References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-7-1645-2007

Estimation of a "radiatively correct" black carbon specific absorption during the Mexico City Metropolitan Area (MCMA) 2003 field campaign

Barnard

J. C.

¹ Kassianov

E. I.

¹ Ackerman

T. P.

¹ ³ Johnson

² ⁴ Zuberi

² ⁵ Molina

L. T.

² Molina

M. J.

² ⁴

Pacific Northwest National Laboratory, Richland, WA, USA

Massachusetts Institute of Technology, Cambridge, MA, USA

now at: University of Washington, Seattle, WA, USA

now at: University of California, San Diego, CA, USA

now at: GEO2 Technologies, Woburn, MA, USA

27 03 2007

7 6 1645 1655

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

This article is available from http://www.atmos-chem-phys.net/7/1645/2007/acp-7-1645-2007.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/7/1645/2007/acp-7-1645-2007.pdf

During the Mexico City Metropolitan Area (MCMA) field campaign of 2003, measurements of the shortwave radiation field allowed the inference of the black carbon (BC) specific absorption, αλ, defined as the monochromatic absorption cross section per unit mass (with units of m2/g). The averaged values of αλ derived from the method here are either 8.9 m2/g or 8.2 m2/g at 500 nm, depending upon the physical and optical parameters assumed for BC. These results are reasonably consistent with those of Schuster et al. (2005), 9.5 m2/g, and Baumgartner et al. (2002), 7.0 m2/g, both measured at 550 nm. The αλ values reported in this paper should only be considered effective, "radiatively correct" values because when used in radiative transfer calculations the calculated irradiances match the measured irradiances at 500 nm. The specific absorption so defined can assume a wide range of values, depending upon: (1) the assumptions made prior to the retrieval (e.g., shell/core aerosol configuration), and (2) values chosen for BC density and refractive index. The range of possible values is large, corresponding to a "worst case" uncertainty of about ±70%, assuming that all errors are additive and of the same sign so that no error cancellation occurs.

References 1

Ackerman, T. P. and Toon, O. B.: Absorption of visible radiation in atmosphere containing mixtures of absorbing and non-absorbing particles, Appl. Opt., 20, 3661–3668, 1981.

Arnott, W. P., Moosmüller, H., Sheridan, P. J., Ogren, J. A., Raspet, R., Slaton, W. V., Hand, J. L., Kreidenweis, S. M., and Collett, J. L.: Photoacoustic and filter-based ambient aerosol light absorption measurements: Instrument comparisons and the role of relative humidity, J. Geophys. Res., 108(D1), 4034, doi:10.1029/2002JD002165,2003.

Baumgartner, D., Raga, G., Kok, G., Ogren, J., Rosas, I., Baez, A., and Novakov, T.: On the evolution of aerosol properties at a mountain site above Mexico City, J. Geophys. Res., 105, 22 243–22 253, 2000.

Baumgartner, D., Raga, G., Peralta, O., Rosas, I., Castro, T., Kuhlbusch, T., John, A., Petzold, A.: Diagnosing black carbon trends in large urban areas using carbon monoxide measurements, J. Geophys. Res., 107(D21) 8342, doi:10.1029/2001JD000626, 2002.

Bergstrom, R. W., Russell, P. B., and Hignett, P.: Wavelength dependence of the absorption of black carbon particles: Predictions and results from the TARFOX experiment and implications for the aerosol single scattering albedo, J. Atmos. Sci., 59, 567–577, 2002.

Bohren, C. F. and Huffman, D. R.: Absorption and scattering of light by small particles, John Wiley & Sons, New York, 1983.

Bond, T. C. and Bergstrom, R. W.: Light absorption by carbonaceous particles: An investigative review, Aerosol Sci. Technol., 40, 27–67, 2006.

Bond, T. C., Habib, G., and Bergstrom, R. W.: Limitations in the enhancement of visible light absorption due to mixing state, J. Geophys. Res., 111, D20211, doi:10.1029/2006JD007315. 2006.

Chung, S. H. and Seinfeld, J. H.: Global distribution and climate forcing of carbonaceous aerosols, J. Geophys. Res., 107(D19), 4407, doi:10.1029/2001JD001397, 2002.

Chylek, P., Videen, G., Ngo, D., Pinnick, R. G., and Klett, J. D.: Effect of black carbon on the optical-properties and climate forcing of sulfate aerosols, J. Geophys. Res., 100(D8), 16 325–16 332, 1995.

Dubovik, O. and King, M. D.: A lexible inversion algorithm for retrieval of aerosol optical properties from Sun and sky radiance measurements, J. Geophys. Res., 105(D16), 20 673–20 696, 2000.

Dubovik, O., Holben, B., Eck, T. F., Smirnov, A., Kaufman, Y. J., King, M. D., Tanré, D., and Slutsker, I.: Variability of absorption amd optical properties of key aerosol types observed in worldwide locations, J. Atmos. Sci., 59, 590–608, 2002.

Fast, J. D. and Zhong, S. Y.: Meteorological factors associated with inhomogeneous ozone concentrations within the Mexico City basin, J. Geophys. Res., 103(D15), 18 927–18 946, 1998.

Fuller, K. A., Malm, W. C., and Kreidenweis, S. M.: Effects of mixing on extinction by carbonaceous particles, J. Geophys. Res., 104(D13), 15 941–15 954, 1999.

Gaffney, J. S., Marley, N. A., Cunningham, M. M., and Doskey, P. V.: Measurements of peroxyacyl nitrates (PANS) in Mexico City: implications for megacity air quality impacts on regional scales, Atmos. Environ., 33(30), 5003–5012, 1999.

Goering, C. D., L'Ecuyer, T. S., Stephens, G. L., Slusser, J. R., Scott, G., Davis, J., Barnard, J. C., and Madronich, S.: Simultaneous retrievals of column ozone and aerosol optical properties from direct and diffuse solar irradiance measurements, J. Geophys. Res., 110, D05204, doi:10.1029/2004JD005330, 2005.

Harrison, L., Michalsky, J., and Berndt, J.: Automated multifilter rotating shadow-band radiometer: an instrument for optical depth and radiation measurements, Appl. Opt., 33, 5118–5125, 1994.

Heintzenberg, J., Charlson, R. J., Clarke, A. D., Liousse, C., Ramaswamy, V., Shine, K. P., Wendisch, M., and Helas, G.: Measurements and modeling of aerosol single-scattering albedo: Progress, problems, and prospects, Beitr. Phys. Atmosph., 70, 249–263, 1997.

Holben, B. N., Eck, T. F., Slutsker, I., Tanre, D., Buis, J. P., Setzer, A., Vermote, E., Reagan, J. A., Kaufman, Y., Nakajima, T., Lavenu, F., Jankowiak, I., and Smirnov, A.: AERONET – A federated instrument network and data archive for aerosol characterization, Remot. Sens. Environ., 66, 1–16, 1998.

Horvath, H.: Atmospheric light-absorption – a review, Atmos. Environ., 27(3), 293–317, 1993.

Jacobson, M. Z.: Isolating nitrated and aromatic aerosols and nitrated aromatic gases as sources of ultraviolet light absorption, J. Geophys. Res., 104(D3), 3527–3542, 1999.

Jacobson, M. Z.: A physically-based treatment of elemental carbon optics: Implications for global direct forcing of aerosols, Geophys. Res. Lett., 27(2), 217–220, 2000.

Jacobson, M. Z.: Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols, Nature, 409(6821), 695–697, 2001.

Johnson, K. S., Zuberi, B., Molina, L. T., Molina, M. J., Iedema, M. J., Cowin, J. P., Gaspar, J. D., Wang, C., and Laskin, A.: Processing of soot in an urban environment: case study from the Mexico City Metropolitan Area, Atmos. Chem. Phys., 5, 3033–3043, 2005.

Kassianov, E. I., Barnard, J. C., and Ackerman, T. P.: Retrieval of aerosol microphysical properties using surface MFRSR data: Modeling and observations, J. Geophys. Res., 110, D09201, doi:10.1029/2004JD005337, 2005.

King, M., Byrne, D., Herman, B., and Reagan, J.: Aerosol size distribution obtained by inversion of spectral optical depth measurements, J. Atmos. Sci., 35, 2153–2167, 1978.

Kirchstetter, T. W., Novakov, T., and Hobbs, P. V.: Evidence that the spectral dependence of light absorption by aerosols is affected by organic carbon, J. Geophys. Res., 109, D21208, doi:10.1029/2004JD004999, 2004.

Lesins, G., Chylek, P., and Lohmann, U.: A study of internal and external mixing scenarios and its effect on aerosol optical properties and direct radiative forcing, J. Geophys. Res., 107(D10), 4094, doi:10.1029/2001JD00973,2002.

Liousse, C., Cachier, H., and Jennings, S. G.: Optical and thermal measurements of black carbon aerosol content in different environments - variation of the specific attenuation cross-section, sigma (sigma), Atmos. Environ., 27(8), 1203–1211, 1993.

Liu, L. and Mishchenko, M. I.: Effects of aggregation on scattering and radiative properties of soot aerosols, J. Geophys. Res., 110, D11211, doi:10.1029/2004JD005649, 2005.

Long, C. N. and Ackerman, T. P.: Identification of clear skies from broadband pyranometer measurements and calculation of downwelling shortwave cloud effects, J. Geophys. Res., 105(D12), 15 609–15 626, 2000.

Marley, N. A., Gaffney, J. S., Baird, C., Blazer, C. A., Drayton, P. J., and Frederick, J. E.: An empirical method for the determination of the complex refractive index of size-fractionated atmospheric aerosols for radiative transfer calculations, Aerosol Sci. Technol., 34(6), 535–549, 2001.

Michalsky, J. J., Schlemmer, J. A., Berkheiser, W. E., Berndt, J. L., Harrison, L. C., Laulainen, N. S., Larson, N. R., and Barnard, J. C.: Multi-year measurements of aerosol optical depth in the atmospheric radiation measurement and quantitative links programs., J. Geophys. Res., 106(D11), 12 099–12 107, 2001.

Molina, M. J., Molina, L. T., West, J., Sosa, G., Sheinbaum-Pardo, C., San-Martini, F., Zavala, M. A., McRae, G.: Air pollution science in the MCMA: Understanding source-receptor relationships through emissions inventories, measurements, and modeling, in: Air Quality in the Mexico Megacity: An Integrated Assessent, edited by: Molina, M. J. and Molina, L. T., Kluwer Academic Publishers, Dordrecht, The Netherlands, 2002, pp. 137–202.

Moosmüller, H., Arnott, W. P., Rogers, C. F., Chow, J. C., Frazier, C. A., Sherman, L. E., and Dietrich, D. L.: Photoacoustic and filter measurements related to aerosol light absorption during the Northern Front Range Air Quality Study (Colorado 1996/1997), J. Geophys. Res., 103(D21), 28 149–28 157, 1998.

Park, K., Kittleson, D. B., Zachariah, M. R., and McMurry, P. H.: Measurement of inherent material density of nanoparticle agglomerates, J. Nanoparticle Res., 6, 267–272, 2004.

Penner, J. E., Chuang, C. C., and Grant, K.: Climate forcing by carbonaceous and sulfate aerosols, Clim. Dyn., 14(12), 839–851, 1998.

Petters, J. L., Saxena, V. K., Slusser, J. R., Wenny, B. N., and Madronich, S.: Aerosol single scattering albedo retrieved from measurements of surface UV irradiance and a radiative transfer model, J. Geophys. Res., 108(D9), 4288, doi:10.1029/2002JD002360, 2003.

Petzold, A., Kopp, C., and Niessner, R.: The dependence of the specific attenuation cross-section on black carbon mass fraction and particle size, Atmos. Environ., 31(5), 661–672, 1997.

Riemer, N., Vogel, H., Vogel, B., and Fiedler, F.: Modeling aerosols on the mesoscale-gamma: Treatment of soot aerosol and its radiative effects, J. Geophys. Res., 108(D19), 4601, doi:10.1029/2003JD003448, 2003.

Salcedo, D., Onasch, T. B., Dzepina, K., Canagaratna, M. R., Zhang, Q., Huffman, J. A., DeCarlo, P. F., Jayne, J. T., Mortimer, P., Worsnop, D. R., Kolb, C. E., Johnson, K. S., Zuberi, B., Marr, L. C., Volkamer, R., Molina, L. T., Molina, M. J., Cardenas, B., Bernabé, R. M., Márquez, C., Gaffney, J. S., Marley, N. A., Laskin, A., Shutthanandan, V., Xie, Y., Brune, W., Lesher, R., Shirley, T., and Jimenez, J. L.: Characterization of ambient aerosols in Mexcico City during the MCMA-2003 campaign with Aerosol Mass Spectrometry: Results from the CENICA supersite, Atmos. Chem. Phys., 5, 925–946, 2006.

Sato, M., Hansen, J., Koch, D., Lacis, A., Ruedy, R., Dubovik, O., Holben, B., Chin, M., and Novakov, T.: Global atmospheric black carbon inferred from AERONET, Proceedings National Academy Sci. US, 100, 6319–6324, 2003.

Schnaiter, M., Horvath, H., Möhler, O., Naumann, K.-H., Saathoff, H., and Schöck, O. W.: UV-VIS-NIR spectral optical properties of soot and soot-containing aerosols, J. Aerosol Sci., 34, 1421–1444, 2003.

Schuster, G. L.: Inferring the specific absorption and concentration of black carbon from AERONET aerosol retrievals, Ph. D. thesis, The Pennsylvania State University, 2004.

Schuster, G. L., Dubovik, O., Holben, B. N., and Clothiaux, E. E.: Inferring black carbon content and specific absorption from AERONET retrievals, J. Geophys. Res., 101, D10S17, doi:10.1029/2004JD004548, 2005.

Schuster, G. L., Dubovik, O., and Holben, B. N.: Angstrom exponent and bimodal aerosol size distributions, J. Geophys. Res., 111, D07207, doi:10.1029/2005JD006328, 2006.

Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics, John Wiley & Sons, New York, 1998.

Sokolik, I. N. and Toon, O. B.: Incorporation of mineralogical composition of aerosols into models of radiative properties of mineral aerosol from the UV to IR wavelengths, J. Geophys. Res., 104(D8), 9423–9444, 1999.

Toon, O. B., Pollack, J. B., and Khare, B. N.: Optical constants of several atmospheric aerosol species – ammonium sulfate, aluminum oxide, and sodium chloride, J. Geophys. Res., 81(33), 5733–5748, 1976.

Waggoner, A. P., Weiss, R. E., Ahlquist, N. C., Covert, D. S., Will, S., and Charlson, R. J.: Optical characteristics of atmospheric aerosols, Atmos. Environ., 15(10–1), 1891–1909, 1981.

Whiteman, C. D., Zhong, S., Bian, X., Fast, J. D., and Doran, J. C.: Boundary layer evolution and regional-scale diurnal circulations over the Mexico Basin and Mexican plateau, J. Geophys. Res., 105(D8), 10 081–10 102, 2000.

Wu, J.-S., Krishnan, S. S., and Feath, G. M.: Refractive indices at visible wavelengths of soot emitted from buoyant turbulent diffusion flames, J. Heat Transfer, 119, 230–237, 1997.