Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 8 23 2008 10.5194/acp-8-6925-2008 http://www.atmos-chem-phys.net/8/6925/2008/ http://www.atmos-chem-phys.net/8/6925/2008/acp-8-6925-2008.html http://www.atmos-chem-phys.net/8/6925/2008/acp-8-6925-2008.pdf 6925 6938 2008-12-01 Measurements of the relation between aerosol properties and microphysics and chemistry of low level liquid water clouds in Northern Finland H. Lihavainen heikki.lihavainen@fmi.fi V.-M. Kerminen M. Komppula A.-P. Hyvärinen J. Laakia S. Saarikoski U. Makkonen N. Kivekäs R. Hillamo M. Kulmala Y. Viisanen Finnish Meteorological Institute, P.O. Box 503, 00 101 Helsinki, Finland Finnish Meteorological Institute, P.O. Box 1627, 70 211 Kuopio, Finland University of Helsinki, Dept. of Physics, P.O. Box 64, 00 014 Univ. of Helsinki, Finland Physical and chemical properties of boundary layer clouds, together with relevant aerosol properties, were investigated during the first Pallas Cloud Experiment (First Pace) conducted in northern Finland between 20 October and 9 November 2004. Two stations located 6 km apart from each other at different altitudes were employed in measurements. The low-altitude station was always below the cloud layer, whereas the high-altitude station was inside clouds about 75% of the time during the campaign. Direct measurements of cloud droplet populations showed that our earlier approach of determining cloud droplet residual particle size distributions and corresponding activated fractions using continuous aerosol number size distribution measurements at the two stations is valid, as long as the cloud events are carefully screened to exclude precipitating clouds and to make sure the same air mass has been measured at both stations. We observed that a non-negligible fraction of cloud droplets originated from Aitken mode particles even at moderately-polluted air masses. We found clear evidence on first indirect aerosol effect on clouds but demonstrated also that no simple relation between the cloud droplet number concentration and aerosol particle number concentration exists for this type of clouds. The chemical composition of aerosol particles was dominated by particulate organic matter (POM) and sulphate in continental air masses and POM, sodium and chlorine in marine air masses. The inorganic composition of cloud water behaved similarly to that of the aerosol phase and was not influenced by inorganic trace gases. Aalto, P., Hämeri, K., Becker, E., Weber, J., 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 B, 53, 344–358, 2001. Abdul-Razzak, H. and Ghan, S. J.: A parameterization of aerosol activation 2. Multiple aerosol types, J. Geophys. Res., 105, 6837–6844. 2000. Anttila, T. and Kerminen, V.-M.: Influence of organic compounds on the cloud droplet activation: a model investigation concidering the volatility, water solubility, and surface activity of organic matter, J. Geophys. Res., 107(D22), 4662, doi:10.1029/2001JD001482, 2002. Baker, M. B. and Peter, T.: Small-scale cloud processes and climate, Nature, 451, 299–300, 2008. Baltensperger, U., Schwikowski, M., Jost, D. T., Nyeki, S., Gäggeler, H. W., and Poulida, O: Scavenging of atmospheric constituents in mixed phase clouds at the high-alpine site Jungfraujoch: Part I: Basic concept and cloud scavenging, Atmos. Environ., 32, 3975–3983, 1998.. Baron, P. A. and Willike, K.: Aerosol Measurement, second edition, John Wiley and Sons, New York, 143–195, 2001. Baumgardner, D., Strapp, W., and Dye, J.E.: Evaluation of the forward scattering spectrometer probe, Part II. Correction for coincidence and dead-time losses, J. Atmos. Ocean. Tech., 2, 626–632, 1985. Brenguier, J.: Coincidence and dead-time corrections for particle counters. part ii: High concentration measurements with an FSSP, J. Atmos. Ocean. Tech., 6, 585–598, 1989. Bulgin, C. E., Palmer, P. I., Thomas, G. E., Arnold, C. P. G., Campmany, E., Carboni, E., Grainger, R. G., Poulsen, C., Siddans, R., and Lawrence, B. N.: Regional and seasonal variations of the Twomey indirect effect as observed by the ASTR-2 satellite instrument, Geophys. Res. Lett., 35, L02822, doi:10.1029/2007GL031394, 2008. Decesari, S., Facchini, M. C., Fuzzi, S., McFiggans, G. B., Coe, H., and Bower, K. N.: The water-soluble organic component of size-segregated aerosol,cloud water and wet depositions from Jeju Island during ACE-Asia, Atmos. Environ., 39, 211–222, 2005. Ekman, A. M. L., Engtröm, A., and Wang, C.: The effect of aerosol composition and concentration on the development and anvil properties of a deep convective cloud, Q. J. Roy. Meteor. Soc., 133, 1439–1452, 2007. Elbert, W., Hoffman, M. R., Krämer, M., Schmit, G., and Andreae, M. O.: Control of solute concentrations in cloud and fog water by liquid water content, Atmos. Environ., 34, 1109–1122, 2000. Ervens, B., Feingold, G., and Kreidenweis, S. M.: Influence of water-soluble organic carbon on cloud drop number concentration, J. Geophys. Res., 110, D18211, doi: 10.1029/2004JD005634, 2005. Feingold, G., Eberhard, W. L., Veron, D. E., and Previdi, M.: First measurements of the Twomey indirect effect using ground-based remote sensors, Geophys. Res. Lett., 30, 1287, doi:10.1029/2002GL016633, 2003. Fountoukis, C. and Nenes, A.: Continued development of a cloud droplet formation parameterization for global climate models, J. Geophys. Res., 110, D11212, doi:10.1029/2004JD005591, 2005. Freud, E., Rosenfeld, D., Andreae, M. O., Costa, A. A., and Artaxo, P.: Robust relations between CCN and the vertical evolution of cloud drop size distribution in deep convective clouds, Atmos. Chem. Phys., 8, 1661–1675, 2008. Gultepe, I., Isaac, G. A., Leaitch, W. R., and Banic, C. M.: Parameterizations of marine stratus microphysics based on in-situ observations: Implications for GCMs, J. Clim., 9, 345–357, 1996. Haglund, J. S. and McFarland, A. R.: A Circumferential Slot Virtual Impactor, Aerosol Sci. Technol., 38, 664–674, 2004. Hatakka, J., Aalto, T., Aaltonen, V., Aurela, M., Hakola, H., Komppula, M,. Laurila, T., Lihavainen, H., Paatero, J., Salminen, K., and Viisanen, Y.: Boreal Environ. Res., 8, 365–384, 2003. Henning, S., Weintgartner, E., Schmidt, S., Wendisch, M., Gäggeler, H. W., and Baltensberger, U.: Size-dependent aerosol activation at the high-alpine site Jungfraujoch (3580 m a.s.l.), Tellus B, 54, 82–95, 2002. Hoppel, W. A., Frick, G. M., and Larson, R. E.: Effect of nonprecipitating clouds on the aerosol size distribution in the marine boundary layer, Geophys. Res. Lett., 13, 125–128, 1986. IPCC: Summary for Policymakers. The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, in: Climate Change 2007, 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, United Kingdom and New York, NY, USA, 4~pp., 2007. Jokinen, V. and Mäkelä, J. M.: Closed-loop arrangement with critical orifice for DMA sheath/excess flow system, J. Aerosol Sci., 28, 643–648, 1997. Junge, C. E.: Air chemistry and radioactivity, Academic Press, New York, 291–295, 1963. Kivekäs, N., Kerminen, V. M., Anttila, T., Korhonen, H., Lihavainen, H., Komppula, M., and Kulmala, M.: Parameterization of cloud droplet activation using a simplified treatment of the aerosol number size distribution, J. Geophys. Res., 113, D15207, doi:10.1029/2007JD009676, 2008. Komppula, M., Lihavainen, H., Kerminen, V.-M., Kulmala, M., and Viisanen, Y.: Measurements of cloud droplet activation of aerosol particles at a clean subarctic background site, J. Geophys. Res., 110, D06204, doi:10.1029/2004JD005200, 2005. Koren, I., Remer, L. A., Kaufman, Y. J., Rudich, Y., and Martins, J. V.: On the twilight zone between clouds and aerosols, Geophys. Res. Lett., 34, L8805, doi:10.1029/2007GL029253, 2007. Korhonen, H., Kerminen, V.-M., Lehtinen, K. E. J., and Kulmala, M.: CCN activation and cloud processing in sectional aerosol models with low size resolution, Atmos. Chem. Phys., 5, 2561–2570, 2005. Korhonen, P. and Viisanen, Y.: A Fogwater Collector for High Flow Velocities, J. Aerosol Sci., 26, Suppl~1, S805–S806, 1995. Kulmala, M., Korhonen, P., Vesala, T., Hansson, H.-C., Noone, K., and Svenningsson, B.: The effect of hygroscopicity on cloud droplet formation, Tellus B,48, 347–360, 1996 Liu, Y., Daum, P. H., McGraw, R. L., Miller, M. A., and Niu, S.: Theoretical expression for the autoconversion rate of the cloud droplet number concentration, Geophys. Res. Lett., 34, L16821, doi:10.1029/2007GL030389, 2007. 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 high efficiency virtual impactor, Aerosol Sci. Technol., 9, 167–176, 1988. Lu, M.-L. and Seinfeld, J. H.: Effect of aerosol number concentration on cloud droplet dispersion: A large-eddy simulation study and implications for aerosol indirect forcing, J. Geophys. Res., 111, D02207, doi:10.1029/2005JD006419, 2006. Maenhaut, W., Hillamo, R., Mäkelä, T., Jaffrezo, J.-L., Bergin, J.-L., and Davidson, M. H.: A new cascade impactor for aerosol sampling with subsequent PIXE analysis, Nucl. Instrum. Meth. B, 109/110, 482–487, 1996. Marinoni, A., Laj, P., Sellegri, K., and Mailhot, G.: Cloud chemistry at the Puy de Dôme: variability and relationships with environmental factors, Atmos. Chem. Phys., 4, 715–728, 2004. Martin, G. M., Johnson, D. W., and Spice, A.: The measurements and parameterization of effective radius of droplets in warm stratocumulus clouds, J. Atmos Sci., 51, 1823–1842, 1994. Martinsson, B. G, Frank, G., Cedefelt, S., Swietlicki, E., Berg, O. H., Zhou, J., Bower, K. N., Bradbury, C., Birmili, W., Stratmann, F., Wendisch, M., Wiedensohler, A., and Yuskiewicz, B.A: Droplet nucleation and growth in orographic cloud in relation to the aerosol population, Atmos. Res., 50, 289–315, 1999. Mauger, G. S. and Norris, J. R.: Meteorological bias in satellite estimates of aerosol-cloud relationships, Geophys. Res. Lett., 34, L16824, doi:10.1029/2007GL029952, 2007. McComiskey, A. and Feingold, G.: Quantifying error in the radiative forcing of the first indirect effect, Geophys. Res. Lett., 35, L02810, doi:10.1029/2007GL032667, 2008. McFarland, A. R., Gong, H., Muyshondt, A., Wente, W. B., and Anand, N. K.: Aerosol Deposition in Bends with Turbulent Flow, Environ. Sci. Technol., 31, 3371–3377, 1997. McFarquhar, G. M. and Heymsfield, A. J.: Parameterization of INDOEX microphysical measurements and calculations of cloud susceptibility: Applications for climate studies, J. Geophys. Res., 106, 28 675–28 698, 2001. Myhre, G., Stordal, F., Johnsrud, M., Kaufman, Y. J., Rosenfeld, D., Storelvmo, T., Kristjansson, J. E., Berntsen, T. K., Myhre, A., and Isaksen, I. S. A.: Aerosol-cloud interaction inferred from MODIS satellite data and global aerosol models, Atmos. Chem. Phys., 7, 3081–3101, 2007. Möller, D., Acker, K., and Wieprecht, W.: A relationship between liquid water content and chemical composition on clouds, Atmos. Res., 41, 321–335, 1996. Nenes, A., Ghan, S., Abdul-Razzak, H., Chuang, P., and Seinfeld, J. H.: Kinetic limitations on cloud droplet formation and impact on cloud albedo, Tellus B, 53, 133–149, 2001. Penner, J. E., Quaas, J., Storelvmo, T., Takemura, T., Boucher, O., Guo, H., Kirkevåg, A., Kristjánsson, J. E., and Seland, Ø.: Model intercomparison of indirect aerosol effects, Atmos. Chem. Phys., 6, 3391–3405, 2006. Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics, John Wiley and Sons, New Jersey, 790~pp., 2006 Quaas, J., Boucher, O., Bellouin, N., and Kinne, S.: Satellite-based estimate of the direct and indirect aerosol climate forcing, J. Geophys. Res., 113, D05204, doi:10.1029/2007JD008962, 2008. Romakkaniemi, S., Kokkola, H., and Laaksonen, A.: Soluble trace gas effect on cloud condensation nuclei activation: Influence of initial equilibration on cloud model results, J. Geophys. Res., 110, D15202, doi:10.1029/2004JD005364, 2005. Rosenfeld, D. and Lensky, I. M.: Satellite-based insights into precipitation formation processes in continental and maritime convective clouds, B. Am. Meteorol. Soc., 79, 2457–2476, 1998. Saarikoski, S., Mäkelä, T., Hillamo, R., Aalto, P. P., Kerminen, V-M., and Kulmala, M.: Physico-chemical characterization and mass closure of size-segregated atmospheric aerosols in Hyytiälä, Finland, Boreal Environ. Res., 10, 385–400, 2005. Sorjamaa, R. and Laaksonen, A.: The influence of surfactant properties on critical supersaturations of cloud condensation nuclei, J. Aerosol Sci., 37, 1730–1736, 2006. Song, C. H. and Carmichael, G. R.: The aging process of naturally emitted aerosol (sea-salt and mineral aerosol) during long range transport, Atmos. Environ., 33, 2203–2218, 1999. 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, L06808, doi:10.1029/2007GL033038, 2008. Stohl, A. and Seibert, P.: Accuracy of trajectories as determined from the conservation of meteorological tracers, Q J Roy. Meteor. Soc., 125, 1465–1484, 1998. Twohy, C. H., Petters, M. D., Snider, J. R., Stevens, B., Tahnk, W., Wetzel, M., Russel, L., and Burnet, F.: Evaluation of the aerosol indirect effect in marine stratocumulus clouds: Droplet number, size, liquid water path, and radiative impact, J. Geophys. Res., 110, D08203, doi:10.1029/2004JD005116, 2005. Twomey, S.: Pollution and the planetary albedo, Atmos. Environ., 8, 1251–1256, 1974. Winklmayr, W., Reischl, G. P., Linder, A. O., and Berner, A.: A new electromobility spectrometer for the measurement of aerosol size distribution in the size range 1 to 1000 nm, J. Aerosol Sci., 22, 289–296, 1991.