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  1. Free, publicly-accessible full text available October 13, 2023
  2. Abstract. Smoke from wildfires is a significant source of air pollution, which can adversely impact air quality and ecosystems downwind. With the recently increasing intensity and severity of wildfires, the threat to air quality is expected to increase. Satellite-derived biomass burning emissions can fill in gaps in the absence of aircraft or ground-based measurement campaigns and can help improve the online calculation of biomass burning emissions as well as the biomass burning emissions inventories that feed air quality models. This study focuses on satellite-derived NOx emissions using the high-spatial-resolution TROPOspheric Monitoring Instrument (TROPOMI) NO2 dataset. Advancements and improvements to the satellite-based determination of forest fire NOx emissions are discussed, including information on plume height and effects of aerosol scattering and absorption on the satellite-retrieved vertical column densities. Two common top-down emission estimation methods, (1) an exponentially modified Gaussian (EMG) and (2) a flux method, are applied to synthetic data to determine the accuracy and the sensitivity to different parameters, including wind fields, satellite sampling, noise, lifetime, and plume spread. These tests show that emissions can be accurately estimated from single TROPOMI overpasses.The effect of smoke aerosols on TROPOMI NO2 columns (via air mass factors, AMFs) is estimated, and these satellitemore »columns and emission estimates are compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America. Our results indicate that applying an explicit aerosol correction to the TROPOMI NO2 columns improves the agreement with the aircraft observations (by about 10 %–25 %). The aircraft- and satellite-derived emissions are in good agreement within the uncertainties. Both top-down emissions methods work well; however, the EMG method seems to output more consistent results and has better agreement with the aircraft-derived emissions. Assuming a Gaussian plume shape for various biomass burning plumes, we estimate an average NOx e-folding time of 2 ±1 h from TROPOMI observations. Based on chemistry transport model simulations and aircraft observations, the net emissions of NOx are 1.3 to 1.5 times greater than the satellite-derived NO2 emissions. A correction factor of 1.3 to 1.5 should thus be used to infer net NOx emissions from the satellite retrievals of NO2.« less
  3. Abstract

    During the summer of 2018, the upward-pointing Wyoming Cloud Lidar (WCL) was deployed on board the University of Wyoming King Air (UWKA) research aircraft for the Biomass Burning Flux Measurements of Trace Gases and Aerosols (BB-FLUX) field campaign. This paper describes the generation of calibrated attenuated backscatter coefficients and aerosol extinction coefficients from the WCL measurements. The retrieved aerosol extinction coefficients at the flight level strongly correlate (correlation coefficient, rr > 0.8) with in situ aerosol concentration and carbon monoxide (CO) concentration, providing a first-order estimate for converting WCL extinction coefficients into vertically resolved CO and aerosol concentration within wildfire smoke plumes. The integrated CO column concentrations from the WCL data in nonextinguished profiles also correlate (rr = 0.7) with column measurements by the University of Colorado Airborne Solar Occultation Flux instrument, indicating the validity of WCL-derived extinction coefficients. During BB-FLUX, the UWKA sampled smoke plumes from more than 20 wildfires during 35 flights over the western United States. Seventy percent of flight time was spent below 3 km above ground level (AGL) altitude, although the UWKA ascended up to 6 km AGL to sample the top of some deep smoke plumes. The upward-pointing WCL observed a nearly equalmore »amount of thin and dense smoke below 2 km and above 5 km due to the flight purpose of targeted fresh fire smoke. Between 2 and 5 km, where most of the wildfire smoke resided, the WCL observed slightly more thin smoke than dense smoke due to smoke spreading. Extinction coefficients in dense smoke were 2–10 times stronger, and dense smoke tended to have larger depolarization ratio, associated with irregular aerosol particles.

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  4. Abstract. Chamber oxidation experiments conducted at the Fire Sciences Laboratory in 2016 are evaluated to identify important chemical processes contributing to the hydroxy radical (OH) chemistry of biomass burning non-methane organic gases (NMOGs). Based on the decay of primary carbon measured by proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS), it is confirmed that furans and oxygenated aromatics are among the NMOGs emitted from western United States fuel types with the highest reactivities towards OH. The oxidation processes and formation of secondary NMOG masses measured by PTR-ToF-MS and iodide-clustering time-of-flight chemical ionization mass spectrometry (I-CIMS) is interpreted using a box model employing a modified version of the Master Chemical Mechanism (v. 3.3.1) that includes the OH oxidation of furan, 2-methylfuran, 2,5-dimethylfuran, furfural, 5-methylfurfural, and guaiacol. The model supports the assignment of major PTR-ToF-MS and I-CIMS signals to a series of anhydrides and hydroxy furanones formed primarily through furan chemistry. This mechanism is applied to a Lagrangian box model used previously to model a real biomass burning plume. The customized mechanism reproduces the decay of furans and oxygenated aromatics and the formation of secondary NMOGs, such as maleic anhydride. Based on model simulations conducted with and without furans, it is estimated that furansmore »contributed up to 10 % of ozone and over 90 % of maleic anhydride formed within the first 4 h of oxidation. It is shown that maleic anhydride is present in a biomass burning plume transported over several days, which demonstrates the utility of anhydrides as markers for aged biomass burning plumes.« less