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ABSTRACT: Different methods of determining formation rates of 3 nm particles are compared, basing on analysis of simulated data, but the results are valid for analyses of experimental particle size distribution data as well. The study shows that the method of determining formation rates indirectly from measured number concentration data of 3–6 nm particles is generally in good agreement with the theoretical calculation with a systematic error of 0–20%. While this is often accurate enough, a simple modification to the approximative equation for the formation rate is recommended. Additionally, the temporal connection between the concentration of the nucleating vapour and the formation rate is studied. It is concluded that the often used power-law connecting these two is inaccurate.
Atmospheric Chemistry and Physics Discussions. 01/2010;
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ABSTRACT: We carried out column model simulations to study particle fluxes and deposition and to evaluate different particle formation mechanisms at a boreal forest site in Finland. We show that kinetic nucleation of sulphuric acid cannot be responsible for new particle formation alone as the vertical profile of particle number distribution does not correspond to observations. Instead organic induced nucleation leads to good agreement confirming the relevance of the aerosol formation mechanism including organic compounds emitted by biosphere. Simulation of aerosol concentration inside the atmospheric boundary layer during nucleation days shows highly dynamical picture, where particle formation is coupled with chemistry and turbulent transport. We have demonstrated suitability of our turbulent mixing scheme in reproducing most important characteristics of particle dynamics inside the atmospheric boundary layer. Deposition and particle flux simulations show that deposition affects noticeably only the smallest particles at the lowest part of the atmospheric boundary layer.
Atmospheric Chemistry and Physics Discussions. 01/2010;
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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 or ternary H2O-H2SO4-NH3 nucleation was assumed. We investigated the factors that affect the sulphuric acid dependence during the early stages of particle growth, and tried 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. The simulations yielded a linear dependence between the particle number concentration at 3 nm and sulphuric acid, when a low saturation vapour pressure for the condensable organic vapour was assumed, or when nucleation took place at ~2 nm instead of ~1 nm. Comparison of results with activation and ternary nucleation showed that ternary nucleation cannot explain the experimentally observed linear or square dependence on sulphuric acid.
Atmospheric Chemistry and Physics Discussions. 01/2008;
