Airborne Observations Constrain Heterogeneous Nitrogen and Halogen Chemistry on Tropospheric and Stratospheric Biomass Burning Aerosol

Author:

Decker Zachary C. J.1234ORCID,Novak Gordon A.12,Aikin Kenneth12ORCID,Veres Patrick R.15,Neuman J. Andrew12,Bourgeois Ilann126,Bui T. Paul7ORCID,Campuzano‐Jost Pedro23ORCID,Coggon Matthew M.12ORCID,Day Douglas A.23ORCID,DiGangi Joshua P.8ORCID,Diskin Glenn S.8ORCID,Dollner Maximilian9ORCID,Franchin Alessandro1210,Fredrickson Carley D.11ORCID,Froyd Karl D.12ORCID,Gkatzelis Georgios I.1212ORCID,Guo Hongyu23,Hall Samuel R.10ORCID,Halliday Hannah8ORCID,Hayden Katherine13,Holmes Christopher D.14ORCID,Jimenez Jose L.23ORCID,Kupc Agnieszka129,Lindaas Jakob15ORCID,Middlebrook Ann M.1,Moore Richard H.8ORCID,Nault Benjamin A.16ORCID,Nowak John B.8ORCID,Pagonis Demetrios2317,Palm Brett B.511ORCID,Peischl Jeff12ORCID,Piel Felix M.1819,Rickly Pamela S.1220,Robinson Michael A.123ORCID,Rollins Andrew W.1ORCID,Ryerson Thomas B.1ORCID,Schill Gregory P.1ORCID,Sekimoto Kanako21,Thompson Chelsea R.1ORCID,Thornhill Kenneth L.822ORCID,Thornton Joel A.11ORCID,Ullmann Kirk10ORCID,Warneke Carsten1ORCID,Washenfelder Rebecca A.123,Weinzierl Bernadett9ORCID,Wiggins Elizabeth B.8ORCID,Williamson Christina J.122425,Winstead Edward L.822ORCID,Wisthaler Armin1819ORCID,Womack Caroline C.12,Brown Steven S.13ORCID

Affiliation:

1. NOAA Chemical Sciences Laboratory (CSL) Boulder CO USA

2. Cooperative Institute for Research in Environmental Sciences University of Colorado Boulder Boulder CO USA

3. Department of Chemistry University of Colorado Boulder Boulder CO USA

4. Now at Laboratory of Atmospheric Chemistry Paul Scherrer Institute (PSI) Villigen Switzerland

5. Now at National Center for Atmospheric Research Boulder CO USA

6. Now at Université Savoie Mont Blanc INRAE CARRTEL Thonon‐les‐Bains France

7. NASA Ames Research Center Moffett Field CA USA

8. NASA Langley Research Center Hampton VA USA

9. Faculty of Physics Aerosol Physics and Environmental Physics University of Vienna Vienna Austria

10. Atmospheric Chemistry Observations and Modeling Laboratory National Center for Atmospheric Research Boulder CO USA

11. Department of Atmospheric Sciences University of Washington Seattle WA USA

12. Now at Institute of Energy and Climate Research IEK‐8: Troposphere Forschungszentrum Jülich GmbH Jülich Germany

13. Air Quality Research Division (AQRD) Environment and Climate Change Canada Toronto ON Canada

14. Department of Earth, Ocean, and Atmospheric Science Florida State University Tallahassee FL USA

15. Department of Atmospheric Science Colorado State University Fort Collins CO USA

16. Center for Aerosol and Cloud Chemistry Aerodyne Research, Inc. Billerica MA USA

17. Now at Department of Chemistry and Biochemistry Weber State University Ogden UT USA

18. Institute for Ion Physics and Applied Physics University of Innsbruck Innsbruck Austria

19. Department of Chemistry University of Oslo Oslo Norway

20. Now at Colorado Department of Public Health and Environment Denver CO USA

21. Graduate School of Nanobioscience Yokohama City University Yokohama Japan

22. Science Systems and Applications, Inc. (SSAI) Hampton VA USA

23. Now at Cooperative Institute for Research in Environmental Sciences University of Colorado Boulder Boulder CO USA

24. Now at Finnish Meteorological Institute Helsinki Finland

25. Now at Institute for Atmospheric and Earth System Research/Physics Faculty of Science University of Helsinki Helsinki Finland

Abstract

AbstractHeterogeneous chemical cycles of pyrogenic nitrogen and halides influence tropospheric ozone and affect the stratosphere during extreme Pyrocumulonimbus (PyroCB) events. We report field‐derived N2O5 uptake coefficients, γ(N2O5), and ClNO2 yields, φ(ClNO2), from two aircraft campaigns observing fresh smoke in the lower and mid troposphere and processed/aged smoke in the upper troposphere and lower stratosphere (UTLS). Derived φ(ClNO2) varied across the full 0–1 range but was typically <0.5 and smallest in a PyroCB (<0.05). Derived γ(N2O5) was low in agricultural smoke (0.2–3.6 × 10−3), extremely low in mid‐tropospheric wildfire smoke (0.1 × 10−3), but larger in PyroCB processed smoke (0.7–5.0 × 10−3). Aged biomass burning aerosol in the UTLS had a higher γ(N2O5) of 17 × 10−3 that increased with sulfate and liquid water, but that was 1–2 orders of magnitude lower than values for aqueous sulfuric aerosol used in stratospheric models.

Publisher

American Geophysical Union (AGU)

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