Airborne Observations Constrain Heterogeneous Nitrogen and Halogen Chemistry on Tropospheric and Stratospheric Biomass Burning Aerosol
2024
Decker, Zachary C. J. | Novak, Gordon A. | Aikin, Kenneth | Veres, Patrick R. | Neuman, J. Andrew | Bourgeois, Ilann | Bui, T. Paul | Campuzano‐Jost, Pedro | Coggon, Matthew M. | Day, Douglas A. | DiGangi, Joshua P. | Diskin, Glenn S. | Dollner, Maximilian | Franchin, Alessandro | Fredrickson, Carley D. | Froyd, Karl D. | Gkatzelis, Georgios I. | Guo, Hongyu | Hall, Samuel R. | Halliday, Hannah | Hayden, Katherine | Holmes, Christopher D. | Jimenez, Jose L. | Kupc, Agnieszka | Lindaas, Jakob | Middlebrook, Ann M. | Moore, Richard H. | Nault, Benjamin A. | Nowak, John B. | Pagonis, Demetrios | Palm, Brett B. | Peischl, Jeff | Piel, Felix M. | Rickly, Pamela S. | Robinson, Michael A. | Rollins, Andrew W. | Ryerson, Thomas B. | Schill, Gregory P. | Sekimoto, Kanako | Thompson, Chelsea R. | Thornhill, Kenneth L. | Thornton, Joel A. | Ullmann, Kirk | Warneke, Carsten | Washenfelder, Rebecca A. | Weinzierl, Bernadett | Wiggins, Elizabeth B. | Williamson, Christina J. | Winstead, Edward L. | Wisthaler, Armin | Womack, Caroline C. | Brown, Steven S. | Ilmatieteen laitos | Finnish Meteorological Institute | 0000-0002-5188-9378
Heterogeneous 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.
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