Accurately quantifying wildfire impacts on ozone air quality is challenging due to complex physical and chemical processes in wildfire smoke. Here we use measurements from the 2018 WE-CAN aircraft campaign to parameterize emissions of reactive nitrogen (NOy) from wildfires into PAN (37%), NO3- (27%), and NO (36%) in a global chemistry-climate model with 13 km horizontal resolution over the contiguous US. The NOy partitioning, compared with emitting all NOy as NO, reduces model ozone bias in near-fire smoke plumes sampled by the aircraft but significantly enhances ozone downwind when Canadian smoke plumes reach cities in Washington state, Utah, Colorado, and Texas. Using multi-platform observations, we identify the smoke-influenced days with daily maximum 8-h average (MDA8) ozone of 70-85 ppbv in Spokane, Salt Lake City, Denver and Dallas. On these days, mixing of wildfire smoke into urban pollution enhance simulated MDA8 ozone by 10–20 ppbv.

Wildfires inject aerosols into the atmosphere at varying altitudes, modifying long-range transport, which impacts Earth’s climate system and air quality. Most global climate models use prescribed fixed-height injections, not accounting for the dynamic variability of wildfires. In this study, we enhance the injection method of biomass burning aerosols implemented in the Geophysical Fluid Dynamic Laboratory’s Atmospheric Model version 4.0, shifting to a more mechanistic approach. We test several injection height schemes to assess their impact on the Earth’s radiation budget by performing 18-year global simulations. Comparison of modeled injection height from the mechanistic scheme with observations indicates error within instrumental uncertainty (less than 500 meters). Aerosol Optical Depth (AOD) is systematically underestimated due to biases in the emission dataset, but the mechanistic scheme significantly reduces this bias by up to 0.5 optical depth units during extreme wildfire seasons over boreal forests. In term of the vertical profile of the aerosol extinction coefficient, a comparison with satellite observations indicates significant improvement below 4 km altitude. Dynamic injection of biomass burning emissions changed the net radiative flux at top of the atmosphere regionally (±1.5 Wm-2) and reduced it by -0.38 Wm-2 at the surface globally, relative to a baseline with no fire emissions. The temperature gradient anomaly associated with the dynamic injection of absorbing aerosols affects the atmospheric stability and circulation patterns. This study highlights the need to implement dynamic injection of fire emissions to simulate more accurately the atmospheric distribution of aerosols and their interactions with Earth’s climate system.

We assess the effective radiative forcing due to ozone-depleting substances using models participating in the Aerosols and Chemistry Model Intercomparison Project (AerChemMIP). A large inter-model spread in this globally averaged quantity necessitates an “emergent constraint” approach whereby we link the radiative forcing to the amount of ozone depletion simulated during 1979-2000, excluding two volcanically perturbed periods. During this period ozone-depleting substances were increasing, and several merged satellite-based climatologies document the ensuing decline of total-column ozone. We use these analyses to come up with effective radiative forcing magnitudes. For all of these satellite climatologies we find an effective radiative forcing outside or on the edge of the previously published “likely” range given by the 5th Assessment Report of IPCC, implying an offsetting effect of ozone depletion and/or other atmospheric feedbacks of -0.4 to -0.25 Wm-2, which is in absolute terms is larger than the previous best estimate of -0.15 Wm-2.

We quantify the impacts of halogenated ozone-depleting substances (ODSs), methane, N2O, CO2, and short-lived ozone precursors on total and partial ozone column changes between 1850 and 2014 using CMIP6 Aerosol and Chemistry Model Intercomparison Project (AerChemMIP) simulations. We find that whilst substantial ODS-induced ozone loss dominates the stratospheric ozone changes since the 1970s, the increases in short-lived ozone precursors and methane lead to increases in tropospheric ozone since the 1950s that make increasingly important contributions to total column ozone (TCO) changes. Our results show that methane impacts stratospheric ozone changes through its reaction with atomic chlorine leading to ozone increases, but this impact will decrease with declining ODSs. The N2O increases mainly impact ozone through NOx-induced ozone destruction in the stratosphere, having an overall small negative impact on TCO. CO2 increases lead to increased global stratospheric ozone due to stratospheric cooling. However, importantly CO2 increases cause TCO to decrease in the tropics. Large interannual variability obscures the responses of stratospheric ozone to N2O and CO2 changes. Substantial inter-model differences originate in the models’ representations of ODS-induced ozone depletion. We find that, although the tropospheric ozone trend is driven by the increase in its precursors, the stratospheric changes significantly impact the upper tropospheric ozone trend through modified stratospheric circulation and stratospheric ozone depletion. The speed-up of stratospheric overturning (i.e. decreasing age of air) is driven mainly by ODS and CO2; increases. Changes in methane and ozone precursors also modulate the cross-tropopause ozone flux.

The COVID-19 pandemic led to a widespread reduction in aerosol emissions. Anecdotal effects on air quality and visibility were widely reported. Less known are the impacts on the planetary energy balance. Using satellite observations and climate model simulations, we 15 study the underlying mechanisms of the large, precipitous decreases in solar clear-sky reflection (3.8 W m-2 or 7%) and aerosol optical depth (0.16 or 32%) over the East Asian Marginal Seas in March 2020. By separating the impacts due to meteorology and emissions in the model simulations, we find that about one-third of the anomalies can be attributed to pandemic-related emission reductions, and the rest to weather variability and long-term emission trends. The 20 current observational and modeling capabilities will be critical for monitoring, understanding, and predicting the radiative forcing and climate impacts of the ongoing crisis.

Using nine chemistry-climate and eight associated no-chemistry models, we investigate the persistence and timing of cold episodes occurring in the Arctic and Antarctic stratosphere during the period 1980-2014. We find systematic differences in behavior between members of these model pairs. In a first group of chemistry models whose dynamical configurations mirror their no-chemistry counterparts, we find an increased persistence of such cold polar vortices, such that these cold episodes both start earlier and last longer, relative to the times of occurrence of the lowest temperatures. Also the date of occurrence of the lowest temperatures, both in the Arctic and the Antarctic, is delayed by 1-3 weeks in chemistry models, versus their no-chemistry counterparts. This behavior exacerbates a widespread problem occurring in most or all models, a delayed occurrence, in the median, of the most anomalously cold day during such cold winters. In a second group of model pairs there are differences beyond just ozone chemistry. In particular, here the chemistry models feature more levels in the stratosphere, a raised model top, and differences in non-orographic gravity wave drag versus their no-chemistry counterparts. Such additional dynamical differences can completely mask the above influence of ozone chemistry. The results point towards a need to retune chemistry-climate models versus their no-chemistry counterparts.

We describe the baseline model configuration and simulation characteristics of GFDL’s Atmosphere Model version 4.1 (AM4.1), which builds on developments at GFDL over 2013–2018 for coupled carbon-chemistry-climate simulation as part of the sixth phase of the Coupled Model Intercomparison Project. In contrast with GFDL’s AM4.0 development effort, which focused on physical and aerosol interactions and which is used as the atmospheric component of CM4.0, AM4.1 focuses on comprehensiveness of Earth system interactions. Key features of this model include doubled horizontal resolution of the atmosphere (~200 km to ~100 km) with revised dynamics and physics from GFDL’s previous-generation AM3 atmospheric chemistry-climate model. AM4.1 features improved representation of atmospheric chemical composition, including aerosol and aerosol precursor emissions, key land-atmosphere interactions, comprehensive land-atmosphere-ocean cycling of dust and iron, and interactive ocean-atmosphere cycling of reactive nitrogen. AM4.1 provides vast improvements in fidelity over AM3, captures most of AM4.0’s baseline simulations characteristics and notably improves on AM4.0 in the representation of aerosols over the Southern Ocean, India, and China—even with its interactive chemistry representation—and in its manifestation of sudden stratospheric warmings in the coldest months. Distributions of reactive nitrogen and sulfur species, carbon monoxide, and ozone are all substantially improved over AM3. Fidelity concerns include degradation of upper atmosphere equatorial winds and of aerosols in some regions.