Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 9 11 2009 10.5194/acp-9-3721-2009 http://www.atmos-chem-phys.net/9/3721/2009/ http://www.atmos-chem-phys.net/9/3721/2009/acp-9-3721-2009.html http://www.atmos-chem-phys.net/9/3721/2009/acp-9-3721-2009.pdf 3721 3730 2009-06-09 Primary and secondary contributions to aerosol light scattering and absorption in Mexico City during the MILAGRO 2006 campaign G. Paredes-Miranda gparedes@physics.unr.edu W. P. Arnott J. L. Jimenez A. C. Aiken J. S. Gaffney N. A. Marley Department of Physics, University of Nevada Reno, and the Desert Research Institute, Reno, NV, USA Deptartment of Chemistry and Biochemistry and CIRES University of Colorado, Boulder, CO, USA Department of Chemistry, University of Arkansas, Little Rock, AK, USA Graduate Institute of Technology, University of Arkansas, Little Rock, AK, USA A photoacoustic spectrometer, a nephelometer, an aethalometer, and an aerosol mass spectrometer were used to measure at ground level real-time aerosol light absorption, scattering, and chemistry at an urban site located in North East Mexico City (Instituto Mexicano del Petroleo, Mexican Petroleum Institute, denoted by IMP), as part of the Megacity Impact on Regional and Global Environments field experiment, MILAGRO, in March 2006. Photoacoustic and reciprocal nephelometer measurements at 532 nm accomplished with a single instrument compare favorably with conventional measurements made with an aethalometer and a TSI nephelometer. The diurnally averaged single scattering albedo at 532 nm was found to vary from 0.60 to 0.85 with the peak value at midday and the minimum value at 07:00 a.m. local time, indicating that the Mexico City plume is likely to have a net warming effect on local climate. The peak value is associated with strong photochemical generation of secondary aerosol. It is estimated that the photochemical production of secondary aerosol (inorganic and organic) is approximately 75% of the aerosol mass concentration and light scattering in association with the peak single scattering albedo. A strong correlation of aerosol scattering at 532 nm and total aerosol mass concentration was found, and an average mass scattering efficiency factor of 3.8 m²/g was determined. Comparisons of photoacoustic and aethalometer light absorption with oxygenated organic aerosol concentration (OOA) indicate a very small systematic bias of the filter based measurement associated with OOA and the peak aerosol single scattering albedo. Aiken, A. C., DeCarlo, P. F., Kroll, J. H., Worsnop, D. R., Huffman, J. A., Docherty, K., Ulbrich, I. M., Mohr, C., Kimmel, J. R., Sueper, D., Zhang, Q., Sun, Y., Trimborn, A., Northway, M., Ziemann, P. J., Canagaratna, M. R., Onasch, T. B., Alfarra, R., Prevot, A. S. H., Dommen, J., Duplissy, J., Metzger, A., Baltensperger, U., and Jimenez, J. L.: O/C and OM/OC Ratios of Primary, Secondary, and Ambient Organic Aerosols with High Resolution Time-of-Flight Aerosol Mass Spectrometry, Environ. Sci. Technol., 42, 4478–4485, 2008. Aiken, A. C., Salcedo, D., Cubison, M. J., de Foy, B., Wiedinmyer, C., Huffman, A., DeCarlo, P. F., Ulbrich, I., Docherty, K., Sueper, D., Kimmel, J. R., Worsnop, D., Trimborn, A., Northway, M., Wehrli, M. N., Szidat, S., Prevot, A. S. H., Baltensperger, U., Noda, J., Wacker, L., Stone, E. A., Schauer, J. J., Volkamer, R., Fortner, E., Knighton, B., Wang, J., Laskin, A., Zheng, J., Zhang, R., Gaffney, J., Marley, N. A., Querol, X., Paredes-Miranda, G., Arnott, W. P., Molina, L. T., Sosa, G., and Jimenez, J. L.: Mexico City Aerosol Analysis during MILAGRO using High Resolution Aerosol Mass Spectrometry at the Urban Supersite (T0). Part 1: Overall Fine Particle Composition and Organic Source Apportionment., Atmos. Chem. Phys. Discuss., 9, 8377–8427, 2009. Anderson, T. L., Covert, D. S., Marshall, S. F., Laucks, M. L., Charlson, R. J., Waggoner, A. P., Ogren, J. A., Caldow, R., Holm, R. L., Quant, F. R., Sem, G. J., Wiedensohler, A., Ahlquist, N. A., and Bates, T. S.: Performance characteristics of a high sensitivity, three wavelength, total scatter/backscatter nephelometer, Journal of Atmospheric and Oceanic Technology, 13, 967–986, 1996. Andreae, M. O.: The dark side of aerosols, Nature, 409, 671–672, 2001. Andreae, M. O. and Gelencsér, A.: Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols, Atmos. Chem. Phys., 6, 3131–3148, 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 a 3 wavelength nephelometer, Aerosol Sci. Technol., 39, 17–29, 2005. Arnott, W. P., Moosmüller, H., Rogers, C. F., Jin, T., and Bruch, R.: Photoacoustic spectrometer for measuring light absorption by aerosols: Instrument description, Atmos. Environ., 33, 2845–2852, 1999. Arnott, W. P., Moosmüller, H., and Walker, J. W.: Nitrogen dioxide and kerosene-flame soot calibration of photoacoustic instruments for measurement of light absorption by aerosols., Rev. Sci. Inst., 71(7), 4545–4552, 2000. Bergin, M. H., Cass, G. R., Xu, J., Fang, C., Zeng, L. M., Yu, T., Salmon, L. G., Kiang, C. S., Tang, X. Y., Zhang, Y. H., and Chameides, W. L.: Aerosol radiative, physical, and chemical properties in Beijing during June 1999., J. Geophys. Res., 106(D16), 17969–17980, 2001. Bond, T. C., Anderson, T. L., and Campbell, D.: Calibration and Intercomparison of Filter-Based Measurements of Visible Light Absorption by Aerosols, Aerosol Sci. Technol., 30(6), 582–600, 1999. Bond, T. C. and Bergstrom, R. W.: Light absorption by carbonaceous particles: An investigative review., Aerosol Sci. Technol., 40, 27–67, 2006. Canagaratna, M. R., Jayne, J. T., Jimenez, J. L., Allan, J. D., Alfarra, M. R., Zhang, Q., Onasch, T. B., Drewnick, F., Coe, H., Middlebrook, A., Delia, A., Williams, L. R., Trimborn, A. M., Northway, M. J., DeCarlo, P. F., Kolb, C. E., Davidovits, P., and Worsnop, D. R.: Chemical and Microphysical Characterization of Ambient Aerosols with the Aerodyne Aerosol Mass Spectrometer, Mass Spectrom. Rev., 26, 185–222, 2007. Charlson, R. J., Schwartz, S. E., Hales, J. M., Cess, R. D., Coakley, J. A., Hansen, J. E., and Hofmann, D. J.: Climate Forcing by Anthropogenic Aerosols, Science, 255, 423–429, 1992. de Almeida Castanho, A., Prinn, R., Martins, V., Herold, M., Ichoku, C., and Molina, L.: Analysis of Visible/SWIR surface reflectance ratios for aerosol retrievals from satellite in Mexico City urban area., Atmos. Chem. Phys., 7, 5467–5477, 2007. de Foy, B., Varela, J. R., Molinta, L. T., and Molina, M. J.: Rapid ventilation of the Mexico City basin and regional fate of the urban plume, Atmos. Chem. Phys., 6, 2321–2335, 2006. DeCarlo, P. F., Dunlea, E. J., Kimmel, J. R., Aiken, A. C., Sueper, D., Crounse, J., Wennberg, P. O., Emmons, L., Shinozuka, Y., Clarke, A., Zhou, J., Tomlinson, J., Collins, D. R., Knapp, D., Weinheimer, A. J., Montzka, D. D., Campos, T., and Jimenez, J. L.: Fast Airborne Aerosol Size and Chemistry Measurements with the High Resolution Aerosol Mass Spectrometer during the MILAGRO Campaign, Atmos. Chem. Phys., 8, 4027–4048, 2008. DeCarlo, P. F., Kimmel, J. R., Trimborn, A., Northway, M. J., Jayne, J. T., Aiken, A. C., Gonin, M., Fuhrer, K., Horvath, T., Docherty, K., Worsnop, D. R., and Jimenez., J. L.: Field-Deployable, High-Resolution, Time-of-Flight Aerosol Mass Spectrometer, Anal. Chem., 78, 8281–8289, 2006. Haywood, J. M. and Ramaswamy, V.: Global sensitivity studies of the direct radiative forcing due to anthropogenic sulfate and black carbon aerosols, J. Geophys. Res., 103(D6), 6043–6058, 1998. Herndon, S. C., Onasch, T. B., Wood, E. C., Kroll, J. H., Canagaratna, M. R., Jayne, J. T., Zavala, M. J. A., Knighton, W. B., Mazzoleni, C., Dubey, M. K., Ulbrich, I. M., Jimenez, J. L., Seila, R., de Gow, J. A., de Foy, B., Fast, J. D., Molina, L. T., Kolb, C. E., and Worsnop, D.: Correlation of secondary organic aerosol with odd oxygen in Mexico City, Geophys. Res. Lett., 35, L15804, doi:10.1029/2008GL034058, 2008. Huffman, J., Jayne, J., Drewnick, F., Aiken, A., Onasch, T., Worsnop, D., and Jimenez, J.: Design, Modeling, Optimization, and Experimental Tests of a Particle Beam Width Probe for the Aerodyne Aerosol Mass Spectrometer, Aerosol Sci. Technol., 39(12), 21, 2005. Jacobson, M. Z.: Strong Radiative Heating due to the Mixing State of Black Carbon in Atmospheric Aerosols, Nature, 409, 695–697, 2001. Jauregui, E. and Luyando, E.: Global radiation attenuation by air pollution and its effects on the thermal climate in Mexico City, Int. J. Climatol., 19(6), 683–694, 1999. Jimenez, J. L., Bahreini, R., Cocker, D. R., Zhuang, H., Varutbangkul, V., Flagan, R. C., Seinfeld, J. H., O'Dowd, C. and Hoffmann, T.: New Particle Formation from Photooxidation of Diiodomethane (CH2I2), J. Geophys. Res.-Atmos., 108, (D10), 4318, doi:10.1029/2002JD002452, 2003. Johnson, K. S., Zuberi, B., Molina, L. T., Molina, M. J., Iedema, M. J., Cowin, J. P., Gaspar, D. J., 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. 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:10.1029/2004JD00499, 2004. Lack, D. A., Cappa, C. D., Covert, D. S., Baynard, T., Massoli, P., Sierau, B., Bates, T. S., Quinn, P. K., Lovejoy, E. R., and Ravishankara, A. R.: Bias in Filter Based Aerosol Absorption Measurements Due to Organic Aerosol Loading: Evidence from Ambient Measurements, Aerosol Sci. Technol., 42(12), 1033–1041, 2008. 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, doi:10.1029/2007JD009699, 2008. Mar, E., Sheinbaum, N. A., and Luna, N.: Inventario de emisiones y posibles politicas de mitigacion de gases contaminantes provenientes del sector transporte del area metropolitana de la ciudad de Mexico, Preceedings, Contaminacion Atmosferica III, Instituto de Geofisica, UNAM, 313–339, 2001. Mayol-Bracero, O. L., Gabriel, R., Andreae, M. O., Kirchsteter, T. W., Novakov, T., Ogren, J., Sheridan, P., and Streets, D. G.: Carbonaceous aerosols over the Indian Ocean during the Indian Ocean Experiment (INDOEX): Chemical characterization, optical properties, and probable sources, J. Geophys. Res., 107(D19), 8030, doi:10.1029/2000JD0039, 2002. McComiskey, A., Schwartz, S. E., Schmid, B., Guan, H., Lewis, E. R., Ricchiazzi, P., and Ogren, J. A.: Direct aerosol forcing: Calculation from observables and sensitivities to inputs, J. Geophys. Res., 113, D09202, doi:10.1029/2007JD009170, 2008. Molina, L. T., Kolb, C. E., de Foy, B., Lamb, B. K., Brune, W. H., Jimenez, J. L., Ramos- Villegas, R., Sarmiento, J., Paramo-Figueroa, V. H., Cardenas, B., Gutierrez-Avedoy, V., and Molina, M. J.: Air Quality in North America's Most Populous City – Overview of the MCMA-2003 Campaign., Atmos. Chem. Phys., 7, 2447–2473, 2007. Paatero, P. and Tapper, U.: Positive matrix factorization: A non-negative factor model with optimal utilization of error estimates of data values, Environmetrics, 5, 111–126, 1994. Querol, X., Pey, J., Minguillon, M. C., Perez, N., Alastuey, A., Viana, M., Moreno, T., Bernabe, R. M., Blanco, S., Cardenas, B., Vega, E., Sosa, G., Escalona, S., Ruiz, H., and Artinano, B.: PM speciation and sources in Mexico during MILAGRO campaign, Atmos. Chem. Phys., 8, 111–128, 2008. Rahmah, A. A., Arnott, W. P., and Moosmüller, H.: Integrating nephelometer with a low truncation angle and an extended calibration scheme, Measurement Sci. Technol., 17, 1723–1732, 2006. Salcedo, D., Onasch, T. B., Canagaratha, M., Dzepina, K., Huffman, J. A., Jayne, J. T., Worsnop, D., Kolb, C., Weimer, S., Drewnick, F., Allan, J., A., D. and Jimenez, J.: Technical Note: Use of a beam width probe in an Aerosol Mass Spectrometer to monitor particle collection efficiency in the field., Atmos. Chem. Phys., 7, 549–556, 2007. 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., Bernabe, R. M., Marquez, 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 Mexico City during the MCMA-2003 campaign with Aerosol Mass Spectrometry: results from the CENICA Supersite, Atmos. Chem. Phys., 6, 925–946, 2006. Sheridan, P. J., Arnott, W. P., Ogren, J. A., Anderson, B. E., Atkinson, D. B., Covert, D. S., Moosmuller, H., Petzold, A., Schmid, B., Strawa, A. W., Varma, R., and Virkkula, A.: The Reno aerosol optics study: An Evaluation of Aerosol Absorption Measurement Methods, Aerosol Sci. Technol., 39, 1–16, 2005. Stone, E. A., Snyder, D. C., Sheesley, R. J., Sullivan, A. P., Weber, R. J., and Schauer, J. J.: Source apportionment of fine organic aerosol in Mexico City during the MILAGRO experiment 2006, Atmos. Chem. Phys., 8, 1249–1259, 2008. Subramanian, R., Roden, C. A., Boparai, P., and Bond, T. C.: Yellow beads and missing particles: Trouble ahead for filter-based absorption measurements., Aerosol Sci. Technol., 41, 630–637, 2007. Sun, H., Biedermann, L., and Bond, T. C.: Color of brown carbon: A model for ultraviolet and visible light absorption by organic carbon aerosol, Geophys. Res. Lett., 34, L17813, doi:10.1029/2007GL029797, 2007. Ulbrich, I. M., Canagaratna, M. R., Zhang, Q., Worsnop, D. R. and Jimenez, J. L.: Interpretation of Organic Components from Positive Matrix Factorization of Aerosol Mass Spectrometric Data, Atmos. Chem. Phys. Discuss., 8, 6729–6791, 2008. Virkkula, A., Mäkelä, T., Hillamo, R., Yli-Tuomi, T., Hirsikko, A., Hämeri, K., and Koponen, I. K.: A simple procedure for correcting loading effects of aethalometer data, J. Air Waste Manage., 57, 1214–1222, 2007. Volkamer, R., Jimenez, J. L., Martini, F. S., Dzepina, K., Zhang, Q., Salcedo, D., Molina, L. T., Worsnop, D. R., and Molina, M. J.: Secondary organic aerosol formation from anthropogenic air pollution: Rapid and higher than expected, Geophys. Res. Lett., 33, L178111, doi:10.1029/2006GL026899, 2006. Volkamer, R., Martini, F. S., Molina, L. T., Salcedo, D., Jimenez, J. L., and Molina, M. J.: A missing sink for gas-phase glyoxal in Mexico City: Formation of secondary organic aerosol Geophys. Res. Lett., 34, L19807, doi:10.1029/2007GL030752, 2007. Weingartner, E., Saathoff, H., Schnaiter, M., Streit, N., Bitnar, B., and Baltensperger, U.: Absorption of light by soot particles: determination of the absorption coefficient by means of aethalometers, J. Aerosol Sci., 34, 1445–1463, 2003. Yokelson, R. J., Urbanski, S. P., Atlas, E. L., Toohey, D. W., Alvarado, E. C., Crounse, J. D., Wennberg, P. O., Fisher, M. E., Wold, C. E., Campos, T. L., Adachi, K., Buseck, P. R., and Hao, W. M.: Emissions from Forest Fires near Mexico City, Atmos. Chem. Phys., 7, 5569–5584, 2007. Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H., Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L., Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch, T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J., Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and Dominance of Oxygenated Species in Organic Aerosols in Anthropogenically–-Influenced Northern Hemisphere Mid-latitudes, Geophys. Res. Lett., 34, L13801, doi:10.1029/2007GL029979, 2007. Zhang, Q., Worsnop, D. R., Canagaratna, M. R., and Jimenez, J. L.: Hydrocarbon-like and oxygenated organic aerosols in Pittsburgh: Insights into sources and processes of organic aerosols, Atmos. Chem. Phys., 5, 3289–3311, 2005.