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Abstract Wildfires emit large amounts of black carbon and light-absorbing organic carbon, known as brown carbon, into the atmosphere. These particles perturb Earth’s radiation budget through absorption of incoming shortwave radiation. It is generally thought that brown carbon loses its absorptivity after emission in the atmosphere due to sunlight-driven photochemical bleaching. Consequently, the atmospheric warming effect exerted by brown carbon remains highly variable and poorly represented in climate models compared with that of the relatively nonreactive black carbon. Given that wildfires are predicted to increase globally in the coming decades, it is increasingly important to quantify these radiative impacts. Here we present measurements of ensemble-scale and particle-scale shortwave absorption in smoke plumes from wildfires in the western United States. We find that a type of dark brown carbon contributes three-quarters of the short visible light absorption and half of the long visible light absorption. This strongly absorbing organic aerosol species is water insoluble, resists daytime photobleaching and increases in absorptivity with night-time atmospheric processing. Our findings suggest that parameterizations of brown carbon in climate models need to be revised to improve the estimation of smoke aerosol radiative forcing and associated warming. 

Abstract. During the first phase of the Biomass Burn Operational Project (BBOP) fieldcampaign, conducted in the Pacific Northwest, the DOE G-1 aircraft was usedto follow the time evolution of wildfire smoke from near the point ofemission to locations 2–3.5 h downwind. In nine flights we maderepeated transects of wildfire plumes at varying downwind distances andcould thereby follow the plume's time evolution. On average there was littlechange in dilution-normalized aerosol mass concentration as a function ofdownwind distance. This consistency hides a dynamic system in which primaryaerosol particles are evaporating and secondary ones condensing. Organicaerosol is oxidized as a result. On all transects more than 90 % ofaerosol is organic. In freshly emitted smoke aerosol, NH4+ isapproximately equivalent to NO3. After 2 h of daytime aging, NH4+ increased and is approximately equivalent tothe 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 movingaerosol from the Aitken to accumulation modes but yields only a minor increase in MSE. As absorption remained nearly constant with age, the timeevolution of single scatter albedo was controlled by age-dependentscattering. 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 observedage dependence in SSA would change the direct radiative effect of a wildfire plume from near zero near the fire to a cooling effect downwind.