scholarly journals Relative Importance of Black Carbon, Brown Carbon and Absorption Enhancement from Clear Coatings in Biomass Burning Emissions

2016 ◽  
Author(s):  
Anonymous
Keyword(s):  
Black Carbon ◽  
Biomass Burning ◽  
Absorption Enhancement ◽  
Relative Importance ◽  
Brown Carbon

scholarly journals Exploiting simultaneous observational constraints on mass and absorption to estimate the global direct radiative forcing of black carbon and brown carbon

2014 ◽  
Vol 14 (20) ◽  
pp. 10989-11010 ◽  
Author(s):  
X. Wang ◽  
C. L. Heald ◽  
D. A. Ridley ◽  
J. P. Schwarz ◽  
J. R. Spackman ◽  
...  
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Biomass Burning ◽  
Radiative Forcing ◽  
Model Simulation ◽  
Anthropogenic Sources ◽  
Absorption Enhancement ◽  
Brown Carbon ◽  
Direct Radiative Forcing ◽  
Improved Model

Abstract. Atmospheric black carbon (BC) is a leading climate warming agent, yet uncertainties on the global direct radiative forcing (DRF) remain large. Here we expand a global model simulation (GEOS-Chem) of BC to include the absorption enhancement associated with BC coating and separately treat both the aging and physical properties of fossil-fuel and biomass-burning BC. In addition we develop a global simulation of brown carbon (BrC) from both secondary (aromatic) and primary (biomass burning and biofuel) sources. The global mean lifetime of BC in this simulation (4.4 days) is substantially lower compared to the AeroCom I model means (7.3 days), and as a result, this model captures both the mass concentrations measured in near-source airborne field campaigns (ARCTAS, EUCAARI) and surface sites within 30%, and in remote regions (HIPPO) within a factor of 2. We show that the new BC optical properties together with the inclusion of BrC reduces the model bias in absorption aerosol optical depth (AAOD) at multiple wavelengths by more than 50% at AERONET sites worldwide. However our improved model still underestimates AAOD by a factor of 1.4 to 2.8 regionally, with the largest underestimates in regions influenced by fire. Using the RRTMG model integrated with GEOS-Chem we estimate that the all-sky top-of-atmosphere DRF of BC is +0.13 Wm−2 (0.08 Wm−2 from anthropogenic sources and 0.05 Wm−2 from biomass burning). If we scale our model to match AERONET AAOD observations we estimate the DRF of BC is +0.21 Wm−2, with an additional +0.11 Wm−2 of warming from BrC. Uncertainties in size, optical properties, observations, and emissions suggest an overall uncertainty in BC DRF of −80%/+140%. Our estimates are at the lower end of the 0.2–1.0 Wm−2 range from previous studies, and substantially less than the +0.6 Wm−2 DRF estimated in the IPCC 5th Assessment Report. We suggest that the DRF of BC has previously been overestimated due to the overestimation of the BC lifetime (including the effect on the vertical profile) and the incorrect attribution of BrC absorption to BC.

scholarly journals Exploiting simultaneous observational constraints on mass and absorption to estimate the global direct radiative forcing of black carbon and brown carbon

2014 ◽  
Vol 14 (11) ◽  
pp. 17527-17583 ◽  
Author(s):  
X. Wang ◽  
C. L. Heald ◽  
D. A. Ridley ◽  
J. P. Schwarz ◽  
J. R. Spackman ◽  
...  
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Biomass Burning ◽  
Radiative Forcing ◽  
Model Simulation ◽  
Anthropogenic Sources ◽  
Absorption Enhancement ◽  
Brown Carbon ◽  
Direct Radiative Forcing ◽  
Improved Model

Abstract. Atmospheric black carbon (BC) is a leading climate warming agent, yet uncertainties on the global direct radiative forcing (DRF) remain large. Here we expand a global model simulation (GEOS-Chem) of BC to include the absorption enhancement associated with BC coating and separately treat both the aging and physical properties of fossil fuel and biomass burning BC. In addition we develop a global simulation of Brown Carbon (BrC) from both secondary (aromatic) and primary (biomass burning and biofuel) sources. The global mean lifetime of BC in this simulation (4.4 days) is substantially lower compared to the AeroCom I model means (7.3 days), and as a result, this model captures both the mass concentrations measured in near-source airborne field campaigns (ARCTAS, EUCAARI) and surface sites within 30%, and in remote regions (HIPPO) within a factor of two. We show that the new BC optical properties together with the inclusion of BrC reduces the model bias in Absorption Aerosol Optical Depth (AAOD) at multiple wavelengths by more than 50% at AERONET sites worldwide. However our improved model still underestimates AAOD by a factor of 1.4 to 2.8 regionally, with largest underestimates in regions influenced by fire. Using the RRTMG model integrated with GEOS-Chem we estimate that the all-sky top-of-atmosphere DRF of BC is +0.13 W m−2 (0.08 W m−2 from anthropogenic sources and 0.05 W m−2 from biomass burning). If we scale our model to match AERONET AAOD observations we estimate the DRF of BC is +0.21 W m−2, with an additional +0.11 W m−2 of warming from BrC. Uncertainties in size, optical properties, observations, and emissions suggest an overall uncertainty in BC DRF of −80% / +140%. Our estimates are at the lower end of the 0.2–1.0 W m−2 range from previous studies, and substantially less than the +0.6 W m−2 DRF estimated in the IPCC 5th Assessment Report. We suggest that the DRF of BC has previously been overestimated due to the overestimation of the BC lifetime and the incorrect attribution of BrC absorption to BC.

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

2016 ◽  
Vol 16 (15) ◽  
pp. 9549-9561 ◽  
Author(s):  
Rudra P. Pokhrel ◽  
Nick L. Wagner ◽  
Justin M. Langridge ◽  
Daniel A. Lack ◽  
Thilina Jayarathne ◽  
...  
Keyword(s):  
Black Carbon ◽  
Biomass Burning ◽  
Single Scattering ◽  
Emission Factors ◽  
Single Scattering Albedo ◽  
Biomass Fuels ◽  
Brown Carbon ◽  
Pearson's R ◽  
Biomass Burning Aerosol ◽  
Pearson’S R

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.

Experimental evidence of the lensing effect suppression for atmospheric black carbon containing brown coatings

2020 ◽  
Author(s):  
Vaios Moschos ◽  
Martin Gysel-Beer ◽  
Robin L. Modini ◽  
Joel C. Corbin ◽  
Dario Massabò ◽  
...  
Keyword(s):  
Black Carbon ◽  
Radiative Forcing ◽  
Wavelength Dependence ◽  
Chem Phys ◽  
Absorption Enhancement ◽  
Visible Spectroscopy ◽  
Scanning Mobility Particle Sizer ◽  
Absorption Data ◽  
Brown Carbon ◽  
Aerosol Radiative Forcing

<p>Accounting for the wavelength- and source-dependent optical absorption properties of the abundant light-absorbing organic (brown) carbon (BrC) and the mixing state of atmospheric black carbon (BC) are essential to reduce the large uncertainty in aerosol radiative forcing. Estimation of BrC absorption online by subtraction is highly uncertain and may be biased if not decoupled from the potential BC absorption enhancement (lensing) due to non-refractory (organic and inorganic) coating acquisition.</p><p>Here, the reported total particulate absorption is based on long-term, filter-based seven-wavelength Aethalometer (AE33 model) data, corrected for multiple scattering effects with Multi-Wavelength Absorbance Analyzer (5λ MWAA) measurements. Using ultraviolet-visible spectroscopy absorbance measurements along with particle size distributions obtained by a scanning mobility particle sizer, we have conducted Mie calculations to assess the importance of source-specific extractable particulate BrC (Moschos et al., 2018) versus BC absorption.</p><p>For the species-specific optical closure, the wavelength dependence of bare BC absorption is estimated using MWAA measurements upon successive filter extractions to remove the influence of BrC/coatings. The lensing contribution, supported by observations from field-emission scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy, is estimated at longer wavelengths using a refined proxy for the BC coating thickness. The approach is validated independently by applying a novel positive matrix factorization-based approach on the calibrated total AE33 absorption data.</p><p>Based on the observational constraints established in this study, we demonstrate for various distinct case studies that the interplay between lensing and BrC absorption results in lower than expected BC absorption at shorter wavelengths. This indicates that the volume additivity assumption is not valid for particulate absorption by internally mixed heterogeneous atmospheric aerosol populations. These comprehensive experimental analyses verify the BC lensing suppression predicted for simplified core-shell structures containing moderately absorbing BrC (Lack & Cappa, 2010). The implications discussed in this work are relevant for co-emitted species from biomass burning or aged plumes with high BrC to BC mass/absorption ratio.</p><p> </p><p><strong>References</strong></p><p>Moschos, V., Kumar, N. K., Daellenbach, K. R., Baltensperger, U., Prévôt, A. S. H., and El Haddad, I.: Source apportionment of brown carbon absorption by coupling ultraviolet-visible spectroscopy with aerosol mass spectrometry, Environ. Sci. Tech. Lett., 5, 302-308, https://doi.org/10.1021/acs.estlett.8b00118, 2018.</p><p>Lack, D. A. and Cappa, C. D.: Impact of brown and clear carbon on light absorption enhancement, single scatter albedo and absorption wavelength dependence of black carbon, Atmos. Chem. Phys., 10, 4207–4220, https://doi.org/10.5194/acp-10-4207-2010, 2010.</p>

The aging process of ambient black carbon and brown carbon from biomass burning emission during MOYA-2017 aircraft campaign

2020 ◽  
Author(s):  
HuiHui Wu ◽  
Jonathan Taylor ◽  
Justin Langridge ◽  
Chenjie Yu ◽  
Paul Williams ◽  
...  
Keyword(s):  
Black Carbon ◽  
Biomass Burning ◽  
Aging Process ◽  
Atmospheric Dispersion ◽  
Chemical Properties ◽  
Carbonaceous Aerosol ◽  
Brown Carbon ◽  
Research Aircraft ◽  
Flaming Combustion ◽  
The Uk

<p>The biomass burning over West Africa during the dry season (December – February) is a globally significant source of trace gases and carbonaceous aerosol particles in the atmosphere. The MOYA-2017 (Methane Observations Yearly Assessments 2017) campaign were conducted using the UK FAAM Bae-146 airborne research aircraft, to investigate biomass burning emissions in this region. Research sorties were flown out of Senegal, with some flights directly over terrestrial fires and others sampling transported smokes over the Atlantic ocean.</p><p>The aircraft was equipped with a variety of aerosol-related instruments to measure submicron aerosol chemical properties (aerosol mass spectrometer, AMS and single-particle soot photometer, SP2) and absorption at different wavelengths (Photoacoustic spectrometer, PAS, measure at 405, 514 and 658 nm). In this study, we focus on the aging process of ambient black carbon (BC) and brown carbon (BrC) from biomass burning, in time scale from (<0.5) h to (9 – 15) h. The transport age of smokes was estimated using Met Office's Numerical Atmospheric-dispersion Modelling Environment (NAME).</p><p>The sampled smokes during MOYA-2017 were controlled by flaming-phase combustion. The enhancement ratios of BC with respect to CO ranged from 14 to 26 (ng m<sup>–3</sup> / ppbv) at sources. Our measurements show that count and mass median diameters of BC core size were relatively stable, which were around 106 and 190 nm respectively. Average BC coating thickness increased from (1.16 ± 0.03) to (1.71 ± 0.06) after approximately half-day transport. Average absorption angstrom exponents (AAE<sub>405-658</sub>) increased from (1.1 ± 0.1) to (1.8 ± 0.3), suggesting that BrC contributed little in the very freshly emitted aerosols (<0.5 h) and were formed during aging process. In order to investigate the importance of BrC in this area, we also attributed the measured aerosol absorption into BC and BrC separately. By linking AAE<sub>405-658</sub> with organic (OA) composition measured by the AMS, we found that the increasing AAE<sub>405-658</sub> is positively correlated with O/C ratio (oxygenation) of the OA. These data indicate that BrC in smokes controlled by flaming combustion is likely to be from the condensation of semi-volatile OA during cooling stage of smokes, and from the aged primary OA or secondary OA formation.</p>

scholarly journals Aerosol light absorption and the role of extremely low volatility organic compounds

2020 ◽  
Vol 20 (19) ◽  
pp. 11625-11637
Author(s):  
Antonios Tasoglou ◽  
Evangelos Louvaris ◽  
Kalliopi Florou ◽  
Aikaterini Liangou ◽  
Eleni Karnezi ◽  
...  
Keyword(s):  
Black Carbon ◽  
Organic Compounds ◽  
Light Absorption ◽  
Absorption Enhancement ◽  
Scanning Mobility Particle Sizer ◽  
Brown Carbon ◽  
Aerosol Absorption ◽  
Aerosol Mass ◽  
Particle Sizer

Abstract. A month-long set of summertime measurements in a remote area in the Mediterranean is used to quantify aerosol absorption and the role of black and brown carbon. The suite of instruments included a high-resolution aerosol mass spectrometer (HR-ToF-AMS) and a scanning mobility particle sizer (SMPS), both coupled to a thermodenuder and an Aethalometer, a photoacoustic extinctiometer (PAX405), and a single particle soot photometer (SP2). The average refractory black carbon (rBC) concentration during the campaign was 0.14 µg m−3, representing 3 % of the fine aerosol mass. The measured light absorption was two or more times higher than that of fresh black carbon (BC). Mie theory indicated that the absorption enhancement due to the coating of BC cores by nonrefractory material could explain only part of this absorption enhancement. The role of brown carbon (BrC) and other non-BC light-absorbing material was then investigated. A good correlation (R2=0.76) between the unexplained absorption and the concentration of extremely low volatility organic compounds (ELVOCs) mass was found.

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