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.

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.