The link between atmospheric radicals and newly formed particles at a spruce forest site in Germany

B. Bonn, E. Bourtsoukidis, T. S. Sun, H. Bingemer, L. Rondo, U. Javed, J. Li, R. Axinte, X. Li, T. Brauers, H. Sonderfeld, R. Koppmann, Andrey Sogachev, S. Jacobi, D. V. Spracklen

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Abstract

It has been claimed for more than a century that atmospheric new particle formation is primarily influenced by the presence of sulfuricacid. However, the activation process of sulfuric acid related clusters into detectable particles is still an unresolved topic. In this study we focus onthe PARADE campaign measurements conducted during August/September 2011 at Mt Kleiner Feldberg in central Germany. During this campaign a set ofradicals, organic and inorganic compounds and oxidants and aerosol properties were measured or calculated. We compared a range of organic and inorganic nucleation theories, evaluating their ability to simulate measured particle formation rates at 3 nm in diameter (J3) for a variety of different conditions. Nucleation mechanisms involving only sulfuric acid tentatively captured the observed noon-time daily maximum in J3, but displayed an increasing difference to J3 measurements during the rest of the diurnal cycle. Including large organic radicals, i.e. organic peroxy radicals (RO2) deriving from monoterpenes and their oxidation products, in the nucleation mechanism improved the correlation between observed and simulated J3. This supports a recently proposed empirical relationship for new particle formation that has been used in global models. However, the best match between theory and measurements for the site of interest was found for an activation process based on large organic peroxy radicals and stabilised Criegee intermediates (sCI). This novel laboratory-derived algorithm simulated the daily pattern and intensity of J3 observed in the ambient data. In this algorithm organic derived radicals are involved in activation and growth and link the formation rate of smallest aerosol particles with OH during day-time and NO3 during night-time. Because the RO2 lifetime is controlled by HO2 and NO we conclude that peroxy radicals and NO seem to play an important role for ambient radical chemistry not only with respect to oxidation capacity but also for the activation process of new particle formation. This is supposed to have significant impact of atmospheric radical species on aerosol chemistry and should be taken into account when studying the impact of new particles in climate feedback cycles.
Original languageEnglish
JournalAtmospheric Chemistry and Physics
Pages (from-to)10823-10843
ISSN1680-7316
DOIs
Publication statusPublished - 2014

Bibliographical note

© Author(s) 2014. This work is distributed under the Creative Commons Attribution 3.0 License.

Cite this

Bonn, B., Bourtsoukidis, E., Sun, T. S., Bingemer, H., Rondo, L., Javed, U., ... Spracklen, D. V. (2014). The link between atmospheric radicals and newly formed particles at a spruce forest site in Germany. Atmospheric Chemistry and Physics, 10823-10843. https://doi.org/10.5194/acp-14-10823-2014
Bonn, B. ; Bourtsoukidis, E. ; Sun, T. S. ; Bingemer, H. ; Rondo, L. ; Javed, U. ; Li, J. ; Axinte, R. ; Li, X. ; Brauers, T. ; Sonderfeld, H. ; Koppmann, R. ; Sogachev, Andrey ; Jacobi, S. ; Spracklen, D. V. / The link between atmospheric radicals and newly formed particles at a spruce forest site in Germany. In: Atmospheric Chemistry and Physics. 2014 ; pp. 10823-10843.
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abstract = "It has been claimed for more than a century that atmospheric new particle formation is primarily influenced by the presence of sulfuricacid. However, the activation process of sulfuric acid related clusters into detectable particles is still an unresolved topic. In this study we focus onthe PARADE campaign measurements conducted during August/September 2011 at Mt Kleiner Feldberg in central Germany. During this campaign a set ofradicals, organic and inorganic compounds and oxidants and aerosol properties were measured or calculated. We compared a range of organic and inorganic nucleation theories, evaluating their ability to simulate measured particle formation rates at 3 nm in diameter (J3) for a variety of different conditions. Nucleation mechanisms involving only sulfuric acid tentatively captured the observed noon-time daily maximum in J3, but displayed an increasing difference to J3 measurements during the rest of the diurnal cycle. Including large organic radicals, i.e. organic peroxy radicals (RO2) deriving from monoterpenes and their oxidation products, in the nucleation mechanism improved the correlation between observed and simulated J3. This supports a recently proposed empirical relationship for new particle formation that has been used in global models. However, the best match between theory and measurements for the site of interest was found for an activation process based on large organic peroxy radicals and stabilised Criegee intermediates (sCI). This novel laboratory-derived algorithm simulated the daily pattern and intensity of J3 observed in the ambient data. In this algorithm organic derived radicals are involved in activation and growth and link the formation rate of smallest aerosol particles with OH during day-time and NO3 during night-time. Because the RO2 lifetime is controlled by HO2 and NO we conclude that peroxy radicals and NO seem to play an important role for ambient radical chemistry not only with respect to oxidation capacity but also for the activation process of new particle formation. This is supposed to have significant impact of atmospheric radical species on aerosol chemistry and should be taken into account when studying the impact of new particles in climate feedback cycles.",
author = "B. Bonn and E. Bourtsoukidis and Sun, {T. S.} and H. Bingemer and L. Rondo and U. Javed and J. Li and R. Axinte and X. Li and T. Brauers and H. Sonderfeld and R. Koppmann and Andrey Sogachev and S. Jacobi and Spracklen, {D. V.}",
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Bonn, B, Bourtsoukidis, E, Sun, TS, Bingemer, H, Rondo, L, Javed, U, Li, J, Axinte, R, Li, X, Brauers, T, Sonderfeld, H, Koppmann, R, Sogachev, A, Jacobi, S & Spracklen, DV 2014, 'The link between atmospheric radicals and newly formed particles at a spruce forest site in Germany', Atmospheric Chemistry and Physics, pp. 10823-10843. https://doi.org/10.5194/acp-14-10823-2014

The link between atmospheric radicals and newly formed particles at a spruce forest site in Germany. / Bonn, B.; Bourtsoukidis, E.; Sun, T. S.; Bingemer, H.; Rondo, L.; Javed, U.; Li, J.; Axinte, R.; Li, X.; Brauers, T.; Sonderfeld, H.; Koppmann, R.; Sogachev, Andrey; Jacobi, S.; Spracklen, D. V.

In: Atmospheric Chemistry and Physics, 2014, p. 10823-10843.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - The link between atmospheric radicals and newly formed particles at a spruce forest site in Germany

AU - Bonn, B.

AU - Bourtsoukidis, E.

AU - Sun, T. S.

AU - Bingemer, H.

AU - Rondo, L.

AU - Javed, U.

AU - Li, J.

AU - Axinte, R.

AU - Li, X.

AU - Brauers, T.

AU - Sonderfeld, H.

AU - Koppmann, R.

AU - Sogachev, Andrey

AU - Jacobi, S.

AU - Spracklen, D. V.

N1 - © Author(s) 2014. This work is distributed under the Creative Commons Attribution 3.0 License.

PY - 2014

Y1 - 2014

N2 - It has been claimed for more than a century that atmospheric new particle formation is primarily influenced by the presence of sulfuricacid. However, the activation process of sulfuric acid related clusters into detectable particles is still an unresolved topic. In this study we focus onthe PARADE campaign measurements conducted during August/September 2011 at Mt Kleiner Feldberg in central Germany. During this campaign a set ofradicals, organic and inorganic compounds and oxidants and aerosol properties were measured or calculated. We compared a range of organic and inorganic nucleation theories, evaluating their ability to simulate measured particle formation rates at 3 nm in diameter (J3) for a variety of different conditions. Nucleation mechanisms involving only sulfuric acid tentatively captured the observed noon-time daily maximum in J3, but displayed an increasing difference to J3 measurements during the rest of the diurnal cycle. Including large organic radicals, i.e. organic peroxy radicals (RO2) deriving from monoterpenes and their oxidation products, in the nucleation mechanism improved the correlation between observed and simulated J3. This supports a recently proposed empirical relationship for new particle formation that has been used in global models. However, the best match between theory and measurements for the site of interest was found for an activation process based on large organic peroxy radicals and stabilised Criegee intermediates (sCI). This novel laboratory-derived algorithm simulated the daily pattern and intensity of J3 observed in the ambient data. In this algorithm organic derived radicals are involved in activation and growth and link the formation rate of smallest aerosol particles with OH during day-time and NO3 during night-time. Because the RO2 lifetime is controlled by HO2 and NO we conclude that peroxy radicals and NO seem to play an important role for ambient radical chemistry not only with respect to oxidation capacity but also for the activation process of new particle formation. This is supposed to have significant impact of atmospheric radical species on aerosol chemistry and should be taken into account when studying the impact of new particles in climate feedback cycles.

AB - It has been claimed for more than a century that atmospheric new particle formation is primarily influenced by the presence of sulfuricacid. However, the activation process of sulfuric acid related clusters into detectable particles is still an unresolved topic. In this study we focus onthe PARADE campaign measurements conducted during August/September 2011 at Mt Kleiner Feldberg in central Germany. During this campaign a set ofradicals, organic and inorganic compounds and oxidants and aerosol properties were measured or calculated. We compared a range of organic and inorganic nucleation theories, evaluating their ability to simulate measured particle formation rates at 3 nm in diameter (J3) for a variety of different conditions. Nucleation mechanisms involving only sulfuric acid tentatively captured the observed noon-time daily maximum in J3, but displayed an increasing difference to J3 measurements during the rest of the diurnal cycle. Including large organic radicals, i.e. organic peroxy radicals (RO2) deriving from monoterpenes and their oxidation products, in the nucleation mechanism improved the correlation between observed and simulated J3. This supports a recently proposed empirical relationship for new particle formation that has been used in global models. However, the best match between theory and measurements for the site of interest was found for an activation process based on large organic peroxy radicals and stabilised Criegee intermediates (sCI). This novel laboratory-derived algorithm simulated the daily pattern and intensity of J3 observed in the ambient data. In this algorithm organic derived radicals are involved in activation and growth and link the formation rate of smallest aerosol particles with OH during day-time and NO3 during night-time. Because the RO2 lifetime is controlled by HO2 and NO we conclude that peroxy radicals and NO seem to play an important role for ambient radical chemistry not only with respect to oxidation capacity but also for the activation process of new particle formation. This is supposed to have significant impact of atmospheric radical species on aerosol chemistry and should be taken into account when studying the impact of new particles in climate feedback cycles.

U2 - 10.5194/acp-14-10823-2014

DO - 10.5194/acp-14-10823-2014

M3 - Journal article

SP - 10823

EP - 10843

JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

SN - 1680-7316

ER -