Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms
-
Published:2006-09-11
Issue:12
Volume:6
Page:4079-4091
-
ISSN:1680-7324
-
Container-title:Atmospheric Chemistry and Physics
-
language:en
-
Short-container-title:Atmos. Chem. Phys.
Author:
Sihto S.-L.,Kulmala M.,Kerminen V.-M.,Dal Maso M.,Petäjä T.,Riipinen I.,Korhonen H.,Arnold F.,Janson R.,Boy M.,Laaksonen A.,Lehtinen K. E. J.
Abstract
Abstract. We have investigated the formation and early growth of atmospheric secondary aerosol particles building on atmospheric measurements. The measurements were part of the QUEST 2 campaign which took place in spring 2003 in Hyytiälä (Finland). During the campaign numerous aerosol particle formation events occurred of which 15 were accompanied by gaseous sulphuric acid measurements. Our detailed analysis of these 15 events is focussed on nucleation and early growth (to a diameter of 3 nm) of fresh particles. It revealed that new particle formation seems to be a function of the gaseous sulphuric acid concentration to the power from one to two when the time delay between the sulphuric acid and particle number concentration is taken into account. From the time delay the growth rates of freshly nucleated particles from 1 nm to 3 nm were determined. The mean growth rate was 1.2 nm/h and it was clearly correlated with the gaseous sulphuric acid concentration. We tested two nucleation mechanisms – recently proposed cluster activation and kinetic type nucleation – as possible candidates to explain the observed dependences, and determined experimental nucleation coefficients. We found that some events are dominated by the activation mechanism and some by the kinetic mechanism. Inferred coefficients for the two nucleation mechanisms are the same order of magnitude as chemical reaction coefficients in the gas phase and they correlate with the product of gaseous sulphuric acid and ammonia concentrations. This indicates that besides gaseous sulphuric acid also ammonia has a role in nucleation.
Publisher
Copernicus GmbH
Subject
Atmospheric Science
Reference46 articles.
1. Bernd, T., Böge, O., Stratmann, F., Heintzenberg, J., and Kulmala, M.: Rapid formation of new sulfuric acid particles at near-atmospheric conditions, Science, 307(5710), 698–700, 2005. 2. Birmili, W. and Wiedensohler, A.: The influence of meteorological parameters on ultrafine particle production at a continental site, J. Aerosol Sci., 29, S1015–1016, 1998. 3. Birmili, W., Berresheim, H., Plass-Dülmer, C., Elste, T., Gilge, S., Wiedensohler, A., and Uhrner, U.: The Hohenpeissenberg aerosol formation experiment (HAFEX): a long-term study including size-resolved aerosol, H2SO4, OH, and monoterpenes measurements, Atmos. Chem. Phys., 3, 361–376, 2003. 4. Boy, M., Kulmala, M., Ruuskanen, T. M., Pihlatie, M., Reissell, A., Aalto, P. P., Keronen, P., Dal Maso, M., Hellen, H., Hakola, H., Jansson, R., Hanke, M., and Arnold, F.: Sulphuric acid closure and contribution to nucleation mode particle growth, Atmos. Chem. Phys., 5, 863–878, 2005. 5. Cabada, J. C., Khlystov, A., Wittig, A. E., Pilinis, C., and Pandis, S. N.: Light scattering by fine particles during the Pittsburgh Air Quality Study: Measurements and modelling, J. Geophys. Res., 109, D16S03, https://doi.org/10.1029/2003JD004155, 2004.
Cited by
408 articles.
订阅此论文施引文献
订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献
|
|