Large contribution of biomass burning emissions to ozone throughout the global remote troposphere
Creators
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Bourgeois, Ilann1, 2
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Peischl, Jeff1, 2
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Neuman, J. Andrew1, 2
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Brown, Steven S.2, 3
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Thompson, Chelsea R.1, 2
- Aikin, Kenneth C.1, 2
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Allen, Hannah M.4
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Angot, Hélène5
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Apel, Eric C.6
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Baublitz, Colleen B.7, 8
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Brewer, Jared F.9
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Campuzano-Jost, Pedro1, 3
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Commane, Róisín7, 8
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Crounse, John D.4
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Daube, Bruce C.9
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DiGangi, Joshua P.10
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Diskin, Glenn S.10
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Emmons, Louisa K.6
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Fiore, Arlene7, 8
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Gkatzelis, Georgios I.1, 2
- Hills, Alan6
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Hornbrook, Rebecca S.6
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Huey, L. Gregory11
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Jimenez, Jose L.1, 3
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Kim, Michelle4
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Lacey, Forrest6
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McKain, Kathryn1, 2
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Murray, Lee T.12
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Nault, Benjamin A.1, 3
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Parrish, David D.1, 2
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Ray, Eric1, 2
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Sweeney, Colm2
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Tanner, David11
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Wofsy, Steven C.9
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Ryerson, Thomas B.2
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1.
Cooperative Institute for Research in Environmental Sciences
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2.
National Oceanic and Atmospheric Administration
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3.
University of Colorado Boulder
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4.
California Institute of Technology
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5.
Institute of Arctic and Alpine Research
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6.
National Center for Atmospheric Research
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7.
Columbia University
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Lamont-Doherty Earth Observatory
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9.
Harvard University
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10.
Langley Research Center
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11.
Georgia Institute of Technology
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12.
University of Rochester
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.
Additional Information
© 2021 the Author(s). Published by PNAS. This open access article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND). Edited by Mark Thiemens, University of California San Diego, La Jolla, CA; received May 24, 2021; accepted November 3, 2021. We thank the ATom leadership team, science team, and DC-8 pilots and crew for contributions to the ATom measurements. ATom was funded in response to NASA ROSES-2013 NRA NNH13ZDA001N-EVS2. We acknowledge support from the US National Oceanic and Atmospheric Administration Atmospheric Chemistry, Carbon Cycle, and Climate (AC4) Program. This material is based upon work supported by the National Center for Atmospheric Research, which is a major facility sponsored by the NSF under Cooperative Agreement No. 1852977. We thank O. Cooper, E. Fischer, P. Wennberg, S. McKeen, and M. Trainer for helpful discussions. Author contributions: I.B. and T.B.R. designed research; I.B., J.P., J.A.N., S.S.B., C.R.T., H.M.A., E.C.A., C.B.B., J.F.B., P.C.-J., R.C., J.D.C., B.C.D., J.P.D., G.S.D., L.K.E., A.M.F., G.I.G., A.H., R.S.H., L.G.H., J.L.J., M.K., F.L., K.M., L.T.M., B.A.N., E.R., C.S., D.T., S.C.W., and T.B.R. performed research; D.D.P. contributed new reagents/analytic tools; I.B., J.P., J.A.N., S.S.B., C.R.T., K.C.A., H.M.A., H.A., E.C.A., C.B.B., J.F.B., P.C.-J., R.C., J.D.C., B.C.D., J.P.D., G.S.D., L.K.E., A.M.F., G.I.G., A.H., R.S.H., L.G.H., J.L.J., M.K., F.L., K.M., L.T.M., B.A.N., D.D.P., E.R., C.S., D.T., S.C.W., and T.B.R. analyzed data; and I.B., J.P., J.A.N., and S.S.B. wrote the paper. Data Availability Measurements and modeling work data have been deposited in https://daac.ornl.gov/ATOM/guides/ATom_merge.html (https://doi.org/10.3334/ORNLDAAC/1581). ATom and modeling work data used in this study are published through the Distributed Active Archive Center for Biogeochemical Dynamics. The authors declare no competing interest. This article is a PNAS Direct Submission. This article contains supporting information online at https://www.pnas.org/lookup/suppl/doi:10.1073/pnas.2109628118/-/DCSupplemental.Attached Files
Published - e2109628118.full.pdf
Supplemental Material - pnas.2109628118.sapp.pdf
Files
e2109628118.full.pdf
Additional details
Identifiers
- PMCID
- PMC8719870
- Eprint ID
- 112572
- Resolver ID
- CaltechAUTHORS:20211220-117169800
Related works
- Describes
- 10.3334/ORNLDAAC/1581 (DOI)
- https://daac.ornl.gov/ATOM/guides/ATom_merge.html (URL)
Funding
- NASA
- NNH13ZDA001N-EVS2
- National Oceanic and Atmospheric Administration (NOAA)
- NSF
- AGS-1852977
Dates
- Created
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2021-12-20Created from EPrint's datestamp field
- Updated
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2022-01-24Created from EPrint's last_modified field