Parameterizations of US wildfire and prescribed fire emission ratios and emission factors based on FIREX-AQ aircraft measurements

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Citation of Original Publication

Gkatzelis, Georgios I., Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, et al. “Parameterizations of US Wildfire and Prescribed Fire Emission Ratios and Emission Factors Based on FIREX-AQ Aircraft Measurements.” Atmospheric Chemistry and Physics 24, no. 2 (January 23, 2024): 929–56. https://doi.org/10.5194/acp-24-929-2024.

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This work was written as part of one of the author's official duties as an Employee of the United States Government and is therefore a work of the United States Government. In accordance with 17 U.S.C. 105, no copyright protection is available for such works under U.S. Law.
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Abstract

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 (NOᵧ) 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, NOᵧ, and black carbon than with CO. More than half of the NOᵧ in fresh plumes is NO₂ with an R² of 0.95 and a ratio of NO₂ to NOᵧ of 0.55 ± 0.05 ppbv ppbv⁻¹, highlighting that fast photochemistry had already occurred in the sampled fire plumes. The ratio of NOᵧ 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.