References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-9-5433-2009

Organic composition of single and submicron particles in different regions of western North America and the eastern Pacific during INTEX-B 2006

Day

D. A.

¹ Takahama

¹ Gilardoni

¹ ² Russell

L. M.

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

03 08 2009

9 15 5433 5446

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.

This article is available from http://www.atmos-chem-phys.net/9/5433/2009/acp-9-5433-2009.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/9/5433/2009/acp-9-5433-2009.pdf

Single particles were collected 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 spectroscopy (STXM-NEXAFS). Bulk submicron particles were also collected and organic functional group and elemental concentrations were quantified with Fourier transform infrared (FTIR) spectroscopy and X-ray fluorescence (XRF). Single particle spectra 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. The types of particle spectra most commonly observed aloft were similar to those observed during a previous study over the northwestern Pacific, indicating that long-range transport may have been an important particle source. Single particle spectra provided evidence that condensation and surface-limited oxidation contributed to particle growth. Organic mass (OM) concentrations ranged from 1 to 7 μg m−3 and averaged 2.4–4.1 μg m−3. Alkane functional groups were the largest fraction of OM, averaging 1.9–2.1 μg m−3 or 50–76% of OM, followed by alcohol functional groups (0.35–0.39 μg m−3, 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−3). Oxygen-to-carbon ratios were relatively constant in the Central Valley but variable for the Continental air masses. 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 and processing of organic aerosol.

References 1

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., Liu, S., Takahama, S., Russell, L. M., Allan, J. D., Steinbrecher, R., Jimenez, J. L., De Carlo, P. F., Dunlea, E. J., and Baumgardner, D.: Characterization of organic ambient aerosol during MIRAGE 2006 on three platforms, Atmos. Chem. Phys., 9, 5417–5432, 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., 9, 3523–3546, 2009.

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.: Aerosol organic-mass-to-organic- carbon ratio measurements, Environ. Sci. Technol., 37, 2982–2987, doi:10.1021/es026123w, 2003.

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, 114, D00F05, doi:10.1029/2008JD011275, 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., 9, 2301–2318, 2009.

Spracklen, D. V., Bonn, B., and Carslaw, K. S.: Boreal forests, aerosols and the impacts on clouds and climate, Philos. T. Roy. Soc. 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. Tech., 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.