Molecular-Size-Separated Brown Carbon Absorption for Biomass-Burning Aerosol at Multiple Field Sites

2017 ◽  
Vol 51 (6) ◽  
pp. 3128-3137 ◽  
Author(s):  
Robert A. Di Lorenzo ◽  
Rebecca A. Washenfelder ◽  
Alexis R. Attwood ◽  
Hongyu Guo ◽  
Lu Xu ◽  
...  
2016 ◽  
Vol 16 (15) ◽  
pp. 9549-9561 ◽  
Author(s):  
Rudra P. Pokhrel ◽  
Nick L. Wagner ◽  
Justin M. Langridge ◽  
Daniel A. Lack ◽  
Thilina Jayarathne ◽  
...  

Abstract. 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.


2016 ◽  
Vol 50 (21) ◽  
pp. 11815-11824 ◽  
Author(s):  
Peng Lin ◽  
Paige K. Aiona ◽  
Ying Li ◽  
Manabu Shiraiwa ◽  
Julia Laskin ◽  
...  

2020 ◽  
Author(s):  
Igor Konovalov ◽  
Nikolai Golovushkin ◽  
Matthias Beekmann ◽  
Valerii Kozlov

<p>Wildfires in Siberia are a major source of aerosol in Northern Eurasia. Biomass burning (BB) aerosol can significantly impact the Earth’s radiative balance through absorption and scattering of solar radiation, interactions with clouds and changes of surface albedo due to deposition of black and brown carbon on ice and snow. There is growing evidence that atmospheric aging of BB aerosol can be associated with profound but diverse chemical and physical transformations which, in most cases, are not adequately represented in chemistry-transport and climate models that are widely used in assessments of radiative and climate effects of atmospheric pollutants.</p><p>An idea of this study is to identify changes in the optical properties of aging BB aerosol using absorption and extinction aerosol optical depths (AAOD and AOD) retrieved from the OMI and MODIS satellite observations and to elucidate key processes behind these changes using the Mie-theory-based calculations along with simulations with chemistry-transport and microphysical box models involving representation of the evolution of organic particulate matter within the VBS framework. The study focuses on a major outflow of BB plumes from Siberia into the European part of Russia in July 2016. The analysis of the satellite data is complemented by the original results of biomass burning aerosol aging experiments in a large aerosol chamber. </p><p>The results indicate that the BB aerosol evolution during the first 10-20 hours features strong secondary organic aerosol (SOA) formation resulting in a substantial increase in the particle single scattering albedo. Further evolution is affected by the loss of organic matter, probably due to evaporation and oxidation. The results also indicate that although brown carbon contained in the primary aerosol is rapidly lost (consistently with available independent observations) due to evaporation and photochemical destruction of chromospheres, it is partly replaced by weakly absorbing low-volatile SOA.</p><p>In general, this study reveals that aging BB aerosol from wildfires in Siberia undergoes major physical and chemical transformations that have to be taken into account in assessments of the impact of Siberian fires on the radiative balance in Northern Eurasia and the Arctic. It also proposes a practical way to address these complex transformations in chemistry-transport and climate models.</p><p>The study was supported by the Russian Science Foundation (grant agreement No. 19-77-20109).</p><p>References</p><ol><li>Konovalov, I.B., Beekmann, M., Berezin, E.V., Formenti, P., and Andreae, M.O.: Probing into the aging dynamics of biomass burning aerosol by using satellite measurements of aerosol optical depth and carbon monoxide, Atmos. Chem. Phys., 17, 4513–4537, 2017.</li> <li>Konovalov, I.B., Lvova, D.A., Beekmann, M., Jethva, H., Mikhailov, E.F., Paris, J.-D., Belan, B.D., Kozlov, V.S., Ciais, P., and Andreae, M.O.: Estimation of black carbon emissions from Siberian fires using satellite observations of absorption and extinction optical depths, Atmos. Chem. Phys., 18, 14889–14924, 2018.</li> <li>Konovalov, I.B., Beekmann, M., Golovushkin, N.A., and Andreae, M.O.: Nonlinear behavior of organic aerosol in biomass burning plumes: a microphysical model analysis, Atmos. Chem. Phys., 19, 12091–12119, 2019.</li> </ol>


2019 ◽  
Vol 54 (3) ◽  
pp. 1395-1405 ◽  
Author(s):  
Chunlin Li ◽  
Quanfu He ◽  
Anusha Priyadarshani Silva Hettiyadura ◽  
Uwe Käfer ◽  
Guy Shmul ◽  
...  

2013 ◽  
Vol 13 (5) ◽  
pp. 2415-2422 ◽  
Author(s):  
D. A. Lack ◽  
R. Bahreini ◽  
J. M. Langridge ◽  
J. B. Gilman ◽  
A. M. Middlebrook

Abstract. Traditional gas and particle phase chemical markers used to identify the presence of biomass burning (BB) emissions were measured for a large forest fire near Boulder, Colorado. Correlation of the organic matter mass spectroscopic m/z 60 with measured particle light absorption properties found no link at 532 nm, and a strong correlation at 404 nm. Non-black carbon absorption at 404 nm was well correlated to the ratio of the mass fractions of particulate organic matter (POM) that was m/z 60 (f60) to m/z 44 (f44). The f60 to f44 ratio did not fully explain the variability in non-BC absorption, due to contributions of brown carbon (BrC) absorption and absorption due to internal mixing of POM with black carbon (BC). The absorption Ångstrom exponent (ÅAbs) showed a good correlation to f60/f44; however the best correlation resulted from the mass absorption efficiency (MAE) of BrC at 404 nm (MAEPOM-404 nm) and f60/f44. This result indicates that the absorption of POM at low visible and UV wavelengths is linked to emissions of organic matter that contribute to the m/z 60 mass fragment, although they do not contribute to 532 nm absorption. m/z 60 is often attributed to levoglucosan and related compounds. The linear relationship between MAEPOM-404 nm and f60/f44 suggests that the strength of BrC absorption for this fire can be predicted by emissions of f60-related organic matter.


2017 ◽  
Vol 122 (10) ◽  
pp. 5441-5456 ◽  
Author(s):  
Nir Bluvshtein ◽  
Peng Lin ◽  
J. Michel Flores ◽  
Lior Segev ◽  
Yinon Mazar ◽  
...  

2015 ◽  
Vol 42 (2) ◽  
pp. 653-664 ◽  
Author(s):  
R. A. Washenfelder ◽  
A. R. Attwood ◽  
C. A. Brock ◽  
H. Guo ◽  
L. Xu ◽  
...  

2016 ◽  
Author(s):  
Rudra P. Pokhrel ◽  
Nick L. Wagner ◽  
Justin M. Langridge ◽  
Daniel A. Lack ◽  
Thilina Jayarathne ◽  
...  

Abstract. Single scattering albedo (SSA) and absorption angstrom 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 significant contributions to the absorption coefficient of biomass burning aerosol. SSA and AAE cannot be directly inferred 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 the MCE of a large number of fuels are available. 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 = 0.99 ± 0.07 at 532 and 660 nm, SSA = 0.93 ± 0.06 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 Yucatan Peninsula of Mexico.


2021 ◽  
Vol 13 (10) ◽  
pp. 2001
Author(s):  
Antonella Boselli ◽  
Alessia Sannino ◽  
Mariagrazia D’Emilio ◽  
Xuan Wang ◽  
Salvatore Amoruso

During the summer of 2017, multiple huge fires occurred on Mount Vesuvius (Italy), dispersing a large quantity of ash in the surrounding area ensuing the burning of tens of hectares of Mediterranean scrub. The fires affected a very large area of the Vesuvius National Park and the smoke was driven by winds towards the city of Naples, causing daily peak values of particulate matter (PM) concentrations at ground level higher than the limit of the EU air quality directive. The smoke plume spreading over the area of Naples in this period was characterized by active (lidar) and passive (sun photometer) remote sensing as well as near-surface (optical particle counter) observational techniques. The measurements allowed us to follow both the PM variation at ground level and the vertical profile of fresh biomass burning aerosol as well as to analyze the optical and microphysical properties. The results evidenced the presence of a layer of fine mode aerosol with large mean values of optical depth (AOD > 0.25) and Ångstrom exponent (γ > 1.5) above the observational site. Moreover, the lidar ratio and aerosol linear depolarization obtained from the lidar observations were about 40 sr and 4%, respectively, consistent with the presence of biomass burning aerosol in the atmosphere.


Sign in / Sign up

Export Citation Format

Share Document