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The impacts of climate change on tropospheric transport, diagnosed from a carbon monoxide (CO)-like tracer species emitted from global CO sources, are evaluated from an ensemble of four chemistry-climate models (CCMs) contributing to the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). Model time-slice simulations for present-day and end-of-The-21st-century conditions were performed under the Representative Concentrations Pathway (RCP) climate scenario RCP 8.5. All simulations reveal a strong seasonality in transport, especially over the tropics. The highest CO-Tracer mixing ratios aloft occur during boreal winter when strong vertical transport is co-located with biomass burning emission source regions. A consistent and robust decrease in future CO-Tracer mixing ratios throughout most of the troposphere, especially in the tropics, and an increase around the tropopause is found across the four CCMs in both winter and summer. Decreases in CO-Tracer mixing ratios in the tropical troposphere are associated with reduced convective mass fluxes in this region, which in turn may reflect a weaker Hadley cell circulation in the future climate. Increases in CO-Tracer mixing ratios near the tropopause are largely attributable to a rise in tropopause height enabling lofting to higher altitudes, although a poleward shift in the mid-latitude jets may also play a minor role in the extratropical upper troposphere. An increase in CO-Tracer mixing ratios also occurs near the Equator, centred over equatorial and Central Africa, extending from the surface to the mid-Troposphere. This is most likely related to localised decreases in convection in the vicinity of the Intertropical Convergence Zone (ITCZ), resulting in larger CO-Tracer mixing ratios over biomass burning regions and smaller mixing ratios downwind.

Quantifying the variable impacts of wildfire smoke on ozone air quality is challenging. Here we use airborne measurements from the 2018 Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE‐CAN) to parameterize emissions of reactive nitrogen (NOy) from wildfires into peroxyacetyl nitrate (PAN; 37%), NO3− (27%), and NO (36%) in a global chemistry‐climate model with 13 km spatial 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 and enhances ozone downwind by 5–10 ppbv when Canadian smoke plumes travel to Washington, Utah, Colorado, and Texas. Using multi‐platform observations, we identify the smoke‐influenced days with daily maximum 8‐hr average (MDA8) ozone of 70–88 ppbv in Kennewick, Salt Lake City, Denver and Dallas. On these days, wildfire smoke enhanced MDA8 ozone by 5–25 ppbv, through ozone produced remotely during plume transport and locally via interactions of smoke plume with urban emissions. Plain Language Summary: Wildfires have torn across western North America over the last decade. Smoke from wildland fires in Canada can travel thousands of kilometers to US cities and reacts with urban pollution to create harmful ozone, a criteria pollutant regulated by the US Environmental Protection Agency. Accurately quantifying this impact is needed to inform US air quality policy, but is challenging due to complex physical and chemical processes. In this study, we analyze surface and airborne measurements, alongside a new variable‐resolution global chemistry‐climate model, to better understand these processes. We show that the near‐field conversion of nitrogen oxide (NOx) emissions from wildfires to peroxyacetyl nitrate (PAN) and other more oxidized forms reduces their localized impacts on ozone. PAN is the principal tropospheric reservoir for NOx radicals. When aged smoke plumes descend southward from Canada toward US cities, higher temperatures cause PAN to decompose and thus help production of ozone during smoke transport. On days when the observed ozone levels exceed the air quality limit (70 ppbv for 8‐hr average), wildfire smoke can contribute 5–25 ppbv. Key Points: Sequestration of wildfire NOx emissions in Canada as peroxyacetyl nitrate (PAN) enhances the downwind impacts on US O3 air qualityPyrogenic volatile organic compounds and PAN decomposition increase the contribution of aged Canadian smoke plumes to O3 in US citiesAccounting for these effects in a high‐resolution chemistry‐climate model improves simulation of smoke‐impacted high‐O3 events in US cities [ABSTRACT FROM AUTHOR]

The Fires, Asian, and Stratospheric Transport–Las Vegas Ozone Study (FAST-LVOS) was conducted in May and June of 2017 to study the transport of ozone (O 3) to Clark County, Nevada, a marginal non-attainment area in the southwestern United States (SWUS). This 6-week (20 May–30 June 2017) field campaign used lidar, ozonesonde, aircraft, and in situ measurements in conjunction with a variety of models to characterize the distribution of O 3 and related species above southern Nevada and neighboring California and to probe the influence of stratospheric intrusions and wildfires as well as local, regional, and Asian pollution on surface O 3 concentrations in the Las Vegas Valley (≈ 900 m above sea level, a.s.l.). In this paper, we describe the FAST-LVOS campaign and present case studies illustrating the influence of different transport processes on background O 3 in Clark County and southern Nevada. The companion paper by Zhang et al. (2020) describes the use of the AM4 and GEOS-Chem global models to simulate the measurements and estimate the impacts of transported O 3 on surface air quality across the greater southwestern US and Intermountain West. The FAST-LVOS measurements found elevated O 3 layers above Las Vegas on more than 75 % (35 of 45) of the sample days and show that entrainment of these layers contributed to mean 8 h average regional background O 3 concentrations of 50–55 parts per billion by volume (ppbv), or about 85–95 µ g m -3. These high background concentrations constitute 70 %–80 % of the current US National Ambient Air Quality Standard (NAAQS) of 70 ppbv (≈ 120 µ g m -3 at 900 m a.s.l.) for the daily maximum 8 h average (MDA8) and will make attainment of the more stringent standards of 60 or 65 ppbv currently being considered extremely difficult in the interior SWUS. [ABSTRACT FROM AUTHOR]

The Fires, Asian, and Stratospheric Transport-Las Vegas Ozone Study (FAST-LVOS) was conducted in May and June of 2017 to study the transport of ozone (O3) to Clark County, Nevada, a marginal non-attainment area in the Southwestern U.S. (SWUS). This 6-week (20 May-30 June 2017) field campaign used lidar, ozonesonde, aircraft, and in-situ measurements in conjunction with a variety of models to characterize the distribution of O3 and related species above southern Nevada and neighbouring California, and to probe the influence of stratospheric intrusions, wildfires, and local, regional, and Asian pollution on surface O3 concentrations in Las Vegas and the surrounding area. In this paper, we describe the FAST-LVOS campaign and present case studies illustrating the influence of different transport processes on background O3 and air quality attainment in the SWUS. The measurements found elevated O3 layers above Las Vegas on more than 75% (35 of 45) of the sample days, and show that entrainment of these layers contributed to mean 8-h average background O3 concentrations of 50-55 parts-per-billion by volume (ppbv) across southern Nevada. These background concentrations constitute 70-80% of the current U.S. National Ambient Air Quality Standard (NAAQS) of 70 ppbv, and illustrate some of the challenges facing air quality managers tasked with O3 attainment in the SWUS during late spring and early summer. The companion paper by Zhang et al. (2020) describes the use of the AM4 and GEOS-Chem global models to estimate the impacts of transported O3 on surface air quality in the Southwestern U.S. and Intermountain West during the FAST-LVOS campaign. [ABSTRACT FROM AUTHOR]

Using observations and model simulations (ESM4.1) during 1988–2018, we show large year‐to‐year variability in western U.S. PM2.5 pollution caused by regional and distant fires. Widespread wildfires, combined with stagnation, caused summer PM2.5 pollution in 2017 and 2018 to exceed 2 standard deviations over long‐term averages. ESM4.1 with a fire emission inventory constrained by satellite‐derived fire radiative energy and aerosol optical depth captures the observed surface PM2.5 means and extremes above the 35 μg/m3 U.S. air quality standard. However, aerosol emissions from the widely used Global Fire Emissions Database (GFED) must be increased by 5 times for ESM4.1 to match observations. On days when observed PM2.5 reached 35–175 μg/m3, wildfire emissions can explain 90% of total PM2.5, with smoke transported from Canada contributing 25–50% in northern states, according to model sensitivity simulations. Fire emission uncertainties pose challenges to accurately assessing the impacts of fire smoke on air quality, radiation, and climate. Plain Language Summary: Frequent and intense wildfires harm public health over the western United States. In order to understand how wildfires affect fine particulate air quality, we analyze surface and satellite measurements and computer model simulations of weather and atmospheric chemistry over the past 30 years. We show that widespread fires and regional transport of fire smoke are the main causes of year‐to‐year changes in summertime particle pollution measured at western U.S. surface sites. The U.S. Environmental Protection Agency defines daily particle concentration above 35 μg/m3 as unhealthy. In the summers of 2017–2018, record‐breaking wildfires, combined with stable weather conditions, resulted in daily particle concentration of 35 to 175 μg/m3 across western U.S. sites. These particle pollution extremes are twice as severe as long‐term average conditions. Wildfire emissions contributed 90% of particle levels on these periods. Notably, transport of fire smoke from southwestern Canada can explain 25% to 50% of particle pollution in northern states such as Washington. Our model successfully simulates these pollution extremes when applying a fire emission data set constrained by satellite observations of total particle abundances. Our results indicate fourfold to fivefold underestimates of particle emissions from the widely used Global Fire Emissions Database not constrained by satellite observations. Key Points: Large interannual variations of western U.S. fine particulate pollution in summer were driven by regional and distant firesWidespread wildfires and stagnation in 2017–2018 caused fine particulate extremes to exceed 2 standard deviations over long‐term averagesObservations and model analyses indicate fourfold to fivefold underestimate of aerosol emissions from the widely used Global Fire Emissions Database [ABSTRACT FROM AUTHOR]