A large source of low-volatility secondary organic aerosol

Mikael Ehn; Joel A. Thornton; Einhard Kleist; Mikko Sipilä; Heikki Junninen; Iida Pullinen; Monika Springer; Florian Rubach; Ralf Tillmann; Ben Lee; Felipe Lopez-Hilfiker; Stefanie Andres; Ismail Hakki Acir; Matti Rissanen; Tuija Jokinen; Siegfried Schobesberger; Juha Kangasluoma; Jenni Kontkanen; Tuomo Nieminen; Theo Kurtén; Lasse Bo Nielsen; Solvejg Jørgensen; Henrik Grum Kjærgaard; Manjula Canagaratna; Miikka Dal Maso; Torsten Berndt; Tuukka Petäjä; Andreas Wahner; Veli Matti Kerminen; Markku Kulmala; Douglas R. Worsnop; Jürgen Wildt; Thomas F. Mentel

doi:10.1038/nature13032

A large source of low-volatility secondary organic aerosol

Mikael Ehn^*, Joel A. Thornton, Einhard Kleist, Mikko Sipilä, Heikki Junninen, Iida Pullinen, Monika Springer, Florian Rubach, Ralf Tillmann, Ben Lee, Felipe Lopez-Hilfiker, Stefanie Andres, Ismail Hakki Acir, Matti Rissanen, Tuija Jokinen, Siegfried Schobesberger, Juha Kangasluoma, Jenni Kontkanen, Tuomo Nieminen, Theo KurténLasse Bo Nielsen, Solvejg Jørgensen, Henrik Grum Kjærgaard, Manjula Canagaratna, Miikka Dal Maso, Torsten Berndt, Tuukka Petäjä, Andreas Wahner, Veli Matti Kerminen, Markku Kulmala, Douglas R. Worsnop, Jürgen Wildt, Thomas F. Mentel

^*Corresponding author for this work

Department of Chemistry

862 Citations (Scopus)

Abstract

Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.

Original language	English
Journal	Nature
Volume	506
Issue number	7489
Pages (from-to)	476-479
Number of pages	4
ISSN	0028-0836
DOIs	https://doi.org/10.1038/nature13032
Publication status	Published - 2014

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Ehn, M., Thornton, J. A., Kleist, E., Sipilä, M., Junninen, H., Pullinen, I., Springer, M., Rubach, F., Tillmann, R., Lee, B., Lopez-Hilfiker, F., Andres, S., Acir, I. H., Rissanen, M., Jokinen, T., Schobesberger, S., Kangasluoma, J., Kontkanen, J., Nieminen, T., ... Mentel, T. F. (2014). A large source of low-volatility secondary organic aerosol. Nature, 506(7489), 476-479. https://doi.org/10.1038/nature13032

Ehn, M, Thornton, JA, Kleist, E, Sipilä, M, Junninen, H, Pullinen, I, Springer, M, Rubach, F, Tillmann, R, Lee, B, Lopez-Hilfiker, F, Andres, S, Acir, IH, Rissanen, M, Jokinen, T, Schobesberger, S, Kangasluoma, J, Kontkanen, J, Nieminen, T, Kurtén, T, Nielsen, LB, Jørgensen, S , Kjærgaard, HG, Canagaratna, M, Maso, MD, Berndt, T, Petäjä, T, Wahner, A, Kerminen, VM, Kulmala, M, Worsnop, DR, Wildt, J & Mentel, TF 2014, 'A large source of low-volatility secondary organic aerosol', Nature, vol. 506, no. 7489, pp. 476-479. https://doi.org/10.1038/nature13032

@article{d627100ff9974bea97ece715e5f11e58,

title = "A large source of low-volatility secondary organic aerosol",

abstract = "Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.",

author = "Mikael Ehn and Thornton, {Joel A.} and Einhard Kleist and Mikko Sipil{\"a} and Heikki Junninen and Iida Pullinen and Monika Springer and Florian Rubach and Ralf Tillmann and Ben Lee and Felipe Lopez-Hilfiker and Stefanie Andres and Acir, {Ismail Hakki} and Matti Rissanen and Tuija Jokinen and Siegfried Schobesberger and Juha Kangasluoma and Jenni Kontkanen and Tuomo Nieminen and Theo Kurt{\'e}n and Nielsen, {Lasse Bo} and Solvejg J{\o}rgensen and Kj{\ae}rgaard, {Henrik Grum} and Manjula Canagaratna and Maso, {Miikka Dal} and Torsten Berndt and Tuukka Pet{\"a}j{\"a} and Andreas Wahner and Kerminen, {Veli Matti} and Markku Kulmala and Worsnop, {Douglas R.} and J{\"u}rgen Wildt and Mentel, {Thomas F.}",

year = "2014",

doi = "10.1038/nature13032",

language = "English",

volume = "506",

pages = "476--479",

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T1 - A large source of low-volatility secondary organic aerosol

AU - Ehn, Mikael

AU - Thornton, Joel A.

AU - Kleist, Einhard

AU - Sipilä, Mikko

AU - Junninen, Heikki

AU - Pullinen, Iida

AU - Springer, Monika

AU - Rubach, Florian

AU - Tillmann, Ralf

AU - Lee, Ben

AU - Lopez-Hilfiker, Felipe

AU - Andres, Stefanie

AU - Acir, Ismail Hakki

AU - Rissanen, Matti

AU - Jokinen, Tuija

AU - Schobesberger, Siegfried

AU - Kangasluoma, Juha

AU - Kontkanen, Jenni

AU - Nieminen, Tuomo

AU - Kurtén, Theo

AU - Nielsen, Lasse Bo

AU - Jørgensen, Solvejg

AU - Kjærgaard, Henrik Grum

AU - Canagaratna, Manjula

AU - Maso, Miikka Dal

AU - Berndt, Torsten

AU - Petäjä, Tuukka

AU - Wahner, Andreas

AU - Kerminen, Veli Matti

AU - Kulmala, Markku

AU - Worsnop, Douglas R.

AU - Wildt, Jürgen

AU - Mentel, Thomas F.

PY - 2014

Y1 - 2014

N2 - Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.

AB - Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.

U2 - 10.1038/nature13032

DO - 10.1038/nature13032

M3 - Letter

C2 - 24572423

AN - SCOPUS:84896830977

SN - 0028-0836

VL - 506

SP - 476

EP - 479

JO - Nature

JF - Nature

IS - 7489

ER -

A large source of low-volatility secondary organic aerosol

Abstract

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