The Hunga Tonga-Hunga Ha’apai (HTHH) volcanic eruption in January 2022 injected extreme amounts of water vapor (H2O) and a moderate amount of the aerosol precursor (SO2) into the Southern Hemisphere (SH) stratosphere. The H2O and aerosol perturbations have persisted and resulted in large-scale SH stratospheric cooling, equatorward shift of the Antarctic polar vortex, and slowing of the Brewer-Dobson circulation associated with a substantial ozone reduction in the SH winter midlatitudes. Chemistry-climate model simulations forced by realistic HTHH inputs of H2O and SO2 reproduce the observed stratospheric cooling and circulation effects, demonstrating the observed behavior is due to the volcanic influences. Furthermore, the combination of aerosol transport to polar latitudes and a cold polar vortex enhances springtime Antarctic ozone loss, consistent with observed polar ozone behavior in 2022.

Fire emissions are an important component of global models, which help to understand the influence of sources, transport and chemistry on atmospheric composition. Global fire emission inventories can vary substantially due to the assumptions made in the emission creation process, including the defined vegetation type, fire detection, fuel loading, fraction of vegetation burned and emissions factors. Here, we focus on the uncertainty in emission factors and the resulting impact on modeled composition. Our study uses the Community Atmosphere Model with chemistry (CAM-chem) to model atmospheric composition for 2014, a year chosen for the relatively quiet El Niño Southern Oscillation activity. We focus on carbon monoxide (CO), a trace gas emitted from incomplete combustion and also produced from secondary oxidation of volatile organic compounds (VOCs). Fire is a major source of atmospheric CO and VOCs. Modeled CO from four fire emission inventories (CMIP6/GFED4s, QFED2.5, GFAS1.2 and FINN1.5) are compared after being implemented in CAM-chem. Multiple sensitivity tests are performed based on CO and VOC emission factor uncertainties. We compare model output in the 14 basis regions defined by the Global Fire Emissions Database (GFED) team and evaluate against CO observations from the Measurements of Pollution in the Troposphere (MOPITT) satellite-based instrument. For some regions, emission factor uncertainty spans the results found by using different inventories. Finally, we use modeled ozone (O3) to briefly investigate how emission factor uncertainty influences the atmospheric oxidative environment. Overall, accounting for emission factor uncertainty when modeling atmospheric chemistry can lend a range of uncertainty to simulated results.

Water vapor in the stratosphere is primarily controlled by temperatures in the tropical upper troposphere and lower stratosphere. However, the direct impact of deep convection on the global lower stratospheric water vapor budget is still an actively debated issue. Two complementary modeling approaches are used to investigate the convective impact in boreal winter and summer. Backward trajectory model simulations coupled with a detailed treatment of cloud microphysical processes indicate that convection moistens the global lower stratosphere by approximately 0.3 ppmv (~10% increase) in boreal winter and summer 2010. The diurnal peak in convection is responsible for about half of the total convective moistening during boreal winter and nearly all of the convective moistening during boreal summer. Deep convective cloud tops overshooting the local tropopause have relatively minor effect on global lower stratospheric water vapor (~1% increase). A forward trajectory model coupled with a simplified cloud module is used to esimate the relative magnitude of the interannual variability of the convective impact during 2006-2016. Combing the results from the two models, we find that the convective impact on the global lower stratospheric water vapor during 2006-2016 is approximately 0.3 ppmv with year-to-year variations of up to 0.1 ppmv. The dominant mechanism of convective hydration of the lower stratosphere is via the detrainment of saturated air and ice into the tropical uppermost troposphere. Convection shifts the relative humidity distribution of subsaturated air parcels in the upper troposphere toward higher relative humidity values, thereby increasing the water vapor in the stratosphere.

Atmospheric carbon monoxide (CO) has been decreasing globally for the last two decades. Recently, positive fire trends in Northern Hemisphere boreal regions may have impacted the decreasing CO. Additionally, time-varying air quality policies will have different impacts on atmospheric composition and related trends. Aerosols are co-emitted with CO from both fires and anthropogenic sources. Consequently, a combined trend analysis of CO and aerosol optical depth (AOD) measurements from space can help elucidate the drivers of regional differences in the CO trend. We use valuable long-term records from two instruments aboard the Terra satellite. Measurements of Pollution in the Troposphere (MOPITT) CO and AOD from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument are examined hemispherically and in sub-regions to determine trends between 2002 and 2018. The records are further split into two sub-periods in order to examine temporal stability in the trend values. We also assess the CO trends in monthly percentile values to use seasonal information when interpreting trend contributions. Our focus is on four major population centers: Southeast USA, Europe, Northeast China and North India, as well as biomass burning regions in both hemispheres. Our results show that globally, CO declines faster in the first half of the record compared to the second half. Both atmospheric species are important when interpreting trends in the smaller regions. Northern Hemisphere boreal fire regions show a regime-shift in their seasonality for both CO and AOD, which may counteract the downward trend in CO. Anthropogenic regions with minimal air quality management such as North India become more globally relevant as the global CO trend weakens. We also find clear evidence of the atmospheric impact of policy choices. Overall, we observe that local changes in biomass burning and air quality can counteract the global downward trend in CO.

Since June 2017, the Stratospheric Aerosol and Gas Experiment III instrument on the International Space Station (SAGE III/ISS) has been providing vertical profiles of upper tropospheric to stratospheric water vapor (WV) retrieved from solar occultation transmission measurements. The goal of this paper is to evaluate the publicly released SAGE III/ISS beta version 5.1 WV retrieval through intercomparison with independent satellite- and balloon-based measurements, and to present recommendations for SAGE III/ISS data quality screening criteria. Overall, we find that SAGE III/ISS provides high quality water vapor measurements. Low quality profiles are predominately due to retrieval instabilities in the upper stratosphere that cause step-like changes in the profile, and aerosol/cloud-related interferences (below ~20 km). Above 35 km, the retrieved uncertainty and noise in the data rapidly grow with increasing altitude due to relatively low extinction signal from water vapor. Below the tropopause, retrieved uncertainty increases with decreasing altitude due to enhanced molecular scattering and aerosol extinction. After screening low-quality data using the procedures described herein, SAGE III/ISS WV is shown to be in good agreement with independent satellite and balloon-based measurements. From 20 – 40 km, SAGE III/ISS WV v5.1 data exhibit a bias of 0.0 to -0.5 ppmv (~10 %) relative to the independent data, depending on the instrument and altitude. Despite its status as a beta version, the level of SAGE III/ISS WV agreement with independent data is similar to previous SAGE instruments, and therefore the data are suitable for scientific studies of stratospheric water vapor.

Changes in aerosol optical depth, both positive and negative, are observed across the globe during the 21rst Century. However, attribution of these changes to specific sources is largely uncertain as there are multiple contributing natural and anthropogenic sources that produce aerosols either directly or through secondary chemical reactions. Here we show that satellite-based changes in small-mode AOD between 2002 and 2019 observed in data from MISR can primarily be explained by changes, either directly or indirectly, in combustion emissions. We quantify combustion emissions using MOPITT total column CO observations and the adjoint of the GEOS-Chem global chemistry and transport model. The a priori fire emissions are taken from the Global Fire Emission Data base with small fires (GFED4s) but with fixed a priori for non-fire emissions. Aerosol precursor and direct emissions are updated by re-scaling them with the monthly ratio of the CO posterior to prior emissions. The correlation between modeled and observed AOD improves from a mean of 0.15 to 0.81 for the four industrial regions considered and from 0.52 to 0.75 for the four wildfire-dominant regions considered. Using these updated emissions in the GEOS-Chem global chemistry transport model, our results indicate that surface PM2.5 have declined across many regions of the globe during the 21rst century. For example, PM2.5 over China has declined by ~30% with smaller fractional declines in E. USA and Europe (from fossil emissions) and in S. America (from fires). These results highlight the importance of forest management and cleaner combustion sources in improving air-quality.

Wildfire emissions can vary substantially between different inventories due to the assumptions made in the emission creation process, including the defined vegetation type, fire detection, fuel loading, fraction of vegetation burned and emissions factors. Here, we focus on the uncertainty in emission factors and the resulting impact on modeled composition. We use the Community Atmosphere Model with chemistry (CAM-chem) to simulate 2014 atmospheric composition and focus on carbon monoxide (CO), a trace gas emitted from incomplete combustion and also produced from secondary oxidation of volatile organic compounds (VOCs). Fire is a major source of atmospheric CO and VOCs. Multiple simulations are compared, from an ensemble using four fire emission inventories (CMIP6/GFED4s, QFED2.5, GFAS1.2 and FINN1.5) and a range of sensitivity tests based on CO and VOC emission factor uncertainties. We compare model output and evaluate against CO observations from the Measurements of Pollution in the Troposphere (MOPITT) satellite-based instrument. For some regions, emission factor uncertainty spans the results found by using different inventories. Finally, we use modeled ozone (O3) to investigate how emission factor uncertainty influences the atmospheric oxidative environment. Overall, accounting for emission factor uncertainty lends a range of uncertainty to simulated results.