Limited Long‐Term Photolysis of Stratospheric Organic Aerosols With Implications for CESM Modeling

Abstract Organic aerosol (OA) is an important constituent of the Earth's atmosphere, yet the extent of its destruction by photolysis remains an active research question. Recent laboratory studies reveal evidence for rapid short‐term photolysis for secondary OA, but the rate declines to negligible levels over time. Here we use the stratosphere to investigate long‐term OA photolysis because of the relatively simple sources and sinks of OA in this region. Airborne campaign observations show that the organic content in organic‐sulfate aerosols remains stable with altitude and time in the stratosphere, indicating no significant photolysis. Satellite observations of the 2020 Australian wildfires reveal OA persists over a year in the stratosphere, consistent with model simulations excluding long‐term photolysis. These findings suggest long‐term OA photolysis is negligible in the real atmosphere. The current Community Earth System Model (CESM) significantly underestimates the abundance of stratospheric OA due to assumed rapid photolysis. We add this well‐validated mechanism into CESM by turning off secondary OA photolysis after it is 50 days old, effectively simulating stratospheric OA consistent with observations. In summary, multiple lines of evidence confirm that the long‐term photolysis of OA is negligible or extremely slow. Incorporating this mechanism into CESM addresses a key model deficiency, improving simulation of stratospheric OA.

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Publication Details

Journal
Journal of Advances in Modeling Earth Systems
Published
2025-11-01
DOI
https://doi.org/10.1029/2025ms005084
Primary Topic
Atmospheric Ozone and Climate
Type
article
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article

Limited Long‐Term Photolysis of Stratospheric Organic Aerosols With Implications for CESM Modeling

Susan Solomon, Gregory P. Schill, Pengfei Yu, Simone Tilmes et al.
Journal of Advances in Modeling Earth Systems
Atmospheric Ozone and Climate
article

Limited Long‐Term Photolysis of Stratospheric Organic Aerosols With Implications for CESM Modeling

Susan Solomon, Gregory P. Schill, Pengfei Yu, Simone Tilmes, Jian Guan, Daniel M. Murphy, Douglas Edward Kinnison, Kane A. Stone, Michael J. Lawler
article en

Abstract

Abstract Organic aerosol (OA) is an important constituent of the Earth's atmosphere, yet the extent of its destruction by photolysis remains an active research question. Recent laboratory studies reveal evidence for rapid short‐term photolysis for secondary OA, but the rate declines to negligible levels over time. Here we use the stratosphere to investigate long‐term OA photolysis because of the relatively simple sources and sinks of OA in this region. Airborne campaign observations show that the organic content in organic‐sulfate aerosols remains stable with altitude and time in the stratosphere, indicating no significant photolysis. Satellite observations of the 2020 Australian wildfires reveal OA persists over a year in the stratosphere, consistent with model simulations excluding long‐term photolysis. These findings suggest long‐term OA photolysis is negligible in the real atmosphere. The current Community Earth System Model (CESM) significantly underestimates the abundance of stratospheric OA due to assumed rapid photolysis. We add this well‐validated mechanism into CESM by turning off secondary OA photolysis after it is 50 days old, effectively simulating stratospheric OA consistent with observations. In summary, multiple lines of evidence confirm that the long‐term photolysis of OA is negligible or extremely slow. Incorporating this mechanism into CESM addresses a key model deficiency, improving simulation of stratospheric OA.

Journal of Advances in Modeling Earth SystemsVol. 17(11)
NSF National Center for Atmospheric Research (US), Jinan University (CN), Cooperative Institute for Research in Environmental Sciences (US), University of Colorado Boulder (US), NOAA Chemical Sciences Laboratory (US), Massachusetts Institute of Technology (US)
Openalex Percentile: Top 61%
Atmospheric Ozone and Climate
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