Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

Top-of-atmosphere radiative forcing affected by brown carbon in the upper troposphere

Nature Geoscience volume 10, pages 486–489 (2017)Cite this article

Subjects

Abstract

Carbonaceous aerosols affect the global radiative balance by absorbing and scattering radiation, which leads to warming or cooling of the atmosphere, respectively. Black carbon is the main light-absorbing component. A portion of the organic aerosol known as brown carbon also absorbs light. The climate sensitivity to absorbing aerosols rapidly increases with altitude, but brown carbon measurements are limited in the upper troposphere. Here we present aircraft observations of vertical aerosol distributions over the continental United States in May and June 2012 to show that light-absorbing brown carbon is prevalent in the troposphere, and absorbs more short-wavelength radiation than black carbon at altitudes between 5 and 12 km. We find that brown carbon is transported to these altitudes by deep convection, and that in-cloud heterogeneous processing may produce brown carbon. Radiative transfer calculations suggest that brown carbon accounts for about 24% of combined black and brown carbon warming effect at the tropopause. Roughly two-thirds of the estimated brown carbon forcing occurs above 5 km, although most brown carbon is found below 5 km. The highest radiative absorption occurred during an event that ingested a wildfire plume. We conclude that high-altitude brown carbon from biomass burning is an unappreciated component of climate forcing.

This is a preview of subscription content, access via your institution

Access options

Buy this article

  • Purchase on Springer Link
  • Instant access to full article PDF
Buy now

Prices may be subject to local taxes which are calculated during checkout

Figure 1: Aerosol absorption by BC and BrC measured during the DC3 campaign.
Figure 2: Instantaneous clear-sky direct radiative forcing estimates of aerosols using the DC3 data.
Figure 3: Measured outflow/inflow ratio of multiple gaseous and aerosol species using the convection samples from DC3.

Similar content being viewed by others

References

  1. Myhre, G. et al. in Climate Change 2013: The Physical Science Basis (eds Stocker, T. F. et al.) 659–740 (IPCC, Cambridge Univ. Press, 2013).

    Google Scholar 

  2. Kirchstetter, T. W., Novakov, T. & Hobbs, P. V. Evidence that the spectral dependence of light absorption by aerosols is affected by organic carbon. J. Geophys. Res. 109, D21208 (2004).

    Article  Google Scholar 

  3. Alexander, D. T. L., Crozier, P. A. & Anderson, J. R. Brown carbon spheres in East Asian outflow and their optical properties. Science 321, 833–836 (2008).

    Article  Google Scholar 

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

    Article  Google Scholar 

  5. Zhang, X. et al. Light-absorbing soluble organic aerosol in Los Angeles and Atlanta: a contrast in secondary organic aerosol. Geophys. Res. Lett. 38, L21810 (2011).

    Google Scholar 

  6. Kirchstetter, T. W. & Thatcher, T. L. Contribution of organic carbon to wood smoke particulate matter absorption of solar radiation. Atmos. Chem. Phys. 12, 6067–6072 (2012).

    Article  Google Scholar 

  7. 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. 121, 7383–7414 (2016).

    Google Scholar 

  8. Hecobian, A. et al. Water-Soluble Organic Aerosol material and the light-absorption characteristics of aqueous extracts measured over the Southeastern United States. Atmos. Chem. Phys. 10, 5965–5977 (2010).

    Article  Google Scholar 

  9. Liu, J. et al. Size-resolved measurements of brown carbon in water and methanol extracts and estimates of their contribution to ambient fine-particle light absorption. Atmos. Chem. Phys. 13, 12389–12404 (2013).

    Article  Google Scholar 

  10. Liu, J. et al. Brown carbon in the continental troposphere. Geophys. Res. Lett. 41, 2191–2195 (2014).

    Article  Google Scholar 

  11. Liu, J. et al. Brown carbon aerosol in the North American continental troposphere: sources, abundance, and radiative forcing. Atmos. Chem. Phys. 15, 7841–7858 (2015).

    Article  Google Scholar 

  12. Forrister, H. et al. Evolution of brown carbon in wildfire plumes. Geophys. Res. Lett. 42, 4623–4630 (2015).

    Article  Google Scholar 

  13. Arola, A. et al. Inferring absorbing organic carbon content from AERONET data. Atmos. Chem. Phys. 11, 215–225 (2011).

    Article  Google Scholar 

  14. Chung, C. E., Ramanathan, V. & Decremer, D. Observationally constrained estimates of carbonaceous aerosol radiative forcing. Proc. Natl Acad. Sci. USA 109, 11624–11629 (2012).

    Article  Google Scholar 

  15. Wang, X. et al. Deriving brown carbon from multi-wavelength absorption measurements: method and application to AERONET and surface observations. Atmos. Chem. Phys. Discuss. 2016, 1–33 (2016).

    Google Scholar 

  16. Feng, Y., Ramanathan, V. & Kotamarthi, V. R. Brown carbon: a significant atmospheric absorber of solar radiation? Atmos. Chem. Phys. 13, 8607–8621 (2013).

    Article  Google Scholar 

  17. Wang, X. et al. Exploiting simultaneous observational constraints on mass and absorption to estimate the global direct radiative forcing of black carbon and brown carbon. Atmos. Chem. Phys. 14, 10989–11010 (2014).

    Article  Google Scholar 

  18. Jo, D. S., Park, R. J., Lee, S., Kim, S. W. & Zhang, X. A global simulation of brown carbon: implications for photochemistry and direct radiative effect. Atmos. Chem. Phys. 16, 3413–3432 (2016).

    Article  Google Scholar 

  19. Saleh, R. et al. Contribution of brown carbon and lensing to the direct radiative effect of carbonaceous aerosols from biomass and biofuel burning emissions. J. Geophys. Res. 120, 10285–10296 (2015).

    Google Scholar 

  20. Hodnebrog, Ø, Myhre, G. & Samset, B. H. How shorter black carbon lifetime alters its climate effect. Nat. Commun. 5, 5065 (2014).

    Article  Google Scholar 

  21. Ban-Weiss, G. A., Cao, L., Bala, G. & Caldeira, K. Dependence of climate forcing and response on the altitude of black carbon aerosols. Clim. Dynam. 38, 897–911 (2012).

    Article  Google Scholar 

  22. Koch, D. & Del Genio, A. D. Black carbon semi-direct effects on cloud cover: review and synthesis. Atmos. Chem. Phys. 10, 7685–7696 (2010).

    Article  Google Scholar 

  23. Barth, M. C. et al. The deep convective clouds and chemistry (DC3) field campaign. Bull. Am. Meteorol. Soc. 96, 1281–1309 (2015).

    Article  Google Scholar 

  24. Toon, O. B. et al. Planning, implementation, and scientific goals of the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field mission. J. Geophys. Res. 121, 4967–5009 (2016).

    Google Scholar 

  25. Corr, C. A. et al. Observational evidence for the convective transport of dust over the central United States. J. Geophys. Res. 121, 1306–1319 (2016).

    Google Scholar 

  26. Desyaterik, Y. et al. Speciation of “brown” carbon in cloud water impacted by agricultural biomass burning in eastern China. J. Geophys. Res. 118, 7389–7399 (2013).

    Google Scholar 

  27. Gilardoni, S. et al. Direct observation of aqueous secondary organic aerosol from biomass-burning emissions. Proc. Natl Acad. Sci. USA 113, 10013–10018 (2016).

    Article  Google Scholar 

  28. Laskin, A., Laskin, J. & Nizkorodov, S. A. Chemistry of atmospheric brown carbon. Chem. Rev. 115, 4335–4382 (2015).

    Article  Google Scholar 

  29. Koch, D. et al. Evaluation of black carbon estimations in global aerosol models. Atmos. Chem. Phys. 9, 9001–9026 (2009).

    Article  Google Scholar 

  30. Liu, Y., Stanturf, J. & Goodrick, S. Trends in global wildfire potential in a changing climate. For. Ecol. Manage. 259, 685–697 (2010).

    Article  Google Scholar 

  31. Washenfelder, R. A. et al. Biomass burning dominates brown carbon absorption in the rural southeastern United States. Geophys. Res. Lett. 42, 653–664 (2015).

    Article  Google Scholar 

  32. Schwarz, J. P. et al. Aircraft measurements of black carbon vertical profiles show upper tropospheric variability and stability. Geophys. Res. Lett. 44, 1132–1140 (2017).

    Article  Google Scholar 

  33. DeCarlo, P. F. et al. Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer. Anal. Chem. 78, 8281–8289 (2006).

    Article  Google Scholar 

  34. Bond, T. C., Anderson, T. L. & Campbell, D. Calibration and intercomparison of filter-based measurements of visible light absorption by aerosols. Aerosol Sci. Technol. 30, 582–600 (1999).

    Article  Google Scholar 

  35. Virkkula, A. Correction of the calibration of the 3-wavelength particle soot absorption photometer (3λ PSAP). Aerosol Sci. Technol. 44, 706–712 (2010).

    Article  Google Scholar 

  36. Anderson, T. L. & Ogren, J. A. Determining aerosol radiative properties using the TSI 3563 integrating nephelometer. Aerosol Sci. Technol. 29, 57–69 (1998).

    Article  Google Scholar 

  37. Bela, M. M. et al. Wet scavenging of soluble gases in DC3 deep convective storms using WRF-Chem simulations and aircraft observations. J. Geophys. Res. 121, 4233–4242 (2016).

    Google Scholar 

  38. Barth, M. C. et al. Convective transport and scavenging of peroxides by thunderstorms observed over the central US during DC3. J. Geophys. Res. 121, 4272–4295 (2016).

    Google Scholar 

  39. Ricchiazzi, P., Yang, S., Gautier, C. & Sowle, D. SBDART: a research and teaching software tool for plane-parallel radiative transfer in the earth’s atmosphere. Bull. Am. Meteorol. Soc. 79, 2101–2114 (1998).

    Article  Google Scholar 

  40. Olson, M. R. et al. Investigation of black and brown carbon multiple-wavelength-dependent light absorption from biomass and fossil fuel combustion source emissions. J. Geophys. Res. 120, 6682–6697 (2015).

    Article  Google Scholar 

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

    Article  Google Scholar 

  42. Zarzycki, C. M. & Bond, T. C. How much can the vertical distribution of black carbon affect its global direct radiative forcing? Geophys. Res. Lett. 37, L20807 (2010).

    Article  Google Scholar 

  43. Jethva, H., Torres, O. & Ahn, C. Global assessment of OMI aerosol single-scattering albedo using ground-based AERONET inversion. J. Geophys. Res. 119, 9020–9040 (2014).

    Google Scholar 

  44. Jethva, H. & Torres, O. Satellite-based evidence of wavelength-dependent aerosol absorption in biomass burning smoke inferred from Ozone Monitoring Instrument. Atmos. Chem. Phys. 11, 10541–10551 (2011).

    Article  Google Scholar 

  45. Torres, O. et al. Aerosols and surface UV products from Ozone Monitoring Instrument observations: an overview. J. Geophys. Res. 112, D24S47 (2007).

    Article  Google Scholar 

Download references

Acknowledgements

All data used in this paper were collected as part of the NASA DC3 and SEAC4RS missions and became available to the general public on 15 October 2014 through the NASA data archive. Georgia Tech researchers were funded through NASA Radiation Sciences Program grant NNX14AP74G. NASA Tropospheric Composition Program supported J.D. through grant NNX12AB80G, and P.C.-J. and J.L.J. through grants NNX12AC03G and NNX15AT96G. H.F. was supported by the National Science Foundation Graduate Research Fellowship under Grant No. DGE-1650044. The authors thank G. Chen and C. Corr for discussion with Y.Z.

Author information

Authors and Affiliations

  1. School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, Georgia, 30332, USA

    Yuzhong Zhang, Haviland Forrister, Yuhang Wang, Athanasios Nenes & Rodney J. Weber

  2. Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, Washington, 99352, USA

    Jiumeng Liu

  3. Earth Systems Research Center, Institute for the Study of Earth, Oceans, and Space, University of New Hampshire, Durham, New Hampshire, 03824, USA

    Jack Dibb

  4. Chemistry and Dynamics Branch, NASA Langley Research Center, Hampton, Virginia, 23681, USA

    Bruce Anderson

  5. Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, Colorado, 80305, USA

    Joshua P. Schwarz & Anne E. Perring

  6. Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, Colorado, 80309, USA

    Anne E. Perring, Jose L. Jimenez & Pedro Campuzano-Jost

  7. Department of Chemistry and Biogeochemistry, University of Colorado Boulder, Boulder, Colorado, 80309, USA

    Jose L. Jimenez & Pedro Campuzano-Jost

  8. School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia, 30332, USA

    Athanasios Nenes

  9. Institute of Environmental Research and Sustainable Development, National Observatory of Athens, Palea Penteli, GR-15236, Greece

    Athanasios Nenes

  10. Institute for Chemical Engineering Science, Foundation for Research and Technology Hellas, Patra, GR-26504, Greece

    Athanasios Nenes

Authors
  1. Yuzhong Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Haviland Forrister
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Jiumeng Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Jack Dibb
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Bruce Anderson
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Joshua P. Schwarz
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Anne E. Perring
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Jose L. Jimenez
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Pedro Campuzano-Jost
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Yuhang Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Athanasios Nenes
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. Rodney J. Weber
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

Y.Z., Y.W., A.N. and R.J.W. designed the study. Y.Z. performed the analysis and calculation. J.L., J.D., B.A., J.P.S., A.E.P., J.L.J., P.C.-J. and R.J.W. conducted and analysed the aircraft measurements. Y.Z., H.F., Y.W., A.N. and R.J.W. discussed the results. Y.Z., Y.W., A.N. and R.J.W. wrote the paper. J.L.J., J.L., H.F., J.D. and J.P.S. provided input on the paper for revision before submission.

Corresponding author

Correspondence to Rodney J. Weber.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary Information

Supplementary Information (PDF 785 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhang, Y., Forrister, H., Liu, J. et al. Top-of-atmosphere radiative forcing affected by brown carbon in the upper troposphere. Nature Geosci 10, 486–489 (2017). https://doi.org/10.1038/ngeo2960

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/ngeo2960

This article is cited by

Search

Advanced search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing