Aerosol climate effects are intimately tied to interactions with water. Here we combine hygroscopicity measurements with direct observations about the phase of secondary organic aerosol (SOA) particles to show that water uptake by slightly oxygenated SOA is an adsorption‐dominated process under subsaturated conditions, where low solubility inhibits water uptake until the humidity is high enough for dissolution to occur. This reconciles reported discrepancies in previous hygroscopicity closure studies. We demonstrate that the difference in SOA hygroscopic behavior in subsaturated and supersaturated conditions can lead to an effect up to about 30% in the direct aerosol forcing—highlighting the need to implement correct descriptions of these processes in atmospheric models. Obtaining closure across the water saturation point is therefore a critical issue for accurate climate modeling.

Abstract. Gaseous sulphuric acid is a key precursor for new particle formation in the atmosphere. Previous experimental studies have confirmed a strong correlation between the number concentrations of freshly formed particles and the ambient concentrations of sulphuric acid. This study evaluates a body of experimental gas phase sulphuric acid concentrations, as measured by Chemical Ionization Mass Spectrometry (CIMS) during six intensive measurement campaigns and one long-term observational period. The campaign datasets were measured in Hyytiälä,

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.

Abstract. We analyse the development of a radiation fog event and its gradual transition from optically thin fog in a stable boundary layer to well-mixed optically thick fog. A comparison of observations and a detailed large-eddy simulation demonstrate that aerosol growth and activation is the key process in determining the onset of adiabatic fog. Weak turbulence and low supersaturations lead to the growth of aerosol particles which can significantly affect the visibility but do not significantly interact with the long-wave radiation, allowing the atmosphere to remain stable. Only when a substantial fraction of the aerosol activates into cloud droplets can the fog interact with the radiation, becoming optically thick and well mixed. Modifications to the parameterisation of cloud droplet numbers in fog, resulting in lower and more realistic concentrations, are shown to give significant improvements to an NWP model, which initially struggled to accurately simulate the transition. Finally, the consequences of this work for common aerosol activation parameterisations used in climate models are discussed, demonstrating that many schemes are reliant on an artificial minimum value when activating aerosol in fog, and adjustment of this minimum can significantly affect the sensitivity of the climate system to aerosol radiative forcing.

Abstract. Modification of cloud albedo by controlled emission of sea spray particles into the atmosphere has been suggested as a possible geoengineering option to slow global warming. Previous global studies have imposed changes in cloud drop concentration in low level clouds to explore the radiative and climatic effects. Here, we use a global aerosol transport model to quantify how an imposed flux of sea spray particles affects the natural aerosol processes, the particle size distribution, and concentrations of cloud drops. We assume that the proposed fleet of vessels emits sea spray particles with a wind speed-dependent flux into four regions of persistent stratocumulus cloud off the western coasts of continents. The model results show that fractional changes in cloud drop number concentration (CDNC) vary substantially between the four regions because of differences in wind speed (which affects the spray efficiency of the vessels), transport and particle deposition rates, and because of variations in aerosols from natural and anthropogenic sources. Using spray emission rates comparable to those implied by previous studies we find that the predicted CDNC changes are very small (maximum 20%) and in one of the four regions even negative. The weak or negative effect is because the added particles suppress the in-cloud supersaturation and prevent existing aerosol particles from forming cloud drops. A scenario with five times higher emissions (considerably higher than previously assumed) increases CDNC on average by 45-163%, but median concentrations are still below the 375 cm −3 assumed in previous studies. An inadvertent effect of the spray emissions is that sulphur dioxide concenCorrespondence to: H. Korhonen (hannele.korhonen@fmi.fi) trations are suppressed by 1-2% in the seeded regions and sulphuric acid vapour by 64-68% due to chemical reactions on the additional salt particles. The impact of this suppression on existing aerosol is negligible in the model, but should be investigated further in the real environment so that inadvertent impacts can be excluded.

[1] Climate-aerosol model ECHAM5.5-HAM2 was used to investigate how geoengineering with artificial sea salt emissions would affect marine clouds and the Earth's radiative balance. Prognostic cloud droplet number concentration and interaction of aerosol particles with clouds and radiation were calculated explicitly, thus making this the first time that aerosol direct effects of sea spray geoengineering are considered. When a wind speed dependent baseline geoengineering flux was applied over all oceans (total annual emissions 443.9 Tg), we predicted a radiative flux perturbation (RFP) of À5.1 W m À2 , which is enough to counteract warming from doubled CO 2 concentration. When the baseline flux was limited to three persistent stratocumulus regions (3.3% of Earth's surface, total annual emissions 20.6 Tg), the RFP was À0.8 Wm À2 resulting mainly from a 74-80% increase in cloud droplet number concentration and a 2.5-4.4 percentage point increase in cloud cover. Multiplying the baseline mass flux by 5 or reducing the injected particle size from 250 to 100 nm had comparable effects on the geoengineering efficiency with RFPs À2.2 and À2.1 Wm À2 , respectively. Within regions characterized with persistent stratocumulus decks, practically all of the radiative effect originated from aerosol indirect effects. However, when all oceanic regions were seeded, the direct effect with the baseline flux was globally about 29% of the total radiative effect. Together with previous studies, our results indicate that there are still large uncertainties associated with the sea spray geoengineering efficiency due to variations in e.g., background aerosol concentration, updraft velocity, cloud altitude and onset of precipitation.Citation: Partanen, A.-I., H. Kokkola, S. Romakkaniemi, V.-M. Kerminen, K. E. J. Lehtinen, T. Bergman, A. Arola, and H. Korhonen (2012), Direct and indirect effects of sea spray geoengineering and the role of injected particle size, J. Geophys.

Abstract. In this paper, we present the implementation and evaluation of the aerosol microphysics module SALSA2.0 in the framework of the aerosol–chemistry–climate model ECHAM-HAMMOZ. It is an alternative microphysics module to the default modal microphysics scheme M7 in ECHAM-HAMMOZ. The SALSA2.0 implementation within ECHAM-HAMMOZ is evaluated against observations of aerosol optical properties, aerosol mass, and size distributions, comparing also to the skill of the M7 implementation. The largest differences between the implementation of SALSA2.0 and M7 are in the methods used for calculating microphysical processes, i.e., nucleation, condensation, coagulation, and hydration. These differences in the microphysics are reflected in the results so that the largest differences between SALSA2.0 and M7 are evident over regions where the aerosol size distribution is heavily modified by the microphysical processing of aerosol particles. Such regions are, for example, highly polluted regions and regions strongly affected by biomass burning. In addition, in a simulation of the 1991 Mt. Pinatubo eruption in which a stratospheric sulfate plume was formed, the global burden and the effective radii of the stratospheric aerosol are very different in SALSA2.0 and M7. While SALSA2.0 was able to reproduce the observed time evolution of the global burden of sulfate and the effective radii of stratospheric aerosol, M7 strongly overestimates the removal of coarse stratospheric particles and thus underestimates the effective radius of stratospheric aerosol. As the mode widths of M7 have been optimized for the troposphere and were not designed to represent stratospheric aerosol, the ability of M7 to simulate the volcano plume was improved by modifying the mode widths, decreasing the standard deviations of the accumulation and coarse modes from 1.59 and 2.0, respectively, to 1.2 similar to what was observed after the Mt. Pinatubo eruption. Overall, SALSA2.0 shows promise in improving the aerosol description of ECHAM-HAMMOZ and can be further improved by implementing methods for aerosol processes that are more suitable for the sectional method, e.g., size-dependent emissions for aerosol species and size-resolved wet deposition.

Abstract. Challenges in understanding the aerosol-cloud interactions and their impacts on global climate highlight the need for improved knowledge of the underlying physical processes and feedbacks as well as their interactions with cloud and boundary layer dynamics. To pursue this goal, increasingly sophisticated cloud-scale models are needed to complement the limited supply of observations of the interactions between aerosols and clouds. For this purpose, a new large-eddy simulation (LES) model, coupled with an interactive sectional description for aerosols and clouds, is introduced. The new model builds and extends upon the well-characterized UCLA Large-Eddy Simulation Code (UCLALES) and the Sectional Aerosol module for Large-Scale Applications (SALSA), hereafter denoted as UCLALES-SALSA. Novel strategies for the aerosol, cloud and precipitation bin discretisation are presented. These enable tracking the effects of cloud processing and wet scavenging on the aerosol size distribution as accurately as possible, while keeping the computational cost of the model as low as possible. The model is tested with two different simulation set-ups: a marine stratocumulus case in the DYCOMS-II campaign and another case focusing on the formation and evolution of a nocturnal radiation fog. It is shown that, in both cases, the size-resolved interactions between aerosols and clouds have a critical influence on the dynamics of the boundary layer. The results demonstrate the importance of accurately representing the wet scavenging of aerosol in the model. Specifically, in a case with marine stratocumulus, precipitation and the subsequent removal of cloud activating particles lead to thinning of the cloud deck and the formation of a decoupled boundary layer structure. In radiation fog, the growth and sedimentation of droplets strongly affect their radiative properties, which in turn drive new droplet formation. The size-resolved diagnostics provided by the model enable investigations of these issues with high detail. It is also shown that the results remain consistent with UCLALES (without SALSA) in cases where the dominating physical processes remain well represented by both models.