Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 9 1 2009 10.5194/acpd-9-1621-2009 http://www.atmos-chem-phys-discuss.net/9/1621/2009/ http://www.atmos-chem-phys-discuss.net/9/1621/2009/acpd-9-1621-2009.html http://www.atmos-chem-phys-discuss.net/9/1621/2009/acpd-9-1621-2009.pdf 1621 1668 2009-01-16 The time evolution of aerosol size distribution over the Mexico City plateau L. I. Kleinman kleinman@bnl.gov S. R. Springston J. Wang P. H. Daum Y.-N. Lee L. J. Nunnermacker G. I. Senum J. Weinstein-Lloyd M. L. Alexander J. Hubbe J. Ortega R. A. Zaveri M. R. Canagaratna J. Jayne BJ. Brookhaven National Laboratory, Upton, New York, USA SUNY, Old Westbury, NY, USA Pacific Northwest National Laboratory, Richland, WA, USA Aerodyne Research Inc., Billerica, MA, USA As part of the MILAGRO field campaign, the DOE G-1 aircraft was used to make measurements over and downwind of Mexico City with the objective of determining growth characteristics of aerosols from a megacity urban source. This study focuses on number concentration and size distributions. It is found that a 5-fold increase in aerosol volume is accompanied by about a 5-fold increase in accumulation mode number concentration. There is growth in aerosol volume because there are more accumulation mode particles, not because particles are larger. Condensation and volume growth laws were examined to see whether either is consistent with observations. Condensation calculations show that the growth of Aitken mode particles into the accumulation mode size range gives the required increase in number concentration. There are minimal changes in the accumulation mode size distribution with age, consistent with observations. Volume-growth in contrast yields a population of large particles, distinctly different from what is observed. Detailed model calculations are required to translate our observations into specific information on the volatility and properties of secondary organic aerosol. Albrecht, B.: Aerosols, cloud microphysics, and fractional cloudiness, Science, 245, 1227–1230, 1989. Bowman, F. K., Odum, J. R., Seinfeld, J. H., and Pandis, S. N.: Mathematical model for gas-particle partitioning of secondary organic aerosols, Atmos. Environ., 31, 3921–3931, 1997. Brock, C. A., Washenfelder, R. A., Trainer, M., et al.: Particle growth in the plumes of coal-fired power plants, J. Geophys. Res., 107, 4155, doi:10.1029/2001JD001062, 2002. Brock, C. A., Sullivan, A. P., Peltier, R. E., et al.: Sources of particulate matter in the northeastern United States in summer: 2. Evolution of chemical and microphysical properties, J. Geophys. Res., 113, D08302, doi:10.1029/2007JD009241, 2008. Camredon, M., Aumont, B., Lee-Taylor, J., and Madronich, S.: The SOA/VOC/NOx system: an explicit model of secondary organic aerosol formation, Atmos. Chem. Phys., 7, 5599–5610, 2007. DeCarlo, P. F., Dunlea, E. J., Kimmel, J. R., et al.: Fast airborne aerosol size and chemistry measurements above Mexico City and Central Mexico during the MILAGRO campaign, Atmos. Chem. Phys., 8, 4027–4048, 2008. de Foy, B., Varela, J. R., Molina, 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. Doran, J. C., Barnard, J. C., Arnott, W. P., et al.: The T1-T2 study: evolution of aerosol properties downwind of Mexico City, Atmos. Chem. Phys., 7, 1585–1598, 2007. Drewnick , F., Hings, S. S., DeCarlo, P., Jayne, J. T., Gonin, M., Fuhrer, K., Weimer, S., Jimenez, J. L., Demerjian, K. L., Borrmann, S., and Worsnop, D. R.: A new time-of-flight Aerosol Mass Spectrometer (TOF-AMS) - Instrument Description and first field deployment, Aerosol Sci. and Tech., 39, 637–658, 2005. Fast, J. D. and Zhong, S.: Meteorological factors associated with inhomogeneous ozone concentrations within the Mexico City basin, J. Geophys. Res., 103(D15), 18927–18946, 1998. Ferrare, R., Hostetler, C., Hair, J., Cook, A., Harper, D., Burton, S., Clayton, M., Clarke, A., Russell, P., and Redemann, J.: Airborne High Spectral Resolution Lidar Aerosol Measurements During MILAGRO and TEXAQS/GoMACCS, Ninth Conference on Atmospheric Chemistry, 2007 Annual AMS Conference, San Antonio, TX, USA, January 2007. Greishop, A. P., Donahue, N. M., and Robinson, A. L.: Is the gas-phase partitioning in alpha-pinene secondary organic aerosol reversible? Geophys. Res. Lett., 34, L14810, doi:10.1029/2007GL029987, 2007. Griffin, R. J., Dabdub, D., and Seinfeld, J. H.: Secondary organic aerosol 1. Atmospheric chemical mechanism for production of molecular constituents, J. Geophys. Res., 107, 4332 doi:10.1029/2001JD000541, 2002. Hennigan, C. J., Sullivan, A. P., Fountoukis, C. I., Nenes, A., Hecobian, A., Vargas, I., Peltier, R. E., Case Hanks, A. T., Huey, L. G., Lefer, B. L., Russell, A. G., and Weber, R. J.: On the volatility and production mechanisms of newly formed nitrate and water soluble organic aerosol in Mexico City, Atmos. Chem. Phys., 8, 3761–3768, 2008. Herndon, S. C., Onasch, T. B., Wood, E. C., et al.: The correlation of secondary organic aerosol with odd oxygen in Mexico City, Geophys. Res. Lett., 35, L15804, doi:10.1029/2008GL034058, 2008. Kalberer, M., Paulson, D., Sax, M., Steinbacher, M., Dommen, J., Prevot, A. S. H., Fisseha, R., Weingartner, E., Frankevich, V., Zenobi, R., and Baltensperger, U.: Identification of polymers as major components of atmospheric organic aerosols, Science, 303, 1659–1662, 2004. Kleinman, L. I., Daum, P. H., Lee, Y.-N., Senum, G. I., Springston, S. R., Wang, J., Berkowitz, C., Hubbe, J., Zaveri, R. A., Brechtel, F. J., Jayne, J., Onasch, T. B., and Worsnop, D.: Aircraft observations of aerosol composition and ageing in New England and Mid-Atlantic States during the summer 2002 New England Air Quality Study field campaign, J. Geophys. Res., 112, D09310, doi:10.1029/2006JD007786, 2007. Kleinman, L. I., Springston, S. R., Daum, P. H., Lee, Y.-N., Nunnermacker, L. J., Senum, G. I., Wang, J., Weinstein-Lloyd, J., Alexander, M. L., Hubbe, J., Ortega, J., Canagaratna, M. R., and Jayne, J.: The time evolution of aerosol composition over the Mexico City plateau, Atmos. Chem. Phys., 8, 1559–1575, 2008. Kroll, J. H., Chan, A. W. H., Ng, N. L., Flagan, R. C., and Seinfeld, J. H.: Reactions of semivolatile organics and their effects on secondary organic aerosol formation, Environ. Sci. Technol., 41, 3545–3550, 2007. Kroll, J. H. and Seinfeld, J. H.: Chemistry of secondary organic aerosol: Formation and evolution of low-volatility organics in the atmosphere, Atmos. Environ., 42, 3593–3624 , 2008. Liu, P. S. K., Deng, R., Smith, K. A., Williams, L. R., Jayne, J. T., Canagaratna, M. R., Moore, K., Onasch, T. B., Worsnop, D. R., and Deshler, T. : Transmission efficiency of an aerodynamic focusing lens system: Comparison of model calculations and laboratory measurements for the aerodyne aerosol Mass Spectrometer, Aerosol Sci. Technol., 41, 721–733, 2007. Maria, S. F., Russell, L. M., Gilles, M. K., and Myneni, S. C. B.: Organic aerosol growth mechanisms and their climate-forcing implications, Science, 306, 1921–1924, 2004. Marcolli, C., Luo, B. P., Peter, T., and Wienhold, F. G.: Internal mixing of the organic aerosol by gas phase diffusion of semivolatile organic compounds, Atmos. Chem. Phys., 4, 2593–2599, 2004. McMurry, P. H., Rader, D. J., and Stith, J. L.: Studies of aerosol formation in power plant plumes – I. Growth laws for secondary aerosols in power plant plumes: Implications for chemical conversion mechanisms, Atmos. Environ., 15, 2315–2327, 1981. Miyakawa, T., Takegawa, N., and Kondo, Y.: Photochemical evolution of submicron aerosol chemical composition in the Tokyo megacity region in summer, J. Geophys. Res., 113, D14304, doi:10.1029/2007JD009493, 2008. Molina, L. T., Madronich, S., Gaffney, J. S., and Singh, H. B.: Overview of MILAGRO/INTEX-B campaign, in IGACtivities Newsletter of the International Global Atmospheric Chemistry Project, 38, 2–15 April 2008. Nunnermacker, L. J., Weinstein-Lloyd, B. J., Hillery, B., Giebel, B., Kleinman, L. I., Springston, S. R., Daum, P. H., Gaffney, J., Marley, N., and Huey, G.: Aircraft and ground-based measurements of hydroperoxides during the 2006 MILAGRO field campaign, Atmos. Chem. Phys., 8, 7619–7636, 2008. Odum, J. R., Hoffmann, T., Bowman, F., Collins, D., and Seinfeld, J. H.: Gas/particle partitioning and secondary organic aerosol yields, Environ. Sci. Technol., 30, 2580–2585, 1996. Pankow, J. F.: An absorption model of gas/particle partitioning of organic compounds in the atmosphere, Atmos. Environ., 28, 185–188, 1994. Pankow, J. F.: Gas/particle partitioning of neutral and ionizing compounds to single and multi-phase particles. 1. United modeling framework, Atmos. Environ., 37, 3323–3333, 2003. Press, W. H., Flannery, B. P., Teukolsky, S. A., and Vetterling, W. T.: Numerical Recipes, The Art of Scientific Computing, Cambridge University Press, p 507, 1986. Robinson, A. L., Donahue, N. M., Shrivastava, M. K., Weitkamp, E. A., Sage, A. M., Greishop, A. P., Lane, T. E., Pierce, J. R., and Pandis, S. N.: Rethinking organic aerosol: Semivolatile emissions and photochemical aging, Science, 315, 1259–1262, 2007. Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics, From Air Pollution to Climate Change, ISBN~0-471-17816-0, John Wiley & Sons, NY, USA, 1998. Schwartz, S. E.: The whitehouse effect - Shortwave radiate forcing of climate by anthropogenic aerosol: An overview, J. Aerosol. Sci., 27, 359–382, 1996. Song C., Zaveri, R. A., Alexander, M. L., Thornton, J. A., Madronich, S., Ortega, J. V., Zelenyuk, A., Yu, X.-Y., Laskin, A., and Maughan, D.: Effect of hydrophobic primary organic aerosol on secondary organic aerosol formation from ozonolysis of a-pinene, Geophys. Res. Lett., 34, L20803, doi:10.1029/2007GL030720, 2007.. Twomey, S. A.: Pollution and the planetary albedo, Atmos. Environ., 8, 1251–1256, 1974. Volkamer, R., Jimenez, J. L., San Martini, F., 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, L17811, doi:10.1029/2006GL026899, 2006. Wang, J.: Aerosol size distribution and CCN spectrum observed at T0 site during MILAGRO, DOE Atmospheric Science Program meeting, Boulder, CO, USA, 25–27 October, 2006. Wang, J., Collins, D., Covert, D., Elleman, R., Ferrare, R. A., Gasparini, R., Jonsson, H., Ogren, J., Sheridan, P., and Tsay, S.-C.: Temporal variation of aerosol properties at a rural continental site and study of aerosol evolution through growth law analysis, J. Geophys. Res., 111, D18203, doi:10.1029/2005JD006704, 2006. Wexler, A. S. and Seinfeld, J. H.: The distribution of ammonium salts among a size and composition dispersed aerosol, Atmos. Environ., 24A, 1231–1246, 1990. Zaveri, R. A., Zaveri, R., Alexander, L., Ortega, J., et al.: Evolution of Trace Gases and Aerosols in the Mexico City Pollution Outflow during a Long Range Transport Event, Proceedings of the 27th Annual Conference of the American Association for Aerosol Research, Orlando, FL, USA, 20–24 October 2008. Zaveri, R. A., Easter, R. C., Fast, J. D., and Peters, L. K.: Model for Simulating Aerosol Interactions and Chemistry (MOSAIC), J. Geophys. Res., 113, D13204, doi:10.1029/2007JD008782, 2008. Zhang, Q., Worsnop, D. R., Canagaratna, M. R., and Jimenex, 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. Zhang, Y., Seigneur, C., Seinfeld, J. H., Jacobson, M., Clegg, S. L., and Binkowski, F. S.: A comparative review of inorganic aerosol thermodynamic equilibrium modules: Similarities, differences, and their likely causes, Atmos. Environ., 34, 117–137, 2000. Zhang, Y., Pun, B., Vijayaraghavan, K., Wu, S.-Y., Seigneur, C., Pandis, S. N., Jacobson, M. Z., Nenes, A., and Seinfeld, J. H.: Development and application of the Model of Aerosol Dynamics, Reaction, ionization, and Dissolution (MADRID), J. Geophys. Res., 109, D01202, doi:10.1029/2003JD003501, 2004.