References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-9-7067-2009

Aerosol- and updraft-limited regimes of cloud droplet formation: influence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN)

Reutter

¹ ² Su

¹ Trentmann

² ⁴ Simmel

³ Rose

¹ Gunthe

S. S.

¹ Wernli

² Andreae

M. O.

¹ Pöschl

Max Planck Institute for Chemistry, Biogeochemistry Department, Mainz, Germany

Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany

Leibniz Institute for Tropospheric Research, Leipzig, Germany

now at: German Weather Service, DWD Offenbach, Germany

24 09 2009

9 18 7067 7080

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We have investigated the formation of cloud droplets under pyro-convective conditions using a cloud parcel model with detailed spectral microphysics and with the κ-Köhler model approach for efficient and realistic description of the cloud condensation nucleus (CCN) activity of aerosol particles. Assuming a typical biomass burning aerosol size distribution (accumulation mode centred at 120 nm), we have calculated initial cloud droplet number concentrations (NCD) for a wide range of updraft velocities (w=0.25–20 m s−1) and aerosol particle number concentrations (NCN=200–105 cm−3) at the cloud base. Depending on the ratio between updraft velocity and particle number concentration (w/NCN), we found three distinctly different regimes of CCN activation and cloud droplet formation: (1) An aerosol-limited regime that is characterized by high w/NCN ratios (>≈10−3 m s−1 cm3), high maximum values of water vapour supersaturation (Smax>≈0.5%), and high activated fractions of aerosol particles (NCN/NCN>≈90%). In this regime NCD is directly proportional to NCN and practically independent of w. (2) An updraft-limited regime that is characterized by low w/NCN ratios (<≈10−4 m s−1 cm3), low maximum values of water vapour supersaturation (Smax<≈0.2%), and low activated fractions of aerosol particles (NCD/NCN<≈20%). In this regime NCD is directly proportional to w and practically independent of NCN. (3) An aerosol- and updraft-sensitive regime (transitional regime), which is characterized by parameter values in between the two other regimes and covers most of the conditions relevant for pyro-convection. In this regime NCD depends non-linearly on both NCN and w. In sensitivity studies we have tested the influence of aerosol particle size distribution and hygroscopicity on NCD. Within the range of effective hygroscopicity parameters that is characteristic for continental atmospheric aerosols (κ≈0.05–0.6), we found that NCD depends rather weakly on the actual value of κ. A compensation of changes in κ and Smax leads to an effective buffering of NCD. Only for aerosols with very low hygroscopicity (κ<0.05) and also in the updraft-limited regime for aerosols with higher than average hygroscopicity (κ>0.3) did the relative sensitivities ∂lnNCD/∂lnκ≈ (ΔNCD/NCD)/(Δκ/κ) exceed values of ~0.2, indicating that a 50% difference in κ would change NCD by more than 10%. The influence of changing size distribution parameters was stronger than that of particle hygroscopicity. Nevertheless, similar regimes of CCN activation were observed in simulations with varying types of size distributions (polluted and pristine continental and marine aerosols with different proportions of nucleation, Aitken, accumulation, and coarse mode particles). In general, the different regimes can be discriminated with regard to the relative sensitivities of NCD against w and NCN (∂lnNCD/∂lnw and ∂lnNCD/∂lnNCN). We propose to separate the different regimes by relative sensitivity ratios, (∂lnNCD/∂lnw)/(∂lnNCD/∂lnNCN) of 4:1 and 1:4, respectively. The results of this and related studies suggest that the variability of initial cloud droplet number concentration in convective clouds is mostly dominated by the variability of updraft velocity and aerosol particle number concentration in the accumulation and Aitken mode. Coarse mode particles and the variability of particle composition and hygroscopicity appear to play major roles only at low supersaturation in the updraft-limited regime of CCN activation (Smax<0.2%).

References 1

% vor jede Referenz Altaratz, O., Koren, I., Reisin, T., Kostinski, A., Feingold, G., Levin, Z., and Yin, Y.: Aerosols' influence on the interplay between condensation, evaporation and rain in warm cumulus cloud, Atmos. Chem. Phys., 8, 15–24, 2008.

Andreae, M. O., Artaxo, P., Fischer, H., Freitas, S. R., Gregoire, J.-M., Hansel, A., Hoor, P., Kormann, R., Krejci, R., Lange, L., Lelieveld, J., Lindinger, W., Longo, K., Peters, W., de Reus, M., Scheeren, B., Silva Dias, M. A. F., Ström, J., van Velthofen, P. F. J., and Williams, J.: Transport of biomass burning smoke to the upper troposphere by deep convection in the equatorial region, Geophys. Res. Lett., 28, 951–954, 2001.

Andreae, M. O., Rosenfeld, D., Artaxo, P., Costa, A. A., Frank, G. P., Longo, K. M., and Silva-Dias, M. A. F.: Smoking Rain Clouds over the Amazon, Science, 303, 1337–1342, 2004.

Andreae, M. O. and Rosenfeld, D.: Aerosol-cloud-precipitation interactions. Part 1: The nature and sources of cloud-active aerosols, Earth Sci. Rev., 89, 13–41, doi:10.1016/j.earscirev.2008.03.001, 2008.

Asa-Awuku, A., Engelhart, G. J., Lee, B. H., Pandis, S. N., and Nenes, A.: Relating CCN activity, volatility, and droplet growth kinetics of �-caryophyllene secondary organic aerosol, Atmos. Chem. Phys., 9, 795–812, 2009.

Chuang, C. C., Penner, J. E., and Edwards, L. L.: Nucleation Scavenging of Smoke Particles and Simulated Drop Size Distributions over Large Biomass Fires, J. Atmos. Sci, 49(14), 1264–1275, 1992.

Cubison, M. J., Ervens, B., Feingold, G., Docherty, K. S., Ulbrich, I. M., Shields, L., Prather, K., Hering, S., and Jimenez, J. L.: The influence of chemical composition and mixing state of Los Angeles urban aerosol on CCN number and cloud properties, Atmos. Chem. Phys., 8, 5649–5667, 2008.

Diehl, K., Simmel, M., and Wurzler, S.: Numerical sensitivity studies on the impact of aerosol properties and drop freezing modes on the glaciation, microphysics, and dynamics of clouds, J. Geophys. Res., 111, D07202, doi:10.1029/2005JD005884, 2006.

Diehl, K., Simmel, M., and Wurzler, S.: Effects of drop freezing on microphysics of an ascending cloud parcel under biomass burning conditions, Atmos. Environ., 41, 303–314, 2007.

Ekman, A. M. L., Krejci, R., Engstrom, A., Ström, J., de Reus, M., Williams, J., and Andreae, M. O.: Do organics contribute to small particle formation in the Amazonian upper troposphere?, Geophys. Res. Lett., 35, L17810, doi:10.1029/2008GL034970, 2008.

Ervens, B., Feingold, G., and Kreidenweis, S. M.: The influence of water soluble organic carbon on cloud drop number concentration, J. Geophys. Res., 110, D18211, doi:10.1029/2004JD005634, 2005.

Engelhart, G. J., Asa-Awuku, A., Nenes, A., and Pandis, S. N.: CCN activity and droplet growth kinetics of fresh and aged monoterpene secondary organic aerosol, Atmos. Chem. Phys., 8, 3937–3949, 2008.

Feingold, G.: Modeling of the first indirect effect: Analysis of measurement requirements, Geophys. Res. Lett., 19, p 1997, doi:10.1029/2003GL017967, 2003.

Feingold, G. and Siebert, H.: Cloud-aerosol interactions from the micro to cloud scale, edited by: Heintzenberg, J. and Charlson, R. J., MIT Press, Cambridge, 319–338, 2009.

Fromm, M., Alfred, J., Hoppel, K., Hornstein, J., Bevilacqua, R., Shettle, E., Servranckx, R., Li, Z., and Stocks., B.: Observations of boreal forest fire smoke in the stratosphere by POAM III, SAGE II, and lidar in 1998, Geophys. Res. Lett., 27(9), 1407–1410, 2000.

Fromm, M. and Servranckx, R.: Transport of forest fire smoke above the tropopause by supercell convection, Geophys. Res. Lett., 30(10), 1542, doi:10.1029/2002GL016820, 2003.

Fromm, M., Bevilacqua, R., Servranckx, R., Rosen, J., Thayer, J. P., Herman, J., and Larko, D.: Pyro-cumulonimbus injection of smoke to the stratosphere: Observations and impact of a super blowup in northwestern Canada on 3–4 August 1998, J. Geophys. Res., 110, D08205, doi:10.1029/2004JD005350, 2005.

Gunthe, S. S., King, S. M., Rose, D., Chen, Q., Roldin, P., Farmer, D. K., Jimenez, J. L., Artaxo, P., Andreae, M. O., Martin, S. T., and Pöschl, U.: Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity, Atmos. Chem. Phys. Discuss., 9, 3811–3870, 2009a.

Gunthe, S., Su, H., Pöschl, U., et al.: Aerosol- and updraft-limited regimes of CCN activation over blue and green oceans, in preparation, 2009b.

Hegg, D. A.: Dependence of Marine Stratocumulus Formation on Aerosols, Geophys. Res. Lett., 26(10), 1429–1432, 1999.

Helsper, C., Fissan, H. J., Muggli, J., and Scheidweiler, A.: Particle number distribution of aerosols from test fires, J. Atmos. Sci., 11, 439–446, 1980.

Hjelmfelt, M. R., Farley, R. D., and Chen, P. C. S.: A preliminary numerical study into the effects of coal development on cloud and precipitation processes in the Northern Great Plains, J. Appl. Meteorol., 17(6), 846–857, 1978.

IAPSAG: WMO/IUGG International Aerosol Precipitation Science Assessment Group (IAPSAG) Report: Aerosol Pollution Impact on Precipitation: A Scientific Review, Geneva, World Meteorological Organization, 482~pp., 2007.

IPCC: 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., Tignor, M., and Miller, H. L., Cambridge University Press, Cambridge and New York, 996~pp., 2007.

Janhäll, S., Andreae, M. O., and Pöschl, U.: Biomass burning aerosol emissions from vegetation fires: particle number and mass emission factors and size distributions, Atmos. Chem. Phys. Discuss., 9, 17183–17217, 2009.

Jiang, H. J., Wang, B., Goya, K., Hocke, K., Eckermann, S. D., Ma, J., Wu, D. L., and Read W. G.: Geographical distribution and interseasonal variability of tropical deep convection: UARS MLS observations and analyses, J. Geophys. Res., 109, D03111, doi:10.1029/2003JD003756, 2004.

Kivekas, 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(D15), D15207, doi:10.1029/2007JD009485, 2008.

Khain, A. P., BenMoshe, N., and Pokrovsky, A.: Factors determining the impact of aerosols on surface precipitation from clouds: An attempt at classification, J. Atmos. Sci., 65, 1721–1748, 2008.

Kreidenweis, S. M., Petters, M. D., and Chuang, P. Y.: Cloud particle precursors, in: Clouds in the perturbed climate system – their relationship to energy balance, atmospheric dynamics, and precipitation, edited by: Heintzenberg, J. and Charlson, R. J., MIT Press, Cambridge, 291–317, 2009.

Köhler, H.: The nucleus in the growth of hygroscopic droplets, T. Faraday Soc., 32, 1152–1161, 1936.

Laaksonen, A., Vesala, T., Kulmala, M., Winkler, P. M., and Wagner, P. E.: Commentary on cloud modelling and the mass accommodation coefficient of water, Atmos. Chem. Phys., 5, 461–464, 2005.

Lance, S., Nenes, A., and Rissman, T. A.: Chemical and dynamical effects on cloud droplet number: Implications for estimates of the aerosol indirect effect, J. Geophys. Res., 109(D22), D22208, doi:10.1029/2004JD004596, 2004.

Liu, S.,Hu, M., Wu, Z., Wehner, B., Wiedensohler, A., and Cheng, Y.: Aerosol number size distribution and new particle formation at a rural/coastal site in Pearl River Delta (PRD) of China, Atmos. Environ., 42, 6275–6283, 2008.

Lohmann, U., Broekhuizen, K., Leatich, R. Shantz, and Abbatt, J.: How efficient is cloud droplet formation of organic aerosols, Geophys. Res. Lett., 31, L05108, doi:10.1029/2003GL018999, 2004.

Luderer, G., Trentmann, J., Winterrath, T., Textor, C., Herzog, M., Graf, H. F., and Andreae, M. O.: Modeling of biomass smoke injection into the lower stratosphere by a large forest fire (Part II): sensitivity studies, Atmos. Chem. Phys., 6, 5261–5277, 2006.

McFiggans, G., Artaxo, P., Baltensperger, U., Coe, H., Facchini, M. C., Feingold, G., Fuzzi, S., Gysel, M., Laaksonen, A., Lohmann, U., Mentel, T. F., Murphy, D. M., O'Dowd, C. D., Snider, J. R., and Weingartner, E.: The effect of physical and chemical aerosol properties on warm cloud droplet activation, Atmos. Chem. Phys., 6, 2593–2649, 2006.

Mikhailov, E., Vlasenko, S., Martin, S. T., Koop, T., and Pöschl, U.: Amorphous and crystalline aerosol particles interacting with water vapor – Part 1: Microstructure, phase transitions, hygroscopic growth and kinetic limitations, Atmos. Chem. Phys. Discuss., 9, 7333–7412, 2009.

Molina, L. T., Kolb, C. E., de Foy, B., Lamb, B. K., Brune, W. H., Jimenez, J. L., Ramos-Villegas, R., Sarmiento, J., Paramo-Figueroa, V. H., Cardenas, B., Gutierrez-Avedoy, V., and Molina, M. J.: Air quality in North America's most populous city � overview of the MCMA-2003 campaign, Atmos. Chem. Phys., 7, 2447–2473, 2007.

Mönkkönen, P., Koponen, I. K., Lehtinen, K. E. J., Hämeri, K., Uma, R., and Kulmala, M.: Measurements in a highly polluted Asian mega city: observations of aerosol number size distribution, modal parameters and nucleation events, Atmos. Chem. Phys., 5, 57–66, 2005.

Murphey, H. V., Wakimoto, R. M., Flamant, C., and Kingsmill., D. E.: Dryline on 19 June 2002 during IHOP. Part I: Airborne Doppler and LEANDRE II Analyses of the Thin Line Structure and Convection Initiation, Mon. Weather Rev., 134, 406–430, 2006.

Nenes, A., Ghan, S., Abdul-Razzak, H., Chuang, P. Y., and Seinfeld, J. H.: Kinetic limitations on cloud droplet formation and impact on cloud albedo, Tellus, 53(2), 133–149, 2001.

Penner, J. E., Dong, X., and Chen, Y.: Observational evidence of a change in radiative forcing due to the indirect aerosol effect, Nature, 427, 231–234, 2004.

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, 2007.

Phillips, V. T. J., Donner, L. J., and Garner, S. T.: Nucleation processes in deep convection simulated by a cloud-system-resolving model with double-moment bulk microphysics, J. Atmos. Sci., 64, 738–761, 2007.

Pitzer, K. S. and Mayorga, G.: Thermodynamics of electrolytes. II. Acitivity and osmotic coefficients for strong electrolytes with one or both ions univalent, J. Phys. Chem., 77, 2300–2308, 1973.

Pöschl, U., Rudich, Y., and Ammann, M.: Kinetic model framework for aerosol and cloud surface chemistry and gas-particle interactions – Part 1: General equations, parameters, and terminology, Atmos. Chem. Phys., 7, 5989–6023, 2007.

Pöschl, U., Rose, D., and Andreae M. O.: Climatologies of cloud-related aerosols – Part 2: Particle hygroscopicity and cloud condensation nucleus activity, in: Clouds in the perturbed climate system – Their relationship to energy balance, atmospheric dynamics, and precipitation, edited by: Heintzenberg, J. and Charlson, R. J., MIT Press, Cambridge, 58–72, 2009.

Posselt, R. and Lohmann, U.: Influence of Giant CCN on warm rain processes in the ECHAM5 GCM, Atmos. Chem. Phys., 8, 3769–3788, 2008.

Pruppacher, H. R. and Klett, J. D.: Microphysics of clouds and precipitation, Kluwer Academics Publishers, 1997.

Ramanathan, V., Crutzen, P. J., Kiehl, J. T., and Rosenfeld, D.: Aerosols, Climate, and the Hydrological Cycle, Science, 294, 2119–2124, 2001a.

Ramanathan, V., Crutzen, P. J., Lelieveld, J., et al.: Indian Ocean Experiment: An integrated analysis of the climate forcing and effects of the great Indo-Asian haze, J. Geophys. Res., 106, 28371–28398, 2001b.

Reid, J. S. and Hobbs, P. V.: Physical and optical properties of young smoke from individual biomass fires in Brazil, J. Geophys. Res., 103, 32013–32030, 1998.

Reid, J. S., Koppmann, R., Eck, T. F., and Eleuterio, D. P.: A review of biomass burning emissions part II: intensive physical properties of biomass burning particles, Atmos. Chem. Phys., 5, 799–825, 2005.

Rissmann, T. A., Nenes, A., and Seinfeld, J. H.: Chemical amplification (or dampening) if the Towmey effect: Conditions derived from droplet activation theory, J. Atmos. Sci., 61(8), 919–930, 2004.

Robinson, R. A. and Stokes, R. H.: Electrolyte Solutions, (revised), London: Butterworth, 1959.

Rose, D., Gunthe, S. S., Mikhailov, E., Frank, G. P., Dusek, U., Andreae, M. O., and Pöschl, U.: Calibration and measurement uncertainties of a continuous-flow cloud condensation nuclei counter (DMT-CCNC): CCN activation of ammonium sulfate and sodium chloride aerosol particles in theory and experiment, Atmos. Chem. Phys., 8, 1153–1179, 2008a.

Rose, D., Nowak, A., Achtert, P., Wiedensohler, A., Hu, M., Shao, M., Zhang, Y., Andreae, M. O., and Pöschl, U.: Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 1: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity, Atmos. Chem. Phys. Discuss., 8, 17343–17392, 2008b.

Rosenfeld, D.: Suppression of rain and snow by urban and industrial air pollution, Science, 287(5459), 1793–1796, 2000.

Rosenfeld, D.: Aerosols, clouds, and climate, Science, 312, 1323–1324, 2006.

Rosenfeld, D., Fromm, M., Trentmann, J., Luderer, G., Andreae, M. O., and Servranckx, R.: The Chisholm firestorm: observed microstructure, precipitation and lightning activity of a pyro-cumulonimbus, Atmos. Chem. Phys., 7, 645–659, 2007.

Rosenfeld, D., Lohmann, U., Raga, G. B., O'Dowd, C. D., Kulmala, M., Fuzzi, S., Reissell, A., and Andreae, M. O., Flood or drought: How do aerosols affect precipitation?, Science, 321, 1309–1313, 2008.

Ruehl, C. R., Chuang, P. Y., and Nenes, A.: How quickly do cloud droplets form on atmospheric particles?, Atmos. Chem. Phys., 8, 1043–1055, 2008.

Segal, Y. and Khain, A.: Dependence of droplet concentration on aerosol conditions in different cloud types: Application to droplet concentration parameterization of aerosol conditions, J. Geophys. Rev., 111, D15204, doi:10.1029/2005JD006561, 2006.

Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics, Wiley & Sons, 2006.

Simmel, M. and Wurzler, S.: Condensation and activation in sectional cloud microphysical models, Atmos. Res., 80, 218–236, 2005.

Simmel, M., Trautmann, T., and Tetzlaff, G.: Numerical solution of the stochastic collection equation – comparison of the Linear Discrete Method with other methods, Atmos. Res., 61, 135–148, 2002.

Su, H., Reutter, P., Trentmann, J., Rose, D., Gunthe, S., Simmel, M., Nowak, A., Wiedensohler, A., Achtert, P., Hu, M., Shao, M., Zhang, Y. H., Zhu, T., and Pöschl, U.: Cloud parcel modelling of CCN activation in megacity air based on observations from Beijing, Geophys. Res. Abstracts, Vol. 11, EGU2009-11107-2, 2009

Trentmann, J., Luderer, G., Winterrath, T., Fromm, M. D., Servranckx, R., Textor, C., Herzog, M., Graf, H.-F., and Andreae, M. O.: Modeling of biomass smoke injection into the lower stratosphere by a large forest fire (Part~I): reference simulation, Atmos. Chem. Phys., 6, 5247–5260, 2006.

Twomey, S.: Atmospheric aerosols, Elsevier Scientific Pub. Co., 320~pp., 1977.

Wang, P. K.: Moisture plumes above thunderstorm anvils and their contributions to cross-tropopause transport of water vapour in midlatitudes, J. Geophys. Res., 108(D6), 4194, doi:10.1029/2002JD002581, 2003.

Wiedensohler, A., Cheng, Y. F., Nowak, A., Wehner, B., Achtert, P., Berghof, M., Birmili, W., Wu, Z. J., Hu, M., Zhu, T., Takegawa, N., Kita, K., Kondo, Y., Lou, S. R., Hofzumahaus, A., Holland, F., Wahner, A., Gunthe, S. S., Rose, D., and Pöschl, U.: Rapid Aerosol Particle Growth and Increase of Cloud Condensation Nucleus (CCN) Activity by Secondary Aerosol Formation: a Case Study for Regional Air Pollution in North Eastern China, J. Geophys. Res., 114, D00G08, doi:10.1029/2008JD010884, 2009.

Zhang, Y. H., Hu, M., Zhong, L. J., Wiedensohler, A., Liu, S. C., Andreae, M. O., Wang, W., and Fan, S. J.: Regional integrated experiments on air quality over Pearl River Delta 2004 (PRIDE-PRD2004): Overview., Atmos. Env., 42(25), 6157–6173, 2008.