Abstract. We present the laboratory results of immersion freezing efficiencies of cellulose particles at supercooled temperature (T) conditions. Three types of chemically homogeneous cellulose samples are used as surrogates that represent supermicron and submicron ice-nucleating plant structural polymers. These samples include microcrystalline cellulose (MCC), fibrous cellulose (FC) and nanocrystalline cellulose (NCC). Our immersion freezing dataset includes data from various ice nucleation measurement techniques available at 17 different institutions, including nine dry dispersion and 11 aqueous suspension techniques. With a total of 20 methods, we performed systematic accuracy and precision analysis of measurements from all 20 measurement techniques by evaluating T-binned (1 ∘C) data over a wide T range (−36 ∘C <T<-4 ∘C). Specifically, we intercompared the geometric surface area-based ice nucleation active surface site (INAS) density data derived from our measurements as a function of T, ns,geo(T). Additionally, we also compared the ns,geo(T) values and the freezing spectral slope parameter (Δlog(ns,geo)/ΔT) from our measurements to previous literature results. Results show all three cellulose materials are reasonably ice active. The freezing efficiencies of NCC samples agree reasonably well, whereas the diversity for the other two samples spans ≈ 10 ∘C. Despite given uncertainties within each instrument technique, the overall trend of the ns,geo(T) spectrum traced by the T-binned average of measurements suggests that predominantly supermicron-sized cellulose particles (MCC and FC) generally act as more efficient ice-nucleating particles (INPs) than NCC with about 1 order of magnitude higher ns,geo(T).
Abstract. The Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) campaign was carried out north-west of Svalbard (Norway) between 23 May and 6 June 2017. The objective of ACLOUD was to study Arctic boundary layer and mid-level clouds and their role in Arctic amplification. Two research aircraft (Polar 5 and 6) jointly performed 22 research flights over the transition zone between open ocean and closed sea ice. Both aircraft were equipped with identical instrumentation for measurements of basic meteorological parameters, as well as for turbulent and radiative energy fluxes. In addition, on Polar 5 active and passive remote sensing instruments were installed, while Polar 6 operated in situ instruments to characterize cloud and aerosol particles as well as trace gases. A detailed overview of the specifications, data processing, and data quality is provided here. It is shown that the scientific analysis of the ACLOUD data benefits from the coordinated operation of both aircraft. By combining the cloud remote sensing techniques operated on Polar 5, the synergy of multi-instrument cloud retrieval is illustrated. The remote sensing methods were validated using truly collocated in situ and remote sensing observations. The data of identical instruments operated on both aircraft were merged to extend the spatial coverage of mean atmospheric quantities and turbulent and radiative flux measurement. Therefore, the data set of the ACLOUD campaign provides comprehensive in situ and remote sensing observations characterizing the cloudy Arctic atmosphere. All processed, calibrated, and validated data are published in the World Data Center PANGAEA as instrument-separated data subsets (Ehrlich et al., 2019b, https://doi.org/10.1594/PANGAEA.902603).
Abstract. To date, only a few studies have investigated the potential of coal fly ash particles to trigger heterogeneous ice nucleation in cloud droplets. The presented measurements aim at expanding the sparse dataset and improving process understanding of how physicochemical particle properties can influence the freezing behavior of coal fly ash particles immersed in water. Firstly, immersion freezing measurements were performed with two single particle techniques, i.e., the Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the SPectrometer for Ice Nuclei (SPIN). The effect of suspension time on the efficiency of the coal fly ash particles when immersed in a cloud droplet is analyzed based on the different residence times of the two instruments and employing both dry and wet particle generation. Secondly, two cold-stage setups, one using microliter sized droplets (Leipzig Ice Nucleation Array) and one using nanoliter sized droplets (WeIzmann Supercooled Droplets Observation on Microarray setup) were applied. We found that coal fly ash particles are comparable to mineral dust in their immersion freezing behavior when being dry generated. However, a significant decrease in immersion freezing efficiency was observed during experiments with wet-generated particles in LACIS and SPIN. The efficiency of wet-generated particles is in agreement with the cold-stage measurements. In order to understand the reason behind the deactivation, a series of chemical composition, morphology, and crystallography analyses (single particle mass spectrometry, scanning electron microscopy coupled with energy dispersive X-ray microanalysis, X-ray diffraction analysis) were performed with dry- and wet-generated particles. From these investigations, we conclude that anhydrous CaSO4 and CaO – which, if investigated in pure form, show the same qualitative immersion freezing behavior as observed for dry-generated coal fly ash particles – contribute to triggering heterogeneous ice nucleation at the particle–water interface. The observed deactivation in contact with water is related to changes in the particle surface properties which are potentially caused by hydration of CaSO4 and CaO. The contribution of coal fly ash to the ambient population of ice-nucleating particles therefore depends on whether and for how long particles are immersed in cloud droplets.
The custom-built Portable Fine Particle Concentrator (PFPC) is evaluated for the measurement of ice nucleating particles (INPs) in the atmosphere. The concentrations of INPs in remote regions of the atmosphere are very low, often close to instrumental detection limits. The PFPC is a dual slit-nozzle virtual impactor where particles are concentrated from an input flow of 250 LPM (litres per minute) into an output flow of 10 LPM. The enrichment factors for ambient particles with diameters between 0.4 and 2.5 µm were found to be 21 ± 5 at sea level and 18 ± 2 at a field station 3580 meters above sea level for the PFPC operated in horizontal configuration. Similar enhancement factors (16 ± 5) in the concentrations of INPs measured by the Horizontal Ice Nucleation Chamber at the high altitude station were observed when the air mass was characterized by high numbers of particles larger than 0.5 µm. When the number size distribution was dominated by particles smaller than 0.5 µm, the INP enrichment factor was considerably lower. Corroborating short-term measurements were provided by additional INP-measuring instruments, the Fast Ice Nucleus CHamber and the Frankfurt Ice Deposition Freezing Experiment. Results from two aerosol mass spectrometers also indicate significant particle enhancement using the PFPC. These results indicate that the PFPC can be usefully deployed to improve the detection efficiency of ambient INP measurements.
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