References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-12-6173-2012

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

Chung

C. E.

¹ Kim

S.-W.

² Lee

³ Yoon

S.-C.

² Lee

Dept. Environmental Science & Engineering, Gwangju Institute of Science and Technology, Gwangju, Korea

School of Earth & Environmental Sciences, Seoul National University, Seoul, Korea

Dept. Earth & Environmental Sciences, Korea University, Seoul, Korea

17 07 2012

12 14 6173 6184

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.

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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.

References 1

Adachi, K. and Buseck, P. R.: Internally mixed soot, sulfates, and organic matter in aerosol particles from Mexico City, Atmos. Chem. Phys., 8, 6469–6481, http://dx.doi.org/10.5194/acp-8-6469-2008doi:10.5194/acp-8-6469-2008, 2008.

Adler, G., Riziq, A. A., Erlick, C., and Rudich, Y.: Effect of intrinsic organic carbon on the optical properties of fresh diesel soot, P. Natl. Acad. Sci. USA, 107, 6699–6704, 2010.

Alexander, D. T. L., Crozier, P. A., and Anderson, J. R.: Brown carbon spheres in East Asian outflow and their optical properties, Science, 321, 833–836, 2008.

Andreae, M. O. and Gelencsér, A.: Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols, Atmos. Chem. Phys., 6, 3131–3148, http://dx.doi.org/10.5194/acp-6-3131-2006doi:10.5194/acp-6-3131-2006, 2006.

Arnott, W. P., Hamasha, K., Moosmüller, H., Sheridan, P. J., and Ogren, J. A.: Towards aerosol light-absorption measurements with a 7-wavelength aethalometer: Evaluation with a photoacoustic instrument and 3-wavelength nephelometer, Aerosol Sci. Tech., 39, 17–29, 2005.

Bergstrom, R. W., Pilewskie, P., Russell, P. B., Redemann, J., Bond, T. C., Quinn, P. K., and Sierau, B.: Spectral absorption properties of atmospheric aerosols, Atmos. Chem. Phys., 7, 5937–5943, http://dx.doi.org/10.5194/acp-7-5937-2007doi:10.5194/acp-7-5937-2007, 2007.

Birch, M. E. and Cary, R. A.: Elemental carbon-based method for monitoring occupational exposures to particulate diesel exhaust, Aerosol Sci. Tech., 25, 221–241, 1996.

Chakrabarty, R. K., Moosmüller, H., Chen, L.-W. A., Lewis, K., Arnott, W. P., Mazzoleni, C., Dubey, M. K., Wold, C. E., Hao, W. M., and Kreidenweis, S. M.: Brown carbon in tar balls from smoldering biomass combustion, Atmos. Chem. Phys., 10, 6363–6370, http://dx.doi.org/10.5194/acp-10-6363-2010doi:10.5194/acp-10-6363-2010, 2010.

Cheng, Y., He, K.-B., Zheng, M., Duan, F.-K., Du, Z.-Y., Ma, Y.-L., Tan, J.-H., Yang, F.-M., Liu, J.-M., Zhang, X.-L., Weber, R. J., Bergin, M. H., and Russell, A. G.: Mass absorption efficiency of elemental carbon and water-soluble organic carbon in Beijing, China, Atmos. Chem. Phys., 11, 11497–11510, http://dx.doi.org/10.5194/acp-11-11497-2011doi:10.5194/acp-11-11497-2011, 2011.

Chow, J. C., Watson, J. G., Louie, P. K. K., Chen, L. W. A., and Sin, D.: Comparison of PM$_2.5$ carbon measurement methods in Hong Kong, China, Environ. Pollut., 137, 334–344, 2005.

Chung, C. E., Lee, K., and Müller, D.: Effect of internal mixture on black carbon radiative forcing, Tellus B, 64, 1–13, http://dx.doi.org/10.3402/tellusb.v64i0.10925doi:10.3402/tellusb.v64i0.10925, 2012.

Clarke, A. D., Shinozuka, Y., Kapustin, V. N., Howell, S., Huebert, B., Doherty, S., Anderson, T., Covert, D., Anderson, J., Hua, X., Moore, K. G., II, McNaughton, C., Carmichael, G., and Weber, R.: Size distributions and mixtures of dust and black carbon aerosol in Asian outflow: Physiochemistry and optical properties, J. Geophys. Res., 109, D15S09, http://dx.doi.org/10.1029/2003jd004378doi:10.1029/2003jd004378, 2004.

Clarke, A., McNaughton, C., Kapustin, V., Shinozuka, Y., Howell, S., Dibb, J., Zhou, J., Anderson, B., Brekhovskikh, V., Turner, H., and Pinkerton, M.: Biomass burning and pollution aerosol over North America: Organic components and their influence on spectral optical properties and humidification response, J. Geophys. Res.-Atmos., 112, D12S18, http://dx.doi.org/10.1029/2006JD007777doi:10.1029/2006JD007777, 2007

Collaud Coen, M., Weingartner, E., Apituley, A., Ceburnis, D., Fierz-Schmidhauser, R., Flentje, H., Henzing, J. S., Jennings, S. G., Moerman, M., Petzold, A., Schmid, O., and Baltensperger, U.: Minimizing light absorption measurement artifacts of the Aethalometer: evaluation of five correction algorithms, Atmos. Meas. Tech., 3, 457–474, http://dx.doi.org/10.5194/amt-3-457-2010doi:10.5194/amt-3-457-2010, 2010.

Cross, E. S., Onasch, T. B., Ahern, A., Wrobel, W., Slowik, J. G., Olfert, J., Lack, D. A., Massoli, P., Cappa, C. D., Schwarz, J. P., Spackman, J. R., Fahey, D. W., Sedlacek, A., Trimborn, A., Jayne, J. T., Freedman, A., Williams, L. R., Ng, N. L., Mazzoleni, C., Dubey, M., Brem, B., Kok, G., Subramanian, R., Freitag, S., Clarke, A., Thornhill, D., Marr, L. C., Kolb, C. E., Worsnop, D. R., and Davidovits, P.: Soot Particle Studies – Instrument Inter-Comparison – Project Overview, Aerosol Sci. Tech., 44, 592–611, http://dx.doi.org/10.1080/02786826.2010.482113doi:10.1080/02786826.2010.482113, 2010.

Dee, D. P., Uppala, S. M., Simmons, A. J., Berrisford, P., Poli, P., Kobayashi, S., Andrae, U., Balmaseda, M. A., Balsamo, G., Bauer, P., Bechtold, P., Beljaars, A. C. M., van de Berg, L., Bidlot, J., Bormann, N., Delsol, C., Dragani, R., Fuentes, M., Geer, A. J., Haimberger, L., Healy, S. B., Hersbach, H., Hólm, E. V., Isaksen, L., Kållberg, P., Köhler, M., Matricardi, M., McNally, A. P., Monge-Sanz, B. M., Morcrette, J. J., Park, B. K., Peubey, C., de Rosnay, P., Tavolato, C., Thépaut, J. N., and Vitart, F.: The ERA-Interim reanalysis: configuration and performance of the data assimilation system, Q. J. Roy. Meteor. Soc., 137, 553–597, 2011.

Eck, T. F., Holben, B. N., Sinyuk, A., Pinker, R. T., Goloub, P., Chen, H., Chatenet, B., Li, Z., Singh, R. P., Tripathi, S. N., Reid, J. S., Giles, D. M., Dubovik, O., O'Neill, N. T., Smirnov, A., Wang, P., and Xia, X.: Climatological aspects of the optical properties of fine/coarse mode aerosol mixtures, J. Geophys. Res., 115, D19205, http://dx.doi.org/10.1029/2010jd014002doi:10.1029/2010jd014002, 2010.

Flowers, B. A., Dubey, M. K., Mazzoleni, C., Stone, E. A., Schauer, J. J., Kim, S.-W., and Yoon, S. C.: Optical-chemical-microphysical relationships and closure studies for mixed carbonaceous aerosols observed at Jeju Island; 3-laser photoacoustic spectrometer, particle sizing, and filter analysis, Atmos. Chem. Phys., 10, 10387–10398, http://dx.doi.org/10.5194/acp-10-10387-2010doi:10.5194/acp-10-10387-2010, 2010.

Forster, P., Ramaswamy, V., Artaxo, P., Berntsen, T., Betts, R., Fahey, D. W., Haywood, J., Lean, J., Lowe, D. C., Myhre, G., Nganga, J., Prinn, R., Raga, G., Schulz, M., and Van Dorland, R.: Changes in Atmospheric Constituents and in Radiative Forcing, in: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K. B., Tignor, M., and Miller, H. L.. Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 2007.

Gadhavi, H. and Jayaraman, A.: Absorbing aerosols: contribution of biomass burning and implications for radiative forcing, Ann. Geophys., 28, 103–111, http://dx.doi.org/10.5194/angeo-28-103-2010doi:10.5194/angeo-28-103-2010, 2010.

Gyawali, M., Arnott, W. P., Lewis, K., and Moosmüller, H.: In situ aerosol optics in Reno, NV, USA during and after the summer 2008 California wildfires and the influence of absorbing and non-absorbing organic coatings on spectral light absorption, Atmos. Chem. Phys., 9, 8007–8015, http://dx.doi.org/10.5194/acp-9-8007-2009doi:10.5194/acp-9-8007-2009, 2009.

Hansen, A. D.: The Aethalometer – User manual, 2005.

Hess, M., Koepke, P., and Schult, I.: Optical Properties of Aerosols and Clouds: The Software Package OPAC, B. Am. Meteorol. Soc., 79, 831–844, 1998.

Hoffer, A., Gelencsér, A., Guyon, P., Kiss, G., Schmid, O., Frank, G. P., Artaxo, P., and Andreae, M. O.: Optical properties of humic-like substances (HULIS) in biomass-burning aerosols, Atmos. Chem. Phys., 6, 3563–3570, http://dx.doi.org/10.5194/acp-6-3563-2006doi:10.5194/acp-6-3563-2006, 2006.

Huebert, B. J., Bates, T., Russell, P. B., Shi, G., Kim, Y. J., Kawamura, K., Carmichael, G., and Nakajima, T.: An overview of ACE-Asia: Strategies for quantifying the relationships between Asian aerosols and their climatic impacts, J. Geophys. Res., 108, 8633, http://dx.doi.org/10.1029/2003jd003550doi:10.1029/2003jd003550, 2003.

Jung, J., Lee, H., Kim, Y. J., Liu, X., Zhang, Y., Hu, M., and Sugimoto, N.: Optical properties of atmospheric aerosols obtained by in situ and remote measurements during 2006 Campaign of Air Quality Research in Beijing (CAREBeijing-2006), J. Geophys. Res., 114, D00G02, http://dx.doi.org/10.1029/2008jd010337doi:10.1029/2008jd010337, 2009.

Katrinak, K. A., Rez, P., Perkes, P. R., and Buseck, P. R.: Fractal geometry of carbonaceous aggregates from an urban aerosol, Environ. Sci. Tech., 27, 539–547, 1993.

Kim, K. W., He, Z., and Kim, Y. J.: Physicochemical characteristics and radiative properties of Asian dust particles observed at Kwangju, Korea, during the 2001 ACE-Asia intensive observation period, J. Geophys. Res., 109, D19S02, http://dx.doi.org/10.1029/2003jd003693doi:10.1029/2003jd003693, 2004.

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, http://dx.doi.org/10.1029/2004jd004999doi:10.1029/2004jd004999, 2004.

Lamarque, J.-F., Bond, T. C., Eyring, V., Granier, C., Heil, A., Klimont, Z., Lee, D., Liousse, C., Mieville, A., Owen, B., Schultz, M. G., Shindell, D., Smith, S. J., Stehfest, E., Van Aardenne, J., Cooper, O. R., Kainuma, M., Mahowald, N., McConnell, J. R., Naik, V., Riahi, K., and van Vuuren, D. P.: Historical (1850–2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols: methodology and application, Atmos. Chem. Phys., 10, 7017–7039, http://dx.doi.org/10.5194/acp-10-7017-2010doi:10.5194/acp-10-7017-2010, 2010.

Lawrence, M. G. and Lelieveld, J.: Atmospheric pollutant outflow from southern Asia: a review, Atmos. Chem. Phys., 10, 11017–11096, http://dx.doi.org/10.5194/acp-10-11017-2010doi:10.5194/acp-10-11017-2010, 2010.

Lee, S., Yoon, S. C., Kim, S. W., Kim, Y. P., Ghim, Y. S., Kim, J. H., Kang, C. H., Kim, Y. J., Chang, L. S., and Lee, S. J.: Spectral dependency of light scattering/absorption and hygroscopicity of pollution and dust aerosols in Northeast Asia, Atmos. Environ., 50, 246–254, http://dx.doi.org/10.1016/j.atmosenv.2011.12.026doi:10.1016/j.atmosenv.2011.12.026, 2012.

Lewis, K., Arnott, W. P., Moosmüller, H., and Wold, C. E.: Strong spectral variation of biomass smoke light absorption and single scattering albedo observed with a novel dual-wavelength photoacoustic instrument, J. Geophys. Res., 113, D16203, http://dx.doi.org/10.1029/2007jd009699doi:10.1029/2007jd009699, 2008.

Moffet, R. C. and Prather, K. A.: In-situ measurements of the mixing state and optical properties of soot with implications for radiative forcing estimates, P. Natl. Acad. Sci., 106, 11872, http://dx.doi.org/10.1073/pnas.0900040106doi:10.1073/pnas.0900040106, 2009.

Nakajima, T., Yoon, S.-C., Ramanathan, V., Shi, G.-Y., Takemura, T., Higurashi, A., Takamura, T., Aoki, K., Sohn, B.-J., Kim, S.-W., Tsuruta, H., Sugimoto, N., Shimizu, A., Tanimoto, H., Sawa, Y., Lin, N.-H., Lee, C.-T., Goto, D., and Schutgens, N.: Overview of the Atmospheric Brown Cloud East Asian Regional Experiment 2005 and a study of the aerosol direct radiative forcing in east Asia, J. Geophys. Res., 112, D24S91, http://dx.doi.org/10.1029/2007jd009009doi:10.1029/2007jd009009, 2007.

Park, R. J., Jacob, D. J., Palmer, P. I., Clarke, A. D., Weber, R. J., Zondlo, M. A., Eisele, F. L., Bandy, A. R., Thornton, D. C., Sachse, G. W., and Bond, T. C.: Export efficiency of black carbon aerosol in continental outflow: Global implications, J. Geophys. Res.-Atmos., 110, D11205, doi:10.1029/2004JD005432, 2005.

Polidori, A., Turpin, B., Lim, H. J., Cabada, J., Subramanian, R., Pandis, S., and Robinson, A.: Local and regional secondary organic aerosol: Insights from a year of semi-continuous carbon measurements at Pittsburgh, Aerosol Sci. Tech., 40, 861–872, 2006.

Quinn, P. K., Coffman, D. J., Bates, T. S., Welton, E. J., Covert, D. S., Miller, T. L., Johnson, J. E., Maria, S., Russell, L., Arimoto, R., Carrico, C. M., Rood, M. J., and Anderson, J.: Aerosol optical properties measured on board the Ronald H. Brown during ACE-Asia as a function of aerosol chemical composition and source region, J. Geophys. Res.-Atmos., 109, D19S01, http://dx.doi.org/10.1029/2003JD004010doi:10.1029/2003JD004010, 2004.

Russell, P. B., Bergstrom, R. W., Shinozuka, Y., Clarke, A. D., DeCarlo, P. F., Jimenez, J. L., Livingston, J. M., Redemann, J., Dubovik, O., and Strawa, A.: Absorption Angstrom Exponent in AERONET and related data as an indicator of aerosol composition, Atmos. Chem. Phys., 10, 1155–1169, http://dx.doi.org/10.5194/acp-10-1155-2010doi:10.5194/acp-10-1155-2010, 2010.

Russell, L. M., Bahadur, R., and Ziemann, P. J.: Identifying organic aerosol sources by comparing functional group composition in chamber and atmospheric particles, P. Natl. Acad. Sci. USA, 108, 3516–3521, 2011.

Schnaiter, M., Linke, C., Möhler, O., Naumann, K. H., Saathoff, H., Wagner, R., Schurath, U., and Wehner, B.: Absorption amplification of black carbon internally mixed with secondary organic aerosol, J. Geophys. Res., 110, D19204, http://dx.doi.org/10.1029/2005jd006046doi:10.1029/2005jd006046, 2005.

Watson, A. Y. and Valberg, P. A.: Carbon Black and Soot: Two Different Substances, AIHAJ – American Industrial Hygiene Association, 62, 218–228, http://dx.doi.org/10.1080/15298660108984625doi:10.1080/15298660108984625, 2001.

Yang, M., Howell, S. G., Zhuang, J., and Huebert, B. J.: Attribution of aerosol light absorption to black carbon, brown carbon, and dust in China – interpretations of atmospheric measurements during EAST-AIRE, Atmos. Chem. Phys., 9, 2035–2050, http://dx.doi.org/10.5194/acp-9-2035-2009doi:10.5194/acp-9-2035-2009, 2009.