References

AMTD

Atmospheric Measurement Techniques Discussions

AMTD

1867-8610

Copernicus GmbH

Göttingen, Germany

10.5194/amtd-4-6315-2011

Initial investigation of the wavelength dependence of optical properties measured with a new multi-pass aerosol extinction differential optical absorption spectrometer (AE-DOAS)

Chartier

R. T.

¹ Greenslade

M. E.

¹ ²

University of New Hampshire, Department of Chemistry, Durham, NH 03824, USA

now at: RTI International, Research Triangle Park, NC, USA

12 10 2011

4 5 6315 6349

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-meas-tech-discuss.net/4/6315/2011/amtd-4-6315-2011.html

The full text article is available as a PDF file from http://www.atmos-meas-tech-discuss.net/4/6315/2011/amtd-4-6315-2011.pdf

Atmospheric aerosols directly affect climate by scattering and absorbing radiation. The magnitude of the impact is dependent upon the wavelength of light, but is often estimated near 550 nm. When light scattering and absorption by aerosols is approximated, the wavelength dependence of the refractive index for specific components is lost. As a result, climate models would have inherent uncertainties for aerosol contributions to radiative forcing when considering the entire solar spectrum. An aerosol extinction differential optical absorption spectrometer has been developed to directly measure aerosol extinction at mid-ultraviolet to near infrared wavelengths. The instrument consists of a spectrometer coupled to a closed White-type multi-pass gas cell with an adjustable path length of up to approximately 20 m. Laboratory measurements of various gases are compared with known absorption cross sections. Additionally, the extinction of monodisperse samples of polystyrene latex spheres are measured and compared to Mie theory generated with refractive index values from the literature to validate the new instrument. The polystyrene experiments also emphasize the ability of the new instrument to retrieve the wavelength dependent refractive index, especially in the ultraviolet wavelength regions where variability is expected. The spectrometer will be a significant advancement for determining wavelength dependent complex refractive indices in future laboratory studies as well as provide the ability to monitor ambient aerosol light extinction.

References 1

Abo Riziq, A., Erlick, C., Dinar, E., and Rudich, Y.: Optical properties of absorbing and non-absorbing aerosols retrieved by cavity ring down (CRD) spectroscopy, Atmos. Chem. Phys., 7, 1523–1536, http://dx.doi.org/10.5194/acp-7-1523-2007doi:10.5194/acp-7-1523-2007, 2007.

AIRMAP: http://airmap.unh.edu/, last access: 29 September 2011.

Andreae, M. O. and Gelencsér, A.: Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols, Atmos. Chem. Phys., 6, 3131–3148, http://dx.doi.org/10.5194/acp-6-3131-2006doi:10.5194/acp-6-3131-2006, 2006.

Andreae, M. O., Schmid, O., Yang, H., Chand, D., Yu, J. Z., Zeng, L. M., and Zhang, Y. H.: Optical properties and chemical composition of the atmospheric aerosol in urban Guangzhou, China, Atmos. Environ., 42, 6335–6350, 2008.

Ångström, A.: On the atomspheric transmission of sun radiation and on dust in the air, Geografiska Ann. A., 11, 156–166, 1929.

Ångström, A.: On the atmospheric transmission of sun radiaiton. II., Geografiska Ann. A., 12, 130–159, 1930.

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, http://dx.doi.org/10.5194/acp-6-1657-2006doi:10.5194/acp-6-1657-2006, 2006.

Baynard, T., Lovejoy, E. R., Pettersson, A., Brown, S. S., Lack, D., Osthoff, H., Massoli, P., Ciciora, S., Dube, W. P., and Ravishankara, A. R.: Design and application of a pulsed cavity ring-down aerosol extinction spectrometer for field measurements, Aerosol Sci. Technol., 41, 447–462, 2007.

Bergstrom, R. W., Russell, P. B., and Hignett, P.: Wavelength dependence of the absorption of black carbon particles: Predictions and results from the TARFOX experiment and implications for the aerosol single scattering albedo, J. Atmos. Sci., 59, 567–577, 2002.

Bogumil, K., Orphal, J., Homann, T., Voigt, S., Spietz, P., Fleischmann, O. C., Vogel, A., Hartmann, M., Kromminga, H., Bovensmann, H., Frerick, J., and Burrows, J. P.: Measurements of molecular absorption spectra with the SCIAMACHY pre-flight model: instrument characterization and reference data for atmospheric remote-sensing in the 230–2380 nm region, J. Photoch. Photobio. A., 157, 167–184, 2003.

Bohren, C. F. and Huffman, D. K.: Absorption and Scattering of Light by Small Particles, Wiley, New York, 1983.

Bond Research Group: Aerosol characterization: Mie calculation: http://www.hiwater.org/Mie_calcs.html, last access: 29 September 2011.

Bond, T. C.: Spectral dependence of visible light absorption by carbonaceous particles emitted from coal combustion, Geophys. Res. Lett., 28, 4075–4078, 2001.

Bond, T. C. and Bergstrom, R. W.: Light absorption by carbonaceous particles: An investigative review, Aerosol Sci. Technol., 40, 27–67, 2006.

Bones, D. L., Henricksen, D. K., Mang, S. A., Gonsior, M., Bateman, A. P., Nguyen, T. B., Cooper, W. J., and Nizkorodov, S. A.: Appearance of strong absorbers and fluorophores in limonene-O<sub>3</sub> secondary organic aerosol due to NH$_4^+$-mediated chemical aging over long time scales, J. Geophys. Res.-Atmos., 115, D05203, http://dx.doi.org/10.1029/2009JD012864doi:10.1029/2009JD012864, 2010.

Boundy, R. H. and Boyer, R. F. (Eds.): Styrene, Its Polymers, Copolymers and Derivatives, Reinhold Publishing Corp., NY, 523–525, 1952.

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

Butler, T. J. A., Mellon, D., Kim, J., Litman, J., and Orr-Ewing, A. J.: Optical-Feedback Cavity Ring-Down Spectroscopy Measurements of Extinction by Aerosol Particles, J. Phys. Chem. A., 113, 3963–3972, 2009.

Cai, Y., Zelenyuk, A., and Imre, D.: A high resolution study of the effect of morphology on the mass spectra of single PSL particles with Na-containing layers and nodules, Aerosol Sci. Technol., 40, 1111–1122, 2006.

Chen, Y. and Bond, T. C.: Light absorption by organic carbon from wood combustion, Atmos. Chem. Phys., 10, 1773–1787, http://dx.doi.org/10.5194/acp-10-1773-2010doi:10.5194/acp-10-1773-2010, 2010.

Dinar, E., Abo Riziq, A., Spindler, C., Erlick, C., Kiss, G., and Rudich, Y.: The complex refractive index of atmospheric and model humic-like substances (HULIS) retrieved by a cavity ring down aerosol spectrometer (CRD-AS), Faraday Discuss., 137, 279–295, 2008.

Eck, T. F., Holben, B. N., Reid, J. S., Dubovik, O., Smirnov, A., O'Neill, N. T., Slutsker, I., and Kinne, S.: Wavelength dependence of the optical depth of biomass burning, urban, and desert dust aerosols, J. Geophys. Res.-Atmos., 104, 31333–31349, 1999.

Erlick, C., Haspel, M., and Rudich, Y.: Simultaneous retrieval of the complex refractive indices of the core and shell of coated aerosol particles from extinction measurements using simulated annealing, Appl. Optics, 50, 4393–4402, 2011.

Flores, J. M., Trainic, M., Borrmann, S., and Rudich, Y.: Effective broadband refractive index retrieval by a white light optical particle counter, Phys. Chem. Chem. Phys., 11, 7943–7950, 2009.

Freedman, M. A., Hasenkopf, C. A., Beaver, M. R., and Tolbert, M. A.: Optical Properties of Internally Mixed Aerosol Particles Composed of Dicarboxylic Acids and Ammonium Sulfate, J. Phys. Chem. A, 113, 13584–13592, 2009.

French, R. H., Winey, K. I., Yang, M. K., and Qiu, W. M.: Optical properties and van der Waals-London dispersion interactions of polystyrene determined by vacuum ultraviolet spectroscopy and spectroscopic ellipsometry, Aust. J. Chem., 60, 251–263, 2007.

Galli, M., Guazzotti, S. A., and Prather, K. A.: Improved lower particle size limit for aerosol time-of-flight mass spectrometry, Aerosol Sci. Technol., 34, 381–385, 2001.

Ge, J. M., Su, J., Ackerman, T. P., Fu, Q., Huang, J. P., and Shi, J. S.: Dust aerosol optical properties retrieval and radiative forcing over northwestern China during the 2008 China-US joint field experiment, J. Geophys. Res.-Atmos., 115, D00K12, http://dx.doi.org/10.1029/2009JD013263doi:10.1029/2009JD013263, 2010.

Hecobian, A., Zhang, X., Zheng, M., Frank, N., Edgerton, E. S., and Weber, R. J.: Water-Soluble Organic Aerosol material and the light-absorption characteristics of aqueous extracts measured over the Southeastern United States, Atmos. Chem. Phys., 10, 5965–5977, http://dx.doi.org/10.5194/acp-10-5965-2010doi:10.5194/acp-10-5965-2010, 2010.

Hoffer, A., Gelencsér, A., Guyon, P., Kiss, G., Schmid, O., Frank, G. P., Artaxo, P., and Andreae, M. O.: Optical properties of humic-like substances (HULIS) in biomass-burning aerosols, Atmos. Chem. Phys., 6, 3563–3570, http://dx.doi.org/10.5194/acp-6-3563-2006doi:10.5194/acp-6-3563-2006, 2006.

Hönninger, G., von Friedeburg, C., and Platt, U.: Multi axis differential optical absorption spectroscopy (MAX-DOAS), Atmos. Chem. Phys., 4, 231–254, http://dx.doi.org/10.5194/acp-4-231-2004doi:10.5194/acp-4-231-2004, 2004.

IPCC: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Solomon, S., D. Qin, M. Manning, Z. Chen, M. Marquis, K.B. Averyt, M. Tignor and H.L. Miller, Cambridge University Press, Cambridge, UK and New York, US, 996, 2007.

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, http://dx.doi.org/10.5194/acp-5-1053-2005doi:10.5194/acp-5-1053-2005, 2005.

Kim, H., Barkey, B., and Paulson, S. E.: Real refractive indices of alpha- and beta-pinene and toluene secondary organic aerosols generated from ozonolysis and photo-oxidation, J. Geophys. Res.-Atmos., 115, D24212, http://dx.doi.org/10.1029/2010JD014549doi:10.1029/2010JD014549, 2010.

Kirchstetter, T. W., Novakov, T., and Hobbs, P. V.: Evidence that the spectral dependence of light absorption by aerosols is affected by organic carbon, J. Geophys. Res.-Atmos., 109, D21208, http://dx.doi.org/10.1029/2004JD004999doi:10.1029/2004JD004999, 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.

Lang-Yona, M., Rudich, Y., Segre, E., Dinar, E., and Abo-Riziq, A.: Complex Refractive Indices of Aerosols Retrieved by Continuous Wave-Cavity Ring Down Aerosol Spectrometer, Anal. Chem., 81, 1762–1769, 2009.

Lang-Yona, N., Abo-Riziq, A., Erlick, C., Segre, E., Trainic, M., and Rudich, Y.: Interaction of internally mixed aerosols with light, Phys. Chem. Chem. Phys., 12, 21–31, 2010.

Liu, B. Y. H., Romay, F. J., Dick, W. D., Woo, K. S., and Chiruta, M.: A Wide-Range Particle Spectrometer for Aerosol Measurement from 0.010 μm to 10 μm, Aerosol Air Qual. Res., 10, 125–139, 2010.

Ma, X. Y., Lu, J. Q., Brock, R. S., Jacobs, K. M., Yang, P., and Hu, X. H.: Determination of complex refractive index of polystyrene microspheres from 370 to 1610 nm, Phys. Med. Biol., 48, 4165–4172, 2003.

Mack, L. A., Levin, E. J. T., Kreidenweis, S. M., Obrist, D., Moosmüller, H., Lewis, K. A., Arnott, W. P., McMeeking, G. R., Sullivan, A. P., Wold, C. E., Hao, W.-M., Collett Jr., J. L., and Malm, W. C.: Optical closure experiments for biomass smoke aerosols, Atmos. Chem. Phys., 10, 9017–9026, http://dx.doi.org/10.5194/acp-10-9017-2010doi:10.5194/acp-10-9017-2010, 2010.

Marley, N. A., Gaffney, J. S., Tackett, M., Sturchio, N. C., Heraty, L., Martinez, N., Hardy, K. D., Marchany-Rivera, A., Guilderson, T., MacMillan, A., and Steelman, K.: The impact of biogenic carbon sources on aerosol absorption in Mexico City, Atmos. Chem. Phys., 9, 1537–1549, http://dx.doi.org/10.5194/acp-9-1537-2009doi:10.5194/acp-9-1537-2009, 2009.

Massoli, P., Kebabian, P. L., Onasch, T. B., Hills, F. B., and Freedman, A.: Aerosol Light Extinction Measurements by Cavity Attenuated Phase Shift (CAPS) Spectroscopy: Laboratory Validation and Field Deployment of a Compact Aerosol Particle Extinction Monitor, Aerosol Sci. Technol., 44, 428–435, 2010.

Massoli, P., Bates, T. S., Quinn, P. K., Lack, D. A., Baynard, T., Lerner, B. M., Tucker, S. C., Brioude, J., Stohl, A., and Williams, E. J.: Aerosol optical and hygroscopic properties during TexAQS-GoMACCS 2006 and their impact on aerosol direct radiative forcing, J. Geophys. Res.-Atmos., 114, D00F07, http://dx.doi.org/10.1029/2008JD011604doi:10.1029/2008JD011604, 2009.

Mätzler, C.: MATLAB Functions for Mie Scattering and Absorption – Version 2. Research Report (No 2002-11), Institut für Angewandte Physik, 2002.

Mellon, D., King, S. J., Kim, J., Reid, J. P., and Orr-Ewing, A. J.: Measurements of Extinction by Aerosol Particles in the Near-Infrared Using Continuous Wave Cavity Ring-Down Spectroscopy, J. Phys. Chem. A, 115, 774–783, 2011.

Meyrahn, H., Pauly, J., Schneider, W., and Warneck, P.: Quantum Yields for the Photodissociation of Acetone in Air and an Estimate for the Life Time of Acetone in the Lower Troposphere, J. Atmos. Chem., 4, 277–291, 1986.

Miles, R. E. H., Rudic, S., Orr-Ewing, A. J., and Reid, J. P.: Influence of Uncertainties in the Diameter and Refractive Index of Calibration Polystyrene Beads on the Retrieval of Aerosol Optical Properties Using Cavity Ring Down Spectroscopy, J. Phys. Chem. A, 114, 7077–7084, 2010a.

Miles, R. E. H., Rudic, S., Orr-Ewing, A. J., and Reid, J. P.: Measurements of the wavelength dependent extinction of aerosols by cavity ring down spectroscopy, Phys. Chem. Chem. Phys., 12, 3914–3920, 2010b.

Moffet, R. C. and Prather, K. A.: In-situ measurements of the mixing state and optical properties of soot with implications for radiative forcing estimates, P. Natl. Acad. Sci. USA, 106, 11872–11877, 2009.

Mogili, P. K., Yang, K. H., Young, M. A., Kleiber, P. D., and Grassian, V. H.: Environmental aerosol chamber studies of extinction spectra of mineral dust aerosol components: Broadband IR-UV extinction spectra, J. Geophys. Res.-Atmos., 112, D21204, http://dx.doi.org/10.1029/2007JD008890doi:10.1029/2007JD008890, 2007.

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

Moosmüller, H., Chakrabarty, R. K., Ehlers, K. M., and Arnott, W. P.: Absorption Ångström coefficient, brown carbon, and aerosols: basic concepts, bulk matter, and spherical particles, Atmos. Chem. Phys., 11, 1217–1225, http://dx.doi.org/10.5194/acp-11-1217-2011doi:10.5194/acp-11-1217-2011, 2011.

Nikolov, I. D. and Ivanov, C. D.: Optical plastic refractive measurements in the visible and the near-infrared regions, Appl. Optics, 39, 2067–2070, 2000.

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.

Platt, U. and Stutz, J.: Differential Optical Absorption Spectroscopy: Principles and Applications, Springer, New York, 2008.

Schnaiter, M., Horvath, H., Mohler, O., Naumann, K. H., Saathoff, H., and Schock, O. W.: UV-VIS-NIR spectral optical properties of soot and soot-containing aerosols, J. Aerosol Sci., 34, 1421–1444, 2003.

Schnaiter, M., Schmid, O., Petzold, A., Fritzsche, L., Klein, K. F., Andreae, M. O., Helas, G., Thielmann, A., Gimmler, M., Mohler, O., Linke, C., and Schurath, U.: Measurement of wavelength-resolved light absorption by aerosols utilizing a UV-VIS extinction cell, Aerosol Sci. Technol., 39, 249–260, 2005.

Si, F. Q., Xie, P. H., Dou, K., Zhan, K., Liu, Y., Xu, J., and Liu, W. Q.: Determination of the atmospheric aerosol optical density by multi axis differential optical absorption spectroscopy, Acta Phys. Sin.-Ch Ed., 59, 2867–2872, 2010.

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.

Spindler, C., Riziq, A. A., and Rudich, Y.: Retrieval of aerosol complex refractive index by combining cavity ring down aerosol spectrometer measurements with full size distribution information, Aerosol Sci. Technol., 41, 1011–1017, 2007.

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. Ocean. Tech., 20, 454–465, 2003.

Strawa, A. W., Elleman, R., Hallar, A. G., Covert, D., Ricci, K., Provencal, R., Owano, T. W., Jonsson, H. H., Schmid, B., Luu, A. P., Bokarius, K., and Andrews, E.: Comparison of in situ aerosol extinction and scattering coefficient measurements made during the Aerosol Intensive Operating Period, J. Geophys. Res., 111, D05S03, http://dx.doi.org/10.1029/2005JD006056doi:10.1029/2005JD006056, 2006.

Takashima, H., Irie, H., Kanaya, Y., Shimizu, A., Aoki, K., and Akimoto, H.: Atmospheric aerosol variations at Okinawa Island in Japan observed by MAX-DOAS using a new cloud-screening method, J. Geophys. Res.-Atmos., 114, D18213, http://dx.doi.org/10.1029/2009JD011939doi:10.1029/2009JD011939, 2009.

Thermo Fisher Scientific: http://www.thermo.fr/eThermo/CMA/PDFs/Various/File_3936.pdf, last access: 29 September 2011.

Thermo Fisher Scientific: http://www.thermoscientific.com/wps/portal/ts/products/detail?navigationId=L10397&categoryId=87439&productId=11962886, last access: 29 September 2011.

Virkkula, A., Ahlquist, N. C., Covert, D. S., Sheridan, P. J., Arnott, W. P., and Ogren, J. A.: A three-wavelength optical extinction cell for measuring aerosol light extinction and its application to determining light absorption coefficient, Aerosol Sci. Technol., 39, 52–67, 2005.

Voigt, S., Orphal, J., Bogumil, K., and Burrows, J. P.: The temperature dependence (203–293~K) of the absorption cross sections of O<sub>3</sub> in the 230–850 nm region measured by Fourier-transform spectroscopy, J. Photoch. Photobio. A, 143, 1–9, 2001.

White, J. U.: Long optical paths of large aperture, J. Opt. Soc. Am., 32, 285–288, 1942.

Yang, M., Howell, S. G., Zhuang, J., and Huebert, B. J.: Attribution of aerosol light absorption to black carbon, brown carbon, and dust in China – interpretations of atmospheric measurements during EAST-AIRE, Atmos. Chem. Phys., 9, 2035–2050, http://dx.doi.org/10.5194/acp-9-2035-2009doi:10.5194/acp-9-2035-2009, 2009.