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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.

 

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. 

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. 

Open questions about the modulation of near‐surface trace gas variability by stratosphere‐troposphere tracer transport complicate efforts to identify anthropogenic sources of gases such as CFC‐11 and N₂O and disentangle them from dynamical influences. In this study, we explore one model's modulation of lower stratospheric tracer advection by the quasi‐biennial oscillation (QBO) of stratospheric equatorial zonal‐mean zonal winds at 50 hPa. We assess instances of coherent modulation versus disruption through phase unlocking with the seasonal cycle in the model and in observations. We quantify modeled advective contributions to the temporal rate of change of stratospheric CFC‐11 and N₂O at extratropical and high‐latitudes by calculating a transformed Eulerian mean (TEM) budget across isentropic surfaces from a 10‐member WACCM4 ensemble simulation. We find that positive interannual variability in seasonal tracer advection generally occurs in the easterly QBO phase, as in previous work, and briefly discuss physical mechanisms. Individual simulations of the 10‐member ensemble display phase‐unlocking disruptions from this general pattern due to seasonally varying synchronizations between the model's repeating 28‐month QBO cycle and the 12‐month seasonal cycle. We find that phase locking and unlocking patterns of tracer advection calculations inferred from observations fall within the envelope of the ensemble member results. Our study bolsters evidence for variability in the interannual stratospheric dynamical influence of CFC‐11 near‐surface concentrations by assessing the QBO modulation of lower stratospheric advection via synchronization with the annual cycle. It identifies a likely cause of variations in the QBO influence on tropospheric abundances.

 

Chemistry Climate Models (CCMs) are essential tools for characterizing and predicting the role of atmospheric composition and chemistry in Earth's climate system. This study demonstrates the use of airborne in situ observations to diagnose the representation of chemical composition and transport by CCMs. Process‐based diagnostics using dynamical and chemical coordinates are presented which minimize the spatial and temporal sampling differences between airborne in situ measurements and CCM grid points. The chosen process is the chemical impact of the Asian summer monsoon (ASM), where deep convection serves as a rapid transport pathway for surface emissions to reach the upper troposphere and lower stratosphere (UTLS). We examine two CCM configurations for their representation of the ASM UTLS using a set of airborne observations from south Asia. The diagnostics reveal good model performance at representing tropospheric tracer distribution throughout the troposphere and lower stratosphere, and excellent representation of chemical aging in the lower stratosphere when chemical loss is dominated by photolysis. Identified model limitations include the use of zonally averaged mole fraction boundary conditions for species with sufficiently short tropospheric lifetimes, which may obscure enhanced regional emissions sources. Overall, the diagnostics underscore the skill of current‐generation models at representing pollution transport from the boundary layer to the stratosphere via the ASM mechanism, and demonstrate the strength of airborne in situ observations toward characterizing this representation.

 

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.

 

The possibility of commercial and business supersonic aircraft that fly in the lower stratosphere is being discussed and specific designs are under consideration. Emissions from supersonic transports have raised crucial environmental concerns regarding ozone and climate. The atmospheric response is sensitive to a range of factors regarding aircraft types, designs, and deployment parameters. This study conducts a series of sensitivity experiments of possible future cruise altitudes to evaluate the potential atmospheric response for a fleet of supersonic aircraft assumed to be fully operational in 2050. Cruise emissions in the sensitivity studies were varied in 2 km bands over the 13–23 km altitude range. We show that the supersonic aircraft can induce both ozone increase and decrease depending on altitude primarily as a result of emissions of nitrogen oxides, and the changes in total column ozone depend on the cruise altitude. The total column ozone change is shown to have a small increase flying from 13 to 17 km, with the ozone impact not very dependent on cruise altitude. As cruise altitude transitions from 17 to 23 km, the ozone impact transitions from production to depletion and the column ozone depletion strongly depends on cruise altitude. We also explore the seasonal ozone loss, changes in ozone, and climate radiative forcing per unit of fuel burn as a function of cruise altitude. The climate impact of water vapor emissions shows a larger effect associated with higher cruise altitude, with more than 1 mW m⁻² Tg⁻¹ yr for cruise altitudes above 19 km.

 

The Hunga Tonga‐Hunga Ha'apai (HTHH) volcanic eruption in January 2022 injected unprecedented amounts of water vapor (H₂O) and a moderate amount of the aerosol precursor sulfur dioxide (SO₂) into the Southern Hemisphere (SH) tropical stratosphere. The H₂O and aerosol perturbations have persisted during 2022 and early 2023 and dispersed throughout the atmosphere. Observations show large‐scale SH stratospheric cooling, equatorward shift of the Antarctic polar vortex and slowing of the Brewer‐Dobson circulation. Satellite observations show substantial ozone reductions over SH winter midlatitudes that coincide with the largest circulation anomalies. Chemistry‐climate model simulations forced by realistic HTHH inputs of H₂O and SO₂qualitatively reproduce the observed evolution of the H₂O and aerosol plumes over the first year, and the model exhibits stratospheric cooling, circulation changes and ozone effects similar to observed behavior. The agreement demonstrates that the observed stratospheric changes are caused by the HTHH volcanic influences.

 

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.