Semi-empirical parameterization of size-dependent atmospheric nanoparticle growth in continental environments

by S. A K Häkkinen, H. E. Manninen, T. Yli-Juuti, J. Merikanto, M. K. Kajos, T. Nieminen, S. D. D'Andrea, A. Asmi, J. R. Pierce, M. Kulmala, I. Riipinen show all authors
Atmospheric Chemistry and Physics ()
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Abstract

The capability to accurately yet efficiently represent atmospheric\nnanoparticle growth by biogenic and anthropogenic secondary organics is\na challenge for current atmospheric large-scale models. It is, however,\ncrucial to predict nanoparticle growth accurately in order to reliably\nestimate the atmospheric cloud condensation nuclei (CCN) concentrations.\nIn this work we introduce a simple semi-empirical parameterization for\nsub-20 nm particle growth that distributes secondary organics to the\nnanoparticles according to their size and is therefore able to reproduce\nparticle growth observed in the atmosphere. The parameterization\nincludes particle growth by sulfuric acid, secondary organics from\nmonoterpene oxidation (SORG(MT)) and an additional condensable vapor of\nnon-monoterpene organics ({''}background{''}). The performance of the\nproposed parameterization was investigated using ambient data on\nparticle growth rates in three diameter ranges (1.5-3 nm, 3-7 nm and\n7-20 nm). The growth rate data were acquired from particle / air ion\nnumber size distribution measurements at six continental sites over\nEurope. The longest time series of 7 yr (2003-2009) was obtained from a\nboreal forest site in Hyytiala, Finland, while about one year of data\n(2008-2009) was used for the other stations. The extensive ambient\nmeasurements made it possible to test how well the parameterization\ncaptures the seasonal cycle observed in sub-20 nm particle growth and to\ndetermine the weighing factors for distributing the SORG(MT) for\ndifferent sized particles as well as the background mass flux\n(concentration). Besides the monoterpene oxidation products, background\norganics with a concentration comparable to SORGMT, around 6x10(7)\ncm(-3) (consistent with an additional global SOA yield of 100 Tg yr(-1))\nwas needed to reproduce the observed nanoparticle growth. Simulations\nwith global models suggest that the ``background{''} could be linked to\nsecondary biogenic organics that are formed in the presence of\nanthropogenic pollution.

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