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Deep convection within the Asian summer monsoon (ASM) transports surface level air into the upper troposphere‐lower stratosphere (UTLS). This work aims to understand the distribution of NO₂, NO, and NO_xin the UTLS ASM anticyclone from satellite measurements. Observations of NO₂from the Optical Spectrograph and InfraRed Imager System, the Atmospheric Chemistry Experiment ‐ Fourier Transform Spectrometer (ACE‐FTS), and the Stratospheric Aerosol and Gas Experiment III on the International Space Station are considered. The PRATMO photochemical box model is used to quantify the NO_xphotochemistry, and to derive the NO_xconcentration using OSIRIS NO₂and O₃observations. The satellite data show a relative minimum in NO₂over the ASM in the summer months, while the corresponding NO and NO_xanomalies are elevated, mainly due to low O₃and cold temperatures within the ASM. The observations within the ASM show reasonable agreement to simulations from the Whole Atmosphere Community Climate Model.

 

Massive Australian wildfires lofted smoke directly into the stratosphere in the austral summer of 2019/20. The smoke led to increases in optical extinction throughout the midlatitudes of the southern hemisphere that rivalled substantial volcanic perturbations. Previous studies have assumed that the smoke became coated with sulfuric acid and water and would deplete the ozone layer through heterogeneous chemistry on those surfaces, as is routinely observed following volcanic enhancements of the stratospheric sulfate layer. Here, observations of extinction and reactive nitrogen species from multiple independent satellites that sampled the smoke region are compared to one another and to model calculations. The data display a strong decrease in reactive nitrogen concentrations with increased aerosol extinction in the stratosphere, which is a known fingerprint for key heterogeneous chemistry on sulfate/H 2 O particles (specifically the hydrolysis of N 2 O 5 to form HNO 3 ). This chemical shift affects not only reactive nitrogen but also chlorine and reactive hydrogen species and is expected to cause midlatitude ozone layer depletion. Comparison of the model ozone to observations suggests that N 2 O 5 hydrolysis contributed to reduced ozone, but additional chemical and/or dynamical processes are also important. These findings suggest that if wildfire smoke injection into the stratosphere increases sufficiently in frequency and magnitude as the world warms due to climate change, ozone recovery under the Montreal Protocol could be impeded, at least sporadically. Modeled austral midlatitude total ozone loss was about 1% in March 2020, which is significant compared to expected ozone recovery of about 1% per decade. 

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.

 

Abstract. Smoke from wildfires is a significant source of air pollution, which can adversely impact air quality and ecosystems downwind. With the recently increasing intensity and severity of wildfires, the threat to air quality is expected to increase. Satellite-derived biomass burning emissions can fill in gaps in the absence of aircraft or ground-based measurement campaigns and can help improve the online calculation of biomass burning emissions as well as the biomass burning emissions inventories that feed air quality models. This study focuses on satellite-derived NOx emissions using the high-spatial-resolution TROPOspheric Monitoring Instrument (TROPOMI) NO2 dataset. Advancements and improvements to the satellite-based determination of forest fire NOx emissions are discussed, including information on plume height and effects of aerosol scattering and absorption on the satellite-retrieved vertical column densities. Two common top-down emission estimation methods, (1) an exponentially modified Gaussian (EMG) and (2) a flux method, are applied to synthetic data to determine the accuracy and the sensitivity to different parameters, including wind fields, satellite sampling, noise, lifetime, and plume spread. These tests show that emissions can be accurately estimated from single TROPOMI overpasses.The effect of smoke aerosols on TROPOMI NO2 columns (via air mass factors, AMFs) is estimated, and these satellite columns and emission estimates are compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America. Our results indicate that applying an explicit aerosol correction to the TROPOMI NO2 columns improves the agreement with the aircraft observations (by about 10 %–25 %). The aircraft- and satellite-derived emissions are in good agreement within the uncertainties. Both top-down emissions methods work well; however, the EMG method seems to output more consistent results and has better agreement with the aircraft-derived emissions. Assuming a Gaussian plume shape for various biomass burning plumes, we estimate an average NOx e-folding time of 2 ±1 h from TROPOMI observations. Based on chemistry transport model simulations and aircraft observations, the net emissions of NOx are 1.3 to 1.5 times greater than the satellite-derived NO2 emissions. A correction factor of 1.3 to 1.5 should thus be used to infer net NOx emissions from the satellite retrievals of NO2. 

Decreases in stratospheric NO_xassociated with enhanced aerosol have been observed after large volcanic eruptions, for example, after the eruption of Mount Pinatubo in 1991. While the 1991 Mount Pinatubo eruption was the last large explosive eruption, recent studies have shed light on the impacts of moderate‐sized eruptions since the year 2000 on the global stratospheric aerosol budget. We use an ensemble of simulations from a coupled climate‐chemistry model to quantify and analyze changes in NO and NO₂(NO_x), N₂O₅, HNO₃, ClO, and ClONO₂during periods of increased stratospheric volcanic aerosol concentrations since 2000. By using an ensemble approach, we are able to distinguish forced responses from internal variability. We also compare the model ensemble results to satellite measurements of these changes in atmospheric composition, including measurements from the Optical Spectrograph and Infrared Imaging Spectrometer on the Odin satellite and the Aura Microwave Limb Sounder. We find decreases in stratospheric NO_xconcentrations up to 20 hPa, consistent with increases in stratospheric HNO₃concentrations. The HNO₃perturbations also extend higher, up to 5 hPa, associated with periods of increased volcanic aerosol concentrations in both model simulations and observations, though correlations with volcanic aerosol are considerably higher in the model simulations. The model simulates increases in ClO at altitudes and magnitudes similar to the NO_xreductions, but this response is below the detectable limit in the available observations (100 pptv). We also demonstrate the value of accounting for transport‐related anomalies of atmospheric trace gases by regression onto N₂O anomalies.