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  1. Free, publicly-accessible full text available July 3, 2024
  2. The fractal dimension is a key parameter in quantifying the morphology of aerosol aggregates, which is necessary to understand their radiative impact. Here we used Transmission Electron Microscopy (TEM) images to determine 2D fractal dimensions using the nested square and box-grid method and used two different empirical equations to obtain the 3D fractal dimensions. The values ranged from 1.70 ± 0.05 for pine to 1.82 ± 0.07 for Eucalyptus, with both methods giving nearly identical results using one of the empirical equations and the other overestimated the 3D values significantly when compared to other values in the literature. The values we obtained are comparable to the fractal dimensions of fresh aerosols in the literature and were dependent on fuel type and combustion condition. Although these methods accurately calculated the fractal dimension, they have shortcomings if the images are not of the highest quality. While there are many ways of determining the fractal dimension of linear features, we conclude that the application of every method requires careful consideration of a range of methodological concerns. 
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    Free, publicly-accessible full text available February 1, 2024
  3. Abstract. Light absorbing organic carbon, or brown carbon (BrC), can be a significantcontributor to the visible light absorption budget. However, the sources ofBrC and the contributions of BrC to light absorption are not wellunderstood. Biomass burning is thought to be a major source of BrC.Therefore, as part of the WE-CAN (Western Wildfire Experiment for CloudChemistry, Aerosol Absorption and Nitrogen) study, BrC absorption data werecollected on board the National Science Foundation/National Center for Atmospheric Research (NSF/NCAR) C-130 aircraft as it intercepted smoke fromwildfires in the western US in July–August 2018. BrC absorptionmeasurements were obtained in near real-time using two techniques. The firstcoupled a particle-into-liquid sampler (PILS) with a liquid waveguidecapillary cell and a total organic carbon analyzer for measurements ofwater-soluble BrC absorption and WSOC (water-soluble organic carbon). Thesecond employed a custom-built photoacoustic aerosol absorption spectrometer(PAS) to measure total absorption at 405 and 660 nm. The PAS BrC absorption at 405 nm (PAS total Abs 405 BrC) was calculated by assuming the absorption determined by the PAS at 660 nm was equivalent to the black carbon (BC) absorption and the BC aerosol absorption Ångström exponent was 1. Data from the PILS and PAS were combined to investigate the water-soluble vs. total BrC absorption at 405 nm in the various wildfire plumes sampled during WE-CAN. WSOC, PILS water-soluble Abs 405, and PAS total Abs 405 tracked each other in and out of the smoke plumes. BrC absorption was correlated with WSOC (R2 value for PAS =0.42 and PILS =0.60) and CO (carbon monoxide) (R2 value for PAS =0.76 and PILS =0.55) for all wildfires sampled. The PILS water-soluble Abs 405 was corrected for thenon-water-soluble fraction of the aerosol using the calculated UHSAS(ultra-high-sensitivity aerosol spectrometer) aerosol mass. The correctedPILS water-soluble Abs 405 showed good closure with the PAS total Abs 405BrC with a factor of ∼1.5 to 2 difference. This differencewas explained by particle vs. bulk solution absorption measured by the PASvs. PILS, respectively, and confirmed by Mie theory calculations. DuringWE-CAN, ∼ 45 % (ranging from 31 % to 65 %) of the BrCabsorption was observed to be due to water-soluble species. The ratio of BrC absorption to WSOC or ΔCO showed no clear dependence on firedynamics or the time since emission over 9 h. 
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  5. Abstract

    Long‐term exposure to ambient fine particulate matter (PM2.5) is the second leading risk factor of premature death in Sub‐Saharan Africa. We use GEOS‐Chem to quantify the effects of (a) trash burning, (b) residential solid‐fuel burning, and (c) open biomass burning (BB) (i.e., landscape fires) on ambient PM2.5and PM2.5‐attributable mortality in Africa. Using a series of sensitivity simulations, we excluded each of the three combustion sources in each of five African regions. We estimate that in 2017 emissions from these three combustion sources within Africa increased global ambient PM2.5by 2%, leading to 203,000 (95% confidence interval: 133,000–259,000) premature mortalities yr−1globally and 167,000 premature mortalities yr−1in Africa. BB contributes more ambient PM2.5‐related premature mortalities per year (63%) than residential solid‐fuel burning (29%) and trash burning (8%). Open BB in Central Africa leads to the largest number of PM2.5‐attributed mortalities inside the region, while trash burning in North Africa and residential solid‐fuel burning in West Africa contribute the most regional mortalities for each source. Overall, Africa has a unique ambient air pollution profile because natural sources, such as windblown dust and BB, contribute strongly to ambient PM2.5levels and PM2.5‐related mortality. Air pollution policies may need to focus on taking preventative measures to avoid exposure to ambient PM2.5from these less‐controllable sources.

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  6. null (Ed.)
    Abstract. An accurate measurement of the optical properties of aerosol is critical for quantifying the effect of aerosol on climate. Uncertainties persist and results of measurements vary significantly. Biomass burning (BB) aerosol has been extensively studied through both field and laboratory environments for North American fuels to understand the changes in opticaland chemical properties as a function of aging. There is a need for a widersampling of fuels from different regions of the world for laboratory studies. This work represents the first such study of the optical andchemical properties of wood fuel samples commonly used for domestic purposes ineast Africa. In general, combustion temperature or modified combustionefficiency (MCE) plays a major role in the optical properties of the emitted aerosol. For fuels combusted with MCE of 0.974±0.015, which is referred to as flaming-dominated combustion, the single-scattering albedo (SSA) values were in the range of 0.287 to 0.439, while for fuels combusted with MCE of 0.878±0.008, which is referred to as smoldering-dominated combustion, the SSA values were in the range of 0.66 to 0.769. There is a clear but very small dependence of SSA on fuel type. A significant increase in the scattering and extinction cross section (with no significant change inabsorption cross section) was observed, indicating the occurrence of chemistry, even during dark aging for smoldering-dominated combustion. Thisfact cannot be explained by heterogeneous oxidation in the particle phase,and we hypothesize that secondary organic aerosol formation is potentiallyhappening during dark aging. After 12 h of photochemical aging, BB aerosolbecomes highly scattering with SSA values above 0.9, which can be attributedto oxidation in the chamber. Aging studies of aerosol from flaming-dominatedcombustion were inconclusive due to the very low aerosol number concentration. We also attempted to simulate polluted urban environments byinjecting volatile organic compounds (VOCs) and BB aerosol into the chamber, but no distinct difference was observed when compared to photochemical aging in the absence of VOCs. 
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  7. null (Ed.)
    Abstract. There are many fuels used for domestic purposes in east Africa, producing a significant atmospheric burden of the resulting aerosols, which includes biomass burning particles. However, the aerosol physicochemical properties are poorly understood. Here, the combustion of eucalyptus, acacia, and olive fuels was performed at 500 and 800 ∘C in a tube furnace, followed by immediate filter collection for fresh samples or introduction into a photochemical chamber to simulate atmospheric photochemical aging under the influence of anthropogenic emissions. The aerosol generated in the latter experiment was collected onto filters after 12 h of photochemical aging. 500 and 800 ∘C were selected to simulate smoldering and flaming combustion, respectively, and to cover a range of combustion conditions. Methanol extracts from Teflon filters were analyzed by ultra-performance liquid chromatography interfaced to both a diode array detector and an electrospray ionization high-resolution quadrupole time-of-flight mass spectrometer (UPLC/DAD-ESI-HR-QTOFMS) to determine the light absorption properties of biomass burning organic aerosol constituents chemically characterized at the molecular level. Few chemical or UV–visible (UV: ultraviolet) differences were apparent between samples for the fuels when combusted at 800 ∘C. Differences in single-scattering albedo (SSA) between fresh samples at this temperature were attributed to compounds not captured in this analysis, with eucalyptol being one suspected missing component. For fresh combustion at 500 ∘C, many species were present; lignin pyrolysis and distillation products are more prevalent in eucalyptus, while pyrolysis products of cellulose and at least one nitro-aromatic species were more prevalent in acacia. SSA trends areconsistent with this, particularly if the absorption of those chromophoresextends to the 500–570 nm region. Upon aging, both show that resorcinolor catechol was removed to the highest degree, and both aerosol types weredominated by loss of pyrolysis and distillation products, though they differed in the specific compounds being consumed by the photochemical aging process. 
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  8. Abstract

    Biomass burning (BB) is a major source of pollutants that impact local, regional, and global climate, air quality, and public health. However, the influence of burning conditions and fuel type on the emission factors of pollutants is still not well understood. Here, we present the results from a laboratory study of emission factors (EFs) of pollutants from six different sub‐Saharan African biomass fuels combusted under a wide range of burning conditions, ranging from smoldering to flaming. We found that particulate matter (PM) and carbon monoxide (CO) EFs (g (kg wood)−1) are highly sensitive to the burning conditions, with an order of magnitude variation between flaming and smoldering burning conditions. Nitric oxide (NO) EF shows a fuel type dependence, with higher NO EFs for fuels with larger nitrogen content. While CO is not generally a proxy for PM2.5emissions, in this work a correlation was found between CO and PM emissions generated by combustion of seven wood fuels with moisture content (dry basis) <10% in a tube furnace and measured from a laboratory smog chamber with a temperature of ∼21–24°C and an RH below 5%. Unlike total PM, EFs of inorganic particle‐phase species do not show dependence on burning conditions. Finally, we showed that burning biomass fuels in a tube furnace would be a useful experimental approach to study BB emission under controlled burning conditions.

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  9. The evolution of organic aerosol (OA) and brown carbon (BrC) in wildfire plumes, including the relative contributions of primary versus secondary sources, has been uncertain in part because of limited knowledge of the precursor emissions and the chemical environment of smoke plumes. We made airborne measurements of a suite of reactive trace gases, particle composition, and optical properties in fresh western US wildfire smoke in July through August 2018. We use these observations to quantify primary versus secondary sources of biomass-burning OA (BBPOA versus BBSOA) and BrC in wildfire plumes. When a daytime wildfire plume dilutes by a factor of 5 to 10, we estimate that up to one-third of the primary OA has evaporated and subsequently reacted to form BBSOA with near unit yield. The reactions of measured BBSOA precursors contribute only 13 ± 3% of the total BBSOA source, with evaporated BBPOA comprising the rest. We find that oxidation of phenolic compounds contributes the majority of BBSOA from emitted vapors. The corresponding particulate nitrophenolic compounds are estimated to explain 29 ± 15% of average BrC light absorption at 405 nm (BrC Abs405) measured in the first few hours of plume evolution, despite accounting for just 4 ± 2% of average OA mass. These measurements provide quantitative constraints on the role of dilution-driven evaporation of OA and subsequent radical-driven oxidation on the fate of biomass-burning OA and BrC in daytime wildfire plumes and point to the need to understand how processing of nighttime emissions differs.

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