References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-7-1523-2007

Optical properties of absorbing and non-absorbing aerosols retrieved by cavity ring down (CRD) spectroscopy

Abo Riziq

¹ Erlick

² Dinar

¹ Rudich

Department of Environmental Sciences, Weizmann Institute of Science, Rehovot 76100, Israel

Department of Atmospheric Sciences, The Hebrew University of Jerusalem, Jerusalem 91904, Israel

21 03 2007

7 6 1523 1536

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

This article is available from http://www.atmos-chem-phys.net/7/1523/2007/acp-7-1523-2007.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/7/1523/2007/acp-7-1523-2007.pdf

Application of cavity ring down (CRD) spectrometry for measuring the optical properties of pure and mixed laboratory-generated aerosols is presented. The extinction coefficient (αext), extinction cross section (σext) and extinction efficiency (Qext) were measured for polystyrene spheres (PSS), ammonium sulphate ((NH4)2(SO4), sodium chloride (NaCl), glutaric acid (GA), and Rhodamine-590 aerosols. The refractive indices of the different aerosols were retrieved by comparing the measured extinction efficiency of each aerosol type to the extinction predicted by Mie theory. Aerosols composed of sodium chloride and glutaric acid in different mixing ratios were used as model for mixed aerosols of two non-absorbing materials, and their extinction and complex refractive index were derived. Aerosols composed of Rhodamine-590 and ammonium sulphate in different mixing ratios were used as model for mixing of absorbing and non-absorbing species, and their optical properties were derived. The refractive indices of the mixed aerosols were also calculated by various optical mixing rules. We found that for non-absorbing mixtures, the linear rule, Maxwell-Garnett rule, and extended effective medium approximation (EEMA), give comparable results, with the linear mixing rule giving a slightly better fit than the others. Overall, calculations for the mixed aerosols are not as good as for single component aerosols. For absorbing mixtures, the differences between the refractive indices calculated using the mixing rules and those retrieved by CRD are generally higher.

References 1

Bates, T. S., Anderson, T. L., Baynard, T., Bond, T., Boucher, O., Carmichael, G., Clarke, A., Erlick, C., Guo, H., Horowitz, L., Howell, S., Kulkarni, S., Maring, H., McComiskey, A., Middlebrook, A., Noone, K., O'Dowd, C. D., Ogren, J., Penner, J., Quinn, P. K., Ravishankara, A. R., Savoie, D. L., Schwartz, S. E., Shinozuka, Y., Tang, Y., Weber, R. J., and Wu, Y.: Aerosol direct radiative effects over the northwest atlantic, northwest pacific, and north indian oceans: Estimates based on in-situ chemical and optical measurements and chemical transport modeling, Atmos. Chem. Phys., 6, 1657–1732, 2006.

Bellouin, N., Boucher, O., Haywood, J., and Reddy, M. S.: Global estimate of aerosol direct radiative forcing from satellite measurements, Nature, 438, 1138–1141, 2005.

Bohren, C. F. and Huffman, D. R.: Absorption and scattering of light by small particles, Wiley, New York, 1983.

Bohren, C. F. and Clothiaux, E. E.: Fundamentals of atmospheric radiation, Wiley-VCH, 2006.

Born, M. and Wolf, E.: Principles of optics, 7th ed., Cambridge University Press, 1999.

Brown, S. S., Stark, H., Ciciora, S. J., McLaughlin, R. J., and Ravishankara, A. R.: Simultaneous in situ detection of atmospheric no3 and n2o5 via cavity ring-down spectroscopy, Rev. Sci. Inst., 73, 3291–3301, 2002.

Bulatov, V., Chen, Y. H., Khalmanov, A., and Schechter, I.: Absorption and scattering characterization of airborne microparticulates by a cavity ringdown technique, Anal. Bioanal. Chem., 384, 155–160, 2006.

Bulatov, V., Fisher, M., and Schechter, I.: Aerosol analysis by cavity-ring-down laser spectroscopy, Analytica Chimica Acta, 466, 1–9, 2002.

Ch\'ylek, P., Videen, G., Geldart, D. J. W., Dobbie, J. S., and Tso, H. C. W.: Effective medium approximations for heterogeneous particles, in: Light scattering by nonspherical particles, theory, measurements, and applications, pp. 273–308, edited by: Mishchenko, M. I., Hovenier, J. W., and Travis, L. D., Academic Press, 2000.

Chylek, P., Ramaswamy, V., and Cheng, R. J.: Effect of graphitic carbon on the albedo of clouds, J. Atmos. Sci., 41, 3076–3084, 1984.

d'Almeida, G. A., Koepke, P., and Shettle, E. P.: Atmospheric aerosols, global climatology and radiative characteristics, A. Deepak Publishing, Hampton, Va, 1991.

Erlick, C.: Effective refractive indices of water and sulfate drops containing absorbing inclusions, J. Atmos. Sci., 63, 754–763, 2006.

Falkovich, A. H., Schkolnik, G., Ganor, E., and Rudich, Y.: Adsorption of organic compounds pertinent to urban environments onto mineral dust particles, J. Geophys. Res., 109, D02208, doi:10.1029/2003JD003919, 2004.

Gosse, S. F., Wang, M. Y., Labrie, D., and Chylek, P.: Imaginary part of the refractive index of sulfates and nitrates in the o.7–2.8 mum spectral region, Appl. Opt., 36, 3622–3634, 1997.

Hansen, J., Sato, M., Ruedy, R., Nazarenko, L., Lacis, A., Schmidt, G. A., Russell, G., Aleinov, I., Bauer, M., Bauer, S., Bell, N., Cairns, B., Canuto, V., Chandler, M., Cheng, Y., Del Genio, A., Faluvegi, G., Fleming, E., Friend, A., Hall, T., Jackman, C., Kelley, M., Kiang, N., Koch, D., Lean, J., Lerner, J., Lo, K., Menon, S., Miller, R., Minnis, P., Novakov, T., Oinas, V., Perlwitz, J., Perlwitz, J., Rind, D., Romanou, A., Shindell, D., Stone, P., Sun, S., Tausnev, N., Thresher, D., Wielicki, B., Wong, T., Yao, M., and Zhang, S.: Efficacy of climate forcings, J. Geophys. Res., 110, D18104, doi:10.1029/2005JD005776, 2005.

Jacobson, M. C.: Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols, Nature, 409, 695–697, 2001.

Jacobson, M. Z.: Analysis of aerosol interactions with numerical techniques for solving coagulation, nucleation, condensation, dissolution, and reversible chemistry among multiple size distributions, J. Geophys. Res., 107(D19), 4366, doi:10.1029/2001JD002044, 2002.

Jacobson, M. Z.: Effects of externally-through-internally-mixed soot inclusions within clouds and precipitation on global climate, J. Phys. Chem. A, 110, 6860–6873, 2006.

Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: A review, Atmos. Chem. Phys., 5, 1053–1123, 2005.

Kaufman, Y. J., Koren, I., Remer, L. A., Rosenfeld, D., and Rudich, Y.: The effect of smoke, dust, and pollution aerosol on shallow cloud development over the atlantic ocean, Proc. Natl. Acad. Sci. USA, 102, 11 207–11 212, 2005.

Kaufman, Y. J., Tanre, D., and Boucher, O.: A satellite view of aerosols in the climate system, Nature, 419, 215–223, 2002.

Koren, I., Kaufman, Y. J., Remer, L. A., and Martins, J. V.: Measurement of the effect of amazon smoke on inhibition of cloud formation, Science, 303, 1342–1345, 2004.

Lack, D. A., Lovejoy, E. R., Baynard, T., Pettersson, A., and Ravishankara, A. R.: Aerosol absorption measurement using photoacoustic spectroscopy: Sensitivity, calibration, and uncertainty developments, Aerosol. Sci. Technol., 40, 697–708, 2006.

Lide, D. R.: Crc handbook of chemistry and physics, 78 ed., CRC Press LLC, Boca Raton, Florida, USA, 1997.

Lohmann, U. and Feichter, J.: Global indirect aerosol effects: A review, Atmos. Chem. Phys., 5, 715–737, 2005.

Maria, S. F., Russell, L. M., Gilles, M. K., and Myneni, S. C. B.: Organic aerosol growth mechanisms and their climate-forcing implications, Science, 306, 1921–1924, 2004.

Menon, S., Hansen, J., Nazarenko, L., and Luo, Y.: Climate effects of black carbon aerosols in china and india, Science, 297, 2250–2253, 2002.

Moosmuller, H., Varma, R., and Arnott, W. P.: Cavity ring-down and cavity-enhanced detection techniques for the measurement of aerosol extinction, Aero. Sci. Tech., 39, 30–39, 2005.

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, doi:10.1029/2006JD007340, 2006.

O'Keefe, A. and Deacon, D. A. G.: Cavity ring-down optical spectrometer for absorption-measurements using pulsed laser sources, Rev. Sci. Inst., 59, 2544–2551, 1988.

Pettersson, A., Lovejoy, E. R., Brock, C. A., Brown, S. S., and Ravishankara, A. R.: Measurement of aerosol optical extinction at 532 nm with pulsed cavity ring down spectroscopy, J. Aerosol Sci., 35, 995–1011, 2004.

Posfai, M., Xu, H. F., Anderson, J. R., and Buseck, P. R.: Wet and dry sizes of atmospheric aerosol particles: An afm-tem study, Geophys. Res. Lett., 25, 1907–1910, 1998.

Press, W. H., Teukolsky, S. A., Vetterling, W. T., and Flannery, B. R.: Numerical recipes in c, the art of scientific computer, 2nd edition, Cambridge University Press, New York, 1992.

Ramanathan, V., Chung, C., Kim, D., Bettge, T., Buja, L., Kiehl, J. T., Washington, W. M., Fu, Q., Sikka, D. R., and Wild, M.: Atmospheric brown clouds: Impacts on south asian climate and hydrological cycle, Proc. Natl. Acad. Sci. USA, 102, 5326–5333, 2005.

Ramanathan, V., Crutzen, P. J., Kiehl, J. T., and Rosenfeld, D.: Atmosphere - aerosols, climate, and the hydrological cycle, Science, 294, 2119–2124, 2001.

Russell, L. M., Maria, S. F., and Myneni, S. C. B.: Mapping organic coatings on atmospheric particles, Geophys. Res. Lett., 29, 16, doi:10.1029/2002GL014874, 2002.

Sappey, A. D., Hill, E. S., Settersten, T., and Linne, M. A.: Fixed-frequency cavity ringdown diagnostic for atmospheric particulate matter, Optics Lett., 23, 954–956, 1998.

Scherer, J. J., Paul, J. B., Collier, C. P., OKeefe, A., Rakestraw, D. J., and Saykally, R. J.: Cavity ringdown laser spectroscopy: A new ultrasensitive absorption technique, Spectroscopy, 11, 46–50, 1996.

Scherer, J. J., Paul, J. B., OKeefe, A., and Saykally, R. J.: Cavity ringdown laser absorption spectroscopy: History, development, and application to pulsed molecular beams, Chem. Rev., 97, 25–51, 1997.

Sihvola, A. and Sharma, R.: Scattering corrections for maxwell garnett mixing rule, Microwave and Optical Technology Letters, 22, 229–231, 1999.

Smith, J. D. and Atkinson, D. B.: A portable pulsed cavity ring-down transmissometer for measurement of the optical extinction of the atmospheric aerosol, Analyst, 126, 1216–1220, 2001.

Stelson, A. W.: Urban aerosol refractive-index prediction by partial molar refraction approach, Environ. Sci. Technol., 24, 1676–1679, 1990.

Strawa, A. W., Castaneda, R., Owano, T., Baer, D. S., and Paldus, B. A.: The measurement of aerosol optical properties using continuous wave cavity ring-down techniques, J. Atmos. Oceanic Technol., 20, 454–465, 2003.

Tang, I. N.: Thermodynamic and optical properties of mixed-salt aerosols of atmospheric importance, J. Geophys. Res., 102, 1883–1893, 1997.

Tervahattu, H., Hartonen, K., Kerminen, V. M., Kupiainen, K., Aarnio, P., Koskentalo, T., Tuck, A. F., and Vaida, V.: New evidence of an organic layer on marine aerosols, J. Geophys. Res., 107, 4053, 2002.

Thompson, J. E., Smith, B. W., and Winefordner, J. D.: Monitoring atmospheric particulate matter through cavity ring-down spectroscopy, Anal. Chem., 74, 1962–1967, 2002.

Vander Wal, R. L. and Ticich, T. M.: Cavity ringdown and laser-induced incandescence measurements of soot, Appl. Opt., 38, 1444–1451, 1999.

Yu, H., Kaufman, Y. J., Chin, M., Feingold, G., Remer, L. A., Anderson, T. L., Balkanski, Y., Bellouin, N., Boucher, O., Christopher, S., DeCola, P., Kahn, R., Koch, D., Loeb, N., Reddy, M. S., Schulz, M., Takemura, T., and Zhou, M.: A review of measurement-based assessments of the aerosol direct radiative effect and forcing, Atmos. Chem. Phys., 6, 613–666, 2006.