Article | Published:

Major secondary aerosol formation in southern African open biomass burning plumes

Nature Geoscience (2018) | Download Citation


Open biomass burning contributes significantly to air quality degradation and associated human health impacts over large areas. It is one of the largest sources of reactive trace gases and fine particles to Earth’s atmosphere and consequently a major source of cloud condensation nuclei on a global scale. However, there is a large uncertainty in the climate effect of open biomass burning aerosols due to the complexity of their constituents. Here, we present an exceptionally large dataset on southern African savannah and grassland fire plumes and their atmospheric evolution, based on 5.5 years of continuous measurements from 2010 to 2015. We find that the mass of submicrometre aerosols more than doubles on average, in only three hours of daytime ageing. We also evaluate biomass burning aerosol particle size distributions and find a large discrepancy between the observations and current model parameterizations, especially in the 30–100 nm range. We conclude that accounting for near-source secondary organic aerosol formation and using measurement-based size distribution parameterizations in smoke plumes is essential to better constrain the climate and air quality effects of savannah and grassland fires.

Access optionsAccess options

Rent or Buy article

Get time limited or full article access on ReadCube.

from $8.99

All prices are NET prices.

Additional information

Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.


  1. 1.

    Andreae, M. O. & Merlet, P. Emission of trace gases and aerosols from biomass burning. Global Biogeochem. Cycles 15, 955–966 (2001).

  2. 2.

    van der Werf, G. R. et al. Global fire emissions estimates during 1997–2016. Earth Syst. Sci. Data 9, 697–720 (2017).

  3. 3.

    Akagi, S. K. et al. Emission factors for open and domestic biomass burning for use in atmospheric models. Atmos. Chem. Phys. 11, 4039–4072 (2011).

  4. 4.

    Hatch, L. E. et al. Multi-instrument comparison and compilation of non-methane organic gas emissions from biomass burning and implications for smoke-derived secondary organic aerosol precursors. Atmos. Chem. Phys. 17, 1471–1489 (2017).

  5. 5.

    Johnston, F. H. et al. Estimated global mortality attributable to smoke from landscape fires. Environ. Health Perspect. 120, 695–701 (2012).

  6. 6.

    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).

  7. 7.

    Spracklen, D. V., Carslaw, K. S., Pöschl, U., Rap, A. & Forster, P. M. Global cloud condensation nuclei influenced by carbonaceous combustion aerosol. Atmos. Chem. Phys. 11, 9067–9087 (2011).

  8. 8.

    Reid, J. S., Koppmann, R., Eck, T. F. & Eleuterio, D. P. A review of biomass burning emissions part II: intensive physical properties of biomass burning particles. Atmos. Chem. Phys. 5, 799–825 (2005).

  9. 9.

    Janhäll, S., Andreae, M. O. & Pöschl, U. Biomass burning aerosol emissions from vegetation fires: particle number and mass emission factors and size distributions. Atmos. Chem. Phys. 10, 1427–1439 (2010).

  10. 10.

    Engelhart, G. J., Hennigan, C. J., Miracolo, M. A., Robinson, A. L. & Pandis, S. N. Cloud condensation nuclei activity of fresh primary and aged biomass burning aerosol. Atmos. Chem. Phys. 12, 7285–7293 (2012).

  11. 11.

    Liu, S. et al. Aerosol single scattering albedo dependence on biomass combustion efficiency: laboratory and field studies. Geophys. Res. Lett. 41, 742–748 (2013).

  12. 12.

    May, A. A. et al. Aerosol emissions from prescribed fires in the United States: a synthesis of laboratory and aircraft measurements. J. Geophys. Res. Atmos. 119, 11826–11849 (2014).

  13. 13.

    Saleh, R. et al. Brownness of organics in aerosols from biomass burning linked to their black carbon content. Nat. Geosci. 7, 647–650 (2014).

  14. 14.

    Liu, X. et al. Agricultural fires in the southeastern US during SEAC4RS: emissions of trace gases and particles and evolution of ozone, reactive nitrogen, and organic aerosol. J. Geophys. Res. Atmos. 121, 7383–7414 (2016).

  15. 15.

    Liu, X. et al. Airborne measurements of western US wildfire emissions: comparison with prescribed burning and air quality implications. J. Geophys. Res. Atmos. 122, 6108–6129 (2017).

  16. 16.

    Yokelson, R. J. et al. Emissions from biomass burning in the Yucatan. Atmos. Chem. Phys. 9, 5785–5812 (2009).

  17. 17.

    Akagi, S. K. et al. Evolution of trace gases and particles emitted by a chaparral fire in California. Atmos. Chem. Phys. 12, 1397–1421 (2012).

  18. 18.

    Vakkari, V. et al. Rapid changes in biomass burning aerosols by atmospheric oxidation. Geophys. Res. Lett. 41, 2644–2651 (2014).

  19. 19.

    Carrico, C. M. et al. Rapidly evolving ultrafine and fine mode biomass smoke physical properties: comparing laboratory and field results. J. Geophys. Res. Atmos. 121, 5750–5768 (2016).

  20. 20.

    Jolleys, M. D. et al. Characterizing the aging of biomass burning organic aerosol by use of mixing ratios: a meta-analysis of four regions. Environ. Sci. Technol. 46, 13093–13102 (2012).

  21. 21.

    May, A. A. et al. Observations and analysis of organic aerosol evolution in some prescribed fire smoke plumes. Atmos. Chem. Phys. 15, 6323–6335 (2015).

  22. 22.

    Collier, S. et al. Regional Influence of aerosol emissions from wildfires driven by combustion efficiency: insights from the BBOP campaign. Environ. Sci. Technol. 50, 8613–8622 (2016).

  23. 23.

    Tkacik, D. S. et al. A dual-chamber method for quantifying the effects of atmospheric perturbations on secondary organic aerosol formation from biomass burning emissions. J. Geophys. Res. Atmos. 122, 6043–6058 (2017).

  24. 24.

    Kondo, Y. et al. Emissions of black carbon, organic, and inorganic aerosols from biomass burning in North America and Asia in 2008. J. Geophys. Res. Atmos. 116, D08204 (2011).

  25. 25.

    Bian, Q. et al. Secondary organic aerosol formation in biomass-burning plumes: theoretical analysis of lab studies and ambient plumes. Atmos. Chem. Phys. 17, 5459–5475 (2017).

  26. 26.

    Labonne, M., Bréon, F.-M. & Chevallier, F. Injection height of biomass burning aerosols as seen from a spaceborne lidar. Geophys. Res. Lett. 34, L11806 (2007).

  27. 27.

    Roberts, G., Wooster, M. J. & Lagoudakis, E. Annual and diurnal african biomass burning temporal dynamics. Biogeosciences 6, 849–866 (2009).

  28. 28.

    Reddington, C. L. et al. Analysis of particulate emissions from tropical biomass burning using a global aerosol model and long-term surface observations. Atmos. Chem. Phys. 16, 11083–11106 (2016).

  29. 29.

    Lee, L. A. et al. The magnitude and causes of uncertainty in global model simulations of cloud condensation nuclei. Atmos. Chem. Phys. 13, 8879–8914 (2013).

  30. 30.

    Dentener, F. et al. Emissions of primary aerosol and precursor gases in the years 2000 and 1750 prescribed data-sets for AeroCom. Atmos. Chem. Phys. 6, 4321–4344 (2006).

  31. 31.

    Stier, P. et al. The aerosol-climate model ECHAM5-HAM. Atmos. Chem. Phys. 5, 1125–1156 (2005).

  32. 32.

    Vakkari, V. et al. Reevaluating the contribution of sulfuric acid and the origin of organic compounds in atmospheric nanoparticle growth. Geophys. Res. Lett. 42, 10486–10493 (2015).

  33. 33.

    Sakamoto, K. M., Laing, J. R., Stevens, R. G., Jaffe, D. A. & Pierce, J. R. The evolution of biomass-burning aerosol size distributions due to coagulation: dependence on fire and meteorological details and parameterization. Atmos. Chem. Phys. 16, 7709–7724 (2016).

  34. 34.

    Jaars, K. et al. Measurements of biogenic volatile organic compounds at a grazed savannah grassland agricultural landscape in South Africa. Atmos. Chem. Phys. 16, 15665–15688 (2016).

  35. 35.

    Friedl, M. A. et al. Global land cover mapping from MODIS: algorithms and early results. Remote Sens. Environ. 83, 287–302 (2002).

  36. 36.

    Petäjä, T. et al. Transportable aerosol characterization trailer with trace gas chemistry: design, instruments and verification. Aerosol Air Qual. Res. 13, 421–435 (2013).

  37. 37.

    Wiedensohler, A. et al. Mobility particle size spectrometers: harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions. Atmos. Meas. Tech. 5, 657–685 (2012).

  38. 38.

    Lee, B. H. et al. Measurement of the ambient organic aerosol volatility distribution: application during the Finokalia Aerosol Measurement Experiment (FAME-2008). Atmos. Chem. Phys. 10, 12149–12160 (2010).

  39. 39.

    Hyvärinen, A.-P. et al. Correction for a measurement artifact of the Multi-Angle Absorption Photometer (MAAP) at high black carbon mass concentration levels. Atmos. Meas. Tech. 6, 81–90 (2013).

  40. 40.

    Shiraiwa, M., Kondo, Y., Iwamoto, T. & Kita, K. Amplification of light absorption of black carbon by organic coating. Aerosol Sci. Tech. 44, 46–54 (2010).

  41. 41.

    Pokhrel, R. P. et al. Relative importance of black carbon, brown carbon, and absorption enhancement from clear coatings in biomass burning emissions. Atmos. Chem. Phys. 17, 5063–5078 (2017).

  42. 42.

    Petzold, A. et al. Evaluation of multiangle absorption photometry for measuring aerosol light absorption. Aerosol Sci. Tech. 39, 40–51 (2005).

  43. 43.

    Venter, A. D. et al. An air quality assessment in the industrialised western Bushveld Igneous Complex, South Africa. S. Afr. J. Sci. 108, 1059 (2012).

  44. 44.

    Seibert, P. & Frank, A. Source-receptor matrix calculation with a Lagrangian particle dispersion model in backward mode. Atmos. Chem. Phys. 4, 51–63 (2004).

  45. 45.

    Stohl, A., Forster, C., Frank, A., Seibert, P. & Wotawa, G. Technical note: the Lagrangian particle dispersion model FLEXPART version 6.2. Atmos. Chem. Phys. 5, 2461–2474 (2005).

  46. 46.

    Roberts, G. J. & Wooster, M. J. Fire detection and fire characterization over Africa using Meteosat SEVIRI. IEEE Trans. Geosci. Remote Sens. 46, 1200–1218 (2008).

  47. 47.

    Roy, D. P., Boschetti, L., Justice, C. O. & Ju, J. The collection 5 MODIS burned area product—global evaluation by comparison with the MODIS active fire product. Remote Sens. Environ. 112, 3690–3707 (2008).

  48. 48.

    Friedl, M. A. et al. MODIS Collection 5 global land cover: algorithm refinements and characterization of new datasets. Remote Sens. Environ. 114, 168–182 (2010).

  49. 49.

    Yokelson, R. J. et al. Emissions of formaldehyde, acetic acid, methanol, and other trace gases from biomass fires in North Carolina measured by airborne Fourier transform infrared spectroscopy. J. Geophys. Res. Atmos. 104, 30109–30125 (1999).

  50. 50.

    Seinfeld, J. H. & Pandis, S. N. Atmospheric Chemistry and Physics: From Air Pollution to Climate Change 3rd edn (John Wiley & Sons, Hoboken, 2016).

  51. 51.

    Fuchs, N. A. The Mechanics of Aerosols (Pergamon Press, London, 1964).

Download references


V.V. is beneficiary of an AXA Research Fund postdoctoral grant. Financial support by North-West University, South Africa and Academy of Finland (grant no. 307331) is gratefully acknowledged.

Author information


  1. Finnish Meteorological Institute, Research and Development, Helsinki, Finland

    • Ville Vakkari
    •  & Mika Aurela
  2. North-West University, Unit for Environmental Sciences and Management, Potchefstroom, South Africa

    • Johan P. Beukes
    • , Miroslav Josipovic
    •  & Pieter G. van Zyl
  3. Tampere University of Technology, Laboratory of Physics, Tampere, Finland

    • Miikka Dal Maso


  1. Search for Ville Vakkari in:

  2. Search for Johan P. Beukes in:

  3. Search for Miikka Dal Maso in:

  4. Search for Mika Aurela in:

  5. Search for Miroslav Josipovic in:

  6. Search for Pieter G. van Zyl in:


J.P.B., M.J. and P.G.v.Z. carried out the measurements at Welgegund while V.V. and M.A. contributed to measurement design. M.D.M. carried out aerosol dynamic simulations. V.V. analysed data and wrote most of the paper. All authors commented on the manuscript during the writing process.

Competing interests

The authors declare no competing interests.

Corresponding author

Correspondence to Ville Vakkari.

Supplementary information

  1. Supplementary Information

    Supplementary Figures and Tables.

About this article

Publication history