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Black-carbon absorption enhancement in the atmosphere determined by particle mixing state

Nature Geoscience volume 10, pages 184–188 (2017)Cite this article

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Abstract

Atmospheric black carbon makes an important but poorly quantified contribution to the warming of the global atmosphere. Laboratory and modelling studies have shown that the addition of non-black-carbon materials to black-carbon particles may enhance the particles’ light absorption by 50 to 60% by refracting and reflecting light. Real-world experimental evidence for this ‘lensing’ effect is scant and conflicting, showing that absorption enhancements can be less than 5% or as large as 140%. Here we present simultaneous quantifications of the composition and optical properties of individual atmospheric black-carbon particles. We show that particles with a mass ratio of non-black carbon to black carbon of less than 1.5, which is typical of fresh traffic sources, are best represented as having no absorption enhancement. In contrast, black-carbon particles with a ratio greater than 3, which is typical of biomass-burning emissions, are best described assuming optical lensing leading to an absorption enhancement. We introduce a generalized hybrid model approach for estimating scattering and absorption enhancements based on laboratory and atmospheric observations. We conclude that the occurrence of the absorption enhancement of black-carbon particles is determined by the particles’ mass ratio of non-black carbon to black carbon.

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Figure 1: Measured and modelled optical properties as a function of mass ratio.
Figure 2: BC optical properties and mass ratios from a wide range of sources.
Figure 3: Annually averaged global distributions of MR at the surface for insoluble and soluble Aitken mode aerosol modelled using GLOMAP.

References

  1. Bond, T. C. et al. Bounding the role of black carbon in the climate system: a scientific assessment. J. Geophys. Res. 118, 5380–5552 (2013).

    Google Scholar 

  2. Bond, T. C., Habib, G. & Bergstrom, R. W. Limitations in the enhancement of visible light absorption due to mixing state. J. Geophys. Res. 111, D20211 (2006).

    Article  Google Scholar 

  3. Fuller, K. A., Malm, W. C. & Kreidenweis, S. M. Effects of mixing on extinction by carbonaceous particles. J. Geophys. Res. 104, 15941–15954 (1999).

    Article  Google Scholar 

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

    Article  Google Scholar 

  5. Adachi, K., Chung, S. H. & Buseck, P. R. Shapes of soot aerosol particles and implications for their effects on climate. J. Geophys. Res. 115, D15206 (2010).

    Article  Google Scholar 

  6. China, S., Mazzoleni, C., Gorkowski, K., Aiken, A. C. & Dubey, M. K. Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles. Nat. Commun. 4, 2122 (2013).

    Article  Google Scholar 

  7. Liu, D. et al. Single particle characterization of black carbon aerosols at a tropospheric alpine site in Switzerland. Atmos. Chem. Phys. 10, 7389–7407 (2010).

    Article  Google Scholar 

  8. Sedlacek, A. J., Lewis, E. R., Kleinman, L., Xu, J. & Zhang, Q. Determination of and evidence for non-core-shell structure of particles containing black carbon using the Single-Particle Soot Photometer (SP2). Geophys. Res. Lett. 39, L06802 (2012).

    Google Scholar 

  9. Moteki, N., Kondo, Y. & Adachi, K. Identification by single-particle soot photometer of black carbon particles attached to other particles: laboratory experiments and ground observations in Tokyo. J. Geophys. Res. 119, 1031–1043 (2014).

    Google Scholar 

  10. Ristimäki, J., Vaaraslahti, K., Lappi, M. & Keskinen, J. Hydrocarbon condensation in heavy-duty diesel exhaust. Environ. Sci. Technol. 41, 6397–6402 (2007).

    Article  Google Scholar 

  11. Liu, D. et al. The effect of complex black carbon microphysics on the determination of the optical properties of brown carbon. Geophys. Res. Lett. 42, 613–619 (2015).

    Article  Google Scholar 

  12. Moteki, N., Kondo, Y. & Nakamura, S.-I. Method to measure refractive indices of small nonspherical particles: application to black carbon particles. J. Aerosol Sci. 41, 513–521 (2010).

    Article  Google Scholar 

  13. Taylor, J. W. et al. Assessment of the sensitivity of core/shell parameters derived using the single-particle soot photometer to density and refractive index. Atmos. Meas. Tech. 8, 1701–1718 (2015).

    Article  Google Scholar 

  14. Bond, T. C. & Bergstrom, R. W. Light absorption by carbonaceous particles: an investigative review. Aerosol Sci. Tech. 40, 27–67 (2006).

    Article  Google Scholar 

  15. Cappa, C. D. et al. Radiative absorption enhancements due to the mixing state of atmospheric black carbon. Science 337, 1078–1081 (2012).

    Article  Google Scholar 

  16. Liu, S. et al. Enhanced light absorption by mixed source black and brown carbon particles in UK winter. Nat. Commun. 6, 8435 (2015).

    Article  Google Scholar 

  17. Liu, D. et al. Size distribution, mixing state and source apportionment of black carbon aerosol in London during wintertime. Atmos. Chem. Phys. 14, 10061–10084 (2014).

    Article  Google Scholar 

  18. McMeeking, G. et al. Impacts of nonrefractory material on light absorption by aerosols emitted from biomass burning. J. Geophys. Res. 119, 12272–12286 (2014).

    Google Scholar 

  19. Peng, J. et al. Markedly enhanced absorption and direct radiative forcing of black carbon under polluted urban environments. Proc. Natl Acad. Sci. USA 113, 4266–4271 (2016).

    Article  Google Scholar 

  20. Mann, G. et al. Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model. Geosci. Model Dev. 3, 519–551 (2010).

    Article  Google Scholar 

  21. Liu, D. et al. Carbonaceous aerosols contributed by traffic and solid fuel burning at a polluted rural site in Northwestern England. Atmos. Chem. Phys. 11, 1603–1619 (2011).

    Article  Google Scholar 

  22. Liu, D. et al. Size distribution, mixing state and source apportionment of black carbon aerosol in London during wintertime. Atmos. Chem. Phys. 14, 10061–10084 (2014).

    Article  Google Scholar 

  23. Canonaco, F., Crippa, M., Slowik, J., Baltensperger, U. & Prévôt, A. SoFi, an IGOR-based interface for the efficient use of the generalized multilinear engine (ME-2) for the source apportionment: ME-2 application to aerosol mass spectrometer data. Atmos. Meas. Tech. 6, 3649–3661 (2013).

    Article  Google Scholar 

  24. Crippa, M. et al. Wintertime aerosol chemical composition and source apportionment of the organic fraction in the metropolitan area of Paris. Atmos. Chem. Phys. 13, 961–981 (2013).

    Article  Google Scholar 

  25. Olfert, J. & Collings, N. New method for particle mass classification—the Couette centrifugal particle mass analyzer. J. Aerosol Sci. 36, 1338–1352 (2005).

    Article  Google Scholar 

  26. Moteki, N. & Kondo, Y. Effects of mixing state on black carbon measurements by laser-induced incandescence. Aerosol Sci. Tech. 41, 398–417 (2007).

    Article  Google Scholar 

  27. Bond, T. C. & Bergstrom, R. W. Light absorption by carbonaceous particles: an investigative review. Aerosol. Sci. Tech. 40, 27–67 (2006).

    Article  Google Scholar 

  28. Adler, G., Riziq, A. A., Erlick, C. & Rudich, Y. Effect of intrinsic organic carbon on the optical properties of fresh diesel soot. Proc. Natl Acad. Sci. USA 107, 6699–6704 (2010).

    Article  Google Scholar 

  29. Gao, R. et al. A novel method for estimating light-scattering properties of soot aerosols using a modified single-particle soot photometer. Aerosol Sci. Tech. 41, 125–135 (2007).

    Article  Google Scholar 

  30. Lack, D. A. et al. Absorption enhancement of coated absorbing aerosols: validation of the photo-acoustic technique for measuring the enhancement. Aerosol Sci. Tech. 43, 1006–1012 (2009).

    Article  Google Scholar 

  31. Liu, D. et al. The effect of complex black carbon microphysics on the determination of the optical properties of brown carbon. Geophys. Res. Lett. 42, 613–619 (2015).

    Article  Google Scholar 

  32. Park, K., Cao, F., Kittelson, D. B. & McMurry, P. H. Relationship between particle mass and mobility for diesel exhaust particles. Environ. Sci. Technol. 37, 577–583 (2003).

    Article  Google Scholar 

  33. Cross, E. S. et al. Laboratory and ambient particle density determinations using light scattering in conjunction with aerosol mass spectrometry. Aerosol Sci. Tech. 41, 343–359 (2007).

    Article  Google Scholar 

  34. Young, D. et al. Investigating the annual behaviour of submicron secondary inorganic and organic aerosols in London. Atmos. Chem. Phys. 15, 6351–6366 (2015).

    Article  Google Scholar 

  35. Nakao, S. et al. Density and elemental ratios of secondary organic aerosol: application of a density prediction method. Atmos. Environ. 68, 273–277 (2013).

    Article  Google Scholar 

  36. Abdul-Khalek, I. S. & Kittelson, D. B. Real Time Measurement of Volatile and Solid Exhaust Particles Using a Catalytic Stripper Report No. 0148-7191 (SAE Technical Paper, 1995).

    Google Scholar 

  37. Mann, G. et al. Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model. Geosci. Model Dev. 3, 519–551 (2010).

    Article  Google Scholar 

  38. Mann, G. et al. Intercomparison of modal and sectional aerosol microphysics representations within the same 3-D global chemical transport model. Atmos. Chem. Phys. 12, 4449–4476 (2012).

    Article  Google Scholar 

  39. Peña, O. & Pal, U. Scattering of electromagnetic radiation by a multilayered sphere. Comput. Phys. Comm. 180, 2348–2354 (2009).

    Article  Google Scholar 

Download references

Acknowledgements

This work was supported through the UK Natural Environment Research Council (NERC) through the Com-Part (grant ref: NE/K014838/1), ClearfLo (grant ref: NE/H003150/1), MC4 (grant ref: NE/H008136/1), SAMBBA (grant refs: NE/J010073/1; NE/J009822/1), GASSP (grant refs: NE/J023515/1; NE/J024252/1) projects and a PhD studentships for S.H. (grant ref: NE/L002469/1) and J.W.T. The studentship of E.R.-V. was supported by the National Council of Science and Technology—Mexico (CONACyT; registry no: 217687). The Manchester chamber has received funding from the European Union’s Framework 7 EUROCHAMP2 Network and currently from the Horizon 2020 research and innovation programme through the EUROCHAMP-2020 Infrastructure Activity under grant agreement no. 730997.

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Author notes

  1. Shaofei Kong

    Present address: Present address: School of Environmental Studies, China University of Geosciences (Wuhan), Wuhan 430074, China,

Authors and Affiliations

  1. Centre for Atmospheric Sciences, School of Earth and Environmental Sciences, University of Manchester, Manchester M13 9PL, UK

    Dantong Liu, James Whitehead, M. Rami Alfarra, Ernesto Reyes-Villegas, Shaofei Kong, Paul I. Williams, Yu-Chieh Ting, Sophie Haslett, Jonathan W. Taylor, Michael J. Flynn, William T. Morgan, Gordon McFiggans, Hugh Coe & James D. Allan

  2. National Centre for Atmospheric Science, Manchester M13 9PL, UK

    M. Rami Alfarra, Paul I. Williams & James D. Allan

  3. Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds LS2 9JT, UK

    Dominick V. Spracklen & Carly L. Reddington

  4. School of Atmospheric Physics, Nanjing University of Information Science & Technology, Nanjing 210044, China

    Shaofei Kong

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Contributions

J.D.A., D.L., M.R.A. and G.M. designed the research; J.D.A., D.L., J.W., M.R.A., E.R.-V., S.K., J.W.T., P.I.W., Y.-C.T., M.J.F. and S.H. performed experiments; D.L., E.R.-V., J.W.T. and W.T.M. performed data analysis; D.V.S and C.L.R. performed model simulation; D.L., J.D.A., H.C., G.M. and E.R.-V. wrote the paper.

Corresponding authors

Correspondence to Dantong Liu or James D. Allan.

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The authors declare no competing financial interests.

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Liu, D., Whitehead, J., Alfarra, M. et al. Black-carbon absorption enhancement in the atmosphere determined by particle mixing state. Nature Geosci 10, 184–188 (2017). https://doi.org/10.1038/ngeo2901

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