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Abstract Wildfires emit mixtures of light‐absorbing aerosols (including black and brown carbon, BC and BrC, respectively) and more purely scattering organic aerosol (OA). BC, BrC, and OA interactions are complex and dynamic and evolve with aging in the atmosphere resulting in large uncertainties in their radiative forcing. We report microphysical, optical, and chemical measurements of multiple plumes from the Woodbury Fire (AZ, USA) observed at Los Alamos, NM, after 11–18 hr of atmospheric transit. This includes periods where the plumes exhibited little entrainment as well as periods that had become more dilute after mixing with background aerosol. Aerosol mass absorption cross sections (MAC) were enhanced by a factor of 1.5–2.2 greater than bare BC at 870 nm, suggesting lensing by nonabsorbing coatings following a core‐shell morphology. Larger MAC enhancement factors of 1.9–5.1 at 450 nm are greater than core‐shell morphology can explain and are attributed to BrC. MAC of OA (MACOrg) at 450 nm was largest in intact portions of the plumes (peak value bounded between 0.6 and 0.9 m2/g [Org]) and decreased with plume dilution. We report a strong correlation between MACOrg(450 nm) with the fC2H4O2(a tracer for levoglucosan‐like species) of coatings and of bulk OA indicating that BrC in the Woodbury Fire was coemitted with levoglucosan, a primary aerosol. fC2H4O2and MACOrg(450 nm) are shown to vary between the edge and the core of plumes, demonstrating enhanced oxidation of OA and BrC bleaching near plume edges. Our process‐level finding can inform parameterizations of mixed BC, BrC, and OA properties for wildfire plumes in climate models.
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Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition
Black carbon (BC) absorbs solar radiation, leading to a strong but uncertain warming effect on climate. A key challenge in modeling and quantifying BC’s radiative effect on climate is predicting enhancements in light absorption that result from internal mixing between BC and other aerosol components. Modeling and laboratory studies show that BC, when mixed with other aerosol components, absorbs more strongly than pure, uncoated BC; however, some ambient observations suggest more variable and weaker absorption enhancement. We show that the lower-than-expected enhancements in ambient measurements result from a combination of two factors. First, the often used spherical, concentric core-shell approximation generally overestimates the absorption by BC. Second, and more importantly, inadequate consideration of heterogeneity in particle-to-particle composition engenders substantial overestimation in absorption by the total particle population, with greater heterogeneity associated with larger model–measurement differences. We show that accounting for these two effects—variability in per-particle composition and deviations from the core-shell approximation—reconciles absorption enhancement predictions with laboratory and field observations and resolves the apparent discrepancy. Furthermore, our consistent model framework provides a path forward for improving predictions of BC’s radiative effect on climate.
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- Award ID(s):
- 1638307
- PAR ID:
- 10193704
- Date Published:
- Journal Name:
- Proceedings of the National Academy of Sciences
- Volume:
- 117
- Issue:
- 10
- ISSN:
- 0027-8424
- Page Range / eLocation ID:
- 5196 to 5203
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1073/pnas.1919723117
