Ice multiplication processes are known to be responsible for the higher concentration of ice particles versus ice nucleating particles in clouds, but the exact secondary ice formation mechanisms remain to be quantified. Recent in-cloud observations and modeling studies have suggested the importance of secondary ice production upon shattering of freezing drizzle droplets. In one of our previous studies, four categories of secondary ice formation during freezing of supercooled droplets have been identified: breakup, cracking, jetting, and bubble bursts. In this work, we extend the study to include pure water and an aqueous solution of analog sea salt drizzle droplets moving at terminal velocity with respect to the surrounding cold humid air. We observe an enhancement in the droplet shattering probability as compared to the stagnant air conditions used in the previous study. Under free-fall conditions, bubble bursts are the most common secondary ice production mode in sea salt drizzle droplets, while droplet fragmentation controls the secondary ice production in pure water droplets.

The freezing process of a supercooled water droplet freely falling through air is a remarkably dynamic and eventful process. During freezing from the outside in, the volume increase of liquid water upon solidification leads to a pressure rise inside the droplet. The pressure is released in various ways, e.g. by cracking or by complete fragmentation of the ice shell. These processes may be the source of secondary ice particles that are emitted during droplet freezing. In this study, the surface temperature of freezing drizzle-sized water droplets was measured with a high-resolution infrared thermography system, while recording the changes in shape and structure of the droplet by a high-speed video camera. The droplets were levitated in an electrodynamic trap under controlled conditions with respect to temperature, humidity and airflow velocity. Measurement of the surface temperature during freezing allowed for determination of the absolute pressure inside the liquid core. During the freezing of a droplet the pressure rise is interrupted many times by rapid pressure release events, each being a possible source of secondary ice. Pressure release events were three times more frequent for droplets freezing under free-fall conditions compared to droplets freezing in stagnant air. Naturally occurring sea salt content (< 100 mg/L) does not inhibit the pressure buildup inside freezing drizzle droplets.

Abstract. Feldspar is an important constituent of airborne mineral dust. Some alkali feldspars exhibit particularly high ice nucleation (IN) activity. This has been related to structural similarities of the ice (101‾0) prism planes and the (100) planes of alkali feldspar. Here the effect of generating feldspar surfaces with close to (100) orientation by means of chemically induced fracturing on the IN activity of alkali feldspar was investigated experimentally. To this end, gem-quality K-rich alkali feldspar was shifted towards more Na-rich compositions by cation exchange with an NaCl–KCl salt melt at 850 ∘C. By this procedure, a system of parallel cracks with an orientation close to the (100) plane of the feldspar was induced. Droplet-freezing assay experiments performed on grain mounts of the cation-exchanged alkali feldspars revealed an increase in the overall density of ice-nucleating active site (INAS) density with respect to the untreated feldspar. In addition, annealing at 550 ∘C subsequent to primary cation exchange further enhanced the INAS density and led to IN activity at exceptionally high temperatures. Although very efficient in experiment, fracturing by cation exchange with an alkali halide salt is unlikely to be of relevance in the conditioning of alkali feldspars in nature. However, parting planes with similar orientation as the chemically induced cracks may be generated in lamellar microstructures resulting from the exsolution of initially homogeneous alkali feldspar, a widespread phenomenon in natural alkali feldspar known as perthite formation. Perthitic alkali feldspars indeed show the highest IN activity. We tentatively ascribe this phenomenon to the preferential exposure of feldspar crystal surfaces oriented sub-parallel to (100).

Abstract. Feldspar is an important constituent of airborne mineral dust. Some alkali feldspars exhibit particularly high ice nucleation (IN) activity. This has been related to structural similarities of the ice (10-10) prism planes and the (100) planes of alkali feldspar. Here the effect of generating surfaces with close to (100) orientation by means of chemically induced fracturing on the IN activity of alkali feldspar was investigated experimentally. Gem quality K-rich alkali feldspar was shifted towards more Na-rich compositions by cation exchange with an NaCl-KCl salt melt at 850 °C, and a system of parallel cracks with an orientation close to (100) was induced. Droplet freezing assay experiments performed on grain mounts of the cation exchanged alkali feldspars revealed an increase of the overall density of ice nucleating active sites (INAS) with respect to the untreated feldspar. In addition, annealing at 550 °C subsequent to primary cation exchange further enhanced the INAS density and lead to IN activity at exceptionally high temperatures. Although very efficient in experiment, fracturing by cation exchange is unlikely to be of relevance in the conditioning of alkali feldspars in nature. However, parting planes with similar orientation as the chemically induced cracks may be generated in lamellar microstructures resulting from the exsolution of initially homogeneous alkali feldspar, a widespread phenomenon in natural alkali feldspar known as perthite formation. Perthitic alkali feldspars indeed show the highest IN activity. We ascribe this phenomenon to the preferential exposure of crystal surfaces oriented sub-parallel to (100).

Crystallization of supercooled liquid water in most natural environments starts with heterogeneous nucleation of ice induced by a nucleation site. Mineral surfaces, which form the majority of aqueous interfaces in...