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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. 

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.

 

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.

 

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.

 

Quantifying the width of the tropics has important implications for understanding climate variability and the atmospheric response to anthropogenic forcing. Considerable effort has been placed on quantifying the width of the tropics at tropospheric levels, but substantially less effort has been placed on quantifying the width at stratospheric levels. Here we probe tropical width in the stratosphere using chemical tracers, which are accessible by direct measurement. Two new tracer‐based width metrics are developed, denoted here as the “1σ method” and the gradient weighted latitude (GWL) method. We evaluate widths from three tracers, CH₄, N₂O, and SF₆. We demonstrate that unlike previously proposed stratospheric width methods using tracers, these metrics perform consistently throughout the depth of the stratosphere, at all times of year and on coarse temporal data. The GWL tracer‐based widths correlate well with the turnaround latitude and the critical level, where wave dissipation occurs, in the upper and midstratosphere during certain months of the year. In the lower stratosphere, the deseasonalized tracer‐based widths near the tropical tropopause correlate with the deseasonalized tropopause‐height based metrics. We also find that tracer‐tracer width correlations are strongest at pressure levels where their chemical lifetimes are similar. These metrics represent another useful way to estimate stratospheric tropical width and explore any changes under anthropogenic forcing.

 

Abstract The Whole Atmosphere Community Climate Model, version 4 (WACCM4), is used to investigate the influence of stratospheric conditions on the development of sudden stratospheric warmings (SSWs). To this end, targeted experiments are performed on selected modeled SSW events. Specifically, the model is reinitialized three weeks before a given SSW, relaxing the surface fluxes, winds, and temperature below 10 km to the corresponding fields from the free-running simulation. Hence, the tropospheric wave evolution is unaltered across the targeted experiments, but the stratosphere itself can evolve freely. The stratospheric zonal-mean state is then altered 21 days prior to the selected SSWs and rerun with an ensemble of different initial conditions. It is found that a given tropospheric evolution concomitant with the development of an SSW does not uniquely determine the occurrence of an event and that the stratospheric conditions are relevant to the subsequent evolution of the stratospheric flow toward an SSW, even for a fixed tropospheric evolution. It is also shown that interpreting the meridional heat flux at 100 hPa as a proxy of the tropospheric injection of wave activity into the stratosphere should be regarded with caution and that stratospheric dynamics critically influence the heat flux at that altitude. 

The El Niño‐driven fire season in Indonesia in September–October 2015 produced the largest fire emissions on record since NASA's EOS satellites started making observations of tropospheric pollutants from space. In this study, measurements of carbon monoxide (CO) from the Measurement of Pollution in the Troposphere (MOPITT) on Terra and the Microwave Limb Sounder are used to characterize the anomalously high CO emitted during the 2015 Indonesian fire season transported into the tropical upper troposphere and stratosphere. The satellite measurements indicate that CO emitted from wildfires was transported into the upper troposphere with time lags up to ∼2 months and continued to be transported into the stratosphere, which resulted in higher concentrations of CO extending up to ∼20 hPa by the end of 2016. Hydrogen cyanide (HCN) measured by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE‐FTS) confirms that anomalously high HCN emitted from the same wildfires was also transported into the tropical stratosphere and persisted throughout 2017. Simulations of CO from the Community Atmosphere Model with Chemistry (CAM‐chem) show a significant increase in CO concentrations in the troposphere in October 2015. However, comparisons between CAM‐chem and MOPITT CO suggest that the model underestimates the amount of CO even with doubled emissions of CO in October 2015. Both the satellite measurements and the model simulations show that the pollution emitted from the wildfires over Indonesia was transported to and persisted in the tropical stratosphere much longer than the previous El‐Niño driven fire events due to unprecedented amount of the fire emissions.