scholarly journals Black carbon over Mexico: the effect of atmospheric transport on mixing state, mass absorption cross-section, and BC/CO ratios

2009 ◽  
Vol 9 (2) ◽  
pp. 9081-9115 ◽  
Author(s):  
R. Subramanian ◽  
G. L. Kok ◽  
D. Baumgardner ◽  
A. Clarke ◽  
Y. Shinozuka ◽  
...  

Abstract. A single particle soot photometer (SP2) was operated on the NCAR C-130 during the MIRAGE campaign (part of MILAGRO), sampling black carbon (BC) over Mexico. The highest BC concentrations were measured over Mexico City (sometimes as much as 2μg/m3) and over hill-fires to the south of the city. As expected, older, diluted air masses had lower BC concentrations. A comparison of carbon monoxide (CO) and BC suggests a CO background of around 65 ppbv, and a background-corrected BC/COnet ratio of 3.1 (ng/m3 STP)/ppbv (±25%). This ratio is similar for fresh emissions over Mexico City, as well as for aged airmasses. Comparison of light absorption measured with a particle soot absorption photometer (PSAP) and the SP2 BC suggests a BC mass-normalized absorption cross-section (MAC) of 10.3 m2g−1 (±30%) at 660 nm (or 12.4 m2g−1 @ 550 nm, assuming MAC is inversely dependent on wavelength). This appears independent of aging and similar to the expected absorption cross-section for aged BC, but values, particularly in fresh emissions, could be biased high due to instrument artifacts. SP2-derived BC coating indicators show a prominent thinly-coated BC mode over the Mexico City Metropolitan Area (MCMA), while older air masses show both thinly-coated and thickly-coated BC. BC mass per particle of the thinly-coated mode appears to increase as the air mass ages, possibly due to coagulation and/or increased coating of the particles containing smaller BC masses. Differences in the coating indicator patterns for similarly-aged air masses may be due to differences in atmospheric processing on each day, including mixing with non-MCMA air masses.

2010 ◽  
Vol 10 (1) ◽  
pp. 219-237 ◽  
Author(s):  
R. Subramanian ◽  
G. L. Kok ◽  
D. Baumgardner ◽  
A. Clarke ◽  
Y. Shinozuka ◽  
...  

Abstract. A single particle soot photometer (SP2) was operated on the NCAR C-130 during the MIRAGE campaign (part of MILAGRO), sampling black carbon (BC) over Mexico. The highest BC concentrations were measured over Mexico City (sometimes as much as 2 μg/m3) and over hill-fires to the south of the city. The age of plumes outside of Mexico City was determined using a combination of HYSPLIT trajectories, WRF-FLEXPART modeling and CMET balloon tracks. As expected, older, diluted air masses had lower BC concentrations. A comparison of carbon monoxide (CO) and BC suggests a CO background of around 65 ppbv, and a background-corrected BC/COnet ratio of 2.89±0.89 (ng/m3-STP)/ppbv (average ± standard deviation). This ratio is similar for fresh emissions over Mexico City, as well as for aged airmasses. Comparison of light absorption measured with a particle soot absorption photometer (PSAP) and the SP2 BC suggests a BC mass-normalized absorption cross-section (MAC) of 10.9±2.1 m2/g at 660 nm (or 13.1 m2/g @ 550 nm, assuming MAC is inversely dependent on wavelength). This appears independent of aging and similar to the expected absorption cross-section for aged BC, but values, particularly in fresh emissions, could be biased high due to instrument artifacts. SP2-derived BC coating indicators show a prominent thinly-coated BC mode over the Mexico City Metropolitan Area (MCMA), while older air masses show both thinly-coated and thickly-coated BC. Some 2-day-old plumes do not show a prominent thickly-coated BC mode, possibly due to preferential wet scavenging of the likely-hydrophilic thickly-coated BC.


2008 ◽  
Vol 8 (3) ◽  
pp. 10189-10225 ◽  
Author(s):  
J. C. Barnard ◽  
R. Volkamer ◽  
E. I. Kassianov

Abstract. Data taken from the MCMA-2003 and the 2006 MILAGRO field campaigns are used to examine the absorption of solar radiation by the organic component of aerosols. Using irradiance data from a Multi-Filter Rotating Shadowband Radiometer (MFRSR) and an actinic flux spectroradiometer (SR), we derive aerosol single scattering albedo, π0,λ, as a function of wavelength, λ. We find that in the near-UV spectral range (250 to 400 nm) π0,λ is much lower compared to π0,λ at 500 nm indicating enhanced absorption in the near-UV range. Absorption by elemental carbon, dust, or gas cannot account for this enhanced absorption leaving the organic part of the aerosol as the only possible absorber. We use data from a surface deployed Aerodyne Aerosol Mass Spectrometer (AMS) along with the inferred π0,λ to estimate the Mass Absorption Cross section (MAC) for the organic carbon. We find that the MAC is about 10.5 m2/g at 300 nm and falls close to zero at about 500 nm; values that are roughly consistent with other estimates of organic carbon MAC. These MAC values can be considered as "radiatively correct" because when used in radiative transfer calculations the calculated irradiances/actinic fluxes match those measured at the wavelengths considered here. For an illustrative case study described here, we estimate that the light absorption by the "brown" (organic) carbonaceous aerosol can add about 40% to the light absorption of black carbon in Mexico City. This contribution will vary depending on the relative abundance of organic carbon relative to black carbon. Furthermore, our analysis indicates that organic aerosol would slow down photochemistry by selectively scavenging the light reaching the ground at those wavelengths that drive photochemical reactions. Finally, satellite retrievals of trace gases that are used to infer emissions currently assume that the MAC of organic carbon is zero. For trace gases that are retrieved using wavelengths shorter then 420 nm (i.e. SO2, HCHO, halogenoxides, NO2), the assumption of non-zero MAC values will induce an upward correction to the inferred emissions. This will be particularly relevant in polluted urban atmospheres and areas of biomass burning where organic aerosols are particularly abundant.


2020 ◽  
Author(s):  
Jie Luo ◽  
Yongming Zhang ◽  
Qixing Zhang

Abstract. In this work, we developed a numerical method to investigate the effects of black carbon morphology on the estimation of brown carbon (BrC) absorption using the Absorption Ångström exponent (AAE) method. Pseudo measurements of the total absorption were generated based on several morphologically mixed black carbon (BC) models, then the BrC absorption was inferred based on different AAE methods. By comparing the estimated BrC absorption with True BrC absorption, we found that both AAE = 1 and Mie AAE methods do not provide accurate estimation for the BrC absorption, and the estimated BrC absorption can deviate several times from True BrC absorption. The newly proposed Wavelength Dependent AAE (WDA) method does not necessarily improve the estimations, sometimes it may even provide worse estimations than the AAE = 1 and Mie AAE methods. Fixing the fractal dimension to be 1.8, the deviation between the estimated BrC mass absorption cross-section (MAC) and True BrC MAC can reach approximately 9 m2/g, which is far more than brown carbon MAC itself. Therefore, the estimation of BrC absorption based on the AAE method should carefully consider the morphological effects of BC. Our findings highlight the BC morphological effects on the BrC absorption estimation.


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