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

Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M.St Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. Digangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu GuoJohnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. Mckeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, Carsten Warneke

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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 (FIREXAQ). 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 nitrogencontaining 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.

Original languageEnglish
Pages (from-to)929-956
Number of pages28
JournalAtmospheric Chemistry and Physics
Volume24
Issue number2
DOIs
StatePublished - Jan 23 2024

Funding

Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Megan M. Bela, Ilann Bourgeois, Joseph M. Katich, Aaron Lamplugh, Stuart A. McKeen, J. Andrew Neuman, Jeff Peischl, Pamela S. Rickly, Michael A. Robinson, Rebecca H. Schwantes, Caroline C. Womack, and Carsten Warneke were supported by the NOAA cooperative agreement with CIRES (grant no. NA17OAR4320101). Robert J. Yokelson and Vanessa Selimovic were supported by NOAA (grant no. NA16OAR4310100) and NSF (grant no. 1748266). Jakob Lindaas, Glenn M. Wolfe, Reem Hannun, Jason M. St. Clair, and Thomas F. Hanisco were supported by the NASA Tropospheric Composition Program and NOAA Climate Program Office's Atmospheric Chemistry, Carbon Cycle and Climate (AC4) program (grant no. NA17OAR4310004). Demetrios Pagonis, Benjamin A. Nault, Hongyu Guo, Pedro Campuzano-Jost, Douglas A. Day, Melinda K. Schueneman, and Jose L. Jimenez were supported by NASA (grant nos. 80NSSC18K0630 and 80NSSC21K1451). Alan Fried was supported by NASA TCP (grant no. 80NSSC18K0628). The University of Innsbruck team was supported by the Austrian Federal Ministry for Transport, Innovation, and Technology (BMVIT, FFG, ASAP). Felix Piel received funding from the European Union's Horizon 2020 Research and Innovation program (IMPACT EU ITN (grant no. 674911)). Lu Xu, Krystal T. Vasquez, Hannah Allen, John D. Crounse, and Paul O. Wennberg were supported by NASA (grant nos. 80NSSC18K0660 and 80NSSC21K1704). This material is based upon work supported by the National Center for Atmospheric Research, sponsored by the National Science Foundation under cooperative agreement (grant no. 1852977).The article processing charges for this open-access publication were covered by the Forschungszentrum Jülich.

FundersFunder number
Impact Technologies674911, 80NSSC18K0660, 80NSSC21K1704
1852977, 1748266
National Aeronautics and Space AdministrationNA17OAR4310004, 80NSSC18K0630, 80NSSC21K1451, 80NSSC18K0628
National Oceanic and Atmospheric Administration
National Center for Atmospheric Research
Cooperative Institute for Research in Environmental SciencesNA17OAR4320101, NA16OAR4310100

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