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In this paper, we present the design, development, and characteristics of the novel aerosol mass spectrometer ERICA (ERC Instrument for Chemical composition of Aerosols; ERC – European Research Council) and selected results from the first airborne field deployment. The instrument combines two well-established methods of real-time in situ measurements of fine particle chemical composition. The first method is the laser desorption and ionization technique, or laser ablation technique, for single-particle mass spectrometry (here with a frequency-quadrupled Nd:YAG laser at λ = 266 nm). The second method is a combination of thermal particle desorption, also called flash vaporization, and electron impact ionization (like the Aerodyne aerosol mass spectrometer). The same aerosol sample flow is analyzed using both methods simultaneously, each using time-of-flight mass spectrometry. By means of the laser ablation, single particles are qualitatively analyzed (including the refractory components), while the flash vaporization and electron impact ionization technique provides quantitative information on the non-refractory components (i.e., particulate sulfate, nitrate, ammonia, organics, and chloride) of small particle ensembles. These techniques are implemented in two consecutive instrument stages within a common sample inlet and a common vacuum chamber. At its front end, the sample air containing the aerosol particles is continuously injected via an aerodynamic lens. All particles which are not ablated by the Nd:YAG laser in the first instrument stage continue their flight until they reach the second instrument stage and impact on the vaporizer surface (operated at 600 ∘C). The ERICA is capable of detecting single particles with vacuum aerodynamic diameters (dva) between ∼ 180 and 3170 nm (d50 cutoff). The chemical characterization of single particles is achieved by recording cations and anions with a bipolar time-of-flight mass spectrometer. For the measurement of non-refractory components, the particle size range extends from approximately 120 to 3500 nm (d50 cutoff; dva), and the cations are detected with a time-of-flight mass spectrometer. The compact dimensions of the instrument are such that the ERICA can be deployed on aircraft, at ground stations, or in mobile laboratories. To characterize the focused detection lasers, the ablation laser, and the particle beam, comprehensive laboratory experiments were conducted. During its first deployments the instrument was fully automated and operated during 11 research flights on the Russian high-altitude research aircraft M-55 Geophysica from ground pressure and temperature to 20 km altitude at 55 hPa and ambient temperatures as low as −86 ∘C. In this paper, we show that the ERICA is capable of measuring reliably under such conditions.

The Erd\H{o}s-Simonovits stability theorem states that for all \epsilon >0 there exists \alpha >0 such that if G is a K_{r+1}-free graph on n vertices with e(G) > ex(n,K_{r+1}) - \alpha n^2, then one can remove \epsilon n^2 edges from G to obtain an r-partite graph. F\"uredi gave a short proof that one can choose \alpha=\epsilon. We give a bound for the relationship of \alpha and \varepsilon which is asymptotically sharp as \epsilon \to 0., Comment: 12 pages, 1 figure

The aim of this study is to show how a newly developed aerodynamic lens system (ALS), a delayed ion extraction (DIE), and better electric shielding improve the efficiency of the Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA). These improvements are applicable to single-particle laser ablation mass spectrometers in general. To characterize the modifications, extensive size-resolved measurements with spherical polystyrene latex particles (PSL; 150–6000 nm) and cubic sodium chloride particles (NaCl; 400–1700 nm) were performed. Measurements at a fixed ALS position show an improved detectable particle size range of the new ALS compared to the previously used Liu-type ALS, especially for supermicron particles. At a lens pressure of 2.4 hPa, the new ALS achieves a PSL particle size range from 230 to 3240 nm with 50 % detection efficiency and between 350 and 2000 nm with 95 % detection efficiency. The particle beam divergence was determined by measuring the detection efficiency at variable ALS positions along the laser cross sections and found to be minimal for PSL at about 800 nm. Compared to measurements by single-particle mass spectrometry (SPMS) instruments using Liu-type ALSs, the minimum particle beam divergence is shifted towards larger particle sizes. However, there are no disadvantages compared to the Liu-type lenses for particle sizes down to 200 nm. Improvements achieved by using the DIE and an additional electric shielding could be evaluated by size-resolved measurements of the hit rate, which is the ratio of laser pulses yielding a detectable amount of ions to the total number of emitted laser pulses. In particular, the hit rate for multiply charged particles smaller than 500 nm is significantly improved by preventing an undesired deflection of these particles in the ion extraction field. Moreover, it was found that by using the DIE the ion yield of the ablation, ionization, and ion extraction process could be increased, resulting in up to 7 times higher signal intensities of the cation spectra. The enhanced ion yield results in a larger effective width of the ablation laser beam, which in turn leads to a hit rate of almost 100 % for PSL particles in the size range from 350 to 2000 nm. Regarding cubic NaCl particles the modifications of the ALABAMA result in an up to 2 times increased detection efficiency and an up to 5 times increased hit rate. The need for such instrument modifications arises in particular for measurements of particles that are present in low number concentrations such as ice-nucleating particles (INPs) in general, but also aerosol particles at high altitudes or in pristine environments. Especially for these low particle number concentrations, improved efficiencies help to overcome the statistical limitations of single-particle mass spectrometer measurements. As an example, laboratory INP measurements carried out in this study show that the application of the DIE alone increases the number of INP mass spectra per time unit by a factor of 2 to 3 for the sampled substances. Overall, the combination of instrument modifications presented here resulted in an increased measurement efficiency of the ALABAMA for different particle types and particles shape as well as for highly charged particles.

We present a novel and compact design of a constant-pressure inlet (CPI) developed for use in airborne aerosol mass spectrometry. In particular, the inlet system is optimized for aerodynamic lenses commonly used in aerosol mass spectrometers, in which efficient focusing of aerosol particles into a vacuum chamber requires a precisely controlled lens pressure, typically of a few hectopascals. The CPI device can also be used in condensation particle counters (CPCs), cloud condensation nucleus counters (CCNCs), and gas-phase sampling instruments across a wide range of altitudes and inlet pressures. The constant pressure is achieved by changing the inner diameter of a properly scaled O-ring that acts as a critical orifice. The CPI control keeps air pressure and thereby mass flow rate (≈0.1 L min−1) upstream of an aerodynamic lens constant, deviating at most by only ±2 % from a preset value. In our setup, a pressure sensor downstream of the O-ring maintains control of the pinch mechanism via a feedback loop and setpoint conditions are reached within seconds. The device was implemented in a few instruments, which were successfully operated on different research aircraft covering a wide range of ambient pressures, from sea level up to about 55 hPa. Details of operation and the quality of aerosol particle transmission were evaluated by laboratory experiments and in-flight data with a single-particle mass spectrometer.

Primary ice formation in mixed-phase clouds is initiated by a minute subset of the ambient aerosol population, called ice-nucleating particles (INPs). The knowledge about their atmospheric concentration, composition, and source in cloud-relevant environments is still limited. During the 2017 joint INUIT/CLACE (Ice Nuclei research UnIT/CLoud-Aerosol Characterization Experiment) field campaign, observations of INPs as well as of aerosol physical and chemical properties were performed, complemented by source region modeling. This aimed at investigating the nature and sources of INPs. The campaign took place at the High-Altitude Research Station Jungfraujoch (JFJ), a location where mixed-phase clouds frequently occur. Due to its altitude of 3580ma.s.l., the station is usually located in the lower free troposphere, but it can also receive air masses from terrestrial and marine sources via long-range transport. INP concentrations were quasi-continuously detected with the Horizontal Ice Nucleation Chamber (HINC) under conditions representing the formation of mixed-phase clouds at 31 degrees C. The INP measurements were performed in parallel to aerosol measurements from two single-particle mass spectrometers, the Aircraft-based Laser ABlation Aerosol MAss Spectrometer (ALABAMA) and the laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF). The chemical identity of INPs is inferred by correlating the time series of ion signals measured by the mass spectrometers with the time series of INP measurements. Moreover, our results are complemented by the direct analysis of ice particle residuals (IPRs) by using an ice-selective inlet (IceCVI) coupled with the ALABAMA. Mineral dust particles and aged sea spray particles showed the highest correlations with the INP time series. Their role as INPs is further supported by source emission sensitivity analysis using atmospheric transport modeling, which confirmed that air masses were advected from the Sahara and marine environments during times of elevated INP concentrations and ice-active surface site densities. Indeed, the IPR analysis showed that, by number, mineral dust particles dominated the IPR composition (similar to 58 %), and biological and metallic particles are also found to a smaller extent (similar to 10% each). Sea spray particles are also found as IPRs (17 %), and their fraction in the IPRs strongly varied according to the increased presence of small IPRs, which is likely due to an impact from secondary ice crystal formation. This study shows the capability of combining INP concentration measurements with chemical characterization of aerosol particles using single-particle mass spectrometry, source region modeling, and analysis of ice residuals in an environment directly relevant for mixed-phase cloud formation., Atmospheric Chemistry and Physics, 21 (22), ISSN:1680-7375, ISSN:1680-7367

Digital Terrain Models (DTM) play an important role for digital twins of the built environment. However, if the Building Information Modeling method (BIM) is used, many engineers find it difficult to provide BIM-compliant terrain models. We present a small tool with which classic DTM, which have been created by landsurveyors or geospatial engineers, can be converted into the format Industry Foundation Classes (IFC) in order to be used in openBIM projects. This paper first clarifies the use cases and then goes into detail on possible configurations of the transformation process. With the presented software tool IfcTerrain the user may select different export options concerning IFC object type of the terrain, geometric representation, georeferencing or the annotation with metadata. IfcTerrain is free and open source and was developed in the context of an educational institution.

Building Information Modeling (BIM) is a method for the digital collaborative design, construction and operation of buildings. However, in order to realize a complete view on needed work and expenses of a building, the surrounding landscape elements must be considered as well. Within this paper, the BIM authoring tool Autodesk Revit and the open BIM data model and exchange format Industry Foundation Classes (IFC) has been investigated for its capability to represent landscape elements like a terrain model, retaining walls, and ways. Therefore, a feasibility study has been carried out including the surveying of real-world landscape objects like terrain, buildings, ways and paths, playgrounds, and retaining walls, in order to use actual existing objects instead of idealized, theoretical elements. The aim was to develop and evaluate a workflow from the surveying over the modeling in BIM-able software to the export of an IFC data file. Therefore, the general modeling concepts of BIM and their suitability and limitations for representing landscape elements has been investigated. Experiences made within the project are discussed and first solutions and concepts are recommended. In addition, this paper reports from the buildingSmart International working group “Site, Landscape, and Urban Planning”, their current work and future goals, in order to extend IFC for landscape objects. Additionally, a concept for level of information need referring to landscape elements is shown.

A consortium of polar scientists combined observational forces in a field campaign of unprecedented complexity to uncover the secrets of clouds and their role in Arctic amplification. Two research aircraft, an icebreaker research vessel, an ice-floe camp including an instrumented tethered balloon, and a permanent ground-based measurement station were employed in this endeavour. Clouds play an important role in Arctic amplification. This term represents the recently observed enhanced warming of the Arctic relative to the global increase of near-surface air temperature. However, there are still important knowledge gaps regarding the interplay between Arctic clouds and aerosol particles, surface properties, as well as turbulent and radiative fluxes that inhibit accurate model simulations of clouds in the Arctic climate system. In an attempt to resolve this so-called Arctic cloud puzzle, two comprehensive and closely coordinated field studies were conducted: the ”Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD)” aircraft campaign, and the ”Physical feedbacks of Arctic boundary layer, Sea ice, Cloud and AerosoL (PASCAL)” ice breaker expedition. Both observational studies were performed in the framework of the German ”ArctiC Amplification:Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)3” project. They took place in the vicinity of Svalbard (Norway) in May and June 2017. ACLOUD and PASCAL explored four pieces of the Arctic cloud puzzle: Cloud properties, aerosol impact on clouds, atmospheric radiation, and turbulent-dynamical processes. The two instrumented Polar 5 and Polar 6 aircraft, the icebreaker research vessel (RV) Polarstern, an ice-floe camp including an instrumented tethered balloon, and the permanent, ground-based measurement station at Ny-Ålesund (Svalbard) were employed to observe Arctic low and mid-level, mixed-phase clouds, and to investigate related atmospheric and surface processes. The Polar 5 aircraft served as a remote sensing observatory examining the clouds from above by downward-looking sensors; the Polar 6 aircraft operated as a flying in-situ measurement laboratory sampling inside and below the clouds. Most of the collocated Polar 5/6 flights were conducted either above RV Polarstern or over the Ny-Ålesund station, both of which monitored the clouds from below using similar but upward-looking remote sensing techniques as the Polar 5 aircraft. Several of the flights were carried out underneath collocated satellite tracks. The paper motivates the scientific objectives of the ACLOUD/PASCAL observations and describes the measured quantities, retrieved parameters, and the applied complementary instrumentation. Furthermore, it discusses selected measurement results, and poses critical research questions to be answered in future papers analyzing the data from the two field campaigns.

A triangle $T'$ is $\varepsilon$-similar to another triangle $T$ if their angles pairwise differ by at most $\varepsilon$. Given a triangle $T$, $\varepsilon>0$ and $n\in\mathbb{N}$, B\'ar\'any and F\"uredi asked to determine the maximum number of triangles $h(n,T,\varepsilon)$ being $\varepsilon$-similar to $T$ in a planar point set of size $n$. We show that for almost all triangles $T$ there exists $\varepsilon=\varepsilon(T)>0$ such that $h(n,T,\varepsilon)=n^3/24 (1+o(1))$. Exploring connections to hypergraph Tur\'an problems, we use flag algebras and stability techniques for the proof., Comment: 20 pages

A well-known conjecture by Erdős states that every triangle-free graph on n vertices can be made bipartite by removing at most \(n^2/25\) edges. This conjecture was known for graphs with edge density at least 0.4 and edge density at most 0.172. Here, we will extend the edge density for which this conjecture is true; we prove the conjecture for graphs with edge density at most 0.2486 and for graphs with edge density at least 0.3197. Further, we prove that every triangle-free graph can be made bipartite by removing at most \(n^2/23.5\) edges improving the previously best bound of \(n^2/18\).

We analyse aerosol particle composition measurements from five research missions between 2014 and 2018 to assess the meridional extent of particles containing meteoric material in the upper troposphere and lower stratosphere (UTLS). Measurements from the Jungfraujoch mountaintop site and a low-altitude aircraft mission show that meteoric material is also present within middle- and lower-tropospheric aerosol but within only a very small proportion of particles. For both the UTLS campaigns and the lower- and mid-troposphere observations, the measurements were conducted with single-particle laser ablation mass spectrometers with bipolar-ion detection, which enabled us to measure the chemical composition of particles in a diameter range of approximately 150 nm to 3 µm. The five UTLS aircraft missions cover a latitude range from 15 to 68∘ N, altitudes up to 21 km, and a potential temperature range from 280 to 480 K. In total, 338 363 single particles were analysed, of which 147 338 were measured in the stratosphere. Of these total particles, 50 688 were characterized by high abundances of magnesium and iron, together with sulfuric ions, the vast majority (48 610) in the stratosphere, and are interpreted as meteoric material immersed or dissolved within sulfuric acid. It must be noted that the relative abundance of such meteoric particles may be overestimated by about 10 % to 30 % due to the presence of pure sulfuric acid particles in the stratosphere which are not detected by the instruments used here. Below the tropopause, the observed fraction of the meteoric particle type decreased sharply with 0.2 %–1 % abundance at Jungfraujoch, and smaller abundances (0.025 %–0.05 %) were observed during the lower-altitude Canadian Arctic aircraft measurements. The size distribution of the meteoric sulfuric particles measured in the UTLS campaigns is consistent with earlier aircraft-based mass-spectrometric measurements, with only 5 %–10 % fractions in the smallest particles detected (200–300 nm diameter) but with substantial (> 40 %) abundance fractions for particles from 300–350 up to 900 nm in diameter, suggesting sedimentation is the primary loss mechanism. In the tropical lower stratosphere, only a small fraction (< 10 %) of the analysed particles contained meteoric material. In contrast, in the extratropics the observed fraction of meteoric particles reached 20 %–40 % directly above the tropopause. At potential temperature levels of more than 40 K above the thermal tropopause, particles containing meteoric material were observed in much higher relative abundances than near the tropopause, and, at these altitudes, they occurred at a similar abundance fraction across all latitudes and seasons measured. Above 440 K, the observed fraction of meteoric particles is above 60 % at latitudes between 20 and 42∘ N. Meteoric smoke particles are transported from the mesosphere into the stratosphere within the winter polar vortex and are subsequently distributed towards low latitudes by isentropic mixing, typically below a potential temperature of 440 K. By contrast, the findings from the UTLS measurements show that meteoric material is found in stratospheric aerosol particles at all latitudes and seasons, which suggests that either isentropic mixing is effective also above 440 K or that meteoric fragments may be the source of a substantial proportion of the observed meteoric material.

A novel approach for a robust computation of positional relations of two-dimensional geometric features is presented which guarantees reliable results, provided that the initial data is valid. The method is based on the use of integer coordinates and a method to generate a complete, gap-less and non-overlapping spatial decomposition. The spatial relationships of two geometric features are then represented using DE-9IM matrices. These allow the spatial relationships to be represented compactly. The DE-9IM matrices are based on the spatial decomposition using explicit neighborhood relations. No further geometric calculations are required for their computation. Based on comparative tests, it could be proven that this approach, up to a predictable limit, provides correct results and thus offers advantages over classical methods for the calculation of spatial relationships. This novel method can be used in all fields, especially where guaranteed reliable results are required.:Introduction Related Research Materials and Methods Results Discussion Outlook Author Contributions Funding Institutional Review Board Statement Informed Consent Statement Data Availability Statement Conflicts of Interest Abbreviations References

In this paper we analyze aerosol particle composition measurements from five research missions conducted between 2014 and 2018 sampling the upper troposphere and lower stratosphere (UTLS), to assess the meridional extent of particles containing meteoric material. Additional data sets from a ground based study and from a low altitude aircraft mission are used to confirm the existence of meteoric material in lower tropospheric particles. Single particle laser ablation techniques with bipolar ion detection were used to measure the chemical composition of particles in a size range of approximately 150 nm to 3 μm. The five UTLS aircraft missions cover a latitude range from 15 to 68° N, altitudes up to 21 km, and a potential temperature range from 280 to 480 K. In total, 338 363 single particles were analyzed, of which 147 338 particles were measured in the stratosphere. Of these particles, 50 688 were characterized by high abundances of magnesium, iron, and rare iron oxide compounds, together with sulfuric acid. This particle type was found almost exclusively in the stratosphere (48 610 particles) and is interpreted as meteoric material immersed or dissolved within stratospheric sulfuric acid particles. Below the tropopause, the observed fraction of this particle type decreases sharply. However, small fractional abundances were observed below 3000 m a.s.l. in the Canadian Arctic and also at the Jungfraujoch high altitude station (3600 m a.s.l.). Thus, the removal pathway by sedimentation and/or mixing into the troposphere is confirmed. In the tropical lower stratosphere, only a small fraction (

The aim of this study is to show how a newly developed aerodynamic lens system (ALS), a delayed ion extraction (DIE) and better electric shielding improve the efficiency of the Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA). These improvements are applicable to single particle laser ablation mass spectrometers in general. To characterize the modifications extensive size-resolved measurements with spherical polystyrene latex particles (PSL; 150–000 nm) and cubic sodium chloride particles (NaCl; 400–1700 nm) were performed. Measurements at a fixed ALS position show an improved detectable particle size range of the new ALS compared to the previously used Liu-type ALS, especially for super-micron particles. At a lens pressure of 2.4 hPa, the new ALS achieves a PSL particle size range from 230 nm to 3240 nm with 50 % detection efficiency and between 350 nm and 2000 nm with 95 % detection efficiency. The particle beam divergence was determined by measuring the detection efficiency at variable ALS positions along the laser cross sections and found to be minimal for PSL at about 800 nm. Compared to measurements of SPMS instruments using Liu-type ALSs, the minimum particle beam divergence is shifted towards larger particle sizes. However, there are no disadvantages compared to the Liu-type lenses for particle sizes down to 200 nm. Improvements achieved by using the DIE and an additional electric shielding could be evaluated by size-resolved measurements of the hit rate, which is the ratio of laser pulses yielding a detectable amount of ions to the total number of emitted laser pulses. In particular, the hit rate for multiply charged particles smaller 500 nm is significantly improved by preventing an undesired deflection of these particles in the ion extraction field. Moreover, it was found that by using the DIE the ion yield of the ablation, ionization and ion extraction process could be increased, resulting in up to seven times higher signal intensities of the cation spectra. The enhanced ion yield results in a larger effective width of the ablation laser beam, which in turn leads to a hit rate of almost 100 % for PSL particles in the size range from 350 nm to 2000 nm. Regarding cubic NaCl particles the modifications of the ALABMA result in a up to two times increased detection efficiency and a up to five times increased hit rate. The need for such instrument modifications arises in particular for measurements of particles that are present in low number concentrations such as ice nucleation particles (INP) in general, but also aerosol particles at high altitudes or in pristine environments. Especially for these low particle number concentrations improved efficiencies help to overcome statistical limitations of single particle mass spectrometer measurements. As an example laboratory INP measurements carried out in this study show that the application of the DIE alone increases the number of INP mass spectra per time unit by a factor of two to three for the sampled substances. Overall, the combination of instrument modifications presented here resulted in an increased measurement efficiency of the ALABAMA for different particle types, particles shapes and for highly charged particles.

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).

The Electronic Journal of Combinatorics, 27 (1), ISSN:1097-1440, ISSN:1077-8926

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 (EFs) 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 EF 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. Copyright © 2019 American Association for Aerosol Research

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 micro-crystalline cellulose (MCC), fibrous cellulose (FC) and nano-crystalline cellulose (NCC). Our experimental data show that particles resembling the MCC lab particle occur also in the atmosphere. Our immersion freezing dataset includes data from various ice nucleation measurement techniques available at seventeen different institutions, including nine dry dispersion and eleven aqueous suspension techniques. With a total of twenty methods, we performed systematic accuracy and precision analysis of measurements from all twenty measurement techniques by evaluating T-binned (1 °C) data over a wide T range (−36 °C T 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 that freezing efficiencies of NCC samples agree reasonably well, whereas the diversity for the other two samples spans for ~ 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 suggest that predominantly supermicron-sized (giant hereafter) cellulose particles (MCC and FC) generally act as more efficient ice-nucleating particles than NCC with about one order of magnitude higher ns,geo(T). Further, our results indicate significant diversity between dry and aqueous suspension measurement techniques. The ratios of the individual measurements (ns,ind) to the log average of ns,geo(T) range 0.6–1.4 across the examined T range. In general, the ratios of the log average of dry dispersion measurements are higher than those of aqueous suspension measurements. The observed discrepancy may be due to non-uniform active site density for different sizes and/or the alteration in physico-chemical properties of cellulose by liquid-suspending it. Unless otherwise defined, the cellulose system may not be an ideal calibrant. Given such a distinct difference between two subgroups of immersion freezing techniques, standardization of our methods, especially INP sampling and treatment, may be one approach to reduce the measurement diversity and valiability when we deal with a complex material like cellulose. A community-wide effort to identify specimen-specific limitations and characteristics of each technique, as well as consolidating the ns,geo(T) parameterization, is an alternative approach to achieve overall precise and accurate ice-nucleating particle measurements.

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 physico-chemical particle properties 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 and the Spectrometer for Ice Nuclei. 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 (Weizman 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) was 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 of the particle surface propertieswhich 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.