Solar radiation modification (SRM) is increasingly discussed as a potential method to ameliorate some negative effects of climate change. However, unquantified uncertainties in physical and environmental impacts of SRM impede informed debate and decision making. Some uncertainties are due to lack of understanding of processes determining atmospheric effects of SRM and/or a lag in development of their representation in models, meaning even high-quality model intercomparisons will not necessarily reveal or address them. Although climate models at multiple scales are advancing in complexity, there are specific areas of uncertainty where additional model development (often requiring new observations) could significantly advance understanding of SRM's effects, and improve our ability to assess and weigh potential risks against those of choosing to not use SRM. We convene expert panels in the areas of atmospheric science most critical to understanding the three most widely discussed forms of SRM. Each identifies three key modeling gaps relevant to either stratospheric aerosols, cirrus, or low-altitude marine clouds. Within each area, key challenges remain in capturing impacts due to complex interactions in aerosol physics, atmospheric chemistry/dynamics, and aerosol-cloud interactions. Across all three, in addition to arguing for more observations, the panels argue that model development work to either leverage different capabilities of existing models, bridge scales across which relevant processes operate, or address known modeling gaps could advance understanding. By focusing on these knowledge gaps we believe the modeling community could advance understanding of SRM's physical risks and potential benefits, allowing better-informed decision-making about whether and how to use SRM.

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.

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.

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.