Parameterization of single-scattering albedo (SSA) and absorption Ångström exponent (AAE) with EC/OC for aerosol emissions from biomass burning

Single-scattering albedo (SSA) and absorption Ångström exponent (AAE) are two critical parameters in determining the impact of absorbing aerosol on the Earth\u27s radiative balance. Aerosol emitted by biomass burning represent a significant fraction of absorbing aerosol globally, but it remains difficult to accurately predict SSA and AAE for biomass burning aerosol. Black carbon (BC), brown carbon (BrC), and non-absorbing coatings all make substantial contributions to the absorption coefficient of biomass burning aerosol. SSA and AAE cannot be directly predicted based on fuel type because they depend strongly on burn conditions. It has been suggested that SSA can be effectively parameterized via the modified combustion efficiency (MCE) of a biomass burning event and that this would be useful because emission factors for CO and CO2, from which MCE can be calculated, are available for a large number of fuels. Here we demonstrate, with data from the FLAME-4 experiment, that for a wide variety of globally relevant biomass fuels, over a range of combustion conditions, parameterizations of SSA and AAE based on the elemental carbon (EC) to organic carbon (OC) mass ratio are quantitatively superior to parameterizations based on MCE. We show that the EC/OC ratio and the ratio of EC/(EC + OC) both have significantly better correlations with SSA than MCE. Furthermore, the relationship of EC/(EC + OC) with SSA is linear. These improved parameterizations are significant because, similar to MCE, emission factors for EC (or black carbon) and OC are available for a wide range of biomass fuels. Fitting SSA with MCE yields correlation coefficients (Pearson\u27s r) of ∼0.65 at the visible wavelengths of 405, 532, and 660 nm while fitting SSA with EC/OC or EC/(EC + OC) yields a Pearson\u27s r of 0.94-0.97 at these same wavelengths. The strong correlation coefficient at 405 nm (r = 0.97) suggests that parameterizations based on EC/OC or EC/(EC + OC) have good predictive capabilities even for fuels in which brown carbon absorption is significant. Notably, these parameterizations are effective for emissions from Indonesian peat, which have very little black carbon but significant brown carbon (SSA = 0.990 ± 0.001 at 532 and 660 nm, SSA = 0.937 ± 0.011 at 405 nm). Finally, we demonstrate that our parameterization based on EC/(EC + OC) accurately predicts SSA during the first few hours of plume aging with data from Yokelson et al. (2009) gathered during a biomass burning event in the Yucatán Peninsula of Mexico

Relative importance of black carbon, brown carbon, and absorption enhancement from clear coatings in biomass burning emissions

A wide range of globally significant biomass fuels were burned during the fourth Fire Lab at Missoula Experiment (FLAME-4). A multi-channel photoacoustic absorption spectrometer (PAS) measured dry absorption at 405, 532, and 660 nm and thermally denuded (250 °C) absorption at 405 and 660 nm. Absorption coefficients were broken into contributions from black carbon (BC), brown carbon (BrC), and lensing following three different methodologies, with one extreme being a method that assumes the thermal denuder effectively removes organics and the other extreme being a method based on the assumption that black carbon (BC) has an Ångström exponent of unity. The methodologies employed provide ranges of potential importance of BrC to absorption but, on average, there was a difference of a factor of 2 in the ratio of the fraction of absorption attributable to BrC estimated by the two methods. BrC absorption at shorter visible wavelengths is of equal or greater importance to that of BC, with maximum contributions of up to 92 % of total aerosol absorption at 405 nm and up to 58 % of total absorption at 532 nm. Lensing is estimated to contribute a maximum of 30 % of total absorption, but typically contributes much less than this. Absorption enhancements and the estimated fraction of absorption from BrC show good correlation with the elemental-carbon-to-organic-carbon ratio (EC/OC) of emitted aerosols and weaker correlation with the modified combustion efficiency (MCE). Previous studies have shown that BrC grows darker (larger imaginary refractive index) as the ratio of black to organic aerosol (OA) mass increases. This study is consistent with those findings but also demonstrates that the fraction of total absorption attributable to BrC shows the opposite trend: increasing as the organic fraction of aerosol emissions increases and the EC/OC ratio decreases

Fractal Dimensions of Biomass Burning Aerosols from TEM Images Using the Box-Grid and Nested Squares Methods

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

Refractive Indices of Biomass Burning Aerosols Obtained from African Biomass Fuels Using RDG Approximation

Biomass burning (BB) aerosols contribute to climate forcing, but much is still unknown about the extent of this forcing, owing partially to the high level of uncertainty regarding BB aerosol optical properties. A key optical parameter is the refractive index (RI), which influences the absorbing and scattering properties of aerosols. This quantity is not measured directly, but it is obtained by fitting the measured scattering cross section and extinction cross section to a theoretical model using the RI as a fitting parameter. We used the Rayleigh–Debye–Gans (RDG) approximation to retrieve the complex RI of freshly emitted BB aerosol from two fuels (eucalyptus and olive) from Africa in the spectral range of 500–580 nm. Experimental measurements were carried out using cavity ring-down spectroscopy to measure extinction over the range of wavelengths of 500–580 nm and nephelometry to measure scattering at three wavelengths of 450, 550, and 700 nm for size-selected BB aerosol particles. The fuels were combusted in a tube furnace at a temperature of 800 °C, which is representative of the flaming stage of burning. Filter samples were collected and imaged using tunneling electron microscopy to obtain information on the morphology and size of the particles, which was used in the RDG calculations. The mean radii of the monomers were 27.8 and 31.5 nm for the eucalyptus and the olive fuels, respectively. The components of the retrieved complex RI were in the range of 1.31 ≤ n ≤ 1.56 and 0.045 ≤ k ≤ 0.468. The real and complex parts of the RI increase with increasing particle mobility diameter. The real part of the RI is lower, and the imaginary part is higher than what was recommended in literature for black carbon generated by propane or field measurements from fires of mixed wood samples. Fuel dependent results from controlled laboratory experiments can be used in climate modeling efforts and to constrain field measurements from biomass burning

Investigating Carbonaceous Aerosol and Its Absorption Properties From Fires in the Western United States (WE‐CAN) and Southern Africa (ORACLES and CLARIFY)

Biomass burning (BB) produces large quantities of carbonaceous aerosol (black carbon and organic aerosol, BC and OA, respectively), which significantly degrade air quality and impact climate. BC absorbs radiation, warming the atmosphere, while OA typically scatters radiation, leading to cooling. However, some OA, termed brown carbon (BrC), also absorbs visible and near UV radiation; although, its properties are not well constrained. We explore three aircraft campaigns from important BB regions with different dominant fuel and fire types (Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen [WE-CAN] in the western United States and ObseRvations of Aerosols above CLouds and their intEractionS and Cloud-Aerosol-Radiation Interactions and Forcing for Year downwind of southern Africa) and compare them with simulations from the global chemical transport model, GEOS-Chem using GFED4s. The model generally captures the observed vertical profiles of carbonaceous BB aerosol concentrations; however, we find that BB BC emissions are underestimated in southern Africa. Our comparisons suggest that BC and/or BrC absorption is substantially higher downwind of Africa than in the western United States and, while the Saleh et al. (2014, https://doi.org/10.1038/ngeo2220) and FIREX parameterizations based on the BC:OA ratio improve model-observation agreement in some regions, they do not sufficiently differentiate absorption characteristics at short wavelengths. We find that photochemical whitening substantially decreases the burden and direct radiative effect of BrC (annual mean of +0.29 W m−2 without whitening and +0.08 W m−2 with). Our comparisons suggest that whitening is required to explain WE-CAN observations; however, the importance of whitening for African fires cannot be confirmed. Qualitative comparisons with the OMI UV aerosol index suggest our standard BrC whitening scheme may be too fast over Africa