Two-years of stratospheric chemistry perturbations from the 2019–2020 Australian wildfire smoke

<p>The very large pyrocumulonimbus events that occurred during the Australian summer of 2019–2020 caused extremely unusual partitioning of stratospheric chlorine in the Southern Hemisphere midlatitude and Antarctic regions not only in 2020 but also in 2021. This was likely caused by enhanced H...

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Main Authors: K. Stone, S. Solomon, P. Yu, D. M. Murphy, D. Kinnison, J. Guan
Format: Article
Language:English
Published: Copernicus Publications 2025-07-01
Series:Atmospheric Chemistry and Physics
Online Access:https://acp.copernicus.org/articles/25/7683/2025/acp-25-7683-2025.pdf
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author K. Stone
S. Solomon
P. Yu
D. M. Murphy
D. Kinnison
J. Guan
author_facet K. Stone
S. Solomon
P. Yu
D. M. Murphy
D. Kinnison
J. Guan
author_sort K. Stone
collection DOAJ
description <p>The very large pyrocumulonimbus events that occurred during the Australian summer of 2019–2020 caused extremely unusual partitioning of stratospheric chlorine in the Southern Hemisphere midlatitude and Antarctic regions not only in 2020 but also in 2021. This was likely caused by enhanced HCl solubility in organic species that increased heterogeneous chemistry. Here, we show that observed HCl and <span class="inline-formula">ClONO<sub>2</sub></span> values remain outside the pre-wildfire satellite range, measured from 2005 until just prior to the event, in both the Southern Hemisphere midlatitude and Antarctic regions in 2021. Through model simulations, we replicate this prolonged multiyear chemical perturbation, in good agreement with observations. This was achieved by calculating the HCl solubility in mixed wildfire and sulfate aerosols consistent with assumptions of (1) liquid–liquid phase separation and (2) linear dependence on organic and sulfate composition. The model simulations also suggest that the Australian pyrocumulonimbus organic aerosols contributed to low midlatitude ozone values in 2020 and 2021. A marked, photochemically controlled seasonality of the chemical perturbations and ozone depletion is also observed and simulated, and its underlying chemical drivers are identified. This work highlights that lower concentrations of smoke still had profound effects on stratospheric heterogeneous chemistry more than a year after the 2019–2020 wildfire event.</p>
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issn 1680-7316
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spelling doaj-art-a2012eebe6684917aec8ef141b4649142025-08-20T03:29:57ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242025-07-01257683769710.5194/acp-25-7683-2025Two-years of stratospheric chemistry perturbations from the 2019–2020 Australian wildfire smokeK. Stone0S. Solomon1P. Yu2D. M. Murphy3D. Kinnison4J. Guan5Department of Earth, Atmospheric, and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA 02139, USADepartment of Earth, Atmospheric, and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA 02139, USAInstitute for Environmental and Climate Research, College of Environment and Climate, Jinan University, Guangzhou, ChinaChemical Sciences Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305, USAAtmospheric Chemistry Observations & Modeling Laboratory, NSF National Center for Atmospheric Research, Boulder, CO 80307, USADepartment of Earth, Atmospheric, and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA 02139, USA<p>The very large pyrocumulonimbus events that occurred during the Australian summer of 2019–2020 caused extremely unusual partitioning of stratospheric chlorine in the Southern Hemisphere midlatitude and Antarctic regions not only in 2020 but also in 2021. This was likely caused by enhanced HCl solubility in organic species that increased heterogeneous chemistry. Here, we show that observed HCl and <span class="inline-formula">ClONO<sub>2</sub></span> values remain outside the pre-wildfire satellite range, measured from 2005 until just prior to the event, in both the Southern Hemisphere midlatitude and Antarctic regions in 2021. Through model simulations, we replicate this prolonged multiyear chemical perturbation, in good agreement with observations. This was achieved by calculating the HCl solubility in mixed wildfire and sulfate aerosols consistent with assumptions of (1) liquid–liquid phase separation and (2) linear dependence on organic and sulfate composition. The model simulations also suggest that the Australian pyrocumulonimbus organic aerosols contributed to low midlatitude ozone values in 2020 and 2021. A marked, photochemically controlled seasonality of the chemical perturbations and ozone depletion is also observed and simulated, and its underlying chemical drivers are identified. This work highlights that lower concentrations of smoke still had profound effects on stratospheric heterogeneous chemistry more than a year after the 2019–2020 wildfire event.</p>https://acp.copernicus.org/articles/25/7683/2025/acp-25-7683-2025.pdf
spellingShingle K. Stone
S. Solomon
P. Yu
D. M. Murphy
D. Kinnison
J. Guan
Two-years of stratospheric chemistry perturbations from the 2019–2020 Australian wildfire smoke
Atmospheric Chemistry and Physics
title Two-years of stratospheric chemistry perturbations from the 2019–2020 Australian wildfire smoke
title_full Two-years of stratospheric chemistry perturbations from the 2019–2020 Australian wildfire smoke
title_fullStr Two-years of stratospheric chemistry perturbations from the 2019–2020 Australian wildfire smoke
title_full_unstemmed Two-years of stratospheric chemistry perturbations from the 2019–2020 Australian wildfire smoke
title_short Two-years of stratospheric chemistry perturbations from the 2019–2020 Australian wildfire smoke
title_sort two years of stratospheric chemistry perturbations from the 2019 2020 australian wildfire smoke
url https://acp.copernicus.org/articles/25/7683/2025/acp-25-7683-2025.pdf
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