Abstract. Despite growing evidence that the ocean is an important source of ice-nucleating particles (INPs) in the atmosphere, our understanding of the properties and concentrations of INPs in ocean surface waters remains limited. We have investigated INPs in sea surface microlayer and bulk seawater samples collected in the Canadian Arctic during the summer of 2016. Consistent with our 2014 studies, we observed that INPs were ubiquitous in the microlayer and bulk seawaters; heat and filtration treatments reduced INP activity, indicating that the INPs were likely heat-labile biological materials between 0.22 and 0.02 µm in diameter; there was a strong negative correlation between salinity and freezing temperatures; and concentrations of INPs could not be explained by chlorophyll a concentrations. Unique in the current study, the spatial distributions of INPs were similar in 2014 and 2016, and the concentrations of INPs were strongly correlated with meteoric water (terrestrial runoff plus precipitation). These combined results suggest that meteoric water may be a major source of INPs in the sea surface microlayer and bulk seawater in this region, or meteoric water may be enhancing INPs in this region by providing additional nutrients for the production of marine microorganisms. In addition, based on the measured concentrations of INPs in the microlayer and bulk seawater, we estimate that the concentrations of INPs from the ocean in the Canadian Arctic marine boundary layer range from approximately 10−4 to <10-6 L−1 at −10 ∘C.
Mineral dust particles are one of the most abundant types of ice nucleating particles in the atmosphere. During atmospheric transport, these particles can be coated with water-soluble solutes, which can modify their ice nucleating ability. Although previous studies have shown that even low concentrations of water-soluble solutes can modify the ice nucleating properties of mineral dust particles, our understanding of this topic is far from complete. We examined the effects of a series of alkali metal nitrates at low concentrations (5 × 10 −5 M to 5 × 10 −3 M) on the surface composition and immersion freezing of potassium-rich feldspar (K-rich feldspar). Immersion freezing was investigated with the droplet freezing technique, and the surface composition was investigated with cryogenic X-ray photoelectron spectroscopy. K + increased the median freezing temperature of the droplets, while the other alkali metal cations either had no effect or decreased the median freezing temperature. The changes in the median freezing temperature of the droplets due to the presence of nitrates followed the order K + ≥ Li + ≥ Na + ≥ Rb + ≥ Cs + and, except for Cs + , were correlated to the K/Al ratio at the surface of K-rich feldspar. The K/Al ratio is possibly an indicator of the abundance of certain types of K-bearing microcline surfaces that drive the immersion freezing of K-rich feldspar, while Cs + likely influences the immersion freezing of K-rich feldspar by an additional mechanism, possibly blocking ice nucleation sites by adsorption. Our work also shows that the cation charge density (charge density over the surface area of a single cation) is not a good predictor of the effects of cations on the immersion freezing of K-rich feldspar in our experiments.
Abstract. Modelling studies suggest that the climate and the hydrological cycle are sensitive to the concentrations of ice-nucleating particles (INPs). However, the concentrations, composition, and sources of INPs in the atmosphere remain uncertain. Here, we report daily concentrations of INPs in the immersion freezing mode and tracers of mineral dust (Al, Fe, Ti, and Mn), sea spray aerosol (Na+ and Cl−), and anthropogenic aerosol (Zn, Pb, NO3-, NH4+, and non-sea-salt SO42-) at Alert, Canada, during a 3-week campaign in March 2016. In total, 16 daily measurements of INPs are reported. The average INP concentrations measured in the immersion freezing mode were 0.005±0.002, 0.020±0.004, and 0.186±0.040 L−1 at −15, −20, and −25 ∘C, respectively. These concentrations are within the range of concentrations measured previously in the Arctic at ground level or sea level. Mineral dust tracers all correlated with INPs at −25 ∘C (correlation coefficient, R, ranged from 0.70 to 0.76), suggesting that mineral dust was a major contributor to the INP population at −25 ∘C. Particle dispersion modelling suggests that the source of the mineral dust may have been long-range transport from the Gobi Desert. Sea spray tracers were anti-correlated with INPs at −25 ∘C (R=-0.56). In addition, INP concentrations at −25 ∘C divided by mass concentrations of aluminum were anti-correlated with sea spray tracers (R=-0.51 and −0.55 for Na+ and Cl−, respectively), suggesting that the components of sea spray aerosol suppressed the ice-nucleating ability of mineral dust in the immersion freezing mode. Correlations between INPs and anthropogenic aerosol tracers were not statistically significant. These results will improve our understanding of INPs in the Arctic during spring.
<p>EGU Abstract</p><p>&#160;</p><p>A wide range of materials including mineral dust, soil dust, and bioaerosols have been shown to act as ice nuclei in the atmosphere. During atmospheric transport, these materials can become coated with inorganic and organic solutes which may impact their ability to nucleate ice. While a number of studies have investigated the impact of solutes at low concentrations on ice nucleation by mineral dusts, very few studies have examined their impact on non-mineral dust ice nuclei.</p><p>We studied the effect of dilute (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> solutions (0.05 M) on immersion freezing of a variety of non-mineral dust ice nucleating substances including bacteria, fungi, sea ice diatom exudates, sea surface microlayer, and humic substances using the droplet freezing technique. We also studied the effect of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> on immersion freezing of mineral dust particles for comparison purposes. (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> had no effect on the median freezing temperature of 9 of the 10 tested non-mineral dust materials. There was a small but statistically significant decrease in the median freezing temperature of the bacteria <em>X. campestris</em> (change in median freezing temperature &#160;= -0.43 &#177; 0.19 &#176;C) in the presence of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4 </sub>compared to pure water. Conversely, (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> increased the median freezing temperature of four different mineral dusts (potassium-rich feldspar, Arizona test dust, kaolinite, montmorillonite) by 3 &#176;C to 9 &#176;C and increased the ice nucleation active site density per gram of material&#160;by a factor of ~10 to ~30.</p><p>This significant difference in the response of mineral dust and non-mineral dust ice nucleating substances when exposed to (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> suggests that they nucleate ice and/or interact with (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> via different mechanisms. This difference suggests that the relative importance of mineral dust to non-mineral dust particles for ice nucleation in mixed-phase clouds could increase as these particles become coated with (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> in the atmosphere. This difference also suggests that the addition of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> to atmospheric samples of unknown composition could be used as an indicator or assay for the presence of mineral dust ice nuclei.</p>
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