Atmos. Chem. Phys. Discuss., 13, 18233-18276, 2013
© Author(s) 2013. This work is distributed
under the Creative Commons Attribution 3.0 License.
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Size-resolved measurements of brown carbon and estimates of their contribution to ambient fine particle light absorption based on water and methanol extracts
J. Liu1, M. Bergin1,2, H. Guo1, L. King1, N. Kotra2, E. Edgerton3, and R. J. Weber1
1School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
2School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA, USA
3Atmospheric Research and Analysis, Inc, Cary, N. Carolina, USA

Abstract. Light absorbing organic carbon, often termed brown carbon, has the potential to significantly contribute to the visible light absorption budget, particularly at shorter wavelengths. Currently, the relative contributions of particulate brown carbon to light absorption, as well as the sources of brown carbon are poorly understood. With this in mind field measurements were made at both urban (Atlanta), and rural (Yorkville) sites in Georgia. Measurements in Atlanta were made at both a central site and a road side site adjacent to a main highway near the city center. Fine particle brown carbon optical absorption is estimated based on Mie calculations using direct size resolved measurements of chromophores in filter extracts. Size-resolved atmospheric aerosol samples were collected using a cascade impactor and analyzed for water-soluble organic carbon (WSOC), organic and elemental carbon (OC and EC), and solution light absorption spectra of water and methanol extracts. Methanol extracts were more light-absorbing than water extracts for all size ranges and wavelengths. Absorption refractive indices of the organic extracts were calculated from solution measurements for a range of wavelengths and used with Mie theory to predict the light absorption by fine particles comprised of these components, under the assumption that brown carbon and other aerosol components were externally mixed. For all three sites, chromophores were predominately in the accumulation mode with an aerodynamic mean diameter of 0.5 μm, an optically effective size range resulting in predicted particle light absorption being a factor of 2 higher than bulk solution absorption. Fine particle absorption was also measured with a Multi-Angle Absorption Photometer (MAAP) and seven-wavelength Aethalometer. Scattering-corrected aethalometer and MAAP absorption were in good agreement at 670 nm and Mie-estimated absorption based on size-resolved EC data were within 30% of these optical instruments. When applied to solution measurements, at all sites, Mie-predicted brown carbon absorption at 350 nm contributed a significant fraction (20 to 40%) relative to total light absorption, with highest contributions at the rural site where organic to elemental carbon ratios were highest. Brown carbon absorption, however, was highest by the roadside site due to vehicle emissions. The multi-wavelength aethalometer did not detect brown carbon, having an absorption Ã…ngstrom exponent near one. Although the results are within the estimated Aethalometer uncertainties, the direct measurement of brown carbon in solution definitively shows that it is present and this Mie analysis suggests it is optically important in the near UV range in both a rural and urban environment during summer when biomass burning emissions are low.

Citation: Liu, J., Bergin, M., Guo, H., King, L., Kotra, N., Edgerton, E., and Weber, R. J.: Size-resolved measurements of brown carbon and estimates of their contribution to ambient fine particle light absorption based on water and methanol extracts, Atmos. Chem. Phys. Discuss., 13, 18233-18276, doi:10.5194/acpd-13-18233-2013, 2013.
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