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- ItemOn microphysical processes of noctilucent clouds (NLC): Observations and modeling of mean and width of the particle size-distribution(Göttingen : Copernicus, 2010) Baumgarten, G.; Fiedler, J.; Rapp, M.Noctilucent clouds (NLC) in the polar summer mesopause region have been observed in Norway (69° N, 16° E) between 1998 and 2009 by 3-color lidar technique. Assuming a mono-modal Gaussian size distribution we deduce mean and width of the particle sizes throughout the clouds. We observe a quasi linear relationship between distribution width and mean of the particle size at the top of the clouds and a deviation from this behavior for particle sizes larger than 40 nm, most often in the lower part of the layer. The vertically integrated particle properties show that 65% of the data follows the linear relationship with a slope of 0.42±0.02 for mean particle sizes up to 40 nm. For the vertically resolved particle properties (Δz = Combining double low line 0.15 km) the slope is comparable and about 0.39±0.03. For particles larger than 40 nm the distribution width becomes nearly independent of particle size and even decreases in the lower part of the layer. We compare our observations to microphysical modeling of noctilucent clouds and find that the distribution width depends on turbulence, the time that turbulence can act (cloud age), and the sampling volume/time (atmospheric variability). The model results nicely reproduce the measurements and show that the observed slope can be explained by eddy diffusion profiles as observed from rocket measurements. © 2010 Author(s).
- ItemTreatment of non-ideality in the SPACCIM multiphase model - Part 1: Model development(München : European Geopyhsical Union, 2016) Rusumdar, A.J.; Wolke, R.; Tilgner, A.; Herrmann, H.Ambient tropospheric deliquesced particles generally comprise a complex mixture of electrolytes, organic compounds, and water. Dynamic modeling of physical and chemical processes in this complex matrix is challenging. Thus, up-to-date multiphase chemistry models generally do not consider non-ideal solution effects. Therefore, the present study was aimed at presenting further development of the SPACCIM (Spectral Aerosol Cloud Chemistry Interaction Model) through treatment of solution non-ideality, which has not been considered before. The present paper firstly describes the model developments including (i) the implementation of solution non-ideality in aqueous-phase reaction kinetics in the SPACCIM framework, (ii) the advancements in the coupling scheme of microphysics and multiphase chemistry and (iii) the required adjustments of the numerical schemes, especially in the sparse linear solver and the calculation of the Jacobian. Secondly, results of sensitivity investigations are outlined, aiming at the evaluation of different activity coefficient modules and the examination of the contributions of different intermolecular forces to the overall activity coefficients. Finally, first results obtained with the new model framework are presented. The SPACCIM parcel model was developed and, so far, applied for the description of aerosol–cloud interactions. To advance SPACCIM also for modeling physical and chemical processes in deliquesced particles, the solution non-ideality has to be taken into account by utilizing activities in reaction terms instead of aqueous concentrations. The main goal of the extended approach was to provide appropriate activity coefficients for solved species. Therefore, an activity coefficient module was incorporated into the kinetic model framework of SPACCIM. Based on an intercomparison of different activity coefficient models and the comparison with experimental data, the AIOMFAC approach was implemented and extended by additional interaction parameters from the literature for mixed organic–inorganic systems. Moreover, the performance and the capability of the applied activity coefficient module were evaluated by means of water activity measurements, literature data and results of other activity coefficient models. Comprehensive comparison studies showed that the SpactMod (SPACCIM activity coefficient module) is valuable for predicting the thermodynamic behavior of complex mixtures of multicomponent atmospheric aerosol particles. First simulations with a detailed chemical mechanism have demonstrated the applicability of SPACCIM-SpactMod. The simulations indicate that the treatment of solution non-ideality might be needed for modeling multiphase chemistry processes in deliquesced particles. The modeled activity coefficients imply that chemical reaction fluxes of chemical processes in deliquesced particles can be both decreased and increased depending on the particular species involved in the reactions. For key ions, activity coefficients on the order of 0.1–0.8 and a strong dependency on the charge state as well as the RH conditions are modeled, implying a lowered chemical processing of ions in concentrated solutions. In contrast, modeled activity coefficients of organic compounds are in some cases larger than 1 under deliquesced particle conditions and suggest the possibility of an increased chemical processing of organic compounds. Moreover, the model runs have shown noticeable differences in the pH values calculated with and without consideration of solution non-ideality. On average, the predicted pH values of the simulations considering solution non-ideality are −0.27 and −0.44 pH units lower under 90 and 70 % RH conditions, respectively. More comprehensive results of detailed SPACCIM-SpactMod studies on the multiphase processing in organic–inorganic mixtures of deliquesced particles are described in a companion paper.