Ice nucleation efficiency of natural dust samples in the immersion mode

Abstract

A total of 12 natural surface dust samples, which were surface-collected on four continents, most of them in dust source regions, were investigated with respect to their ice nucleation activity. Dust collection sites were distributed across Africa, South America, the Middle East, and Antarctica. Mineralogical composition has been determined by means of X-ray diffraction. All samples proved to be mixtures of minerals, with major contributions from quartz, calcite, clay minerals, K-feldspars, and (Na, Ca)-feldspars. Reference samples of these minerals were investigated with the same methods as the natural dust samples. Furthermore, Arizona test dust (ATD) was re-evaluated as a benchmark. Immersion freezing of emulsion and bulk samples was investigated by differential scanning calorimetry. For emulsion measurements, water droplets with a size distribution peaking at about 2 μm, containing different amounts of dust between 0.5 and 50 wt% were cooled until all droplets were frozen. These measurements characterize the average freezing behaviour of particles, as they are sensitive to the average active sites present in a dust sample. In addition, bulk measurements were conducted with one single 2 mg droplet consisting of a 5 wt% aqueous suspension of the dusts/minerals. These measurements allow the investigation of the best icenucleating particles/sites available in a dust sample. All natural dusts, except for the Antarctica and ATD samples, froze in a remarkably narrow temperature range with the heterogeneously frozen fraction reaching 10% between 244 and 250 K, 25% between 242 and 246 K, and 50% between 239 and 244 K. Bulk freezing occurred between 255 and 265 K. In contrast to the natural dusts, the reference minerals revealed ice nucleation temperatures with 2-3 times larger scatter. Calcite, dolomite, dolostone, and muscovite can be considered ice nucleation inactive. For microcline samples, a 50% heterogeneously frozen fraction occurred above 245K for all tested suspension concentrations, and a microcline mineral showed bulk freezing temperatures even above 270 K. This makes microcline (KAlSi3O8/ an exceptionally good ice-nucleating mineral, superior to all other analysed K-feldspars, (Na, Ca)-feldspars, and the clay minerals. In summary, the mineralogical composition can explain the observed freezing behaviour of 5 of the investigated 12 natural dust samples, and partly for 6 samples, leaving the freezing efficiency of only 1 sample not easily explained in terms of its mineral reference components. While this suggests that mineralogical composition is a major determinant of ice-nucleating ability, in practice, most natural samples consist of a mixture of minerals, and this mixture seems to lead to remarkably similar ice nucleation abilities, regardless of their exact composition, so that global models, in a first approximation, may represent mineral dust as a single species with respect to ice nucleation activity. However, more sophisticated representations of ice nucleation by mineral dusts should rely on the mineralogical composition based on a source scheme of dust emissions.