Atmospheric Chemistry and Physics
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10.5194/acp-6-3443-2006
http://www.atmos-chem-phys.net/6/3443/2006/
http://www.atmos-chem-phys.net/6/3443/2006/acp-6-3443-2006.html
http://www.atmos-chem-phys.net/6/3443/2006/acp-6-3443-2006.pdf
3443
3462
2006-08-21
Spectral light absorption by ambient aerosols influenced by biomass burning in the Amazon Basin. I: Comparison and field calibration of absorption measurement techniques
O. Schmid
oschmid@mpch-mainz.mpg.de
P. Artaxo
W. P. Arnott
D. Chand
L. V. Gatti
G. P. Frank
A. Hoffer
M. Schnaiter
M. O. Andreae
Max Planck Institute for Chemistry, Department of Biogeochemistry, P.O. Box 3060, 55020 Mainz, Germany
University of São Paulo, Institute of Physics, São Paulo, Brazil
Desert Research Institute, Division of Atmospheric Science, Reno, NV, USA
Institute of Nuclear Energy Research, Atmospheric Chemistry Laboratory, São Paulo, SP, Brazil
Research Center Karlsruhe, Institute of Meteorology and Climate Research, P.O.~Box 3640, 76021 Karlsruhe, Germany
now at: GSF-Research Center for Environment and Health, Institute for Inhalation Biology, P.O. Box 1129, 85758 Neuherberg/Munich, Germany
Spectral aerosol light absorption is an important parameter for the
assessment of the radiation budget of the atmosphere. Although on-line
measurement techniques for aerosol light absorption, such as the
Aethalometer and the Particle Soot Absorption Photometer (PSAP), have been
available for two decades, they are limited in accuracy and spectral
resolution because of the need to deposit the aerosol on a filter substrate
before measurement. Recently, a 7-wavelength (λ) Aethalometer
became commercially available, which covers the visible (VIS) to
near-infrared (NIR) spectral range (λ=450–950 nm), and
laboratory calibration studies improved the degree of confidence in these
measurement techniques. However, the applicability of the laboratory
calibration factors to ambient conditions has not been investigated
thoroughly yet.
<P>
As part of the LBA-SMOCC (Large scale Biosphere atmosphere experiment in
Amazonia – SMOke aerosols, Clouds, rainfall and Climate) campaign from
September to November 2002 in the Amazon basin we performed an extensive
field calibration of a 1-λ PSAP and a 7-λ Aethalometer
utilizing a photoacoustic spectrometer (PAS, 532 nm) as reference device.
Especially during the dry period of the campaign, the aerosol population was
dominated by pyrogenic emissions. The most pronounced artifact of
integrating-plate type attenuation techniques (e.g. Aethalometer, PSAP) is
due to multiple scattering effects within the filter matrix. For the PSAP,
we essentially confirmed the laboratory calibration factor by Bond et al. (1999).
On the other hand, for the Aethalometer we found a multiple
scattering enhancement of 5.23 (or 4.55, if corrected for aerosol
scattering), which is significantly larger than the factors previously
reported (~2) for laboratory calibrations. While the exact reason for
this discrepancy is unknown, the available data from the present and
previous studies suggest aerosol mixing (internal versus external) as a
likely cause. For Amazonian aerosol, we found no absorption enhancement due
to hygroscopic particle growth in the relative humidity (<i>RH</i>) range between
40% and 80%. However, a substantial bias in PSAP sensitivity that
correlated with both <i>RH</i> and temperature (T) was observed for 20%<<i>RH</i><30%
and 24°C<T<26°C, respectively. In addition,
both PSAP and Aethalometer demonstrated no sensitivity to gaseous
adsorption. Although very similar in measurement principle, the PSAP and
Aethalometer require markedly different correction factors, which is
probably due to the different filter media used. Although on-site
calibration of the PSAP and Aethalometer is advisable for best data
quality, we recommend a set of "best practice" correction factors for
ambient sampling based on the data from the present and previous studies.
For this study, the estimated accuracies of the absorption coefficients
determined by the PAS, PSAP and Aethalometer were 10, 15 and 20% (95%
confidence level), respectively.
Ackerman, A. S., Toon, O. B., Stevens, D. E., Heymsfield, A. J., Ramanathan, V., and Welton, E. J.: Reduction of tropical cloudiness by soot, Science, 288, 1042–1047, 2000.
Andreae, M. O., Artaxo, P., Brandão, C., Carswell, F. E., Ciccioli, P., da Costa, A. L., Culf, A. D., Esteves, J. L., Gash, J. H. C., Grace, J., Kabat, P., Lelieveld, J., Malhi, Y., Manzi, A. O., Meixner, F. X., Nobre, A. D., Nobre, C., Ruivo, M. D. L. P., Silva-Dias, M. A., Stefani, P., Valentini, R., von Jouanne, J., and Waterloo, M. J.: Biogeochemical cycling of carbon, water, energy, trace gases and aerosols in Amazonia: The LBA-EUSTACH experiments, J. Geophys. Res., 107, 8066, doi:10.1029/2001JD000524, 2002.
Andreae, M. O., Rosenfeld, D., Artaxo, P., Costa, A. A., Frank, G. P., Longo, K. M., and Silva-Dias, M. A. F.: Smoking rain clouds over the Amazon, Science, 303, 1337–1342, 2004.
Arnott, W. P., Hamasha, K., Moosmüller, H., Sheridan, P. J., and Ogren, J. A.: Towards aerosol light-absorption measurements with a 7-wavelength aethalometer: Evaluation with a photoacoustic instrument and 3-wavelength nephelometer, Aerosol Sci. Technol., 39, 17–29, 2005.
Arnott, W. P., Moosmüller, H., Rogers, C. F., Jin, T., and Bruch, R.: Photoacoustic spectrometer for measuring light absorption by aerosol: Instrument description, Atmos. Environ., 33, 2845–2852, 1999.
Arnott, W. P., Moosmüller, H., Sheridan, P. J., Ogren, J. A., Raspet, R., Slaton, W. V., Hand, J. L., Kreidenweis, S. M., and Collett, J. L.: Photoacoustic and filter-based ambient aerosol light absorption measurements: Instrument comparisons and the role of relative humidity, J. Geophys. Res., 108, 4034, doi:10.1029/2002JD002165, 2003.
Arnott, W. P., Moosmüller, H., and Walker, J. W.: Nitrogen dioxide and kerosene-flame soot calibration of photoacoustic instruments for measurement of light absorption by aerosols, Rev. Sci. Instrum., 71, 4545–4552, 2000.
Ballach, J., Hitzenberger, R., Schultz, E., and Jaeschke, W.: Development of an improved optical transmission technique for black carbon (BC) analysis, Atmos. Environ., 35, 2089–2100, 2001.
Bohren, C. F. and Huffman, D. R.: Absorption and scattering of light by small particles, Wiley, New York, USA, 1983.
Bond, T. C., Anderson, T. L., and Campbell, D.: Calibration and intercomparison of filter-based measurements of visible light absorption by aerosols, Aerosol Sci. Technol., 30, 582–600, 1999.
Chand, D., Guyon, P., Artaxo, P., Schmid, O., Frank, G. P., Rizzo, L. V., Mayol-Bracero, O. L., Gatti, L. V., and Andreae, M. O.: Optical and physical properties of aerosols in the boundary layer and free troposphere over the Amazon Basin during the biomass burning season, Atmos. Chem. Phys, 6, 2911–2925, 2006.
Dubovik, O., Holben, B., Eck, T. F., Smirnov, A., Kaufman, Y. J., King, M. D., Tanre, D., and Slutsker, I.: Variability of absorption and optical properties of key aerosol types observed in worldwide locations, J. Atmos. Sci. 59, 590–608, 2002
Fuller, K. A., Malm, W. C., and Kreidenweis, S. M.: Effects of mixing on extinction by carbonaceous particles, J. Geophys. Res.-Atmos., 104, 15 941–15 954, 1999.
Gundel, L. A., Dod, R. L., Rosen, H., and Novakov, T.: The relationship between optical attenuation and black carbon concentration for ambient and source particles, Sci. Total Environ., 36, 197–202, 1984.
Guyon, P., Boucher, O., Graham, B., Beck, J., Mayol-Bracero, O. L., Roberts, G. C., Maenhaut, W., Artaxo, P., and Andreae, M. O.: Refractive index of aerosol particles over the Amazon tropical forest during LBA-EUSTACH 1999, J. Aerosol Sci., 34, 883–907, 2003a.
Guyon, P., Graham, B., Beck, J., Boucher, O., Gerasopoulos, E., Mayol-Bracero, O. L., Roberts, G. C., Artaxo, P., and Andreae, M. O.: Physical properties and concentration of aerosol particles over the Amazon tropical forest during background and biomass burning conditions, Atmos. Che. Phys., 3, 951–967, 2003b.
Guyon, P., Graham, B., Roberts, G. C., Mayol-Bracero, O. L., Maenhaut, W., Artaxo, P., and Andreae, M. O.: Sources of optically active aerosol particles over the Amazon forest, Atmos. Environ., 38, 1039–1051, 2004.
Hansen, A. D. A., Rosen, H., and Novakov, T.: The aethalometer – an instrument for the real-time measurement of optical absorption by aerosol particles, Sci. Total Environ., 36, 191–196, 1984.
Heintzenberg, J. and Charlson, R. J.: Design and applications of the integrating nephelometer: A review, American Meteorological Society, 13, 987–1000, 1996.
Horvath, H.: Atmospheric light-absorption – a review, Atmospheric Environment Part a – General Topics, 27, 293–317, 1993.
Kirchstetter, T. W., Corrigan, C. E., and Novakov, T.: Laboratory and field investigation of the adsorption of gaseous organic compounds onto quartz filters, Atmos. Environ., 35, 1663–1671, 2001.
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, 1208, doi:10.1029/2004JD004999, 2004.
Kirkman, G. A., Gut, A., Ammann, C., Gatti, L. V., Cordova, A. M., Moura, M. A. L., Andreae, M. O., and Meixner, F. X.: Surface exchange of nitric oxide, nitrogen dioxide, and ozone at a cattle pasture in Rondonia, Brazil, J. Geophys. Res., 107, 8083, doi:10.1029/2001JD000523, 2002.
Kopp, C., Petzold, A., and Niessner, R.: Investigation of the specific attenuation cross-section of aerosols deposited on fiber filters with a polar photometer to determine black carbon, J. Aerosol Sci., 30, 1153–1163, 1999.
Liousse, C., Cachier, H., and Jennings, S. G.: Optical and thermal measurements of black carbon aerosol content in different environments: Variation of the specific attenuation cross-section, sigma (s), Atmos. Environ., 27A, 1203–1211, 1993.
Mader, B. T., Flagan, R. C., and Seinfeld, J. H.: Airborne measurements of atmospheric carbonaceous aerosols during ACE-Asia, J. Geophys. Res., 23, 4704, doi:10.1029/2002JD002221, 2002.
Marple, V. A., Rubow, K. L., and Behm, S. M.: A Microorifice Uniform Deposit Impactor (Moudi) – Description, Calibration, and Use, Aerosol Sci. Technol., 14, 434–446, 1991.
McMurry, P. H.: A review of atmospheric aerosol measurements, Atmos. Environ., 34, 1959–1999, 2000.
Moosmüller, H., Arnott, W. P., Rogers, C. F., Chow, J. C., Frazier, C. A., Sherman, L. E., and Dietrich, D. L.: Photoacoustic and filter measurements related to aerosol light absorption during the Northern Front Range Air Quality Study (Colorado 1996/1997), J. Geophys. Res.-Atmos., 103, 28 149–28 157, 1998.
Penner, J. E., Andreae, M. O., Annegarn, H., Barrie, L., Feichter, J., Hegg, D., Jayaraman, A., Leaitch, R., Murphy, D., Nganga, J., and Pitari, G.: Aerosols, their Direct and Indirect Effects, in: Climate Change 2001: The Scientific Basis. Contribution of Working Group I to the Third Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Houghton, J. T., Ding, Y., Griggs, D. J., Noguer, M., van der Linden, P. J., Dai, X., Maskell, K., and Johnson, C. A., p. 289–348, Cambridge University Press, Cambridge, UK, and New York, NY, USA, 2001.
Petzold, A., Kopp, C., and Niessner, R.: The dependence of the specific attenuation cross section on black carbon mass fraction and particle size, Atmos. Environ., 31, 661–672, 1997.
Petzold, A., Schloesser, H., Sheridan, P. J., Arnott, W. P., Ogren, J. A., and Virkkula, A.: Evaluation of multiangle absorption photometry for measuring aerosol light absorption, Aerosol Sci. Technol., 39, 40–51, 2005.
Petzold, A. and Schönlinner, M.: Multi-angle absorption photometry – a new method for the measurement of aerosol light absorption and atmospheric black carbon, J. Aerosol Sci., 35, 421–441, 2004.
Raspet, R., Slaton, W. V., Arnott, W. P., and Moosmüller, H.: Evaporation-condensation effects on resonant photoacoustics of volatile aerosols, J. Atmos. Oceanic Technol., 20, 685–695, 2003.
Redemann, J., Russell, P. B., and Hamill, P.: Dependence of aerosol light absorption and single-scattering albedo on ambient relative humidity for sulfate aerosols with black carbon cores, J. Geophys. Res.-Atmos., 106, 27 485–27 495, 2001.
Reid, J. S., Hobbs, P. V., Liousse, C., Martins, J. V., Weiss, R. E., and Eck, T. F.: Comparisons of techniques for measuring shortwave absorption and black carbon content of aerosols from biomass burning in Brazil, J. Geophys. Res.-Atmos., 103, 32 031–32 040, 1998.
Rissler, J., Vestin, A., Swietlicki, E., Fisch, G., Zhou, J., Artaxo, P., and Andreae, M. O.: Size distribution and hygroscopic properties of aerosol particles from dry-season biomass burning in Amazonia, Atmos. Chem. Phys., 6, 471–491, 2006.
Rosencwaig, A.: Photoacoustics and photoacoustic spectroscopy, Wiley, New York, 1980.
Saathoff, H., Moehler, O., Schurath, U., Kamm, S., Dippel, B., and Mihelcic, D.: The AIDA soot aerosol characterisation campaign 1999, J. Aerosol Sci., 34, 1277–1296, 2003.
Schmid, H., Laskus, L., Abraham, H. J., Baltensperger, U., Lavanchy, V., Bizjak, M., Burba, P., Cachier, H., Crow, D., Chow, J., Gnauk, T., Even, A., ten Brink, H. M., Giesen, K. P., Hitzenberger, R., Hueglin, E., Maenhaut, W., Pio, C., Carvalho, A., Putaud, J. P., Toom-Sauntry, D., and Puxbaum, H.: Results of the "carbon conference" international aerosol carbon round robin test stage I, Atmos. Environ., 35, 2111–2121, 2001.
Schnaiter, M., Schmid, O., Petzold, A., Fritzsche, L., Klein, K.-F., Andreae, M. O., Helas, G., Thielmann, A., Gimmler, M., Möhler, 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.
Sheridan, P. J., Arnott, W. P., Ogren, J. A., Andrews, E., Atkinson, D. B., Covert, D. S., Moosmüller, H., Petzold, A., Schmid, B., Strawa, A. W., Varma, R., and Virkkula, A.: The Reno aerosol optics study: An evaluation of aerosol absorption measurement methods, Aerosol Sci. Technol., 39, 1–16, 2005.
Terhune, R. W. and Anderson, J. E.: Spectrophone measurements of the absorption of visible light by aerosols in the atmosphere, Opt. Lett., 1, 70–72, 1977.
Truex, T. J. and Anderson, J. E.: Mass monitoring of carbonaceous aerosols with a spectrophone, Atmos. Environ., 13, 507–509, 1979.
Virkkula, A., Ahlquist, N. C., Covert, D. S., Arnott, W. P., Sheridan, P. J., Quinn, P. K., and Coffman, D. J.: Modification, calibration and a field test of an instrument for measuring light absorption by particles, Aerosol Sci. Technol., 39, 68–83, 2005a.
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, 2005b.
Weingartner, E., Saathoff, H., Schnaiter, M., Streit, N., Bitnar, B., and Baltensperger, U.: Absorption of light by soot particles: determination of the absorption coefficient by means of aethalometers, J. Aerosol Sci., 34, 1445–1463, 2003.
Wex, H., Neususs, C., Wendisch, M., Stratmann, F., Koziar, C., Keil, A., Wiedensohler, A., and Ebert, M.: Particle scattering, backscattering, and absorption coefficients: An in situ closure and sensitivity study, J. Geophys. Res.-Atmos., 107, 8122, doi:10.1029/2000JD000234, 2002.