Abstract. Large cloud condensation nuclei (CCN) (e.g., aged dust particles and seasalt) cannot attain their equilibrium size during the typical timescale of cloud droplet activation. Cloud activation parameterizations applied to aerosol with a large fraction of large CCN often do not account for this limitation adequately and can give biased predictions of cloud droplet number concentration (CDNC). Here we present a simple approach to address this problem that can easily be incorporated into cloud activation parameterizations. This method is demonstrated with activation parameterizations based on the "population splitting" concept of Nenes and Seinfeld (2003); it is shown that accounting for large CCN effects eliminates a positive bias in CDNC where the aerosol dry geometric diameter is greater than 0.5 µm. The method proposed here can also be extended to include the water vapor depletion from pre-existing droplets and ice crystals in global and regional atmospheric models.

[1] Aerosol-cloud interaction studies to date consider aerosol with a substantial fraction of soluble material as the sole source of cloud condensation nuclei (CCN). Emerging evidence suggests that mineral dust can act as good CCN through water adsorption onto the surface of particles. This study provides a first assessment of the contribution of insoluble dust to global CCN and cloud droplet number concentration (CDNC). Simulations are carried out with the NASA Global Modeling Initiative chemical transport model with an online aerosol simulation, considering emissions from fossil fuel, biomass burning, marine, and dust sources. CDNC is calculated online and explicitly considers the competition of soluble and insoluble CCN for water vapor. The predicted annual average contribution of insoluble mineral dust to CCN and CDNC in cloud-forming areas is up to 40 and 23.8%, respectively. Sensitivity tests suggest that uncertainties in dust size distribution and water adsorption parameters modulate the contribution of mineral dust to CDNC by 23 and 56%, respectively. Coating of dust by hygroscopic salts during the atmospheric aging causes a twofold enhancement of the dust contribution to CCN; the aged dust, however, can substantially deplete in-cloud supersaturation during the initial stages of cloud formation and can eventually reduce CDNC. Considering the hydrophilicity from adsorption and hygroscopicity from solute is required to comprehensively capture the dust-warm cloud interactions. The framework presented here addresses this need and can be easily integrated in atmospheric models.

[1] Several different ice nucleation parameterizations in two different General Circulation Models (GCMs) are used to understand the effects of ice nucleation on the mean climate state, and the Aerosol Indirect Effects (AIE) of cirrus clouds on climate. Simulations have a range of ice microphysical states that are consistent with the spread of observations, but many simulations have higher present-day ice crystal number concentrations than in-situ observations. These different states result from different parameterizations of ice cloud nucleation processes, and feature different balances of homogeneous and heterogeneous nucleation. Black carbon aerosols have a small (À0.06 Wm À2 ) and not statistically significant AIE when included as ice nuclei, for nucleation efficiencies within the range of laboratory measurements. Indirect effects of anthropogenic aerosols on cirrus clouds occur as a consequence of increasing anthropogenic sulfur emissions with different mechanisms important in different models. In one model this is due to increases in homogeneous nucleation fraction, and in the other due to increases in heterogeneous nucleation with coated dust. The magnitude of the effect is the same however. The resulting ice AIE does not seem strongly dependent on the balance between homogeneous and heterogeneous ice nucleation. Regional effects can reach several Wm À2 . Indirect effects are slightly larger for those states with less homogeneous nucleation and lower ice number concentration in the base state. The total ice AIE is estimated at 0.27 AE 0.10 Wm À2 (1s uncertainty). This represents a 20% offset of the simulated total shortwave AIE for ice and liquid clouds of À1.6 Wm À2 .

[1] This work presents a new physically based parameterization of cirrus cloud formation for use in large-scale models which is robust, computationally efficient, and links chemical effects (e.g., water activity and water vapor deposition effects) with ice formation via homogenous freezing. The parameterization formulation is based on ascending parcel theory and provides expressions for the ice crystal size distribution and the crystal number concentration, explicitly considering the effects of aerosol size and number, updraft velocity, and deposition coefficient. The parameterization is evaluated against a detailed numerical cirrus cloud parcel model (developed during this study), the equations of which are solved using a novel Lagrangian particle-tracking scheme. Over a broad range of cirrus-forming conditions, the parameterization reproduces the results of the parcel model within a factor of 2 and with an average relative error of À15%. If numerical model simulations are used to constrain the parameterization, error further decreases to 1 ± 28%.

Abstract.We investigated the impact of mineral dust particles on clouds, radiation and atmospheric state during a strong Saharan dust event over Europe in May 2008, applying a comprehensive online-coupled regional model framework that explicitly treats particle microphysics and chemical composition. Sophisticated parameterizations for aerosol activation and ice nucleation, together with two-moment cloud microphysics are used to calculate the interaction of the different particles with clouds depending on their physical and chemical properties.The impact of dust on cloud droplet number concentration was found to be low, with just a slight increase in cloud droplet number concentration for both uncoated and coated dust. For temperatures lower than the level of homogeneous freezing, no significant impact of dust on the number and mass concentration of ice crystals was found, though the concentration of frozen dust particles reached up to 100 l −1 during the ice nucleation events. Mineral dust particles were found to have the largest impact on clouds in a temperature range between freezing level and the level of homogeneous freezing, where they determined the number concentration of ice crystals due to efficient heterogeneous freezing of the dust particles and modified the glaciation of mixed phase clouds.Our simulations show that during the dust events, ice crystals concentrations were increased twofold in this temperature range (compared to if dust interactions are neglected).This had a significant impact on the cloud optical properties, causing a reduction in the incoming short-wave radiation at the surface up to −75 W m −2 . Including the direct interaction of dust with radiation caused an additional reduction in the incoming short-wave radiation by 40 to 80 W m −2 , and the incoming long-wave radiation at the surface was increased significantly in the order of +10 W m −2 .The strong radiative forcings associated with dust caused a reduction in surface temperature in the order of −0.2 to −0.5 K for most parts of France, Germany, and Italy during the dust event. The maximum difference in surface temperature was found in the East of France, the Benelux, and Western Germany with up to −1 K. This magnitude of temperature change was sufficient to explain a systematic bias in numerical weather forecasts during the period of the dust event.