Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 10 3 2010 10.5194/acp-10-1227-2010 http://www.atmos-chem-phys.net/10/1227/2010/ http://www.atmos-chem-phys.net/10/1227/2010/acp-10-1227-2010.html http://www.atmos-chem-phys.net/10/1227/2010/acp-10-1227-2010.pdf 1227 1247 2010-02-04 An aerosol chamber investigation of the heterogeneous ice nucleating potential of refractory nanoparticles R. W. Saunders O. Möhler M. Schnaiter S. Benz R. Wagner H. Saathoff P. J. Connolly R. Burgess B. J. Murray M. Gallagher R. Wills J. M. C. Plane j.m.c.plane@leeds.ac.uk School of Chemistry, University of Leeds, Woodhouse Lane, Leeds LS2 9JT, UK Institute for Meteorology and Climate Research, Karlsruhe Institute of Technology (KIT), 76021 Karlsruhe, Germany School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Oxford Road, Manchester M13 9PL, UK Nanoparticles of iron oxide (crystalline and amorphous), silicon oxide and magnesium oxide were investigated for their propensity to nucleate ice over the temperature range 180–250 K, using the AIDA chamber in Karlsruhe, Germany. All samples were observed to initiate ice formation via the deposition mode at threshold ice super-saturations (RHithresh) ranging from 105% to 140% for temperatures below 220 K. Approximately 10% of amorphous Fe2O3 particles (modal diameter = 30 nm) generated in situ from a photochemical aerosol reactor, led to ice nucleation at RHithresh = 140% at an initial chamber temperature of 182 K. Quantitative analysis using a singular hypothesis treatment provided a fitted function [ns(190 K)=10(3.33×sice)+8.16] for the variation in ice-active surface site density (ns:m−2) with ice saturation (sice) for Fe2O3 nanoparticles. This was implemented in an aerosol-cloud model to determine a predicted deposition (mass accommodation) coefficient for water vapour on ice of 0.1 at temperatures appropriate for the upper atmosphere. Classical nucleation theory was used to determine representative contact angles (θ) for the different particle compositions. For the in situ generated Fe2O3 particles, a slight inverse temperature dependence was observed with θ = 10.5° at 182 K, decreasing to 9.0° at 200 K (compared with 10.2° and 11.4° respectively for the SiO2 and MgO particle samples at the higher temperature). These observations indicate that such refractory nanoparticles are relatively efficient materials for the nucleation of ice under the conditions studied in the chamber which correspond to cirrus cloud formation in the upper troposphere. The results also show that Fe2O3 particles do not act as ice nuclei under conditions pertinent for tropospheric mixed phase clouds, which necessarily form above ~233 K. At the lower temperatures (<150 K) where noctilucent clouds form during summer months in the high latitude mesosphere, higher contact angles would be expected, which may reduce the effectiveness of these particles as ice nuclei in this part of the atmosphere. Archuleta, C. M., DeMott, P. J., and Kreidenweis, S. M.: Ice nucleation by surrogates for atmospheric mineral dust/sulphate particles at cirrus temperatures, Atmos. Chem. Phys., 5, 2617–2634, 2005. Baragiola, R. A.: Water ice on outer solar system surfaces: basic properties and radiation effects, Planet Space Sci., 51, 953–961, 2003. Bardeen, C. G., Toon, O. B., Jensen, E. J., Marsh, D. R., and Harvey, V. L.: Numerical simulations of the three-dimensional distribution of meteoric dust in the mesosphere and upper stratosphere, J. Geophys. Res., 113, D17202, doi:10.1029/2007JD009515, 2008. Benz, S., Megahed, K., Möhler, O., Saathoff, H., Wagner, R., and Schurath, U.: T-dependent rate measurements of homogeneous ice nucleation in cloud droplets using a large atmospheric simulation chamber, J. Photochem. Photobiol. A, 176, 208–217, 2005. Biermann, U. M., Presper, T., Koop, T., Mößinger, J., Crutzen, P. J. and Peter, Th.: The unsuitability of meteoritic and other nuclei for polar stratospheric cloud freezing, Geophys. Res. Lett., 23, 1693–1696, 1996. Bigg, E. K. and Giutronich, J.: Ice nucleating properties of meteoritic material, J. Atmos. Sci., 24, 46–49, 1967 Bogdan, A. and Kulmala, M.: Aerosol silica as a possible candidate for the heterogeneous formation of nitric acid hydrates in the stratosphere, Geophys. Res. Lett., 26, 1433–1436, 1999. Bogdan, A.: Fumed silica as a host for study of large surface-to-volume ratio problems in finely divided aqueous systems: Implications for the atmosphere, in: Adsorption on Silica Surfaces, edited by: Papirer, E., Marcel Decker Inc., New York, USA, 689–739, 2000. Choularton, T. W. and Latham, J.: Measurements of the deposition coefficient for ice, and its application to cirrus seeding, Q. J. Roy. Meteorol. Soc., 103, 307–318, 1977. Connolly, P. J., Möhler, O., Field, P. R., Saathoff, H., Burgess, R., Choularton, T., and Gallagher, M.: Studies of heterogeneous freezing by three different desert dust samples, Atmos. Chem. Phys., 9, 2805–2824, 2009. Cotton, R. J., Benz, S., Field, P. R., Möhler, O., and Schnaiter, M.: Technical note: a numerical test-bed for detailed ice nucleation studies in the AIDA cloud simulation chamber, Atmos. Chem. Phys., 7, 243–256, 2007. Curtius, J., Weigel, R., Vossing, H.-J., Wernli, H., Werner, A., Volk, C.-M., Konopka, P., Krebsbach, M., Schiller, C., Roiger, A., Schlager, H., Dreiling, V., and Borrmann, S.: Observations of meteoritic material and implications for aerosol nucleation in the winter Arctic lower stratosphere derived from in-situ particle measurements, Atmos. Chem. Phys., 5, 3053–3069, 2005. Cziczo, D. J., Thomson, D. S., and Murphy, D. M.: Ablation, flux, and atmospheric implications of meteors inferred from stratospheric aerosol, Science, 291, 1772–1775, 2001. Cziczo, D. J., Murphy, D. M., Hudson, P. K. and Thomson, D. S.: Single particle measurements of the chemical composition of cirrus ice residue during CRYSTAL-FACE, J. Geophys. Res.,109, D04201, doi:1029/2003JD004032, 2004. DeCarlo, P. F., Slowik, J. G., Worsnop, D. R., Davidovits, P., and Jimenez, J. L.: Particle morphology and density characterisation by combined mobility and aerodynamic diameter measurements. Part 1: Theory, Aerosol Sci. Technol., 38, 1185–1205, 2004. Dymarska, M., Murray, B. J., Sun, L., Eastwood, M., Knopf, D. A., and Bertram, A. K.: Deposition ice nucleation on soot at temperatures relevant for the lower troposphere, J. Geophys. Res., 111, D04204, doi:10.1029/2005JD006627, 2006. Ebert, V., Teichert, H., Giesemann, C., Saathoff, H., and Schurath, U.: Fibre-coupled in-situ laser absorption spectrometer for the selective detection of water vapour traces down to the ppb-level, Tech. Mess., 72, 23–30, 2005. Evans, L. F.: Requirements of an ice nucleus, Nature, 206, 822 pp., 1965. Farlow, N. H., Ferry, G. V., and Blanchard, M. B.: Examination of surfaces exposed to a noctilucent cloud, August 1, 1968, J. Geophys. Res., 75, 6736–6750, 1970. Field, P. R., Möhler, O., Connolly, P., Krämer, M., Cotton, R., Heymsfield, A. J., Saathoff, H., and Schnaiter, M.: Some ice nucleation characteristics of Asian and Saharan desert dust, Atmos. Chem. Phys., 6, 2991–3006, 2006. Fletcher, N. H.: Size effect in heterogeneous nucleation, J. Chem. Phys., 29, 572–576, 1958. Fletcher, N. H.: On ice-crystal production by aerosol particles, J. Meteorol., 16, 173–180, 1959. Fletcher, N. H.: Active sites and ice crystal nucleation, J. Atmos. Sci., 26, 1266–1271, 1969. Gadsden, M. and Schroder, W.: Noctilucent Clouds, Springer-Verlag, Berlin, Germany, 1989. Gumbel, J. and Witt, G.: Cluster ions and ice particle nucleation: Positive feedback at the summer mesopause, Geophys. Res. Lett., 29, 1782, doi:10.1029/2002GL015146, 2002. Gumbel, J. and Megner, L.: Charged meteoric smoke as ice nuclei in the mesosphere: Part 1. – A review of basic concepts, J. Atmos. Sol.-Terr. Phys., 71, 1225–1235, 2009. Hemenway, C. L., Soberman, R. K., and Witt, G.: Particle sampling from noctilucent clouds, Nature, 199, 269–270, 1963. Hervig, M. E., Gordley, L. L., Deaver, L. E., Siskind, D. E., Stevens, M. H., Russell III, J. M., Bailey, S. M., Megner, L., and Bardeen, C. G.: First satellite observations of meteoric smoke in the middle atmosphere, Geophys. Res. Lett., 36, L18805, doi:10.1029/2009GL039737, 2009. Hoppe, U.-P. and Fritts, D. C.: High-resolution measurements of vertical velocity with the European incoherent scatter VHF radar. 1. Motion field characteristics and measurement biases, J. Geophys. Res., 100D(8), 16813–16825, 1995. Hunten, D. M., Turco, R. P., and Toon, O. B.: Smoke and dust particles of meteoric origin in the mesosphere and stratosphere, J. Atmos. Sci., 37, 1342–1357, 1980. Kärcher, B., Möhler, O., DeMott, P. J., Pechtl, S., and Yu, F.: Insights into the role of soot aerosols in cirrus cloud formation, Atmos. Chem. Phys., 7, 4203–4227, 2007. Keesee, R. G.: Nucleation and particle formation in the upper atmosphere, J. Geophys. Res., 94, 14683–14692, 1989. Köhler, T. M., Gail, H.-P., and Sedlmayr, E.: MgO dust nucleation in M stars: calculation of cluster properties and nucleation rates, Astron. Astrophys., 320, 553–567, 1996. Koop, T., Luo, B., Tsias, A., and Peter, T.: Water activity as the determinant for homogeneous ice nucleation in aqueous solutions, Nature, 406, 611–614, 2000. Kopcewicz, B. and Kopcewicz, M.: Mössbauer study of iron-containing atmospheric aerosols, Struct. Chem., 2, 303–312, 1991. Lanci, L., Kent, D. V., and Biscaye, B. E.: Meteoric smoke concentration in the Vostok ice core estimated from superparamagnetic relaxation and some consequences for estimates of Earth accretion rate, Geophys. Res. Lett., 34, L10803, doi:10.1029/2007GL029811, 2007. Lübken, F.-J.: Thermal structure of the Arctic summer mesosphere, J. Geophys. Res., 104, 9135–9149, 1999. Magee, N., Moyle. A. M., and Lamb, D.: Experimental determination of the deposition coefficient of small cirrus-like ice crystals near −50°C, Geophys. Res. Lett., 33, L17813, doi:10.1029/2006GL026665, 2006. Megner, L., Siskind, D. E., Rapp, M., and Gumbel, J.: Global and temporal distribution of meteoric smoke: A two-dimensional simulation study, J. Geophys. Res., 113, D03202, doi:10.1029/2007JD009054, 2008a. Megner, L., Gumbel J., Rapp, M., and Siskind, D. E.: Reduced meteoric smoke particle density at the summer pole – Implications for mesospheric ice particle nucleation, Adv. Space Res., 41, 41–49, 2008b. Möhler, O., Stetzer, O., Schaefers, S., Linke, C., Schnaiter, M., Tiede, R., Saathoff, H., Krämer, M., Mangold, A., Budz, P., Zink, P., Schreiner, J., Mauersberger, K., Haag, W., Kärcher, B., and Schurath, U.: Experimental investigation of homogeneous freezing of sulphuric acid particles in the aerosol chamber AIDA, Atmos. Chem. Phys., 3, 211–223, 2003. Möhler, O., Büttner, S., Linke, C., Schnaiter, M., Saathoff, H., Stetzer, O., Wagner, R., Krämer, M., Mangold, A., Ebert, V., and Schurath, U.: Effect of sulfuric acid coating on heterogeneous ice nucleation by soot aerosol particles, J. Geophys. Res., 110, D11210, doi:11210.11029/12004JD005169, 2005. Möhler, O., Field, P. R., Connolly, P., Benz, S., Saathoff, H., Schnaiter, M., Wagner, R., Cotton, R., Krämer, M., Mangold, A., and Heymsfield, A. J.: Efficiency of the deposition mode ice nucleation on mineral dust particles, Atmos. Chem. Phys., 6, 3007–3021, 2006. Möhler, O., Benz, S., Saathoff, H., Schnaiter, M., Wagner, R., Schneider, J., Walter, S., Ebert, V., and Wagner, S.: The effect of organic coating on the heterogeneous ice nucleation efficiency of mineral dust aerosols, Environ. Res. Lett., 3, 1–8, 2008. Mossop, S. C.: Stratospheric particles at 20 km, Nature, 199, 325–326, 1963. Murphy, D. M., Thomson, D. S., and Mahoney, M. J.: In situ measurements of organics, meteoritic material, mercury, and other elements in aerosols at 5~to 19~kilometers, Science, 282, 1664–1669, 1998. Murphy, D. M. and Koop, T.: Review of the vapour pressures of ice and supercooled water for atmospheric applications, Q. J. Roy. Meteorol. Soc., 131, 1539–1565, 2005. Murray, B. J., Knopf, D. A., and Bertram, A. K.: The formation of cubic ice under conditions relevant to the Earth's atmosphere, Nature, 434, 202–205, 2005. Murray, B. J. and Jensen, E. J.: Homogeneous nucleation of amorphous solid water particles in the upper mesosphere, J. Atmos. Sol.-Terr. Phys., 72, 51–61, 2010. Murray, B. J., Bull, S., Wilson, T. W., and Wills, R.: Heterogeneous ice nucleation by illite clay under conditions relevant for the Earth's atmosphere, in preparation, 2010. Park, G.-S., Shindo, D., Waseda, Y., and Sugimoto, T.: Internal structure analysis of monodispersed pseudocubic hematite particles by electron microscopy, J. Colloid Interf. Sci., 177, 198–207, 1996. Plane, J. M. C. and Helmer, M.: Laboratory study of the reactions Mg + O3 and MgO + O3: Implications for the chemistry of magnesium in the upper atmosphere, Faraday Discuss., 100, 411–430, 1995. Plane, J. M. C.: The role of sodium bicarbonate in the nucleation of noctilucent clouds, Ann. Geophys., 18, 807–814, 2000. Pruppacher, H. R. and Klett, J. D.: Microphysics of Clouds and Precipitation, Kluwer Academic Publishers, Dordrecht, The Netherlands, 1997. Rapp, M. and Lübken, F.-J.: Polar mesosphere summer echoes (PMSE): review of observations and current understanding, Atmos. Chem. Phys., 4, 2601–2633, 2004. Rapp, M., Hedin, J., Strelnikova, I., Friedrich, M., Gumbel, J., and Lübken, F.-J.: Observations of positively charged nanoparticles in the nighttime polar mesosphere, Geophys. Res. Lett., 32, L23821, doi:10.1029/2005GL024676, 2005. Rapp, M. and Thomas, G. E.: Modeling the microphysics of mesospheric ice particles: assessment of current capabilities and basic sensitivities, J. Atmos. Sol.-Terr. Phys., 68, 715–744, 2006. Rapp, M.: Charging of mesospheric aerosol particles: the role of photodetachment and photoionization from meteoric smoke and ice particles, Ann. Geophys., 27, 2417–2422, 2009. Reid, G. C.: The nucleation and growth of ice particles in the upper mesosphere, Adv. Space Res., 20, 1285–1291, 1997. Roddy, A. F.: Role of meteoric particles in noctilucent clouds, Irish Astron. J., 16, 194–202, 1984. Rosinski, J. and Snow, R. H.: Secondary particulate matter from meteor vapors, J. Meteorol., 18, 736–745, 1961. Saunders, R. W. and Plane, J. M. C.: A laboratory study of meteor smoke analogues; composition, optical properties and growth kinetics, J. Atmos. Sol.-Terr. Phys., 68, 2182–2202, 2006. Seele, C. and Hartogh, P.: Water vapour of the polar middle atmosphere: annual variation and summer mesosphere conditions as observed by ground-based microwave spectroscopy, Geophys. Res. Lett., 26, 1517–1520, 1999. Seifert, M., Tiede, R., Schnaiter, M., Linke, C., Möhler, O., Schurath, U., and Ström, J.: Operation and performance of a differential mobility particle sizer and a TSI 3010 condensation particle counter at stratospheric temperatures and pressures, J. Aero. Sci., 35, 981–993, 2004. Shilling, J. E., Tolbert, M. A., Toon, O. B., Jensen, E. J., Murray, B. J., and Bertram, A. K.: Measurements of the vapour pressure of cubic ice and their implications for atmospheric ice clouds, Geophys. Res. Lett., 33, L17801, doi:10.1029/2006GL026671, 2006. Strelnikova, I., Rapp, M., Raizada, S., and Sulzer, M.: Meteor smoke particle properties derived from Arecibo incoherent scatter radar observations, Geophys. Res. Lett., 34, L15815, doi:10.1029/2007GL030635, 2007. Sugimoto, T. and Sakata, K.: Preparation of monodisperse pseudocubic $\alpha $-Fe2O3 particles from condensed ferric hydroxide gel, J. Colloid Interf. Sci., 152, 587–590, 1992. Trainer, M. G., Toon, O. B., and Tolbert, M. A.: Measurements of depositional ice nucleation on insoluble substrates at low temperatures: Implications for Earth and Mars, J. Phys. Chem. C, 113, 2036–2040, 2009. Turco, R. P., Toon, R. B., Hamill, P., and Whitten, R. C.: Effects of meteoric debris on stratospheric aerosols and gases, J. Geophys. Res., 86, 1113–1128, 1981. von Zahn, U. and Meyer, W.: Mesopause temperatures in polar summer, J. Geophys. Res., 94, 14647–14651, 1989. von Cossart, G., Fiedler, J., and von Zahn, U.: Size distributions of NLC particles as determined from 3-color observations of NLC by ground-based lidar, Geophys. Res. Lett., 26, 1513–1516, 1999. Vondrak, T., Plane, J. M. C., Broadley, S., and Janches, D.: A chemical model of meteoric ablation, Atmos. Chem. Phys., 8, 7015–7031, 2008. Wagner, R., Benz, S., Möhler, O., Saathoff, H., and Schurath, U.: Probing ice clouds by broadband mid-infrared extinction spectroscopy: Case studies from ice nucleation experiments in the AIDA aerosol and cloud chamber, Atmos. Chem. Phys., 6, 4775–4800, 2006. Wagner, R., Benz, S., Möhler, O., Saathoff, H., Schnaiter, M., and Leisner, T.: Influence of particle aspect ratio on the mid infrared extinction spectra of wavelength-sized ice crystals, J. Phys. Chem. A, 111, 13003–13022, 2007. Whalley, E.: Cubic ice in nature, J. Phys. Chem., 87, 4174–4179, 1983. Zasetsky, A. Y., Petelina, S. V., and Svishchev, I. M.: Thermodynamics of homogeneous nucleation of ice particles in the polar summer mesosphere, Atmos. Chem. Phys., 9, 965–971, 2009. Zondlo, M. A., Hudson, P. K., Prenni, A. J. and Tolbert, M. A.: Chemistry and microphysics of polar stratospheric clouds and cirrus clouds, Annu. Rev. Phys. Chem., 51, 473–499, 2000.