Abstract

An inversion method for the characterization of atmospheric condensed phases from infrared (IR) spectra is described. The method is tested with both synthetic IR spectra and the spectra of particles that flow in a cryogenic flow tube. The method is applied to the IR spectra recorded by the Atmospheric Trace Molecule Spectroscopy instrument carried by the Space Shuttle during three missions in 1992, 1993, and 1994. The volume density and particle size distribution for sulfate aerosol are obtained as a function of altitude. The density and size distribution of ice particles in several cirrus clouds are also retrieved. The probable radius of the ice particles in the high-altitude (10–15-km) cirrus clouds is found to be approximately 6–7 μm.

© 2004 Optical Society of America

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2003 (6)

R. McGraw, D. T. Wu, “Kinetic extensions of the nucleation theorem,” J. Chem. Phys. 118, 9337–9347 (2003).
[CrossRef]

L. S. Rothman, A. Barbe, D. C. Benner, L. R. Brown, C. Camy-Peyret, M. R. Carleer, K. Chance, C. Clerbaux, V. Dana, V. M. Devi, A. Fayt, J. M. Flaud, R. R. Gamache, A. Goldman, D. Jacquemart, K. W. Jucks, W. J. Lafferty, J.-Y. Mandin, S. T. Massie, V. Nemtchinov, D. A. Newnham, A. Perrin, C. P. Rinsland, J. Schroeder, K. M. Smith, M. A. H. Smith, K. Tang, R. A. Toth, J. Vander Auwera, P. Varanasi, K. Yoshino, “The HITRAN molecular spectroscopic database: edition of 2000 including updates through 2001,” J. Quant. Spectrosc. Radiat. Transfer 82, 5–44 (2003).
[CrossRef]

T. Deshler, M. E. Hervig, D. J. Hofmann, J. M. Rosen, J. B. Liley, “Thirty years of in situ stratospheric aerosol size distribution measurements from Laramie, Wyoming (41 °N), using balloon-borne instruments,” J. Geophys. Res. 108(D5), 4167, doi:10.1029/2002JD002514 (2003).

O. Jourdan, S. Oshchepkov, J.-F. Gayet, V. Shcherbakov, H. Isaka, “Statistical analysis of cloud light scattering and microphysical properties obtained from airborne measurements,” J. Geophys. Res. 108(D5), 4155, doi:10.1029/2002JD002723 (2003).

P. R. Field, A. J. Baran, P. H. Kaye, E. Hirst, R. Greenaway, “A test of cirrus ice crystal scattering phase functions,” Geophys. Res. Lett. 30, 1752, doi:10.1029/2003GLO17482 (2003).
[CrossRef]

B. Karcher, J. Strom, “The roles of dynamical variability and aerosols in cirrus cloud formation,” Atmos. Chem. Phys. 3, 823–838 (2003).
[CrossRef]

2002 (6)

B. H. Kahn, A. Eldering, F. W. Irion, F. P. Mills, B. Sen, M. R. Gunson, “Cloud identification in Atmospheric Trace Molecule Spectroscopy infrared occultation measurements,” Appl. Opt. 41, 2768–2780 (2002).
[CrossRef] [PubMed]

F. W. Irion, M. R. Gunson, G. C. Toon, A. Y. Chang, A. Eldering, E. Mahieu, G. L. Manney, H. A. Michelsen, E. J. Moyer, M. J. Newchurch, G. B. Osterman, C. P. Rinsland, R. J. Salawitch, B. Sen, Y. L. Yung, R. Zander, “Atmospheric Trace Molecule Spectroscopy (ATMOS) Experiment Version 3 data retrievals,” Appl. Opt. 41, 6968–6979 (2002).
[CrossRef] [PubMed]

H.-M. Hung, S. T. Martin, “Infrared spectroscopic evidence for the ice formation mechanisms active in aerosol flow tubes,” Appl. Spectrosc. 56, 1067–1081 (2002).
[CrossRef]

A. Y. Zasetsky, J. J. Sloan, R. Escribano, D. Fernandez, “A new method for the quantitative identification of the composition, size and density of stratospheric aerosols from high resolution IR satellite measurements,” Geophys. Res. Lett. 29, 2071, doi:10-1029/2002GL015816 (2002).
[CrossRef]

M. Matsumoto, S. Saito, I. Ohmine, “Molecular dynamics simulation of the ice nucleation and growth process leading to water freezing,” Nature 416, 409–413 (2002).
[CrossRef] [PubMed]

Y. J. Kaufman, D. Tanré, O. Boucher, “A satellite view of aerosols in the climate system,” Nature 419, 215–223 (2002).
[CrossRef] [PubMed]

2001 (3)

A. Aballe, M. Bethencourt, F. J. Botana, M. Marcos, J. M. Sánchez-Amaya, “Use of wavelets to study electrochemical noise transients,” Electrochim. Acta 46, 2353–2361 (2001).
[CrossRef]

C. Timmreck, “Three-dimensional simulation of stratospheric background aerosol: first results of a multiannual general circulation model simulation,” J. Geophys. Res. 106(D22), 28313–28332 (2001).
[CrossRef]

K.-M. Lee, J. H. Park, S. T. Massie, W. Choi, “Extinction coefficients and properties of Pinatubo aerosol determined from Halogen Occultation Experiment (HALOE) data,” J. Geophys. Res. 106(D22), 28333–28345 (2001).
[CrossRef]

2000 (4)

U. M. Biermann, B. P. Luo, T. Peter, “Absorption spectra and optical constants of binary and ternary solutions of H2SO4, HNO3, and H2O in the mid infrared at atmospheric temperatures,” J. Phys. Chem. A 104, 783–793 (2000).
[CrossRef]

A. K. Bertram, T. Koop, L. T. Molina, M. J. Molina, “Ice formation in (NH4)2SO4-H2O particles,” J. Phys. Chem. A 104, 584–588 (2000).
[CrossRef]

A. K. Bertram, D. B. Dickens, J. J. Sloan, “Supercooling of type 1 polar stratospheric clouds: the freezing of submicron nitric acid aerosols having HNO3 mol fractions less than 0.5,” J. Geophys. Res. 105(D7), 9283–9290 (2000).
[CrossRef]

T. Koop, B. P. Luo, A. Tsias, T. Peter, “Water activity as the determinant for homogeneous ice nucleation in aqueous solutions,” Nature 406, 611–614 (2000).
[CrossRef] [PubMed]

1999 (3)

P. R. ten Wolde, D. W. Oxtoby, D. Frenkel, “Chain formation in homogeneous gas-liquid nucleation of polar fluids,” J. Chem. Phys. 111, 4762–4773 (1999).
[CrossRef]

A. Laaksonen, R. McGraw, H. Vehkamäki, “Liquid-drop formalism and free-energy surfaces in binary homogeneous nucleation theory,” J. Chem. Phys. 111, 2019–2027 (1999).
[CrossRef]

Y. Sasano, M. Suzuki, T. Yokota, H. Kanzawa, “Improved limb atmospheric spectrometer (ILAS) for stratospheric ozone layer measurements by solar occultation technique,” Geophys. Res. Lett. 26, 197–200 (1999).
[CrossRef]

1998 (3)

I. Kusaka, Z. G. Wang, J. H. Seinfeld, “Binary nucleation of sulfuric acid-water: Monte Carlo simulation,” J. Chem. Phys. 108, 6829–6848 (1998).
[CrossRef]

C. P. Rinsland, M. R. Gunson, P. H. Wang, R. F. Arduini, B. A. Baum, P. Minnis, A. Goldman, M. C. Abrams, R. Zander, E. Mahieu, R. J. Salawitch, H. A. Michelsen, F. W. Irion, M. J. Newchurch, “ATMOS/ATLAS 3 infrared profile measurements of clouds in the tropical and subtropical upper troposphere,” J. Quant. Spectrosc. Radiat. Transfer 60, 903–919 (1998).
[CrossRef]

M. I. Mishchenko, L. D. Travis, “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).
[CrossRef]

1997 (3)

J. Ström, B. Strauss, T. Anderson, F. Schröder, J. Heintzenberg, P. Wendling, “In situ observations of the microphysical properties of young cirrus clouds,” J. Atmos. Sci. 54, 2542–2553 (1997).
[CrossRef]

T. Peter, “Microphysics and heterogeneous chemistry of polar stratospheric clouds,” Annu. Rev. Phys. Chem. 48, 785–822 (1997).
[CrossRef] [PubMed]

K. S. Carslaw, T. Peter, S. L. Clegg, “Modeling the composition of liquid stratospheric aerosols,” Rev. Geophys. 35, 125–154 (1997).
[CrossRef]

1996 (2)

M. R. Gunson, M. M. Abbas, M. C. Abrams, M. Allen, L. R. Brown, T. L. Brown, A. Y. Chang, A. Goldman, F. W. Irion, L. L. Lowes, E. Mahieu, G. L. Manney, H. A. Michelsen, M. J. Newchurch, C. P. Rinsland, R. J. Salawitch, G. P. Stiller, G. C. Toon, Y. L. Yung, R. Zander, “The Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment: deployment on the ATLAS Space Shuttle missions,” Geophys. Res. Lett. 23, 2333–2336 (1996).
[CrossRef]

S. T. Massie, T. Deshler, G. E. Thomas, J. L. Mergenthaler, J. M. Russell, “Evolution of the infrared properties of the Mount Pinatubo aerosol cloud over Laramie, Wyoming,” J. Geophys. Res. 101(D17), 23007–23019 (1996).
[CrossRef]

1995 (4)

G. K. Yue, L. W. Thomason, L. R. Poole, P.-H. Wang, D. Baumgardner, J. E. Dye, “Aerosol surface areas deduced from early 1993 SAGE II data and comparisons with stratospheric photochemistry, aerosols, and dynamics expedition measurements,” Geophys. Res. Lett. 22, 2933–2936 (1995).
[CrossRef]

M. L. Clapp, D. R. Worsnop, R. E. Miller, “Frequency-dependent optical constants of water ice obtained directly from aerosol extinction spectra,” J. Phys. Chem. 99, 6317–6326 (1995).
[CrossRef]

K. S. Carslaw, S. L. Clegg, P. Brimblecombe, “A thermodynamic model of the system Hcl-Hno3–H2So4–H2O, including solubilities of Hbr, from less-than-200 to 328 K,” J. Phys. Chem. 99, 11557–11574 (1995).
[CrossRef]

O. V. Dubovik, T. V. Lapyonok, S. L. Oshchepkov, “Improved technique for data inversion: optical sizing of multicomponent aerosols,” Appl. Opt. 34, 8422–8436 (1995).
[CrossRef] [PubMed]

1994 (3)

B. T. Draine, P. J. Flatau, “Discrete-dipole approximation for scattering calculations,” J. Opt. Soc. Am. A 11, 1491–1499 (1994).
[CrossRef]

C. P. Rinsland, G. K. Yue, M. R. Gunson, R. Zander, M. C. Abrams, “Mid-infrared extinction by sulfate aerosols from the Mt Pinatubo eruption,” J. Quant. Spectrosc. Radiat. Transfer 52, 241–252 (1994).
[CrossRef]

M. I. Mishchenko, L. D. Travis, “T-matrix computations of light scattering by large spheroidal particles,” Opt. Commun. 109, 16–21 (1994).
[CrossRef]

1993 (1)

T. Deshler, B. J. Johnson, W. R. Rozier, “Balloonborne measurements of Pinatubo aerosol during 1991 and 1992 at 41 °N: vertical profiles, size distribution, and volatility,” Geophys. Res. Lett. 20, 1435–1438 (1993).
[CrossRef]

1992 (1)

J. P. D. Abbatt, K. D. Beyer, A. F. Fucaloro, J. R. McMahon, P. J. Wooldridge, R. Zhang, M. J. Molina, “Interaction of HCl vapor with water-ice: implications for the stratosphere,” J. Geophys. Res. 97(D14), 15819–15826 (1992).

1982 (1)

D. Kashchiev, “On the relation between nucleation work, nucleus size, and nucleation rate,” J. Chem. Phys. 76, 5098–5102 (1982).
[CrossRef]

1962 (1)

D. L. Phillips, “A technique for the numerical solution of certain integral equations of the first kind,” J. Assoc. Comput. Mach. 9, 84–97 (1962).
[CrossRef]

Aballe, A.

A. Aballe, M. Bethencourt, F. J. Botana, M. Marcos, J. M. Sánchez-Amaya, “Use of wavelets to study electrochemical noise transients,” Electrochim. Acta 46, 2353–2361 (2001).
[CrossRef]

Abbas, M. M.

M. R. Gunson, M. M. Abbas, M. C. Abrams, M. Allen, L. R. Brown, T. L. Brown, A. Y. Chang, A. Goldman, F. W. Irion, L. L. Lowes, E. Mahieu, G. L. Manney, H. A. Michelsen, M. J. Newchurch, C. P. Rinsland, R. J. Salawitch, G. P. Stiller, G. C. Toon, Y. L. Yung, R. Zander, “The Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment: deployment on the ATLAS Space Shuttle missions,” Geophys. Res. Lett. 23, 2333–2336 (1996).
[CrossRef]

Abbatt, J. P. D.

J. P. D. Abbatt, K. D. Beyer, A. F. Fucaloro, J. R. McMahon, P. J. Wooldridge, R. Zhang, M. J. Molina, “Interaction of HCl vapor with water-ice: implications for the stratosphere,” J. Geophys. Res. 97(D14), 15819–15826 (1992).

Abrams, M. C.

C. P. Rinsland, M. R. Gunson, P. H. Wang, R. F. Arduini, B. A. Baum, P. Minnis, A. Goldman, M. C. Abrams, R. Zander, E. Mahieu, R. J. Salawitch, H. A. Michelsen, F. W. Irion, M. J. Newchurch, “ATMOS/ATLAS 3 infrared profile measurements of clouds in the tropical and subtropical upper troposphere,” J. Quant. Spectrosc. Radiat. Transfer 60, 903–919 (1998).
[CrossRef]

M. R. Gunson, M. M. Abbas, M. C. Abrams, M. Allen, L. R. Brown, T. L. Brown, A. Y. Chang, A. Goldman, F. W. Irion, L. L. Lowes, E. Mahieu, G. L. Manney, H. A. Michelsen, M. J. Newchurch, C. P. Rinsland, R. J. Salawitch, G. P. Stiller, G. C. Toon, Y. L. Yung, R. Zander, “The Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment: deployment on the ATLAS Space Shuttle missions,” Geophys. Res. Lett. 23, 2333–2336 (1996).
[CrossRef]

C. P. Rinsland, G. K. Yue, M. R. Gunson, R. Zander, M. C. Abrams, “Mid-infrared extinction by sulfate aerosols from the Mt Pinatubo eruption,” J. Quant. Spectrosc. Radiat. Transfer 52, 241–252 (1994).
[CrossRef]

Allen, M.

M. R. Gunson, M. M. Abbas, M. C. Abrams, M. Allen, L. R. Brown, T. L. Brown, A. Y. Chang, A. Goldman, F. W. Irion, L. L. Lowes, E. Mahieu, G. L. Manney, H. A. Michelsen, M. J. Newchurch, C. P. Rinsland, R. J. Salawitch, G. P. Stiller, G. C. Toon, Y. L. Yung, R. Zander, “The Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment: deployment on the ATLAS Space Shuttle missions,” Geophys. Res. Lett. 23, 2333–2336 (1996).
[CrossRef]

Anderson, T.

J. Ström, B. Strauss, T. Anderson, F. Schröder, J. Heintzenberg, P. Wendling, “In situ observations of the microphysical properties of young cirrus clouds,” J. Atmos. Sci. 54, 2542–2553 (1997).
[CrossRef]

Arduini, R. F.

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Figures (9)

Fig. 1
Fig. 1

Top panel, χ as a function of parameter γ (solid curve); dotted curve, the χ values obtained assuming a three-mode log-normal approximation; dashed curve, the entropy (see Appendix B). The bottom panel shows the volume size distributions that correspond to the γ values shown in the top plot.

Fig. 2
Fig. 2

Synthetic extinction spectrum (points) for the mixture of liquid water and ice aerosols together with its best fit (solid curve). A log-normal distribution with a mean radius of 1.0 μm and a dispersion of 0.4 was used for the water particles. The ice particles have a mean radius of 5.0 μm and a dispersion of 0.2. Normally distributed noise having an intensity of 25% of the total with zero mean and unit dispersion was added.

Fig. 3
Fig. 3

Retrieval results for a mixture of water and ice particles. The retrieved values (curves) and the original distribution functions (filled diamonds) are shown as a function of the noise intensity added to the synthetic spectra.

Fig. 4
Fig. 4

Extinction spectra of liquid water at 300 K (squares) and ice aerosols at 228 K (triangles) together with their best fits (solid curves). Spectra are offset for clarity. The bottom plot shows the volume density size distributions for liquid water and ice aerosols retrieved by use of the above spectra.

Fig. 5
Fig. 5

Average vertical profiles of the volume density for sulfate aerosol observed in ATMOS missions.

Fig. 6
Fig. 6

Size distributions of the sulfate aerosol for several tangent altitudes. The distribution functions are the averages over observations made in 1992.

Fig. 7
Fig. 7

Comparison of cloud-free (left panels) and prominent cirrus cloud (right panels) ATMOS observations.

Fig. 8
Fig. 8

Vertical profiles of the volume density for ice aerosol (cirrus clouds). The three cirrus cloud events were chosen based on the results of Refs. 39 and 40.

Fig. 9
Fig. 9

Ice particle size distributions for the cirrus cloud events. The corresponding volume density vertical profiles are shown in Fig. 8.

Equations (13)

Equations on this page are rendered with MathJax. Learn more.

χ=min|W-1·K·P-τextS+γ·S·P|21/2,
K·P=Kext1, Kext2,KextN·p1, p2,pNT,
γ·S1··0·S2······0··SNp1p2·pN=0,
Sk,li=1 if k=l; Sk,li=-3 if k=l+1;Sk,li=3 if k=l+2; Sk,li=-1 if k=l+3;for k=1  M, l=1  M-3;Sk,li=0 otherwise.
pji0, i=1  N, j=1  M,
χ2=minK·P-τ2, subject to 1· P0 and S·P=0,
P=Ly1y2,
SK1·L=S˜0K˜1K˜21112.
χ2=minK˜2·y2-τ˜2, subject to 11y1+12y20,
ΔFs=Aσ=3σ4i=1MPVriri,
ΔS=-k i=1MlogPVri.
ΔF=ΔFs-ΔST.
ΔFγ=3σ4i=1MPVri, γri+kT i=1MlogPVri, γ.

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