Look Within: Intraplume Differences on Smoke Aerosol Aging Driven by Concentration Gradients

Abstract The evolution of organic aerosol (OA) composition and aerosol size distributions within smoke plumes are uncertain due to variability in the rates of OA evaporation/condensation and coagulation within a plume. It remains unclear how the evolution varies across different parts of individual plumes. We use a large eddy simulation model coupled with aerosol‐microphysics and radiation models to simulate the Williams Flats fire sampled during the Fire Influence on Regional to Global Environments and Air Quality field campaign. At aircraft altitude, the model captures observed aerosol changes through 4 hr of aging. The model evolution of primary OA (POA), oxidized POA (OPOA), and secondary OA (SOA) shows that >90% of the SOA formation occurs before the first transect (∼40 min of aging). Lidar observations and the model show a significant amount of smoke in the planetary boundary layer (PBL) and free troposphere (FT) with the model having equal amounts of smoke in the PBL and FT. Due to faster initial dilution, PBL concentrations are more than a factor of two lower than the FT concentrations, resulting in slower coagulational growth in the PBL. A 20 K temperature decrease with height in the PBL influences faster POA evaporation near the surface, while net OA evaporation in the FT is driven by continued dilution after the first aircraft transect. Net OA condensation in the PBL after the first transect is the result of areas with higher OH concentration leading to OPOA formation. Our results motivate the need for systematic observations of the vertical gradients of aerosol size and composition within smoke plumes.

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Publication Details

Journal
Journal of Geophysical Research Atmospheres
Published
2025-02-26
DOI
https://doi.org/10.1029/2024jd042359
Citations
1
Primary Topic
Atmospheric chemistry and aerosols
Type
article
Field-Weighted Citation Impact
1.30

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article

Look Within: Intraplume Differences on Smoke Aerosol Aging Driven by Concentration Gradients

Claire Robinson, Nicole A. June, Pedro Campuzano‐Jost, M. J. Alvarado et al.
1 citations
Journal of Geophysical Research Atmospheres
Atmospheric chemistry and aerosols
1.30
article

Look Within: Intraplume Differences on Smoke Aerosol Aging Driven by Concentration Gradients

Claire Robinson, Nicole A. June, Pedro Campuzano‐Jost, M. J. Alvarado, K. L. Thornhill, Taylor Shingler, Matthew Mitchell Coggon, Richard H. Moore, Marikate Mountain, Jeffrey R. Pierce, Jeff Peischl, Kevin J. Sanchez, Elizabeth B. Wiggins, Hongyu Guo, Demetrios Pagonis, Edward L. Winstead, Shantanu H. Jathar, Jose Luis Jimenez, Archana Dayalu
article en
1 citations

Abstract

Abstract The evolution of organic aerosol (OA) composition and aerosol size distributions within smoke plumes are uncertain due to variability in the rates of OA evaporation/condensation and coagulation within a plume. It remains unclear how the evolution varies across different parts of individual plumes. We use a large eddy simulation model coupled with aerosol‐microphysics and radiation models to simulate the Williams Flats fire sampled during the Fire Influence on Regional to Global Environments and Air Quality field campaign. At aircraft altitude, the model captures observed aerosol changes through 4 hr of aging. The model evolution of primary OA (POA), oxidized POA (OPOA), and secondary OA (SOA) shows that >90% of the SOA formation occurs before the first transect (∼40 min of aging). Lidar observations and the model show a significant amount of smoke in the planetary boundary layer (PBL) and free troposphere (FT) with the model having equal amounts of smoke in the PBL and FT. Due to faster initial dilution, PBL concentrations are more than a factor of two lower than the FT concentrations, resulting in slower coagulational growth in the PBL. A 20 K temperature decrease with height in the PBL influences faster POA evaporation near the surface, while net OA evaporation in the FT is driven by continued dilution after the first aircraft transect. Net OA condensation in the PBL after the first transect is the result of areas with higher OH concentration leading to OPOA formation. Our results motivate the need for systematic observations of the vertical gradients of aerosol size and composition within smoke plumes.

Journal of Geophysical Research AtmospheresVol. 130(5)
Weber State University (US), Langley Research Center (US), Cooperative Institute for Research in Environmental Sciences (US), University of Colorado Boulder (US), NOAA Chemical Sciences Laboratory (US), Science Systems and Applications (United States) (US), Atmospheric and Environmental Research (US), Colorado State University (US)
National Science Foundation, National Aeronautics and Space Administration, National Oceanic and Atmospheric Administration
Openalex Percentile: Top 25%
Atmospheric chemistry and aerosols
1.30
DOISourceOpenAlex
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