Abstract. This study presents ISORROPIA II, a thermodynamic equilibrium model for the K+–Ca2+–Mg2+–NH4+–Na+–SO42−–NO3−–Cl−–H2O aerosol system. A comprehensive evaluation of its performance is conducted against water uptake measurements for laboratory aerosol and predictions of the SCAPE2 thermodynamic module over a wide range of atmospherically relevant conditions. The two models agree well, to within 13% for aerosol water content and total PM mass, 16% for aerosol nitrate and 6% for aerosol chloride and ammonium. Largest discrepancies were found under conditions of low RH, primarily from differences in the treatment of water uptake and solid state composition. In terms of computational speed, ISORROPIA II was more than an order of magnitude faster than SCAPE2, with robust and rapid convergence under all conditions. The addition of crustal species does not slow down the thermodynamic calculations (compared to the older ISORROPIA code) because of optimizations in the activity coefficient calculation algorithm. Based on its computational rigor and performance, ISORROPIA II appears to be a highly attractive alternative for use in large scale air quality and atmospheric transport models.

[1] This study presents continued development of the Nenes and Seinfeld (2003) cloud droplet activation parameterization. First, we expanded the formulation to (1) allow for a lognormal representation of aerosol size distribution, and (2) include a size-dependant mass transfer coefficient for the growth of water droplets to accommodate the effect of size (and potentially organic films) on the droplet growth rate. The performance of the new scheme is evaluated by comparing the parameterized cloud droplet number concentration with that of a detailed numerical activation cloud parcel model. The resulting modified parameterization robustly and closely tracks the parcel model simulations, even for low values of the accommodation coefficient (average error 4.1 ± 1.3%). The modifications to include the effect of accommodation coefficient do not increase the computational cost but substantially improve the parameterization performance. This work offers a robust, computationally efficient and first-principles approach for directly linking complex chemical effects (e.g., surface tension depression, changes in water vapor accommodation, solute contribution from partial solubility) on aerosol activation within a global climate modeling framework.Citation: Fountoukis, C., and A. Nenes (2005), Continued development of a cloud droplet formation parameterization for global climate models,

Abstract. This paper synthesizes the available scientific information connecting atmospheric nucleation with subsequent cloud condensation nuclei (CCN) formation. We review both observations and model studies related to this topic, and discuss the potential climatic implications. We conclude that CCN production associated with atmospheric nucleation is both frequent and widespread phenomenon in many types of continental boundary layers, and probably also over a large fraction of the free troposphere. The contribution of nucleation to the global CCN budget spans a relatively large uncertainty range, which, together with our poor understanding of aerosol-cloud interactions, results in major uncertainties in the radiative forcing by atmospheric aerosols. In order to better quantify the role of atmospheric nucleation in CCN formation and Earth System behavior, more information is needed on (i) the factors controlling atmospheric CCN production and (ii) the properties of both primary and secondary CCN and their interconnections. In future investigations, more emphasis should be put on combining field measurements with regional and large-scale model studies.

We present a new aerosol microphysics and gas aerosol partitioning submodel (Global Modal-aerosol eXtension, GMXe) implemented within the ECHAM/MESSy Atmospheric Chemistry model (EMAC, version 1.8). The submodel is computationally efficient and is suitable for medium to long term simulations with global and regional models. The aerosol size distribution is treated using 7 log-normal modes and has the same microphysical core as the M7 submodel (Vignati et al., 2004). <br><br> The main developments in this work are: (i) the extension of the aerosol emission routines and the M7 microphysics, so that an increased (and variable) number of aerosol species can be treated (new species include sodium and chloride, and potentially magnesium, calcium, and potassium), (ii) the coupling of the aerosol microphysics to a choice of treatments of gas/aerosol partitioning to allow the treatment of semi-volatile aerosol, and, (iii) the implementation and evaluation of the developed submodel within the EMAC model of atmospheric chemistry. <br><br> Simulated concentrations of black carbon, particulate organic matter, dust, sea spray, sulfate and ammonium aerosol are shown to be in good agreement with observations (for all species at least 40% of modeled values are within a factor of 2 of the observations). The distribution of nitrate aerosol is compared to observations in both clean and polluted regions. Concentrations in polluted continental regions are simulated quite well, but there is a general tendency to overestimate nitrate, particularly in coastal regions (geometric mean of modelled values/geometric mean of observed data ≈2). In all regions considered more than 40% of nitrate concentrations are within a factor of two of the observations. Marine nitrate concentrations are well captured with 96% of modeled values within a factor of 2 of the observations

Abstract. In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.

Abstract. Measurements of cloud condensation nuclei (CCN) concentrations (cm −3 ) between 0.2 and 1.0% supersaturation, aerosol size distribution and chemical composition were performed at a remote marine site in the eastern Mediterranean, from September to October 2007 during the FAME07 campaign. Most of the particles activate at ∼0.6% supersaturation, characteristic of the aged nature of the aerosol sampled. Application of Köhler theory, using measurements of bulk composition, size distribution, and assuming that organics are insoluble resulted in agreement between predicted and measured CCN concentrations within 7±11% for all supersaturations, with a tendency for CCN underprediction (16±6%; r 2 =0.88) at the lowest supersaturations (0.21%). Including the effects of the water-soluble organic fraction (which represent around 70% of the total organic content) reduces the average underprediction bias at the low supersaturations, resulting in a total closure error of 0.6±6%. Using threshold droplet growth analysis, the growth kinetics of ambient CCN is consistent with NaCl calibration experiments; hence the presence of aged organics does not suppress the rate of water uptake in this environment. The knowledge of the soluble salt fraction is sufficient for the description of the CCN activity in this area.

Abstract. Fast measurements of aerosol and gas-phase constituents coupled with the ISORROPIA-II thermodynamic equilibrium model are used to study the partitioning of semivolatile inorganic species and phase state of Mexico City aerosol sampled at the T1 site during the MILAGRO 2006 campaign. Overall, predicted semivolatile partitioning agrees well with measurements. PM 2.5 is insensitive to changes in ammonia but is to acidic semivolatile species. For particle sizes up to 1µm diameter, semi-volatile partitioning requires 15-30 min to equilibrate; longer time is typically required during the night and early morning hours. Aerosol and gas-phase speciation always exhibits substantial temporal variability, so that aerosol composition measurements (bulk or size-resolved) obtained over large integration periods are not reflective of its true state. When the aerosol sulfate-to-nitrate molar ratio is less than unity, predictions improve substantially if the aerosol is assumed to follow the deliquescent phase diagram. Treating crustal species as "equivalent sodium" (rather than explicitly) in the thermodynamic equilibrium calculations introduces important biases in predicted aerosol water uptake, nitrate and ammonium; neglecting crustals further increases errors dramatiCorrespondence to: A. Nenes (athanasios.nenes@gatech.edu) cally. This suggests that explicitly considering crustals in the thermodynamic calculations is required to accurately predict the partitioning and phase state of aerosols.

Abstract. PMCAMx-2008, a detailed three-dimensional chemical transport model (CTM), was applied to Europe to simulate the mass concentration and chemical composition of particulate matter (PM) during May 2008. The model includes a state-of-the-art organic aerosol module which is based on the volatility basis set framework treating both primary and secondary organic components as semivolatile and photochemically reactive. The model performance is evaluated against high time resolution aerosol mass spectrometer (AMS) ground and airborne measurements. Overall, organic aerosol is predicted to account for 32 % of total PM 1 at ground level during May 2008, followed by sulfate (30 %), crustal material and sea-salt (14 %), ammonium (13 %), nitrate (7 %), and elemental carbon (4 %). The model predicts that fresh primary OA (POA) is a small contributor to organic PM concentrations in Europe during late spring, and that oxygenated species (oxidized primary and biogenic secondary) dominate the ambient OA. The Mediterranean region is the only area in Europe where sulfate concentrations are predicted to be much higher than the OA, while organic matter is predicted to be the dominant PM 1 species in cenCorrespondence to: S. N. Pandis (spyros@andrew.cmu.edu) tral and northern Europe. The comparison of the model predictions with the ground measurements in four measurement stations is encouraging. The model reproduces more than 94 % of the daily averaged data and more than 87 % of the hourly data within a factor of 2 for PM 1 OA. The model tends to predict relatively flat diurnal profiles for PM 1 OA in many areas, both rural and urban in agreement with the available measurements. The model performance against the high time resolution airborne measurements at multiple altitudes and locations is as good as its performance against the ground level hourly measurements. There is no evidence of missing sources of OA aloft over Europe during this period.