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Secondary organic aerosol reduced by mixture of atmospheric vapours

Nature volume 565, pages 587–593 (2019)Cite this article

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Abstract

Secondary organic aerosol contributes to the atmospheric particle burden with implications for air quality and climate. Biogenic volatile organic compounds such as terpenoids emitted from plants are important secondary organic aerosol precursors with isoprene dominating the emissions of biogenic volatile organic compounds globally. However, the particle mass from isoprene oxidation is generally modest compared to that of other terpenoids. Here we show that isoprene, carbon monoxide and methane can each suppress the instantaneous mass and the overall mass yield derived from monoterpenes in mixtures of atmospheric vapours. We find that isoprene ‘scavenges’ hydroxyl radicals, preventing their reaction with monoterpenes, and the resulting isoprene peroxy radicals scavenge highly oxygenated monoterpene products. These effects reduce the yield of low-volatility products that would otherwise form secondary organic aerosol. Global model calculations indicate that oxidant and product scavenging can operate effectively in the real atmosphere. Thus highly reactive compounds (such as isoprene) that produce a modest amount of aerosol are not necessarily net producers of secondary organic particle mass and their oxidation in mixtures of atmospheric vapours can suppress both particle number and mass of secondary organic aerosol. We suggest that formation mechanisms of secondary organic aerosol in the atmosphere need to be considered more realistically, accounting for mechanistic interactions between the products of oxidizing precursor molecules (as is recognized to be necessary when modelling ozone production).

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Fig. 1: Reduced SOA mass and yield of α-pinene by product scavenging and OH• scavenging by isoprene.
Fig. 2: The reduction of the SOA yield of α-pinene by isoprene as a function of the isoprene consumption relative to that of α-pinene.
Fig. 3: HOM monomer/dimer distribution in the presence and absence of isoprene illustrating the product scavenging effect.
Fig. 4: Suppression of α-pinene SOA in the presence of CO, illustrating the generality of the product-scavenging effect.
Fig. 5: Atmospheric implications of product scavenging and OH• scavenging.

Data availability

All data used are shown as figures or tables in the manuscript or in Supplementary Information. Raw data are available from the corresponding author on reasonable request.

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Acknowledgements

The EMEP modelling work was funded partially by EMEP under UNECE. Computer time for EMEP model runs was supported by the Research Council of Norway through the NOTUR project EMEP (NN2890K) for the central processing unit (CPU) time, and NorStore project European Monitoring and Evaluation Programme (NS9005K) for storage of data. The research presented is a contribution to the Swedish strategic research area ‘ModElling the Regional and Global Earth system’ (MERGE). This work was supported by Formas (grant numbers 214-2010-1756 and 942-2015-1537); the Swedish Research Council (grant number 2014-5332) and the European Research Council (Starting grant number 638703, ‘COALA’). Å.M.H. acknowledges Formas (grant number 214-2013-1430) and Vinnova, Sweden’s Innovation Agency (grant number 2013-03058), including support for her research stay at Forschungszentrum Jülich. The participation of the Manchester group was facilitated by the UK Natural Environment Research Council (NERC)-funded CCN-Vol project (NE/L007827/1) and National Centre for Atmospheric Science (NCAS) funding. J.A.T. was supported by a grant from the U.S. Department of Energy Office of Science: DE-SC0018221.

Reviewer information

Nature thanks F. Yu, P. Ziemann and the other anonymous reviewer(s) for their contribution to the peer review of this work.

Author information

Author notes

  1. Iida Pullinen

    Present address: Department of Applied Physics, University of Eastern Finland, Kuopio, Finland

  2. Sebastian Schmitt

    Present address: TSI, Aachen, Germany

  3. Cheng Wu

    Present address: Department of Environmental Science and Analytical Chemistry, Stockholm University, Stockholm, Sweden

  4. Carl J. Percival

    Present address: Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA, USA

Authors and Affiliations

  1. School of Earth and Environmental Sciences, University of Manchester, Manchester, UK

    Gordon McFiggans, Michael Le Breton, M. Rami Alfarra, Thomas J. Bannan, Carl J. Percival, Michael Priestley & David Topping

  2. Institut für Energie- und Klimaforschung, IEK-8, Forschungszentrum Jülich, Jülich, Germany

    Thomas F. Mentel, Jürgen Wildt, Iida Pullinen, Sungah Kang, Sebastian Schmitt, Monika Springer, Ralf Tillmann, Cheng Wu, Defeng Zhao & Astrid Kiendler-Scharr

  3. Institut für Bio- und Geowissenschaften, IBG-2, Forschungszentrum Jülich, Jülich, Germany

    Jürgen Wildt & Einhard Kleist

  4. Department of Atmospheric and Oceanic Sciences and Institute of Atmospheric Sciences, Fudan University, Shanghai, China

    Defeng Zhao

  5. Atmospheric Science, Department of Chemistry and Molecular Biology, University of Gothenburg, Gothenburg, Sweden

    Mattias Hallquist, Cameron Faxon, Michael Le Breton & Robert Bergström

  6. IVL Swedish Environmental Research Institute, Gothenburg, Sweden

    Åsa M. Hallquist

  7. Department of Earth, Space and Environment, Chalmers University of Technology, Gothenburg, Sweden

    David Simpson & Robert Bergström

  8. EMEP MSC-W, Norwegian Meteorological Institute, Oslo, Norway

    David Simpson

  9. Swedish Meteorological and Hydrological Institute, Norrköping, Sweden

    Robert Bergström

  10. Atmospheric Chemistry Services, Okehampton, UK

    Michael E. Jenkin

  11. Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland

    Mikael Ehn

  12. Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA

    Joel A. Thornton

  13. National Centre for Atmospheric Science (NCAS), University of Manchester, Manchester, UK

    M. Rami Alfarra & David Topping

  14. I. Physikalisches Institut, Universität zu Köln, Cologne, Germany

    Astrid Kiendler-Scharr

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Contributions

G.M., T.F.M. and J.W. edited the manuscript and Supplementary Information. G.M., T.F.M., J.W., A.K.-S., M.H., D.S. and M.E.J. conceptualized and planned the study, and conducted data interpretation. J.W., I.P., S.K., E.K., S.S., M.S., R.T., C.W., D.Z., C.F., M.L.B., Å.M.H., M.R.A., T.J.B., C.J.P., M.P. and D.T. conducted data collection and analysis. D.S., R.B. and M.E.J. contributed the global model calculations. J.A.T., M.E., Å.M.H. and M.H. provided specific inputs to the manuscript and Supplementary Information. All co-authors discussed the results and commented on the manuscript and Supplementary Information.

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Correspondence to Thomas F. Mentel.

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The supplement contains one single pdf file. The material is ordered in 9 sections, which describe in detail the experiments and the applied methods. It contains Figures (17) and Tables (5), and additional references (69). The supplement provides all additional information which informed our findings

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McFiggans, G., Mentel, T.F., Wildt, J. et al. Secondary organic aerosol reduced by mixture of atmospheric vapours. Nature 565, 587–593 (2019). https://doi.org/10.1038/s41586-018-0871-y

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