06 Apr 2020

06 Apr 2020

Review status: a revised version of this preprint is currently under review for the journal ACP.

Dilution impacts on smoke aging: Evidence in BBOP data

Anna L. Hodshire1, Emily Ramnarine1, Ali Akherati2, Matthew L. Alvarado3, Delphine K. Farmer4, Shantanu H. Jathar2, Sonia M. Kreidenweis1, Chantelle R. Lonsdale3, Timothy B. Onasch5, Stephen R. Springston6, Jian Wang6,a, Yang Wang7,b, Lawrence I. Kleinman6, Arthur J. Sedlacek III6, and Jeffrey R. Pierce1 Anna L. Hodshire et al.
  • 1Department of Atmospheric Science, Colorado State University, Fort Collins, CO80523, United States
  • 2Department of Mechanical Engineering, Colorado State University, Fort Collins, CO80523, United States
  • 3Atmospheric and Environmental Research, Inc., Lexington, MA02421, United States
  • 4Department of Chemistry, Colorado State University, Fort Collins, CO80523, United States
  • 5Aerodyne Research Inc., Billerica, MA01821, United States
  • 6Environmental and Climate Sciences Department, Brookhaven National Laboratory, Upton, NY11973, United States
  • 7Center for Aerosol Science and Engineering, Washington University, St. Louis, MO63130, United States
  • anow at: Center for Aerosol Science and Engineering, Washington University, St. Louis, MO 63130, United States
  • bnow at: Department of Civil, Architectural and Environmental Engineering, Missouri University of Science and Technology, Rolla, Missouri 65409, United States

Abstract. Biomass burning emits vapors and aerosols into the atmosphere that can rapidly evolve as smoke plumes travel downwind and dilute, affecting climate- and health-relevant properties of the smoke. To date, theory has been unable to explain variability in smoke evolution. Here, we use observational data from the BBOP field campaign and show that initial smoke concentrations can help predict changes in smoke aerosol aging markers, number, and diameter. Because initial field measurements of plumes are generally > 10 minutes downwind, smaller plumes will have already undergone substantial dilution relative to larger plumes. However, the extent to which dilution has occurred prior to the first observation is not a measurable quantity. Hence, initial observed concentrations can serve as an indicator of dilution, which impacts photochemistry and aerosol evaporation. Cores of plumes have higher concentrations than edges. By segregating the observed plumes into cores and edges, we infer that particle aging, evaporation, and coagulation occurred before the first measurement, and we find that edges generally undergo higher increases in oxidation tracers, more decreases in semivolatile compounds, and less coagulation than the cores.

Anna L. Hodshire et al.

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Status: final response (author comments only)
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Anna L. Hodshire et al.

Anna L. Hodshire et al.


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Short summary
Biomass burning emits particles and vapors that can impact both health and climate. Here, we investigate the role of dilution in the evolution of aerosol size and composition in observed US wildfire smoke plumes. Centers of plumes dilute more slowly than edges. We see differences in concentrations and composition between the centers and edges both in the first measurement and in subsequent measurements. Our findings support the hypothesis that plume dilution influences smoke aging.