Abstract
In this study bulk airborne aerosol composition measured by the PILS-IC (integration time of 3 min 24 s) during TRACE-P P3B Flight 10 are used to investigate the ionic chemical composition and mixing state of biomass burning particles. A biomass burning plume, roughly 3–4 days old, moderately influenced by urban pollution aerosols recorded in the Philippine Sea is investigated. Focusing on the fine particle NO3−, SO42−, K+, NH4+, and water-soluble organics, the observed correlations and nearly 1-to-1 molar ratios between K+ and NO3− and between NH4+ and (SO42−+ inferred Organics) suggest the presence of fine-mode KNO3, (NH4)2SO4, and NH4(Organics) aerosols. Under the assumption that these ion pairs existed, and because KNO3 is thermodynamically less favored than K2SO4 in a mixture of NO3−, SO42−, K+, NH4+, and Organic anions, the measurements suggest that aerosols could be composed of biomass burning particles (KNO3) mixed to a large degree externally with the (NH4)2SO4 aerosols. A “closed-mode” thermodynamic aerosol simulation predicts that a degree of external mixing (by SO42− mass) of 60 to 100% is necessary to achieve the observed ionic associations in terms of the existence of KNO3. However, the degree of external mixing is most likely larger than 90%, based on both the presence of KNO3 and the amounts of NH4NO3. Calculations are also shown that the aerosol mixing state significantly impacts particle growth by water condensation/evaporation. In the case of P3B Flight #10, the internal mixture is generally more hygroscopic than the external mixture. This method for estimating particle mixing state from bulk aerosol data is less definitive than single particle analysis, but because the data are quantitative, it may provide a complementary method to single particle chemical analysis.
Article PDF
Similar content being viewed by others
Explore related subjects
Discover the latest articles, news and stories from top researchers in related subjects.Avoid common mistakes on your manuscript.
References
Adams, P. J., Seinfeld, J. H., and Koch, D. M., 1999: Global concentrations of tropospheric sulfate, nitrate, and ammonium aerosol simulated in a general circulation model, J. Geophys. Res. 104(D11), 13791–13823.
Allan, J. D., Alfarra, M. R., Bower, K. N., Williams, P. I., Gallagher, M. W., Jimenez, J. L., McDonald, A. G., Nemitz, E., Canagaratna, M. R., Jayne, J. T., Coe, H., and Worsnop, D. R., 2003: Quantitative sampling using an Aerodyne aerosol mass spectrometer – 2. Measurements of fine particulate chemical composition in two U.K. cities, J. Geophys. Res. 108(D3), 4091.
Andreae, M. O., 1983: Soot carbon and excess fine potassium: Long-range transport of combustion-derived aerosols, Science 220, 1148–1151.
Andreae, M. O., 1988: Biomass-burning emissions and associated haze layers over Amazonia, J. Geophys. Res. 93, 1509.
Andreae, M. O. and Merlet, P., 2001: Emission of trace gases and aerosols from biomass burning, Global Biogeochem. Cycles 15, 955–966.
Bassett, M. E. and Seinfeld, J. H., 1983: Atmospheric equilibrium model of sulfate and nitrate aerosols, Atmos. Env. 17, 2237–2252.
Clarke, A.D., Shinozuka, Y., Kapustin, V. N., Howell, S., Huebert, B., Masonis, S., Anderson, T., Covert, D., Weber, R., Anderson, J., Zin, H., Moore II, K. G., and McNaughton, C., 2004: Size-distributions and mixtures of black carbon and dust aerosol in Asian outflow: Physico-chemistry, optical properties, and implications for CCN (in preparation).
Cooke, W. F. and Wilson, J. J. N., 1996: A global black carbon aerosol model, J. Geophys. Res. 101, 19395–19409.
Covert, D. S. and Heintzenberg, J., 1984: Measurement of the degree of internal/external mixing of hygroscopic compounds and soot in atmospheric aerosol, Sci. Total Environ. 36, 347– 352.
Day, D. E., Malm, W. C., and Kreidenweis, S. M., 2000: Aerosol light scattering measurements as a function of relative humidity, J. Air Water Manage. Assoc., 710–716.
Eldering, A. and Cass, G. R., 1996: Source-oriented model for air pollutant effects on visibility, J. Geophys. Res. 101, 19343–19369.
Fuchs N. A. and Sutugin, A. G., 1970: Highly Dispersed Aerosol, Ann Arbor Science, Ann Arbor, MI.
Gao S., Hegg, D. A., Hobbs, P. V., Kirchstetter, T. W., Magi, B. I., and Sadilek, M., 2003: Watersoluble organic components in aerosols associated with savanna fires in southern Africa: Identification, evolution, and distribution, J. Geophys. Res. 108(D13), 8491, doi:10.1029/002002JD002324.
Guazzotti, S. A., Coffee, K. R., and Prather, K. A., 2001: Continuous measurements of size-resolved particle chemistry during INDOEX – Intensive Field Phase 99, J. Geophys. Res. 106(D22), 28607–28627.
Haywood, J. M., Roberts, D. L., Slingo, A., Edwards, J. M., and Shine, K. P., 1997: General circulation model calculations of the direct radiative forcing by anthropogenic sulfate and fossil-fuel soot aerosol, J. Climate 10, 1562–1577.
Hinds, W. C., 1982: Aerosol Technology: Properties, Behavior, and Measurement of Airborne Particles, Wiley, New York.
Huebert, B. J., Howell, S. G., Covert, D., Bertram, T., Clarke, A. C., Anderson, J. R., Lafleur, B. G., Seebaugh, R., Wilson, J. C., Gesler, D., Blomquist, B., and Fox, J. PELTI: Measuring the passing efficiency of an airborne low turbulence aerosol inlet. Aerosol Sci. Technol. (in review).
Jacob, D. J., Crawford, J., Kleb, M. M., Conners, V. S., Bendura, R. J., Raper, J. L., Sachse, G. W., Gille, J., Emmons, L., and Herald, J. C., 2003: Transport and chemical evolution over the Pacific (TRACE-P) mission: Design, execution, and first results, J. Geophys. Res. 108(D20), 8781, doi:10.10291/2002JD003276.
Jacobson, M. Z., Tabazadeh, A., and Turco, R. P., 1996: Simulating equilibrium with aerosols and non-equilibrium between gases and aerosols, J. Geophys. Res. 101, 9079–9091.
Janicke, R., 1993: Aerosols–Clouds–Climate interactions, in P. V. Hobbs (ed.), Tropospheric Aerosols, Academic Press, San Diego, CA, pp. 1–31.
Kaufman, Y. J. and Fraser, R. S., 1997: The effect of smoke particles on clouds and climate forcing, Science 277, 1636–1639.
Kim, Y. P. and Seinfeld, J. H., 1993a: Atmospheric gas-aerosol equilibrium I. Thermodynamic model, Aerosol Sci. Technol. 19, 157–181.
Kim, Y. P. and Seinfeld, J. H., 1993b: Atmospheric gas-aerosol equilibrium II. Thermodynamic model, Aerosol Sci. Technol. 19, 182–198.
Kleeman, M. J., Cass, G. R., and Eldering, A., 1997: Modeling the airborne particle complex as a source-oriented external mixture, J. Geophys. Res. 102, 21355–21372.
Korhnon, P., Kulmala, M., Laaksonen, A., Viisanen, Y., McGraw, R., and Seinfeld, J. H., 1999: Ternary nucleation of H2SO4, NH3, and H2O in the atmosphere, J. Geophys. Res. 104, 26349– 26353.
Li, J., Posfai, M., Hobbs, P. V., and Buseck, P., 2003: Individual aerosol particles from biomass burning in southern Africa: 2. Compositions and aging of inorganic particles, J. Geophys. Res. 108(D13),~8484, doi:10.1029/002002JD002310.
Ma, Y., Rodney, R. J., Lee, Y.-N., Thornton, D. C., Bandy, A. R., Clarke, A. D., Blake, D. R., Sachse, G. W., Fuelberg, H. E., Kiley, C. M., Woo, J.-H., Streets, D. G., Carmichael, G. R., and Eisele, F. L., 2003: The characteristics and influence of biosmoke on fine particle ionic composition measured in Asian outflow during TRACE-P, J. Geophys. Res. 108, 8816, doi:10.1029/2002JD003128.
Malm, W. C., Day, D. E., and Kreidenweis, S. M., 2000a: Light scattering characteristics of aerosols as a function of relative humidity: Part I – A comparison of measured scattering and aerosol concentrations using the theoretical models, J. Air Water Manage. Assoc. 686–700.
Malm, W. C., Day, D. E., and Kreidenweis, S. M., 2000b: Light scattering characteristics of aerosols as a function of relative humidity: Part II – A comparison of measured scattering and aerosol concentrations using the statistical models, J. Air Water Manage. Assoc. 701–709.
Meng, Z., Seinfeld, J. H., Saxena, P., and Kim, Y. P., 1995: Atmospheric gas-aerosol equilibrium IV. Thermodynamics of carbonates, Aerosol Sci. Technol. 23, 131–154.
Meng, Z., Dabdub, D., and Seinfeld, J. H., 1998: Size-resolved and chemically resolved model of atmospheric aerosol dynamics, J. Geophys. Res. 103, 3419–3435.
Meszaros, A. and Meszaros, E., 1989: Sulfate formation on elemental carbon particles, Aerosol Sci. Technol. 10, 337–342.
Murphy, D. M., Thomas, D. S., and Mahoney, T. M. J. 1998: In situ measurements of organics, meteoritic material, mercury, and other elements in aerosols at 5 to 19 kilometers, Science 282, 1664–1669.
Napari, I., Kulmala, M., and Vehkamaki, H., 2002: Ternary nucleation of inorganic acids, ammonia, and water, J. Chem. Phys. 117, 8418–8425.
Neuman J. A., Nowak, J. B., Brock, C. A., Trainer, M., Fehsenfeld, F. C., Holloway, J. S., Hübler, G., Hudson, P. K., Murphy, D. M., Nicks Jr., D. K., Orsini, D., Parrish, D. D., Ryerson, T. B., Sueper, D. T., Sullivan, A., and Weber, R., 2003: Variability in ammonium nitrate formation and nitric acid depletion with altitude and location over California, J. Geophys. Res. Atmos. 108(D17), 4557, doi:10.1029/2003JD003616.
Novakov, T., Chang, S. G., and Harker, A. B., 1974: Sulfates as pollution particles: Catalytic formation on carbon (soot) particles, Science 186, 259–261.
Orsini, D., Ma, Y., Sullivan, A., Sierau, B., Baumann, K., and Weber, R., 2003: Refinements to the particle-into-liquid sampler (PILS) for ground and airborne measurements of water soluble aerosol composition, Atmos. Enviorn 37, 1243–1259.
Parungo, F., Nagomoto, C., Zhou, M., Hansen, A. D., and Harris, J., 1994: Aeolian transport of aerosol black carbon from China to ocean, Atmos. Enviorn 28, 3251–3260.
Parungo, F. C., et~al., 1996: Asian Dust Storms and Their Effects on Radiation and Climate, Technical Report 2959, STC, National Oceanic and Atmospheric Administration, Silver Springs, MD.
Penner, J. E., Dickinson, R. E., and O’Neil, C. A., 1992: Effects of aerosol from biomass burning on the global radiation budget, Science 256, 1432–1434.
Posfai, M., Simonics, R., Li, J., Hobbs, P. V., and Buseck, P. R., 2003: Individual aerosol particles from biomass burning in southern Africa: 1. Compositions and size distributions of carbonaceous particles, J. Geophys. Res. 108(D13), 8483, doi:10.1029/002002JD002291.
Seinfeld, J. H. and Pandis, S. N., 1998: Atmospheric Chemistry and Physics, Wiley, New York, pp. 537–539.
Sinha, P., Hobbs, P. V., Yokelson, R. J., Bertschi, I. T., Blake, D. R., Simpson, I. J., Gao, S., Kirchstetter, T. W., and Novakov, T., 2003: Emissions of trace gases and particles from savanna fires in southern Africa, J. Geophys. Res. 108(D13), 8487, doi:10.1029/2002JD002325.
Stokes, R. H. and Robinson, R. A., 1966: Interactions in aqueous nonelectrolyte solutions. I. Solute–solvent equilibria, J. Phys. Chem. 70, 2126–2130.
Tabazadeh, A., Jacobson, M. Z., Singh, H. B., Toon, O. B., Lin, J. S., Chatfield, R. B., Thakur, A. N., Talbot, R. W., and Dibb, J. E., 1998: Nitric acid scavenging by mineral and biomass burning aerosols, Geophys. Res. Lett. 25, 4185–4188.
Talbot, R. W., Andreae, M. O., Andreae, T. W., and Harris, R. C., 1988: Regional aerosol chemistry of the Amazon basin during the dry season, J. Geophys. Res. 93, 1499.
Talbot, R. W., Dibb, J. E., and Loomis, M. B., 1998: Influence of vertical transport on free tropospheric aerosols over the central USA in springtime, Geophys. Res. Lett. 25, 1367– 1370.
Tang, I. N., 1996: Chemical and size effects of hygroscopic aerosols on light scattering coefficients, J. Geophys. Res. 101, 19245–19250.
Tang, I. N., 1997: Thermodynamic and optical properties of mixed-salt aerosols of atmospheric importance, J. Geophys. Res. 102, 1883–1893.
Weber, R. J., McMurry, P. H., Mauldin, L., Tanner, D. J., Eisele, F. L., Brechtel, F. J., Kreidenweis, S. M., Kok, G. L., Schillawski, R. D., and Baumgarden, D., 1998: A study of new particle formation and growth involving biogenic and trace gas species measured during ACE1, J. Geophys. Res. 103, 16385–16396.
Weber, R. J., Orsini, D., Daun, Y., Lee, Y.-N., Klotz, P., and Brechtel, F., 2001: A particle-into-liquid collector for rapid measurements of aerosol chemical composition, Aerosol Sci. Technol. 35, 718–727.
Wexler, A. S., Lurmann, F. W., and Seinfeld, J. H., 1994: Modeling urban and regional aerosols – I. Model development, Atmos. Env. 28, 531–546.
Yamasoe, M. A., Artaxo, P., Miguel, A. H., and Allen, A. G., 2000: Chemical composition of aerosol particles from direct emissions of vegetation fires in the Amazon Basin: Watersoluble species and trace elements, Atmos. Env. 34, 1641–1653.
Zhang, D., Zhang, J., Shi, G., Iwasaka, Y., Matsuki, A., and Trochkine, D., 2003: Mixture state of individual Asian dust particles at a coastal site of Qingdao, China, Atmos. Enviorn 37, 3895–3901.
Zhang, X. Q., McMurry, P. H., Hering, S. V., and Casuccio, G. S., 1993: Mixing characteristics and water content of submicron aerosols measured in Los Angeles and at the Grand Canyon, Atmos. Enviorn 27A, 1593–1607.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Song, C.H., Ma, Y., Orsini, D. et al. An Investigation into the Ionic Chemical Composition and Mixing State of Biomass Burning Particles Recorded During TRACE-P P3B Flight#10. J Atmos Chem 51, 43–64 (2005). https://doi.org/10.1007/s10874-005-5727-9
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1007/s10874-005-5727-9