Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 10 3 2010 10.5194/acpd-10-6641-2010 http://www.atmos-chem-phys-discuss.net/10/6641/2010/ http://www.atmos-chem-phys-discuss.net/10/6641/2010/acpd-10-6641-2010.html http://www.atmos-chem-phys-discuss.net/10/6641/2010/acpd-10-6641-2010.pdf 6641 6679 2010-03-10 The Finokalia Aerosol Measurement Experiment – 2008 (FAME-08): an overview M. Pikridas A. Bougiatioti L. Hildebrandt G. J. Engelhart E. Kostenidou C. Mohr A. S. H. Prevot G. Kouvarakis P. Zarmpas J. F. Burkhart B.-H. Lee M. Psichoudaki N. Mihalopoulos C. Pilinis A. Stohl U. Baltensperger M. Kulmala S. N. Pandis spyros@andrew.cmu.edu Department of Chemical Engineering, University of Patras, Greece Institute of Chemical Engineering and High Temperatures (ICE-HT), FORTH, Patras, Greece Department of Chemistry, University of Crete, Greece Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, USA Paul Scherrer Institut, Laboratory of Atmospheric Chemistry, Villigen, Switzerland Norwegian Institute for Air Research, Kjeller, Norway Department of Environment, University of the Aegean, Mytilene, Greece Department of Physics, University of Helsinki, Helsinki, Finland A month (4 May to 8 June 2008) of ambient aerosol, air ion and gas phase sampling (Finokalia Aerosol Measurement Experiment 2008, FAME-08) was conducted at Finokalia, on the island of Crete, Greece. The purpose of the study was to characterize the physical and chemical properties of aged aerosol and to investigate new particle formation. Measurements included aerosol and air ion size distributions, size-resolved chemical composition, organic aerosol thermal volatility, water uptake and particle optical properties (light scattering and absorption). Statistical analysis of the aerosol mass concentration variations revealed the absence of diurnal patterns suggesting the lack of strong local sources. Sulfates accounted for approximately half of the particulate matter less than 1 micrometer in diameter (PM₁) and organics for 26%. The PM₁ organic aerosol fraction was highly oxidized with 80% water soluble. The supermicrometer particles were dominated by crustal components (50%), sea salt (24%) and nitrates (16%). The organic carbon to elemental carbon (OC/EC) ratio correlated with ozone measurements but with a one-day lag. The average OC/EC ratio for the study period was equal to 5.4. For three days air masses from North Africa resulted in a 6-fold increase of particulate matter less than 10 micrometers in diameter (PM₁₀) and a decrease of the OC/EC ratio by a factor of 2. Back trajectory analysis, based on FLEXPART footprint plots, identified five source regions (Athens, Greece, Africa, other continental and marine), each of which influenced the PM₁ aerosol composition and properties. Marine air masses had the lowest PM₁ concentrations and air masses from the Balkans, Turkey and Eastern Europe the highest. Albrecht, B. A.: Aerosols, cloud microphysics, and fractional cloudiness, Science, 245, 1227–1230, 1989 An, W. J., Pathak, R. K., Lee, B. H., and Pandis, S. N.: Aerosol volatility measurement using an improved thermodenuder: Application to secondary organic aerosol, J. Aerosol Sci., 38, 305–314, 2007. Bartzis,~J. G., Andronopoulos, S., Kulmala, M., Larsen, B., Lazaridis, M.,~Lohse, C., Mirabel, P. and~Pilinis,~C.: The BOND Project: The Marseille and Athens Experimental Campaign. An Overview, J. of Aerosol Sci. (European~Aerosol~Conference~Budapest,~Hungary~6–10~September~2004),~p 1167, 2004. Cabada, J. C., Pandis, S. N., Subramanian, R., Robinson, A. L., Polidori, A., and Turpin, B.: Estimating the secondary organic aerosol contribution to PM$_2.5$ using the EC tracer method, Aerosol Sci. Technol., 38(S1),140–155, 2004. Cruz, C. N. and Pandis, S. N.: Deliquescence and hygroscopic growth of mixed inorganic-organic atmospheric aerosol, Environ. Sci. Technol., 34, 4313–4319, 2000. Dick, W. D., Saxena, P., and McMurry, P. H.: Estimation of water uptake by organic compounds in submicron aerosols measured during the Southeastern Aerosol and Visibility Study, J. Geophys. Res., 105, 1471–1479, 2000. Eleftheriadis, K., Colbeck, I., Housiadas, C., Lazaridis, M., Mihalopoulos, N., Mitsakou, C., Smolik, J., and Zdimal, V.: Size distribution, composition and origin of the submicron aerosol in the marine boundary layer during the eastern Mediterranean "SUB-AERO" experiment, Atmos. Environ., 40, 6245–6260, 2006. Gerasopoulos, E., Kouvarakis, G., Babasakalis, P., Vrekoussis, M., Putaud, J. P., and Mihalopoulos, N.: Origin and variability of particulate matter (PM$_10$) mass concentrations over the Eastern Mediterranean, Atmos. Environ., 40, 4679–4690, 2006. Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prevot, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, 2009. Hildebrandt, L., Engelhart, G. J., Mohr, C., Kostenidou, E., Lanz, V. A., Bougiatioti, A., DeCarlo, P. F., Prévôt, A. S. H., Baltensperger, U., Mihalopoulos, N., Donahue, N. M., and Pandis, S. N.: Aged organic aerosol in the Eastern Mediterranean: The Finokalia Aerosol Measurement Experiment-2008, Atmos. Chem. Phys. Discuss., 10, 1847–1900, 2010. Jayne, J. T., Leard, D. C., Zhang, X., Davidovits, P., Smith, K. A., Kolb, C. E., and Worsnop, D. R.: Development of an aerosol mass spectrometer for size and composition analysis of submicron particles, Aerosol Sci. Technol., 33, 49–70, 2000. Jimenez, J. L., Jayne, J. T., Shi, Q., Kolb, C. E., Worsnop, D. R., Yourshaw, I., Seinfeld, J. H., Flagan, R. C., Zhang, X., Smith, K. A., Morris, J., and Davidovits, P.: Ambient aerosol sampling using the Aerodyne Aerosol Mass Spectrometer, J. Geophys. Res., 108 (D7), 8425, doi:10.1029/2001JD001213, 2003. Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang, Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken, A. C., Docherty, K. D., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L., Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y. L., Tian, J., Laaksonen, A. T. R., Rautiainen, J., Vaattovaara, P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J., Dunlea, E. J., Huffman, J. A., Onasch, T. B., Alfarra, M. R., Williams, P. I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M., Williams, L. R., Wood, E. C., Kolb, C. E., Baltensperger, U., and Worsnop, D. R.: Evolution of organic aerosol in the atmosphere, Science, 326, 1525–1529, 2009. Kalivitis, N., Gerasopoulos, E., Vrekoussis, M., Kouvarakis, G., Kubilay, N., Hatzianastassiou, N., Vardavas, I., and Mihalopoulos, N.: Dust transport over the eastern Mediterranean derived from Total Ozone Mapping Spectrometer, Aerosol Robotic Network, and surface measurements. J. Geophys. Res., 112, D03202, doi:10.1029/2006JD007510, 2007. Kalivitis, N., Birmili, W., Stock, M., Wehner, B., Massling, A, Wiedensohler, A., Gerasopoulos, E., and Mihalopoulos, N.: Particle size distributions in the Eastern Mediterranean troposphere, Atmos. Chem. Phys., 8, 6729–6738, 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. Kavouras, I. G. and Stephanou, E. G.: Particle size distribution of organic primary and secondary aerosol constituents in urban, background marine, and forest atmosphere, J. Geophys. Res., 107(D8), 4069, doi:10.1029/2000JD000278, 2002. Khlystov, A., Wyers, G. P., and Slanina, J.: The steam-jet aerosol collector, Atmos. Environ., 29, 2229–2234, 1995. Khlystov, A., Stanier, C. O., Takahama, S., and Pandis, S. N.: Water content of ambient aerosol during the Pittsburgh Air Quality Study, J. Geophys. Res., 110, D07S10, doi:10.1029/2004JD004651, 2005. Kostenidou, E., Pathank, R. K., and Pandis, S. N.: An algorithm for the calculation of secondary organic aerosol density combining AMS and SMPS data, Aerosol Sci. Technol., 41, 1002–1010, 2007 Koulouri, E., Saarikoski, S., Theodosi, C., Markaki, Z., Gerasopoulos, E., Kouvarakis, G., Makela, T., Hillamo, R., and Mihalopoulos, N.: Chemical composition and sources of fine and coarse aerosol particles in the Eastern Mediterranean, Atmos. Environ., 42, 6542–6550, 2008. Kouvarakis, G., Tsigaridis, K., Kanakidou, M., and Mihalopoulos, N.: Temporal variations of surface regional background ozone over Crete Island in the Southeast Mediterranean, J. Geophys. Res., 105, 399–407, 2000. Kouvarakis, G., Doukelis, Y., Mihalopoulos, N., Rapsomanikis, S., Sciare, J., and Blumthaler, M.: Chemical, physical, and optical characterization of aerosols during PAUR II experiment, J. Geophys. Res., 107, 8141, doi:10.1029/2000JD000291, 2002. Kulmala, M., Vehkamäki, H., Petäjä, T., Dal Maso, M., Lauri, A., Kerminen, V. M., Birmili, W., and McMurry, P. H.: Formation and growth rates of ultrafine atmospheric particles: a review of observations, J. Aerosol Sci., 35, 143–176. 2004. Kulmala, M. and Kerminen, V. M.: On the formation and growth of atmospheric nanoparticles, Atmos. Res., 90, 132–150, 2008. Kulmala, M., Asmi, A., Lappalainen, H. K., Carslaw, K. S., Pöschl, U., Baltensperger, U., Hov, Ø., Brenquier, J.-L., Pandis, S. N., Facchini, M. C., Hansson, H.-C., Wiedensohler, A., and O'Dowd, C. D.: Introduction: European Integrated Project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) - integrating aerosol research from nano to global scales, Atmos. Chem. Phys., 9, 2825–2841, 2009. Lazaridis, M., Dzumbova, L., Kopanakis, I., Ondracek, J., Glytsos, T., Aleksandropoulou, V., Voulgarakis, A., Katsivela, E., Mihalopoulos, N., and Eleftheriadis, K.: PM$_10$ and PM$_2.5$ levels in the Eastern Mediterranean (Akrotiri Research Station, Crete, Greece), Water Air Soil Pollut., 189, 85–101, 2008. Lee, B. H., Kostenidou, E., Hildebrandt, L., Riipinen, I., Engelhart, G. J., Mihalopoulos, N., Prevot, A. S. H., Baltensperger, U., and Pandis, S. N.: Measurement of the ambient organic aerosol volatility distribution: Application during the Finokalia Aerosol Measurement Experiment (FAME-2008), Atmos. Chem. Phys., in preparation, 2010. Lim, H. and Turpin, B. J.: Origins of primary and secondary organic aerosol in Atlanta: Results of time-resolved measurements during the Atlanta Supersite Experiment. Environ. Sci. Technol., 36, 4489–4496, 2002. Lohmann U. and Feichter J.: Global indirect aerosol effects: a review, Atmos. Chem. Phys., 5, 715–737, 2005. Loo, B. W. and Cork, C. P.: Development of a high efficiency virtual impactor, Aerosol Sci. Technol., 9, 167–176, 1988. 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. Meyer, N. K., Duplissy, J., Gysel, M., Metzger, A., Dommen, J., Weingartner, E., Alfarra, M. R., Prevot, A. S. H., Fletcher, C., Good, N., McFiggans, G., Jonsson, A. M., Hallquist, M., Baltensperger, U., and Ristovski, Z. D.: Analysis of the hygroscopic and volatile properties of ammonium sulphate seeded and unseeded SOA particles, Atmos. Chem. Phys., 9, 721–732, 2009. Mihalopoulos, N., Stephanou, E., Kanakidou, M., Pilitsidis, S., and Bousquet, P.: Tropospheric aerosol ionic composition above the Eastern Mediterranean Area, Tellus B, 314–326, 1997. Mirme,~A., Tamm,~E., Mordas,~G., Vana,~M., Uin,~J., Mirme,~S., Bernotas,~T., Laakso,~L., Hirsikko,~A., and Kulmala,~M.: A wide-range multi-channel Air Ion Spectrometer, Boreal Environ. Res., 12, 247–264, 2007. Moulin, C., Lambert, C. E., Dayan, U., Masson, V., Ramonet, M., Bousquet, P., Legrand, M., Balkanski, Y. J., Guelle, W., Marticorena, B., Bergametti, G., and Dulac, F.: Satellite climatology of African dust transport in the Mediterranean atmosphere, J. Geophys. Res., 103, 13137–13144, 1998. Pope, C. A., Ezzati, M., and Dockery, D. W.: Fine-particulate air pollution and life expectancy in the United States, New Engl. J. Med. 360, 376–386, 2009. Pope, C. A.: Respiratory hospital admission associated with PM$_10$ pollution in Utah, Salt Lake and Cache Valleys, Arch Environ. Health, 7, 46–90, 1991. Robinson, A. L., Donahue, N. M., Shrivastava, M. K., Weitkamp, E. A., Sage, A. M., Grieshop, A. P., Lane, T. E., Pierce, J. R., and Pandis, S. N.: Rethinking organic aerosols: Semivolatile emissions and photochemical aging, Science, 315, 1259–1262, 2007. Saarikoski, S., Timonen, H., Saarnio, K., Aurela, M., Järvi, L., Keronen, P., Kerminen V. M., and Hillamo, R.: Sources of organic carbon in fine particulate matter in northern European urban air, Atmos. Chem. Phys. 8, 6281–6295, 2008. Sciare, J., Bardouki, H., Moulin, C., and Mihalopoulos, N.: Aerosol sources and their contribution to the chemical composition of aerosols in the Eastern Mediterranean Sea during summertime, Atmos. Chem. Phys., 3, 291–302, 2003a. Sciare, J., Cachier, H., Oikonomou, K., Ausset, P., Sarda-Esteve, R., and Mihalopoulos, N.: Characterization of carbonaceous aerosols during the MINOS campaign in Crete, July–August 2001: a multi-analytical approach, Atmos. Chem. Phys., 3, 1743–1757, 2003b. Sciare, J., Oikonomou, K., Cachier, H., Mihalopoulos, N., Andreae, M., O., Maenhaut, W., and Estève, R., S.: Aerosol mass closure and reconstruction of the light scattering coefficient over the Eastern Mediterranean Sea during the MINOS campaign, Atmos. Chem. Phys., 5, 2253–2265, 2005. Sciare, J., Oikonomou, K., Favez, O., Liakakou, E., Markaki, Z., Cachier, H., and Mihalopoulos, N.: Long-term measurements of carbonaceous aerosols in the Eastern Mediterranean: evidence of long-range transport of biomass burning, Atmos. Chem. Phys., 8, 5551–5563, 2008. Seibert, P. and Frank, A.: Source-receptor matrix calculation with a Lagrangian particle dispersion model in backward mode, Atmos. Chem. Phys., 4, 51–63, 2004. Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: from Air Pollution to Climate Change, John Wiley, New York, USA, 381–384, 1998. Schneider, J., Borrmann, S., Wollny, A. G., Blasner, M., Mihalopoulos, N., Oikonomou, K., Sciare, J., Teller, A., Levin, Z., and Worsnop, D. R.: Online mass spectrometric aerosol measurements during the MINOS campaign (Crete, August 2001), Atmos. Chem. Phys., 4, 65–80, 2004. Stanier, C. O., Khlystov, A., and Pandis, S. N.: Nucleation events during the Pittsburgh Air Quality Study: Description and relation to key meteorological, gas-phase, and aerosol parameters. Aerosol Sci. Technol, 38(S1), 253–264, 2004a. Stanier, C. O., Khlystov, A., Chan, R., Mandiro, M., and Pandis, S. N.: A method for the in-situ measurement of fine aerosol water content of ambient aerosols: the Dry-Ambient Aerosol Size Spectrometer (DAASS), Aerosol Sci. Technol., 38, Supplement 1, 215–228, 2004b. Stohl, A., Forster, V., Frank, A., Seibert, P., and Wotawa, G.: Technical Note : The Lagrangian particle dispersion model FLEXPART version 6.2, Atmos. Chem. Phys., 5, 2461–2474, 2005. Schwartz, J., Dockery, D. W., and Neas L., M.: Is daily mortality associated specifically with fine particles?, J. Air Waste Manag. Assoc., 46, 927–939, 1996. Turpin, B. J. and Lim, H. J.: Species contributions to PM2.5 mass concentrations: revisiting common assumptions for estimating organic mass, Aerosol Sci. Technol., 35, 602–610, 2001. Twomey, S.: The influence of pollution on the shortwave cloud albedo of clouds, J. Atmos. Sci., 34, 1149–1154, 1977. Wang, Z., Hopke, P. K., Ahmadi, G., Cheng, Y. S., and Baron, P. A.: Fibrous particle deposition in human nasal passage: The influence of particle length, flow rate, and geometry of nasal airway, J. Aerosol Sci., 39, 1040–1054, 2008. Wheater C. P. and Cook, P. A.: Using Statistics to Understand the Environment, Routledge, New York, USA, 124–137, 2000.