Large contribution of biomass burning emissions to ozone throughout the global remote troposphere

Ilann Bourgeois; Jeff Peischl; J Andrew Neuman; Steven S Brown; Chelsea R Thompson; Kenneth C Aikin; Hannah M Allen; Hélène Angot; Eric C Apel; Colleen B Baublitz; Jared F Brewer; Pedro Campuzano-Jost; Róisín Commane; John D Crounse; Bruce C Daube; Joshua P DiGangi; Glenn S Diskin; Louisa K Emmons; Arlene M Fiore; Georgios I Gkatzelis; Alan Hills; Rebecca S Hornbrook; L Gregory Huey; Jose L Jimenez; Michelle Kim; Forrest Lacey; Kathryn McKain; Lee T Murray; Benjamin A Nault; David D Parrish; Eric Ray; Colm Sweeney; David Tanner; Steven C Wofsy; Thomas B Ryerson

doi:10.1073/pnas.2109628118

Large contribution of biomass burning emissions to ozone throughout the global remote troposphere

Proc Natl Acad Sci U S A. 2021 Dec 28;118(52):e2109628118. doi: 10.1073/pnas.2109628118.

Authors

Ilann Bourgeois^{1

2}, Jeff Peischl^{1

2}, J Andrew Neuman^{3

2}, Steven S Brown^{2

4}, Chelsea R Thompson^{3

2}, Kenneth C Aikin^{3

2}, Hannah M Allen⁵, Hélène Angot⁶, Eric C Apel⁷, Colleen B Baublitz^{8

9}, Jared F Brewer¹⁰, Pedro Campuzano-Jost^{3

4}, Róisín Commane^{8

9}, John D Crounse¹¹, Bruce C Daube¹⁰, Joshua P DiGangi¹², Glenn S Diskin¹², Louisa K Emmons⁷, Arlene M Fiore^{8

9}, Georgios I Gkatzelis^{3

2}, Alan Hills⁷, Rebecca S Hornbrook⁷, L Gregory Huey¹³, Jose L Jimenez^{3

4}, Michelle Kim¹¹, Forrest Lacey⁷, Kathryn McKain^{3

14}, Lee T Murray¹⁵, Benjamin A Nault^{3

4}, David D Parrish^{3

2}, Eric Ray^{3

2}, Colm Sweeney¹⁴, David Tanner¹³, Steven C Wofsy¹⁰, Thomas B Ryerson²

Affiliations

¹ Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309; [email protected] [email protected].
² National Oceanic and Atmospheric Administration Chemical Sciences Laboratory, Boulder, CO 80305.
³ Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309.
⁴ Department of Chemistry, University of Colorado, Boulder, CO 80309.
⁵ Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125.
⁶ Institute of Arctic and Alpine Research, University of Colorado, Boulder, CO 80309.
⁷ Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO 80301.
⁸ Department of Earth and Environmental Sciences, Columbia University, Palisades, NY 10964.
⁹ Lamont-Doherty Earth Observatory, Columbia University, Palisades, NY 10964.
¹⁰ School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138.
¹¹ Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125.
¹² NASA Langley Research Center, Hampton, VA 23681.
¹³ School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30332.
¹⁴ National Oceanic and Atmospheric Administration Global Monitoring Laboratory, Boulder, CO 80305.
¹⁵ Department of Earth and Environmental Sciences, University of Rochester, Rochester, NY 14627.

Abstract

Ozone is the third most important anthropogenic greenhouse gas after carbon dioxide and methane but has a larger uncertainty in its radiative forcing, in part because of uncertainty in the source characteristics of ozone precursors, nitrogen oxides, and volatile organic carbon that directly affect ozone formation chemistry. Tropospheric ozone also negatively affects human and ecosystem health. Biomass burning (BB) and urban emissions are significant but uncertain sources of ozone precursors. Here, we report global-scale, in situ airborne measurements of ozone and precursor source tracers from the NASA Atmospheric Tomography mission. Measurements from the remote troposphere showed that tropospheric ozone is regularly enhanced above background in polluted air masses in all regions of the globe. Ozone enhancements in air with high BB and urban emission tracers (2.1 to 23.8 ppbv [parts per billion by volume]) were generally similar to those in BB-influenced air (2.2 to 21.0 ppbv) but larger than those in urban-influenced air (-7.7 to 6.9 ppbv). Ozone attributed to BB was 2 to 10 times higher than that from urban sources in the Southern Hemisphere and the tropical Atlantic and roughly equal to that from urban sources in the Northern Hemisphere and the tropical Pacific. Three independent global chemical transport models systematically underpredict the observed influence of BB on tropospheric ozone. Potential reasons include uncertainties in modeled BB injection heights and emission inventories, export efficiency of BB emissions to the free troposphere, and chemical mechanisms of ozone production in smoke. Accurately accounting for intermittent but large and widespread BB emissions is required to understand the global tropospheric ozone burden.

Keywords: ATom; biomass burning; ozone; troposphere; urban.

Publication types

Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

Air Pollutants* / analysis
Air Pollutants* / chemistry
Air Pollution*
Atmosphere
Biomass*
Ecosystem
Fires
Ozone* / analysis
Ozone* / chemistry

Substances

Air Pollutants
Ozone