The composition of high‐altitude ice clouds is still a matter of intense discussion. The constituents in question are ice and nitric acid hydrates, but the exact phase composition of clouds and its formation mechanisms are still unknown. In this work, conclusive evidence for a long‐predicted phase, alpha‐nitric acid trihydrate (alpha‐NAT), is presented. This phase was characterized by a combination of X‐ray and neutron diffraction experiments, allowing a convincing structure solution. Furthermore, vibrational spectra (infrared and inelastic neutron scattering) were recorded and compared with theoretical calculations. A strong interaction between water ice and alpha‐NAT was found, which explains the experimental spectra and the phase‐transition kinetics. On the basis of these results, we propose a new three‐step mechanism for NAT formation in high‐altitude ice clouds.
Abstract. Mineral dust particles from deserts are amongst the most common ice nucleating particles in the atmosphere. The mineralogy of desert dust differs depending on the source region and can further fractionate during the dust emission processes. Mineralogy to a large extent explains the ice nucleation behavior of desert aerosol, but not entirely. Apart from pure mineral dust, desert aerosol particles often exhibit a coating or are mixed with small amounts of biological material. Aging on the ground or during atmospheric transport can deactivate nucleation sites, thus strong ice nucleating minerals may not exhibit their full potential. In the partner paper of this work, it was shown that mineralogy determines most but not all of the ice nucleation behavior in the immersion mode found for desert dust. In this study, the influence of semi-volatile organic compounds and the presence of crystal water on the ice nucleation behavior of desert aerosol is investigated. This work focuses on the deposition and condensation ice nucleation modes at temperatures between 238 and 242 K of 18 dust samples sourced from nine deserts worldwide. Chemical imaging of the particles' surface is used to determine the cause of the observed differences in ice nucleation. It is found that, while the ice nucleation ability of the majority of the dust samples is dominated by their quartz and feldspar content, in one carbonaceous sample it is mostly caused by organic matter, potentially cellulose and/or proteins. In contrast, the ice nucleation ability of an airborne Saharan sample is found to be diminished, likely by semi-volatile species covering ice nucleation active sites of the minerals. This study shows that in addition to mineralogy, other factors such as organics and crystal water content can alter the ice nucleation behavior of desert aerosol during atmospheric transport in various ways.
Abstract. Birch pollen are known to release ice-nucleating macromolecules (INM), but little is known about the production and release of INM from other parts of the tree. We examined the ice nucleation activity of samples from 10 different birch trees (Betula spp.). Samples were taken from nine birch trees in Tyrol, Austria, and from one tree in a small urban park in Vienna, Austria. Filtered aqueous extracts of 30 samples of leaves, primary wood (new branch wood, green in colour, photosynthetically active), and secondary wood (older branch wood, brown in colour, with no photosynthetic activity) were analysed in terms of ice nucleation activity using VODCA (Vienna Optical Droplet Crystallization Analyser), a cryo microscope for emulsion samples. All samples contained ice-nucleating particles in the submicron size range. Concentrations of ice nuclei ranged from 6.7×104 to 6.1×109 mg−1 sample. Mean freezing temperatures varied between −15.6 and −31.3 ∘C; the range of temperatures where washes of birch pollen and dilutions thereof typically freeze. The freezing behaviour of three concentrations of birch pollen washing water (initial wash, 1 : 100, and 1 : 10 000) were significantly associated with more than a quarter of our samples, including some of the samples with highest and lowest activity. This indicates a relationship between the INM of wood, leaves, and pollen. Extracts derived from secondary wood showed the highest concentrations of INM and the highest freezing temperatures. Extracts from the leaves exhibited the highest variation in INM and freezing temperatures. Infrared spectra of the extracts and tested birch samples show qualitative similarity, suggesting the chemical components may be broadly similar.
New tools and technology are needed to study microorganisms in freshwater environments. Little is known about spatial distribution and ice nucleation activity (INA) of microorganisms in freshwater lakes. We developed a system to collect water samples from the surface of lakes using a 3D-printed sampling device tethered to a drone (DOWSE, DrOne Water Sampling SystEm). The DOWSE was used to collect surface water samples at different distances from the shore (1, 25, and 50 m) at eight different freshwater lakes in Austria in June 2018. Water samples were filtered, and microorganisms were cultured on two different media types, TSA (a general growth medium) and KBC (a medium semi-selective for bacteria in the genus Pseudomonas). Mean concentrations (colony forming units per mL, or CFU/mL) of bacteria cultured on TSA ranged from 19,800 (Wörthersee) to 210,500 (Gosaulacke) CFU/mL, and mean concentrations of bacteria cultured on KBC ranged from 2590 (Ossiachersee) to 11,000 (Vorderer Gosausee) CFU/mL. There was no significant difference in sampling distance from the shore for concentrations of microbes cultured on TSA (p = 0.28). A wireless bathymetry sensor was tethered to the drone to map temperature and depth across the sampling domain of each of the lakes. At the 50 m distance from the shore, temperature ranged from 17 (Hinterer Gosausee, and Gosaulacke) to 26 • C (Wörthersee), and depth ranged from 2.8 (Gosaulacke) to 11.1 m (Grundlsee). Contour maps of concentrations of culturable bacteria across the drone sampling domain revealed areas of high concentrations (hot spots) in some of the lakes. The percentage of ice-nucleation active (ice+) bacteria cultured on KBC ranged from 0% (0/64) (Wörthersee) to 58% (42/72) (Vorderer Gosausee), with a mean of 28% (153/544) for the entire sample set. Future work aims to elucidate the structure and function of entire microbial assemblages within and among the Austrian lakes.
A force-level theory of the rheology of entangled rod and chain polymer liquids. I. Tube deformation, microscopic yielding, and the nonlinear elastic limit
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