References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-10-11223-2010

On the roles of sulphuric acid and low-volatility organic vapours in the initial steps of atmospheric new particle formation

Paasonen

¹ Nieminen

¹ Asmi

² Manninen

H. E.

¹ Petäjä

¹ Plass-Dülmer

³ Flentje

³ Birmili

⁴ Wiedensohler

⁴ Hõrrak

⁵ Metzger

⁶ Hamed

⁷ Laaksonen

² ⁷ Facchini

M. C.

⁸ Kerminen

V.-M.

¹ ² Kulmala

¹ ⁹

University of Helsinki, Helsinki, Finland

Finnish Meteorology Institute, Helsinki, Finland

Meteorological Observatory Hohenpeissenberg, German Meteorological Service, Germany

Institute for Tropospheric Research, Leipzig, Germany

University of Tartu, Tartu, Estonia

Ionicon Analytik GmbH, Innsbruck, Austria

University of Eastern Finland, Kuopio, Finland

Institute of Atmospheric Sciences and Climate, Bologna, Italy

Stockholm University, Stockholm, Sweden

30 11 2010

10 22 11223 11242

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

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Sulphuric acid and organic vapours have been identified as the key components in the ubiquitous secondary new particle formation in the atmosphere. In order to assess their relative contribution and spatial variability, we analysed altogether 36 new particle formation events observed at four European measurement sites during EUCAARI campaigns in 2007–2009. We tested models of several different nucleation mechanisms coupling the formation rate of neutral particles (J) with the concentration of sulphuric acid ([H2SO4]) or low-volatility organic vapours ([org]) condensing on sub-4 nm particles, or with a combination of both concentrations. Furthermore, we determined the related nucleation coefficients connecting the neutral nucleation rate J with the vapour concentrations in each mechanism. The main goal of the study was to identify the mechanism of new particle formation and subsequent growth that minimizes the difference between the modelled and measured nucleation rates. At three out of four measurement sites – Hyytiälä (Finland), Melpitz (Germany) and San Pietro Capofiume (Italy) – the nucleation rate was closely connected to squared sulphuric acid concentration, whereas in Hohenpeissenberg (Germany) the low-volatility organic vapours were observed to be dominant. However, the nucleation rate at the sulphuric acid dominant sites could not be described with sulphuric acid concentration and a single value of the nucleation coefficient, as K in J=K [H2SO4]2, but the median coefficients for different sites varied over an order of magnitude. This inter-site variation was substantially smaller when the heteromolecular homogenous nucleation between H2SO4 and organic vapours was assumed to take place in addition to homogenous nucleation of H2SO4 alone, i.e., J=KSA1[H2SO4]2+KSA2[H2SO4][org]. By adding in this equation a term describing homomolecular organic vapour nucleation, Ks3[org]2, equally good results were achieved. In general, our results suggest that organic vapours do play a role, not only in the condensational growth of the particles, but also in the nucleation process, with a site-specific degree.

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