How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation

Boris Bonn, Markku Kulmala, Ilona Riipinen, Sanna-Liisa Sihto, Taina M Ruuskanen

    Research output: Contribution to journalArticleScientificpeer-review

    Abstract

    New particle formation has been observed to take place all around the world. However, because of the inability to determine the chemical composition of the smallest clusters or particles, indirect tools such as the correlation between nucleation rate and measured sulfuric acid concentrations have been used to infer the nucleation mechanism. In this study we describe the observed correlation with gaseous sulfuric acid concentrations by interactions of sesquiterpene oxidation products with sulfuric acid. Two formation pathways of nucleation initiating molecules are considered. The interaction of sulfuric acid with organic sulfates, which are formed from stabilized Criegee intermediates (sCIs, formed from sesquiterpenes), can be used to explain the observed squared relationship between particle formation rate and ambient sulfuric acid concentrations. The corresponding linear dependence is explained with the participation of secondary ozonides, which are formed from sCIs and aldehydes. Both pathways are negatively affected by increasing water vapor concentration as observed in recent studies. In order to check the assumptions made we apply the derived nucleation coefficients to measurements of the BACCI/QUEST IV campaign made during spring 2005 in Hyytiala, Finland. A reasonable agreement between the measurement data and the predicted nucleation rates is found, giving support for the presented nucleation description.
    Original languageEnglish
    JournalJournal of Geophysical Research
    ISSN0148-0227
    DOIs
    Publication statusPublished - 2008
    MoE publication typeA1 Journal article-refereed

    Cite this

    @article{2f40ce3a5b3840f2b2f17611a3d3a7f3,
    title = "How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation",
    abstract = "New particle formation has been observed to take place all around the world. However, because of the inability to determine the chemical composition of the smallest clusters or particles, indirect tools such as the correlation between nucleation rate and measured sulfuric acid concentrations have been used to infer the nucleation mechanism. In this study we describe the observed correlation with gaseous sulfuric acid concentrations by interactions of sesquiterpene oxidation products with sulfuric acid. Two formation pathways of nucleation initiating molecules are considered. The interaction of sulfuric acid with organic sulfates, which are formed from stabilized Criegee intermediates (sCIs, formed from sesquiterpenes), can be used to explain the observed squared relationship between particle formation rate and ambient sulfuric acid concentrations. The corresponding linear dependence is explained with the participation of secondary ozonides, which are formed from sCIs and aldehydes. Both pathways are negatively affected by increasing water vapor concentration as observed in recent studies. In order to check the assumptions made we apply the derived nucleation coefficients to measurements of the BACCI/QUEST IV campaign made during spring 2005 in Hyytiala, Finland. A reasonable agreement between the measurement data and the predicted nucleation rates is found, giving support for the presented nucleation description.",
    author = "Boris Bonn and Markku Kulmala and Ilona Riipinen and Sanna-Liisa Sihto and Ruuskanen, {Taina M}",
    year = "2008",
    doi = "10.1029/2007JD009327",
    language = "English",
    journal = "Journal of Geophysical Research",
    issn = "0148-0227",
    publisher = "American Geophysical Union",

    }

    How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation. / Bonn, Boris; Kulmala, Markku; Riipinen, Ilona; Sihto, Sanna-Liisa; Ruuskanen, Taina M.

    In: Journal of Geophysical Research, 2008.

    Research output: Contribution to journalArticleScientificpeer-review

    TY - JOUR

    T1 - How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation

    AU - Bonn, Boris

    AU - Kulmala, Markku

    AU - Riipinen, Ilona

    AU - Sihto, Sanna-Liisa

    AU - Ruuskanen, Taina M

    PY - 2008

    Y1 - 2008

    N2 - New particle formation has been observed to take place all around the world. However, because of the inability to determine the chemical composition of the smallest clusters or particles, indirect tools such as the correlation between nucleation rate and measured sulfuric acid concentrations have been used to infer the nucleation mechanism. In this study we describe the observed correlation with gaseous sulfuric acid concentrations by interactions of sesquiterpene oxidation products with sulfuric acid. Two formation pathways of nucleation initiating molecules are considered. The interaction of sulfuric acid with organic sulfates, which are formed from stabilized Criegee intermediates (sCIs, formed from sesquiterpenes), can be used to explain the observed squared relationship between particle formation rate and ambient sulfuric acid concentrations. The corresponding linear dependence is explained with the participation of secondary ozonides, which are formed from sCIs and aldehydes. Both pathways are negatively affected by increasing water vapor concentration as observed in recent studies. In order to check the assumptions made we apply the derived nucleation coefficients to measurements of the BACCI/QUEST IV campaign made during spring 2005 in Hyytiala, Finland. A reasonable agreement between the measurement data and the predicted nucleation rates is found, giving support for the presented nucleation description.

    AB - New particle formation has been observed to take place all around the world. However, because of the inability to determine the chemical composition of the smallest clusters or particles, indirect tools such as the correlation between nucleation rate and measured sulfuric acid concentrations have been used to infer the nucleation mechanism. In this study we describe the observed correlation with gaseous sulfuric acid concentrations by interactions of sesquiterpene oxidation products with sulfuric acid. Two formation pathways of nucleation initiating molecules are considered. The interaction of sulfuric acid with organic sulfates, which are formed from stabilized Criegee intermediates (sCIs, formed from sesquiterpenes), can be used to explain the observed squared relationship between particle formation rate and ambient sulfuric acid concentrations. The corresponding linear dependence is explained with the participation of secondary ozonides, which are formed from sCIs and aldehydes. Both pathways are negatively affected by increasing water vapor concentration as observed in recent studies. In order to check the assumptions made we apply the derived nucleation coefficients to measurements of the BACCI/QUEST IV campaign made during spring 2005 in Hyytiala, Finland. A reasonable agreement between the measurement data and the predicted nucleation rates is found, giving support for the presented nucleation description.

    U2 - 10.1029/2007JD009327

    DO - 10.1029/2007JD009327

    M3 - Article

    JO - Journal of Geophysical Research

    JF - Journal of Geophysical Research

    SN - 0148-0227

    ER -