following the greenhouse gas concentration scenario RCP4.5 and a range of different solar forcings. The reference simulation is forced by perpetual repetition of solar cycle 23 until the year 2199. This reference is compared with grand solar minimum simulations, assuming a strong decline in solar activity of 3.5 and 6.5 W m−2, respectively, that last either until 2199 or recover in the 22nd century. Decreased solar activity by 6.5 W m−2 is found to yield up to a doubling of the GHG-induced stratospheric and mesospheric cooling. Under the grand solar minimum scenario, tropospheric temperatures are also projected to decrease compared to the reference. On the global scale a reduced solar forcing compensates for at most 15 % of the expected greenhouse warming at the end of the 21st and around 25 % at the end of the 22nd century. The regional effects are predicted to be significant, in particular in northern high-latitude winter. In the stratosphere, the reduction of around 15 % of incoming ultraviolet radiation leads to a decrease in ozone production by up to 8 %, which overcompensates for the anticipated ozone increase due to reduced stratospheric temperatures and an acceleration of the Brewer–Dobson circulation. This, in turn, leads to a delay in total ozone column recovery from anthropogenic halogen-induced depletion, with a global ozone recovery to the pre-ozone hole values happening only upon completion of the grand solar minimum.

The eruption of Mt. Tambora in 1815 was the largest volcanic eruption of the past 500 years. The eruption had significant climatic impacts, leading to the 1816 year without a summer, and remains a valuable event from which to understand the climatic effects of large stratospheric volcanic sulfur dioxide injections. The eruption also resulted in one of the strongest and most easily identifiable volcanic sulfate signals in polar ice cores, which are widely used to reconstruct the timing and atmospheric sulfate loading of past eruptions. As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), five state-of-the-art global aerosol models simulated this eruption. We analyse both simulated background (no Tambora) and volcanic (with Tambora) sulfate deposition to polar regions and compare to ice core records. The models simulate overall similar patterns of background sulfate deposition, although there are differences in regional details and magnitude. However, the volcanic sulfate deposition varies considerably between the models with differences in timing, spatial pattern and magnitude. Mean simulated deposited sulfate on Antarctica ranges from 19 to 264 kg km−2 and on Greenland from 31 to 194 kg km−2, as compared to the mean ice-core-derived estimates of roughly 50 kg km−2 for both Greenland and Antarctica. The ratio of the hemispheric atmospheric sulfate aerosol burden after the eruption to the average ice sheet deposited sulfate varies between models by up to a factor of 15. Sources of this inter-model variability include differences in both the formation and the transport of sulfate aerosol. Our results suggest that deriving relationships between sulfate deposited on ice sheets and atmospheric sulfate burdens from model simulations may be associated with greater uncertainties than previously thought.

Ozone fields simulated for the first phase of the Chemistry-Climate Model Initiative (CCMI-1) will be used as forcing data in the 6th Coupled Model Intercomparison Project. Here we assess, using reference and sensitivity simulations produced for CCMI-1, the suitability of CCMI-1 model results for this process, investigating the degree of consistency amongst models regarding their responses to variations in individual forcings. We consider the influences of methane, nitrous oxide, a combination of chlorinated or brominated ozone-depleting substances, and a combination of carbon dioxide and other greenhouse gases. We find varying degrees of consistency in the models' responses in ozone to these individual forcings, including some considerable disagreement. In particular, the response of total-column ozone to these forcings is less consistent across the multi-model ensemble than profile comparisons. We analyse how stratospheric age of air, a commonly used diagnostic of stratospheric transport, responds to the forcings. For this diagnostic we find some salient differences in model behaviour, which may explain some of the findings for ozone. The findings imply that the ozone fields derived from CCMI-1 are subject to considerable uncertainties regarding the impacts of these anthropogenic forcings. We offer some thoughts on how to best approach the problem of generating a consensus ozone database from a multi-model ensemble such as CCMI-1.

To simulate the impacts of volcanic eruptions on the stratosphere, chemistry–climate models that do not include an online aerosol module require temporally and spatially resolved aerosol size parameters for heterogeneous chemistry and aerosol radiative properties as a function of wavelength. For phase 1 of the Chemistry-Climate Model Initiative (CCMI-1) and, later, for phase 6 of the Coupled Model Intercomparison Project (CMIP6) two such stratospheric aerosol data sets were compiled, whose functional capability and representativeness are compared here. For CCMI-1, the SAGE-4λ data set was compiled, which hinges on the measurements at four wavelengths of the SAGE (Stratospheric Aerosol and Gas Experiment) II satellite instrument and uses ground-based lidar measurements for gap-filling immediately after the 1991 Mt Pinatubo eruption, when the stratosphere was too optically opaque for SAGE II. For CMIP6, the new SAGE-3λ data set was compiled, which excludes the least reliable SAGE II wavelength and uses measurements from CLAES (Cryogenic Limb Array Etalon Spectrometer) on UARS, the Upper Atmosphere Research Satellite, for gap-filling following the Mt Pinatubo eruption instead of ground-based lidars. Here, we performed SOCOLv3 (Solar Climate Ozone Links version 3) chemistry–climate model simulations of the recent past (1986–2005) to investigate the impact of the Mt Pinatubo eruption in 1991 on stratospheric temperature and ozone and how this response differs depending on which aerosol data set is applied. The use of SAGE-4λ results in heating and ozone loss being overestimated in the tropical lower stratosphere compared to observations in the post-eruption period by approximately 3 K and 0.2 ppmv, respectively. However, less heating occurs in the model simulations based on SAGE-3λ, because the improved gap-filling procedures after the eruption lead to less aerosol loading in the tropical lower stratosphere. As a result, simulated tropical temperature anomalies in the model simulations based on SAGE-3λ for CMIP6 are in excellent agreement with MERRA and ERA-Interim reanalyses in the post-eruption period. Less heating in the simulations with SAGE-3λ means that the rate of tropical upwelling does not strengthen as much as it does in the simulations with SAGE-4λ, which limits dynamical uplift of ozone and therefore provides more time for ozone to accumulate in tropical mid-stratospheric air. Ozone loss following the Mt Pinatubo eruption is overestimated by up to 0.1 ppmv in the model simulations based on SAGE-3λ, which is a better agreement with observations than in the simulations based on SAGE-4λ. Overall, the CMIP6 stratospheric aerosol data set, SAGE-3λ, allows SOCOLv3 to more accurately simulate the post-Pinatubo eruption period.

The pre-industrial millennium is among the periods selected by the Paleoclimate Model Intercomparison Project (PMIP) for experiments contributing to the sixth phase of the Coupled Model Intercomparison Project (CMIP6) and the fourth phase of the PMIP (PMIP4). The past1000 transient simulations serve to investigate the response to (mainly) natural forcing under background conditions not too different from today, and to discriminate between forced and internally generated variability on interannual to centennial timescales. This paper describes the motivation and the experimental set-ups for the PMIP4-CMIP6 past1000 simulations, and discusses the forcing agents orbital, solar, volcanic, and land use/land cover changes, and variations in greenhouse gas concentrations. The past1000 simulations covering the pre-industrial millennium from 850 Common Era (CE) to 1849 CE have to be complemented by historical simulations (1850 to 2014 CE) following the CMIP6 protocol. The external forcings for the past1000 experiments have been adapted to provide a seamless transition across these time periods. Protocols for the past1000 simulations have been divided into three tiers. A default forcing data set has been defined for the Tier 1 (the CMIP6 past1000) experiment. However, the PMIP community has maintained the flexibility to conduct coordinated sensitivity experiments to explore uncertainty in forcing reconstructions as well as parameter uncertainty in dedicated Tier 2 simulations. Additional experiments (Tier 3) are defined to foster collaborative model experiments focusing on the early instrumental period and to extend the temporal range and the scope of the simulations. This paper outlines current and future research foci and common analyses for collaborative work between the PMIP and the observational communities (reconstructions, instrumental data).

We compare simulations from three high-top (with upper lid above 120 km) and five medium-top (with upper lid around 80 km) atmospheric models with observations of odd nitrogen (NOx = NO + NO2), temperature, and carbon monoxide from seven satellite instruments (ACE-FTS on SciSat, GOMOS, MIPAS, and SCIAMACHY on Envisat, MLS on Aura, SABER on TIMED, and SMR on Odin) during the Northern Hemisphere (NH) polar winter 2008/2009. The models included in the comparison are the 3-D chemistry transport model 3dCTM, the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model, FinROSE, the Hamburg Model of the Neutral and Ionized Atmosphere (HAMMONIA), the Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA), the modelling tools for SOlar Climate Ozone Links studies (SOCOL and CAO-SOCOL), and the Whole Atmosphere Community Climate Model (WACCM4). The comparison focuses on the energetic particle precipitation (EPP) indirect effect, that is, the polar winter descent of NOx largely produced by EPP in the mesosphere and lower thermosphere. A particular emphasis is given to the impact of the sudden stratospheric warming (SSW) in January 2009 and the subsequent elevated stratopause (ES) event associated with enhanced descent of mesospheric air. The chemistry climate model simulations have been nudged toward reanalysis data in the troposphere and stratosphere while being unconstrained above. An odd nitrogen upper boundary condition obtained from MIPAS observations has further been applied to medium-top models. Most models provide a good representation of the mesospheric tracer descent in general, and the EPP indirect effect in particular, during the unperturbed (pre-SSW) period of the NH winter 2008/2009. The observed NOx descent into the lower mesosphere and stratosphere is generally reproduced within 20 %. Larger discrepancies of a few model simulations could be traced back either to the impact of the models' gravity wave drag scheme on the polar wintertime meridional circulation or to a combination of prescribed NOx mixing ratio at the uppermost model layer and low vertical resolution. In March–April, after the ES event, however, modelled mesospheric and stratospheric NOx distributions deviate significantly from the observations. The too-fast and early downward propagation of the NOx tongue, encountered in most simulations, coincides with a temperature high bias in the lower mesosphere (0.2–0.05 hPa), likely caused by an overestimation of descent velocities. In contrast, upper-mesospheric temperatures (at 0.05–0.001 hPa) are generally underestimated by the high-top models after the onset of the ES event, being indicative for too-slow descent and hence too-low NOx fluxes. As a consequence, the magnitude of the simulated NOx tongue is generally underestimated by these models. Descending NOx amounts simulated with medium-top models are on average closer to the observations but show a large spread of up to several hundred percent. This is primarily attributed to the different vertical model domains in which the NOx upper boundary condition is applied. In general, the intercomparison demonstrates the ability of state-of-the-art atmospheric models to reproduce the EPP indirect effect in dynamically and geomagnetically quiescent NH winter conditions. The encountered differences between observed and simulated NOx, CO, and temperature distributions during the perturbed phase of the 2009 NH winter, however, emphasize the need for model improvements in the dynamical representation of elevated stratopause events in order to allow for a better description of the EPP indirect effect under these particular conditions.

We present an overview of state-of-the-art chemistry–climate and chemistry transport models that are used within phase 1 of the Chemistry–Climate Model Initiative (CCMI-1). The CCMI aims to conduct a detailed evaluation of participating models using process-oriented diagnostics derived from observations in order to gain confidence in the models' projections of the stratospheric ozone layer, tropospheric composition, air quality, where applicable global climate change, and the interactions between them. Interpretation of these diagnostics requires detailed knowledge of the radiative, chemical, dynamical, and physical processes incorporated in the models. Also an understanding of the degree to which CCMI-1 recommendations for simulations have been followed is necessary to understand model responses to anthropogenic and natural forcing and also to explain inter-model differences. This becomes even more important given the ongoing development and the ever-growing complexity of these models. This paper also provides an overview of the available CCMI-1 simulations with the aim of informing CCMI data users.

Effects of the Quasi-Biennial Oscillation (QBO) on tropospheric climate are not always strong or they appear only intermittently. Studying them requires long time series of both the QBO and climate variables, which has restricted previous studies to the past 30–50 years. Here we use the benefits of an existing QBO reconstruction back to 1908. We first investigate additional, newly digitized historical observations of stratospheric winds to test the reconstruction. Then we use the QBO time series to analyse atmospheric data sets (reconstructions and reanalyses) as well as the results of coupled ocean–atmosphere–chemistry climate model simulations that were forced with the reconstructed QBO. We investigate effects related to (1) tropical–extratropical interaction in the stratosphere, wave–mean flow interaction and subsequent downward propagation, and (2) interaction between deep tropical convection and stratospheric flow. We generally find weak connections, though some are statistically significant over the 100-year period and consistent with model results. Apparent multidecadal variations in the connection between the QBO and the investigated climate responses are consistent with a small effect in the presence of large variability, with one exception: the imprint on the northern polar vortex, which is seen in recent reanalysis data, is not found in the period 1908–1957. Conversely, an imprint in Berlin surface air temperature is only found in 1908–1957 but not in the recent period. Likewise, in the model simulations both links tend to appear alternatingly, suggesting a more systematic modulation due to a shift in the circulation, for example. Over the Pacific warm pool, we find increased convection during easterly QBO, mainly in boreal winter in observation-based data as well as in the model simulations, with large variability. No QBO effects were found in the Indian monsoon strength or Atlantic hurricane frequency.

The influence of reduced solar forcing (grand solar minimum or geoengineering scenarios like solar radiation management) on the Atlantic Meridional Overturning Circulation (AMOC) is assessed in an ensemble of atmosphere–ocean–chemistry–climate model simulations. Ensemble sensitivity simulations are performed with and without interactive chemistry. In both experiments the AMOC is intensified in the course of the solar radiation reduction, which is attributed to the thermal effect of the solar forcing: reduced sea surface temperatures and enhanced sea ice formation increase the density of the upper ocean in the North Atlantic and intensify the deepwater formation. Furthermore, a second, dynamical effect on the AMOC is identified driven by the stratospheric cooling in response to the reduced solar forcing. The cooling is strongest in the tropics and leads to a weakening of the northern polar vortex. By stratosphere–troposphere interactions, the stratospheric circulation anomalies induce a negative phase of the Arctic Oscillation in the troposphere which is found to weaken the AMOC through wind stress and heat flux anomalies in the North Atlantic. The dynamic mechanism is present in both ensemble experiments. In the experiment with interactive chemistry, however, it is strongly amplified by stratospheric ozone changes. In the coupled system, both effects counteract and weaken the response of the AMOC to the solar forcing reduction. Neglecting chemistry–climate interactions in model simulations may therefore lead to an overestimation of the AMOC response to solar forcing.

Stratospheric water vapour (SWV) is an important component of the Earth's atmosphere as it affects both radiative balance and the chemistry of the atmosphere. Key processes driving changes in SWV include dehydration of air masses transiting the cold-point tropopause (CPT) and methane oxidation. We use a chemistry–climate model to simulate changes in SWV through the 21st century following the four canonical representative concentration pathways (RCPs). Furthermore, we quantify the contribution that methane oxidation makes to SWV following each of the RCPs. Although the methane contribution to SWV maximizes in the upper stratosphere, modelled SWV trends are found to be driven predominantly by warming of the CPT rather than by increasing methane oxidation. SWV changes by −5 to 60 % (depending on the location in the atmosphere and emissions scenario) and increases in the lower stratosphere in all RCPs through the 21st century. Because the lower stratosphere is where water vapour radiative forcing maximizes, SWV's influence on surface climate is also expected to increase through the 21st century.

The enhancement of the stratospheric aerosol layer by volcanic eruptions induces a complex set of responses causing global and regional climate effects on a broad range of timescales. Uncertainties exist regarding the climatic response to strong volcanic forcing identified in coupled climate simulations that contributed to the fifth phase of the Coupled Model Intercomparison Project (CMIP5). In order to better understand the sources of these model diversities, the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP) has defined a coordinated set of idealized volcanic perturbation experiments to be carried out in alignment with the CMIP6 protocol. VolMIP provides a common stratospheric aerosol data set for each experiment to minimize differences in the applied volcanic forcing. It defines a set of initial conditions to assess how internal climate variability contributes to determining the response. VolMIP will assess to what extent volcanically forced responses of the coupled ocean–atmosphere system are robustly simulated by state-of-the-art coupled climate models and identify the causes that limit robust simulated behavior, especially differences in the treatment of physical processes. This paper illustrates the design of the idealized volcanic perturbation experiments in the VolMIP protocol and describes the common aerosol forcing input data sets to be used.

After major volcanic eruptions the enhanced aerosol causes ozone changes due to greater heterogeneous chemistry on the particle surfaces (HET-AER) and from dynamical effects related to the radiative heating of the lower stratosphere (RAD-DYN). We carry out a series of experiments with an atmosphere–ocean–chemistry–climate model to assess how these two processes change stratospheric ozone and Northern Hemispheric (NH) polar vortex dynamics. Ensemble simulations are performed under present day and preindustrial conditions, and with aerosol forcings representative of different eruption strength, to investigate changes in the response behaviour. We show that the halogen component of the HET-AER effect dominates under present-day conditions with a global reduction of ozone (−21 DU for the strongest eruption) particularly at high latitudes, whereas the HET-AER effect increases stratospheric ozone due to N2O5 hydrolysis in a preindustrial atmosphere (maximum anomalies +4 DU). The halogen-induced ozone changes in the present-day atmosphere offset part of the strengthening of the NH polar vortex during mid-winter (reduction of up to −16 m s-1 in January) and slightly amplify the dynamical changes in the polar stratosphere in late winter (+11 m s-1 in March). The RAD-DYN mechanism leads to positive column ozone anomalies which are reduced in a present-day atmosphere by amplified polar ozone depletion (maximum anomalies +12 and +18 DU for present day and preindustrial, respectively). For preindustrial conditions, the ozone response is consequently dominated by RAD-DYN processes, while under present-day conditions, HET-AER effects dominate. The dynamical response of the stratosphere is dominated by the RAD-DYN mechanism showing an intensification of the NH polar vortex in winter (up to +10 m s-1 in January). Ozone changes due to the RAD-DYN mechanism slightly reduce the response of the polar vortex after the eruption under present-day conditions.

We have performed more than 300 atmospheric simulations of the 1991 Pinatubo eruption using the AER 2-D sulfate aerosol model to optimize the initial sulfur mass injection as a function of altitude, which in previous modeling studies has often been chosen in an ad hoc manner (e.g., by applying a rectangular-shaped emission profile). Our simulations are generated by varying a four-parameter vertical mass distribution, which is determined by a total injection mass and a skew-normal distribution function. Our results suggest that (a) the initial mass loading of the Pinatubo eruption is approximately 14 Mt of SO2; (b) the injection vertical distribution is strongly skewed towards the lower stratosphere, leading to a peak mass sulfur injection at 18–21 km; (c) the injection magnitude and height affect early southward transport of the volcanic clouds as observed by SAGE II.

Because tropospheric ozone is both a greenhouse gas and harmful air pollutant, it is important to understand how anthropogenic activities may influence its abundance and distribution through the 21st century. Here, we present model simulations performed with the chemistry–climate model SOCOL, in which spatially disaggregated chemistry and transport tracers have been implemented in order to better understand the distribution and projected changes in tropospheric ozone. We examine the influences of ozone precursor emissions (nitrogen oxides (NOx), carbon monoxide (CO) and volatile organic compounds (VOCs)), climate change (including methane effects) and stratospheric ozone recovery on the tropospheric ozone budget, in a simulation following the climate scenario Representative Concentration Pathway (RCP) 6.0 (a medium-high, and reasonably realistic climate scenario). Changes in ozone precursor emissions have the largest effect, leading to a global-mean increase in tropospheric ozone which maximizes in the early 21st century at 23% compared to 1960. The increase is most pronounced at northern midlatitudes, due to regional emission patterns: between 1990 and 2060, northern midlatitude tropospheric ozone remains at constantly large abundances: 31% larger than in 1960. Over this 70-year period, attempts to reduce emissions in Europe and North America do not have an effect on zonally averaged northern midlatitude ozone because of increasing emissions from Asia, together with the long lifetime of ozone in the troposphere. A simulation with fixed anthropogenic ozone precursor emissions of NOx, CO and non-methane VOCs at 1960 conditions shows a 6% increase in global-mean tropospheric ozone by the end of the 21st century, with an 11 % increase at northern midlatitudes. This increase maximizes in the 2080s and is mostly caused by methane, which maximizes in the 2080s following RCP 6.0, and plays an important role in controlling ozone directly, and indirectly through its influence on other VOCs and CO. Enhanced flux of ozone from the stratosphere to the troposphere as well as climate change-induced enhancements in lightning NOx emissions also increase the tropospheric ozone burden, although their impacts are relatively small. Overall, the results show that under this climate scenario, ozone in the future is governed largely by changes in methane and NOx; methane induces an increase in tropospheric ozone that is approximately one-third of that caused by NOx. Climate impacts on ozone through changes in tropospheric temperature, humidity and lightning NOx remain secondary compared with emission strategies relating to anthropogenic emissions of NOx, such as fossil fuel burning. Therefore, emission policies globally have a critical role to play in determining tropospheric ozone evolution through the 21st century.

Solar radiation is the main source of energy for the Earth's atmosphere and in many respects defines its composition, photochemistry, temperature profile and dynamics. The magnitude of the solar irradiance variability strongly depends on the wavelength, making difficult its representation in climate models. Due to some deficiencies in the applied radiation codes, several models fail to show a clear response in middle stratospheric heating rates to solar spectral irradiance variability; therefore, it is important to evaluate model performance in this respect before doing multiple runs. In this work we evaluate the performance of three generations of ECHAM (4, 5 and 6) solar radiation schemes by a comparison with the reference high-resolution libRadtran code. We found that all original ECHAM radiation codes miss almost all solar signals in the heating rates in the mesosphere. In the stratosphere the two-band ECHAM4 code (E4) has an almost negligible radiative response to solar irradiance changes and the six-band ECHAM5 code (E5c) reproduces only about half of the reference signal, while representation in the ECHAM6 code (E6) is better – it misses a maximum of about 15% in the upper stratosphere. On the basis of the comparison results we suggest necessary improvements to the ECHAM family codes by the inclusion of available parameterizations of the heating rate due to absorption by oxygen (O2) and ozone (O3). Improvement is presented for E5c and E6, and both codes, with the introduced parameterizations, represent the heating rate response to the spectral solar irradiance variability simulated with libRadtran much better without a substantial increase in computer time. The suggested parameterizations are recommended to be applied in the middle-atmosphere version of the ECHAM-5 and 6 models for the study of the solar irradiance influence on climate.

The newly developed atmosphere–ocean–chemistry–climate model SOCOL-MPIOM is presented by demonstrating the influence of chemistry–climate interactions on the climate state and the variability. Therefore, we compare pre-industrial control simulations with (CHEM) and without (NOCHEM) interactive chemistry. In general, the influence of the chemistry on the mean state and the variability is small and mainly restricted to the stratosphere and mesosphere. The atmospheric dynamics mainly differ in polar regions, with slightly stronger polar vortices in the austral and boreal winter, respectively. The strengthening of the vortex is related to larger stratospheric temperature gradients, which are attributed to a parameterisation of the absorption of ozone and oxygen in different wavelength intervals, which is considered in the version with interactive chemistry only. A second reason for the temperature differences between CHEM and NOCHEM is related to diurnal variations in the ozone concentrations in the higher atmosphere, which are missing in NOCHEM. Furthermore, stratospheric water vapour concentrations substantially differ between the two experiments, but their effect on temperature is small. In both setups, the simulated intensity and variability of the northern polar vortex is inside the range of present-day observations. Additionally, the performance of SOCOL-MPIOM under changing external forcings is assessed for the period 1600–2000 using an ensemble of simulations. In the industrial period from 1850 onward SOCOL-MPIOM overestimates the global mean surface air temperature increase in comparison to observational data sets. Sensitivity simulations show that this overestimation can be attributed to a combination of factors: the solar forcing reconstruction, the simulated ozone changes, and incomplete aerosol effects and land use changes.

As the understanding and representation of the impacts of volcanic eruptions on climate have improved in the last decades, uncertainties in the stratospheric aerosol forcing from large eruptions are now linked not only to visible optical depth estimates on a global scale but also to details on the size, latitude and altitude distributions of the stratospheric aerosols. Based on our understanding of these uncertainties, we propose a new model-based approach to generating a volcanic forcing for general circulation model (GCM) and chemistry–climate model (CCM) simulations. This new volcanic forcing, covering the 1600–present period, uses an aerosol microphysical model to provide a realistic, physically consistent treatment of the stratospheric sulfate aerosols. Twenty-six eruptions were modeled individually using the latest available ice cores aerosol mass estimates and historical data on the latitude and date of eruptions. The evolution of aerosol spatial and size distribution after the sulfur dioxide discharge are hence characterized for each volcanic eruption. Large variations are seen in hemispheric partitioning and size distributions in relation to location/date of eruptions and injected SO2 masses. Results for recent eruptions show reasonable agreement with observations. By providing these new estimates of spatial distributions of shortwave and long-wave radiative perturbations, this volcanic forcing may help to better constrain the climate model responses to volcanic eruptions in the 1600–present period. The final data set consists of 3-D values (with constant longitude) of spectrally resolved extinction coefficients, single scattering albedos and asymmetry factors calculated for different wavelength bands upon request. Surface area densities for heterogeneous chemistry are also provided.

In terms of atmospheric impact, the volcanic eruption of Mt. Pinatubo (1991) is the best characterized large eruption on record. We investigate here the model-derived stratospheric warming following the Pinatubo eruption as derived from SAGE II extinction data including recent improvements in the processing algorithm. This method, termed SAGE_4λ, makes use of the four wavelengths (385, 452, 525 and 1024 nm) of the SAGE II data when available, and uses a data-filling procedure in the opacity-induced "gap" regions. Using SAGE_4λ, we derived aerosol size distributions that properly reproduce extinction coefficients also at much longer wavelengths. This provides a good basis for calculating the absorption of terrestrial infrared radiation and the resulting stratospheric heating. However, we also show that the use of this data set in a global chemistry–climate model (CCM) still leads to stronger aerosol-induced stratospheric heating than observed, with temperatures partly even higher than the already too high values found by many models in recent general circulation model (GCM) and CCM intercomparisons. This suggests that the overestimation of the stratospheric warming after the Pinatubo eruption may not be ascribed to an insufficient observational database but instead to using outdated data sets, to deficiencies in the implementation of the forcing data, or to radiative or dynamical model artifacts. Conversely, the SAGE_4λ approach reduces the infrared absorption in the tropical tropopause region, resulting in a significantly better agreement with the post-volcanic temperature record at these altitudes.

The response of atmospheric chemistry and dynamics to volcanic eruptions and to a decrease in solar activity during the Dalton Minimum is investigated with the fully coupled atmosphere–ocean chemistry general circulation model SOCOL-MPIOM (modeling tools for studies of SOlar Climate Ozone Links-Max Planck Institute Ocean Model) covering the time period 1780 to 1840 AD. We carried out several sensitivity ensemble experiments to separate the effects of (i) reduced solar ultra-violet (UV) irradiance, (ii) reduced solar visible and near infrared irradiance, (iii) enhanced galactic cosmic ray intensity as well as less intensive solar energetic proton events and auroral electron precipitation, and (iv) volcanic aerosols. The introduced changes of UV irradiance and volcanic aerosols significantly influence stratospheric dynamics in the early 19th century, whereas changes in the visible part of the spectrum and energetic particles have smaller effects. A reduction of UV irradiance by 15%, which represents the presently discussed highest estimate of UV irradiance change caused by solar activity changes, causes global ozone decrease below the stratopause reaching as much as 8% in the midlatitudes at 5 hPa and a significant stratospheric cooling of up to 2 °C in the mid-stratosphere and to 6 °C in the lower mesosphere. Changes in energetic particle precipitation lead only to minor changes in the yearly averaged temperature fields in the stratosphere. Volcanic aerosols heat the tropical lower stratosphere, allowing more water vapour to enter the tropical stratosphere, which, via HOx reactions, decreases upper stratospheric and mesospheric ozone by roughly 4%. Conversely, heterogeneous chemistry on aerosols reduces stratospheric NOx, leading to a 12% ozone increase in the tropics, whereas a decrease in ozone of up to 5% is found over Antarctica in boreal winter. The linear superposition of the different contributions is not equivalent to the response obtained in a simulation when all forcing factors are applied during the Dalton Minimum (DM) – this effect is especially well visible for NOx/NOy. Thus, this study also shows the non-linear behaviour of the coupled chemistry-climate system. Finally, we conclude that especially UV and volcanic eruptions dominate the changes in the ozone, temperature and dynamics while the NOx field is dominated by the energetic particle precipitation. Visible radiation changes have only very minor effects on both stratospheric dynamics and chemistry.

Previous studies have highlighted the severity of detrimental effects for life on earth after an assumed regionally limited nuclear war. These effects are caused by climatic, chemical and radiative changes persisting for up to one decade. However, so far only a very limited number of climate model simulations have been performed, giving rise to the question how realistic previous computations have been. This study uses the coupled chemistry climate model (CCM) SOCOL, which belongs to a different family of CCMs than previously used, to investigate the consequences of such a hypothetical nuclear conflict. In accordance with previous studies, the present work assumes a scenario of a nuclear conflict between India and Pakistan, each applying 50 warheads with an individual blasting power of 15 kt ("Hiroshima size") against the major population centers, resulting in the emission of tiny soot particles, which are generated in the firestorms expected in the aftermath of the detonations. Substantial uncertainties related to the calculation of likely soot emissions, particularly concerning assumptions of target fuel loading and targeting of weapons, have been addressed by simulating several scenarios, with soot emissions ranging from 1 to 12 Tg. Their high absorptivity with respect to solar radiation leads to a rapid self-lofting of the soot particles into the strato- and mesosphere within a few days after emission, where they remain for several years. Consequently, the model suggests earth's surface temperatures to drop by several degrees Celsius due to the shielding of solar irradiance by the soot, indicating a major global cooling. In addition, there is a substantial reduction of precipitation lasting 5 to 10 yr after the conflict, depending on the magnitude of the initial soot release. Extreme cold spells associated with an increase in sea ice formation are found during Northern Hemisphere winter, which expose the continental land masses of North America and Eurasia to a cooling of several degrees. In the stratosphere, the strong heating leads to an acceleration of catalytic ozone loss and, consequently, to enhancements of UV radiation at the ground. In contrast to surface temperature and precipitation changes, which show a linear dependence to the soot burden, there is a saturation effect with respect to stratospheric ozone chemistry. Soot emissions of 5 Tg lead to an ozone column reduction of almost 50% in northern high latitudes, while emitting 12 Tg only increases ozone loss by a further 10%. In summary, this study, though using a different chemistry climate model, corroborates the previous investigations with respect to the atmospheric impacts. In addition to these persistent effects, the present study draws attention to episodically cold phases, which would likely add to the severity of human harm worldwide. The best insurance against such a catastrophic development would be the delegitimization of nuclear weapons.

We present a vertically resolved zonal mean monthly mean global ozone data set spanning the period 1901 to 2007, called HISTOZ.1.0. It is based on a new approach that combines information from an ensemble of chemistry climate model (CCM) simulations with historical total column ozone information. The CCM simulations incorporate important external drivers of stratospheric chemistry and dynamics (in particular solar and volcanic effects, greenhouse gases and ozone depleting substances, sea surface temperatures, and the quasi-biennial oscillation). The historical total column ozone observations include ground-based measurements from the 1920s onward and satellite observations from 1970 to 1976. An off-line data assimilation approach is used to combine model simulations, observations, and information on the observation error. The period starting in 1979 was used for validation with existing ozone data sets and therefore only ground-based measurements were assimilated. Results demonstrate considerable skill from the CCM simulations alone. Assimilating observations provides additional skill for total column ozone. With respect to the vertical ozone distribution, assimilating observations increases on average the correlation with a reference data set, but does not decrease the mean squared error. Analyses of HISTOZ.1.0 with respect to the effects of El Niño–Southern Oscillation (ENSO) and of the 11 yr solar cycle on stratospheric ozone from 1934 to 1979 qualitatively confirm previous studies that focussed on the post-1979 period. The ENSO signature exhibits a much clearer imprint of a change in strength of the Brewer–Dobson circulation compared to the post-1979 period. The imprint of the 11 yr solar cycle is slightly weaker in the earlier period. Furthermore, the total column ozone increase from the 1950s to around 1970 at northern mid-latitudes is briefly discussed. Indications for contributions of a tropospheric ozone increase, greenhouse gases, and changes in atmospheric circulation are found. Finally, the paper points at several possible future improvements of HISTOZ.1.0.

We present the third generation of the coupled chemistry–climate model (CCM) SOCOL (modeling tools for studies of SOlar Climate Ozone Links). The most notable modifications compared to the previous model version are (1) the dynamical core has been updated with the fifth generation of the middle-atmosphere general circulation model MA-ECHAM (European Centre/HAMburg climate model), and (2) the advection of the chemical species is now calculated by a mass-conserving and shape-preserving flux-form transport scheme instead of the previously used hybrid advection scheme. The whole chemistry code has been rewritten according to the ECHAM5 infrastructure and transferred to Fortran95. In contrast to its predecessors, SOCOLvs3 is now fully parallelized. The performance of the new SOCOL version is evaluated on the basis of transient model simulations (1975–2004) with different horizontal (T31 and T42) resolutions, following the approach of the CCMVal-1 model validation activity. The advanced advection scheme significantly reduces the artificial loss and accumulation of tracer mass in regions with strong gradients that was observed in previous model versions. Compared to its predecessors, SOCOLvs3 generally shows more realistic distributions of chemical trace species, especially of total inorganic chlorine, in terms of the mean state, but also of the annual and interannual variability. Advancements with respect to model dynamics are for example a better representation of the stratospheric mean state in spring, especially in the Southern Hemisphere, and a slowdown of the upward propagation in the tropical lower stratosphere. Despite a large number of improvements model deficiencies still remain. Examples include a too-fast vertical ascent and/or horizontal mixing in the tropical stratosphere, the cold temperature bias in the lowermost polar stratosphere, and the overestimation of polar total ozone loss during Antarctic springtime.