Search

The aging of refractory black carbon (rBC) aerosol by sulfate-driven chemistry has been constrained in coal-fired power-plant plumes using the NOAA WP-3D research aircraft during the Southern Nexus (SENEX) study, which took place in the Southeastern US in June and July of 2013. A Single Particle Soot Photometer (SP2) determined the microphysical properties of rBC-containing particles including single-particle rBC mass and the presence and amount of internally-mixed non-rBC material, hereafter referred to as ―coatings‖. Most power-plant influenced air was associated with very slightly increased amounts of non-refractory material, likely sulfate internally mixed with the rBC, however this increase was statistically insignificant even after semi-Lagrangian exposure for up to 5 h. On average, the increase in coating thickness was 2 ± 4 nm for particles containing 3–5 fg rBC. Similarly, the number fraction of rBC-containing particles that could be identified as internally mixed was increased by plume chemistry by only 1.3 ± 1.3%. These direct measurements of microphysical aging of rBC-containing aerosol by power plant emissions constrain the enhancement of sulfate chemistry on both rBC's column-integrated absorption optical depth, and rBC-containing aerosol's ability to act as cloud condensation nuclei. Appling Mie and ĸ-Köhler theories to the SP2 observations, permits the resulting effect on rBC ambient light-absorption to be capped at the 2–6% level. [ABSTRACT FROM AUTHOR]

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 angstrom exponent of unity. The methodologies employed provide ranges of potential importance of BrC to absorption but, on average, there was a factor of 2 difference in the ratio of the fraction of absorption attributable to brown carbon 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 to organic carbon ratio (EC/OC) of emitted aerosols and weaker correlation with the modified combustion efficiency (MCE). Previous studies have shown that brown carbon 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. [ABSTRACT FROM AUTHOR]

Single-scattering albedo (SSA) and absorption Ångström exponent (AAE) are two critical parameters in determining the impact of absorbing aerosol on the Earth's 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's 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's 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. [ABSTRACT FROM AUTHOR]