Case studies of particle formation events observed in boreal forests: implications for nucleation mechanisms

Aerosol nucleation events observed worldwide may have significant climatic and health implications. However, the specific nucleation mechanisms remain ambiguous. Here, we report case studies of eight nucleation events observed during an intensive field campaign at a boreal forest site (Hyytiala, Finland) in spring 2005. The present analysis is based on comprehensive kinetic simulations using an ion-mediated nucleation (IMN) model in which the key physical and chemical parameters are constrained by a variety of recent measurements. Out of the 22 days of the campaign on which nucleation events were observed, eight major events were selected for detailed analysis on the basis of indications that the observed air masses were relatively homogeneous. In most of these cases, reasonable agreement is found between IMN predictions and field data for a range of variables, including critical nucleation sizes, size-dependent overcharging ratios, and the concentrations of 1.8-3 nm stable clusters and 3-6 nm particles, and their diurnal variations. The possible reasons leading to substantial differences between observation and theory in some cases are also explored. Statistically, roughly 80% of the nucleation events recorded during the Hyytiala campaign exhibited mean size-dependent particle overcharging ratios within the range of, or exceeding, those predicted by the IMN model, suggesting that ion nucleation processes were significant during these events. The nucleation rates calculated using the IMN modeling approach are contrasted with those predicted by other theories/models, and key differences between the results are discussed. In particular, it is concluded that the ion nucleation model originally developed by Lovejoy et al. (2004) significantly under-predicts ion nucleation rates, and cannot explain the new observations from Hyytiala regarding the electrical properties of nanoparticles. We also show that, for the well documented conditions of the Hyytiala project, the binary and ternary homogeneous nucleation rates calculated using the most current theories would fall well below similar to 10(-7) cm(-3) s(-1), and thus would be negligible.