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Satellite-based observations during the Arctic winter of 2009/2010 provide firm evidence that, in contrast to the current understanding, the nucleation of nitric acid trihydrate (NAT) in the polar stratosphere does not only occur on preexisting ice particles. In order to explain the NAT clouds observed over the Arctic in mid-December 2009, a heterogeneous nucleation mechanism is required, occurring via immersion freezing on the surface of solid particles, likely of meteoritic origin. For the first time, a detailed microphysical modelling of this NAT formation pathway has been carried out. Heterogeneous NAT formation was calculated along more than sixty thousand trajectories, ending at Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) observation points. Comparing the optical properties of the modelled NAT with these observations enabled a thorough validation of a newly developed NAT nucleation parameterisation, which has been built into the Zurich Optical and Microphysical box Model (ZOMM). The parameterisation is based on active site theory, is simple to implement in models and provides substantial advantages over previous approaches which involved a constant rate of NAT nucleation in a given volume of air. It is shown that the new method is capable of reproducing observed polar stratospheric clouds (PSCs) very well, despite the varied conditions experienced by air parcels travelling along the different trajectories. In a companion paper, ZOMM is applied to a later period of the winter, when ice PSCs are also present, and it is shown that the observed PSCs are also represented extremely well under these conditions. [ABSTRACT FROM AUTHOR]

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. Differential scanning calorimeter measurements were performed on three different kaolinites (KGa-1b, KGa-2 and K-SA), two illites (Illite NX and Illite SE) and four natural and acidreated montmorillonites (SWy-2, STx-1b, KSF and K-10). The emulsion experiments provide information on the average freezing behaviour characterized by the average nucleation sites. These experiments revealed one to sometimes 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 occurring in only some clay mineral types 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 and montmorillonites showed quite narrow standard peaks with onset temperatures 238K< TDue to image rights restrictions, multiple line equation(s) cannot be graphically displayed. < 242K and best sites with averaged median freezing temperature TDue to image rights restrictions, multiple line equation(s) cannot be graphically displayed. = 257K, but only some featuring a special peak (i.e. KSF, K-10, K- SA and SWy-2) with freezing onsets in the range 240-248K. The illites showed broad standard peaks with freezing onsets at 244K< TDue to image rights restrictions, multiple line equation(s) cannot be graphically displayed. < 246K and best sites with averaged median freezing temperature TDue to image rights restrictions, multiple line equation(s) cannot be graphically displayed. = 262K. The large difference between freezing temperatures of standard and best sites shows that characterizing ice nucleation efficiencies of dust particles on the basis of freezing onset temperatures from bulk experiments, as has been done in some atmospheric studies, is not appropriate. 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 are indeed in 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 (standard and best) to the illites. 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 250-260K at least during dust events. [ABSTRACT FROM AUTHOR]

The ice nucleation ability of volcanic ash particles collected close to the Icelandic volcano Eyjafjallajökull during its eruptions in April and May 2010 is investigated experimentally, in the immersion and deposition modes, and applied to atmospheric conditions by comparison with airborne measurements and microphysical model calculations. The number of ash particles which are active as ice nuclei (IN) is strongly temperature dependent, with a very small minority being active in the immersion mode at temperatures of 250-263 K. Average ash particles show only a moderate effect on ice nucleation, by inducing freezing at temperatures between 236 K and 240 K (i.e. approximately 3-4 K higher than temperatures required for homogeneous ice nucleation, measured with the same instrument). By scaling the results to aircraft and lidar measurements of the conditions in the ash plume days down wind of the eruption, and by applying a simple microphysical model, it was found that the IN active in the immersion mode in the range 250-263 K generally occurred in atmospheric number densities at the lower end of those required to have an impact on ice cloud formation. However, 3-4 K above the homogeneous freezing point, immersion mode IN number densities a few days down wind of the eruption were sufficiently high to have a moderate influence on ice cloud formation. The efficiency of IN in the deposition mode was found to be poor except at very cold conditions (<238K), when they reach an efficiency similar to that of mineral dust with the onset of freezing at 10% supersaturation with respect to ice, and with the frozen fraction nearing its maximum value at a supersaturation 20%. In summary, these investigations suggest volcanic ash particles to have only moderate effects on atmospheric ice formation. [ABSTRACT FROM AUTHOR]

New particle formation (NPF) is the source of over half of the atmosphere's cloud condensation nuclei, thus influencing cloud properties and Earth's energy balance. Unlike in the planetary boundary layer, few observations of NPF in the free troposphere exist. We provide observational evidence that at high altitudes, NPF occurs mainly through condensation of highly oxygenated molecules (HOMs), in addition to taking place through sulfuric acid-ammonia nucleation. Neutral nucleation is more than 10 times faster than ion-induced nucleation, and growth rates are size-dependent. NPF is restricted to a time window of 1 to 2 days after contact of the air masses with the planetary boundary layer; this is related to the time needed for oxidation of organic compounds to form HOMs. These findings require improved NPF parameterization in atmospheric models. [ABSTRACT FROM AUTHOR]