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An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity

Carter, Therese S. and Heald, Colette L. and Kroll, Jesse H. and Apel, Eric C. and Blake, Donald and Coggon, Matthew and Edtbauer, Achim and Gkatzelis, Georgios and Hornbrook, Rebecca S. and Peischl, Jeff and Pfannerstill, Eva Y. and Piel, Felix and Reijrink, Nina G. and Ringsdorf, Akima and Warneke, Carsten and Williams, Jonathan and Wisthaler, Armin and Xu, Lu (2022) An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity. Atmospheric Chemistry and Physics, 22 (18). pp. 12093-12111. ISSN 1680-7324. doi:10.5194/acp-22-12093-2022.

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Fires emit a substantial amount of non-methane organic gases (NMOGs), the atmospheric oxidation of which can contribute to ozone and secondary particulate matter formation. However, the abundance and reactivity of these fire NMOGs are uncertain and historically not well constrained. In this work, we expand the representation of fire NMOGs in a global chemical transport model, GEOS-Chem. We update emission factors to Andreae (2019) and the chemical mechanism to include recent aromatic and ethene and ethyne model improvements (Bates et al., 2021; Kwon et al., 2021). We expand the representation of NMOGs by adding lumped furans to the model (including their fire emission and oxidation chemistry) and by adding fire emissions of nine species already included in the model, prioritized for their reactivity using data from the Fire Influence on Regional to Global Environments (FIREX) laboratory studies. Based on quantified emissions factors, we estimate that our improved representation captures 72 % of emitted, identified NMOG carbon mass and 49 % of OH reactivity from savanna and temperate forest fires, a substantial increase from the standard model (49 % of mass, 28 % of OH reactivity). We evaluate fire NMOGs in our model with observations from the Amazon Tall Tower Observatory (ATTO) in Brazil, Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) and DC3 in the US, and Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) in boreal Canada. We show that NMOGs, including furan, are well simulated in the eastern US with some underestimates in the western US and that adding fire emissions improves our ability to simulate ethene in boreal Canada. We estimate that fires provide 15 % of annual mean simulated surface OH reactivity globally, as well as more than 75 % over fire source regions. Over continental regions about half of this simulated fire reactivity comes from NMOG species. We find that furans and ethene are important globally for reactivity, while phenol is more important at a local level in the boreal regions. This is the first global estimate of the impact of fire on atmospheric reactivity.

Item Type:Article
Related URLs:
URLURL TypeDescription
Carter, Therese S.0000-0001-9124-4630
Heald, Colette L.0000-0003-2894-5738
Kroll, Jesse H.0000-0002-6275-521X
Apel, Eric C.0000-0001-9421-818X
Blake, Donald0000-0002-8283-5014
Coggon, Matthew0000-0002-5763-1925
Edtbauer, Achim0000-0001-8824-2132
Gkatzelis, Georgios0000-0002-4608-3695
Hornbrook, Rebecca S.0000-0002-6304-6554
Peischl, Jeff0000-0002-9320-7101
Pfannerstill, Eva Y.0000-0001-7715-1200
Ringsdorf, Akima0000-0002-1764-6516
Warneke, Carsten0000-0003-3811-8496
Williams, Jonathan0000-0001-5058-695X
Wisthaler, Armin0000-0001-5050-3018
Xu, Lu0000-0002-0021-9876
Additional Information:We thank Kelvin Bates for advice on implementing the aromatic hydrocarbon updates and ethene and ethyne chemistry that were not yet available in the standard GEOS-Chem model. We also thank Mat Evans for discussing source-attribution approaches. We acknowledge Tom Ryerson for making measurements of CO during FIREX-AQ and William Brune for OHR measurements and Teresa Campos for CO measurements during DC3. This research has been supported by the Division of Atmospheric and Geospace Sciences (NSF AGS grant no. 1936642 and cooperative agreement no. 1852977), the National Aeronautics and Space Administration (grant no. 80NSSC18K0633), the National Oceanic and Atmospheric Administration (grant no. NA17OAR4320101), and the Austrian Federal Ministry of Economy, Family and Youth (BMVIT, FFG, ASAP).
Funding AgencyGrant Number
National Oceanic and Atmospheric Administration (NOAA)NA17OAR4320101
Austrian Federal Ministry of Economy, Family and Youth (BMWFJ)UNSPECIFIED
Issue or Number:18
Record Number:CaltechAUTHORS:20220923-942198900.16
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:117130
Deposited By: Melissa Ray
Deposited On:04 Oct 2022 15:22
Last Modified:04 Oct 2022 15:22

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