Modeled source apportionment of black carbon particles coated with a light-scattering shell

Atmospheric Measurement Techniques - Tập 14 Số 5 - Trang 3707-3719
Aki Virkkula1
1Atmospheric Composition Research, Finnish Meteorological Institute, Helsinki, Finland

Tóm tắt

Abstract. The Aethalometer model has been used widely for estimating the contributions of fossil fuel emissions and biomass burning to equivalent black carbon (eBC). The calculation is based on measured absorption Ångström exponents (αabs). The interpretation of αabs is ambiguous since it is well known that it not only depends on the dominant absorber but also on the size and internal structure of the particles, core size, and shell thickness. In this work the uncertainties of the Aethalometer-model-derived apparent fractions of absorption by eBC from fossil fuel and biomass burning are evaluated with a core–shell Mie model. Biomass-burning fractions (BB(%)) were calculated for pure and coated single BC particles for lognormal unimodal and bimodal size distributions of BC cores coated with ammonium sulfate, a scattering-only material. BB(%) was very seldom 0 % even though BC was the only absorbing material in the simulations. The shape of size distribution plays an important role. Narrow size distributions result in higher αabs and BB(%) values than wide size distributions. The sensitivity of αabs and BB(%) to variations in shell volume fractions is the highest for accumulation-mode particles. This is important because that is where the largest aerosol mass is. For the interpretation of absorption Ångström exponents it would be very good to measure BC size distributions and shell thicknesses together with the wavelength dependency of absorption.

Từ khóa


Tài liệu tham khảo

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

Arola, A., Schuster, G., Myhre, G., Kazadzis, S., Dey, S., and Tripathi, S. N.: Inferring absorbing organic carbon content from AERONET data, Atmos. Chem. Phys., 11, 215–225, https://doi.org/10.5194/acp-11-215-2011, 2011.

Bergstrom, R. W., Pilewskie, P., Russell, P. B., Redemann, J., Bond, T. C., Quinn, P. K., and Sierau, B.: Spectral absorption properties of atmospheric aerosols, Atmos. Chem. Phys., 7, 5937–5943, https://doi.org/10.5194/acp-7-5937-2007, 2007.

Bond, T. C. and Bergstrom, R. W.: Light Absorption by Carbonaceous Particles: An Investigative Review, Aerosol Sci. Technol., 40, 27–67, 2006.

Bond, T. C., Doherty, S. J., Fahey, D. W., Forster, P. M., Berntsen, T., DeAngelo, B. J., Flanner, M. G., Ghan, S., Kärcher, B., Koch, D., Kinne, S., Kondo, Y., Quinn, P. K., Sarofim, M. C., Schultz, M. G., Schulz, M., Venkataraman, C., Zhang, H., Zhang, S., Bellouin, N., Guttikunda, S. K., Hopke, P. K., Jacobson, M. Z., Kaiser, J. W., Klimont, Z., Lohmann, U., Schwarz, J. P., Shindell, D., Storelvmo, T., Warren, S. G., and Zender, C.S.: Bounding the role of black carbon in the climate system: A scientific assessment, J. Geophys. Res.-Atmos., 118, 5380–5552, https://doi.org/10.1002/jgrd.50171, 2013.

Cazorla, A., Bahadur, R., Suski, K. J., Cahill, J. F., Chand, D., Schmid, B., Ramanathan, V., and Prather, K. A.: Relating aerosol absorption due to soot, organic carbon, and dust to emission sources determined from in-situ chemical measurements, Atmos. Chem. Phys., 13, 9337–9350, https://doi.org/10.5194/acp-13-9337-2013, 2013.

Chung, C., Ramanathan, V., and Decremer, D.: Observationally constrained estimates of carbonaceous aerosol radiative forcing, P. Natl. Acad. Sci. USA, 109, 11624–11629, 2012.

Chylek, P., Lee, J. E., Romonosky, D. E., Gallo, F., Lou, S., Shrivastava, M., Carrico, C. M., Aiken, A. C., and Dubey, M. K.: Mie scattering captures observed optical properties of ambient biomass burning plumes assuming uniform black, brown, and organic carbon mixtures, J. Geophys. Res.-Atmos., 124, 11406–11427, https://doi.org/10.1029/2019JD031224, 2019.

Devi, J. J., Bergin, M., McKenzie, M., Schauer, J. J., and Weber, R.: Contribution of particulate brown carbon to light absorption in the rural and urban Southeast US, Atmos. Environ., 136, 95–104, 2016.

Feng, Y., Ramanathan, V., and Kotamarthi, V. R.: Brown carbon: a significant atmospheric absorber of solar radiation?, Atmos. Chem. Phys., 13, 8607–8621, https://doi.org/10.5194/acp-13-8607-2013, 2013.

Fuller, G. W., Tremper, A. H., Baker, T. D., Yttri, K. E., and Butterfield, D.: Contribution of wood burning to PM10 in London, Atmos. Environ., 87, 87–94, 2014.

Gyawali, M., Arnott, W. P., Lewis, K., and Moosmüller, H.: In situ aerosol optics in Reno, NV, USA during and after the summer 2008 California wildfires and the influence of absorbing and non-absorbing organic coatings on spectral light absorption, Atmos. Chem. Phys., 9, 8007–8015, https://doi.org/10.5194/acp-9-8007-2009, 2009.

Harrison, R. M., Beddows, D. C., Jones, A. M., Calvo, A., Alves, C., and Pio, C.: An evaluation of some issues regarding the use of aethalometers to measure woodsmoke concentrations, Atmos. Environ., 80, 540–548, 2013.

Healy, R., Sofowote, U., Su, Y., Debosz, J., Noble, M., Jeong, C.-H., Wang, J., Hilker, N., Evans, G., and Doerksen, G.: Ambient measurements and source apportionment of fossil fuel and biomass burning black carbon in Ontario, Atmos. Environ., 161, 34–47, 2017.

Helin, A., Niemi, J., Virkkula, A., Pirjola, L., Teinilä, K., Backman, J., Aurela, M., Saarikoski, S., Rönkkö, T., Asmi, E., and Timonen, H.: Characteristics and source apportionment of black carbon in the Helsinki metropolitan area, Finland, Atmos. Environ., 190, 87–98, https://doi.org/10.1016/j.atmosenv.2018.07.022, 2018.

Herich, H., Hueglin, C., and Buchmann, B.: A 2.5 year's source apportionment study of black carbon from wood burning and fossil fuel combustion at urban and rural sites in Switzerland, Atmos. Meas. Tech., 4, 1409–1420, https://doi.org/10.5194/amt-4-1409-2011, 2011.

Kirchstetter, T. W. and Thatcher, T. L.: Contribution of organic carbon to wood smoke particulate matter absorption of solar radiation, Atmos. Chem. Phys., 12, 6067–6072, https://doi.org/10.5194/acp-12-6067-2012, 2012.

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., 109, D21208, https://doi.org/10.1029/2004JD004999, 2004.

Kondo, Y., Sahu, L., Moteki, N., Khan, F., Takegawa, N., Liu, X., Koike, M., and Miyakawa, T.: Consistency and traceability of black carbon measurements made by laser-induced incandescence, thermal-optical transmittance, and filter-based photo-absorption techniques, Aerosol Sci. Technol., 45, 295–312, https://doi.org/10.1080/02786826.2010.533215, 2011.

Lack, D. A. and Cappa, C. D.: Impact of brown and clear carbon on light absorption enhancement, single scatter albedo and absorption wavelength dependence of black carbon, Atmos. Chem. Phys., 10, 4207–4220, https://doi.org/10.5194/acp-10-4207-2010, 2010.

Lack, D. A. and Langridge, J. M.: On the attribution of black and brown carbon light absorption using the Ångström exponent, Atmos. Chem. Phys., 13, 10535–10543, https://doi.org/10.5194/acp-13-10535-2013, 2013.

Lack, D. A., Langridge, J. M., Bahreini, R., Cappa, C. D., Middlebrook, A. M., and Schwarz, J. P.: Brown carbon and internal mixing in biomass burning particles, P. Natl. Acad. Sci. USA, 109, 14802–14807, 2012.

Laskin, A., Laskin, J., and Nizkorodov, S. A.: Chemistry of Atmospheric Brown Carbon, Chem. Rev., 115, 4335–4382, https://doi.org/10.1021/cr5006167, 2015.

Liu, C., Chung, C. E., Yin, Y., and Schnaiter, M.: The absorption Ångström exponent of black carbon: from numerical aspects, Atmos. Chem. Phys., 18, 6259–6273, https://doi.org/10.5194/acp-18-6259-2018, 2018.

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, https://doi.org/10.5194/acp-11-1217-2011, 2011.

Moteki, N., Kondo, Y., Miyazaki, Y., Takegawa, N., Komazaki, Y., Kurata, G., Shirai, T., Blake, D. R., Miyakawa, T., and Koike, M.: Evolution of mixing state of black carbon particles: Aircraft measurements over the western Pacific in March 2004, Geophys. Res. Lett., 34, L11803, https://doi.org/10.1029/2006GL028943, 2007.

Russell, P. B., Bergstrom, R. W., Shinozuka, Y., Clarke, A. D., DeCarlo, P. F., Jimenez, J. L., Livingston, J. M., Redemann, J., Dubovik, O., and Strawa, A.: Absorption Angstrom Exponent in AERONET and related data as an indicator of aerosol composition, Atmos. Chem. Phys., 10, 1155–1169, https://doi.org/10.5194/acp-10-1155-2010, 2010.

Saleh, R., Hennigan, C. J., McMeeking, G. R., Chuang, W. K., Robinson, E. S., Coe, H., Donahue, N. M., and Robinson, A. L.: Absorptivity of brown carbon in fresh and photo-chemically aged biomass-burning emissions, Atmos. Chem. Phys., 13, 7683–7693, https://doi.org/10.5194/acp-13-7683-2013, 2013.

Sandradewi, J., Prevot, A. S. H., Szidat, S., Perron, N., Alfarra, M. R., Lanz, V. A., Weingartner, E., and Baltensperger, U.: Using aerosol light absorption measurements for the quantitative determination of wood burning and traffic emission contributions to particulate matter, Environ. Sci. Technol., 42, 3316–3323, 2008a.

Sandradewi, J., Prevot, A. S. H., Weingartner, E., Schmidhauser, R., Gysel, M., and Baltensperger, U.: A study of wood burning and traffic aerosols in an Alpine valley using a multi-wavelength Aethalometer, Atmos. Environ., 42, 101–112, 2008b.

Schuster, G. L., Dubovik, O., Arola, A., Eck, T. F., and Holben, B. N.: Remote sensing of soot carbon – Part 2: Understanding the absorption Ångström exponent, Atmos. Chem. Phys., 16, 1587–1602, https://doi.org/10.5194/acp-16-1587-2016, 2016.

Schwarz, J. P., Gao, R. S., Spackman, J. R., Watts, L. A., Thomson, D. S., Fahey, D. W., Ryerson, T. B., Peischl, J., Holloway, J. S., Trainer, M., Frost, G. J., Baynard, T., Lack, D. A., de Gouw, J. A., Warneke, C., and Del Negro, L. A.: Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions, Geophys. Res. Lett., 35, L13810, https://doi.org/10.1029/2008GL033968, 2008.

Shen, Y., Virkkula, A., Ding, A., Wang, J., Chi, X., Nie, W., Qi, X., Huang, X., Liu, Q., Zheng, L., Xu, Z., Petäjä, T., Aalto, P. P., Fu, C., and Kulmala, M.: Aerosol optical properties at SORPES in Nanjing, east China, Atmos. Chem. Phys., 18, 5265–5292, https://doi.org/10.5194/acp-18-5265-2018, 2018.

Shiraiwa, M., Kondo, Y., Moteki, N., Takegawa, N., Sahu, L. K., Takami, A., Hatakeyama, S., Yonemura, S., and Blake, D. R.: Radiative impact of mixing state of black carbon aerosol in Asian outflow, J. Geophys. Res., 113, D24210, https://doi.org/10.1029/2008JD010546, 2008.

Valenzuela, A., Olmo, F. J., Lyamani, H., Antón, M., Titos, G., Cazorla, A., and Alados-Arboledas, L.: Aerosol scattering and absorption Angström exponents as indicators of dust and dust-free days over Granada (Spain), Atmos. Res., 154, 1–13, 2015.

Voshchinnikov, N. V. and Mathis, J. S.: Calculating Cross Sections of Composite Interstellar Grains, Astrophys. J., 526, 257–264, https://doi.org/10.1086/307997, 1999 (code available at: http://www.astro.spbu.ru/staff/ilin2/SOFTWARE/nmie0.html, last access: 21 May 2021).

Wang, X., Heald, C. L., Sedlacek, A. J., de Sá, S. S., Martin, S. T., Alexander, M. L., Watson, T. B., Aiken, A. C., Springston, S. R., and Artaxo, P.: Deriving brown carbon from multiwavelength absorption measurements: method and application to AERONET and Aethalometer observations, Atmos. Chem. Phys., 16, 12733–12752, https://doi.org/10.5194/acp-16-12733-2016, 2016.

Wu, Z. P. and Wang, Y. P.: Electromagnetic scattering for multilayered spheres: recursive algorithms, Radio Science, 26, 1393–1401, 1991.

Zhang, X., Mao, M., Yin, Y., and Tang, S.: The absorption Ångstrom exponent of black carbon with brown coatings: effects of aerosol microphysics and parameterization, Atmos. Chem. Phys., 20, 9701–9711, https://doi.org/10.5194/acp-20-9701-2020, 2020.

Zotter, P., Herich, H., Gysel, M., El-Haddad, I., Zhang, Y., Močnik, G., Hüglin, C., Baltensperger, U., Szidat, S., and Prévôt, A. S. H.: Evaluation of the absorption Ångström exponents for traffic and wood burning in the Aethalometer-based source apportionment using radiocarbon measurements of ambient aerosol, Atmos. Chem. Phys., 17, 4229–4249, https://doi.org/10.5194/acp-17-4229-2017, 2017.