Chemistry transport models (CTMs) 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 atmospheric composition by global CTMs. Process-based diagnostics are developed which minimize the spatial and temporal sampling differences between airborne in situ measurements and CTM grid points. The developed diagnostics make use of dynamical and chemical vertical coordinates as a means of highlighting areas where focused model improvement is needed. The chosen process is the chemical impact of the Asian summer monsoon (ASM), where deep convection serves a unique pathway for rapid transport of surface emissions and pollutants to the stratosphere. Two global CTM configurations are examined for their representation of the ASM upper troposphere and lower stratosphere (UTLS), using airborne observations collected over south Asia. Application of the developed diagnostics to the CTMs reveals the limitations of zonally-averaged surface boundary conditions for species with sufficiently short tropospheric lifetimes, and that species whose stratospheric loss rates are dominated by photolysis have excellent agreement compared to that observed. Overall, the diagnostics demonstrate the strength of airborne observations toward improving model predictions, and highlight the utility of highly-resolved CTMs to improve the understanding of reactive transport of anthropogenic pollutants to the stratosphere.

The Hunga Tonga Hunga-Ha’apai (HTHH) volcanic eruption on 15 January 2022 injected water vapor and SO2 into the stratosphere. Several months after the eruption, significantly stronger westerlies, and a weaker Brewer-Dobson circulation developed in the stratosphere of the Southern Hemisphere and were accompanied by unprecedented temperature anomalies in the stratosphere and mesosphere. In August 2022 the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) satellite instrument observed record-breaking temperature anomalies in the stratosphere and mesosphere that alternate signs with altitude. Ensemble simulations carried out with the Whole Atmosphere Community Climate Model (WACCM6) indicate that the strengthening of the stratospheric westerlies explains the mesospheric temperature changes. The stronger westerlies cause stronger westward gravity wave drag in the mesosphere, accelerating the mesospheric mean meridional circulation. The stronger mesospheric circulation, in turn, plays a dominant role in driving the changes in mesospheric temperatures. This study highlights the impact of large volcanic eruptions on middle atmospheric dynamics and provides insight into their long-term effects in the mesosphere. On the other hand, we could not discern a clear mechanism for the observed changes in stratospheric circulation. In fact, an examination of the WACCM ensemble reveals that not every member reproduces the large changes observed by SABER. We conclude that there is a stochastic component to the stratospheric response to the HTHH eruption.

The impacts of Stratospheric Aerosol Injection (SAI) on the atmosphere and surface climate depend on when and where the sulfate aerosol precursors are injected, as well as on how much surface cooling is to be achieved. We use a set of CESM2(WACCM6) SAI simulations achieving three different levels of global mean surface cooling and demonstrate that unlike some direct surface climate impacts driven by the reflection of solar radiation by sulfate aerosols, the SAI-induced changes in the high latitude circulation and ozone are more complex and could be non-linear. This manifests in our simulations by disproportionally larger Antarctic springtime ozone loss, significantly larger intra-ensemble spread of the Arctic stratospheric jet and ozone responses, and non-linear impacts on the extratropical modes of surface climate variability under the strongest-cooling SAI scenario compared to the weakest one. These potential non-linearities may add to uncertainties in projections of regional surface impacts under SAI.

Following the Hunga Tonga–Hunga Ha’apai (HTHH) eruption in January 2022, stratospheric ozone depletion was observed in the Southern Hemisphere mid-latitudes and Antarctica during the 2022 austral wintertime and springtime. This eruption injected sulfur dioxide and unprecedented amounts of water vapor into the stratosphere. This work examines and quantifies the chemistry contribution of the volcanic materials to the ozone depletion using chemistry-climate model simulations with nudged meteorology. Simulated 2022 ozone and nitrogen oxides (NOx) anomalies show a good agreement with satellite observations. We find that chemistry only contributes up to 6% and 20% ozone destruction at mid-latitudes wintertime and Antarctic springtime respectively. The majority of the ozone depletion is attributed to the internal variability and dynamical changes forced by the eruption. Both the simulation and observations show a significant NOx reduction associated with the HTHH aerosol plume, indicating the enhanced dinitrogen pentoxide hydrolysis on sulfate aerosol.

Simulating whole atmosphere dynamics, chemistry, and physics is computationally expensive. It can require high vertical resolution throughout the middle and upper atmosphere, as well as a comprehensive chemistry and aerosol scheme coupled to radiation physics. An unintentional outcome of the development of one of the most sophisticated and hence computationally expensive model configurations is that it often excludes a broad community of users with limited computational resources. Here, we analyze two configurations of the Community Earth System Model Version 2, Whole Atmosphere Community Climate Model Version 6 (CESM2(WACCM6)) with simplified “middle atmosphere” chemistry at nominal 1 and 2 degree horizontal resolutions. Using observations, a reanalysis, and direct model comparisons, we find that these configurations generally reproduce the climate, variability, and climate sensitivity of the 1 degree nominal horizontal resolution configuration with comprehensive chemistry. While the background stratospheric aerosol optical depth is elevated in the middle atmosphere configurations as compared to the comprehensive chemistry configuration, it is comparable between all configurations during volcanic eruptions. For any purposes other than those needing an accurate representation of tropospheric organic chemistry and secondary organic aerosols, these simplified chemistry configurations deliver reliable simulations of the whole atmosphere that require 35% to 86% fewer computational resources at nominal 1 and 2 degree horizontal resolution, respectively.

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.

The mechanisms underlying decadal variability in Arctic sea ice remain actively debated. Here we show that variability in boreal biomass burning (BB) emissions strongly influences simulated Arctic sea ice on multi-decadal timescales. In particular, we find that a strong acceleration in sea ice decline in the early 21st century in the Community Earth System Model version 2 (CESM2) is related to increased variability in prescribed CMIP6 BB emissions through summertime aerosol-cloud interactions. Furthermore, we find that more than half of the reported improvement in sea ice sensitivity to CO2 emissions and global warming from CMIP5 to CMIP6 can be attributed to the increased BB variability, at least in the CESM. These results highlight a new kind of uncertainty that needs to be considered when incorporating new observational data into model forcing, while also raising questions about the role of BB emissions on the observed Arctic sea ice loss.

Modeling atmospheric chemistry across scales with the Multi-Scale Infrastructure for Chemistry and Aerosols (MUSICA) leverages a new regional refinement capability within the NCAR Community Earth System Model (CESM). This framework allows for simultaneous simulation at human-relevant and policy-relevant scales at the same time as hemispheric and global-scales. Here, we present the development of a regional refined grid over the Australian region and assess initial simulations for the 2019/2020 wildfire season. The Australian wildfire events of 2019/2020 saw large local emissions of pollution with wide-scale impacts across the southeast of the continent, where smoke and haze degraded air quality for many days for millions of people. Hemispheric transport of pollution at low and lofted altitudes also occurred, creating an atmospheric signature over New Zealand and South America, and had a direct influence on climate. These multiple-scale impacts from wildfire in the Australian region make it ideal for testing the new capability of multi-scale modeling.

Stratospheric Aerosol Geoengineering (SAG) is proposed to offset global warming; the use of this approach can impact the hydrological cycle. We use simulations from Coupled Model Intercomparison Project (CMIP5) and Geoengineering Model Intercomparison Project (G3 simulation) to analyze the impacts of SAG on precipitation (P) and to determine its responsible causes in West Africa and Sahel region. CMIP5 Historical data are firstly validated, the results obtained are consistent with those of observations data (CMAP and GPCP). Under the Representative Concentration Pathway (RCP) scenario RCP4.5, a slight increase is found in West Africa Region (WAR) relative to present-day climate. The dynamic processes especially the monsoon shifts are responsible for this change of precipitation. Under RCP4.5, during the monsoon period, reductions in P are 0.86%, 0.80% related to the present-day climate in the Northern Sahel (NSA), Southern Sahel (SSA) respectively while P is increased by 1.04% in WAR. Under SAG, 3.71% of P change (decrease) was associated with a -3.51 value of efficacy in the West African Region (AR). Under G3, a significant decrease of P is found in the West African region. This decrease in monsoon precipitation is mainly explained by changes in dynamics, which leads to weakened monsoon circulation and a shift in the distribution of monsoon precipitation. This result suggests that SAG deployment to balancing all warming can be harmful to rainfall in WAR if the amount of SO2 to be injected in this tropical area is not taken into consideration.

Using the CAM-chem Model, we simulate the response of chemical species in the free troposphere to changes in emissions of primary pollutants during the COVID-19 pandemic. Zonally averaged ozone concentrations in the free troposphere during Northern Hemisphere spring and summer were 5 to 15 % lower than 19-year climatological values, in good quantitative agreement with ozone observations. About one third of this anomaly is attributed to the drastic reduction in air traffic during the pandemic, another third to reductions in surface emissions, the remainder to 2020 meteorological conditions, including the exceptional springtime Arctic stratospheric ozone depletion. The overall COVID-19 reduction in mean northern hemisphere tropospheric ozone in June is less than 5 ppb below 400 hPa, but reaches 8 ppb at 250 hPa. In the Southern Hemisphere, COVID-19 related ozone reductions by 4 to 6% were masked by comparable ozone increases due to other changes in 2020.

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.

We use the global Community Earth System Model to investigate the response of secondary pollutants (ozone O3, secondary organic aerosols SOA) in different parts of the world in response to modified emissions of primary pollutants during the COVID-19 pandemic. We quantify the respective effects of the reductions in NOx and in VOC emissions, which, in most cases, affect oxidants in opposite ways. Using model simulations, we show that the level of NOx has been reduced by typically 40 % in China during February 2020 and by similar amounts in many areas of Europe and North America in mid-March to mid-April 2020, in good agreement with space and surface observations. We show that, relative to a situation in which the emission reductions are ignored and despite the calculated increase in hydroxyl and peroxy radicals, the ozone concentration increased only in a few NOx-saturated regions (northern China, northern Europe and the US) during the winter months of the pandemic when the titration of this molecule by NOx was reduced. In other regions, where ozone is NOx-controlled, the concentration of ozone decreased. SOA concentrations decrease in response to the concurrent reduction in the NOx and VOC emissions. The model also shows that atmospheric meteorological anomalies produced substantial variations in the concentrations of chemical species during the pandemic. In Europe, for example, a large fraction of the ozone increase in February 2020 was associated with meteorological anomalies, while in the North China Plain, enhanced ozone concentrations resulted primarily from reduced emissions of primary pollutants.