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 (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.
This content will become publicly available on December 16, 2024
Wildfires have become larger and more frequent because of climate change, increasing their impact on air pollution. Air quality forecasts and climate models do not currently account for changes in the composition of wildfire emissions during the commonly observed progression from more flaming to smoldering combustion. Laboratory measurements have consistently shown decreased nitrogen dioxide (NO2) relative to carbon monoxide (CO) over time, as they transitioned from more flaming to smoldering combustion, while formaldehyde (HCHO) relative to CO remained constant. Here, we show how daily ratios between column densities of NO2versus those of CO and HCHO versus CO from the Tropospheric Monitoring Instrument (TROPOMI) changed for large wildfires in the Western United States. TROPOMI‐derived emission ratios were lower than those from the laboratory. We discuss reasons for the discrepancies, including how representative laboratory burns are of wildfires, the effect of aerosols on trace gas retrievals, and atmospheric chemistry in smoke plumes.
more » « less- NSF-PAR ID:
- 10484215
- Publisher / Repository:
- Wiley
- Date Published:
- Journal Name:
- Geophysical Research Letters
- Volume:
- 50
- Issue:
- 23
- ISSN:
- 0094-8276
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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