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. Understanding new particle formation and growth is important because of thestrong impact of these processes on climate and air quality. Measurements toelucidate the main new particle formation mechanisms are essential; however,these mechanisms have to be implemented in models to estimate their impacton the regional and global scale. Parameterizations are computationallycheap ways of implementing nucleation schemes in models, but they have theirlimitations, as they do not necessarily include all relevant parameters.Process models using sophisticated nucleation schemes can be useful for thegeneration of look-up tables in large-scale models or for the analysis ofindividual new particle formation events. In addition, some other importantproperties can be derived from a process model that implicitly calculatesthe evolution of the full aerosol size distribution, e.g., the particlegrowth rates. Within this study, a model (SANTIAGO – Sulfuric acid AmmoniaNucleaTIon And GrOwth model) is constructed that simulates new particleformation starting from the monomer of sulfuric acid up to a particle sizeof several hundred nanometers. The smallest sulfuric acid clusterscontaining one to four acid molecules and a varying amount of base (ammonia)are allowed to evaporate in the model, whereas growth beyond the pentamer(five sulfuric acid molecules) is assumed to be entirely collision-controlled. Themain goal of the present study is to derive appropriate thermodynamic dataneeded to calculate the cluster evaporation rates as a function oftemperature. These data are derived numerically from CLOUD (Cosmics LeavingOUtdoor Droplets) chamber new particle formation rates for neutral sulfuricacid–water–ammonia nucleation at temperatures between 208 and 292 K. Thenumeric methods include an optimization scheme to derive the best estimatesfor the thermodynamic data (d H and d S ) and a Monte Carlo method to derivetheir probability density functions. The derived data are compared toliterature values. Using different data sets for d H and d S in SANTIAGOdetailed comparison between model results and measured CLOUD new particleformation rates is discussed.

atmospheric chemistry and physics

New particle formation from sulfuric acid and ammonia: nucleation and growth model based on thermodynamics derived from CLOUD measurements for a wide range of conditions