The historical development of ice nucleating particle concentrations (NINP) is still unknown. Here, we present for the first time NINP from the past 500 years at two Arctic sites derived from ice ...core samples. The samples originate from the EUROCORE ice core (Summit, Central Greenland) and from the Lomo09 ice core (Lomonosovfonna, Svalbard). No long‐term trend is obvious in the measured samples, and the overall range of NINP is comparable to present‐day observations. We observe that the short‐term variations in NINP is larger than the long‐term variability, but neither anthropogenic pollution nor volcanic eruptions seem to have influenced NINP in the measured temperature range. Shape and onset temperature of several INP spectra suggest that INP of biogenic origin contributed to the Arctic INP population throughout the past.
Key Points
No obvious trend of Arctic INP concentrations over the past 500 years is observed
Short‐term variability in INP concentrations is larger than long‐term variation
A contribution of biological sources to the Arctic INP population is likely
Ice nucleating particles (INPs) affect the radiative properties of cold clouds. Knowledge concerning their concentration above ground level and their potential sources is scarce. Here we present the ...first highly temperature resolved ice nucleation spectra of airborne samples from an aircraft campaign during late winter in 2018. Most INP spectra featured low concentration levels (<3 · 10−4 L−1 at −15°C). However, we also found INP concentrations of up to 1.8·10−2 L−1 at −15°C and freezing onsets as high as −7.5°C for samples mainly from the marine boundary layer. Shape and onset temperature of the ice nucleation spectra of those samples as well as heat sensitivity hint at biogenic INP. Colocated measurements additionally indicate a local marine influence rather than long‐range transport. Our results suggest that even in late winter above 80°N a local marine source for biogenic INP, which can efficiently nucleate ice at high temperatures, is present.
Plain Language Summary
Clouds are a key factor in the energy budget of the Arctic atmosphere. Ice nucleating particles (INPs) can modify the radiation properties and lifetime of clouds by affecting the relative abundance of liquid and frozen droplets in a cloud. Despite this important ability, knowledge about the INP concentration above ground level is limited as airborne INP measurements are very scarce in the Arctic. Here we present results from an aircraft campaign, which took place during the late winter of 2018 in latitudes above 80°N. We found INP concentrations at above −15°C, which are similar to those found in midlatitudes. These INPs also initiate freezing already at high temperatures. We found indications that the INPs are biogenic and originate from a local, marine source, rather than being transported from midlatitudes into the Arctic. Due to the presence of numerous cracks, open leads and polynyas in the sea ice in the investigation area, the ocean may provide a source for these biogenic INP in an environment, where sources on land are still shrouded in snow and ice. However, in a warming Arctic contributions from different sources might change, making the characterization of the current state important.
Key Points
Ice nucleating particles on airborne filter samples containing mainly Arctic marine boundary layer aerosol initiate freezing at −7.5°C
At −15°C, concentrations of ice nucleating particles ranged from up to 2 · 10−2 L−1 down to below 10−3 L−1
A local marine source and biogenic origin for the high‐temperature ice nucleating particles is likely
Exceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated
whether anthropogenic PM2.5 may significantly contribute to ice-nucleating ...particles (INP). However, few studies have focused on the
ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the
atmospheric number concentration of INP (NINP) in the range from −6 to −25 ∘C in Beijing. No
correlations between NINP and either PM2.5 or black carbon mass concentrations were found, although both
varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and
either total particle number concentration or number concentrations for particles with diameters >500 nm. Furthermore,
there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or
decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP
concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined
temperature range.
Kaolinite particles from two different sources (Fluka and Clay Minerals Society (CMS)) were examined with respect to their ability to act as ice nuclei (IN). This was done in the water-subsaturated ...regime where often deposition ice nucleation is assumed to occur, and for water-supersaturated conditions, i.e., in the immersion freezing mode. Measurements were done using a flow tube (the Leipzig Aerosol Cloud Interaction Simulator, LACIS) and a continuous-flow diffusion chamber (CFDC). Pure and coated particles were used, with coating thicknesses of a few nanometers or less, where the coating consisted of levoglucosan, succinic acid or sulfuric acid. In general, it was found that the coatings strongly reduced deposition ice nucleation. Remaining ice formation in the water-subsaturated regime could be attributed to immersion freezing, with particles immersed in concentrated solutions formed by the coatings. In the immersion freezing mode, ice nucleation rate coefficients jhet from both instruments agreed well with each other, particularly when the residence times in the instruments were accounted for. Fluka kaolinite particles coated with either levoglucosan or succinic acid showed the same IN activity as pure Fluka kaolinite particles; i.e., it can be assumed that these two types of coating did not alter the ice-active surface chemically, and that the coatings were diluted enough in the droplets that were formed prior to the ice nucleation, so that freezing point depression was negligible. However, Fluka kaolinite particles, which were either coated with pure sulfuric acid or were first coated with the acid and then exposed to additional water vapor, both showed a reduced ability to nucleate ice compared to the pure particles. For the CMS kaolinite particles, the ability to nucleate ice in the immersion freezing mode was similar for all examined particles, i.e., for the pure ones and the ones with the different types of coating. Moreover, jhet derived for the CMS kaolinite particles was comparable to jhet derived for Fluka kaolinite particles coated with sulfuric acid. This is suggestive for the Fluka kaolinite possessing a type of ice-nucleating surface feature which is not present on the CMS kaolinite, and which can be destroyed by reaction with sulfuric acid. This might be potassium feldspar.
Ice-nucleating particles (INPs) can initiate ice formation in clouds at temperatures above −38 ∘C through heterogeneous ice nucleation. As a result, INPs affect cloud microphysical and radiative ...properties, cloud lifetime, and precipitation behavior and thereby ultimately the Earth's climate. Yet, little is known regarding the sources, abundance and properties of INPs, especially in remote regions such as the Arctic. In this study, 2-year-long INP measurements (from July 2018 to September 2020) at Villum Research Station in northern Greenland are presented. A low-volume filter sampler was deployed to collect filter samples for offline INP analysis. An annual cycle of INP concentration (NINP) was observed, and the fraction of heat-labile INPs was found to be higher in months with low to no snow cover and lower in months when the surface was well covered in snow (> 0.8 m). Samples were categorized into three different types based only on the slope of their INP spectra, namely into summer, winter and mix type. For each of the types a temperature-dependent INP parameterization was derived, clearly different depending on the time of the year. Winter and summer types occurred only during their respective seasons and were seen 60 % of the time. The mixed type occurred in the remaining 40 % of the time throughout the year. April, May and November were found to be transition months. A case study comparing April 2019 and April 2020 was performed. The month of April was selected because a significant difference in NINP was observed during these two periods, with clearly higher NINP in April 2020. In parallel to the observed differences in NINP, also a higher cloud-ice fraction was observed in satellite data for April 2020, compared to April 2019. NINP in the case study period revealed no clear dependency on either meteorological parameters or different surface types which were passed by the collected air masses. Overall, the results suggest that the coastal regions of Greenland were the main sources of INPs in April 2019 and 2020, most likely including both local terrestrial and marine sources.
Heterogeneous ice nucleation, a primary pathway for ice formation in the atmosphere, has been described alternately as being stochastic, in direct analogy with homogeneous nucleation, or singular, ...with ice nuclei initiating freezing at deterministic temperatures. We present an idealized, conceptual model to explore the transition between stochastic and singular ice nucleation. This "soccer ball" model treats particles as being covered with surface sites (patches of finite area) characterized by different nucleation barriers, but with each surface site following the stochastic nature of ice embryo formation. The model provides a phenomenological explanation for seemingly contradictory experimental results obtained in our research groups. Even with ice nucleation treated fundamentally as a stochastic process this process can be masked by the heterogeneity of surface properties, as might be typical for realistic atmospheric particle populations. Full evaluation of the model findings will require experiments with well characterized ice nucleating particles and the ability to vary both temperature and waiting time for freezing.
Birch pollen grains are known to be ice nucleating active biological particles. The ice nucleating activity has previously been tracked down to biological macromolecules that can be easily extracted ...from the pollen grains in water. In the present study, we investigated the immersion freezing behavior of these ice nucleating active (INA) macromolecules. Therefore we measured the frozen fractions of particles generated from birch pollen washing water as a function of temperature at the Leipzig Aerosol Cloud Interaction Simulator (LACIS). Two different birch pollen samples were considered, with one originating from Sweden and one from the Czech Republic. For the Czech and Swedish birch pollen samples, freezing was observed to start at −19 and −17 °C, respectively. The fraction of frozen droplets increased for both samples down to −24 °C. Further cooling did not increase the frozen fractions any more. Instead, a plateau formed at frozen fractions below 1. This fact could be used to determine the amount of INA macromolecules in the droplets examined here, which in turn allowed for the determination of nucleation rates for single INA macromolecules. The main differences between the Swedish birch pollen and the Czech birch pollen were obvious in the temperature range between −17 and −24 °C. In this range, a second plateau region could be seen for Swedish birch pollen. As we assume INA macromolecules to be the reason for the ice nucleation, we concluded that birch pollen is able to produce at least two different types of INA macromolecules. We were able to derive parameterizations for the heterogeneous nucleation rates for both INA macromolecule types, using two different methods: a simple exponential fit and the Soccer ball model. With these parameterization methods we were able to describe the ice nucleation behavior of single INA macromolecules from both the Czech and the Swedish birch pollen.
In this study we present results from immersion freezing experiments with size‐segregated mineral dust particles. Besides two already existing data sets for Arizona Test Dust (ATD), and Fluka ...kaolinite, we show two new data sets for illite‐NX, which consists mainly of illite, a clay mineral, and feldspar, a common crustal material. The experiments were carried out with the Leipzig Aerosol Cloud Interaction Simulator. After comparing the different dust samples, it became obvious that the freezing ability was positively correlated with the K‐feldspar content. Furthermore, a comparison of the composition of the ATD, illite‐NX, and feldspar samples suggests that within the K‐feldspars, microcline is more ice nucleation active than orthoclase. A coating with sulfuric acid leads to a decrease in the ice nucleation ability of all mineral dusts, with the effect being more pronounced for the feldspar sample.
Key Points
The freezing ability of mineral dusts correlated with the K‐feldspar contentAmong feldspars, microcline shows a better ice nucleation ability than orthoclaseAfter coating, all investigated dusts feature a similar ice nucleation ability
We derived the range of particle hygroscopicities (κ) that occurs in the atmosphere, based on literature data of measured hygroscopic growth or based on chemical composition. The derived κ‐values ...show that the atmospheric aerosol often is an external mixture with respect to hygroscopicity. Mean κ were derived for urban, rural, and marine aerosols for the different hygroscopic modes. Using these κ and exemplary particle number size distributions for the different aerosols, the number concentration of cloud condensation nuclei (NCCN) was derived for two cases, (1) accounting for the less hygroscopic fraction of particles and (2) assuming all particles to have κ of the more hygroscopic mode. NCCN derived from measured particle hygroscopicity is overestimated for case (2). Overestimation of NCCN is largest for fresh continental aerosol and less pronounced for marine aerosol. With κ derived from bulk aerosol composition data, only the hygroscopicity of more soluble aerosol particles is captured. Bulk or even size‐resolved composition data will be insufficient to predict NCCN under many conditions unless independent information about particle mixing state is available.
During the FROST-2 (FReezing Of duST) measurement campaign conducted at the Leipzig Aerosol Cloud Interaction Simulator (LACIS), we investigated changes in the ice nucleation properties of 300 nm ...Arizona Test Dust mineral particles following thermochemical processing by varying amounts and combinations of exposure to sulphuric acid vapour, ammonia gas, water vapour, and heat. The processed particles' heterogeneous ice nucleation properties were determined in both the water subsaturated and supersaturated humidity regimes at −30 °C and −25 °C using Colorado State University's continuous flow diffusion chamber. The amount of sulphuric acid coating material was estimated by an aerosol mass spectrometer and from CCN-derived hygroscopicity measurements. The condensation of sulphuric acid decreased the dust particles' ice nucleation ability in proportion to the amount of sulphuric acid added. Heating the coated particles in a thermodenuder at 250 °C – intended to evaporate the sulphuric acid coating – reduced their freezing ability even further. We attribute this behaviour to accelerated acid digestion of ice active surface sites by heat. Exposing sulphuric acid coated dust to ammonia gas produced particles with similarly poor freezing potential; however a portion of their ice nucleation ability could be restored after heating in the thermodenuder. In no case did any combination of thermochemical treatments increase the ice nucleation ability of the coated mineral dust particles compared to unprocessed dust. These first measurements of the effect of identical chemical processing of dust particles on their ice nucleation ability under both water subsaturated and mixed-phase supersaturated cloud conditions revealed that ice nucleation was more sensitive to all coating treatments in the water subsaturated regime. The results clearly indicate irreversible impairment of ice nucleation activity in both regimes after condensation of concentrated sulphuric acid. This implies that the sulphuric acid coating caused permanent chemical and/or physical modification of the ice active surface sites; the possible dissolution of the coating during droplet activation did not restore all immersion/condensation-freezing ability.
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