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Heating from wildfires adds buoyancy to the overlying air, often producing plumes that vertically distribute fire emissions throughout the atmospheric column over the fire. The height of the rising wildfire plume is a complex function of the size of the wildfire, fire heat flux, plume geometry, and atmospheric conditions, which can make simulating plume rises difficult with coarser-scale atmospheric models. To determine the altitude of fire emission injection, several plume rise parameterizations have been developed in an effort estimate the height of the wildfire plume rise. Previous work has indicated the performance of these plume rise parameterizations has generally been mixed when validated against satellite observations. However, it is often difficult to evaluate the performance of plume rise parameterizations due to the significant uncertainties associated with fire input parameters such as fire heat fluxes and area. In order to reduce the uncertainties of fire input parameters, we applied an atmospheric modeling framework with different plume rise parameterizations to a well constrained prescribed burn, as part of the RxCADRE field experiment. Initial results found that the model was unable to reasonably replicate downwind smoke for cases when fire emissions were emitted at the surface and released at the top of the plume. However, when fire emissions were distributed below the plume top following a Gaussian distribution, model results were significantly improved.

Fires emit sufficient sulfur to affect local and regional air quality and climate. This study analyzes SO2 emission factors and variability in smoke plumes from US wildfires and agricultural fires, as well as their relationship to sulfate and hydroxymethanesulfonate (HMS) formation. Observed SO2 emission factors for various fuel types show good agreement with the latest reviews of biomass burning emission factors, producing an emission factor range of 0.47–1.2 g SO2 kg^(−1) C. These emission factors vary with geographic location in a way that suggests that deposition of coal burning emissions and application of sulfur-containing fertilizers likely play a role in the larger observed values, which are primarily associated with agricultural burning. A 0-D box model generally reproduces the observed trends of SO2 and total sulfate (inorganic + organic) in aging wildfire plumes. In many cases, modeled HMS is consistent with the observed organosulfur concentrations. However, a comparison of observed organosulfur and modeled HMS suggests that multiple organosulfur compounds are likely responsible for the observations but that the chemistry of these compounds yields similar production and loss rates as that of HMS, resulting in good agreement with the modeled results. We provide suggestions for constraining the organosulfur compounds observed during these flights, and we show that the chemistry of HMS can allow organosulfur to act as an S(IV) reservoir under conditions of pH > 6 and liquid water content >10^(−7) g sm^(−3). This can facilitate long-range transport of sulfur emissions, resulting in increased SO2 and eventually sulfate in transported smoke.

Biomass burning emits an estimated 25 % of global annual nitrogen oxides (NOx), an important constituent that participates in the oxidative chemistry of the atmosphere. Estimates of NOx emission factors, representing the amount of NOx per mass burned, are primarily based on field or laboratory case studies, but the sporadic and transient nature of wildfires makes it challenging to verify whether these case studies represent the behavior of the global fires that occur on earth. Satellite remote sensing provides a unique view of the earth, allowing for the study of emissions and downwind evolution of NOx from a large number of fires. We describe direct estimates of NOx emissions and lifetimes for fires using an exponentially modified Gaussian analysis of daily TROPOspheric Monitoring Instrument (TROPOMI) retrievals of NO2 tropospheric columns. We update the a priori profile of NO2 with a fine-resolution (0.25∘) global model simulation from NASA's GEOS Composition Forecasting System (GEOS-CF), which largely enhances NO2 columns over fire plumes. We derive representative NOx emission factors for six fuel types globally by linking TROPOMI-derived NOx emissions with observations of fire radiative power from Moderate Resolution Imaging Spectroradiometer (MODIS). Satellite-derived NOx emission factors are largely consistent with those derived from in situ measurements. We observe decreasing NOx lifetime with fire emissions, which we infer is due to the increase in both NOx abundance and hydroxyl radical production. Our findings suggest promise for applying space-based observations to track the emissions and chemical evolution of reactive nitrogen from wildfires.

Extensive airborne measurements of non-methane organic gases (NMOGs), methane, nitrogen oxides, reduced nitrogen species, and aerosol emissions from US wild and prescribed fires were conducted during the 2019 NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality campaign (FIREX-AQ). Here, we report the atmospheric enhancement ratios (ERs) and inferred emission factors (EFs) for compounds measured on board the NASA DC-8 research aircraft for nine wildfires and one prescribed fire, which encompass a range of vegetation types. We use photochemical proxies to identify young smoke and reduce the effects of chemical degradation on our emissions calculations. ERs and EFs calculated from FIREX-AQ observations agree within a factor of 2, with values reported from previous laboratory and field studies for more than 80 % of the carbon- and nitrogen-containing species. Wildfire emissions are parameterized based on correlations of the sum of NMOGs with reactive nitrogen oxides (NOy) to modified combustion efficiency (MCE) as well as other chemical signatures indicative of flaming/smoldering combustion, including carbon monoxide (CO), nitrogen dioxide (NO2), and black carbon aerosol. The sum of primary NMOG EFs correlates to MCE with an R2 of 0.68 and a slope of −296 ± 51 g kg−1, consistent with previous studies. The sum of the NMOG mixing ratios correlates well with CO with an R2 of 0.98 and a slope of 137 ± 4 ppbv of NMOGs per parts per million by volume (ppmv) of CO, demonstrating that primary NMOG emissions can be estimated from CO. Individual nitrogen-containing species correlate better with NO2, NOy, and black carbon than with CO. More than half of the NOy in fresh plumes is NO2 with an R2 of 0.95 and a ratio of NO2 to NOy of 0.55 ± 0.05 ppbv ppbv−1, highlighting that fast photochemistry had already occurred in the sampled fire plumes. The ratio of NOy to the sum of NMOGs follows trends observed in laboratory experiments and increases exponentially with MCE, due to increased emission of key nitrogen species and reduced emission of NMOGs at higher MCE during flaming combustion. These parameterizations will provide more accurate boundary conditions for modeling and satellite studies of fire plume chemistry and evolution to predict the downwind formation of secondary pollutants, including ozone and secondary organic aerosol.

During the first phase of the Biomass Burn Operational Project (BBOP) field campaign, conducted in the Pacific Northwest, the DOE G-1 aircraft was used to follow the time evolution of wildfire smoke from near the point of emission to locations 2–3.5 h downwind. In nine flights we made repeated transects of wildfire plumes at varying downwind distances and could thereby follow the plume's time evolution. On average there was little change in dilution-normalized aerosol mass concentration as a function of downwind distance. This consistency hides a dynamic system in which primary aerosol particles are evaporating and secondary ones condensing. Organic aerosol is oxidized as a result. On all transects more than 90 % of aerosol is organic. In freshly emitted smoke aerosol, NH4+ is approximately equivalent to NO3. After 2 h of daytime aging, NH4+ increased and is approximately equivalent to the sum of Cl, SO42, and NO3. Particle size increased with downwind distance, causing particles to be more efficient scatters. Averaged over nine flights, mass scattering efficiency (MSE) increased in ∼ 2 h by 56 % and doubled in one flight. Mechanisms for redistributing mass from small to large particles are discussed. Coagulation is effective at moving aerosol from the Aitken to accumulation modes but yields only a minor increase in MSE. As absorption remained nearly constant with age, the time evolution of single scatter albedo was controlled by age-dependent scattering. Near-fire aerosol had a single scatter albedo (SSA) of 0.8–0.9. After 1 to 2 h of aging SSAs were typically 0.9 and greater. Assuming global-average surface and atmospheric conditions, the observed age dependence in SSA would change the direct radiative effect of a wildfire plume from near zero near the fire to a cooling effect downwind.

Open biomass burning contributes significantly to air quality degradation and associated human health impacts over large areas. It is one of the largest sources of reactive trace gases and fine particles to Earth’s atmosphere and consequently a major source of cloud condensation nuclei on a global scale. However, there is a large uncertainty in the climate effect of open biomass burning aerosols due to the complexity of their constituents. Here, we present an exceptionally large dataset on southern African savannah and grassland fire plumes and their atmospheric evolution, based on 5.5 years of continuous measurements from 2010 to 2015. We find that the mass of submicrometre aerosols more than doubles on average, in only three hours of daytime ageing. We also evaluate biomass burning aerosol particle size distributions and find a large discrepancy between the observations and current model parameterizations, especially in the 30–100 nm range. We conclude that accounting for near-source secondary organic aerosol formation and using measurement-based size distribution parameterizations in smoke plumes is essential to better constrain the climate and air quality effects of savannah and grassland fires.

Formaldehyde (HCHO) is one of the most abundant non-methane volatile organic compounds (VOCs) emitted by fires. HCHO also undergoes chemical production and loss as a fire plume ages, and it can be an important oxidant precursor. In this study, we disentangle the processes controlling HCHO by examining its evolution in wildfire plumes sampled by the NASA DC-8 during the Fire Influence on Regional to Global Environments and Air Quality experiment (FIREX-AQ) field campaign. In 9 of the 12 analyzed plumes, dilution-normalized HCHO increases with physical age (range 1–6 h). The balance of HCHO loss (mainly via photolysis) and production (via OH-initiated VOC oxidation) seems to control the sign and magnitude of this trend. Plume-average OH concentrations, calculated from VOC decays, range from −0.5 (± 0.5) × 106 to 5.3 (± 0.7) × 106 cm−3. The production and loss rates of dilution-normalized HCHO seem to decrease with plume age. Plume-to-plume variability in dilution-normalized secondary HCHO production correlates with OH abundance rather than normalized OH reactivity, suggesting that OH is the main driver of fire-to-fire variability in HCHO secondary production. Analysis suggests an effective HCHO yield of 0.33 (± 0.05) per VOC molecule oxidized for the 12 wildfire plumes. This finding can help connect space-based HCHO observations to the oxidizing capacity of the atmosphere and to VOC emissions.

Aerosol absorption of visible light has an important impact on global radiative forcing. Wildfires are one of the major sources of light-absorbing aerosol, but there remains significant uncertainty about the magnitude, wavelength dependence, and bleaching of absorption from biomass burning aerosol. We collected and analyzed data from 21 western US wildfire smoke plumes during the 2018 Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption and Nitrogen (WE-CAN) airborne measurement campaign to determine the contribution of black carbon (BC), brown carbon (BrC), and lensing to the aerosol mass absorption cross section (MAC). Comparison to commonly used parameterizations and modeling studies suggests that model overestimation of absorption is likely due to incorrect BrC refractive indices. Modelers (Wang et al., 2018; Carter et al., 2021) invoke a bleaching process that decreases the MAC of organic aerosol (OA) to offset the overestimation of absorption in models. However, no evidence of a decreasing MAC is observed in individual WE-CAN fire plumes or in aged plumes from multiple fires. A decrease in OA mass and water-soluble organic carbon (WSOC), both normalized by carbon monoxide (CO) to correct for dilution, is observed with an increasing oxygen-to-carbon (O : C) ratio and a decreasing gas-phase toluene : benzene ratio, when data from all fires are combined in half of the individual fire plumes. This results in a strong decrease in total absorption at 405 nm and a slight decrease at 660 nm with these chemical markers. These results demonstrate that changes in absorption with chemical markers of plume age are the result of decreasing OA rather than changes in the MAC of the organic material itself. While decreasing MAC or OA mass with aging could both be called bleaching and can both correct overestimation of absorption in models, it is important to distinguish between these two effects because decreasing OA mass will also decrease scattering, which will cause a significantly different net radiative effect. We also find that an average of 54 % of non-BC absorption (23 % total absorption) at 660 nm is from water-soluble BrC, confirming that BrC absorption is important across the visible spectrum. Quantification of significant BrC at red wavelengths and observation of bleaching being caused by changes in OA with O : C and toluene : benzene markers of plume age provide important improvements to our understanding of BrC and critical constraints on aerosol absorption in regional and global climate models.

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.

Six months of stratospheric aerosol observations with the European Aerosol Research Lidar Network (EARLINET) from August 2017 to January 2018 are presented. The decay phase of an unprecedented, record-breaking stratospheric perturbation caused by wildfire smoke is reported and discussed in terms of geometrical, optical, and microphysical aerosol properties. Enormous amounts of smoke were injected into the upper troposphere and lower stratosphere over fire areas in western Canada on 12 August 2017 during strong thunderstorm–pyrocumulonimbus activity. The stratospheric fire plumes spread over the entire Northern Hemisphere in the following weeks and months. Twenty-eight European lidar stations from northern Norway to southern Portugal and the eastern Mediterranean monitored the strong stratospheric perturbation on a continental scale. The main smoke layer (over central, western, southern, and eastern Europe) was found at heights between 15 and 20 km since September 2017 (about 2 weeks after entering the stratosphere). Thin layers of smoke were detected at heights of up to 22–23 km. The stratospheric aerosol optical thickness at 532 nm decreased from values > 0.25 on 21–23 August 2017 to 0.005–0.03 until 5–10 September and was mainly 0.003–0.004 from October to December 2017 and thus was still significantly above the stratospheric background (0.001–0.002). Stratospheric particle extinction coefficients (532 nm) were as high as 50–200 Mm−1 until the beginning of September and on the order of 1 Mm−1 (0.5–5 Mm−1) from October 2017 until the end of January 2018. The corresponding layer mean particle mass concentration was on the order of 0.05–0.5 µg m−3 over these months. Soot particles (light-absorbing carbonaceous particles) are efficient ice-nucleating particles (INPs) at upper tropospheric (cirrus) temperatures and available to influence cirrus formation when entering the tropopause from above. We estimated INP concentrations of 50–500 L−1 until the first days in September and afterwards 5–50 L−1 until the end of the year 2017 in the lower stratosphere for typical cirrus formation temperatures of −55 ∘C and an ice supersaturation level of 1.15. The measured profiles of the particle linear depolarization ratio indicated a predominance of nonspherical smoke particles. The 532 nm depolarization ratio decreased slowly with time in the main smoke layer from values of 0.15–0.25 (August–September) to values of 0.05–0.10 (October–November) and < 0.05 (December–January). The decrease of the depolarization ratio is consistent with aging of the smoke particles, growing of a coating around the solid black carbon core (aggregates), and thus change of the shape towards a spherical form. We found ascending aerosol layer features over the most southern European stations, especially over the eastern Mediterranean at 32–35∘ N, that ascended from heights of about 18–19 to 22–23 km from the beginning of October to the beginning of December 2017 (about 2 km per month). We discuss several transport and lifting mechanisms that may have had an impact on the found aerosol layering structures.