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Model intercomparison studies often report a large spread in simulation results, but quantifying the causes of these differences is hindered by the fact that several processes contribute to the model spread simultaneously. Here we use the Multi‐Scale Infrastructure for Chemistry and Aerosols (MUSICA) version 0 to investigate the model resolution dependencies of simulated chemical species, with a focus on the differences between global uniform grid and regional refinement grid simulations with the same modeling framework. We construct two global (ne30 [∼112 km] and ne60 [∼56 km]) and two regional refinement grids over Korea (ne30x8 [∼14 km] and ne30x16 [∼7 km]). The grid resolution can change chemical concentrations by an order of magnitude in the boundary layer, and the importance increases as the species' reactivity increases (e.g., up to 50% and 1,000% changes for ethane and xylenes, respectively). The diurnal cycle of oxidants (OH, O3, and NO3) also varies with the grid resolution, which leads to different oxidation pathways of volatile organic compounds (e.g., the fraction of monoterpenes reacting with NO3 in Seoul around midnight is 90% for ne30, but 65% for ne30x16). The models with high‐resolution grids usually do a better job at reproducing aircraft observations during the KORUS‐AQ campaign, but not always, implying compensating errors in the coarse grid simulations. For example, ozone is better reproduced by the coarse grid due to the artificial mixing of NOx. When developing new chemical mechanisms and evaluating models over urban areas, the uncertainties associated with model resolution should be considered. Plain Language Summary: A new model framework, the Multi‐Scale Infrastructure for Chemistry and Aerosols version 0 (MUSICAv0), has been developed at NCAR to enable a computationally feasible global modeling framework while still resolving chemistry at urban scales. Using the MUSICAv0 framework with different horizontal grid resolutions (∼112, ∼56, ∼14, and ∼7 km), this work examines how much horizontal grid resolution can affect simulated chemical concentrations in 3D chemistry models. Model concentrations can vary up to 10 times between ∼112 and ∼7 km grids over urban areas at the surface. On the other hand, a region‐specific emission inventory with detailed local information is essential for some chemical species, although it is generally less important than the grid resolution for many chemical species. The model with a high‐resolution grid better reproduces observations in general, but in some cases compensating errors result in better comparisons for the coarse grid. This work suggests that the effects of grid resolution should not be ignored when evaluating new chemical mechanisms and chemistry models in future studies, and high grid resolution in 3D models is needed to simulate air pollutants over urban and downwind regions. Key Points: The dependence of simulated chemical species on model resolution is quantified in a single modeling frameworkModel evaluations can be substantially affected by grid resolution, especially for urban surface and aircraft measurements at low altitudesGrid resolution strongly impacts the oxidation of volatile organic compounds through differences in diurnal variation of oxidants [ABSTRACT FROM AUTHOR]

Using the CAM‐chem Model, we simulate the response of chemical species in the free troposphere to scenarios of primary pollutant emission reductions during the COVID‐19 pandemic. Zonally averaged ozone in the free troposphere during Northern Hemisphere spring and summer is found to be 5%–15% lower than 19‐yr climatological values, in good agreement with observations. About one third of this anomaly is attributed to the reduction scenario of air traffic during the pandemic, another third to the reduction scenario of surface emissions, the remainder to 2020 meteorological conditions, including the exceptional springtime Arctic stratospheric ozone depletion. For the combined emission reductions, the overall COVID‐19 reduction in 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%–6% were masked by comparable ozone increases due to other changes in 2020. Plain Language Summary: The reduction in the emissions of primary air pollutants during the 2020 COVID‐19 pandemic has generated perturbations in the chemical state of the atmosphere. A global Earth system model that accounts for chemical, physical, and dynamical processes in the atmosphere and for the coupling between the atmosphere, the ocean and the land surface, indicates that the abundance of tropospheric ozone was significantly reduced during the pandemic in response to realistic scenarios of reduced emissions of primary pollutants associated with restrictions of air traffic and economic activities. These simulated findings are consistent with observed ozone anomalies during the summer of 2020. Key Points: The ozone concentration in the northern extratropical free troposphere was 5%–15% lower in May and June 2020 relative to climatologyA third of this anomaly is attributed to meteorological conditions including stratospheric Arctic air with abnormally low ozoneThe assumed reduction in surface and aircraft emissions associated with the COVID‐19 pandemic can explain an ozone anomaly of 4%–8% [ABSTRACT FROM AUTHOR]

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 volatile organic carbon (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. Plain Language Summary: With the reduction in economic activities following the COVID‐19 pandemic outbreak in early 2020, most emissions of air pollutants (i.e., nitrogen oxides [NOx], carbon monoxide [CO], sulfur dioxide [SO2], volatile organic carbon [VOC], black carbon [BC], organic carbon [OC]) have decreased substantially during several months in different regions of the world. This unintended global experiment offered a glimpse into a potential future in which air quality would be improved. Here, a global atmospheric model is used to assess the changes in the chemical composition of the atmosphere during the pandemic period and in the related chemical processes that lead to the formation of ozone (O3) and secondary organic aerosols (SOA). The study illustrates the nonlinearity of the air quality response to reduced NOx and VOC emissions, which depends on the chemical environment including the background level of nitrogen oxides. Meteorological variability can lead to anomalies in the concentration of chemical species with magnitudes that are as large or even larger than the perturbations due to COVID‐induced changes in the emissions. Key Points: During the COVID‐19 lockdown, the atmospheric concentration of primary pollutants (NOx, VOCs, CO, SO2) was considerably reducedThe concentration of secondary pollutants increased in NOx‐saturated areas and decreased in NOx‐limited areasThe response of the chemical system depends on the relative changes in NOx and VOC emissions, and is affected by weather variability [ABSTRACT FROM AUTHOR]