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Abstract. Wildfire smoke is one of the most significant concerns of human and environmental health, associated with its substantial impacts on air quality, weather, and climate. However, biomass burning emissions and smoke remain among the largest sources of uncertainties in air quality forecasts. In this study, we evaluate the smoke emissions and plume forecasts from 12 state-of-the-art air quality forecasting systems during the Williams Flats fire in Washington State, US, August 2019, which was intensively observed during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field campaign. Model forecasts with lead times within 1 d are intercompared under the same framework based on observations from multiple platforms to reveal their performance regarding fire emissions, aerosol optical depth (AOD), surface PM2.5, plume injection, and surface PM2.5 to AOD ratio. The comparison of smoke organic carbon (OC) emissions suggests a large range of daily totals among the models, with a factor of 20 to 50. Limited representations of the diurnal patterns and day-to-day variations of emissions highlight the need to incorporate new methodologies to predict the temporal evolution and reduce uncertainty of smoke emission estimates. The evaluation of smoke AOD (sAOD) forecasts suggests overall underpredictions in both the magnitude and smoke plume area for nearly all models, although the high-resolution models have a better representation of the fine-scale structures of smoke plumes. The models driven by fire radiative power (FRP)-based fire emissions or assimilating satellite AOD data generally outperform the others. Additionally, limitations of the persistence assumption used when predicting smoke emissions are revealed by substantial underpredictions of sAOD on 8 August 2019, mainly over the transported smoke plumes, owing to the underestimated emissions on 7 August. In contrast, the surface smoke PM2.5 (sPM2.5) forecasts show both positive and negative overall biases for these models, with most members presenting more considerable diurnal variations of sPM2.5. Overpredictions of sPM2.5 are found for the models driven by FRP-based emissions during nighttime, suggesting the necessity to improve vertical emission allocation within and above the planetary boundary layer (PBL). Smoke injection heights are further evaluated using the NASA Langley Research Center's Differential Absorption High Spectral Resolution Lidar (DIAL-HSRL) data collected during the flight observations. As the fire became stronger over 3–8 August, the plume height became deeper, with a day-to-day range of about 2–9 km a.g.l. However, narrower ranges are found for all models, with a tendency of overpredicting the plume heights for the shallower injection transects and underpredicting for the days showing deeper injections. The misrepresented plume injection heights lead to inaccurate vertical plume allocations along the transects corresponding to transported smoke that is 1 d old. Discrepancies in model performance for surface PM2.5 and AOD are further suggested by the evaluation of their ratio, which cannot be compensated for by solely adjusting the smoke emissions but are more attributable to model representations of plume injections, besides other possible factors including the evolution of PBL depths and aerosol optical property assumptions. By consolidating multiple forecast systems, these results provide strategic insight on pathways to improve smoke forecasts.

Abstract. Wildfires are increasing in size across the western US, leading to increases in human smoke exposure and associated negative health impacts. The impact of biomass burning (BB) smoke, including wildfires, on regional air quality depends on emissions, transport, and chemistry, including oxidation of emitted BB volatile organic compounds (BBVOCs) by the hydroxyl radical (OH), nitrate radical (NO3), and ozone (O3). During the daytime, when light penetrates the plumes, BBVOCs are oxidized mainly by O3 and OH. In contrast, at night or in optically dense plumes, BBVOCs are oxidized mainly by O3 and NO3. This work focuses on the transition between daytime and nighttime oxidation, which has significant implications for the formation of secondary pollutants and loss of nitrogen oxides (NOx=NO+NO2) and has been understudied. We present wildfire plume observations made during FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality), a field campaign involving multiple aircraft, ground, satellite, and mobile platforms that took place in the United States in the summer of 2019 to study both wildfire and agricultural burning emissions and atmospheric chemistry. We use observations from two research aircraft, the NASA DC-8 and the NOAA Twin Otter, with a detailed chemical box model, including updated phenolic mechanisms, to analyze smoke sampled during midday, sunset, and nighttime. Aircraft observations suggest a range of NO3 production rates (0.1–1.5 ppbv h−1) in plumes transported during both midday and after dark. Modeled initial instantaneous reactivity toward BBVOCs for NO3, OH, and O3 is 80.1 %, 87.7 %, and 99.6 %, respectively. Initial NO3 reactivity is 10–104 times greater than typical values in forested or urban environments, and reactions with BBVOCs account for >97 % of NO3 loss in sunlit plumes (jNO2 up to 4×10-3s-1), while conventional photochemical NO3 loss through reaction with NO and photolysis are minor pathways. Alkenes and furans are mostly oxidized by OH and O3 (11 %–43 %, 54 %–88 % for alkenes; 18 %–55 %, 39 %–76 %, for furans, respectively), but phenolic oxidation is split between NO3, O3, and OH (26 %–52 %, 22 %–43 %, 16 %–33 %, respectively). Nitrate radical oxidation accounts for 26 %–52 % of phenolic chemical loss in sunset plumes and in an optically thick plume. Nitrocatechol yields varied between 33 % and 45 %, and NO3 chemistry in BB plumes emitted late in the day is responsible for 72 %–92 % (84 % in an optically thick midday plume) of nitrocatechol formation and controls nitrophenolic formation overall. As a result, overnight nitrophenolic formation pathways account for 56 %±2 % of NOx loss by sunrise the following day. In all but one overnight plume we modeled, there was remaining NOx (13 %–57 %) and BBVOCs (8 %–72 %) at sunrise.

SignificanceWe report radiocarbon (14C) measurements of carbonaceous aerosol originating from fires on the islands of Sumatra and Borneo. These data provide information about what types of ecosystems burned and are critical for linking the human health effects of fires to the anthropogenic build-up of atmospheric CO2. Our measurements confirm that peat emissions were the dominant source of aerosols in Singapore during the 2015 El Niño and provide a means for monitoring the success of policies designed to protect peatland areas during future drought events.