Abstract

Abstract. Desert dust is one of the most abundant ice nucleating particle types in the atmosphere. Traditionally, clay minerals were assumed to determine the ice nucleation ability of desert dust and constituted the focus of ice nucleation studies over several decades. Recently some feldspar species were identified to be ice active at much higher temperatures than clay minerals, redirecting studies to investigate the contribution of feldspar to ice nucleation on desert dust. However, so far no study has shown the atmospheric relevance of this mineral phase.For this study four dust samples were collected after airborne transport in the troposphere from the Sahara to different locations (Crete, the Peloponnese, Canary Islands, and the Sinai Peninsula). Additionally, 11 dust samples were collected from the surface from nine of the biggest deserts worldwide. The samples were used to study the ice nucleation behavior specific to different desert dusts. Furthermore, we investigated how representative surface-collected dust is for the atmosphere by comparing to the ice nucleation activity of the airborne samples. We used the IMCA-ZINC setup to form droplets on single aerosol particles which were subsequently exposed to temperatures between 233 and 250 K. Dust particles were collected in parallel on filters for offline cold-stage ice nucleation experiments at 253–263 K. To help the interpretation of the ice nucleation experiments the mineralogical composition of the dusts was investigated. We find that a higher ice nucleation activity in a given sample at 253 K can be attributed to the K-feldspar content present in this sample, whereas at temperatures between 238 and 245 K it is attributed to the sum of feldspar and quartz content present. A high clay content, in contrast, is associated with lower ice nucleation activity. This confirms the importance of feldspar above 250 K and the role of quartz and feldspars determining the ice nucleation activities at lower temperatures as found by earlier studies for monomineral dusts. The airborne samples show on average a lower ice nucleation activity than the surface-collected ones. Furthermore, we find that under certain conditions milling can lead to a decrease in the ice nucleation ability of polymineral samples due to the different hardness and cleavage of individual mineral phases causing an increase of minerals with low ice nucleation ability in the atmospherically relevant size fraction. Comparison of our data set to an existing desert dust parameterization confirms its applicability for climate models. Our results suggest that for an improved prediction of the ice nucleation ability of desert dust in the atmosphere, the modeling of emission and atmospheric transport of the feldspar and quartz mineral phases would be key, while other minerals are only of minor importance.

Highlights

  • Predicting the occurrence and evolution of clouds at temperatures (T ) below 273 K remains a challenge for global and regional climate models (Boucher et al, 2013)

  • Four pathways of ice nucleation are differentiated (Vali et al, 2015): 1. deposition nucleation, where ice forms on an ice nucleating particles (INPs) directly from the vapor phase; 2. condensation freezing, in which ice forms during the process of water condensing on an INP; 3. immersion freezing, where an INP immersed in a supercooled cloud droplet initiates freezing; 4. contact freezing, where the interaction of an INP with the surface of a supercooled droplet either from the outside or inside of the droplet leads to freezing

  • The ice nucleation ability in the immersion mode of 15 natural desert dust samples was quantified by the frozen fraction and ice-active surface site density and compared with the bulk dust mineralogy

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Summary

Introduction

Predicting the occurrence and evolution of clouds at temperatures (T ) below 273 K remains a challenge for global and regional climate models (Boucher et al, 2013). Mineral dust particles have been known as efficient INPs at T ≤ 253 K for more than 60 years (e.g., Isono, 1955, and references given in Hoose and Möhler, 2012; Murray et al, 2012) and have been observed to nucleate ice in the atmosphere in various regions worldwide (Kumai, 1976; DeMott et al, 2003; Chou et al, 2011; Boose et al, 2016a, b). Supercooled cloud droplets can freeze homogeneously at temperatures below 235 K, without the aid of an INP (Schaefer, 1946; Mason and Ludlam, 1950). Condensation freezing, in which ice forms during the process of water condensing on an INP; 3. Immersion freezing, where an INP immersed in a supercooled cloud droplet initiates freezing; 4. Four pathways of ice nucleation are differentiated (Vali et al, 2015): 1. deposition nucleation, where ice forms on an INP directly from the vapor phase; 2. condensation freezing, in which ice forms during the process of water condensing on an INP; 3. immersion freezing, where an INP immersed in a supercooled cloud droplet initiates freezing; 4. contact freezing, where the interaction of an INP with the surface of a supercooled droplet either from the outside or inside of the droplet leads to freezing

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