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- ItemAnalysis of nucleation events in the European boundary layer using the regional aerosol-climate model REMO-HAM with a solar radiation-driven OH-proxy(München : European Geopyhsical Union, 2014) Pietikäinen, J.-P.; Mikkonen, S.; Hamed, A.; Hienola, A.I.; Birmili, W.; Kulmala, M.; Laaksonen, A.This work describes improvements in the regional aerosol–climate model REMO-HAM in order to simulate more realistically the process of atmospheric new particle formation (NPF). A new scheme was implemented to simulate OH radical concentrations using a proxy approach based on observations and also accounting for the effects of clouds upon OH concentrations. Second, the nucleation rate calculation was modified to directly simulate the formation rates of 3 nm particles, which removes some unnecessary steps in the formation rate calculations used earlier in the model. Using the updated model version, NPF over Europe was simulated for the periods 2003–2004 and 2008–2009. The statistics of the simulated particle formation events were subsequently compared to observations from 13 ground-based measurement sites. The new model shows improved agreement with the observed NPF rates compared to former versions and can simulate the event statistics realistically for most parts of Europe.
- ItemFormation and growth of nucleated particles into cloud condensation nuclei: Model-measurement comparison(München : European Geopyhsical Union, 2013) Westervelt, D.M.; Pierce, J.R.; Riipinen, I.; Trivitayanurak, W.; Hamed, A.; Kulmala, M.; Laaksonen, A.; Decesari, S.; Adams, P.J.Aerosol nucleation occurs frequently in the atmosphere and is an important source of particle number. Observations suggest that nucleated particles are capable of growing to sufficiently large sizes that they act as cloud condensation nuclei (CCN), but some global models have reported that CCN concentrations are only modestly sensitive to large changes in nucleation rates. Here we present a novel approach for using long-term size distribution observations to evaluate a global aerosol model's ability to predict formation rates of CCN from nucleation and growth events. We derive from observations at five locations nucleation-relevant metrics such as nucleation rate of particles at diameter of 3 nm (J3), diameter growth rate (GR), particle survival probability (SP), condensation and coagulation sinks, and CCN formation rate (J100). These quantities are also derived for a global microphysical model, GEOS-Chem-TOMAS, and compared to the observations on a daily basis. Using GEOS-Chem-TOMAS, we simulate nucleation events predicted by ternary (with a 10−5 tuning factor) or activation nucleation over one year and find that the model slightly understates the observed annual-average CCN formation mostly due to bias in the nucleation rate predictions, but by no more than 50% in the ternary simulations. At the two locations expected to be most impacted by large-scale regional nucleation, Hyytiälä and San Pietro Capofiume, predicted annual-average CCN formation rates are within 34 and 2% of the observations, respectively. Model-predicted annual-average growth rates are within 25% across all sites but also show a slight tendency to underestimate the observations, at least in the ternary nucleation simulations. On days that the growing nucleation mode reaches 100 nm, median single-day survival probabilities to 100 nm for the model and measurements range from less than 1–6% across the five locations we considered; however, this does not include particles that may eventually grow to 100 nm after the first day. This detailed exploration of new particle formation and growth dynamics adds support to the use of global models as tools for assessing the contribution of microphysical processes such as nucleation to the total number and CCN budget.
- ItemSeasonal variability of Saharan desert dust and ice nucleating particles over Europe(München : European Geopyhsical Union, 2015) Hande, L.B.; Engler, C.; Hoose, C.; Tegen, I.Dust aerosols are thought to be the main contributor to atmospheric ice nucleation. While there are case studies supporting this, a climatological sense of the importance of dust to atmospheric ice nucleating particle (INP) concentrations and its seasonal variability over Europe is lacking. Here, we use a mesoscale model to estimate Saharan dust concentrations over Europe in 2008. There are large differences in median dust concentrations between seasons, with the highest concentrations and highest variability in the lower to mid-troposphere. Laboratory-based ice nucleation parameterisations are applied to these simulated dust number concentrations to calculate the potential INP resulting from immersion freezing and deposition nucleation on these dust particles. The potential INP concentrations increase exponentially with height due to decreasing temperatures in the lower and mid-troposphere. When the ice-activated fraction increases sufficiently, INP concentrations follow the dust particle concentrations. The potential INP profiles exhibit similarly large differences between seasons, with the highest concentrations in spring (median potential immersion INP concentrations nearly 105 m−3, median potential deposition INP concentrations at 120% relative humidity with respect to ice over 105 m−3), about an order of magnitude larger than those in summer. Using these results, a best-fit function is provided to estimate the potential INPs for use in limited-area models, which is representative of the normal background INP concentrations over Europe. A statistical evaluation of the results against field and laboratory measurements indicates that the INP concentrations are in close agreement with observations.