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Rapid evolution of aerosol particles and their optical properties downwind of wildfires in the western US

Journal Article · · Atmospheric Chemistry and Physics (Online)
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Abstract. During the first phase of the Biomass Burn Operational Project (BBOP) field campaign, conducted in the Pacific Northwest, the DOE G-1 aircraft was used to follow the time evolution of wildfire smoke from near the point of emission to locations 2–3.5 h downwind. In nine flights we made repeated transects of wildfire plumes at varying downwind distances and could thereby follow the plume's time evolution. On average there was little change in dilution-normalized aerosol mass concentration as a function of downwind distance. This consistency hides a dynamic system in which primary aerosol particles are evaporating and secondary ones condensing. Organic aerosol is oxidized as a result. On all transects more than 90 % of aerosol is organic. In freshly emitted smoke aerosol, NH4+ is approximately equivalent to NO3. After 2 h of daytime aging, NH4+ increased and is approximately equivalent to the sum of Cl, SO42, and NO3. Particle size increased with downwind distance, causing particles to be more efficient scatters. Averaged over nine flights, mass scattering efficiency (MSE) increased in ∼ 2 h by 56 % and doubled in one flight. Mechanisms for redistributing mass from small to large particles are discussed. Coagulation is effective at moving aerosol from the Aitken to accumulation modes but yields only a minor increase in MSE. As absorption remained nearly constant with age, the time evolution of single scatter albedo was controlled by age-dependent scattering. Near-fire aerosol had a single scatter albedo (SSA) of 0.8–0.9. After 1 to 2 h of aging SSAs were typically 0.9 and greater. Assuming global-average surface and atmospheric conditions, the observed age dependence in SSA would change the direct radiative effect of a wildfire plume from near zero near the fire to a cooling effect downwind.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
Global Environment Research Fund of the Japanese Ministry of the Environment; Japan Society for the Promotion of Science (JSPS); Japanese Ministry of the Environment; NOAA; National Aeronautic and Space Administration (NASA); National Aeronautics and Space Administration (NASA); National Oceanic and Atmospheric Administration (NOAA); National Science Foundation (NSF); USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
AC05-76RL01830; SC0012704; SC0014287; SC0019000
OSTI ID:
1712491
Alternate ID(s):
OSTI ID: 1721685
OSTI ID: 1693390
Report Number(s):
BNL--220014-2020-JAAM; PNNL-SA--152046
Journal Information:
Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 21 Vol. 20; ISSN 1680-7324
Publisher:
European Geosciences UnionCopyright Statement
Country of Publication:
Germany
Language:
English

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