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Stratospheric aerosol perturbation by tropospheric biomass burning and deep convection

Nature Geoscience (2025)Cite this article

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Abstract

The stratosphere is generally considered to be stable, with minimal vertical mixing. However, deep convection can transport low-altitude material above the tropopause. Here we use in situ single-particle measurements from the Dynamics and Chemistry of the Summer Stratosphere mission to show that carbonaceous-sulfate particles from the troposphere account for up to 90% of the stratospheric particles with physical diameter from 0.1 to 1.5 µm in a 4-km layer above the tropopause during an active fire season in 2022. We find that ~43% of the stratospheric carbonaceous-sulfate particles originate from biomass burning. These particles, which are chemically complex and organic-rich, do not remain unchanged once injected into the stratosphere, but form mixtures containing both tropospheric and stratospheric components, indicating perturbation of the stratospheric aerosol layer. We suggest that the increasing frequency and intensity of wildfires combined with increasing deep convection as the climate warms may enhance the delivery of biomass burning products to the lower stratosphere, with implications for ozone chemistry and radiative forcing.

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Fig. 1: Schematic representation of stratospheric dynamics and particles.
Fig. 2: Selected flight tracks and number fractions of stratospheric particles (from 31 May to 27 June 2022).
Fig. 3: Chemical composition of stratospheric particles.
Fig. 4: Vertical profiles of water vapour and particles.
Fig. 5: Vertical profiles of three main stratospheric particle types.

Data availability

DCOTSS aircraft data that support the findings of this study are publicly available at the NASA Atmospheric Science Data Center (https://doi.org/10.5067/ASDC/DCOTSS-Aircraft-Data_1)73. Raw data underlying the figures are available on request.

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Acknowledgements

The DCOTSS mission and subsequent analyses were supported by NASA under grants nos. 80NSSC19K1058 (A.L., D.J.C., D.M.M., F.A.R.-A., G.P.S., J.L.J., M.F., T.E.O., R.C.M., S.A.L.S. and X.S.), 80NSSC19K0326 (F.N.K., J.A.D., J.B.S., J.V.P. and Y.L.), 80NSSC19K0341 (K.P.B.) and 80NSSC19K0347 (C.R.H.). We thank the DCOTSS flight and all the science teams. Special thanks go to the NASA Earth Science Project Office and ER-2 flight and ground crews for their assistance and support. We also thank K. D. Froyd, D. S. Thomson, K. Slovacek, M. Lawler and M. Abou-Ghanem for supporting the development of PALMS-NG. We thank E. Ray for discussions on the two-step process of convective overshoot.

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Authors and Affiliations

  1. Department of Earth, Atmospheric, and Planetary Sciences, Purdue University, West Lafayette, IN, USA

    X. Shen, J. L. Jacquot, D. M. Murphy, A. Laskin & D. J. Cziczo

  2. School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA

    Y. Li, J. A. Dykema, J. V. Pittman, J. B. Smith & F. N. Keutsch

  3. Department of Chemistry, Purdue University, West Lafayette, IN, USA

    S. A. L. Sharpe, T. E. Olayemi, F. A. Rivera-Adorno & A. Laskin

  4. Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA

    G. P. Schill & D. M. Murphy

  5. Department of Atmospheric Sciences, Texas A&M University, College Station, TX, USA

    K. P. Bowman

  6. School of Meteorology, University of Oklahoma, Norman, OK, USA

    C. R. Homeyer

  7. Fraund Consulting, Pleasant Hill, CA, USA

    M. Fraund

  8. Sonoma Technology, Inc, Petaluma, CA, USA

    R. C. Moffet

  9. Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA, USA

    F. N. Keutsch

  10. Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA

    F. N. Keutsch

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  1. X. Shen
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Contributions

X.S. analysed data, produced tables and figures, and was the lead writer of the paper. D.J.C. assisted with data interpretation and preparation of the paper. J.L.J., X.S. and D.J.C. collected data. G.P.S. and D.M.M. had important roles in PALMS-NG development. Y.L., J.A.D. and F.N.K. provided DPOPS results, designed the mini-MOUDI sampling methods and collected filter samples, and helped with discussions on climate impact. S.A.L.S., F.A.R.-A., T.E.O., M.F., R.C.M. and A.L. provided STXM/NEXAFS results, and helped with the discussion on stratospheric ozone impact. J.V.P. provided HUPCRS data and discussions on the tropical origin of the air. J.B.S. was the instrument-aircraft lead and provided water vapour results. C.R.H. was the science investigation manager and data manager for DCOTSS and provided feature analysis results. K.P.B. was the principal investigator of the DCOTSS mission and provided general comments on this paper. All authors contributed to the final text.

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Correspondence to X. Shen.

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Nature Geoscience thanks Jianmin Chen and the other, anonymous, reviewers for their contribution to the peer review of this work. Primary Handling Editors: Camilla Brunello, Xujia Jiang and Carolina Ortiz Guerrero, in collaboration with the Nature Geoscience team.

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Supplementary Background, Notes 1–7, Figs. 1–5 and Table 1.

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Shen, X., Jacquot, J.L., Li, Y. et al. Stratospheric aerosol perturbation by tropospheric biomass burning and deep convection. Nat. Geosci. (2025). https://doi.org/10.1038/s41561-025-01821-1

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