1University of Helsinki, Department of Physics, P.O. Box 64, 00014 University of Helsinki, Finland
2Finnish Meteorological Institute, Climate and Global Change, P.O. Box 503, 00101 Helsinki, Finland
3University of Kuopio, Department of Physics, P.O. Box 1627, 70211 Kuopio, Finland
4Finnish Meteorological Institute, Kuopio Unit, P.O. Box 1627, 70211 Kuopio, Finland
Received: 11 Apr 2008 – Published in Atmos. Chem. Phys. Discuss.: 10 Jun 2008 – Published: 06 May 2009
Abstract. We have performed a series of simulations with an aerosol dynamics box model to study the connection between new particle formation and sulphuric acid concentration. For nucleation either activation mechanism with a linear dependence on the sulphuric acid concentration, kinetic mechanism with a squared dependence on the sulphuric acid concentration or ternary H2O-H2SO4-NH3 nucleation was assumed. The aim was to study the factors that affect the sulphuric acid dependence during the early stages of particle growth, and specifically to find conditions which would yield the linear dependence between the particle number concentration at 3–6 nm and sulphuric acid, as observed in field experiments. The simulations showed that the correlation with sulphuric acid may change during the growth from nucleation size to 3–6 nm size range, the main reason being the size dependent growth rate between 1 and 3 nm. In addition, the assumed size for the nucleated clusters had a crucial impact on the sulphuric acid dependence at 3 nm. A linear dependence between the particle number concentration at 3 nm and sulphuric acid was achieved, when activation nucleation mechanism was used with a low saturation vapour pressure for the condensable organic vapour, or with nucleation taking place at ~2 nm instead of ~1 nm. Simulations with activation, kinetic and ternary nucleation showed that ternary nucleation reproduces too steep dependence on sulphuric acid as compared to the linear or square dependence observed in field measurements.
Sihto, S.-L., Vuollekoski, H., Leppä, J., Riipinen, I., Kerminen, V.-M., Korhonen, H., Lehtinen, K. E. J., Boy, M., and Kulmala, M.: Aerosol dynamics simulations on the connection of sulphuric acid and new particle formation, Atmos. Chem. Phys., 9, 2933-2947, doi:10.5194/acp-9-2933-2009, 2009.