Abstract. Emulsion and bulk freezing experiments were performed to investigate immersion ice nucleation on clay minerals in pure water, using various kaolinites, montmorillonites, illites as well as natural dust from the Hoggar Mountains in the Saharan region. DSC (differential scanning calorimeter) measurements were performed on the kaolinites KGa-1b and KGa-2 from the Clay Mineral Society and kaolinite from Sigma-Aldrich; the montmorillonites SWy-2 and STx-1b from the Clay Mineral Society and the acid treated montmorillonites KSF and K-10 from Sigma Aldrich; the illites NX and SE from Arginotec. The emulsion experiments provide information on the average freezing behaviour characterized by the average nucleation sites. These experiments revealed one to two distinct heterogeneous freezing peaks, which suggest the presence of a low number of qualitatively distinct average nucleation site classes. We refer to the peak at the lowest temperature as "standard peak" and to the one at higher temperatures as "special peak". Conversely, freezing in bulk samples is not initiated by the average nucleation sites, but by a very low number of "best sites". The kaolinites showed quite narrow standard peaks with onset temperatures 239 K < Tonstd < 242 K and best sites with averaged median freezing temperature Tmedbest = 257 K. Only the kaolinite from Sigma Aldrich featured a special peak with freezing onset at 248 K. The illites showed broad standard peaks with freezing onsets at 244 K < Tonstd < 246 K and best sites with averaged median freezing temperature Tmedbest = 262 K. Montmorillonites had standard peaks with onsets 238 K < Tonstd < 240 K and best sites with Tmedbest=257 K. SWy-2, M K10, and KSF featured special peaks with onsets at Tonspcl=247, 240, and 242 K, respectively. M K10 and KSF both from Sigma Aldrich had less intense standard peaks compared to the ones from the Clay Mineral Society suggesting that a fraction of the standard sites are lost by the acid treatment. The acid treatment had however, no evident effect on best sites. Our investigations demonstrate that immersion freezing temperatures of clay minerals strongly depend on the amount of clay mineral present per droplet and on the exact type (location of collection and pre-treatment) of the clay mineral. We suggest that apparently contradictory results obtained by different groups with different setups can indeed be brought into good agreement when only clay minerals of the same type and amount per droplet are compared. The natural sample from the Hoggar Mountains, a region whose dusts have been shown to be composed mainly of illite, showed very similar freezing characteristics to the illites with freezing peak onsets 247 K < Tonstd < 248 K for the average and Tmedbest = 261 K for the best sites. Relating the concentration of best IN to the dust concentration in the atmosphere suggested that the best IN in the Hoggar sample would be common enough downwind of their source region to account for ambient IN number densities in the temperature range of 250–260 K at least during dust events.
Generalisation of Levine's prediction for the distribution of freezing temperatures of droplets: a general singular model for ice nucleation
