Abstract

Optical parameters of simulated ambient individual ammonium sulfate and soot-mixed particles were calculated using the discrete-dipole approximation method with different model geometries. Knowledge of the mixing state and the approximation by a suited idealized geometry reduces the errors of the optical properties by ±50% to ±10%. The influence of the soot content and the mixing state on the optical properties of the total aerosol was estimated. For the total aerosol population, the size distribution and the absolute soot content had the largest influence. The exact geometry of the ammonium sulfate and soot-mixed particles can be neglected.

© 2008 Optical Society of America

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    [CrossRef]
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2007 (1)

B. P. Vester, M. Ebert, E. B. Barnert, J. Schneider, K. Kandler, L. Schütz, and S. Weinbruch, “Composition and mixing state of the urban background aerosol in the Rhein-Main Area (Germany),” Atmos. Environ. 41, 6102-6115 (2007).
[CrossRef]

2006 (1)

M. Kocifaj, M. Gangl, F. Kundracík, H. Horvath, G. Videen, “Simulation of the optical properties of single composite aerosols,” J. Aerosol Sci. 37, 1683-1695 (2006).
[CrossRef]

2005 (1)

M. N. Eremenko, S. V. Petelina, A. Y. Zasetsky, B. Karlsson, C. P. Rinsland, E. J. Llewellyn, and J. J. Sloan, “Shape and composition of PMC particles derived from satellite remote sensing measurements,” Geophys. Res. Lett. 32, doi:10.1029/2005GL023013 (2005).
[CrossRef]

2004 (2)

M. Mallet, J. C. Roger, S. Despiau, J. P. Putaud, O. Dubovik, “A study of the mixing state of black carbon in urban zone,” J. Geophys. Res. 109, doi:10.1029/2003JD003940 (2004).
[CrossRef]

M. Ebert, S. Weinbruch, P. Hoffmann, and H. M. Ortner, “The chemical composition and complex refractive index of rural and urban influenced aerosols determined by individual particle analysis,” Atmos. Environ. 38, 6531-6545(2004).
[CrossRef]

2003 (3)

M. Schnaiter, H. Horvath, O. Möhler, K.-H. Naumann, H. Saathoff, and O. W. Schöck, “UV-VIS-NIR spectral optical properties of soot and soot-containing aerosols,” J. Aerosol Sci. 34, 1421-1444 (2003).
[CrossRef]

N. Riemer, H. Vogel, B. Vogel, and F. Fiedler, “Modeling aerosols on the mesoscale-γ: treatments of soot aerosol and its radiative effects,” J. Geophys. Res. 108, doi:10.1029/2003JD003448 (2003).
[CrossRef]

J. Miao, K.-P. Johnson, S. Buehler, and A. Kokhanovsky, “The potential of polarization measurements from space at mm and sub-mm wavelength for determining cirrus cloud parameters,” Atmos. Chem. Phys. Discuss. 3, 39-48 (2003).

2002 (5)

H. Wex, C. Neusüss, M. Wendisch, F. Stratmann, C. Koziar, A. Keil, and A. Wiedensohler, “Particle scattering, backscattering, and absorption coefficients: An in situ closure and sensitivity study,” J. Geophys. Res. 107, doi:10.1029/2000JD000234 (2002).
[CrossRef]

U. Bundke, G. Hänel, H. Horvarth, W. Kaller, S. Seidl, H. Wx, A. Wiedensohler, M. Wiegner, and V. Freudenthaler, “Aerosol optical properties during the Lindenberg Aerosol Characterization Experiment (LACE98),” J. Geophys. Res. 107, doi: 10.1029/2000JD000188 (2002).
[CrossRef]

G. Lesins, P. Chýlek, and U. Lohmann, “A study of internal and external mixing scenarios and its effects on aerosol optical properties and direct radiative forcing,” J. Geophys. Res. 107, 4094 (2002).
[CrossRef]

A. Ansmann, U. Wandinger, A. Wiedensohler, and U. Leiterer, “Lindenberg Aerosol Characterization Experiment 1998 (LACE98): overview,” J. Geophys. Res. 107, doi: 10.1029/2000JD000233 (2002).
[CrossRef]

M. Ebert, S. Weinbruch, A. Rausch, G. Gorzawski, G. Helas, P. Hofmann, and H. Wex, “The complex refractive index of aerosols during LACE 98 as derived from the analysis of individual particles,” J. Geophys. Res. 107, doi: 10.1029/2000JD000195, (2002).
[CrossRef]

2001 (3)

J. E. Penner, D. Hegg, and R. Leaitch, “Unravelling the role of aerosols in climate change,” Environ. Sci. Technol. 35, 332 A-340 A (2001).

A. Rausch, T. Trautmann, S. Weinbruch, and G. Helas, “Calculation of scattering and absorption of light by irregular shaped and mixed particles,” J. Aerosol Sci. 32, S419-S420(2001).

N. A. Marley, J. S. Gaffney, J. B. Baird, C. A. Blazer, P. J. Drayton, and J. E. Frederick, “An empirical method for the determination of the complex refractive index of size-fractionated atmospheric aerosols for radiative transfer calculations,” Aerosol Sci. Technol. 34, 535-549 (2001).
[CrossRef]

1999 (4)

A. Kirkevåg, T. Iversen, and A. Dahlback, “On radiative effects of black carbon and sulphate aerosols,” Atmos. Environ. 33, 2621-2635 (1999).
[CrossRef]

M. Pósfai, J. R. Anderson, P. R. Buseck, and H. Sievering, “Soot and sulfate aerosol particles in the remote marine troposphere,” J. Geophys. Res. 104, 21685-21693 (1999).
[CrossRef]

K. A. Fuller, W. C. Malm, and S. M. Kreidenweis, “Effects of mixing on extinction by carbonaceous particles,” J. Geophys. Res. 104, 15941-15954 (1999).
[CrossRef]

V. A. Markel and V. M. Shalaev, “Absorption of light by soot particles in micro-droplets of water,” J. Quant. Spectrosc. Radiat. Transfer 63, 321-339 (1999).
[CrossRef]

1998 (4)

J. V. Martins, P. Artaxo, C. Liousse, J. S. Reid, P. V. Hobbs, and Y. J. Kaufman, “Effects of black carbon content, particle size, and mixing on light absorption by aerosols from biomass burning in Brazil,” J. Geophys. Res. 103, 32041-32050(1998).
[CrossRef]

G. Myhre, F. Stordal, K. Restadt, and I. S. A. Isaksen, “Estimation of the radiative forcing due to sulphate and soot aerosols,” Tellus 50B, 463-477 (1998).

H. Laitinen and K. Lumme, “T-matrix method for general star-shaped particles: first results,” J. Quant. Spectrosc. Radiat. Transfer 60, 325-334 (1998).
[CrossRef]

T. Wriedt and A. Doicu, “Formulations of the extended boundary condition method for three-dimensional scattering using the method of discrete sources,” J. Mod. Opt. 45, 119-213(1998).

1997 (2)

A. Fassi-Fihri, K. Shure, and R. Rosset, “Internal and external mixing in atmospheric aerosols by coagulation: impact on the optical and hygroscopic properties of the sulphate-soot system,” Atmos. Environ. 31, 1393-1402 (1997).
[CrossRef]

C. C. Chuang, J. E. Penner, K. E. Taylor, A. S. Grossman, and J. J. Walton, “An assessment of the radiative effects of anthropogenic sulphate,” J. Geophys. Res. 102, 3761-3778 (1997).
[CrossRef]

1996 (2)

S. E. Schwartz, “The Whitehouse effect--shortwave radiative forcing of climate by anthropogenic aerosols: an overview,” J. Aerosol Sci. 27, 359-382 (1996).
[CrossRef]

D. W. Mackowski and M. I. Mishchenko, “Calculations of the T matrix and the scattering matrix for ensembles of spheres,” J. Opt. Soc. Am. A 13, 2266-2278 (1996).

1995 (1)

P. Chýlek, G. Videen, D. Ngo, G. Pinnick, and J. D. Klett, “Effect of black carbon on the optical properties and climate forcing of sulphate aerosol,” J. Geophys. Res. 100, 16325-16332 (1995).
[CrossRef]

1994 (1)

1993 (1)

B. T. Draine and J. Goodmann, “Beyond Clausius-Mossotti: wave propagation on a polarizable point lattice and the discrete dipole approximation,” Astrophys. J. 405, 685-697 (1993).
[CrossRef]

1992 (1)

R. J. Charlson, S. E. Schwartz, J. M. Hales, R. D. Cess, J. A. Coakley, J. E. Hansen, and D. J. Hofmann, “Climate forcing by anthropogenic aerosols,” Science 255, 423-430 (1992).
[CrossRef]

1988 (2)

1984 (1)

P. Chýlek, V. Ramaswamy, and R. J. Cheng, “Effect of graphitic carbon on the albedo of clouds,” J. Atmos. Sci. 41, 3076-3084(1984).
[CrossRef]

1982 (1)

J. R. Ouimette and R. C. Flagan, “The extinction coefficient of multi component aerosols,” Atmos. Environ. 16, 2405-2419(1982).
[CrossRef]

1981 (1)

1973 (1)

E. M. Purcell and C. R. Pennypacker, “Scattering and absorption of light by nonspherical dielectric grains,” Astrophys. J. 186, 705-714 (1973).
[CrossRef]

Ackerman, T. P.

Anderson, J. R.

M. Pósfai, J. R. Anderson, P. R. Buseck, and H. Sievering, “Soot and sulfate aerosol particles in the remote marine troposphere,” J. Geophys. Res. 104, 21685-21693 (1999).
[CrossRef]

Ansmann, A.

A. Ansmann, U. Wandinger, A. Wiedensohler, and U. Leiterer, “Lindenberg Aerosol Characterization Experiment 1998 (LACE98): overview,” J. Geophys. Res. 107, doi: 10.1029/2000JD000233 (2002).
[CrossRef]

Artaxo, P.

J. V. Martins, P. Artaxo, C. Liousse, J. S. Reid, P. V. Hobbs, and Y. J. Kaufman, “Effects of black carbon content, particle size, and mixing on light absorption by aerosols from biomass burning in Brazil,” J. Geophys. Res. 103, 32041-32050(1998).
[CrossRef]

Baird, J. B.

N. A. Marley, J. S. Gaffney, J. B. Baird, C. A. Blazer, P. J. Drayton, and J. E. Frederick, “An empirical method for the determination of the complex refractive index of size-fractionated atmospheric aerosols for radiative transfer calculations,” Aerosol Sci. Technol. 34, 535-549 (2001).
[CrossRef]

Barnert, E. B.

B. P. Vester, M. Ebert, E. B. Barnert, J. Schneider, K. Kandler, L. Schütz, and S. Weinbruch, “Composition and mixing state of the urban background aerosol in the Rhein-Main Area (Germany),” Atmos. Environ. 41, 6102-6115 (2007).
[CrossRef]

Blazer, C. A.

N. A. Marley, J. S. Gaffney, J. B. Baird, C. A. Blazer, P. J. Drayton, and J. E. Frederick, “An empirical method for the determination of the complex refractive index of size-fractionated atmospheric aerosols for radiative transfer calculations,” Aerosol Sci. Technol. 34, 535-549 (2001).
[CrossRef]

Bohren, C. F.

C. F. Bohren and D. R. Huffman, Absorption and Scattering of Light by Small Particles (John Wiley, 1983).

Buehler, S.

J. Miao, K.-P. Johnson, S. Buehler, and A. Kokhanovsky, “The potential of polarization measurements from space at mm and sub-mm wavelength for determining cirrus cloud parameters,” Atmos. Chem. Phys. Discuss. 3, 39-48 (2003).

Bundke, U.

U. Bundke, G. Hänel, H. Horvarth, W. Kaller, S. Seidl, H. Wx, A. Wiedensohler, M. Wiegner, and V. Freudenthaler, “Aerosol optical properties during the Lindenberg Aerosol Characterization Experiment (LACE98),” J. Geophys. Res. 107, doi: 10.1029/2000JD000188 (2002).
[CrossRef]

Buseck, P. R.

M. Pósfai, J. R. Anderson, P. R. Buseck, and H. Sievering, “Soot and sulfate aerosol particles in the remote marine troposphere,” J. Geophys. Res. 104, 21685-21693 (1999).
[CrossRef]

Cess, R. D.

R. J. Charlson, S. E. Schwartz, J. M. Hales, R. D. Cess, J. A. Coakley, J. E. Hansen, and D. J. Hofmann, “Climate forcing by anthropogenic aerosols,” Science 255, 423-430 (1992).
[CrossRef]

Charlson, R. J.

R. J. Charlson, S. E. Schwartz, J. M. Hales, R. D. Cess, J. A. Coakley, J. E. Hansen, and D. J. Hofmann, “Climate forcing by anthropogenic aerosols,” Science 255, 423-430 (1992).
[CrossRef]

Cheng, R. J.

P. Chýlek, V. Ramaswamy, and R. J. Cheng, “Effect of graphitic carbon on the albedo of clouds,” J. Atmos. Sci. 41, 3076-3084(1984).
[CrossRef]

Chuang, C. C.

C. C. Chuang, J. E. Penner, K. E. Taylor, A. S. Grossman, and J. J. Walton, “An assessment of the radiative effects of anthropogenic sulphate,” J. Geophys. Res. 102, 3761-3778 (1997).
[CrossRef]

Chýlek, P.

G. Lesins, P. Chýlek, and U. Lohmann, “A study of internal and external mixing scenarios and its effects on aerosol optical properties and direct radiative forcing,” J. Geophys. Res. 107, 4094 (2002).
[CrossRef]

P. Chýlek, G. Videen, D. Ngo, G. Pinnick, and J. D. Klett, “Effect of black carbon on the optical properties and climate forcing of sulphate aerosol,” J. Geophys. Res. 100, 16325-16332 (1995).
[CrossRef]

P. Chýlek, V. Srivastava, R. G. Pinnick, and R. T. Wang, “Scattering of electromagnetic waves by composite spherical particles: experiment and effective medium approximations,” Appl. Opt. 27, 2396-2404 (1988).

P. Chýlek, V. Ramaswamy, and R. J. Cheng, “Effect of graphitic carbon on the albedo of clouds,” J. Atmos. Sci. 41, 3076-3084(1984).
[CrossRef]

P. Chýlek, G. Videen, D. J. W. Geldart, F. S. Dobbie, and H. C. W. Tso, “Effective medium approximations for heterogeneous particles,” in Light Scattering by Nonspherical Particles, M. I. Mishchenko, J. W. Hovenier, and L. D. Travis, eds. (Academic, 2000), pp. 273-308.

Coakley, J. A.

R. J. Charlson, S. E. Schwartz, J. M. Hales, R. D. Cess, J. A. Coakley, J. E. Hansen, and D. J. Hofmann, “Climate forcing by anthropogenic aerosols,” Science 255, 423-430 (1992).
[CrossRef]

Dahlback, A.

A. Kirkevåg, T. Iversen, and A. Dahlback, “On radiative effects of black carbon and sulphate aerosols,” Atmos. Environ. 33, 2621-2635 (1999).
[CrossRef]

Despiau, S.

M. Mallet, J. C. Roger, S. Despiau, J. P. Putaud, O. Dubovik, “A study of the mixing state of black carbon in urban zone,” J. Geophys. Res. 109, doi:10.1029/2003JD003940 (2004).
[CrossRef]

Dobbie, F. S.

P. Chýlek, G. Videen, D. J. W. Geldart, F. S. Dobbie, and H. C. W. Tso, “Effective medium approximations for heterogeneous particles,” in Light Scattering by Nonspherical Particles, M. I. Mishchenko, J. W. Hovenier, and L. D. Travis, eds. (Academic, 2000), pp. 273-308.

Doicu, A.

T. Wriedt and A. Doicu, “Formulations of the extended boundary condition method for three-dimensional scattering using the method of discrete sources,” J. Mod. Opt. 45, 119-213(1998).

Draine, B. T.

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

B. T. Draine and J. Goodmann, “Beyond Clausius-Mossotti: wave propagation on a polarizable point lattice and the discrete dipole approximation,” Astrophys. J. 405, 685-697 (1993).
[CrossRef]

B. T. Draine, “The discrete-dipole approximation and its application to interstellar graphite grains,” Astrophys. J. 333, 848-872 (1988).
[CrossRef]

B. T. Draine, “The discrete-dipole approximation for light scattering by irregular targets,” in Light Scattering by Nonspherical Particles, M. I. Mishchenko, J. W. Hovenier, and L. D. Travis, eds. (Academic, 2000), p. 690.

B. T. Draine and P. J. Flatau, “DDSCAT,” http://www.astro.princeton.edu/~draine (1998).

B. T. Draine, “BHMIE,” http://atol.ucsd.edu/~pflatau/scatlib (1990).

Drayton, P. J.

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R. J. Charlson, S. E. Schwartz, J. M. Hales, R. D. Cess, J. A. Coakley, J. E. Hansen, and D. J. Hofmann, “Climate forcing by anthropogenic aerosols,” Science 255, 423-430 (1992).
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U. Bundke, G. Hänel, H. Horvarth, W. Kaller, S. Seidl, H. Wx, A. Wiedensohler, M. Wiegner, and V. Freudenthaler, “Aerosol optical properties during the Lindenberg Aerosol Characterization Experiment (LACE98),” J. Geophys. Res. 107, doi: 10.1029/2000JD000188 (2002).
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M. Pósfai, J. R. Anderson, P. R. Buseck, and H. Sievering, “Soot and sulfate aerosol particles in the remote marine troposphere,” J. Geophys. Res. 104, 21685-21693 (1999).
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M. N. Eremenko, S. V. Petelina, A. Y. Zasetsky, B. Karlsson, C. P. Rinsland, E. J. Llewellyn, and J. J. Sloan, “Shape and composition of PMC particles derived from satellite remote sensing measurements,” Geophys. Res. Lett. 32, doi:10.1029/2005GL023013 (2005).
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H. Wex, C. Neusüss, M. Wendisch, F. Stratmann, C. Koziar, A. Keil, and A. Wiedensohler, “Particle scattering, backscattering, and absorption coefficients: An in situ closure and sensitivity study,” J. Geophys. Res. 107, doi:10.1029/2000JD000234 (2002).
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H. Wex, C. Neusüss, M. Wendisch, F. Stratmann, C. Koziar, A. Keil, and A. Wiedensohler, “Particle scattering, backscattering, and absorption coefficients: An in situ closure and sensitivity study,” J. Geophys. Res. 107, doi:10.1029/2000JD000234 (2002).
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H. Wex, C. Neusüss, M. Wendisch, F. Stratmann, C. Koziar, A. Keil, and A. Wiedensohler, “Particle scattering, backscattering, and absorption coefficients: An in situ closure and sensitivity study,” J. Geophys. Res. 107, doi:10.1029/2000JD000234 (2002).
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M. Kocifaj, M. Gangl, F. Kundracík, H. Horvath, G. Videen, “Simulation of the optical properties of single composite aerosols,” J. Aerosol Sci. 37, 1683-1695 (2006).
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[CrossRef]

C. C. Chuang, J. E. Penner, K. E. Taylor, A. S. Grossman, and J. J. Walton, “An assessment of the radiative effects of anthropogenic sulphate,” J. Geophys. Res. 102, 3761-3778 (1997).
[CrossRef]

M. Ebert, S. Weinbruch, A. Rausch, G. Gorzawski, G. Helas, P. Hofmann, and H. Wex, “The complex refractive index of aerosols during LACE 98 as derived from the analysis of individual particles,” J. Geophys. Res. 107, doi: 10.1029/2000JD000195, (2002).
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[CrossRef]

H. Wex, C. Neusüss, M. Wendisch, F. Stratmann, C. Koziar, A. Keil, and A. Wiedensohler, “Particle scattering, backscattering, and absorption coefficients: An in situ closure and sensitivity study,” J. Geophys. Res. 107, doi:10.1029/2000JD000234 (2002).
[CrossRef]

U. Bundke, G. Hänel, H. Horvarth, W. Kaller, S. Seidl, H. Wx, A. Wiedensohler, M. Wiegner, and V. Freudenthaler, “Aerosol optical properties during the Lindenberg Aerosol Characterization Experiment (LACE98),” J. Geophys. Res. 107, doi: 10.1029/2000JD000188 (2002).
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G. Myhre, F. Stordal, K. Restadt, and I. S. A. Isaksen, “Estimation of the radiative forcing due to sulphate and soot aerosols,” Tellus 50B, 463-477 (1998).

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P. Chýlek, G. Videen, D. J. W. Geldart, F. S. Dobbie, and H. C. W. Tso, “Effective medium approximations for heterogeneous particles,” in Light Scattering by Nonspherical Particles, M. I. Mishchenko, J. W. Hovenier, and L. D. Travis, eds. (Academic, 2000), pp. 273-308.

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Figures (7)

Fig. 1
Fig. 1

Influence of target size and dipole number on the accuracy of the DDSCAT calculations (extinction efficiency coefficient) for a spherical target. Mie calculations are given for reference.

Fig. 2
Fig. 2

Optical properties as a function of the number of discrete orientations for Euler angles β, Θ, and Φ for the internal mixing state of an ambient particle (LACE 6%) and two different diameters ( D eff ).

Fig. 3
Fig. 3

TEM bright-field images of mixed sulfate and soot particles. The bold arrows mark the particle surface, and the thin arrows mark the soot inclusions. (a),  (b) Soot inclusions are located close to the surface [(a) LACE 6%—target with 6% volume soot]. (c), (d) Soot inclusions are located in a disk close to the particle center, the so-called sandwich structure [(c) LACE 13%—target with 13% volume soot].

Fig. 4
Fig. 4

Cross section of simulated targets. The dark dots represent the soot inclusions in the sulfate matrix.

Fig. 5
Fig. 5

Optical properties as a function of particle diameter for LACE 6% (left) and LACE 13% (right) model particles (triangle-dashed line) and different simplified model geometries: (a), (b) the extinction efficiency factor; (c), (d) the scattering efficiency factor; (e), (f)  ω; (g), (h) the asymmetry parameter of the phase function; and (i), (j) the backscatter efficiency.

Fig. 6
Fig. 6

Definition and illustration of the different mixing states.

Fig. 7
Fig. 7

b abs , ω, PNC, and volume abundance of external soot and sulfate and soot-mixed particles for different ambient aerosol populations encountered during the LACE 98 field campaign. Different mixing states and soot contents (given as numbers) are considered.

Tables (3)

Tables Icon

Table 1 Refractive Indices ( λ = 550 nm ) for the Different Particle Groups Derived from Individual Particle Analysis [7]

Tables Icon

Table 2 Maximal Difference in Q ext for Coated Spheres between DDA and Mie Code BHCOAT

Tables Icon

Table 3 Comparison of the Extinction Coefficient between the Model Calculations (the Present Work) and the Polar Photometer Measurements [47]

Equations (2)

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

m = m 1 V 1 + m 2 V 2 V 1 + V 2 = n 1 V 1 + n 2 V 2 V 1 + V 2 i k 1 V 1 + k 2 V 2 V 1 + V 2 ,
b ext , abs , sca = π D 2 4 Q ext , abs , sca d N d log D d log D ,

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