Atmospheric Chemistry and Physics Discussions
www.atmos-chem-phys-discuss.net
1680-7367
1680-7375
9
2
2009
10.5194/acpd-9-6657-2009
http://www.atmos-chem-phys-discuss.net/9/6657/2009/
http://www.atmos-chem-phys-discuss.net/9/6657/2009/acpd-9-6657-2009.html
http://www.atmos-chem-phys-discuss.net/9/6657/2009/acpd-9-6657-2009.pdf
6657
6690
2009-03-10
Regional differences in organic composition of submicron and single particles during INTEX-B 2006
D. A. Day
S. Takahama
S. G. Gilardoni
L. M. Russell
lmrussell@ucsd.edu
Scripps Inst. of Oceanography, University of California, San Diego, La Jolla, California, USA
now at: European Commission, Institute for Environment and Sustainability, Ispra (VA), Italy
Organic functional group and elemental concentrations were measured with
Fourier transform infrared (FTIR) spectroscopy and X-ray fluorescence (XRF)
from an aircraft platform as part of the Intercontinental Chemical Transport
Experiment – Phase B (INTEX-B) conducted over the Eastern Pacific and
Western North America. Single particle spectra were obtained using scanning
transmission X-ray microscopy-near edge X-ray absorption fine structure
spectrometry (STXM-NEXAFS). Organic mass (OM) concentrations ranged from 1 to
7 μg m<sup>−3</sup> and averaged 2.4–4.1 μg m<sup>−3</sup>. Alkane functional
groups were the largest fraction of OM, averaging 1.9–2.1 μg m<sup>−3</sup> or
50–76% of OM. Alcohol functional groups comprised the second largest
fraction of OM (0.35–0.39 μg m<sup>−3</sup>, 9–14%). Organic and elemental
concentrations are compared within and among geographical air mass regions:
"Pacific" free troposphere, "Continental" free troposphere, "Seattle"
metropolitan region, and the California "Central Valley". OM concentrations
were highest and most variable in the Central Valley (3.5±2 μg m<sup>−3</sup>).
Alcohol functional group concentrations were highest in the
Continental and Central Valley and lowest in the Pacific and Seattle air
masses. Oxygen-to-carbon ratios were relatively constant in the Central
Valley but variable for the Continental air masses. Most elemental
concentrations did not show large variations among or within air mass
categories. Overall, the OM concentrations showed greater variability within
air mass categories as compared to averages among them, suggesting sampled
air mass regions included a variety of sources, processing, and losses of
organic aerosol. Single particle spectra obtained by STXM-NEXAFS were
classified into metaclasses associated with different sources and atmospheric
processing. Particles with spectra indicative of secondary organic aerosol
production and combustion sources were found at several locations and a range
of altitudes. At lower altitudes, particles with spectra resembling soil dust
and biomass burning fingerprints were commonly observed. Single particle
spectra provided evidence that condensation and surface-limited oxidation
contributed to particle growth.
Ade, H. and Urquhart, S. G.: NEXAFS spectroscopy and microscopy of natural and synthetic polymers, in: Chemical Applications of Synchrotron Radiation, edited by: Sham, T. K. E., World Scientific Publishing, Singapore, 285–355, 2002.
Aiken, A. C., Decarlo, P. F., Kroll, J. H., Worsnop, D. R., Huffman, J. A., Docherty, K. S., Ulbrich, I. M., Mohr, C., Kimmel, J. R., Sueper, D., Sun, Y., Zhang, Q., Trimborn, A., Northway, M., Ziemann, P. J., Canagaratna, M. R., Onasch, T. B., Alfarra, M. 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, doi:10.1021/es703009q, 2008.
Alfarra, M. R., Coe, H., Allan, J. D., Bower, K. N., Boudries, H., Canagaratna, M. R., Jimenez, J. L., Jayne, J. T., Garforth, A. A., Li, S. M., and Worsnop, D. R.: Characterization of urban and rural organic particulate in the lower Fraser valley using two aerodyne aerosol mass spectrometers, Atmos. Environ., 38, 5745–5758, doi:10.1016/j.atmosenv.2004.01.054, 2004.
Bahadur, R., Gazala, H., and Russell, L. M.: Climatology of PM$_2.5$ organic carbon concentrations from a review of ground-based atmospheric measurements by evolved gas analysis, Atmos. Environ., 43, 1591–1602, 2009.
Braun, A.: Carbon speciation in airborne particulate matter with C (1s) NEXAFS spectroscopy, J. Environ. Monitor., 7, 1059–1065, doi:10.1039/b508910g, 2005.
Chung, S. H. and Seinfeld, J. H.: Global distribution and climate forcing of carbonaceous aerosols, J. Geophys. Res., 107, 4407, doi:10.1029/2001JD001397, 2002.
Clarke, A. D., Howell, S., Quinn, P. K., Bates, T. S., Ogren, J. A., Andrews, E., Jefferson, A., Massling, A., Mayol-Bracero, O., Maring, H., Savoie, D., and Cass, G.: INDOEX aerosol: A comparison and summary of chemical, microphysical, and optical properties observed from land, ship, and aircraft, J. Geophys. Res., 107, 8033, doi:803310.1029/2001JD000572, 2002.
Dibb, J. E., Talbot, R. W., Scheuer, E. M., Blake, D. R., Blake, N. J., Gregory, G. L., Sachse, G. W., and Thornton, D. C.: Aerosol chemical composition and distribution during the Pacific Exploratory Mission (PEM) Tropics, J. Geophys. Res., 104, 5785–5800, 1999.
Dunlea, E. J., DeCarlo, P. F., Aiken, A. C., Kimmel, J. R., Peltier, R. E., Weber, R. J., Tomlison, J., Collins, D. R., Shinozuka, Y., McNaughton, C. S., Howell, S. G., Clarke, A. D., Emmons, L. K., Apel, E. C., Pfister, G. G., van Donkelaar, A., Martin, R. V., Millet, D. B., Heald, C. L., and Jimenez, J. L.: Evolution of Asian aerosols during transpacific transport in INTEX-B, Atmos. Chem. Phys. Discuss., 8, 15375–15461, 2008.
Gilardoni, S., Russell, L. M., Sorooshian, A., Flagan, R. C., Seinfeld, J. H., Bates, T. S., Quinn, P. K., Allan, J. D., Williams, B., Goldstein, A. H., Onasch, T. B., and Worsnop, D. R.: Regional variation of organic functional groups in aerosol particles on four US east coast platforms during the International Consortium for Atmospheric Research on Transport and Transformation 2004 campaign, J. Geophys. Res., 112, D10S27, doi:10.1029/2006JD007737, 2007.
Gilardoni, S., Shang, L., Takahama, S., Russell, L. M., Allan, J. D., Steinbrecher, R., Jimenez, J. L., Decarlo, P. F., Dunlea, E. J., and Baumgardner, D.: Characterization of organic ambient aerosol during MIRAGE 2006 on three platforms, Atmos. Chem. Phys. Discuss., 9, 6617–6655, 2009.
Heald, C. L., Jacob, D. J., Park, R. J., Russell, L. M., Huebert, B. J., Seinfeld, J. H., Liao, H., and Weber, R. J.: A large organic aerosol source in the free troposphere missing from current models, Geophys. Res. Lett., 32, L18809, doi:10.1029/2005GL023831, 2005.
Johnson, K. S., de Foy, B., Zuberi, B., Molina, L. T., Molina, M. J., Xie, Y., Laskin, A., and Shutthanandan, V.: Aerosol composition and source apportionment in the Mexico City Metropolitan Area with PIXE/PESA/STIM and multivariate analysis, Atmos. Chem. Phys., 6, 4591–4600, 2006.
Johnson, K. S., Laskin, A., Jimenez, J. L., Shutthanandan, V., Molina, L. T., Salcedo, D., Dzepina, K., and Molina, M. J.: Comparative analysis of urban atmospheric aerosol by particle-induced X-ray emission (PIXE), proton elastic scattering analysis (PESA), and aerosol mass spectrometry (AMS), Environ. Sci. Technol., 42, 6619–6624, doi:10.1021/es800393e, 2008.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, 2005.
Leaitch, W. R., Macdonald, A. M., Anlauf, K. G., Liu, P. S. K., Toom-Sauntry, D., Li, S.-M., Liggio, J., Hayden, K., Wasey, M. A., Russell, L. M., Takahama, S., Liu, S., van Donkelaar, A., Duck, T., Martin, R. V., Zhang, Q., Sun, Y., McKendry, I., Shantz, N. C., and Cubison, M.: Evidence for Asian dust effects from aerosol plume measurements during INTEX-B 2006 near Whistler, BC, Atmos. Chem. Phys. Discuss., 8, 18531–18589, 2008.
Lewis, A. C., Carslaw, N., Marriott, P. J., Kinghorn, R. M., Morrison, P., Lee, A. L., Bartle, K. D., and Pilling, M. J.: A larger pool of ozone-forming carbon compounds in urban atmospheres, Nature, 405, 778–781, 2000.
Liu, S., Takahama, S., Russell, L. M., Gilardoni, S., and Baumgardner, D.: Oxygenated organic functional groups and their sources in single and submicron organic particles in MILAGRO 2006 campaign, Atmos. Chem. Phys. Discuss., 9, 4567–4607, 2009.
Malm, W. C., Sisler, J. F., Huffman, D., Eldred, R. A., and Cahill, T. A.: Spatial and seasonal trends in particle concentration and optical extinction in the United States, J. Geophys. Res., 99, 1347–1370, 1994.
Maria, S. F., Russell, L. M., Turpin, B. J., and Porcja, R. J.: FTIR measurements of functional groups and organic mass in aerosol samples over the Caribbean, Atmos. Environ., 36, 5185–5196, 2002.
Maria, S. F., Russell, L. M., Turpin, B. J., Porcja, R. J., Campos, T. L., Weber, R. J., and Huebert, B. J.: Source signatures of carbon monoxide and organic functional groups in Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) submicron aerosol types, J. Geophys. Res., 108, 8637, doi:10.1029/2003JD003703, 2003.
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, doi:10.1126/science.1103491, 2004.
McKendry, I. G., Macdonald, A. M., Leaitch, W. R., van Donkelaar, A., Zhang, Q., Duck, T., and Martin, R. V.: Trans-Pacific dust events observed at Whistler, British Columbia during INTEX-B, Atmos. Chem. Phys., 8, 6297–6307, 2008.
Middlebrook, A. M., Murphy, D. M., and Thomson, D. S.: Observations of organic material in individual marine particles at Cape Grim during the First Aerosol Characterization Experiment (ACE 1), J. Geophys. Res., 103, 16475–16483, 1998.
Miranda, J., Andrade, E., Lopez-Suarez, A., Ledesma, R., Cahill, T. A., and Wakabayashi, P. H.: A receptor model for atmospheric aerosols from a southwestern site in Mexico City, Atmos. Environ., 30, 3471–3479, 1996.
Novakov, T., Hegg, D. A., and Hobbs, P. V.: Airborne measurements of carbonaceous aerosols on the East Coast of the United States, J. Geophys. Res., 102, 30023–30030, 1997.
Peltier, R. E., Hecobian, A. H., Weber, R. J., Stohl, A., Atlas, E. L., Riemer, D. D., Blake, D. R., Apel, E., Campos, T., and Karl, T.: Investigating the sources and atmospheric processing of fine particles from Asia and the Northwestern United States measured during INTEX B, Atmos. Chem. Phys., 8, 1835–1853, 2008.
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., 109, D19S01, doi:10.1029/2003JD004010, 2004.
Russell, L. M., Maria, S. F., and Myneni, S. C. B.: Mapping organic coatings on atmospheric particles, Geophys. Res. Lett., 29, 1779, doi:10.1029/2002GL014874, 2002.
Russell, L. M., Takahama, S., Liu, S., Hawkins, L. N., Covert, D. S., Quinn, P. K., and Bates, T. S.: Oxygenated fraction and mass of organic aerosol from direct emission and atmospheric processing collected on the R/V Ronald Brown during TEXAQS/GoMACCS 2006, J. Geophys. Res.-A, in press, online available at: http://www.agu.org/contents/journals/ViewPapersInPress.do?journalCode=JD#id2008JD011275, 2009.
Singh, H. B., Brune, W. H., Crawford, J. H., Flocke, F., and Jacob, D. J.: Chemistry and transport of pollution over the Gulf of Mexico and the Pacific: Spring 2006 INTEX-B Campaign overview and first results, Atmos. Chem. Phys. Discuss., 9, 363–409, 2009.
Spracklen, D. V., Bonn, B., and Carslaw, K. S.: Boreal forests, aerosols and the impacts on clouds and climate, Philos. Tr. R. Soc. S.-A, 366, 4613–4626, doi:10.1098/rsta.2008.0201, 2008.
Takahama, S., Gilardoni, S., Russell, L. M., and Kilcoyne, A. L. D.: Classification of multiple types of organic carbon composition in atmospheric particles by scanning transmission X-ray microscopy analysis, Atmos. Environ., 41, 9435–9451, doi:10.1016/j.atmosenv.2007.08.051, 2007.
Tsigaridis, K. and Kanakidou, M.: Global modelling of secondary organic aerosol in the troposphere: a sensitivity analysis, Atmos. Chem. Phys., 3, 1849–1869, 2003.
Tsigaridis, K., Lathiére, J., Kanakidou, M., and Hauglustaine, D. A.: Naturally driven variability in the global secondary organic aerosol over a decade, Atmos. Chem. Phys., 5, 1891–1904, 2005.
Turpin, B. J. and Lim, H. J.: Species contributions to PM$_2.5$ mass concentrations: Revisiting common assumptions for estimating organic mass, Aerosol Sci. Technol., 35, 602–610, 2001.
Zhang, Q., Canagaratna, M. R., Jayne, J. T., Worsnop, D. R. and Jimenez, J. L.: Time- and size-resolved chemical composition of submicron particles in Pittsburgh: Implications for aerosol sources and processes, J. Geophys. Res., 110, D07S09, doi:10.1029/2004JD004649, 2005.
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 midlatitudes, Geophys. Res. Lett., 34, L13801, doi:10.1029/2007GL029979, 2007.