ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-10-1885-2010 Atmospheric data over a solar cycle: no connection between galactic cosmic rays and new particle formation Kulmala M. 1 Riipinen I. 1 2 Nieminen T. 1 Hulkkonen M. 1 Sogacheva L. 1 3 Manninen H. E. 1 Paasonen P. 1 Petäjä T. 1 Dal Maso M. 1 Aalto P. P. 1 Viljanen A. 3 Usoskin I. 4 Vainio R. 1 Mirme S. 5 Mirme A. 5 Minikin A. 6 Petzold A. 6 Hõrrak U. 5 Plaß-Dülmer C. 7 Birmili W. 8 Kerminen V.-M. 3 University of Helsinki, Helsinki, Finland Carnegie Mellon University, Pittsburgh, Pennsylvania, USA Finnish Meteorological Institute, Helsinki, Finland Sodankylä Geophysical Observatory (Oulu Unit), University of Oulu, Sodankylä, Finland University of Tartu, Tartu, Estonia Deutsches Zentrum für Luft- und Raumfahrt (DLR), Wessling, Germany Meteorologisches Observatorium Hohenpeissenberg, Deutscher Wetterdienst (DWD), Hohenpeissenberg, Germany Leibniz Institute for Tropospheric Research, Leipzig, German 18 02 2010 10 4 1885 1898 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/10/1885/2010/acp-10-1885-2010.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/1885/2010/acp-10-1885-2010.pdf

Aerosol particles affect the Earth's radiative balance by directly scattering and absorbing solar radiation and, indirectly, through their activation into cloud droplets. Both effects are known with considerable uncertainty only, and translate into even bigger uncertainties in future climate predictions. More than a decade ago, variations in galactic cosmic rays were suggested to closely correlate with variations in atmospheric cloud cover and therefore constitute a driving force behind aerosol-cloud-climate interactions. Later, the enhancement of atmospheric aerosol particle formation by ions generated from cosmic rays was proposed as a physical mechanism explaining this correlation. Here, we report unique observations on atmospheric aerosol formation based on measurements at the SMEAR II station, Finland, over a solar cycle (years 1996–2008) that shed new light on these presumed relationships. Our analysis shows that none of the quantities related to aerosol formation correlates with the cosmic ray-induced ionisation intensity (CRII). We also examined the contribution of ions to new particle formation on the basis of novel ground-based and airborne observations. A consistent result is that ion-induced formation contributes typically significantly less than 10% to the number of new particles, which would explain the missing correlation between CRII and aerosol formation. Our main conclusion is that galactic cosmic rays appear to play a minor role for atmospheric aerosol formation events, and so for the connected aerosol-climate effects as well.

 References Aalto, 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. Baker, M. B. and Peter, T.: Small-scale cloud processes and climate, Nature, 451, 299–300, 2008. Bazilevskaya, G. A., Usoskin, I. G., Flückiger, E. O., Harrison, R. G., Desorgher, L., Bütikofer, R., Krainev, M. B., Makhmutov, V. S., Stozhkov, Y. I., Svirzhevskaya, A. K., Svirzhevsky, N. S., and Kovaltsov, G. A.: Cosmic ray induced ion production in the atmosphere, Space Sci. Rev., 137, 149–173, 2008. Birmili, W., Wiedensohler, A., Plass-Dülmer, C., and Berresheim, H.: Evolution of newly formed aerosol particles in the continental boundary layer: A case study including OH and H<sub>2</sub>SO<sub>4</sub> measurements, Geophys. Res. Lett., 27, 2205–2208, 2000. Birmili, W., Schepanski, K., Ansmann, A., Spindler, G., Tegen, I., Wehner, B., Nowak, A., Reimer, E., Mattis, I., Müller, K., Brüggemann, E., Gnauk, T., Herrmann, H., Wiedensohler, A., Althausen, D., Schladitz, A., Tuch, T., and Löschau, G.: A case of extreme particulate matter concentrations over Central Europe caused by dust emitted over the southern Ukraine, Atmos. Chem. Phys., 8, 997–1016, 2008. Buenrostro Mazon, S., Riipinen, I., Schultz, D. M., Valtanen, M., Dal Maso, M., Sogacheva, L., Junninen, H., Nieminen, T., Kerminen, V.-M., and Kulmala, M.: Classifying previously undefined days from eleven years of aerosol-particle-size distribution data from the SMEAR~II station, Hyytiälä, Finland, Atmos. Chem. Phys., 9, 667–676, 2009. Carslaw, K. S., Harrison, R. G., and Kirkby, J.: Cosmic rays, clouds, and climate, Science, 298, 1732–1737, 2002. Clement, A. C., Burgman, R., and Norris, J. R.: Observational and model evidence for positive low-level cloud feedback, Science, 325(5939), 460–464, doi:10.1126/science.1171255, 2009. Dal Maso, M., Sogacheva, L., Aalto, P. P., Riipinen, I., Komppula, M., Tunved, P., Korhonen, L., Suur-Uski, V., Hirsikko, A., Kurten, T., Kerminen, V.-M., Lihavainen, H., Viisanen, Y., Hansson, H.-C., and Kulmala, M.: Formation and growth of fresh atmospheric aerosols: eigth years of aerosol size distribution data from SMEAR~II, Hyytiälä, Finland, Boreal Environ. Res., 10, 323–336, 2005. Dickinson, R. E.: Solar variability and the lower atmosphere, B. Am. Meteor. Soc., 56, 1240–1248, 1975. Engler, C., Rose, D., Wehner, B., Wiedensohler, A., Brüggemann, E., Gnauk, T., Spindler, G., Tuch, T., and Birmili, W.: Size distributions of non-volatile particle residuals (D$_\rm p<$800 nm) at a rural site in Germany and relation to air mass origin, Atmos. Chem. Phys., 7, 5785–5802, 2007. 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. Gleeson, L. J. and Axford, W. I.: Solar modulation of galactic cosmic rays, Astrophys. J., 154, 1011–1026, 1968. Hari, P. and Kulmala, M.: Station for Measuring Ecosystem-Atmosphere relations, Boreal Environ. Res., 10, 315–322, 2005. Harrison, R. G. and Stephenson, D. B.: Empirical evidence for a nonlinear effect of galactic cosmic rays on clouds, Philos. T. R. Soc. A, 462, 1221–1223, 2006. Hartman, D. L:. Global Physical Climatology, Academic Press, 411~s, 1994. Hirsikko, A., Paatero, J., Hatakka, J., and Kulmala, M.: $^222$Rn activity concentration, external radiatio dose and air ion production rates in a boreal forest in Finland between March~2000 and June~2006, Boreal Environ. Res., 12, 265–278, 2007. Hock, N., Schneider, J., Borrmann, S., Römpp, A., Moortgat, G., Franze, T., Schauer, C., Pöschl, U., Plass-Dülmer, C., and Berresheim, H.: Rural continental aerosol properties and processes observed during the Hohenpeissenberg Aerosol Characterization Experiment (HAZE2002), Atmos. Chem. Phys., 8, 603–623, 2008. Iida, K., Stolzenburg, M., McMurry, P., 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, doi:1029/2006JD007167, 2006. IPCC: The Scientific Basis: A report of Working Group~I of the Intergovernmental Panel on Climate Change, in: Climate Change 2007: The Physical Science Basis, Contribution of Working Group~I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K. B., Tignor, M., and Miller, H. L., Cambridge University Press, Cambridge, UK and New York, NY, USA, 2007. Jokinen, V. and Mäkelä, J. M.: Closed loop arrangement with critical orifices for DMA sheath/excess flow system, J. Aerosol Sci., 28, 643–648, 1997. 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, 2006. Kristánsson, J. E., Stjern, C. W., Stordal, F., Fjæraa, A. M., Myhre, G., and Jónasson, K.: Cosmic rays, cloud condensation nuclei and clouds - a reassessment using MODIS data, Atmos. Chem. Phys., 8, 7373–7387, 2008. Kulmala, M., Hämeri, K., Aalto, P. P., Mäkelä, J. M., Pirjola, L., Nilsson, E. D., Buzorius, G., Rannik, U., Dal Maso, M., Seidl, W., Hoffmann, T., Janson, R., Hansson, H.-C., Viisanen, Y., Laaksonen, A., and O'Dowd, C. D.: Overview of the international project on biogenic aerosol formation in the boreal forest (BIOFOR), Tellus, 53B, 324–343, 2001. Kulmala, M., Vehkamäki, H., Petäjä, T., Dal Maso, M., Lauri, A., Kerminen, V.-M., Birmili, W., and McMurry, P.: 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.-M.: Toward direct measurement of atmospheric nucleation, Science, 318(5847), 89–92, doi:10.1126/science.1144124, 2007. 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, 2009. Mayaud, P. N.: Derivation, Meaning, and Use of Geomagnetic Indices, AGU, Washington, DC, 1980. Minikin, A., Petzold, A., Ström, J., Krejci, R., Seifert, M., van Velthoven, P., Schlager, H., and Schumann, U.: Aircraft observations of the upper tropospheric fine particle aerosol in the Northern and Southern Hemispheres at midlatitudes, Geophys. Res. Lett., 30, 1503, doi:10.1029/2002GL016458, 2003. 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 Specrometer, Boreal Environ. Res., 12, 247–264, 2007. Mirme, S., Mirme, A., Minikin, A., Petzold, A., Hõrrak, U., Kerminen, V.-M., and Kulmala, M.: Atmospheric sub-3 nm particles at high altitudes, Atmos. Chem. Phys., 10, 437–451, 2010. Mäkelä, J. M., Aalto, P., Jokinen, V., Pohja, T., Nissinen, A., Palmroth, S., Markkanen, T., Seitsonen, K., Lihavainen, H., and Kulmala, M.: Observations of ultrafine aerosol particle formation and growth in boreal forest, Geophys. Res. Lett., 24, 1219–1222, 1997. Mäkelä, J. M., Koponen, I. K., Aalto, P., and Kulmala, M.: One-year data of submicron size modes of tropospheric background aerosol in Southern Finland, J. Aerosol Sci., 31, 595–611, 2000. Palle, E.: Possible satellite perspective effects on the reported correlations between solar activity and clouds, Geophys. Res. Lett., 32, L03802, doi:10.1029/2004GL021167, 2005. Pierce, J. R. and Adams, P. J.: Can cosmic rays affect cloud condensation nuclei by altering new particle formation rates?, Geophys. Res. Lett., 36, L09820, doi:10.1029/2009GL037946, 2009. ' Rangarayan, G. K.: Indices of Geomagnetic Activity, in: Geomagnetism, edited by: Jacobs, J. A., Academic Press, 3, 323–384, 1989. Rohrer, F. and Berresheim, H.: Strong correlation between levels of tropospheric hydroxyl radicals and solar ultra-violet radiation, Nature, 442, 184-187, doi:10.1038/nature04924, 2006. Sloan, T. and Wolfendale, A. W.: Testing the proposed causal link between cosmic rays and cloud cover, Environ. Res. Lett., 3, 1–6, 2008. Sogacheva, L., Saukkonen, L., Nilsson, E. D., Dal Maso, M., Schultz, D., de Leeuw, G., and Kulmala, M.: New aerosol particle formation in different synoptic situations at Hyytiälä, southern Finland, Tellus, 60B, 485–494, 2008. Spracklen, D. V., Carslaw, K. S., Kulmala, M., Kerminen, V.-M., Sihto, S.-L., Riipinen, I., Merikanto, J., Mann, G. W., Chipperfield, P. M., Wiedensohler, A., Birmili, W., and Lihavainen, H:. Contribution of particle formation to global cloud condensation nuclei concentrations, Geophys. Res. Lett., 35, L06808, doi:10.1029/2007GL033038, 2008. Sun, B. and Bradley, R. S.: Solar influences on cosmic rays and cloud formation: A reassessment, J. Geophys. Res., 107(D14), D14206, doi:10.1029/2001JD000560, 2002. Svensmark, H. and Friis Christensen, E.: Variation of cosmic ray flux and global cloud coverage – A missing link in solar-climate relationships, J. Atmos. Sol.-Terr. Phy., 59, 1225–1232, 1997. Svensmark, H., Bondo, T., and Svensmark, J.: Cosmic rays decreases affect atmospheric aerosols and clouds, Geophys. Res. Lett., 36, L15101, doi:10.1029/2009GL038429, 2009. Tinsley, B. A.: Influence of Solar Wind on the Global Electric Circuit, and Inferred Effects on Cloud Microphysics, Temperature, and Dynamics in the Troposphere, Space Sci. Rev., 94, 231–258, 2000. Usoskin, I. G., Alanko-Huotari, K., Kovaltsov, G. A., and Mursula, K.: Solar activity, cosmic rays, and Earth's temperature: A millennium-scale comparison, J. Geophys. Res., 110, A12108, doi:10.1029/2004JA010946, 2005. Usoskin, I. G. and Kovaltsov, G. A.: Cosmic ray induced ionization in the atmosphere: Full modeling and practical applications, J. Geophys. Res., 111, D21206, doi:10.1029/2006JD007150, 2006. Usoskin, I. G. and Kovaltsov, G. A.: Cosmic rays and climate of the Earth: Possible connection, Compt. Rend. Geosci., 340, 441–450, 2008. Usoskin, I. G., Laurent, D., Velinov, P., Storini, M., Flückiger, E. O., Bütikofer, R., Kovaltsov, G. A.: Ionization of the Earth's atmosphere by solar and galactic cosmic rays, Acta Geophys., 57, 88–101, 2009. Weinzierl, B., Petzold, A., Esselborn, M., Wirth, M., Rasp, K., Kandler, K., Schütz, L., Koepke, P., Fiebig, M.: Airborne measurements of dust layer properties, particle size distribution and mixing state of Saharan dust during SAMUM~2006, Tellus, 61B, 96–117, 2009. Winkler, P. M., Steiner, G., Vrtala, 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(5868), 1374–1377, doi:10.1126/science.1149034, 2008. 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, 2008.