scholarly journals Carbonaceous aerosol AAE inferred from in-situ aerosol measurements at the Gosan ABC super site, and the implications for brown carbon aerosol

2012 ◽  
Vol 12 (14) ◽  
pp. 6173-6184 ◽  
Author(s):  
C. E. Chung ◽  
S.-W. Kim ◽  
M. Lee ◽  
S.-C. Yoon ◽  
S. Lee

Abstract. The Mass Absorption Cross section (MAC) and Absorption Ångström Exponent (AAE) have been commonly estimated for ambient aerosols but rarely for black carbon (BC) or organic aerosol (OA) alone in the ambient conditions. Here, we provide estimates of BC (and OA) MAC and AAE in East Asian outflow, by analyzing field data collected at the Gosan ABC super site. At this site, EC (and OC) carbon mass, the aerosol absorption coefficient at 7 wavelengths and PM mass density were continuously measured from October 2009 to June 2010. We remove the absorption data with significant dust influence using the mass ratio of PM10 to PM2.5. The remaining data shows an AAE of about 1.27, which we suggest represent the average carbonaceous aerosol (CA) AAE at Gosan. We find a positive correlation between the mass ratio of OC to EC and CA AAE, and successfully increase the correlation by filtering out data associated with weak absorption signal. After the filtering, absorption coefficient is regressed on OC and EC mass densities. BC and OA MACs are found to be 5.1 (3.8–6.1) and 1.4 (0.8–2.0) m2 g−1 at 520 nm respectively. From the estimated BC and OA MAC, we find that OA contributes about 45% to CA absorption at 520 nm. BC AAE is found to be 0.7–1.0, and is probably even lower considering the instrument bias. OA AAE is found to be 1.6–1.8. Compared with a previous estimate of OA MAC and AAE near biomass burning, our estimates at Gosan strongly suggest that the strongly-absorbing so-called brown carbon spheres are either unrelated to biomass burning or absent near the emission source.

2012 ◽  
Vol 12 (2) ◽  
pp. 4507-4539 ◽  
Author(s):  
C. E. Chung ◽  
S.-W. Kim ◽  
M. Lee ◽  
S.-C. Yoon ◽  
S. Lee

Abstract. Carbon mass of aerosols and its division between EC and OC sources were continuously measured at hourly intervals from October 2009 to June 2010. During this 9-month period, we also measured the aerosol absorption coefficient at 7 wavelengths and obtained PM mass density data at 1-h resolution. The measurement was made at the Gosan ABC super site, which is an ideal location for monitoring long-range transported aerosols from China. We remove the absorption data with significant dust influence using the mass ratio of PM10 to PM2.5. The remaining data shows an Absorption Ångström Exponent (AAE) of about 1.27, which we suggest represent the average carbonaceous aerosol (CA) AAE at Gosan. CA AAE is highest in winter, in which the monthly value is near 1.4. We find a positive correlation between the mass ratio of OC to EC and CA AAE, and successfully increase the correlation by filtering out data associated with weak absorption signal. After the filtering, absorption coefficient is regressed on OC and EC mass densities. Black carbon (BC) and organic aerosol (OA) absorption cross sections per carbon mass are found to be 5.1 (4.2–6.0) and 1.4 (1.1–1.8) m2 g−1 at 520 nm respectively. From the estimated BC & OA MAC, we find that OA contributes about 45% to CA absorption at 520 nm. OA AAE is found to be 1.7 (1.4–2.1). Compared with a previous estimate of OA MAC and AAE, our estimates at Gosan strongly suggest that the strongly-absorbing so-called brown carbon spheres are either unrelated to biomass burning or absent near the emission source.


2012 ◽  
Vol 5 (1) ◽  
pp. 1003-1027 ◽  
Author(s):  
F. Esposito ◽  
M. R. Calvello ◽  
E. Gueguen ◽  
G. Pavese

Abstract. A novel approach for the analysis of aerosol absorption coefficient measurements is presented. A 7-wavelenghts aethalometer has been employed to identify brown carbon (BrC) and black carbon (BC) and to detect organic carbon (OC) in fine atmospheric aerosols (PM2.5). The Magee Aethalometer estimates the BC content in atmospheric particulate by measuring the light attenuation in the aerosols accumulated on a quartz filter, at the standard wavelength λ = 0.88 μm. The known Magee algorithm is based on the hypothesis of a mass absorption coefficient inversely proportional to the wavelength. The new algorithm has been developed and applied to the whole spectral range; it verifies the spectral absorption behavior and, thus, it distinguishes between black and brown carbon. Moreover, it allows also to correct the absorption estimation at the UV wavelength commonly used to qualitatively detect the presence of mixed hydrocarbons. The algorithm has been applied to data collected in Agri Valley, located in Southern Italy, where torched crude oil undergoes a pre-treatment process. The Magee Aethalometer has been set to measure Aerosol absorption coefficients τaer (λ, t) every 5 min. Wavelength dependence of τaer (λ, t) has been analyzed by a best-fit technique and, excluding UV-wavelengths, both the absorption Angstrom coefficient α and the BC (or BrC) concentration have been determined. Finally, daily histograms of α provide information on optical properties of carbonaceous aerosol, while the extrapolation at UV-wavelengths gives information on the presence of semivolatile organic carbon (OC) particles.


2011 ◽  
Vol 11 (3) ◽  
pp. 7291-7319 ◽  
Author(s):  
H. Jethva ◽  
O. Torres

Abstract. We provide satellite-based evidence of the spectral dependence of absorption in biomass burning aerosols over South America using near-UV measurements made by Ozone Monitoring Instrument (OMI) during 2005–2007. Currently, OMAERUV aerosol algorithm characterizes carbonaceous aerosol as "gray" aerosol, meaning no wavelength dependence in aerosol absorption. With this assumption, OMI-derived aerosol optical depth (AOD) is found to be over-estimated significantly compared to that of AERONET at several sites during intense biomass burning events (August–September). The assumption on height of aerosols and other parameters seem to be reasonable and unable to explain large discrepancy in the retrieval. The specific ground-based studies have revealed strong spectral dependence in aerosol absorption in the near-UV region that indicates the presence of organic carbon. A new set of OMI aerosol retrieval with assumed wavelength-dependent aerosol absorption in the near-UV region (Absorption Angstrom Exponent λ−2.5 to −3.0) provided much improved retrieval of AOD with significantly reduced bias. Also, the new retrieval of single-scattering albedo is in better agreement with those of AERONET within the uncertainties (Δω=±0.03). The new smoke aerosol model was also found to be valid over the biomass burning region of central Africa and northern India. Together with suggesting vast improvement in the retrieval of aerosol properties from OMI, present study demonstrates the near-UV capabilities of OMI in separating aerosols containing organics from pure black carbon through OMI-AERONET integrated measurements.


2009 ◽  
Vol 9 (19) ◽  
pp. 7643-7655 ◽  
Author(s):  
B. I. Magi

Abstract. This study characterizes the aerosol over extratropical and tropical southern Africa during the biomass burning season by presenting an aerosol mass apportionment and aerosol optical properties. Carbonaceous aerosol species account for 54% and 83% of the extratropical and tropical aerosol mass, respectively, which is consistent with the fact that the major source of particulate matter in southern Africa is biomass burning. This mass apportionment implies that carbonaceous species in the form of organic carbon (OC) and black carbon (BC) play a critical role in the aerosol optical properties. By combining the in situ measurements of aerosol mass concentrations with concurrent measurements of aerosol optical properties at a wavelength of 550 nm, it is shown that 80–90% of the aerosol scattering is due to carbonaceous aerosol, and the derived mass scattering cross sections (MSC) for OC and BC are 3.9±0.6 m2/g and 1.6±0.2 m2/g, respectively. Derived values of mass absorption cross sections (MAC) for OC and BC are 0.7±0.6 m2/g and 8.2±1.1 m2/g, respectively. The values of MAC imply that ~26% of the aerosol absorption in southern Africa is due to OC, with the remainder due to BC. The results in this study provide important constraints for aerosol properties in a region dominated by biomass burning and should be integrated into climate models to improve aerosol simulations.


2020 ◽  
Author(s):  
HuiHui Wu ◽  
Jonathan Taylor ◽  
Justin Langridge ◽  
Chenjie Yu ◽  
Paul Williams ◽  
...  

<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>


2016 ◽  
Vol 16 (3) ◽  
pp. 1433-1443 ◽  
Author(s):  
J.-F. Yuan ◽  
X.-F. Huang ◽  
L.-M. Cao ◽  
J. Cui ◽  
Q. Zhu ◽  
...  

Abstract. The strong spectral dependence of light absorption of brown carbon (BrC) aerosol is regarded to influence aerosol's radiative forcing significantly. The Absorption Angstrom Exponent (AAE) method has been widely used in previous studies to attribute light absorption of BrC at shorter wavelengths for ambient aerosols, with a theoretical assumption that the AAE of "pure" black carbon (BC) aerosol equals to 1.0. In this study, the AAE method was applied to both urban and rural environments in the Pearl River Delta (PRD) region of China, with an improvement of constraining the realistic AAE of "pure" BC through statistical analysis of on-line measurement data. A three-wavelength photo-acoustic soot spectrometer (PASS-3) and aerosol mass spectrometers (AMS) were used to explore the relationship between the measured AAE and the relative abundance of organic aerosol to BC. The regression and extrapolation analysis revealed that more realistic AAE values for "pure" BC aerosol (AAEBC) were 0.86, 0.82, and 1.02 between 405 and 781 nm, and 0.70, 0.71, and 0.86 between 532 and 781 nm, in the campaigns of urbanwinter, urbanfall, and ruralfall, respectively. Roadway tunnel experiments were conducted and the results further confirmed the representativeness of the obtained AAEBC values for the urban environment. Finally, the average light absorption contributions of BrC (± relative uncertainties) at 405 nm were quantified to be 11.7 % (±5 %), 6.3 % (±4 %), and 12.1 % (±7 %) in the campaigns of urbanwinter, urbanfall, and ruralfall, respectively, and those at 532 nm were 10.0 % (±2 %), 4.1 % (±3 %), and 5.5 % (±5 %), respectively. The relatively higher BrC absorption contribution at 405 nm in the ruralfall campaign could be reasonably attributed to the biomass burning events nearby, which was then directly supported by the biomass burning simulation experiments performed in this study. This paper indicates that the BrC contribution to total aerosol light absorption at shorter wavelengths is not negligible in the highly urbanized and industrialized PRD region.


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Hunter Brown ◽  
Xiaohong Liu ◽  
Rudra Pokhrel ◽  
Shane Murphy ◽  
Zheng Lu ◽  
...  

AbstractUncertainty in the representation of biomass burning (BB) aerosol composition and optical properties in climate models contributes to a range in modeled aerosol effects on incoming solar radiation. Depending on the model, the top-of-the-atmosphere BB aerosol effect can range from cooling to warming. By relating aerosol absorption relative to extinction and carbonaceous aerosol composition from 12 observational datasets to nine state-of-the-art Earth system models/chemical transport models, we identify varying degrees of overestimation in BB aerosol absorptivity by these models. Modifications to BB aerosol refractive index, size, and mixing state improve the Community Atmosphere Model version 5 (CAM5) agreement with observations, leading to a global change in BB direct radiative effect of −0.07 W m−2, and regional changes of −2 W m−2 (Africa) and −0.5 W m−2 (South America/Temperate). Our findings suggest that current modeled BB contributes less to warming than previously thought, largely due to treatments of aerosol mixing state.


2011 ◽  
Vol 11 (4) ◽  
pp. 1491-1503 ◽  
Author(s):  
G. Adler ◽  
J. M. Flores ◽  
A. Abo Riziq ◽  
S. Borrmann ◽  
Y. Rudich

Abstract. In-situ chemical composition measurements of ambient aerosols have been used for characterizing the evolution of submicron aerosols from a large anthropogenic biomass burning (BB) event in Israel. A high resolution Time of Flight Aerosol Mass Spectrometer (HR-RES-TOF-AMS) was used to follow the chemical evolution of BB aerosols during a night-long, extensive nationwide wood burning event and during the following day. While these types of extensive BB events are not common in this region, burning of agricultural waste is a common practice. The aging process of the BB aerosols was followed through their chemical, physical and optical properties. Mass spectrometric analysis of the aerosol organic component showed that aerosol aging is characterized by shifting from less oxidized fresh BB aerosols to more oxidized aerosols. Evidence for aerosol aging during the day following the BB event was indicated by an increase in the organic mass, its oxidation state, the total aerosol concentration, and a shift in the modal particle diameter. The effective broadband refractive index (EBRI) was derived using a white light optical particle counter (WELAS). The average EBRI for a mixed population of aerosols dominated by open fires was m = 1.53(±0.03) + 0.07i(±0.03), during the smoldering phase of the fires we found the EBRI to be m = 1.54(±0.01) + 0.04i(±0.01) compared to m = 1.49(±0.01) + 0.02i(±0.01) of the aged aerosols during the following day. This change indicates a decrease in the overall aerosol absorption and scattering. Elevated levels of particulate Polycyclic Aromatic Hydrocarbons (PAHs) were detected during the entire event, which suggest possible implications for human health during such extensive event.


2019 ◽  
Author(s):  
Alice C. Forello ◽  
Vera Bernardoni ◽  
Giulia Calzolai ◽  
Franco Lucarelli ◽  
Dario Massabò ◽  
...  

Abstract. In this paper, a new methodology coupling aerosol optical and chemical parameters in the same source apportionment study is reported. This approach gives additional relevant information such as estimates for the atmospheric Ångström Absorption Exponent (α) of the sources and Mass Absorption Coefficient (MAC) for fossil fuel emissions at different wavelengths. A multi-time source apportionment study using Multilinear Engine ME-2 was performed on a PM10 dataset with different time resolution (24 hours, 12 hours, and 1 hour) collected during two different seasons in Milan (Italy) in 2016. Samples were optically analysed to retrieve the aerosol absorption coefficient bap (in Mm−1) at four wavelengths (λ = 405 nm, 532 nm, 635 nm and 780 nm) and chemically characterised for elements, ions, levoglucosan, and carbonaceous components. Time-resolved chemically speciated data were coupled with bap multi-wavelength measurements and introduced as input data in the multi-time receptor model; this approach was proven to strengthen the identification of sources being particularly useful when important chemical markers (e.g. levoglucosan, elemental carbon, ...) are not available. The final solution consisted in 8 factors (nitrate, sulphate, resuspended dust, biomass burning, construction works, traffic, industry, aged sea salt); the implemented constraints led to a better physical description of factors and the bootstrap analysis supported the goodness of the solution. As for bap apportionment, consistently to what expected, the two factors assigned to biomass burning and traffic were the main contributors to aerosol absorption in atmosphere. A relevant feature of the approach proposed in this work is the possibility of retrieving many other information about optical parameters; for example, opposite to the more traditional approach used by optical source apportionment models, here we obtained the atmospheric Ångström Absorption Exponent (α) of the sources (α biomass burning = 1.83 and α fossil fuels = 0.80), without any a priori assumption. In addition, an estimate for the Mass Absorption Cross section (MAC) for fossil fuel emissions at four wavelengths was obtained and found to be consistent with literature ranges.


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