Abstract. Dust and black carbon aerosol have long been known to exert potentially important and diverse impacts on cloud droplet formation. Most studies to date focus on the soluble fraction of these particles, and overlook interactions of the insoluble fraction with water vapor (even if known to be hydrophilic). To address this gap, we developed a new parameterization that considers cloud droplet formation within an ascending air parcel containing insoluble (but wettable) particles externally mixed with aerosol containing an appreciable soluble fraction. Activation of particles with a soluble fraction is described through well-established Köhler theory, while the activation of hydrophilic insoluble particles is treated by "adsorption-activation" theory. In the latter, water vapor is adsorbed onto insoluble particles, the activity of which is described by a multilayer Frenkel-Halsey-Hill (FHH) adsorption isotherm modified to account for particle curvature. We further develop FHH activation theory to i) find combinations of the adsorption parameters A FHH , B FHH which yield atmospherically-relevant behavior, and, ii) express activation properties (critical supersaturation) that follow a simple power law with respect to dry particle diameter.The new parameterization is tested by comparing the parameterized cloud droplet number concentration against predictions with a detailed numerical cloud model, considering a wide range of particle populations, cloud updraft conditions, water vapor condensation coefficient and FHH adsorption isotherm characteristics. The agreement between parameterization and parcel model is excellent, with an average error Correspondence to: A. Nenes (nenes@eas.gatech.edu) of 10% and R 2 ∼0.98. A preliminary sensitivity study suggests that the sublinear response of droplet number to Köhler particle concentration is not as strong for FHH particles.

Abstract. This study reports laboratory measurements of cloud condensation nuclei (CCN) activity and droplet activation kinetics of aerosols dry generated from clays, calcite, quartz, and desert soil samples from Northern Africa, East Asia/China, and Northern America. Based on the observed dependence of critical supersaturation, s c , with particle dry diameter, D dry , we found that FHH (Frenkel, Halsey and Hill) adsorption activation theory is a far more suitable framework for describing fresh dust CCN activity than Köhler theory. One set of FHH parameters (A FHH ∼ 2.25 ± 0.75, B FHH ∼ 1.20 ± 0.10) can adequately reproduce the measured CCN activity for all species considered, and also explains the large range of hygroscopicities reported in the literature. Based on a threshold droplet growth analysis, mineral dust aerosols were found to display retarded activation kinetics compared to ammonium sulfate. Comprehensive simulations of mineral dust activation and growth in the CCN instrument suggest that this retardation is equivalent to a reduction of the water vapor uptake coefficient (relative to that for calibration ammonium sulfate aerosol) by 30-80%. These results suggest that dust particles do not require deliquescent material to act as CCN in the atmosphere.

[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.

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.

Abstract. This study reports laboratory measurements of particle size distributions, cloud condensation nuclei (CCN) activity, and droplet activation kinetics of wet generated aerosols from clays, calcite, quartz, and desert soil samples from Northern Africa, East Asia/China, and Northern America. The dependence of critical supersaturation, s c , on particle dry diameter, D dry , is used to characterize particle-water interactions and assess the ability of Frenkel-Halsey-Hill adsorption activation theory (FHH-AT) and Köhler theory (KT) to describe the CCN activity of the considered samples. Wet generated regional dust samples produce unimodal size distributions with particle sizes as small as 40 nm, CCN activation consistent with KT, and exhibit hygroscopicity similar to inorganic salts. Wet generated clays and minerals produce a bimodal size distribution; the CCN activity of the smaller mode is consistent with KT, while the larger mode is less hydrophilic, follows activation by FHH-AT, and displays almost identical CCN activity to dry generated dust. Ion Chromatography (IC) analysis performed on regional dust samples indicates a soluble fraction that cannot explain the CCN activity of dry or wet generated dust. A mass balance and hygroscopicity closure suggests that the small amount of ions (from low solubility compounds like calcite) present in the dry dust dissolve in the aqueous suspension during the wet generation process and give rise to the observed small hygroscopic mode. Overall these results identify an artifact that may question the atmospheric relevance of dust CCN activity studies using the wet generation method.Correspondence to: A. Nenes (athanasios.nenes@gatech.edu) Based on the method of threshold droplet growth analysis, wet generated mineral aerosols display similar activation kinetics compared to ammonium sulfate calibration aerosol. Finally, a unified CCN activity framework that accounts for concurrent effects of solute and adsorption is developed to describe the CCN activity of aged or hygroscopic dusts.

A complex conformational energy landscape determines G-protein-coupled receptor (GPCR) signalling via intracellular binding partners (IBPs), e.g., Gs and β-arrestin. Using 13C methyl methionine NMR for the β1-adrenergic receptor, we identify ligand efficacy-dependent equilibria between an inactive and pre-active state and, in complex with Gs-mimetic nanobody, between more and less active ternary complexes. Formation of a basal activity complex through ligand-free nanobody–receptor interaction reveals structural differences on the cytoplasmic receptor side compared to the full agonist-bound nanobody-coupled form, suggesting that ligand-induced variations in G-protein interaction underpin partial agonism. Significant differences in receptor dynamics are observed ranging from rigid nanobody-coupled states to extensive μs-to-ms timescale dynamics when bound to a full agonist. We suggest that the mobility of the full agonist-bound form primes the GPCR to couple to IBPs. On formation of the ternary complex, ligand efficacy determines the quality of the interaction between the rigidified receptor and an IBP and consequently the signalling level.

[1] This study uses published data on dust-water interactions to examine the importance of including water adsorption effects when describing the hygroscopic and cloud condensation nuclei (CCN) behavior of mineral dust aerosol. Adsorption activation theory (AT) better represents fresh dust-water interactions than Köhler theory (KT), as i) a consistent set of adsorption parameters can describe the hygroscopic behavior of dust (under both sub and supersaturated conditions), and ii) the dependence of critical supersaturation, s c , with particle dry diameter, D dry , is closer to observations. The long adsorption timescale could also contribute to the large differences observed between dry and wet generated dust hygroscopicity. If KT and AT are consistently applied to the same dust size distribution, KT predicts up to tenfold higher CCN and 40% higher droplet number concentration than AT. This profoundly different behavior between the theories suggests that both may be required for a comprehensive description of atmospheric dust CCN activity. Citation: Kumar, P., A. Nenes, and I. N. Sokolik (2009), Importance of adsorption for CCN activity and hygroscopic properties of mineral dust aerosol, Geophys. Res. Lett., 36, L24804,

This study reports laboratory measurements of cloud condensation nuclei (CCN) activity and droplet activation kinetics of aerosols dry-generated from clays, calcite, quartz, and desert soil samples from Northern Africa, East Asia/China, and Northern America. Based on the observed dependence of critical supersaturation, <i>s</i>_c, with particle dry diameter, <i>D</i>_dry, we find that FHH adsorption activation theory is a far more suitable framework for describing fresh dust CCN activity than Köhler theory. One set of FHH parameters (<i>A</i>_FFH ~ 2.25 &plusmn; 0.75, <i>B</i>_FFH ~ 1.20 &plusmn; 0.10) can adequately reproduce the measured CCN activity for all species considered, and also explains the large range of hygroscopicities reported in the literature. Based on threshold droplet growth analysis, mineral dust aerosols were found to display retarded activation kinetics compared to ammonium sulfate. Comprehensive simulations of mineral dust activation and growth in the CCN instrument suggest that this retardation is equivalent to a reduction of the water vapor uptake coefficient (relative to that for calibration ammonium sulfate aerosol) by 30–80%. These results suggest that dust particles do not require deliquescent material to act as CCN in the atmosphere