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.
We analyze the effects of the diurnal cycle of fire emissions (DCFE) and plume rise on U.S. air quality using the MUSICAv0 (Multi‐Scale Infrastructure for Chemistry and Aerosols Version 0) model during the FIREX‐AQ (Fire Influence on Regional to Global Environments and Air Quality) and WE‐CAN (Western wildfire Experiment for Cloud chemistry, Aerosol absorption and Nitrogen) field campaigns. To include DCFE in the model, we employ two approaches: a DCFE climatology and DCFE derived from a satellite fire radiative power product. We also implemented two sets of plume‐rise climatologies, and two plume‐rise parameterizations. We evaluate the model performance with airborne measurements, U.S. EPA Air Quality System surface measurements, and satellite products. Overall, including plume rise improves model agreement with observations such as aircraft observations of CO and NOxfor FIREX‐AQ and WE‐CAN. Applying DCFE also improves model performance, such as for surface PM2.5in fire‐impacted regions. The impact of plume rise is larger than the impact of DCFE. Plume rise can greatly enhance modeled long‐range transport of fire‐emitted pollutants. The simulations with plume‐rise parameterizations generally perform better than the simulations with plume‐rise climatologies during FIREX‐AQ, but not for WE‐CAN. The 2019 Williams Flats Fire case study demonstrates that DCFE and plume rise change fire impacts because fire emissions are subject to different meteorology and chemistry when emitted at different times of a day and altitudes. Moreover, DCFE and plume rise also impact local‐to‐regional meteorology and chemical reaction rates. DCFE and plume rise will be included in future MUSICA versions.
more » « less- NSF-PAR ID:
- 10372051
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Publisher / Repository:
- DOI PREFIX: 10.1029
- Date Published:
- Journal Name:
- Journal of Geophysical Research: Atmospheres
- Volume:
- 127
- Issue:
- 16
- ISSN:
- 2169-897X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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