Future increases in stratospheric water vapour risk amplifying climate change and slowing down the recovery of the ozone layer. However, state-of-the-art climate models strongly disagree on the magnitude of these increases under global warming. Uncertainty primarily arises from the complex processes leading to dehydration of air during its tropical ascent into the stratosphere. Here we derive an observational constraint on this longstanding uncertainty. We use a statistical-learning approach to infer historical co-variations between the atmospheric temperature structure and tropical lower stratospheric water vapour concentrations. For climate models, we demonstrate that these historically constrained relationships are highly predictive of the water vapour response to increased atmospheric carbon dioxide. We obtain an observationally constrained range for stratospheric water vapour changes per degree of global warming of 0.31 ± 0.39 ppmv K⁻¹. Across 61 climate models, we find that a large fraction of future model projections are inconsistent with observational evidence. In particular, frequently projected strong increases (>1 ppmv K⁻¹) are highly unlikely. Our constraint represents a 50% decrease in the 95th percentile of the climate model uncertainty distribution, which has implications for surface warming, ozone recovery and the tropospheric circulation response under climate change.

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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.@en

Water vapor (H₂O) is the source of reactive hydrogen radicals in the middle atmosphere, whereas carbon monoxide (CO), being formed by CO₂photolysis, 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 REFC1SD 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.

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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.

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Recent observations show a significant decrease in lower-stratospheric (LS) ozone concentrations in tropical and mid-latitude regions since 1998. By analysing 31 chemistry climate model (CCM) simulations performed for the Chemistry Climate Model Initiative (CCMI; Morgenstern et al., 2017), we find a large spread in the 1998 2018 trend patterns between different CCMs and between different realizations performed with the same CCM. The latter in particular indicates that natural variability strongly influences LS ozone trends. However none of the model simulations reproduce the observed ozone trend structure of coherent negative trends in the LS. In contrast to the observations, most models show an LS trend pattern with negative trends in the tropics (20 S 20 N) and positive trends in the northern mid-latitudes (30 50 N) or vice versa. To investigate the influence of natural variability on recent LS ozone trends, we analyse the sensitivity of observational trends and the models trend probability distributions for varying periods with start dates from 1995 to 2001 and end dates from 2013 to 2019. Generally, modelled and observed LS trends remain robust for these different periods; however observational data show a change towards weaker mid-latitude trends for certain periods, likely forced by natural variability. Moreover we show that in the tropics the observed trends agree well with the models trend distribution, whereas in the mid-latitudes the observational trend is typically an extreme value of the models distribution. We further investigate the LS ozone trends for extended periods reaching into the future and find that all models develop a positive ozone trend at mid-latitudes, and the trends converge to constant values by the period that spans 1998 2060. Inter-model correlations between ozone trends and transport-circulation trends confirm the dominant role of greenhouse gas (GHG)-driven tropical upwelling enhancement on the tropical LS ozone decrease. Mid-latitude ozone, on the other hand, appears to be influenced by multiple competing factors: an enhancement in the shallow branch decreases ozone, while an enhancement in the deep branch increases ozone, and, furthermore, mixing plays a role here too. Sensitivity simulations with fixed forcing of GHGs or ozonedepleting substances (ODSs) reveal that the GHG-driven increase in circulation strength does not lead to a net trend in LS mid-latitude column ozone. Rather, the positive ozone trends simulated consistently in the models in this region emerge from the decline in ODSs, i.e. the ozone recovery. Therefore, we hypothesize that next to the influence of natural variability, the disagreement of modelled and observed LS mid-latitude ozone trends could indicate a mismatch in the relative role of the response of ozone to ODS versus GHG forcing in the models.

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As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), several climate modeling centers performed a coordinated prestudy 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 fac tor 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.

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Reliable ozone trends after 2000 are essential to detect early ozone recovery. However, the long-term ground-based and satellite ozone profile trends reported in the literature show a high variability. There are multiple reasons for variability in the reported long-term trends such as the measurement timing and the dataset quality.

The Payerne Switzerland microwave radiometer (MWR) ozone trends are significantly positive at 2 % to 3 % per decade in the upper stratosphere (5–1 hPa, 35–48 km), with a high variation with altitude. This is in accordance with the Northern Hemisphere (NH) trends reported by other ground-based instruments in the SPARC LOTUS project. In order to determine what part of the variability between different datasets comes from measurement timing, Payerne MWR and SOCOL v3.0 chemistry–climate model (CCM) trends were estimated for each hour of the day with a multiple linear regression model. Trends were quantified as a function of local solar time (LST). In the middle and upper stratosphere, differences as a function of LST are reported for both the MWR and simulated trends for the post-2000 period. However, these differences are not significant at the 95 % confidence level. In the lower mesosphere (1–0.1 hPa, 48–65 km), the 2010–2018 day- and nighttime trends have been considered. Here again, the variation in the trend with LST is not significant at the 95 % confidence level. Based on these results we conclude that significant trend differences between instruments cannot be attributed to a systematic temporal sampling effect.

The dataset quality is of primary importance in a reliable trend derivation, and multi-instrument comparison analyses can be used to assess the long-term stability of data records by estimating the drift and bias of instruments. The Payerne MWR dataset has been homogenized to ensure a stable measurement contribution to the ozone profiles and to take into account the effects of three major instrument upgrades. At each instrument upgrade, a correction offset has been calculated using parallel measurements or simultaneous measurements by an independent instrument. At pressure levels smaller than 0.59 hPa (above ∼50 km), the homogenization corrections to be applied to the Payerne MWR ozone profiles are dependent on LST. Due to the lack of reference measurements with a comparable measurement contribution at a high time resolution, a comprehensive homogenization of the sub-daily ozone profiles was possible only for pressure levels larger than 0.59 hPa.

The ozone profile dataset from the Payerne MWR, Switzerland, was compared with profiles from the GROMOS MWR in Bern, Switzerland, satellite instruments (MLS, MIPAS, HALOE, SCHIAMACHY, GOMOS), and profiles simulated by the SOCOL v3.0 CCM. The long-term stability and mean biases of the time series were estimated as a function of the measurement time (day- and nighttime). The homogenized Payerne MWR ozone dataset agrees within ±5 % with the MLS dataset over the 30 to 65 km altitude range and within ±10 % of the HARMonized dataset of OZone profiles (HARMOZ, limb and occultation measurements from ENVISAT) over the 30 to 65 km altitude range. In the upper stratosphere, there is a large nighttime difference between Payerne MWR and other datasets, which is likely a result of the mesospheric signal aliasing with lower levels in the stratosphere due to a lower vertical resolution at that altitude. Hence, the induced bias at 55 km is considered an instrumental artifact and is not further analyzed.@en

Recent reconstructions of total solar irradiance (TSI) postulate that quiet-Sun variations could give significant changes to the solar power input to Earth's climate (radiative climate forcings of 0.7–1.1 W m−2 over 1700–2019) arising from changes in quiet-Sun magnetic fields that have not, as yet, been observed. Reconstructions without such changes yield solar forcings that are smaller by a factor of more than 10. We study the quiet-Sun TSI since 1995 for three reasons: (i) this interval shows rapid decay in average solar activity following the grand solar maximum in 1985 (such that activity in 2019 was broadly equivalent to that in 1900); (ii) there is improved consensus between TSI observations; and (iii) it contains the first modelling of TSI that is independent of the observations. Our analysis shows that the most likely upward drift in quiet-Sun radiative forcing since 1700 is between +0.07 and −0.13 W m−2. Hence, we cannot yet discriminate between the quiet-Sun TSI being enhanced or reduced during the Maunder and Dalton sunspot minima, although there is a growing consensus from the combinations of models and observations that it was slightly enhanced. We present reconstructions that add quiet-Sun TSI and its uncertainty to models that reconstruct the effects of sunspots and faculae.@en

The stratospheric ozone layer shields surface life from harmful ultraviolet radiation. Following the Montreal Protocol ban on long-lived ozone-depleting substances (ODSs), rapid depletion of total column ozone (TCO) ceased in the late 1990s, and ozone above 32 km is now clearly recovering. However, there is still no confirmation of TCO recovery, and evidence has emerged that ongoing quasi-global (60∘ S–60∘ N) lower stratospheric ozone decreases may be responsible, dominated by low latitudes (30∘ S–30∘ N). Chemistry–climate models (CCMs) used to project future changes predict that lower stratospheric ozone will decrease in the tropics by 2100 but not at mid-latitudes (30–60∘). Here, we show that CCMs display an ozone decline similar to that observed in the tropics over 1998–2016, likely driven by an increase in tropical upwelling. On the other hand, mid-latitude lower stratospheric ozone is observed to decrease, while CCMs that specify real-world historical meteorological fields instead show an increase up to present day. However, these cannot be used to simulate future changes; we demonstrate here that free-running CCMs used for projections also show increases. Despite opposing lower stratospheric ozone changes, which should induce opposite temperature trends, CCMs and observed temperature trends agree; we demonstrate that opposing model–observation stratospheric water vapour (SWV) trends, and their associated radiative effects, explain why temperature changes agree in spite of opposing ozone trends. We provide new evidence that the observed mid-latitude trends can be explained by enhanced mixing between the tropics and extratropics. We further show that the temperature trends are consistent with the observed mid-latitude ozone decrease. Together, our results suggest that large-scale circulation changes expected in the future from increased greenhouse gases (GHGs) may now already be underway but that most CCMs do not simulate mid-latitude ozone layer changes well. However, it is important to emphasise that the periods considered here are short, and internal variability that is both intrinsic to each CCM and different to observed historical variability is not well-characterised and can influence trend estimates. Nevertheless, the reason CCMs do not exhibit the observed changes needs to be identified to allow models to be improved in order to build confidence in future projections of the ozone layer.@en