References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-12-4647-2012

Aerosol charging state at an urban site: new analytical approach and implications for ion-induced nucleation

Gagné

¹ ⁵ Leppä

² Petäjä

¹ McGrath

M. J.

¹ ⁶ Vana

¹ ³ Kerminen

V.-M.

² Laakso

¹ ² ⁴ Kulmala

Department of Physics, University of Helsinki, P.O. Box 64, 00014 Helsinki, Finland

Finnish Meteorological Institute, Climate Change, P.O. Box 503, 00101 Helsinki, Finland

Institute of Physics, University of Tartu, Ülikooli 18, 50090 Tartu, Estonia

School of Physical and Chemical Sciences, North-West University, Private Bag x6001, Potchefstroom 2520, South Africa

now at: Dept. of Physics and Atmospheric Science, Dalhousie University, Halifax, B3H 3J5, Canada and at Environment Canada, Toronto, M3H 5T4, Canada

now at: Dept. of Biophysics, Graduate School of Science, Kyoto University, Sakyo Kyoto 606-8502, Japan

25 05 2012

12 10 4647 4666

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/12/4647/2012/acp-12-4647-2012.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/4647/2012/acp-12-4647-2012.pdf

The charging state of aerosol populations was determined using an Ion-DMPS in Helsinki, Finland between December 2008 and February 2010. We extrapolated the charging state and calculated the ion-induced nucleation fraction to be around 1.3 % ± 0.4 % at 2 nm and 1.3 % ± 0.5 % at 1.5 nm, on average. We present a new method to retrieve the average charging state for a new particle formation event, at a given size and polarity. We improve the uncertainty assessment and fitting technique used previously with an Ion-DMPS. We also use a new theoretical framework that allows for different concentrations of small ions for different polarities (polarity asymmetry). We extrapolate the ion-induced fraction using polarity symmetry and asymmetry. Finally, a method to calculate the growth rates from the behaviour of the charging state as a function of the particle diameter using polarity symmetry and asymmetry is presented and used on a selection of new particle formation events.

References 1

Aalto, P P., Hämeri, K., Becker, E., Weber, R., Salm, J., Mäkelä, J M., Hoell, C., O'Dowd, C D., Karlsson, H., Hansson, H.-C., Väkevä, M., Koponen, I K., Buzorius, G., and Kulmala, M.: Physical characterization of aerosol particles during nucleation events, Tellus, 53B, 344–358, 2001.

Ahlm, L., Nilsson, E. D., Krejci, R., Mårtensson, E. M., Vogt, M., and Artaxo, P.: A comparison of dry and wet season aerosol number fluxes over the Amazon rain forest, Atmos. Chem. Phys., 10, 3063–3079, http://dx.doi.org/10.5194/acp-10-3063-2010doi:10.5194/acp-10-3063-2010, 2010.

Curtius, J., Lovejoy, E R., and Froyd, K D.: Atmospheric ion-induced aerosol nucleation, Space Sci. Rev., 125, 159–167, 2006.

Dal Maso, M., Kulmala, M., Riipinen, I., Wagner, R., Hussein, T., Aalto, P P., and Lehtinen, K. E J.: Formation and Growth of Fresh Atmospheric Aerosols: Eight Years of Aerosol Size Distribution Data from SMEAR II, Hyytiälä, Finland, Boreal Environ. Res., 10, 323–336, 2005.

Ehn, M., Junninen, H., Petäjä, T., Kurtén, T., Kerminen, V.-M., Schobesberger, S., Manninen, H. E., Ortega, I. K., Vehkamäki, H., Kulmala, M., and Worsnop, D. R.: Composition and temporal behavior of ambient ions in the boreal forest, Atmos. Chem. Phys., 10, 8513–8530, http://dx.doi.org/10.5194/acp-10-8513-2010doi:10.5194/acp-10-8513-2010, 2010.

Ehn, M., Vuollekoski, H., Petäjä, T., Kerminen, V.-M., Vana, M., Aalto, P P., de~Leeuw, G., Ceburnis, D., Dupuy, R., O’Dowd, C D., and Kulmala, M.: Growth rates during coastal and marine new particle formation in western Ireland, J. Geophys. Res., 115, D18218, http://dx.doi.org/10.1029/2010JD014292doi:10.1029/2010JD014292, 2010b.

Gagné, S., Laakso, L., Petäjä, T., Kerminen, V.-M., and Kulmala, M.: Analysis of one year of Ion-DMPS data from the SMEAR II station, Finland, Tellus, 60B, 318–329, 2008.

Gagné, S., Nieminen, T., Kurtén, T., Manninen, H. E., Petäjä, T., Laakso, L., Kerminen, V.-M., Boy, M., and Kulmala, M.: Factors influencing the contribution of ion-induced nucleation in a boreal forest, Finland, Atmos. Chem. Phys., 10, 3743–3757, http://dx.doi.org/10.5194/acp-10-3743-2010doi:10.5194/acp-10-3743-2010, 2010.

Hõrrak, U., Salm, J., and Tammet, H.: Bursts of intermediate ions in atmospheric air, J. Geophys. Res., 103, D12, 13909–13915, 1998.

Hari, P. and Kulmala, M.: Station for Measuring Ecosystem-Atmosphere Relations (SMEAR II), Boreal Env. Res., 10, 315–322, 2005.

Hirsikko, A., Nieminen, T., Gagné, S., Lehtipalo, K., Manninen, H. E., Ehn, M., Hõrrak, U., Kerminen, V.-M., Laakso, L., McMurry, P. H., Mirme, A., Mirme, S., Petäjä, T., Tammet, H., Vakkari, V., Vana, M., and Kulmala, M.: Atmospheric ions and nucleation: a review of observations, Atmos. Chem. Phys., 11, 767–798, http://dx.doi.org/10.5194/acp-11-767-2011doi:10.5194/acp-11-767-2011, 2011.

%Hõrrak, U., Aalto, P. P., Salm, J., Komsaare, K., Tammet, H., Mäkelä, %J. M., Laakso, L., and Kulmala, M.: Variation and balance of positive air ion %concentrations in a boreal forest, Atmos. Chem. Phys., 8, 655–675, 2008. Hõrrak, U., Aalto, P. P., Salm, J., Komsaare, K., Tammet, H., Mäkelä, J. M., Laakso, L., and Kulmala, M.: Variation and balance of positive air ion concentrations in a boreal forest, Atmos. Chem. Phys., 8, 655–675, http://dx.doi.org/10.5194/acp-8-655-2008doi:10.5194/acp-8-655-2008, 2008.

Hoppel, W. A., and Frick, G. M.: Ion-aerosol attachment coefficients and the steady-state charge distribution on aerosol in a bipolar environment, Aerosol Sci. Technol., 5, 1–21, 1986.

Hussein, T., Martikainen, J., Junninen, H., Sogacheva, L., Wagner, R., Dal~Maso, M., Riipinen, I., Aalto, P P., and Kulmala, M.: Observation of regional new particle formation in the urban atmosphere, Tellus, 60B, 509–521, 2008.

Iida, K., Stolzenburg,~M R., McMurry,~P H., Dunn, M J., Smith, J N., Eisele, F., and Keady, P.: Contribution of ion-induced nucleation to new particle formation: Methodology and its application to atmospheric observations in Boulder, Colorado, J. Geophys. Res., 111, d23201, http://dx.doi.org/10.1029/2006JD007167doi:10.1029/2006JD007167, 2006.

Iida, K., Stolzenburg, M R., McMurry, P H., and Smith, J N.: Estimating nanoparticle growth rates from size-dependent charged fractions: Analysis of new particle formation events in Mexico City, J. Geophys. Res., 113, d05207, http://dx.doi.org/10.1029/2007JD009260doi:10.1029/2007JD009260, 2008.

Järvi, L., Hannuniemi, H., Hussein, T., Junninen, H., Aalto, P P., Hillamo, R., Mäkelä, T., Keronen, P., Siivola, E., Vesala, T., and Kulmala, M.: The urban measurement station SMEAR III: Continuous monitoring of air pollution and surface-atmosphere interactions in Helsinki, Finland, Boreal Environ. Res., 14~(suppl. A), 86–109, d05207, http://dx.doi.org/10.1029/2007JD009260doi:10.1029/2007JD009260, 2009.

Kazil, J., Lovejoy, E. R., Barth, M. C., and O'Brien, K.: Aerosol nucleation over oceans and the role of galactic cosmic rays, Atmos. Chem. Phys., 6, 4905–4924, http://dx.doi.org/10.5194/acp-6-4905-2006doi:10.5194/acp-6-4905-2006, 2006.

Kerminen, V.-M. and Kulmala, M.: Analytical formulae connecting the "real" and the "apparent" nucleation rate and the nuclei number concentration for atmospheric nucleation events, J. Aerosol Sci., 33, 609–622, 2002.

Kerminen, V.-M., Anttila, T., Petäjä, T., Laakso, L., Gagné, S., Lehtinen, K. E J., and Kulmala, M.: Charging state of the atmospheric nucleation mode: Implications for separating neutral and ion-induced nucleation, J. Geophys. Res., 112, d21205, http://dx.doi.org/10.1029/2007JD008649doi:10.1029/2007JD008649, 2007.

Kerminen, V.-M., Petäjä, T., Manninen, H E., Paasonen, P., Nieminen, T., Sipilä, M., Junninen, H., Ehn, M., Gagné, S., Laakso, L., Riipinen, I., Vehkamäki, H., Kurtén, T., Ortega, I., Dal~Maso, M., Brus, D., Hyvärinen, A., Lihavainen, H., Leppä, J., Lehtinen, K. E J., Mirme, A., Mirme, S., Hõrrak, U., Berndt, T., Stratmann, F., Birmili, W., Wiedensohler, A., Metzger, A., Dommen, J., Baltensperger, U., Kiendler-Scharr, A., Mentel, A., Wildt, J., Winkler, P., Wagner, P E., Petzgold, A., Minikin, A., Plass-Dülmer, C., Pöschl, U., Laaksonen, A., and Kulmala, M.: Atmospheric nucleation: highlights of the EUCAARI project and future directions, Atmos. Chem. Phys., 10, 10829–10848, http://dx.doi.org/10.5194/acp-10-10829-2010doi:10.5194/acp-10-10829-2010, 2010.

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., Riipinen, I., Sipilä, M., Manninen, H E., Petäjä, T., Junninen, H., Dal Maso, M., Mordas, G., Mirme, A., Vana, M., Hirsikko, A., Laakso, L., Harrison, R M., Hanson, I., Leung, C., Lehtinen, K. E J., and Kerminen, V.: Toward direct measurement of atmospheric nucleation, Science, 318, 89–92, 2007.

Kulmala, M., Riipinen, I., Nieminen, T., Hulkkonen, M., Sogacheva, L., Manninen, H E., Paasonen, P., Petäjä, T., Dal~Maso, M., Aalto, P P., Viljanen, A., Usoskin, I Vainio, R., Mirme, S., Mirme, A., Minikin, A., Petzold, A., Hõrrak, U., Plass-Dülmer, C., Birmili, W., and Kerminen, V.-M.: Atmospheric data over a solar cycle: no connection between galactic cosmic rays and new particle formation, Atmos. Chem. Phys., 10, 1885–1898, http://dx.doi.org/10.5194/acp-10-1885-2010doi:10.5194/acp-10-1885-2010, 2010.

%Laakso, L., Petäjä, T., Lehtinen, K. E J., Kulmala, M., Paatero, J., % Hõrrak, U., Tammet, H., and Joutsensaari, J.: Ion production rate in a % boreal forest based on ion, particle and radiation measurements, Atmos. Chem. % Phys., 4, 1933–1943, 2004. Laakso, L., Petäjä, T., Lehtinen, K. E. J., Kulmala, M., Paatero, J., Hõrrak, U., Tammet, H., and Joutsensaari, J.: Ion production rate in a boreal forest based on ion, particle and radiation measurements, Atmos. Chem. Phys., 4, 1933–1943, http://dx.doi.org/10.5194/acp-4-1933-2004doi:10.5194/acp-4-1933-2004, 2004.

Laakso, L., Gagné, S., Petäjä, T., Hirsikko, A., Aalto, P. P., Kulmala, M., and Kerminen, V.-M.: Detecting charging state of ultra-fine particles: instrumental development and ambient measurements, Atmos. Chem. Phys., 7, 1333–1345, http://dx.doi.org/10.5194/acp-7-1333-2007doi:10.5194/acp-7-1333-2007, 2007.

Laakso, L., Grönholm, T., Kulmala, L., Haapanala, S., Hirsikko, A., Lovejoy, E R., Kazil, J., Kurtén, T., Boy, M., Nilsson, E D., Sogachev, A., Riipinen, I., Stratmann, F., and Kulmala, M.: Hot-air balloon as a platform for boundary layer profile measurements during particle formation, Boreal Environ. Res., 12, 279–294, 2007b.

Laakso, L., Laakso, H., Aalto, P. P., Keronen, P., Petäjä, T., Nieminen, T., Pohja, T., Siivola, E., Kulmala, M., Kgabi, N., Molefe, M., Mabaso, D., Phalatse, D., Pienaar, K., and Kerminen, V.-M.: Basic characteristics of atmospheric particles, trace gases and meteorology in a relatively clean Southern African Savannah environment, Atmos. Chem. Phys., 8, 4823–4839, http://dx.doi.org/10.5194/acp-8-4823-2008doi:10.5194/acp-8-4823-2008, 2008.

Lohmann, U. and Feichter, J.: Global indirect aerosol effects: a review, Atmos. Chem. Phys., 5, 715–737, http://dx.doi.org/10.5194/acp-5-715-2005doi:10.5194/acp-5-715-2005, 2005.

Lovejoy, E R., Curtius, J., and Froyd, K D.: Atmospheric ion-induced nucleation of sulfuric acid and water, J. Geophys. Res., 109, D08204, http://dx.doi.org/10.1029/2003JD004460doi:10.1029/2003JD004460, 2004.

Mäkelä, J M., Salm, J., Smirnov, V V., Koponen, I., Paatero, J., and Pronin, A A.: Electrical charging state of fine and ultrafine particles in boreal forest air, J. Aerosol Sci., 32, S149–S150, 2003.

Manninen, H. E., Nieminen, T., Riipinen, I., Yli-Juuti, T., Gagné, S., Asmi, E., Aalto, P. P., Petäjä, T., Kerminen, V.-M., and Kulmala, M.: Charged and total particle formation and growth rates during EUCAARI 2007 campaign in Hyytiälä, Atmos. Chem. Phys., 9, 4077–4089, http://dx.doi.org/10.5194/acp-9-4077-2009doi:10.5194/acp-9-4077-2009, 2009.

Manninen, H. E., Nieminen, T., Asmi, E., Gagné, S., Häkkinen, S., Lehtipalo, K., Aalto, P., Vana, M., Mirme, A., Mirme, S., Hõrrak, U., Plass-Dülmer, C., Stange, G., Kiss, G., Hoffer, A., Törö, N., Moerman, M., Henzing, B., de Leeuw, G., Brinkenberg, M., Kouvarakis, G. N., Bougiatioti, A., Mihalopoulos, N., O'Dowd, C., Ceburnis, D., Arneth, A., Svenningsson, B., Swietlicki, E., Tarozzi, L., Decesari, S., Facchini, M. C., Birmili, W., Sonntag, A., Wiedensohler, A., Boulon, J., Sellegri, K., Laj, P., Gysel, M., Bukowiecki, N., Weingartner, E., Wehrle, G., Laaksonen, A., Hamed, A., Joutsensaari, J., Petäjä, T., Kerminen, V.-M., and Kulmala, M.: EUCAARI ion spectrometer measurements at 12 European sites – analysis of new particle formation events, Atmos. Chem. Phys., 10, 7907–7927, http://dx.doi.org/10.5194/acp-10-7907-2010doi:10.5194/acp-10-7907-2010, 2010.

Merikanto, J., Spracklen, D. V., Mann, G. W., Pickering, S. J., and Carslaw, K. S.: Impact of nucleation on global CCN, Atmos. Chem. Phys., 9, 8601–8616, http://dx.doi.org/10.5194/acp-9-8601-2009doi:10.5194/acp-9-8601-2009, 2009.

Myhre, G., Berglen, T. F., Johnsrud, M., Hoyle, C. R., Berntsen, T. K., Christopher, S. A., Fahey, D. W., Isaksen, I. S. A., Jones, T. A., Kahn, R. A., Loeb, N., Quinn, P., Remer, L., Schwarz, J. P., and Yttri, K. E.: Modelled radiative forcing of the direct aerosol effect with multi-observation evaluation, Atmos. Chem. Phys., 9, 1365–1392, http://dx.doi.org/10.5194/acp-9-1365-2009doi:10.5194/acp-9-1365-2009, 2009.

Pierce, J. R. and Adams, P. J.: Uncertainty in global CCN concentrations from uncertain aerosol nucleation and primary emission rates, Atmos. Chem. Phys., 9, 1339–1356, http://dx.doi.org/10.5194/acp-9-1339-2009doi:10.5194/acp-9-1339-2009, 2009.

Spracklen, D V., Carslaw, K S., Kulmala, M., Kerminen, V.-M., Sihto, S.-L., Riipinen, I., Merikanto, J., Mann, G W., Chipperfield, M P., Wiedensohler, A., Birmili, W., and Lihavainen, H.: Contribution of particle formation to global cloud condensation nuclei concentrations, Geophys. Res. Lett., 35, L06, 808–812, 2008.

Stevens, B. and Feingold, G.: Untangling aerosol effects on clouds and precipitation in a buffered system, Nature, 461, 607–613, 2009.

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

Svensmark, H., Pedersen, J O., Marsh, N D., Enghoff, M B., and Uggerhøj, U I.: Experimental evidence for the role of ions in particle nucleation under atmospheric conditions, Proc. R. Soc. A, 463, 385–396, 2007.

Tammet, H.: Continuous scanning of the mobility and size distribution of charged clusters and nanometer particles in atmospheric air and the Balanced Scanning Mobility Analyzer BSMA, Atmos. Res., 82, 523–535, 2006.

Twomey, S.: Aerosols, clouds and radiation, Atmos. Environ., 25A, 2435–2442, 1991.

Vana, M., Tamm, E., Hõrrak, U., Mirme, A., Tammet, H., Laakso, L., Aalto, P P., and Kulmala, M.: Charging state of atmospheric nanoparticles during the nucleation burst events, Atmos. Res., 82, 536–546, 2006.

Wiedensohler, A.: An approximation of the bipolar charge distribution for particles in the submicron range, J. Aerosol Sci., 19, 387–389, 1988.

Winkler, P M., Steiner, G., Virtala, A., Vehkamäki, H., Noppel, M., Lehtinen, K. E J., Reischl, G P., Wagner, P E., and Kulmala, M.: Heterogeneous Nucleation Experiments Bridging the Scale from Molecular Ion Clusters to Nanoparticles, Science, 319, 1374–1377, http://dx.doi.org/10.1126/science. 1149034doi:10.1126/science. 1149034, 2008.

Winklmayr, W., Reischl, G P., Lindner, A O., and Berner, A.: A new electromobility spectrometer for the measurement of aerosol size distributions in the size range from 1 to 1000 nm, J. Aerosol Sci., 22, 289–296, 1991.

Yu, F.: From molecular clusters to nanoparticles: second-generation ion-mediated nucleation model, Atmos. Chem. Phys., 6, 5193–5211, http://dx.doi.org/10.5194/acp-6-5193-2006doi:10.5194/acp-6-5193-2006, 2006.

Yu, F.: Ion-mediated nucleation in the atmosphere: Key controlling parameters, implications, and look-up table, J. Geophys. Res., 115, D03 206, http://dx.doi.org/10.1029/2009JD012630doi:10.1029/2009JD012630, 2010.

Yu, F., Wang, Z., Luo, G., and Turco, R.: Ion-mediated nucleation as an important global source of tropospheric aerosols, Atmos. Chem. Phys., 8, 2537–2554, http://dx.doi.org/10.5194/acp-8-2537-2008doi:10.5194/acp-8-2537-2008, 2008.