Abstract. We describe a technique to model the radiative properties of mineral aerosols which accounts for their composition. We compile a data set of refractive indices of major minerals and employ it, along with data on mineralogical composition of dust from various locations, to calculate spectral optical and radiative properties of mineral aerosol mixtures. Such radiative properties are needed for climate modeling and remote sensing applications. We consider external mixtures of individual minerals, as well as mixtures of aggregates. We demonstrate that an external mixture of individual minerals must contain unrealistically high amounts of hematite to have a single scattering albedo lower than 0.9 at 500 nm wavelength. In contrast, aggregation of hematite with quartz or clays can strongly enhance absorption by dust at solar wavelengths. We also simulate the daily mean net (solar + infrared) forcing by dust of varying compositions. We found that, for a given composition and under similar atmospheric conditions, a mixture of aggregates can cause the positive radiative forcing while a mixture of individual minerals gives the negative forcing.

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[1] We report on measurements that were specifically designed to determine iron oxides in mineral dust aerosols needed for improved optical modeling. Atmospheric dust samples as well as samples generated in a wind tunnel from soils were analyzed by a number of analytical techniques for their total and free iron content (bulk and size resolved), hematite and goethite, mineralogy, and size distribution. These samples are representative of several important dust sources in East Asia and northern Africa. A novel data set generated from these measurements enables us to perform an in-depth modeling study of dust optical properties in the solar spectrum. We modeled the iron oxide-clay aggregates, which are the key light-absorbing species, as well as their mixtures with nonabsorbing minerals. A volume fraction of iron oxide in aggregates was determined from measurements. Significant differences in the single-scattering albedo, ! 0 , were found between hematite-and goethite-clay aggregates, although these calculations involved several important assumptions about the partition of hematite and goethite in size-resolved aggregates. Furthermore, we found that variability of the free iron content is large enough to cause important differences in ! 0 of mineral dust originating from different sources. In contrast, this variability has little effect on the extinction coefficient and optical depth. We demonstrate that for the same size distribution, ! 0 calculated from data obtained for Chinese and Tunisian samples show higher values and more distinct wavelength dependence than those of Niger dust. All the above ! 0 differ from ones calculated using the refractive indices of Patterson et al. (1977) or the OPAC model (Hess et al., 1998), which are often used in radiative transfer studies. We conclude that information on a size-resolved content of free iron and a fraction of hematite and goethite in aggregates will need to be known on a regional basis to improve the prediction of the single-scattering albedo at solar wavelengths and hence the radiative impact of atmospheric mineral dust.

Abstract. This paper provides an introduction to the special section of the Journal of Geophysical Research on mineral dust. We briefly review the current experimental and theoretical approaches used to quantify the dust radiative impacts, highlight the outstanding issues, and discuss possible strategies to overcome the emerging problems. We also introduce the contributing papers of this special section. Despite the recent notable advances in dust studies, we demonstrate that the radiative effects of dust remain poorly quantified due to both limited data and incomplete understanding of relative physical and chemical processes. The foremost needs are (1) to quantify the spatial and temporal variations of dust burden in the atmosphere and develop a predictive capability for the size-and composition-resolved dust particle distribution; (2) to develop a quantitative description of the processes that control the spatial and temporal variabilities of dust physical and chemical properties and radiative effects; (3) to develop new instrumentation (especially to measure the dust particle size distribution in a wide range from about 0.01 gm to 100 gm, scattering phase function and light absorption by dust particles); and (4) to develop new techniques for interpreting and merging the diverse information from satellite remote sensing, in situ and ground-based measurements, laboratory studies, and model simulations. Because dust distribution and effects are heterogeneous, both spatially and temporally, a promising strategy to advance our knowledge is to perform comprehensive studies at the targeted regions affected by mineral dust of both natural and anthropogenic origin.

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.

[1] Significant problems with modeling dust emission are highlighted. Not only do dust emission schemes rely on various assumptions, but also their implementation within a regional or global model presents challenges. This paper provides an in-depth comparative analysis of two different physically based schemes that were originally developed by Marticorena and Bergametti (1995) and Shao et al. (1996) with some recent improvements. Both schemes were implemented in a dust module (DuMo) and coupled with the Weather Research and Forecasting (WRF) model. Here we examine the physical parameterizations employed by these schemes, identify the key input parameters, and establish linkages between them by developing a new data set for dust sources in Central and East Asia. The relative importance of the input parameters is assessed through partial derivatives. The major issues involved in implementing the physically based schemes within a regional model are also discussed. Consistent implementation of two state-of-the-art dust schemes within the same regional model enables us to bracket inherent uncertainties in simulated dust emission. The results of a case study based on WRF-DuMo simulations are presented to demonstrate associated biases in the magnitude and spatial patterns of emitted dust vertical fluxes. Also, recommendations on the selection of input parameters, including land and meteorological variables, to achieve an improved modeling of dust emission in Central and East Asia are provided.

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.

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