References

ACP

Atmospheric Chemistry and Physics

ACP

Atmos. Chem. Phys.

1680-7324

Copernicus Publications

Göttingen, Germany

10.5194/acp-13-11595-2013

Chemical composition and hygroscopic properties of aerosol particles over the Aegean Sea

Bezantakos

¹ ² Barmpounis

³ Giamarelou

¹ Bossioli

⁴ Tombrou

⁴ Mihalopoulos

⁵ Eleftheriadis

https://orcid.org/0000-0003-2265-4905

² Kalogiros

⁶ D. Allan

https://orcid.org/0000-0001-6492-4876

⁷ Bacak

⁷ Percival

C. J.

⁷ Coe

⁷ Biskos

¹ ³

Department of Environment, University of the Aegean, Mytilene 81100, Greece

ERL, Inst. of Nuclear Technology & Radiation Protection, NCSR Demokritos, 15310 Ag. Paraskevi, Attiki, Greece

Faculty of Applied Sciences, Delft University of Technology, Delft 2628-BL, the Netherlands

Department of Physics, National and Kapodistrian University of Athens, Athens 15784, Greece

Department of Chemistry, University of Crete, Heraklion 71003, Greece

Institute of Environmental Research and Sustainable Development, National Observatory of Athens, Athens, Greece

School of Earth, Atmospheric and Environmental Science, The University of Manchester, Manchester, UK

29 11 2013

13 22 11595 11608

2013

This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/

This article is available from https://acp.copernicus.org/articles/13/11595/2013/acp-13-11595-2013.html

The full text article is available as a PDF file from https://acp.copernicus.org/articles/13/11595/2013/acp-13-11595-2013.pdf

The chemical composition and water uptake characteristics of sub-micrometre atmospheric particles over the region of the Aegean Sea were measured between 25 August and 11 September 2011 within the framework of the Aegean-Game campaign. High temporal-resolution measurements of the chemical composition of the particles were conducted using an airborne compact time-of-flight aerosol mass spectrometer (cToF-AMS). These measurements were performed during two flights from the island of Crete to the island of Lemnos and back. A hygroscopic tandem differential mobility analyser (HTDMA) located on the island of Lemnos was used to measure the ability of the particles to take up water. The HTDMA measurements showed that the particles in the dominant mode were internally mixed, having hygroscopic growth factors that ranged from 1.00 to 1.59 when exposed to 85% relative humidity. When the aircraft flew near the ground station on Lemnos, the cToF-AMS measurements showed that the organic volume fraction of the particles ranged from 43 to 56%. These measurements corroborate the range of hygroscopic growth factors measured by the HTDMA during that time. Good closure between HTDMA and cToF-AMS measurements was achieved when assuming that the organic species were less hygroscopic and had an average density that corresponds to aged organic species. Using the results from the closure study, the cToF-AMS measurements were employed to determine vertical profiles of a representative aerosol hygroscopic parameter κmix. Calculated κmix values ranged from 0.19 to 0.84 during the first flight and from 0.22 to 0.80 during the second flight. Air masses of different origin as determined by back trajectory calculations can explain the spatial variation in chemical composition and κmix values of the particles observed in the region.

References 1

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., Prévôt, 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, 2008.

Allan, J. D., Jimenez, J. L., Williams, P. I., Alfarra, M. R., Bower, K. N., Jayne, J. T., Coe, H., and Worsnop, D. R.: Quantitative sampling using an aerodyne aerosol mass spectrometer – 1. Techniques of data interpretation and error analysis, J. Geophys. Res.-Atmos., 108, 4090, <a href="http://dx.doi.org/10.1029/2002JD002358">https://doi.org/10.1029/2002JD002358</a>, 2003.

Allan, J. D., Coe, H., Bower, K. N., Alfarra, M. R., Delia, A. E., Jimenez, J. L., Middlebrook, A. M., Drewnick, F., Onasch, T. B., Canagaratna, M. R., Jayne, J. T., and Worsnop, D. R.: A generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data, J. Aerosol Sci., 35, 909–922, 2004.

Biskos, G., Paulsen, D., Russell, L. M., Buseck, P. R., and Martin, S. T.: Prompt deliquescence and efflorescence of aerosol nanoparticles, Atmos. Chem. Phys., 6, 4633–4642, <a href="http://dx.doi.org/10.5194/acp-6-4633-2006">https://doi.org/10.5194/acp-6-4633-2006</a>, 2006a.

Biskos, G., Russel, L. M., Buseck, P. R., and Martin, S. T.: Nanosize effect on the hygroscopic growth factor of aerosol particles, Geoph. Res. Lett., 33, L07801, <a href="http://dx.doi.org/10.1029/2005GL025199">https://doi.org/10.1029/2005GL025199</a>, 2006b.

Biskos, G., Buseck, P. R., and Martin, S. T.: Hygroscopic growth of nucleation-mode acidic sulfate particles, J. Aerosol Sci., 40, 338–347, 2009.

Canagaratna, M. R., Jayne, J. T., Jimenez, J. L., Allan, J. D., Alfarra, M. R., Zhang, Q., Onasch, T. B., Drewnick, F., Coe, H., Middlebrook, A., Delia, A., Williams, L. R., Trimborn, A. M., Northway, M. J., DeCarlo, P. F., Kolb, C. E., Davidovits, P., and Worsnop, D. R.: Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer, Mass Spectrom. Rev., 26, 185–222, 2007.

Clarisse, L., Clerbaux, C., Dentener, F., Hurtmans, D., and Coheur, P.-F.: Global ammonia distribution derived from infrared satellite observations, Nature Geosci., 2, 479–483, 2009.

Clegg, S. L., Brimblecombe, P., and Wexler, A. S.: Thermodynamic model of the system \chemH^+-\chemNH_4^+-\chemSO_4^{2-}-NO3-H2O at tropospheric temperatures, J. Phys. Chem. A, 102, 2137–2154, 1998.

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. Tech., 39, 637-658, 2005.

Duplissy, J., DeCarlo, P. F., Dommen, J., Alfarra, M. R., Metzger, A., Barmpadimos, I., Prevot, A. S. H., Weingartner, E., Tritscher, T., Gysel, M., Aiken, A. C., Jimenez, J. L., Canagaratna, M. R., Worsnop, D. R., Collins, D. R., Tomlinson, J., and Baltensperger, U.: Relating hygroscopicity and composition of organic aerosol particulate matter, Atmos. Chem. Phys., 11, 1155–1165, <a href="http://dx.doi.org/10.5194/acp-11-1155-2011">https://doi.org/10.5194/acp-11-1155-2011</a>, 2011.

Engelhart, G. J., Hildebrandt, L., Kostenidou, E., Mihalopoulos, N., Donahue, N. M., and Pandis, S. N.: Water content of aged aerosol, Atmos. Chem. Phys., 11, 911–920, <a href="http://dx.doi.org/10.5194/acp-11-911-2011">https://doi.org/10.5194/acp-11-911-2011</a>, 2011.

Foltescu, V. L., Selin, E., and Below, M.: Corrections for particle losses and sizing errors during aircraft aerosol sampling using a rosemount inlet and the pms las-x, Atmos. Environ., 29, 449–453, 1995.

Gysel, M., Crosier, J., Topping, D. O., Whitehead, J. D., Bower, K. N., Cubison, M. J., Williams, P. I., Flynn, M. J., McFiggans, G. B., and Coe, H.: Closure study between chemical composition and hygroscopic growth of aerosol particles during TORCH2, Atmos. Chem. Phys., 7, 6131–6144, <a href="http://dx.doi.org/10.5194/acp-7-6131-2007">https://doi.org/10.5194/acp-7-6131-2007</a>, 2007.

Gysel, M. McFiggans, G.B. Coe, H.: Inversion of tandem differential mobility analyser (TDMA) measurements, J. Aerosol Sci., 40, 134-151, 2009.

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. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, 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, <a href="http://dx.doi.org/10.5194/acp-9-5155-2009">https://doi.org/10.5194/acp-9-5155-2009</a>, 2009.

Haywood, J. and Boucher, O.: Estimates of the direct and indirect radiative forcing due to tropospheric aerosols: a review, Rev. Geophys., 38, 513–543, 2000.

Heintzenberg J.: Fine particles in the global troposphere – A review, Tellus B, 41, 149–160, 1989.

Hussein, T., Maso, M. D., Petäjä, T., Koponen I. S., and Paatero, P.: Evaluation of an automatic algorithm for fitting the particle number size distributions, Boreal Environ. Res., 10, 337–355, 2005.

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, <a href="http://dx.doi.org/10.5194/acp-8-6729-2008">https://doi.org/10.5194/acp-8-6729-2008</a>, 2008.

Koulouri, E., Saarikoski, S., Theodosi, C., Markaki, Z., Gerasopoulos, E., Kouvarakis, G., Mäkelä, 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.

Knutson, E. O. and Whitby, K. T.: Aerosol classification by electric mobility: apparatus, theory, and applications, J. Aerosol Sci., 6, 443–451, 1975.

Kreidenweis, S. M., Petters, M. D., and DeMott, P. J.: Single parameter estimates of aerosol water content, Environ. Res. Lett., 3, 035002, <a href="http://dx.doi.org/10.1088/1748-9326/3/3/035002">https://doi.org/10.1088/1748-9326/3/3/035002</a>, 2008.

Lelieveld, J., Berresheim, H., Borrmann, S., Crutzen, P. J., Dentener, F. J., Fisher, H., Feichter, J., Flatau, P. J., Heland, J., Holzinger, R., Korrmann, R., Lawrence, M. G., Levin, Z., Markowitz, K. M., Mihalopoulos, N., Minikin, A., Ramanathan, V., de Reus, M., Roelofs, G. J., Scheeren, H. A., Sciare, J., Schlager, H., Schultz, M., Siegmund, P., Steil, B., Stephanou, E. G., Stier, P., Traub, M., Warneke, C., Williams, J., and Ziereis, H.: Global air pollution crossroads over the Mediterranean, Science, 298, 794–799, 2002.

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. Tech., 41, 721–733, 2007.

Marcolli, C., Luo, B. P. and Peter, T.: Mixing of the organic aerosol fractions: liquids as the thermodynamically stable phases, J. Phys. Chem. A, 108, 2216–2224, 2004.

Middlebrook, A. M., Bahreini, R., Jimenez, J. L., and Canagaratna, M. R.: Evaluation of composition-dependent collection efficiencies for the aerodyne aerosol mass spectrometer using field data, Aerosol Sci. Tech., 46, 258–271, 2012.

Mihalopoulos, N., Stephanou, E., Kanakidou, M., Pilitsidis, S., and Bousquet, P.: Tropospheric aerosol ionic composition above the eastern Mediterranean area, Tellus B 49, 314–326, 1997.

Morgan, W. T., Allan, J. D., Bower, K. N., Highwood, E. J., Liu, D., McMeeking, G. R., Northway, M. J., Williams, P. I., Krejci, R., and Coe, H.: Airborne measurements of the spatial distribution of aerosol chemical composition across Europe and evolution of the organic fraction, Atmos. Chem. Phys., 10, 4065–4083, <a href="http://dx.doi.org/10.5194/acp-10-4065-2010">https://doi.org/10.5194/acp-10-4065-2010</a>, 2010.

Ogren, J. and Charlson, J.: Implications for models and measurements of chemical inhomogenities among cloud droplets, Tellus B, 44, 489–504, 1992.

Park, K., Kim, J. S., and Miller, A. L.: A study on effects of size and structure on hygroscopicity of nanoparticles using a tandem differential mobility analyzer and TEM, J. Nanopart. Res., 11, 175–183, 2009.

Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, <a href="http://dx.doi.org/10.5194/acp-7-1961-2007">https://doi.org/10.5194/acp-7-1961-2007</a>, 2007.

Pikridas, M., Bougiatioti, A., Hildebrandt, L., Engelhart, G. J., Kostenidou, E., Mohr, C., Prévôt, A. S. H., Kouvarakis, G., Zarmpas, P., Burkhart, J. F., Lee, B.-H., Psichoudaki, M., Mihalopoulos, N., Pilinis, C., Stohl, A., Baltensperger, U., Kulmala, M., and Pandis, S. N.: The Finokalia Aerosol Measurement Experiment – 2008 (FAME-08): an overview, Atmos. Chem. Phys., 10, 6793–6806, <a href="http://dx.doi.org/10.5194/acp-10-6793-2010">https://doi.org/10.5194/acp-10-6793-2010</a>, 2010.

Pilinis, C. and Seinfeld, J. H.: Continued development of a general equilibrium model for inorganic multicomponent atmospheric aerosols, Atmos. Environ., 21, 2453–2466, 1987.

Pringle, K. J., Tost, H., Pozzer, A., Pöschl, U., and Lelieveld, J.: Global distribution of the effective aerosol hygroscopicity parameter for CCN activation, Atmos. Chem. Phys., 10, 5241–5255, <a href="http://dx.doi.org/10.5194/acp-10-5241-2010">https://doi.org/10.5194/acp-10-5241-2010</a>, 2010.

Rader, D. J. and McMurry, P. H.: Application of the tandem differential mobility analyzer to studies of droplet growth or evaporation, J. Aerosol Sci., 17, 771–787, 1986.

Salisbury, G., Williams, J., Holzinger, R., Gros, V., Mihalopoulos, N., Vrekoussis, M., Sarda-Estéve, R., Berresheim, H., von Kuhlmann, R., Lawrence, M., and Lelieveld, J.: Ground-based PTR-MS measurements of reactive organic compounds during the MINOS campaign in Crete, July–August 2001, Atmos. Chem. Phys., 3, 925–940, <a href="http://dx.doi.org/10.5194/acp-3-925-2003">https://doi.org/10.5194/acp-3-925-2003</a>, 2003.

Spengler, J. D., Brauer, M., and Koutrakis, P.: Acid air and health, Environ. Sci. Technol., 24, 946–955, 1990.

Stock, M., Cheng, Y. F., Birmili, W., Massling, A., Wehner, B., Müller, T., Leinert, S., Kalivitis, N., Mihalopoulos, N., and Wiedensohler, A.: Hygroscopic properties of atmospheric aerosol particles over the Eastern Mediterranean: implications for regional direct radiative forcing under clean and polluted conditions, Atmos. Chem. Phys., 11, 4251–4271, <a href="http://dx.doi.org/10.5194/acp-11-4251-2011">https://doi.org/10.5194/acp-11-4251-2011</a>, 2011.

Stolzenburg, M. R. and McMurry, P. H.: TDMAFIT user's manual, Particle Technology Laboratory, Department of Mechanical Engineering, Univercity of Minnesota, Minneapolis, 1–61, 1988.

Stolzenburg, M. R. and McMurry, P. H.: An ultrafine aerosol condensation nucleus counter, Aerosol Sci. Technol., 14, 48–65, 1991.

Tombrou, M., Bossioli, E., Kalogiros, J., Allan, J., Bacak, A., Biskos, G., Coe, H.,Dandou, A., Kouvarakis, G., Mihalopoulos, N., Protonotariou, A. P., Szabó-Takács, B., and Triantafillou, E.: Physical and chemical processes of polluted air masses during etesians: Aegean-Game airborne campaign – an outline, in advances in meteorology, climatology and atmospheric physics, Springer Atmospheric Sciences, 1239–1244, Springer-Verlag Berlin Heidelberg, 2012.

Wang, C. S. and Flagan C. R.: Scanning electrical mobility spectrometer, Aerosol Sci. Technol., 13, 230–240, 1990.

Wang, X., Kruis, F. E., and McMurry, P. H.: Aerodynamic focusing of nanoparticles: I. Guidelines for designing aerodynamic lenses for nanoparticles, Aerosol Sci. Tech., 39, 611–623, 2005.

Wex, H., McFiggans, G., Henning, S., and Stratmann, F.: Influence of the external mixing state of atmospheric aerosol on derived CCN number concentrations, Geophys. Res. Lett., 37, L10805, <a href="http://dx.doi.org/10.1029/2010GL043337">https://doi.org/10.1029/2010GL043337</a>, 2010.