Ice Active Site Density Research Articles

Ice nucleation ability of loess from the northwestern United States.

The heterogeneous nucleation of ice processes involving loess particles that influences the formation of mixed-phase clouds are poorly understood. Here, the ice nucleating ability of wind-blown dust or loess accumulated from the past glaciated area was investigated at three temperatures: -26, -30, and -34 °C and at below and above saturation with respect to liquid water conditions. Total six loess samples from different regions across Columbia Basin province, WA, USA were collected, dry dispersed, size-selected at mobility diameter 200 nm, and investigated for their ice nucleation efficiency. To understand the effect of atmospheric processing during long-range transport on their ice nucleating ability, similar experiments were also performed on acid-treated loess samples. Additionally, the ice nucleating properties of Arizona Test Dust (ATD) were investigated as a surrogate for natural mineral dust particles to test the experimental approach. Results show that treated particles have lower ice nucleation efficiency compared to untreated particles at all temperature and saturation with respect to liquid water conditions. Comparison based on ice-active site density (Ns) metric indicate that loess particles at saturation with respect to liquid water conditions are marginally more efficient than the mineral and soil dust values reported in the literature, but they have lower efficiencies than the predicted Ns efficiency of K-feldspar particles at supercooled temperatures greater than -38 °C.

Atmospheric Ice‐Nucleating Particles in the Dusty Tropical Atlantic

AbstractDesert dust is one of the most important atmospheric ice‐nucleating aerosol species around the globe. However, there have been very few measurements of ice‐nucleating particle (INP) concentrations in dusty air close to desert sources. In this study we report the concentration of INPs in dust laden air over the tropical Atlantic within a few days' transport of one of the world's most important atmospheric sources of desert dust, the Sahara. These measurements were performed as part of the Ice in Clouds Experiment‐Dust campaign based in Cape Verde, during August 2015. INP concentrations active in the immersion mode, determined using a droplet‐on‐filter technique, ranged from around 102 m−3 at −12°C to around 105 m−3 at −23°C. There is about 2 orders of magnitude variability in INP concentration for a particular temperature, which is determined largely by the variability in atmospheric dust loading. These measurements were made at altitudes from 30 to 3,500 m in air containing a range of dust loadings. The ice active site density (ns) for desert dust dominated aerosol derived from our measurements agrees with several laboratory‐based parameterizations for ice nucleation by desert dust within 1 to 2 orders of magnitude. The small variability in ns values determined from our measurements (within about 1 order of magnitude) is striking given that the back trajectory analysis suggests that the sources of dust were geographically diverse. This is consistent with previous work, which indicates that desert dust's ice‐nucleating activity is only weakly dependent on source.

Effect of particle surface area on ice active site densities retrieved from droplet freezing spectra

Abstract. Heterogeneous ice nucleation remains one of the outstanding problems in cloud physics and atmospheric science. Experimental challenges in properly simulating particle-induced freezing processes under atmospherically relevant conditions have largely contributed to the absence of a well-established parameterization of immersion freezing properties. Here, we formulate an ice active, surface-site-based stochastic model of heterogeneous freezing with the unique feature of invoking a continuum assumption on the ice nucleating activity (contact angle) of an aerosol particle's surface that requires no assumptions about the size or number of active sites. The result is a particle-specific property g that defines a distribution of local ice nucleation rates. Upon integration, this yields a full freezing probability function for an ice nucleating particle. Current cold plate droplet freezing measurements provide a valuable and inexpensive resource for studying the freezing properties of many atmospheric aerosol systems. We apply our g framework to explain the observed dependence of the freezing temperature of droplets in a cold plate on the concentration of the particle species investigated. Normalizing to the total particle mass or surface area present to derive the commonly used ice nuclei active surface (INAS) density (ns) often cannot account for the effects of particle concentration, yet concentration is typically varied to span a wider measurable freezing temperature range. A method based on determining what is denoted an ice nucleating species' specific critical surface area is presented and explains the concentration dependence as a result of increasing the variability in ice nucleating active sites between droplets. By applying this method to experimental droplet freezing data from four different systems, we demonstrate its ability to interpret immersion freezing temperature spectra of droplets containing variable particle concentrations. It is shown that general active site density functions, such as the popular ns parameterization, cannot be reliably extrapolated below this critical surface area threshold to describe freezing curves for lower particle surface area concentrations. Freezing curves obtained below this threshold translate to higher ns values, while the ns values are essentially the same from curves obtained above the critical area threshold; ns should remain the same for a system as concentration is varied. However, we can successfully predict the lower concentration freezing curves, which are more atmospherically relevant, through a process of random sampling from g distributions obtained from high particle concentration data. Our analysis is applied to cold plate freezing measurements of droplets containing variable concentrations of particles from NX illite minerals, MCC cellulose, and commercial Snomax bacterial particles. Parameterizations that can predict the temporal evolution of the frozen fraction of cloud droplets in larger atmospheric models are also derived from this new framework.

Ice nucleation by fertile soil dusts: relative importance of mineral and biogenic components

Abstract. Agricultural dust emissions have been estimated to contribute around 20% to the global dust burden. In contrast to dusts from arid source regions, the ice-nucleating abilities of which have been relatively well studied, soil dusts from fertile sources often contain a substantial fraction of organic matter. Using an experimental methodology which is sensitive to a wide range of ice nucleation efficiencies, we have characterised the immersion mode ice-nucleating activities of dusts (d < 11 μm) extracted from fertile soils collected at four locations around England. By controlling droplet sizes, which ranged in volume from 10−12 to 10−6 L (concentration = 0.02 to 0.1 wt% dust), we have been able to determine the ice nucleation behaviour of soil dust particles at temperatures ranging from 267 K (−6 °C) down to the homogeneous limit of freezing at about 237 K (−36 °C). At temperatures above 258 K (−15 °C) we find that the ice-nucleating activity of soil dusts is diminished by heat treatment or digestion with hydrogen peroxide, suggesting that a major fraction of the ice nuclei stems from biogenic components in the soil. However, below 258 K, we find that the ice active site densities tend towards those expected from the mineral components in the soils, suggesting that the inorganic fraction of soil dusts, in particular the K-feldspar fraction, becomes increasingly important in the initiation of the ice phase at lower temperatures. We conclude that dusts from agricultural activities could contribute significantly to atmospheric IN concentrations, if such dusts exhibit similar activities to those observed in the current laboratory study.