References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-12-11435-2012

Relationships between particles, cloud condensation nuclei and cloud droplet activation during the third Pallas Cloud Experiment

Anttila

¹ Brus

¹ Jaatinen

² Hyvärinen

A.-P.

¹ Kivekäs

¹ Romakkaniemi

² Komppula

³ Lihavainen

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

University of Eastern Finland, Kuopio Campus, Department of applied physics, P.O. Box 1627, 70211 Kuopio, Finland

Finnish Meteorological Institute, Kuopio Unit, P.O. Box 1627, 70211 Kuopio, Finland

03 12 2012

12 23 11435 11450

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/12/11435/2012/acp-12-11435-2012.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/11435/2012/acp-12-11435-2012.pdf

Concurrent measurement of aerosols, cloud condensation nuclei (CCN) and cloud droplet activation were carried out as a part of the third Pallas Cloud Experiment (PaCE-3) which took place at a ground based site located on northern Finland during the autumn of 2009. In this study, we investigate relationships between the aerosol properties, CCN and size resolved cloud droplet activation. During the investigated cloudy periods, the inferred number of cloud droplets (CDNC) varied typically between 50 and 150 cm−3 and displayed a linear correlation both with the number of particles having sizes over 100 nm and with the CCN concentrations at 0.4% supersaturation. Furthermore, the diameter corresponding to the 50% activation fraction, D50, was generally in the range of 80 to 120 nm. The measured CCN concentrations were compared with predictions of a numerical model which used the measured size distribution and size resolved hygroscopicity as input. Assuming that the droplet surface tension is equal to that of water, the measured and predicted CCN concentrations were generally within 30%. We also simulated size dependent cloud droplet activation with a previously developed air parcel model. By forcing the model to reproduce the experimental values of CDNC, adiabatic estimates for the updraft velocity and the maximum supersaturation reached in the clouds were derived. Performed sensitivity studies showed further that the observed variability in CDNC was driven mainly by changes in the particle size distribution while the variations in the updraft velocity and hygroscopicity contributed to a lesser extent. The results of the study corroborate conclusions of previous studies according to which the number of cloud droplets formed in clean air masses close to the Arctic is determined mainly by the number of available CCN.

References 1

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, 2008.

Anttila,~T., Vaattovaara,~P., Komppula,~M., Hyvärinen,~A.-P., Lihavainen,~H., Kerminen,~V.-M. and Laaksonen,~A.: Size-dependent activation of aerosols into cloud droplets at a subarctic background site during the second Pallas Cloud Experiment (2nd PaCE): method development and data evaluation, Atmos. Chem. Phys., 9, 4841–4854, http://dx.doi.org/10.5194/acp-9-4841-2009doi:10.5194/acp-9-4841-2009, 2009.

Anttila, T.: Sensitivity of cloud droplet formation to the numerical treatment of the particle mixing state, \textitJ. Geophys. Res., 115, D21205, http://dx.doi.org/10.1029/2010JD013995doi:10.1029/2010JD013995, 2010.

Barahona, D., and Nenes, A.: Parameterization of cloud droplet formation in large-scale models: Including effects of entrainment,J. Geophys. Res., 112, D16206, http://dx.doi.org/10.1029/2007JD008473doi:10.1029/2007JD008473, 2007.

Bilde, M. and Svenningsson, B.: CCN activation of slightly soluble organics: the importance of small amounts of inorganic salt and particle phase, Tellus B, 56, 128–134, 2004.

Conant, W. C., VanReken, T. M., Rissman, T. A., Varutbangkul, V., Jonsson, H. H., Nenes, A., Jimenez, J. L., Delia, A. E., Bahreini, R., Roberts, G. C., Flagan, R. C., and Seinfeld, J. H.: Aerosol–cloud drop concentration closure in warm cumulus, J. Geophys. Res., 109, D13204, http://dx.doi.org/10.1029/2003JD004324doi:10.1029/2003JD004324, 2004.

DeCarlo, P. F., Kimmel, J. R., Trimborn, A., Northway, M. J., Jayne, J. T., Aiken, A. C., Gonin, M., Fuhrer, K., Horvath, T., Docherty, K., Worsnop, D. R. and Jimenez, J. L.: Field-Deployable, High-Resolution, Time-of-Flight Aerosol Mass Spectrometer, Anal. Chem., 78, 8281–8289, 2006.

Draxler, R. R. and Rolph, G. D.: HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory) Model access via NOAA ARL READY Website (http://ready.arl.noaa.gov/HYSPLIT.php), NOAA Air Resources Laboratory, Silver Spring, MD, USA, 2012.

Duplissy, J., Gysel, M., Sjogren, S., Meyer, N., Good, N., Kammermann, L., Michaud, V., Weigel, R., Martins dos Santos, S., Gruening, C., Villani, P., Laj, P., Sellegri, K., Metzger, A., McFiggans, G. B., Wehrle, G., Richter, R., Dommen, J., Ristovski, Z., Baltensperger, U., and Weingartner, E.: Intercomparison study of six HTDMAs: results and recommendations, Atmos. Meas. Tech., 2, 363–378, http://dx.doi.org/10.5194/amt-2-363-2009doi:10.5194/amt-2-363-2009, 2009.

Dusek, U., Frank, G. P., Hildebrandt, L., Curtius, J., Schneider, J., Walter, S., Chand, D., Drewnick, F., Hings, S., Jung, D., Borrmann, S., and Andreae, M.O.: Size matters more than chemistry for cloud-nucleating ability of aerosol particles, Science, 312, 1375–1378, 2006.

Forster, P., Ramaswamy, V., Artaxo, P., Berntsen, T., Betts, R., Fahey, D. W., Haywood, J., Lean, J., Lowe, D. C., Myhre, G., Nganga, J., Prinn, R., Raga, G., Schulz, M., and Van Dorland, R.: Changes in Atmospheric Constituents and in Radiative Forcing. 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.

Fountoukis, C., Nenes, A., Meskhidze, N., Bahreini, R., Conant, W. C., Jonsson, H., Murphy, S., Sorooshian, A., Varutbangkul, V., Brechtel, F., Flagan, R. C., and Seinfeld, J. H.: Aerosol-cloud drop concentration closure for clouds sampled during the International Consortium for Atmospheric Research on Transport and Transformation 2004 campaign, J. Geophys Res., 112, D10S30, http://dx.doi.org/10.1029/2006JD007272doi:10.1029/2006JD007272, 2007.

Ghan, S. J. and Schwartz, S. E.: Aerosol properties and processes – A path from field and and laboratory measurements to global climate models, B. Am. Meteorol. Soc., 88, 1059–1083, 2007.

Ghan, S. J., Abdul-Razzak, H., Nenes, A., Ming, Y., Liu, X., Ovchinnikov, M., Shipway, B., Meskhidze, N., Xu, J., and Shi, X.: Droplet nucleation: Physically-based parameterizations and comparative evaluation, J. Adv. Model. Earth Syst., 3, M10001, http://dx.doi.org/10.1029/2011MS000074doi:10.1029/2011MS000074, 2011.

Gillani, N. V., Schwartz, S. E., Leaitch, W. R., Strapp, J. W. and Isaac, G. A.: Field observations in continental stratiform clouds: Partitioning of cloud particles between droplets and unactivated interstitial aerosols, J. Geophys. Res., 100, 18687–18706, http://dx.doi.org/10.1029/95JD01170doi:10.1029/95JD01170, 1995.

Gysel, M., McFiggans, G. B., and Coe, H.: Inversion of tandem differential mobility analyser (TDMA) measurements, J. Aerosol Sci., 40, 134–151, http://dx.doi.org/10.1016/j.jaerosci.2008.07.013doi:10.1016/j.jaerosci.2008.07.013, 2009.

Hatakka, J., Aalto, T., Aaltonen, V., Aurela, M., Hakola, H., Komppula, M., Laurila, T., Lihavainen, H., Paatero, J., Salminen, K., and Viisanen, Y.: Overview of the atmospheric research activities and results at Pallas GAW station, Boreal Environ. Res., 8, 365–384, 2003.

Henning, S., Weingartner, E., Schmidt, S., Wendisch, M., Gäggeler, H. W., and Baltensperger, U.: Size-dependent aerosol activation at the high-alpine site Jungfraujoch (3580 m asl), Tellus, 54B, 82–95, 2002.

Hu, Y., Rodier, S., Xu, K., Sun, W., Huang, J., Lin, B., Zhai, P., and Josset, D.: Occurrence, liquid water content, and fraction of supercooled water clouds from combined CALIOP/IIR/MODIS measurements, J. Geophys. Res., 115, D00H34, http://dx.doi.org/10.1029/2009JD012384doi:10.1029/2009JD012384, 2010.

Hudson, J. G.: Variability of the relationship between particle size and cloud-nucleating ability, Geophys. Res. Lett., 34, L08801, http://dx.doi.org/10.1029/2006GL028850doi:10.1029/2006GL028850, 2007.

Hudson, J. G., Noble, S., and Jha, V.: Stratus cloud supersaturations, Geophys. Res. Lett., 37, L21813, http://dx.doi.org/10.1029/2010GL045197doi:10.1029/2010GL045197, 2010.

Jaatinen, A., Hyvärinen, A.-P., Romakkaniemi, S., Hao, L., Kortelainen, A., Miettinen, P., Komppula, M., Leskinen, A., Anttila, T., Smith, J. N., and Laaksonen, A.: The 3rd Pallas Cloud Experiment: consistency between the hygroscopic growth and CCN activity parameterisations, in preparation, 2012.

Jurányi, Z., Gysel, M., Weingartner, E., DeCarlo, P. F., Kammermann, L., and Baltensperger, U.: Measured and modelled cloud condensation nuclei number concentration at the high alpine site Jungfraujoch, Atmos. Chem. Phys., 10, 7891–7906, http://dx.doi.org/10.5194/acp-10-7891-2010doi:10.5194/acp-10-7891-2010, 2010.

Kammermann, L., Gysel, M., Weingartner, W., Herich, H., Cziczo, D.J., Holst, T., Svenningsson, B., Arneth, A., and Baltensperger, U.: Subarctic atmospheric aerosol composition: 3. Measured and modeled properties of cloud condensation nuclei, J. Geophys. Res., 115, D04202, http://dx.doi.org/10.1029/2009JD012447doi:10.1029/2009JD012447, 2010.

Kivekäs, N., Kerminen, V.-M., Raatikainen, T., Vaattovaara, P., and Lihavainen, H.: Physical and chemical characteristics of the activating particles during the Second Pallas Cloud Experiment (Second PaCE), Boreal. Environ. Res., 14, 515–526, 2009.

Kleinman, L. I., Daum, P. H., Lee, Y.-N., Lewis, E. R., Sedlacek III, A. J., Senum, G. I., Springston, S. R., Wang, J., Hubbe, J., Jayne, J., Min, Q., Yum, S. S., and Allen, G.: Aerosol concentration and size distribution measured below, in, and above cloud from the DOE G-1 during VOCALS-REx, Atmos. Chem. Phys., 12, 207–223, http://dx.doi.org/10.5194/acp-12-207-2012doi:10.5194/acp-12-207-2012, 2012.

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, http://dx.doi.org/10.1029/2004JD005200doi:10.1029/2004JD005200, 2005.

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, http://dx.doi.org/10.5194/acp-5-461-2005doi:10.5194/acp-5-461-2005, 2005

Levin, E. J. T., Prenni, A. J., Petters, M. D., Kreidenweis, S. M., Sullivan, R. C., Atwood, S. A., Ortega, J., DeMott, P. J., and Smith, J. N.: An annual cycle of size-resolved aerosol hygroscopicity at a forested site in Colorado, J. Geophys. Res., 117, D06201, http://dx.doi.org/10.1029/2011JD016854doi:10.1029/2011JD016854, 2012.

Lihavainen,~H., Kerminen,~V.-M., Komppula,~M., Hyvärinen,~A.-P., Laakia,~J., Saarikoski,~S., Makkonen,~U., Kivekäs,~N., Hillamo,~R., Kulmala,~M., and Viisanen,~Y.: Measurements of the relation between aerosol properties and microphysics and chemistry of low level liquid water clouds in Northern Finland, Atmos. Chem. Phys., 8, 6925–6938, http://dx.doi.org/10.5194/acp-8-6925-2008doi:10.5194/acp-8-6925-2008, 2008.

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, http://dx.doi.org/10.5194/acp-6-2593-2006doi:10.5194/acp-6-2593-2006, 2006.

Mertes, S., Lehmann, K., Nowak, A., Massling, A., and Wiedensohler, A.:. Link between aerosol hygroscopic growth and droplet activation observed for hill-capped clouds at connected flow conditions during FEBUKO, Atmos. Environ., 39, 4247–4256, 2005.

Meskhidze, N., Nenes, A., Conant, W. C., and Seinfeld, J. H.: Evaluation of a new cloud droplet activation parameterization with in situ data from CRYSTAL-FACE and CSTRIPE, J. Geophys. Res., 110, D16202, http://dx.doi.org/10.1029/2004JD005703doi:10.1029/2004JD005703, 2005.

Morales, R., Nenes, A., Jonsson, H., Flagan, R. C., and Seinfeld, J. H.: Evaluation of an entraining droplet activation parameterization using in situ cloud data,J. Geophys. Res., 116, D15205, http://dx.doi.org/10.1029/2010JD015324doi:10.1029/2010JD015324, 2011.

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, Ser. B, 53, 133–149, 2001.

Noone, K. J., Ogren, J. A., Hallberg, A., Heintzenberg, J., Ström, J., Hansson, H.-C., Svenningsson, I. B., Wiedensohler, A., Fuzzi, S., Facchini, M. C., Arends, B. G., and Berner, A.: Changes in aerosol size- and phase distributions due to physical and chemical processes in fog, Tellus B 44, 489–504, 1992.

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, http://dx.doi.org/10.5194/acp-6-3391-2006doi:10.5194/acp-6-3391-2006, 2006.

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, http://dx.doi.org/10.5194/acp-7-1961-2007doi:10.5194/acp-7-1961-2007, 2007.

Quinn, P. K., Bates, T. S., Coffman, D. J., and Covert, D. S.: In?uence of particle size and chemistry on the cloud nucleating properties of aerosols, Atmos. Chem. Phys., 8, 1029–1042, http://dx.doi.org/10.5194/acp-8-1029-2008doi:10.5194/acp-8-1029-2008, 2008.

Reutter, P., Su, H., Trentmann, J., Simmel, M., Rose, D., Gunthe, S. S., Wernli, H., Andreae, M. O., and Pöschl, U.: Aerosol- and updraft-limited regimes of cloud droplet formation: influence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN), Atmos. Chem. Phys., 9, 7067–7080, http://dx.doi.org/10.5194/acp-9-7067-2009doi:10.5194/acp-9-7067-2009, 2009.

Roberts, G. C. and Nenes, A.: A continuous-flow streamwise thermal gradient CCN chamber for atmospheric measurements, Aerosol Sci. Tech., 39, 206–221, 2005.

Rogers, R. R. and Yau, M. K., A Short Course in Cloud Physics, Pergamon, Tarrytown, NY, USA, 393 pp., 1989.

Romakkaniemi, S., McFiggans, G., Bower, K. N., Brown, P., Coe, H., and Choularton, T. W.: A comparison between trajectory ensemble and adiabatic parcel modeled cloud properties and evaluation against airborne measurements, J. Geophys. Res., 114, D06214, http://dx.doi.org/10.1029/2008JD011286doi:10.1029/2008JD011286, 2009.

Ruehl, C. R., Chuang, P. Y., and Nenes, A.: Aerosol hygroscopicity at high (99 to 100 %) relative humidities, Atmos. Chem. Phys., 10, 1329–1344, http://dx.doi.org/10.5194/acp-10-1329-2010doi:10.5194/acp-10-1329-2010, 2010.

Snider, J. R. and Brenguier, J. L.: Cloud condensation nuclei and cloud droplet measurements during ACE-2, Tellus B, 52, 828–848, 2000.

Snider, J. R., Guibert, S., Brenguier, J.-L., and Putaud, J.-P.: Aerosol activation in marine stratocumulus clouds: 2. Köhler and parcel theory closure studies, J. Geophys. Res., 108, 8629, http://dx.doi.org/10.1029/2002JD002692doi:10.1029/2002JD002692, 2003.

Svenningsson, B., Hansson, H.-C., Wiedensohler, A., Noone, K. J., Ogren, J. A., Hallberg, A., and Colvile, R.: Hygroscopic growth of aerosol particles and its influence on nucleation scavenging in cloud: experimental results from Kleiner Feldberg, J. Atmos. Chem., 19,129–151, 1994.

Svenningsson, B., Hansson, H.-C., Martinsson, B., Wiedensohler, A., Swietlicki, E., Cederfelt, S.-I., Wendisch, M., Bower, K. N., Choularton, T. W., and Colvile, R. N.: Cloud droplet nucleation scavenging in relation to the size and hygroscopic behaviour of aerosol particles, Atmos. Environ., 31, 2463–2475, 1997.

Twohy, C. H., Petters, M. D., Snider, J. R., Stevens, B., Tahnk, W., Wetzel, M., Russell, 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, http://dx.doi.org/10.1029/2004JD005116doi:10.1029/2004JD005116, 2005.

Verheggen, B., Cozic, J., Weingartner, E., Bower, K., Mertes, S., Connolly, P., Gallagher, M., Flynn, M., Choularton, T., and Baltensperger, U.: Aerosol partitioning between the interstitial and condensed phase in mixed-phase clouds, J. Geophys. Res., 112, D23202, http://dx.doi.org/10.1029/2007JD008714doi:10.1029/2007JD008714, 2007.

Wex, H., Stratmann, F., Hennig, T., Hartmann, S., Niedermeier, D., Nilsson, E., Ocskay, R., Rose, D., Salma, I., and Ziese, M.: Connecting hygroscopic growth at high humidities to cloud activation for different particle types, Environ. Res. Lett., 3, 035004, http://dx.doi.org/10.1088/1748-9326/3/3/035004doi:10.1088/1748-9326/3/3/035004, 2008.

Wiedensohler, A., Birmili, W., Nowak, A., Sonntag, A., Weinhold, K., Merkel, M., Wehner, B., Tuch, T., Pfeifer, S., Fiebig, M., Fjäraa, A. M., Asmi, E., Sellegri, K., Depuy, R., Venzac, H., Villani, P., Laj, P., Aalto, P., Ogren, J. A., Swietlicki, E., Williams, P., Roldin, P., Quincey, P., Hüglin, C., Fierz-Schmidhauser, R., Gysel, M., Weingartner, E., Riccobono, F., Santos, S., Grüning, C., Faloon, K., Beddows, D., Harrison, R., Monahan, C., Jennings, S. G., O'Dowd, C. D., Marinoni, A., Horn, H.-G., Keck, L., Jiang, J., Scheckman, J., McMurry, P. H., Deng, Z., Zhao, C. S., Moerman, M., Henzing, B., de Leeuw, G., Löschau, G., and Bastian, S.: Mobility particle size spectrometers: harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions, Atmos. Meas. Tech., 5, 657–685, http://dx.doi.org/10.5194/amt-5-657-2012doi:10.5194/amt-5-657-2012, 2012.

Yum, S. S., Hudson, J. G., and Xie, Y.: Comparisons of cloud microphysics with cloud condensation nuclei spectra over the summertime Southern Ocean, J. Geophys. Res., 103, 16625–16636, http://dx.doi.org/10.1029/98JD01513doi:10.1029/98JD01513, 1998.