Daytime Oxidized Reactive Nitrogen Partitioning in Western U.S. Wildfire Smoke Plumes

Calahorrano, Julieta F. Juncosa; Lindaas, Jakob; O’Dell, Katelyn; Palm, Brett B.; Peng, Qiaoyun; Flocke, Frank; Pollack, I. B.; Garofalo, Lauren A.; Farmer, Delphine K.; Pierce, Jeffrey R.; Collett, Jeffrey L.; Weinheimer, A. J.; Campos, T.; Hornbrook, R. S.; Hall, Samuel R.; Ullmann, Kirk; Pothier, Matson A.; Apel, E. C.; Permar, Wade; Hu, Lu; Hills, A. J.; Montzka, D.; Tyndall, G. S.; Fischer, Emily V.

doi:10.1029/2020jd033484

Cited by 46 publications

(64 citation statements)

References 96 publications

(221 reference statements)

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“…For the NO x lifetime we derived 2 ± 1 h using the EMG for various fires. This is in good agreement with the results from the WE-CAN campaign that suggested a NO x decay time of 90 min in biomass burning plumes (Juncosa Calahorrano et al, 2021).…”

Section: Emission Comparisonssupporting

confidence: 91%

“…The uncertainties are 6 % for NO and 12 % for NO 2 for concentrations >1 pptv. Further details about the campaign and the measurements can be found in Lindaas et al (2021), Juncosa Calahorrano et al (2021) and Peng et al (2020). Data are publicly available from https://www-air.larc.nasa.gov/cgi-bin/ ArcView/firexaq?MERGE=1 (last accessed: 19 July 2021).…”

Section: We-canmentioning

confidence: 99%

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Biomass burning nitrogen dioxide emissions derived from space with TROPOMI: methodology and validation

Griffin

McLinden

Dammers

et al. 2021

Preprint

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Abstract. Smoke from wildfires is a significant source of air pollution, which can adversely impact air quality and ecosystems downwind. With the recently increasing intensity and severity of wildfires, the threat to air quality is expected to increase. Satellite-derived biomass burning emissions can fill in gaps in the absence of aircraft or ground-based measurement campaigns, and can help improve the on-line calculation of biomass burning emissions as well as the biomass burning emissions inventories that feed air quality models. This study focuses on satellite-derived NOx emissions using the high-spatial resolution TROPOspheric Monitoring Instrument (TROPOMI) NO2 dataset. Advancements and improvements to the satellite based determination of forest fire NOx emissions are discussed, including information on plume height and effects of aerosol scattering on the satellite-retrieved vertical column densities. Two common top-down emission estimation methods, (1) an Exponentially Modified Gaussian (EMG) and (2) a flux method, are applied to synthetic data to determine the accuracy and the sensitivity to different parameters, including wind fields, satellite sampling, noise, lifetime and plume spread. These tests show that emissions can be accurately estimated from single TROPOMI overpasses. The effect of smoke aerosols on TROPOMI NO2 columns (via AMFs) is estimated and these satellite columns and emission estimates are compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America. Our results indicate that applying an explicit aerosol correction to the TROPOMI NO2 columns improve the agreement with the aircraft observations (by about 10–25 %). The aircraft- and satellite-derived emissions are in good agreement within the uncertainties. Both top-down emissions methods work well, however, the EMG method seems to output more consistent results and has better agreement with the aircraft-derived emissions. Assuming a Gaussian plume shape for various biomass burning plumes, we estimate an average NOx e-folding time of 2 ± 1 h from TROPOMI observations. Based on chemistry transport model simulations and aircraft observations, the net emissions of NOx are 1.3 to 1.5 times greater than the satellite-derived NO2 emissions. A correction factor of 1.3 to 1.5 should thus be used to infer net NOx emissions from the satellite retrievals of NO2.

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Section: Emission Comparisonssupporting

confidence: 91%

Section: We-canmentioning

confidence: 99%

Biomass burning nitrogen dioxide emissions derived from space with TROPOMI: methodology and validation

Griffin

McLinden

Dammers

et al. 2021

Preprint

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“…The WE‐CAN field campaign was based on Boise, ID, from July 24 to August 31 and Broomfield, CO from September 1 to 13, 2018. Nineteen flights were conducted by the NSF/NCAR C‐130 research aircraft approximately every 1–3 days and sampled smoke from fires across seven western states (Juncosa Calahorrano et al., 2021; Lindaas et al., 2021). Smoke plumes were typically sampled between 14:00 and 19:00 local time when burning conditions were most active.…”

Section: Methodsmentioning

confidence: 99%

Emissions of Trace Organic Gases From Western U.S. Wildfires Based on WE‐CAN Aircraft Measurements

et al. 2021

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We present emission measurements of volatile organic compounds (VOCs) for western U.S. wildland fires made on the NSF/NCAR C‐130 research aircraft during the Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE‐CAN) field campaign in summer 2018. VOCs were measured with complementary instruments onboard the C‐130, including a proton‐transfer‐reaction time‐of‐flight mass spectrometer (PTR‐ToF‐MS) and two gas chromatography (GC)‐based methods. Agreement within combined instrument uncertainties (<60%) was observed for most co‐measured VOCs. GC‐based measurements speciated the isomeric contributions to selected PTR‐ToF‐MS ion masses and generally showed little fire‐to‐fire variation. We report emission ratios (ERs) and emission factors (EFs) for 161 VOCs measured in 31 near‐fire smoke plume transects of 24 specific individual fires sampled in the afternoon when burning conditions are typically most active. Modified combustion efficiency (MCE) ranged from 0.85 to 0.94. The measured campaign‐average total VOC EF was 26.1 ± 6.9 g kg−1, approximately 67% of which is accounted for by oxygenated VOCs. The 10 most abundantly emitted species contributed more than half of the total measured VOC mass. We found that MCE alone explained nearly 70% of the observed variance for total measured VOC emissions (r2 = 0.67) and >50% for 57 individual VOC EFs representing more than half the organic carbon mass. Finally, we found little fire‐to‐fire variability for the mass fraction contributions of individual species to the total measured VOC emissions, suggesting that a single speciation profile can describe VOC emissions for the wildfires in coniferous ecosystems sampled during WE‐CAN.

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“…A companion manuscript by Calahorrano et al (2021) phase in association with NH 3 , they find that NO 2 oxidation by OH can account for ∼100% of the pNO 3 formation in the Taylor Creek plume, and ∼300% of the pNO 3 formation in Bear Trap. Possible reasons for the overestimation of pNO 3 increases could include an incomplete understanding of OH concentration evolution and uptake of HNO 3 by super-micron particles.…”

Section: Resultsmentioning

confidence: 92%

“…First, for most plumes, ΣNO z is more than 50% of ΣNO y . This is the case for even the first transect of the smoke plumes shown in Figure 4 and is a result of rapid oxidation of NO x in the first tens of minutes after emission (Calahorrano et al., 2021; Peng et al., 2020). Second, the p NH 4 fraction ranges widely between 0.1 and 0.9.…”

Section: Resultsmentioning

confidence: 93%

Empirical Insights Into the Fate of Ammonia in Western U.S. Wildfire Smoke Plumes

et al. 2021

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Wildfires are a major source of gas‐phase ammonia (NH3) to the atmosphere. Quantifying the evolution and fate of this NH3 is important to understanding the formation of secondary aerosol in smoke and its accompanying effects on radiative balance and nitrogen deposition. Here, we use data from the Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE‐CAN) to add new empirical constraints on the e‐folding loss timescale of NH3 and its relationship with particulate ammonium (pNH4) within wildfire smoke plumes in the western U.S. during summer 2018. We show that the e‐folding loss timescale of NH3 with respect to particle‐phase partitioning ranges from ∼24 to ∼4000 min (median of 55 min). Within these same plumes, oxidation of nitrogen oxides is observed concurrent with increases in the fraction of pNH4 in each plume sampled, suggesting that formation of ammonium nitrate (NH4NO3) is likely. We find wide variability in how close our in situ measurements of NH4NO3 are to those expected in a dry thermodynamic equilibrium, and find that NH4NO3 is most likely to form in fresh, dense smoke plumes injected at higher altitudes and colder temperatures. In chemically older smoke we observe correlations between both the fraction of pNH4 and the fraction of particulate nitrate (pNO3) in the aerosol with temperature, providing additional evidence of the presence of NH4NO3 and the influence of injection height on gas‐particle partitioning of NH3.

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Daytime Oxidized Reactive Nitrogen Partitioning in Western U.S. Wildfire Smoke Plumes

Abstract: Biomass burning directly impacts air quality, nutrient cycles, weather, and climate by releasing large amounts of trace gases and particulate matter into the atmosphere (

Cited by 46 publications

References 96 publications

Biomass burning nitrogen dioxide emissions derived from space with TROPOMI: methodology and validation

Biomass burning nitrogen dioxide emissions derived from space with TROPOMI: methodology and validation

Emissions of Trace Organic Gases From Western U.S. Wildfires Based on WE‐CAN Aircraft Measurements

Empirical Insights Into the Fate of Ammonia in Western U.S. Wildfire Smoke Plumes

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