ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-10-9017-2010 Optical closure experiments for biomass smoke aerosols Mack L. A. 1 Levin E. J. T. 1 Kreidenweis S. M. 1 Obrist D. 2 Moosmüller H. 2 Lewis K. A. 3 Arnott W. P. 3 McMeeking G. R. 1 6 Sullivan A. P. 1 Wold C. E. 4 Hao W.-M. 4 Collett Jr. J. L. 1 Malm W. C. 5 Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA Desert Research Institute, Nevada System of Higher Education, Reno, NV, USA Department of Physics, University of Nevada, Reno, NV, USA US Forest Service, RMRS Fire Sciences Laboratory, Missoula, MT, USA Air Resources Division, US National Park Service, Fort Collins, CO, USA now at: Centre for Atmospheric Science, University of Manchester, Manchester, UK 29 09 2010 10 18 9017 9026 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/10/9017/2010/acp-10-9017-2010.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/9017/2010/acp-10-9017-2010.pdf

A series of laboratory experiments at the Fire Laboratory at Missoula (FLAME) investigated chemical, physical, and optical properties of fresh smoke samples from combustion of wildland fuels that are burned annually in the western and southeastern US The burns were conducted in the combustion chamber of the US Forest Service Fire Sciences Laboratory in Missoula, Montana. Here we discuss retrieval of optical properties for a variety of fuels burned in FLAME 2, using nephelometer-measured scattering coefficients, photoacoustically-measured aerosol absorption coefficients, and size distribution measurements. Uncertainties are estimated from various instrument characteristics and instrument calibration studies. Our estimates of single scattering albedo for different dry smoke samples varied from 0.428 to 0.990, indicative of observed wide variations in smoke aerosol chemical composition. In selected case studies, we retrieved the complex refractive index from measurements but show that these are highly sensitive to uncertainties in measured size distributions.

 References Adler, G., Riziq, A. A., Erlick, C. and Rudich, Y.: Effect of intrinsic organic carbon on the optical properties of fresh diesel soot, Proc. Natl. Acad. Sci. USA, 107, 6699–6704, 2010. Anderson, T. L., Covert, D. S., Marshall, S. F., Laucks, M. L., Charlson, R. J., Waggoner, A. P., Ogren, J. A., Caldow, R., Holm, R. L., Quant, F. R., Sem, G. J., Wiedensohler, A., Ahlquist, N. A., and Bates, T. S.: Performance characteristics of a high-sensitivity, three-wavelength, total scatter/backscatter nephelometer, J. Atmos. Ocean. Technol., 13, 967-986, 1996. Anderson, T. L. and Ogren, J. A.: Determining aerosol radiative properties using the TSI 3563 integrating nephelometer, Aerosol Sci. Technol., 29, 57–69, 1998. Arnott, W. P., Moosmüller, H., Rogers, C. F., Jin, T. F. and Bruch, R.: Photoacoustic spectrometer for measuring light absorption by aerosol: instrument description, Atmos. Environ., 33, 2845–2852, 1999. 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. Inst., 71, 4545–4552, 2000. Bae, M. S., Schauer, J. J., DeMinter, J. T., Turner, J. R., Smith, D., and Cary, R. A.: Validation of a semi-continuous instrument for elemental carbon and organic carbon using a thermal-optical method, Atmos. Environ., 38, 2885–2893, 2004. Bond, T. C.: Can warming particles enter global climate discussions?, Environ. Res. Lett., 2, 045030, doi:10.1088/1748-9326/2/4/045030, 2007. Bond, T. C. and Bergstrom, R. W.: Light absorption by carbonaceous particles: An investigative review, Aerosol Sci. Technol., 40, 27–67, 2006. Chakrabarty, R. K., Moosmüller, H., Chen, L. W. A., Lewis, K., Arnott, W. P., Mazzoleni, C., Dubey, M. K., Wold, C. E., Hao, W. M., and Kreidenweis, S. M.: Brown carbon in tar balls from smoldering biomass combustion, Atmos. Chem. Phys., 10, 6363–6370, doi:10.5194/acp-10-6363-2010, 2010. Chakrabarty, R. K., Moosmüller, H., Garro, M. A., Arnott, W. P., Walker, J., Susott, R. A., Babbitt, R. E., Wold, C. E., Lincoln, E. N. and Hao, W. M.: Emissions from the laboratory combustion of wildland fuels: Particle morphology and size, J. Geophys. Res. Atmos., 111, D07204, doi:10.1029/2005JD006659, 2006. Chen, Y. and Bond, T. C.: Light absorption by organic carbon from wood combustion, Atmos. Chem. Phys., 10, 1773–1787, doi:10.5194/acp-10-1773-2010, 2010. Chow, J., Watson, J., Chen, L., Arnott, W., and Moosmüller, H.: Equivalence of elemental carbon by thermal/optical reflectance and transmittance with different temperature protocols, Environ. Sci. Technol., 38, 4414–4422, 2004. Chow, J., Watson, J., Pritchett, L., Pierson, W., Frazier, C., and Purcell, R.: The DRI thermal optical reflectance carbon analysis system – description, evaluation and applications in United-States air-quality studies, Atmos. Environ., 27, 1185–1201, 1993. Chow, J. C., Watson, J. G., Chen, L. W. A., Chang, M. C. O., Robinson, N. F., Trimble, D., and Kohl, S.: The IMPROVE-A temperature protocol for thermal/optical carbon analysis: maintaining consistency with a long-term database, J. Air Waste Manage. Assoc., 57, 1014–1023, 2007. Chylek, P. and Wong, J.: Effect of absorbing aerosols on global radiation budget, Geophys. Res. Lett., 22, 929–931, 1995. DeCarlo, P. F., Slowik, J. G., Worsnop, D. R., Davidovits, P., and Jimenez, J. L.: Particle morphology and density characterization by combined mobility and aerodynamic diameter measurements. Part 1: Theory, Aerosol Sci. Technol., 38, 1185–1205, 2004. Dinar, E., Riziq, A. 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. Garland, R. M., Ravishankara, A. R., Lovejoy, E. R., Tolbert, M. A., and Baynard, T.: Parameterization for the relative humidity dependence of light extinction: Organic-ammonium sulfate aerosol, J. Geophys. Res.-Atmos., 112, D19303, doi:10.1029/2006JD008179, 2007. Hand, J. L., Day, D. E., McMeeking, G. M., Levin, E. J. T., Carrico, C. M., Kreidenweis, S. M., Malm, W. C., Laskin, A., and Desyaterik, Y.: Measured and modeled humidification factors of fresh smoke particles from biomass burning: role of inorganic constituents, Atmos. Chem. Phys., 10, 6179–6194, doi:10.5194/acp-10-6179-2010, 2010. Hand, J. L. and Kreidenweis, S. M.: A new method for retrieving particle refractive index and effective density from aerosol size distribution data, Aerosol Sci. Technol., 36, 1012–1026, 2002. Levin, E. J. T., McMeeking, G. R., Carrico, C., Mack, L., Kreidenweis, S. M., Wold, C. E., Moosmüller, H., Arnott, W. P., Hao, W. M., Collett, J. L., and Malm, W. C.: Biomass burning smoke aerosol properties measured during FLAME, in review, J. Geophys. Res.-Atmos., accepted, 2010. Lewis, K., Arnott, W. P., Moosmüller, H., and Wold, C. E.: Strong spectral variation of biomass smoke light absorption and single scattering albedo observed with a novel dual-wavelength photoacoustic instrument, J. Geophys. Res.-Atmos., 113, D16203, doi:10.1029/2007JD009699, 2008. Lide, D. R.: CRC handbook of chemistry and physics [a ready-reference book of chemical and physical data], CRC Taylor & Francis, 2008. 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, doi:10.1029/2008JD011604, 2009. McMeeking, G. R., Kreidenweis, S. M., Baker, S., Carrico, C. M., Chow, J. C., Collett, J. L., Hao, W. M., Holden, A. S., Kirchstetter, T. W., Malm, W. C., Moosmüller, H., Sullivan, A. P., and Wold, C. E.: Emissions of trace gases and aerosols during the open combustion of biomass in the laboratory, J. Geophys. Res.-Atmos., 114, D19210, doi:10.1029/2009JD011836, 2009. Mikhailov, E., Vlasenko, S., Martin, S. T., Koop, T., and Pöschl, U.: Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations, Atmos. Chem. Phys., 9, 9491–9522, doi:10.5194/acp-9-9491-2009, 2009. Moosmüller, H., Chakrabarty, R. K. and Arnott, W. P.: Aerosol light absorption and its measurement: A review, J. Quant. Spectrosc. Radiat. Transfer, 110, 844–878, 2009. Park, K., Kittelson, D. B., and McMurry, P. H.: Structural properties of diesel exhaust particles measured by transmission electron microscopy (TEM): Relationships to particle mass and mobility, Aerosol Sci. Technol., 38, 881–889, 2004. Ramanathan, V. and Feng, Y.: Air pollution, greenhouse gases and climate change: Global and regional perspectives, Atmos. Environ., 43, 37–50, 2009. Ramanathan, V., Li, F., Ramana, M. V., Praveen, P. S., Kim, D., Corrigan, C. E., Nguyen, H., Stone, E. A., Schauer, J. J., Carmichael, G. R., Adhikary, B. and Yoon, S. C.: Atmospheric brown clouds: Hemispherical and regional variations in long-range transport, absorption, and radiative forcing, J. Geophys. Res.-Atmos., 112, D22S21, doi:10.1029/2006JD008124, 2007. Reid, J. S., Eck, T. F., Christopher, S. A., Koppmann, R., Dubovik, O., Eleuterio, D. P., Holben, B. N., Reid, E. A., and Zhang, J.: A review of biomass burning emissions part III: intensive optical properties of biomass burning particles, Atmos. Chem. Phys., 5, 827–849, doi:10.5194/acp-5-827-2005, 2005. Riziq, A. 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, doi:10.5194/acp-7-1523-2007, 2007. Schmid, O., Chand, D., Karg, E., Guyon, P., Frank, G. P., Swietlicki, E., and Andreae, M. O.: Derivation of the Density and Refractive Index of Organic Matter and Elemental Carbon from Closure between Physical and Chemical Aerosol Properties, Environ. Sci. Technol., 43, 1166–1172, 2009. Slowik, J. G., Stainken, K., Davidovits, P., Williams, L. R., Jayne, J. T., Kolb, C. E., Worsnop, D. R., Rudich, Y., DeCarlo, P. F., and Jimenez, J. L.: Particle morphology and density characterization by combined mobility and aerodynamic diameter measurements. Part 2: Application to combustion-generated soot aerosols as a function of fuel equivalence ratio, Aerosol Sci. Technol., 38, 1206–1222, 2004. 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. Sullivan, A. P., Holden, A. S., Patterson, L. A., McMeeking, G. R., Kreidenweis, S. M., Malm, W. C., Hao, W. M., Wold, C. E., and Collett, J. L.: A method for smoke marker measurements and its potential application for determining the contribution of biomass burning from wildfires and prescribed fires to ambient PM$_2.5$ organic carbon, J. Geophys. Res.-Atmos., 113, D22302, doi:10.1029/2008JD010216, 2008. Tang, I. N.: Chemical and size effects of hygroscopic aerosols on light scattering coefficients, J. Geophys. Res. Atmos., 101, 19245–19250, 1996. Turpin, B. J. and Lim, H. J.: Species contributions to PM$_2.5$ mass concentrations: Revisiting common assumptions for estimating organic mass, Aerosol Sci. Technol., 35, 602–610, 2001. Ward, D. E. and Radke, L. F.: Emission measurements from vegetation fires: A comparative evaluation of methods and results: Fire in the Environment: The Ecological, Atmospheric, and Climatic Importance of Vegetation Fires, edited by: P. J. Crutzen and J.-G. Goldammer, J. Wiley, Chichester, UK, 53–76, 1993.