Dilution impacts on smoke aging: evidence in Biomass Burning Observation Project (BBOP) data
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Published:2021-05-05
Issue:9
Volume:21
Page:6839-6855
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Hodshire Anna L.ORCID, Ramnarine Emily, Akherati AliORCID, Alvarado Matthew L., Farmer Delphine K.ORCID, Jathar Shantanu H.ORCID, Kreidenweis Sonia M.ORCID, Lonsdale Chantelle R., Onasch Timothy B.ORCID, Springston Stephen R.ORCID, Wang JianORCID, Wang YangORCID, Kleinman Lawrence I.ORCID, Sedlacek III Arthur J.ORCID, Pierce Jeffrey R.ORCID
Abstract
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 observed variability in smoke evolution. Here, we use
observational data from the Biomass Burning
Observation Project (BBOP) field campaign and show that initial smoke
organic aerosol mass concentrations can help predict changes in smoke
aerosol aging markers, number concentration, and number mean diameter
between 40–262 nm. Because initial field measurements of plumes are
generally >10 min downwind, smaller plumes will have already
undergone substantial dilution relative to larger plumes and have lower
concentrations of smoke species at these observations closest to the fire.
The extent to which dilution has occurred prior to the first observation is
not a directly measurable quantity. We show that initial observed plume
concentrations can serve as a rough indicator of the extent of dilution
prior to the first measurement, which impacts photochemistry, aerosol
evaporation, and coagulation. Cores of plumes have higher concentrations
than edges. By segregating the observed plumes into cores and edges, we find
evidence that particle aging, evaporation, and coagulation occurred before
the first measurement. We further find that on the plume edges, the organic
aerosol is more oxygenated, while a marker for primary biomass burning
aerosol emissions has decreased in relative abundance compared to the plume
cores. Finally, we attempt to decouple the roles of the initial
concentrations and physical age since emission by performing multivariate
linear regression of various aerosol properties (composition, size) on these
two factors.
Funder
Climate Program Office National Science Foundation Office of Science
Publisher
Copernicus GmbH
Subject
Atmospheric Science
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