Chemical composition and mixing-state of ice residuals sampled within mixed phase clouds
10.5194/acp-11-2805-2011
Crossref journal-article
Copernicus GmbH
Atmospheric Chemistry and Physics (3145)
Abstract

Abstract. During an intensive campaign at the high alpine research station Jungfraujoch, Switzerland, in February/March 2006 ice particle residuals within mixed-phase clouds were sampled using the Ice-counterflow virtual impactor (Ice-CVI). Size, morphology, chemical composition, mineralogy and mixing state of the ice residual and the interstitial (i.e., non-activated) aerosol particles were analyzed by scanning and transmission electron microscopy. Ice nuclei (IN) were identified from the significant enrichment of particle groups in the ice residual (IR) samples relative to the interstitial aerosol. In terms of number lead-bearing particles are enriched by a factor of approximately 25, complex internal mixtures with silicates or metal oxides as major components by a factor of 11, and mixtures of secondary aerosol and carbonaceous material (C-O-S particles) by a factor of 2. Other particle groups (sulfates, sea salt, Ca-rich particles, external silicates) observed in the ice-residual samples cannot be assigned unambiguously as IN. Between 9 and 24% of all IR are Pb-bearing particles. Pb was found as major component in around 10% of these particles (PbO, PbCl2). In the other particles, Pb was found as some 100 nm sized agglomerates consisting of 3–8 nm sized primary particles (PbS, elemental Pb). C-O-S particles are present in the IR at an abundance of 17–27%. The soot component within these particles is strongly aged. Complex internal mixtures occur in the IR at an abundance of 9–15%. Most IN identified at the Jungfraujoch station are internal mixtures containing anthropogenic components (either as main or minor constituent), and it is concluded that admixture of the anthropogenic component is responsible for the increased IN efficiency within mixed phase clouds. The mixing state appears to be a key parameter for the ice nucleation behaviour that cannot be predicted from the sole knowledge of the main component of an individual particle.

Bibliography

Ebert, M., Worringen, A., Benker, N., Mertes, S., Weingartner, E., & Weinbruch, S. (2011). Chemical composition and mixing-state of ice residuals sampled within mixed phase clouds. Atmospheric Chemistry and Physics, 11(6), 2805–2816.

Authors 6
  1. M. Ebert (first)
  2. A. Worringen (additional)
  3. N. Benker (additional)
  4. S. Mertes (additional)
  5. E. Weingartner (additional)
  6. S. Weinbruch (additional)
References 66 Referenced 46
  1. Adachi, K., Chung, S. H., and Buseck, P. R.: Shapes of soot aerosol particles and implications for their effects on climate, J. Geophys. Res., 115, D15206, https://doi.org/10.1029/2009JD012868, 2010. (10.1029/2009JD012868)
  2. Batonneau, Y, Bremard, C., Gengembre, L., Laureyns, J., Le Maguer, A., Le Maguer, D., Perdrix, E., and Sobanska, S.: Speciation of PM10 sources of airborne nonferrous metals within the 3-km zone of lead/zinc smelters, Environ. Sci. Technol., 38, 5281–5289, 2004. (10.1021/es0497173)
  3. Beard, K. V.: Ice initiation in warm-base convective clouds: An assessment of microphysical mechanisms, Atmos. Res., 28, 125–152, 1992. (10.1016/0169-8095(92)90024-5)
  4. Bingemer, H. G., Klein, H., Ebert, M., Haunold, W., Bundke, U., Herrmann, T., Kandler, K., Müller-Ebert, D., Weinbruch, S., and Curtius, J.: Enhanced atmospheric ice nuclei in the Eyjafjallajökull volcanic ash plume over central Europe, in review, 2011. (10.5194/acpd-11-2733-2011)
  5. Cantrell, W. and Heymsfield, A.: Production of ice in tropospheric clouds, Bull. Am. Meteorol. Soc., 86, 795–807, 2005. (10.1175/BAMS-86-6-795)
  6. Chen, Y., Kreidenweis, S. M., McInnes, L. M., Rogers, D. C., and DeMott, P. J.: Single particle analyses of ice nucleating aerosols in the upper troposphere and lower stratosphere, Geophys. Res. Lett., 25, 1391–1394, https://doi.org/10.1029/97GL03261, 1998. (10.1029/97GL03261)
  7. Choel, M., Deboudt, K., Flament, P., Lecornet, G., Perdrix, E., and Sobanska, S.: Fast evolution of tropospheric Pb- and Zn-rich particles in the vicinity of a lead smelter, Atmos. Environ., 40, 4439–4449, 2006. (10.1016/j.atmosenv.2006.04.027)
  8. Cozic, J., Mertes, S., Verheggen, B., Cziczo, D. J., Gallavardin, S.J., Walter, S., Baltensperger, U., and Weingartner, E.: Black carbon enrichment in atmospheric ice particle residuals observed in lower tropospheric mixed phase clouds, J. Geophys. Res., 113, D15209, https://doi.org/10.1029/2007JD009266, 2008. (10.1029/2007JD009266)
  9. 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, https://doi.org/10.1029/2003JD004032, 2004. (10.1029/2003JD004032)
  10. Cziczo, D. J., Stetzer, O, Worringen, A., Ebert, M., Weinbruch, S., Kamphus, M., Gallavardin, S. J., Curtius, J., Bormann, S., Froyd, K. D., Mertes, S., Möhler, O., and Lohmann, U.: Inadvertent Climate Modification Due to Anthropogenic Lead, Nature Geosci., 2, 333–336, 2009. (10.1038/ngeo499)
  11. DeMott, P. J., Cziczo, D. J., Prenni, A. J., Murphy, D. M., Kreidenweis, S. M., Thomson, D. S., Borys, R., and Rogers, D. C.: Measurements of the concentration and composition of nuclei for cirrus formation, Proc. Natl. Acad. Sci. USA, 100, 14655–14660, 2003a. (10.1073/pnas.2532677100)
  12. DeMott, P. J., Sassen, K., Poellot, M. R., Baumgardner, D., Rogers, D. C., Brooks, S. D., Prenni, A. J., and Kreidenweis, S. M.: African dust aerosols as atmospheric ice nuclei Geophys. Res. Lett., 30, 1732, https://doi.org/10.1029/2003GL017410, 2003b. (10.1029/2003GL017410)
  13. Draxler, R., and Rolph, G.D.: HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory) Model access via NOAA ARL READY Website http://www.arl.noaa.gov/ready/hysplit4.htmlS, NOAA Air Resources Laboratory, Silver Spring, MD, 2003.
  14. Durant, A. J., Shaw, R. A., Rose, W. I., Mi, Y. and Ernst, G. G. J.: Ice nucleation and overseeding of ice in volcanic clouds, J. Geophys. Res., 113, D09206, https://doi.org/10.1029/2007JD009064, 2008. (10.1029/2007JD009064)
  15. Eastwood, M. L., Cremel, S., Gehrke, C., Girard, E., and Bertram, A. K.: Ice nucleation on mineral dust particles: Onset conditions, nucleation rates and contact angles, J. Geophys. Res., 113, D22203, https://doi.org/10.1029/2008JD010639, 2008. (10.1029/2008JD010639)
  16. Ebert, M., Weinbruch, S., Rausch, A., Gorzawski, G., Hoffmann, P., Wex, H., and Helas, G.: The complex refractive index of aerosols during LACE 98 as derived from the analysis of individual particles, J. Geophys. Res., 107(D21), 8121, https://doi.org/10.1029/2000JD000195, 2002a. (10.1029/2000JD000195)
  17. Ebert, M., Inerle-Hof, M., and Weinbruch, S.: Environmental scanning electron microscopy as a new technique to determine the hygroscopic behaviour of individual aerosol particles, Atmos. Environ., 36, 5909–5916, 2002b. (10.1016/S1352-2310(02)00774-4)
  18. Ebert, M., Weinbruch, S., Hoffmann, P., and Ortner, H. M.: Chemical Characterization of North Sea Aerosol Particles by Total Reflection X-Ray Fluorescence Analysis and High-Resolution Scanning Electron Microscopy, J. Aerosol Sci., 31, 613–632, 2000c. (10.1016/S0021-8502(99)00549-2)
  19. Ebert, M., Weinbruch, S., Hoffmann, P., and Ortner, H. M.: The chemical characterization and complex refractive index of rural and urban influenced aerosols determined by individual particle analysis, Atmos. Environ., 38, 6531–6545, 2004. (10.1016/j.atmosenv.2004.08.048)
  20. Ebert, M., Worringen, A., Inerle-Hof, M., Benker, N., and Weinbruch, S.: Identification of the ice forming fraction of the atmospheric aerosol in mixed-phase clouds by environmental scanning electron microscopy, Activity Report 2005/2006 International Foundation High Altitude Research Stations JG, Bern Switzerland, 105–112, 2006.
  21. Eidhammer, T., DeMott, P. J., and Kreidenweis, S. M.: A comparison of heterogeneous ice nucleation parameterizations using a parcel model framework, J. Geophys. Res., 114, D06202, https://doi.org/10.1029/2008JD011095, 2009. (10.1029/2008JD011095)
  22. Environmental Protection Agency. Latest findings on National Air Quality, 2002 Status and Trends (US Environmental Protection Agency, 2003); available at: http://www.epa.gov/air/airtrends/aqtrnd02/2002_airtrends_final.pdf, 2002.
  23. Grant, L. O. and Corrin, M. L.: Raw and iodine-treated automobile exhaust as a source of ice nuclei, J. Weather Modification, 5, 238–248, 2001.
  24. Hinz, K.-P., Trimborn, A., Weingartner, E., Henning, S., Baltensberger, U., and Spengler, B.: Aerosol single particle composition at the Jungfraujoch, Aerosol Sci., 36, 123–145, 2005. (10.1016/j.jaerosci.2004.08.001)
  25. Hobbs, P. V., Fullerton, M., and Bluhm, G.: Ice nucleus "storms" in Hawaii, Nature Physical Science, 230, 90–91, 1971. (10.1038/physci230090a0)
  26. Hoose, C.: Biological Ice formation, Nature Geosci., 2, 385–386, 2009. (10.1038/ngeo530)
  27. Isono, K., Komabayasi, M., and Ono, A.: Volcanoes as a sources of atmospheric ice nuclei, Nature, 183, 317–319, 1959. (10.1038/183317a0)
  28. Kamphus, M., Ettner-Mahl, M., Klimach, T., Drewnick, F., Keller, L., Cziczo, D. J., Mertes, S., Borrmann, S., and Curtius, J.: Chemical composition of ambient aerosol, ice residues and cloud droplet residues in mixed-phase clouds: single particle analysis during the Cloud and Aerosol Characterization Experiment (CLACE 6), Atmos. Chem. Phys., 10, 8077–8095, https://doi.org/10.5194/acp-10-8077-2010, 2010. (10.5194/acp-10-8077-2010)
  29. Langer, G.: A study of automobile exhaust as a source of ice nuclei, Preprints of the second National Conference on Weather Modification, American Meteorological Society, Boston, Massachusetts, 242–243, 1970.
  30. Lohmann, U. and Diehl, K.: Sensitivity studies of the importance of dust ice nuclei for the indirect aerosol effect on stratiform mixed phase clouds, J. Atmos. Sci., 63(3), 968–982, 2006. (10.1175/JAS3662.1)
  31. Lohmann, U. and Feichter, J.: Global indirect aerosol effects: a review, Atmos. Chem. Phys., 5, 715–737, https://doi.org/10.5194/acp-5-715-2005, 2005. (10.5194/acp-5-715-2005)
  32. Maki, L. R., Galyan, E. L., Chang-Chien, M., and Caldwell, D.: Ice nucleation induced by Pseudomonas syringae, Appl. Microbiol., 28, 456–459, 1974. (10.1128/am.28.3.456-459.1974)
  33. Mason, B. J.: The Physics of Clouds, Clarendon Press, Oxford, 660 pp., 1971.
  34. Mason, B. J. and Hallet, J.: Ice-Forming Nuclei, Nature, 179, 357–359, 1957. (10.1038/179357b0)
  35. Mazur, P.: Freezing of living cells: Mechanisms and implications, Amer. J. Physiol. Cell Physiol., 16, C125–C142, 1984. (10.1152/ajpcell.1984.247.3.C125)
  36. Mertes, S., Verheggen, B., Walter, S., Ebert, M., Conolly, P., Weingartner, E., Schneider, J., Bower, K., Weinbruch, S., Cozic, J., and Heintzenberg, J.: Counterflow virtual impactor based collection of small ice particles in mixed-phase clouds for the physico-chemical characterisation of tropospheric ice nuclei: sampler description and first case study, Aerosol Sci. Technol., 41, 848–864, 2007. (10.1080/02786820701501881)
  37. Miehe, G.: Algorithmen mit geringem Informationsbedarf zur Phasenanalyse und Gitterkonstantenbestimmung aus Elektronenbeugungsdaten, Ber. Dtsch. Mineral. Ges. Beih. Z. Eur. J. Mineral, 9, 250, 1997.
  38. Möhler, O., DeMott, P. J., Vali, G., and Levin, Z.: Microbiology and atmospheric processes: the role of biological particles in cloud physics, Biogeosciences, 4, 1059–1071, https://doi.org/10.5194/bg-4-1059-2007, 2007. (10.5194/bg-4-1059-2007)
  39. Murphy, D. M., Cziczo, D. J., Froyd, K. D., Hudson, P. K., Matthew, B. M., Middlebrook, A. M., Peltier, R. E., Sullivan, A., Thomson, D. S., and Weber, R. J.: Single-particle mass spectrometry of tropospheric aerosol particles, J. Geophys. Res., 111, D23S32, https://doi.org/10.1029/2006JD007340, 2006. (10.1029/2006JD007340)
  40. Murphy, D. M., Hudson, P. K., Cziczo, D. J., Gallavardin, S., Froyd, K. D., Johnston, M. V., Middlebrook, A. M., Reinard, M. S., Thomson, D. S., Thornberry, T., and Wexler, A. S.: Distribution of lead in single atmospheric particles, Atmos. Chem. Phys., 7, 3195–3210, https://doi.org/10.5194/acp-7-3195-2007, 2007. (10.5194/acp-7-3195-2007)
  41. Parungo, F. P. and Allee, P. A.: Rocket effluent: Its nucleation activity and related properties, J. Appl. Meteor., 17, 1856–1863, 1978. (10.1175/1520-0450(1978)017<1856:REIINA>2.0.CO;2)
  42. Phillips, V. T. J., De Mott, P. J., and Andronache, C.: An empirical parametrization of heterogeneous ice nucleation for multiple chemical species of aerosol, J. Atmos. Sci., 65, 2757–2783, 2008. (10.1175/2007JAS2546.1)
  43. Posfai, M., Anderson, J. R., and Buseck, P. R.: Soot and sulphate aerosol particles in the remote marine atmosphere, J. Geophys. Res., 104, 21685–21693, 1999. (10.1029/1999JD900208)
  44. Prenni, A. J., DeMott, P. J., Twohy, C., Poellot, M. R., Kreidenweis, S. M., Rogers, D. C., Brooks, S. D., Richardson, M. S., and Heymsfield, A. J.: Examinations of ice formation processes in Florida cumuli using ice nuclei measurements of anvil ice crystal particle residues, J. Geophys. Res., 112, D10221, https://doi.org/10.1029/2006JD007549, 2007. (10.1029/2006JD007549)
  45. Reischel, M. T. and Vali, G.: Freezing nucleation in aqueous electrolytes, Tellus, 27, 414–427, 1975. (10.1111/j.2153-3490.1975.tb01692.x)
  46. Richardson, M. S., DeMott, P. J., Kreidenweis, S. M., Cziczo, D. J., Dunlea, E. J., Jimenez, J. L., Thomson, D. S., Ashbaugh, L. L., Borys, R. D., Westphal, D. L., Casuccio, G. S., and Lersch, T. L.: Measurements of heterogeneous ice nuclei in the western United States in springtime and their relation to aerosol characteristics, J. Geophys. Res., 112, D02209, https://doi.org/10.1029/2006JD007500, 2007. (10.1029/2006JD007500)
  47. Roberts, P. and Hallett, J.: A laboratory study of the ice nucleating properties of some mineral particulates, Q. J. Roy. Meteorol. Soc., 94, 25–34, 1968. (10.1002/qj.49709439904)
  48. {'key': 'ref48', 'unstructured': ''}
  49. Rosinski, J.: Cloud condensation nuclei as a real source of ice forming nuclei in continental and marine air masses. Atmos. Res., 38, 351–359, 1995. (10.1016/0169-8095(95)00005-C)
  50. Schäfer, V. J.: Ice nuclei from automobile exhaust and iodine vapour, Science, 154, 1555–1557, 1966. (10.1126/science.154.3756.1555-b)
  51. Schaller, R. C. and Fukuta, N.: Ice nucleation by aerosol particles: Experimental studies using a wedge-shaped ice thermal diffusion chamber, J. Atmos. Sci., 36, 1788–1802, 1979. (10.1175/1520-0469(1979)036<1788:INBAPE>2.0.CO;2)
  52. Schnell, R. C. and Vali, G.: Atmospheric ice nuclei from decomposing vegetation, Nature, 236, 163–165, 1972. (10.1038/236163a0)
  53. Shotyk, W. and Le Roux, G.: Biogeochemistry and Cycling of Lead, in &quot;Biogeochemical Cycles of the Elements&quot;, Vol. 43 of Metal Ions in Biological Systems, edited by: Sigel, A., Sigel, H., Sigel, O. R. K., and Dekker, M., New York, 240–275, 2005. (10.1201/9780824751999.ch10)
  54. Szymer, W. and Zawadzki, I.:, Biogenic and Anthropogenic Sources of Ice-Forming Nulcei: A Review, Bull. Am. Meteorol. Soc., 78(2), 209–228, 1997. (10.1175/1520-0477(1997)078<0209:BAASOI>2.0.CO;2)
  55. Targino, A. C., Krejci, R., Noone, K. J., and Glantz, P.: Single particle analysis of ice crystal residuals observed in orographic wave clouds over Scandinavia during INTACC experiment, Atmos. Chem. Phys., 6, 1977–1990, https://doi.org/10.5194/acp-6-1977-2006, 2006. (10.5194/acp-6-1977-2006)
  56. Twohy, C. H. and Poellot, M. R.: Chemical characteristics of ice residual nuclei in anvil cirrus clouds: evidence for homogeneous and heterogeneous ice formation, Atmos. Chem. Phys., 5, 2289–2297, https://doi.org/10.5194/acp-5-2289-2005, 2005. (10.5194/acp-5-2289-2005)
  57. Utsunomiya, S., Jensen, K. A. , Keeler, G. J., and Ewing, R. C.: Direct identification of trace metals in fine and ultrafine particles in the Detroit urban atmosphere, Environ. Sci. Technol., 38, 2289–2297, 2004. (10.1021/es035010p)
  58. 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 the condensed phase in mixed-phase clouds, J. Geophys. Res., 112, D23202, https://doi.org/10.1029/2007JD008714, 2007. (10.1029/2007JD008714)
  59. Vester, B. P., Ebert, M., Barnert, E. B., Schneider, J., Kandler, K., Schütz, L., and Weinbruch, S.: Composition and mixing state of the urban background aerosol in the Rhein-Main area (Germany), Atmos. Environ., 41(29), 6102–6115, 2007. (10.1016/j.atmosenv.2007.04.021)
  60. Vidaurre, G. and Hallet, J.: Particle Impact and Breakup in Aircraft Measurement, J. Atmos. Ocean. Tech., 26, 97983, https://doi.org/10.1175/2008JTECHA1147.1, 2009. (10.1175/2008JTECHA1147.1)
  61. Wallace J. M. and Hobbs, P. V.: Atmospheric science: an introductory survey, 2nd ed., International Geophysics Series, Academic Press, Elsevier Inc., 483 pp., 2006.
  62. Weingartner, E., Burtscher, H., and Baltensperger, U.: Hygroscopic properties of carbon and diesel soot particles, Atmos. Environ., 31, 2311–2327, 1997. (10.1016/S1352-2310(97)00023-X)
  63. Wentzel, M., Gorzawski, H., Naumann, K.-H., Saathoff, H., and Weinbruch, S.: Transmission electron microscopical and aerosol dynamical characterization of soot aerosols, J. Aerosol Sci., 34, 1347–1370, 2003. (10.1016/S0021-8502(03)00360-4)
  64. Zimmermann F., Ebert, M., Worringen, A., Schütz, L., and Weinbruch, S.: Environmental scanning electron microscopy (ESEM) as a new technique to determine the ice nucleation capability of individual aerosol particles, Atmos. Environ., 41, 8219–8227, 2007. (10.1016/j.atmosenv.2007.06.023)
  65. Zimmermann, F., Ebert, M., Hoffmann, H., Kandler, K., Schütz, L., Worringen, A., and Weinbruch, S.: Ice nucleation properties of the most abundant mineral dust phases, J. Geophys. Res., 113, D23204, https://doi.org/10.1029/2008JD010655, 2008. (10.1029/2008JD010655)
  66. Zuberi, B., Bertram, A. K., Cassa, C. A., Molina, L. T., and Molina, M. J.: Heterogeneous nucleation of ice in (NH4)2SO4-H2O particles with mineral dust immersions, Geophys. Res. Lett., 29, 1504, https://doi.org/10.1029/2001GL014289, 2002. (10.1029/2001GL014289)
Dates
Type When
Created 14 years, 5 months ago (March 25, 2011, 6:59 a.m.)
Deposited 6 months, 2 weeks ago (Feb. 15, 2025, 3:21 p.m.)
Indexed 1 month, 2 weeks ago (July 16, 2025, 7:49 a.m.)
Issued 14 years, 5 months ago (March 25, 2011)
Published 14 years, 5 months ago (March 25, 2011)
Published Online 14 years, 5 months ago (March 25, 2011)
Funders 0

None

@article{Ebert_2011, title={Chemical composition and mixing-state of ice residuals sampled within mixed phase clouds}, volume={11}, ISSN={1680-7324}, url={http://dx.doi.org/10.5194/acp-11-2805-2011}, DOI={10.5194/acp-11-2805-2011}, number={6}, journal={Atmospheric Chemistry and Physics}, publisher={Copernicus GmbH}, author={Ebert, M. and Worringen, A. and Benker, N. and Mertes, S. and Weingartner, E. and Weinbruch, S.}, year={2011}, month=mar, pages={2805–2816} }