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The Antarctic ozone “hole” was discovered in 1985, and man-made ozone- depleting substances (ODS) are its primary cause. Following reductions of ODSs under the Montreal Protocol, signs of ozone recovery have been reported, based largely on observations and broad yet compelling model-data comparisons. While such approaches are highly valuable, they don't provide rigorous statistical detection of the temporal and spatial structure of Antarctic ozone recovery in the presence of internal climate variability. Here, we apply pattern-based detection and attribution methods as employed in climate change studies to separate anthropogenically forced ozone responses from internal variability, relying on trend pattern information as a function of month and height. The analysis uses satellite observations together with single-model and multi-model ensemble simulations to identify and quantify the month-height Antarctic ozone recovery “fingerprint”. We demonstrate that the data and simulations show remarkable agreement in the fingerprint pattern of the ozone response to decreasing ODSs since 2005. We also show that ODS forcing has enhanced ozone internal variability during the austral spring, influencing detection of forced responses and their time of emergence. Our results provide robust statistical and physical evidence that actions taken under the Montreal Protocol to reduce ODSs are indeed resulting in the beginning of Antarctic ozone recovery, defined as increases in ozone consistent with expected month-height patterns. 

Abstract. We analyze tropical ozone (O3) and carbon monoxide (CO) distributions in the upper troposphere (UT) for 2005–2020 using Aura Microwave Limb Sounder (MLS) observations and simulations from the Whole Atmosphere Community Climate Model (WACCM) and two variants of the Community Atmosphere Model with Chemistry (CAM-chem), with each variant using different anthropogenic CO emissions. Trends and variability diagnostics are obtained from multiple linear regression. The MLS zonal mean O3 UT trend for 20° S–20° N is +0.39 ± 0.28 % yr−1; the WACCM and CAM-chem simulations yield similar trends, although the WACCM result is somewhat smaller. Our analyses of gridded MLS data yield positive O3 trends (up to 1.4 % yr−1) over Indonesia and east of that region, as well as over Africa and the Atlantic. These positive mapped O3 trends are generally captured by the simulations but in a more muted way. We find broad similarities (and some differences) between mapped MLS UT O3 trends and corresponding mapped trends of tropospheric column ozone. The MLS zonal mean CO UT trend for 20° S–20° N is −0.25 ± 0.30 % yr−1, while the corresponding CAM-chem trend is 0.0 ± 0.14 % yr−1 when anthropogenic emissions are taken from the Community Emissions Data System (CEDS) version 2. The CAM-chem simulation driven by CAMS-GLOB-ANTv5 emissions yields a tropical mean CO UT trend of 0.22 ± 0.19 % yr−1, in contrast to the slightly negative MLS CO trend. Previously published analyses of total column CO data have shown negative trends. Our tropical composition trend results contribute to continuing international assessments of tropospheric evolution. 

Abstract. Polar stratospheric clouds (PSCs) play a key role in the polar chemistry of the stratosphere. Nitric acid trihydrate (NAT) particles have been shown to lead to denitrification of the lower stratosphere. While the existence of large NAT particles (NAT “rocks”) has been verified by many measurements, especially in the Northern Hemisphere (NH), most current chemistry–climate models use simplified parameterizations, often based on evaluations in the Southern Hemisphere where the polar vortex is stable enough that accounting for NAT rocks is not as important as in the NH. Here, we evaluate the probability density functions of various gaseous species in the polar vortex using one such model, the Whole Atmosphere Community Climate Model (WACCM), and compare these with measurements by the Michelson Interferometer for Passive Atmospheric Sounding onboard the Environmental Satellite (MIPAS/Envisat) and two ozonesonde stations for a range of years and in both hemispheres. Using the maximum difference between the distributions of MIPAS and WACCM as a measure of coherence, we find better agreement for HNO3 when reducing the NAT number density from the standard value of 10−2 used in this model to 5×10-4 cm−3 for almost all spring seasons during the MIPAS period in both hemispheres. The distributions of ClONO2 and O3 are not greatly affected by the NAT density. The average difference between WACCM and ozonesondes supports the need to reduce the NAT number density in the model. Therefore, this study suggests using a NAT number density of 5×10-4 cm−3 for future simulations with WACCM. 

Abstract Chlorinated very short‐lived substances (Cl‐VSLS) are ubiquitous in the troposphere and can contribute to the stratospheric chlorine budget. In this study, we present measurements of atmospheric dichloromethane (CH₂Cl₂), tetrachloroethene (C₂Cl₄), chloroform (CHCl₃), and 1,2‐dichloroethane (1,2‐DCA) obtained during the National Aeronautics and Space Administration (NASA) Atmospheric Tomography (ATom) global‐scale aircraft mission (2016–2018), and use the Community Earth System Model (CESM) updated with recent chlorine chemistry to further investigate their global tropospheric distribution. The measured global average Cl‐VSLS mixing ratios, from 0.2 to 13 km altitude, were 46.6 ppt (CH₂Cl₂), 9.6 ppt (CHCl₃), 7.8 ppt (1,2‐DCA), and 0.84 ppt (C₂Cl₄) measured by the NSF NCAR Trace Organic Analyzer (TOGA) during ATom. Both measurements and model show distinct hemispheric gradients with the mean measured Northern to Southern Hemisphere (NH/SH) ratio of 2 or greater for all four Cl‐VSLS. In addition, the TOGA profiles over the NH mid‐latitudes showed general enhancements in the Pacific basin compared to the Atlantic basin, with up to ∼18 ppt difference for CH₂Cl₂in the mid troposphere. We tagged regional source emissions of CH₂Cl₂and C₂Cl₄in the model and found that Asian emissions dominate the global distributions of these species both at the surface (950 hPa) and at high altitudes (150 hPa). Overall, our results confirm relatively high mixing ratios of Cl‐VSLS in the UTLS region and show that the CESM model does a reasonable job of simulating their global abundance but we also note the uncertainties with Cl‐VSLS emissions and active chlorine sources in the model. These findings will be used to validate future emission inventories and to investigate the fast convective transport of Cl‐VSLS to the UTLS region and their impact on stratospheric ozone. 

Deep convection in the Asian summer monsoon is a significant transport process for lifting pollutants from the planetary boundary layer to the tropopause level. This process enables efficient injection into the stratosphere of reactive species such as chlorinated very short-lived substances (Cl-VSLSs) that deplete ozone. Past studies of convective transport associated with the Asian summer monsoon have focused mostly on the south Asian summer monsoon. Airborne observations reported in this work identify the East Asian summer monsoon convection as an effective transport pathway that carried record-breaking levels of ozone-depleting Cl-VSLSs (mean organic chlorine from these VSLSs ~500 ppt) to the base of the stratosphere. These unique observations show total organic chlorine from VSLSs in the lower stratosphere over the Asian monsoon tropopause to be more than twice that previously reported over the tropical tropopause. Considering the recently observed increase in Cl-VSLS emissions and the ongoing strengthening of the East Asian summer monsoon under global warming, our results highlight that a reevaluation of the contribution of Cl-VSLS injection via the Asian monsoon to the total stratospheric chlorine budget is warranted. 

The catalytic depletion of Antarctic stratospheric ozone is linked to anthropogenic emissions of chlorine and bromine. Despite its larger ozone-depleting efficiency, the contribution of ocean-emitted iodine to ozone hole chemistry has not been evaluated, due to the negligible iodine levels previously reported to reach the stratosphere. Based on the recently observed range (0.77 ± 0.1 parts per trillion by volume [pptv]) of stratospheric iodine injection, we use the Whole Atmosphere Community Climate Model to assess the role of iodine in the formation and recent past evolution of the Antarctic ozone hole. Our 1980–2015 simulations indicate that iodine can significantly impact the lower part of the Antarctic ozone hole, contributing, on average, 10% of the lower stratospheric ozone loss during spring (up to 4.2% of the total stratospheric column). We find that the inclusion of iodine advances the beginning and delays the closure stages of the ozone hole by 3 d to 5 d, increasing its area and mass deficit by 11% and 20%, respectively. Despite being present in much smaller amounts, and due to faster gas-phase photochemical reactivation, iodine can dominate (∼73%) the halogen-mediated lower stratospheric ozone loss during summer and early fall, when the heterogeneous reactivation of inorganic chlorine and bromine reservoirs is reduced. The stratospheric ozone destruction caused by 0.77 pptv of iodine over Antarctica is equivalent to that of 3.1 (4.6) pptv of biogenic very short-lived bromocarbons during spring (rest of sunlit period). The relative contribution of iodine to future stratospheric ozone loss is likely to increase as anthropogenic chlorine and bromine emissions decline following the Montreal Protocol. 

Abstract Wave‐induced adiabatic mixing in the winter midlatitudes is one of the key processes impacting stratospheric transport. Understanding its strength and structure is vital to understanding the distribution of trace gases and their modulation under a changing climate. Age‐of‐air is often used to understand stratospheric transport, and this study proposes refinements to the vertical age gradient theory of Linz et al. (2021),https://doi.org/10.1029/2021JD035199. The theory assumes exchange of air between a well‐mixed tropics and a well‐mixed extratropics, separated by a transport barrier, quantifying the adiabatic mixing flux across the interface using age‐based measures. These assumptions are re‐evaluated and a refined framework that includes the effects of meridional tracer gradients is established to quantify the mixing flux. This is achieved, in part, by computing a circulation streamfunction in age‐potential temperature coordinates to generate a complete distribution of parcel ages being mixed in the midlatitudes. The streamfunction quantifies the “true” age of parcels mixed between the tropics and the extratropics. Applying the revised theory to an idealized and a comprehensive climate model reveals that ignoring the meridional gradients in age leads to an underestimation of the wave‐driven mixing flux. Stronger, and qualitatively similar fluxes are obtained in both models, especially in the lower‐to‐middle stratosphere. While the meridional span of adiabatic mixing in the two models exhibits some differences, they show that the deep tropical pipe, that is, latitudes equatorward of 15° barely mix with older midlatitude air. The novel age‐potential temperature circulation can be used to quantify additional aspects of stratospheric transport. 

Abstract As the leading mode of Pacific variability, El Niño–Southern Oscillation (ENSO) causes vast and widespread climatic impacts, including in the stratosphere. Following discovery of a stratospheric pathway of ENSO to the Northern Hemisphere surface, here we aim to investigate if there is a substantial Southern Hemisphere (SH) stratospheric pathway in relation to austral winter ENSO events. Large stratospheric anomalies connected to ENSO occur on average at high SH latitudes as early as August, peaking at around 10 hPa. An overall colder austral spring Antarctic stratosphere is generally associated with the warm phase of the ENSO cycle, and vice versa. This behavior is robust among reanalysis and six separate model ensembles encompassing two different model frameworks. A stratospheric pathway is identified by separating ENSO events that exhibit a stratospheric anomaly from those that do not and comparing to stratospheric extremes that occur during neutral ENSO years. The tropospheric eddy-driven jet response to the stratospheric ENSO pathway is the most robust in the spring following a La Niña, but extends into summer, and is more zonally symmetric compared to the tropospheric ENSO teleconnection. The magnitude of the stratospheric pathway is weaker compared to the tropospheric pathway and therefore, when it is present, has a secondary role. For context, the magnitude is approximately half that of the eddy-driven jet modulation due to austral spring ozone depletion in the model simulations. This work establishes that the stratospheric circulation acts as an intermediary in coupling ENSO variability to variations in the austral spring and summer tropospheric circulation. 

Abstract The forecast potential of springtime ozone on April surface temperatures at particular locations in the Northern Hemisphere has been previously reported. Evidence suggests that early springtime Arctic stratospheric ozone acts as a proxy for extreme events in the winter polar vortex. Here, using a state‐of‐the‐art chemistry‐climate model, reanalysis and observations, we extend the forecast potential of ozone on surface temperatures to aspects of the Northern Hemisphere cryosphere. Sea ice fraction and sea ice extent differences between years of March high and low Arctic stratospheric ozone extremes show excellent agreement between an ensemble of chemistry‐climate model simulations and observations, with differences occurring not just in April but extending through to the following winter season in some locations. Large snow depth differences are also obtained in regional locations in Russia and along the southeast coast of Alaska. These differences remain elevated until early summer, when snow cover diminishes. Using a conditional empirical model in a leave‐three‐out cross validation method, March total column ozone is able to accurately predict the sign of the observed sea ice extent and snow depth anomalies over 70% of the time during an ozone extreme year, especially in the region of the Bering strait and the Greenland Sea, which could be useful for shipping routes and for testing climate models.