Atmospheric Chemistry and Physics
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12
2006
10.5194/acp-6-4775-2006
http://www.atmos-chem-phys.net/6/4775/2006/
http://www.atmos-chem-phys.net/6/4775/2006/acp-6-4775-2006.html
http://www.atmos-chem-phys.net/6/4775/2006/acp-6-4775-2006.pdf
4775
4800
2006-10-24
Probing ice clouds by broadband mid-infrared extinction spectroscopy: case studies from ice nucleation experiments in the AIDA aerosol and cloud chamber
R. Wagner
S. Benz
O. Möhler
H. Saathoff
U. Schurath
Forschungszentrum Karlsruhe, Institute of Meteorology and Climate Research, Karlsruhe, Germany
Series of infrared extinction spectra of ice crystals were recorded in the
6000–800 cm<sup>−1</sup> wavenumber regime during expansion cooling experiments
in the large aerosol and cloud chamber AIDA of Forschungszentrum Karlsruhe.
Either supercooled sulphuric acid solution droplets or dry mineral dust
particles were added as seed aerosols to initiate ice formation after having
established ice supersaturated conditions inside the chamber. The various
ice nucleation runs were conducted at temperatures between 237 and 195 K,
leading to median sizes of the nucleated ice particles of 1–15 µm.
The measured infrared spectra were fitted with reference spectra from
<b>T</b>-matrix calculations to retrieve the number concentration as well as the
number size distribution of the generated ice clouds. The precise evaluation
of the time-dependent ice particle number concentrations, i.e., the rates of
new ice particle formation, is of particular importance to quantitatively
analyse the ice nucleation experiments in terms of nucleation rates and ice activation spectra. The ice particles were
modelled as finite circular cylinders with aspect ratios ranging from 0.5 to
3.0. Benefiting from the comprehensive diagnostic tools for the
characterisation of ice clouds which are available at the AIDA facility, the
infrared retrieval results with regard to the ice particle number
concentration could be compared to independent measurements with various
optical particle counters. This provided a unique chance to quantitatively
assess potential errors or solution ambiguities in the retrieval procedure
which mainly originate from the difficulty to find an appropriate shape
representation for the aspherical particle habits of the ice crystals. Based
on these inter-comparisons, we demonstrate that there is no standard
retrieval approach which can be routinely applied to all different
experimental scenarios. In particular, the concept to account for the
asphericity of the ice crystals, the a priori constraints which might be imposed on
the unknown number size distribution of the ice crystals (like employing an
analytical distribution function), and the wavenumber range which is
included in the fitting algorithm should be carefully adjusted to each
single retrieval problem.
Archuleta, C. M., DeMott, P. J., and Kreidenweis, S. M.: Ice nucleation by surrogates for atmospheric mineral dust and mineral dust/sulfate particles at cirrus temperatures, Atmos. Chem. Phys., 5, 2617–2634, 2005.
Arnott, W. P., Dong, Y. Y., and Hallett, J., Extinction Efficiency in the Infrared (2–18 $\mu $m) of Laboratory Ice Clouds – Observations of Scattering Minima in the Christiansen Bands of Ice, Appl. Opt., 34, 541–551, 1995.
Arnott, W. P., Liu, Y., Schmitt, C., and Hallett, J.: The Unreasonable Effectiveness of Mimicking Measured Infrared Extinction by Hexagonal Ice Crystals With Mie Ice Spheres, in: OSA symposium on Optical Remote Sensing of the Atmosphere, pp. 216–218, OSA Technical Digest Series (Optical Society of America, Washington D.C.), vol. 5, 1997a.
Arnott, W. P., Schmitt, C., Liu, Y. G., and Hallett, J.: Droplet size spectra and water-vapor concentration of laboratory water clouds: Inversion of Fourier transform infrared (500–5000 cm$^-1)$ optical-depth measurement, Appl. Opt., 36, 5205–5216, 1997b.
Bailey, M., and Hallett, J., Growth rates and habits of ice crystals between −20° and −70°C, J. Atmos. Sci., 61, 514–544, 2004.
Baran, A. J.: Simulation of infrared scattering from ice aggregates by use of a size-shape distribution of circular ice cylinders, Appl. Opt., 42, 2811–2818, 2003.
Baran, A. J.: On the scattering and absorption properties of cirrus cloud, J. Quant. Spectrosc. Radiat. Transfer, 89, 17–36, 2004.
Baran, A. J.: The dependence of cirrus infrared radiative properties on ice crystal geometry and shape of the size-distribution function, Q. J. R. Meteorol. Soc., 131, 1129–1142, 2005.
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.
Bohren, C. F. and Huffman, D. R.: Absorption and Scattering of Light by Small Particles, John Wiley & Sons, Inc., New York, 1983.
Bohren, C. F. and Koh, G.: Forward-scattering corrected extinction by nonspherical particles, Appl. Opt., 24, 1023–1029, 1985.
Clapp, M. L., Miller, R. E., and Worsnop, D. R.: Frequency-Dependent Optical Constants of Water Ice Obtained Directly from Aerosol Extinction Spectra, J. Phys. Chem., 99, 6317–6326, 1995.
Deepak, A. and Box, M. A.: Forwardscattering corrections for optical extinction measurements in aerosol media. 1: Monodispersions, Appl. Opt., 17, 2900–2908, 1978.
Echle, G., von Clarmann, T., and Oelhaf, H.: Optical and microphysical parameters of the Mt. Pinatubo aerosol as determined from MIPAS-B mid-IR limb emission spectra, J. Geophys. Res., 103, 19 193–19 211, 1998.
Eremenko, M. N., Zasetsky, A. Y., Boone, C. D., and Sloan, J. J.: Properties of high-altitude tropical cirrus clouds determined from ACE FTS observations, Geophys. Res. Lett., 32, L15S07, doi:10.1029/2005GL022428, 2005.
Field, P. R., Möhler, O., Connolly, P., Krämer, M., Cotton, R., Heymsfield, A. J., and Schnaiter, M.: Some ice nucleation characteristics of Asian and Saharan desert dust, Atmos. Chem. Phys., 6, 2991–3006, 2006.
Haag, W., Kärcher, B., Schaefers, S., Stetzer, O., Möhler, O., Schurath, U., Krämer, M., and Schiller, C.: Numerical simulations of homogeneous freezing processes in the aerosol chamber AIDA, Atmos. Chem. Phys., 3, 195–210, 2003.
Hill, S. C., Hill, A. C., and Barber, P. W.: Light scattering by size/shape distributions of soil particles and spheroids, Appl. Opt., 23, 1025–1031, 1984.
Hung, H. M. and Martin, S. T.: Infrared spectroscopic evidence for the ice formation mechanisms active in aerosol flow tubes, Appl. Spectrosc., 56, 1067–1081, 2002.
Kahn, B. H., Eldering, A., Clough, S. A., Fetzer, E. J., Fishbein, E., Gunson, M. R., Lee, S. Y., Lester, P. F., and Realmuto, V. J.: Near micron-sized cirrus cloud particles in high-resolution infrared spectra: An orographic case study, Geophys. Res. Lett., 30(8), 1441, doi:10.1029/2003GL016909, 2003.
Kahn, B. H., Eldering, A., Ghil, M., Bordoni, S., and Clough, S. A.: Sensitivity analysis of cirrus cloud properties from high-resolution infrared spectra. Part I: Methodology and synthetic cirrus, J. Climate, 17, 4856–4870, 2004.
Kokhanovsky, A.: Optical properties of terrestrial clouds, Earth-Sci. Rev., 64, 189–241, 2004.
Kokhanovsky, A. A.: Microphysical and optical properties of noctilucent clouds, Earth-Sci. Rev., 71, 127–146, 2005.
Lawson, R. P., Baker, B. A., Schmitt, C. G., and Jensen, T. L.: An overview of microphysical properties of Arctic clouds observed in May and July 1998 during FIRE ACE, J. Geophys. Res., 106, 14 989–15 014, 2001.
Lee, Y. K., Yang, P., Mishchenko, M. I., Baum, B. A., Hu, Y. X., Huang, H. L., Wiscombe, W. J., and Baran, A. J.: Use of circular cylinders as surrogates for hexagonal pristine ice crystals in scattering calculations at infrared wavelengths, Appl. Opt., 42, 2653–2664, 2003.
Libbrecht, K. G. and Yu, H., Crystal growth in the presence of surface melting: supersaturation dependence of the growth of columnar ice crystals, J. Cryst. Growth, 222, 822–831, 2001.
Liu, Y. G., Arnott, W. P., and Hallett, J.: Particle size distribution retrieval from multispectral optical depth: Influences of particle nonsphericity and refractive index, J. Geophys. Res., 104, 31 753–31 762, 1999.
Lynch, D. K., Sassen, K., Starr, D. O., and Stephens, G.: Cirrus, Oxford University Press Inc., USA, 2002.
Mishchenko, M. I.: Light-Scattering by Size Shape Distributions of Randomly Oriented Axially-Symmetrical Particles of a Size Comparable to a Wavelength, Appl. Opt., 32, 4652–4666, 1993.
Mishchenko, M. I. and Travis, L. D.: Capabilities and limitations of a current FORTRAN implementation of the T-matrix method for randomly oriented, rotationally symmetric scatterers, J. Quant. Spectrosc. Radiat. Transfer, 60, 309–324, 1998.
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 Sulphuric Acid Coating on Heterogeneous Ice Nucleation by Soot Aerosol Particles, J. Geophys. Res., 110, D11210, doi:10.1029/2004JD005169, 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., 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.
Moosmüller, H. and Arnott, W. P.: Angular truncation errors in integrating nephelometry, Rev. Sci. Instrum., 74, 3492–3501, 2003.
Press, W. H., Teukolsky, S. A., Vetterling, W. T., and Flannery, B. P.: Numerical Recipes in C: The Art of Scientific Computing, Cambridge University Press, Cambridge, 1992.
Proctor, T. D. and Harris, G. W.: The Turbidity of Suspensions of Irregular Quartz Particles, Aerosol Sci., 5, 81–90, 1974.
Rädel, G., Stubenrauch, C. J., Holz, R., and Mitchell, D. L.: Retrieval of effective ice crystal size in the infrared: Sensitivity study and global measurements from TIROS-N Operational Vertical Sounder, J. Geophys. Res., 108(D9), 4281, doi:10.1029/2002JD002801, 2003.
Rajaram, B., Glandorf, D. L., Curtis, D. B., Tolbert, M. A., Toon, O. B., and Ockman, N.: Temperature-dependent optical constants of water ice in the near infrared: new results and critical review of the available measurements, Appl. Opt., 40, 4449–4462, 2001.
Schmitt, C. G. and Arnott, W. P.: Infrared emission (500–2000 cm$^-1)$ of laboratory ice clouds, J. Quant. Spectrosc. Radiat. Transfer, 63, 701–725, 1999.
Wagner, R., Benz, S., Möhler, O., Saathoff, H., Schnaiter, M., and Schurath, U.: Mid-infrared extinction spectra and optical constants of supercooled water droplets, J. Phys. Chem. A, 109, 7099–7112, 2005a.
Wagner, R., Bunz, H., Linke, C., Möhler, O., Naumann, K. H., Saathoff, H., Schnaiter, M., and Schurath, U.: Chamber Simulations of Cloud Chemistry: The AIDA Chamber, in: Proceedings of the NATO Advances Research Workshop on Environmental Simulation Chambers: Application to Atmospheric Chemical Processes, held in Zakopane, Poland, from 1 to 4 October 2004, edited by: Barnes, I. and Rudzinski, K. J., Springer, 2006.
Wagner, R., Möhler, O., Saathoff, H., Stetzer, O., and Schurath, U.: Infrared spectrum of nitric acid dihydrate – influence of particle shape, J. Phys. Chem. A, 109, 2572–2581, 2005b.
Walters, P. T.: Pratical applications of inverting spectral turbidity data to provide aerosol size distributions, Appl. Opt., 19, 2353–2365, 1980.
Warren, S. G.: Optical constants of ice from the ultraviolet to the microwave, Appl. Opt., 23, 1206–1225, 1984.
White, J. U.: Very long optical paths in air, J. Opt. Soc. Am., 66, 411–416, 1976.
Wind, L. and Szymanski, W. W.: Quantification of scattering corrections to the Beer-Lambert law for transmittance measurements in turbid media, Meas. Sci. Technol., 13, 270–275, 2002.
Yang, P., Gao, B. C., Baum, B. A., Hu, Y. X., Wiscombe, W. J., Tsay, S. C., Winker, D. M., and Nasiri, S. L.: Radiative properties of cirrus clouds in the infrared (8–13 $\mu $m) spectral region, J. Quant. Spectrosc. Radiat. Transfer, 70, 473–504, 2001.
Yang, P., Liou, K. N., and Arnott, W. P.: Extinction efficiency and single-scattering albedo for laboratory and natural cirrus clouds, J. Geophys. Res., 102, 21 825–21 835, 1997.
Yang, P., Wei, H. L., Huang, H. L., Baum, B. A., Hu, Y. X., Kattawar, G. W., Mishchenko, M. I., and Fu, Q.: Scattering and absorption property database for nonspherical ice particles in the near- through far-infrared spectral region, Appl. Opt., 44, 5512–5523, 2005.
Zakharova, N. T. and Mishchenko, M. I.: Scattering properties of needlelike and platelike ice spheroids with moderate size parameters, Appl. Opt., 39, 5052–5057, 2000.
Zasetsky, A. Y., Khalizov, A. F., Earle, M. E., and Sloan, J. J.: Frequency Dependent Complex Refractive Indices of Supercooled Liquid Water and Ice Determined from Aerosol Extinction Spectra, J. Phys. Chem. A, 109, 2760–2764, 2005.
Zasetsky, A. Y., Khalizov, A. F., and Sloan, J. J.: Characterization of atmospheric aerosols from infrared measurements: simulations, testing, and applications, Appl. Opt., 43, 5503–5511, 2004.