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Abstract. Biomass burning emits vapors and aerosols into the atmosphere thatcan rapidly evolve as smoke plumes travel downwind and dilute, affectingclimate- and health-relevant properties of the smoke. To date, theory hasbeen unable to explain observed variability in smoke evolution. Here, we useobservational data from the Biomass BurningObservation Project (BBOP) field campaign and show that initial smokeorganic aerosol mass concentrations can help predict changes in smokeaerosol aging markers, number concentration, and number mean diameterbetween 40–262 nm. Because initial field measurements of plumes aregenerally >10 min downwind, smaller plumes will have alreadyundergone substantial dilution relative to larger plumes and have lowerconcentrations of smoke species at these observations closest to the fire.The extent to which dilution has occurred prior to the first observation isnot a directly measurable quantity. We show that initial observed plumeconcentrations can serve as a rough indicator of the extent of dilutionprior to the first measurement, which impacts photochemistry, aerosolevaporation, and coagulation. Cores of plumes have higher concentrationsthan edges. By segregating the observed plumes into cores and edges, we findevidence that particle aging, evaporation, and coagulation occurred beforethe first measurement. We further find that on the plume edges, the organicaerosol is more oxygenated, while a marker for primary biomass burningaerosol emissions has decreased in relative abundance compared to the plumecores. Finally, we attempt to decouple the roles of the initialconcentrations and physical age since emission by performing multivariatelinear regression of various aerosol properties (composition, size) on thesetwo factors. 

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. 

Abstract. Observations of the organic components of the natural aerosol are scarce in Antarctica, which limits our understanding of natural aerosols and their connection to seasonal and spatial patterns of cloud albedo in the region. From November 2015 to December 2016, the ARM West Antarctic Radiation Experiment (AWARE) measured submicron aerosol properties near McMurdo Station at the southern tip of Ross Island. Submicron organic mass (OM), particle number, and cloud condensation nuclei concentrations were higher in summer than other seasons. The measurements included a range of compositions and concentrations that likely reflected both local anthropogenic emissions and natural background sources. We isolated the natural organic components by separating a natural factor and a local combustion factor. The natural OM was 150 times higher in summer than in winter. The local anthropogenic emissions were not hygroscopic and had little contribution to the CCN concentrations. Natural sources that included marine sea spray and seabird emissions contributed 56% OM in summer but only 3% in winter. The natural OM had high hydroxyl group fraction (55%), 6% alkane, and 6% amine group mass, consistent with marine organic composition. In addition, the Fourier transform infrared (FTIR) spectra showed the natural sources of organic aerosol were characterized by amide group absorption, which may be from seabird populations. Carboxylic acid group contributions were high in summer and associated with natural sources, likely forming by secondary reactions. 

Abstract. Urbanization and deforestation have important impacts on atmosphericparticulate matter (PM) over Amazonia. This study presents observations andanalysis of PM₁ concentration, composition, and opticalproperties in central Amazonia during the dry season, focusing on theanthropogenic impacts. The primary study site was located 70 km downwind ofManaus, a city of over 2 million people in Brazil, as part of theGoAmazon2014/5 experiment. A high-resolution time-of-flight aerosol massspectrometer (AMS) provided data on PM₁ composition, and aethalometermeasurements were used to derive the absorption coefficient b_abs,BrC ofbrown carbon (BrC) at 370 nm. Non-refractory PM₁ mass concentrationsaveraged 12.2 µg m⁻³ at the primary study site, dominated byorganics (83 %), followed by sulfate (11 %). A decrease inb_abs,BrC was observed as the mass concentration of nitrogen-containingorganic compounds decreased and the organic PM₁ O:C ratio increased,suggesting atmospheric bleaching of the BrC components. The organic PM₁was separated into six different classes by positive-matrix factorization(PMF), and the mass absorption efficiency E_abs associated with eachfactor was estimated through multivariate linear regression ofb_abs,BrC on the factor loadings. The largest E_abs values wereassociated with urban (2.04±0.14 m² g⁻¹) and biomass-burning(0.82±0.04 to 1.50±0.07 m² g⁻¹) sources. Together, these sources contributed at least 80 % ofb_abs,BrC while accounting for 30 % to 40 % of the organic PM₁ massconcentration. In addition, a comparison of organic PM₁ compositionbetween wet and dry seasons revealed that only part of the 9-foldincrease in mass concentration between the seasons can be attributed tobiomass burning. Biomass-burning factor loadings increased by 30-fold,elevating its relative contribution to organic PM₁ from about 10 % inthe wet season to 30 % in the dry season. However, most of the PM₁mass (>60 %) in both seasons was accounted for by biogenicsecondary organic sources, which in turn showed an 8-fold seasonalincrease in factor loadings. A combination of decreased wet deposition andincreased emissions and oxidant concentrations, as well as a positivefeedback on larger mass concentrations are thought to play a role in theobserved increases. Furthermore, fuzzy c-means clustering identified threeclusters, namely “baseline”, “event”, and “urban” to representdifferent pollution influences during the dry season. The baseline cluster,representing the dry season background, was associated with a mean massconcentration of 9±3 µg m⁻³. This concentration increasedon average by 3 µg m⁻³ for both the urban and the event clusters.The event cluster, representing an increased influence of biomass burningand long-range transport of African volcanic emissions, was characterized byremarkably high sulfate concentrations. The urban cluster, representing theinfluence of Manaus emissions on top of the baseline, was characterized byan organic PM₁ composition that differed from the other two clusters.The differences discussed suggest a shift in oxidation pathways as well asan accelerated oxidation cycle due to urban emissions, in agreement withfindings for the wet season.

 

We present OH observations made in Amazonas, Brazil during the Green Ocean Amazon campaign (GoAmazon2014/5) from February to March of 2014. The average diurnal variation of OH peaked with a midday (10:00–15:00) average of 1.0 × 10⁶(±0.6 × 10⁶) molecules cm⁻³. This was substantially lower than previously reported in other tropical forest photochemical environments (2–5 × 10⁶molecules cm⁻³) while the simulated OH reactivity was lower. The observational data set was used to constrain a box model to examine how well current photochemical reaction mechanisms can simulate observed OH. We used one near‐explicit mechanism (MCM v3.3.1) and four condensed mechanisms (i.e., RACM2, MOZART‐T1, CB05, CB6r2) to simulate OH. A total of 14 days of analysis shows that all five chemical mechanisms were able to explain the measured OH within instrumental uncertainty of 40% during the campaign in the Amazonian rainforest environment. Future studies are required using more reliable NO_xand VOC measurements to further investigate discrepancies in our understanding of the radical chemistry in the tropical rainforest.