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Dimethyl sulfide (DMS) influences climate via cloud condensation nuclei (CCN) formation resulting from its oxidation products (mainly methanesulfonic acid, MSA, and sulfuric acid, H2SO4). Despite their importance, accurate prediction of MSA and H2SO4from DMS oxidation remains challenging. With comprehensive experiments carried out in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at CERN, we show that decreasing the temperature from +25 to -10 °C enhances the gas-phase MSA production by an order of magnitude from OH-initiated DMS oxidation, while H2SO4production is modestly affected. This leads to a gas-phase H2SO4-to-MSA ratio (H2SO4/MSA) smaller than one at low temperatures, consistent with field observations in polar regions. With an updated DMS oxidation mechanism, we find that methanesulfinic acid, CH3S(O)OH, MSIA, forms large amounts of MSA. Overall, our results reveal that MSA yields are a factor of 2-10 higher than those predicted by the widely used Master Chemical Mechanism (MCMv3.3.1), and the NOxeffect is less significant than that of temperature. Our updated mechanism explains the high MSA production rates observed in field observations, especially at low temperatures, thus, substantiating the greater importance of MSA in the natural sulfur cycle and natural CCN formation. Our mechanism will improve the interpretation of present-day and historical gas-phase H2SO4/MSA measurements. publishedVersion

The formation of ice particles in Earth's atmosphere strongly influences the dynamics and optical properties of clouds and their impacts on the climate system. Ice formation in clouds is often triggered heterogeneously by ice-nucleating particles (INPs) that represent a very low number of particles in the atmosphere. To date, many sources of INPs, such as mineral and soil dust, have been investigated and identified in the low and mid latitudes. Although less is known about the sources of ice nucleation at high latitudes, efforts have been made to identify the sources of INPs in the Arctic and boreal environments. In this study, we investigate the INP emission potential from high-latitude boreal forests in the mixed-phase cloud regime. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiala, Finland, between February and June 2018. The campaign utilized the infrastructure of the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR) II, with additional INP instruments, including the Portable Ice Nucleation Chamber I and II (PINC and PINCii), the SPectrometer for Ice Nuclei (SPIN), the Portable Ice Nucleation Experiment (PINE), the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT) and the Microlitre Nucleation by Immersed Particle Instrument (mu L-NIPI), used to quantify the INP concentrations and sources in the boreal environment. In this contribution, we describe the measurement infrastructure and operating procedures during HyICE-2018, and we report results from specific time periods where INP instruments were run in parallel for inter-comparison purposes. Our results show that the suite of instruments deployed during HyICE-2018 reports consistent results and therefore lays the foundation for forthcoming results to be considered holistically. In addition, we compare measured INP concentrations to INP parameterizations, and we observe good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA., Atmospheric Chemistry and Physics, 22 (8), ISSN:1680-7375, ISSN:1680-7367

Satellite- and aircraft-based mid-infrared measurements of polar stratospheric clouds (PSCs) have provided spectroscopic evidence for the presence of β-NAT (nitric acid trihydrate) particles. Metastable nitric acid hydrate phases such as α-NAT and α-NAD (nitric acid dihydrate) have been frequently observed in laboratory experiments, but not yet detected as a constituent of PSCs in atmospheric measurements. As for the β-NAD modification, its formation was first observed in X-ray diffraction measurements when the low-temperature α-NAD phase was warmed to a temperature above 210 K. Its infrared spectrum has been reported, but so far no optical constants have been derived that could be used as input for infrared retrievals of PSC composition. In this work, we show that β-NAD particles were efficiently formed in isothermal, heterogeneous crystallisation experiments at 190 K from supercooled HNO3/H2O solution droplets containing an embedded mineral dust or meteoric smoke particle analogue. An inversion algorithm based on a T-matrix optical model was used to derive for the first time the mid-infrared complex refractive indices of the β-NAD modification from the measured extinction spectrum of the particles. In contrast to the heterogeneous crystallisation experiments, the α-NAD phase was formed when the HNO3/H2O solution droplets did not contain a solid nucleus and crystallised homogeneously. Using a light scattering detector that recorded two-dimensional scattering patterns of the crystallised NAD particles, we were able to determine predominant shapes of the α- and β-NAD crystals. We found that α-NAD grew into elongated, needle-shaped crystals, while β-NAD particles were compact in shape. This agrees with previously reported images of α- and β-NAD particles grown on the cryo-stage of an Environmental Scanning Electron Microscope.

Earlier chapters of this work have described procedures and protocols that are applicable to most chambers, this chapter has a slightly different focus; we predominantly consider multiphase processes where the applications are on phase transfer of chemical species rather than chemical reactions and the processes are generally occurring in highly specialized chambers. Three areas are described. Firstly, cloud formation processes; here, precise control of physical and thermodynamic properties is required to generate reproducible results. The second area examined is the air/sea interface, looking at the formation of aerosols from nonanoic acid as a surfactant with humic acid as a photosensitizer. The final apparatus described is the Roland von Glasow sea-ice chamber where a detailed protocol for the reproducible formation of sea-ice is given along with an outlook of future work. The systems studied in all three sections are characterized by difficulties in making detailed in situ observations in the real world, either due to the transitory nature of systems or the practical difficulties in accessing the systems. While these specialized simulation chambers may not perfectly reproduce conditions in the real world, the chambers do provide more facile opportunities for making extended and reproducible measurements to investigate fundamental physical and chemical processes, at significantly lower costs.

Atmospheric simulation chambers are often utilized to study the physical properties and chemical reactivity of particles suspended in air. In this chapter, the various approaches employed for the addition of particles to simulation chambers are described in detail. Procedures for the generation of monodispersed seed aerosols, mineral dust, soot particles and bioaerosols are all presented using illustrative examples from chamber experiments. Technical descriptions of the methods used for the addition of whole emissions (gases and particles) from real-world sources such as wood-burning stoves, automobile engines and plants are also included, along with an outline of experimental approaches for investigating the atmospheric processing of these emissions.

Ice growth from vapor deposition is an important process for the evolution of cirrus clouds, but the physics of depositional ice growth at the low temperatures ( K) characteristic of the upper troposphere and lower stratosphere is not well understood. Surface attachment kinetics, generally parameterized as a deposition coefficient αD, control ice crystal habit and also may limit growth rates in certain cases, but significant discrepancies between experimental measurements have not been satisfactorily explained. Experiments on single ice crystals have previously indicated the deposition coefficient is a function of temperature and supersaturation, consistent with growth mechanisms controlled by the crystal's surface characteristics. Here we use observations from cloud chamber experiments in the Aerosol Interactions and Dynamics in the Atmosphere (AIDA) aerosol and cloud chamber to evaluate surface kinetic models in realistic cirrus conditions. These experiments have rapidly changing temperature, pressure, and ice supersaturation such that depositional ice growth may evolve from diffusion limited to surface kinetics limited over the course of a single experiment. In Part 1, we describe the adaptation of a Lagrangian parcel model with the Diffusion Surface Kinetics Ice Crystal Evolution (DiSKICE) model (Zhang and Harrington, 2014) to the AIDA chamber experiments. We compare the observed ice water content and saturation ratios to that derived under varying assumptions for ice surface growth mechanisms for experiments simulating ice clouds between 180 and 235 K and pressures between 150 and 300 hPa. We found that both heterogeneous and homogeneous nucleation experiments at higher temperatures (>205 K) could generally be modeled consistently with either a constant deposition coefficient or the DiSKICE model assuming growth on isometric crystals via abundant surface dislocations. Lower-temperature experiments showed more significant deviations from any depositional growth model, with different ice growth rates for heterogeneous and homogeneous nucleation experiments.

The presence of ice in mixed-phase clouds has a vital impact on their radiative properties, lifetime, and ability to precipitate. Ice crystal formation is initially induced by a rare subset of ambient aerosol particles called ice-nucleating particles (INPs). Despite the importance of INPs on aerosol-cloud interactions and century-long research efforts, the knowledge about their nature and atmospheric abundance still needs improvement. Recent instrument developments allow more automated and continuous INP measurements with a high time resolution, to gain a better understanding of the natural variability of INPs in different locations, and to investigate the identity and source regions of them. Here we present long-term observations of INPs at Storm Peak Laboratory (SPL) located in the Rocky Mountains of Colorado. SPL is at an altitude of 3200 m a.s.l. within the lower free troposphere, and in winter it is a location where mixed-phase clouds frequently occur. Therefore, the present aerosol particles are directly relevant for ice formation in such clouds. The ongoing INP measurements started in October 2021, and are conducted with the Portable Ice Nucleation Experiment (PINE) at conditions resembling the formation of mixed-phase clouds at temperatures between -22°C and -32°C. Results on the short-term and inter-seasonal variability will be presented, with a focus on parallel measurements of aerosol particle properties and meteorology. During the winter months of January and February 2022, we characterized the size of the INPs by selecting ice crystal residuals downstream of PINE using a pumped-counterflow virtual impactor and a novel optical particle counter. As this setup operates continuously, it is capable to investigate INP properties for longer time periods and to improve sampling statistics. In the future, it will be used with other diagnostic instruments, such as a single particle mass spectrometer, giving insights into the size and chemical composition of INPs, and thus allows to have a direct measure of the nature of INPs in ambient air.

Although the coverage of ice-nucleating particle (INP) measurements grows more comprehensively distributed by the year, studies measuring comprehensive aerosol properties often focus extensively on one or two sites at most, and methodology between studies even within the same lab is rarely the same as methods are refined and study aims differ. This inconsistency in part contributes to a sizeable uncertainty in effective radiative forcing estimation in regard to aerosol cloud interactions. To complement our insufficient knowledge of aerosol properties, we compiled and assessed a multitude of aerosol measurements from four sites: Graciosa Island to represent a predominantly marine site (data from autumn 2020), central Oklahoma to represent a mid-latitude terrestrial site (data from autumn 2019), and Utqiagvik, Alaska (data from autumn 2021) and Ny-Ålesund, Svalbard (data from autumn 2019 and 2020) to represent Arctic sites in different longitudes.Here we report both total aerosol concentration as well as information related to two distinct aerosol concentrations: INPs and cloud concentration nuclei (CCN). INPs were measured using a single online and two offline methods, while CCN and total aerosol concentrations were measured with the same methods and similar instrumentation. This dataset can allow a broad-level comparison of several contrasting sites which would be expected to have vastly different INP and CCN activated fractions and total concentrations due to the variety in aerosol sources around the globe. Our spatial variation analysis indicates the aerosol concentrations vary by up to two orders of magnitude between sites (approximately 101 to 103 particles per cubic centimeter), while INP and CCN concentrations measured by two comparable methods vary by an order of magnitude (approximately 101 to 102 INPs per liter, and approximately 101 to 102 CCN per cubic centimeter) and INPs show much less variation than the ranges reported by previous studies. This small range may be due to similarities in INP composition, even as total aerosol population composition varies. For instance, INPs at all sites include a population of dust aerosols (either locally sourced or long-range transported). On the other hand, the total aerosol sources are more divergent between sites, especially between continental and marine-dominant sites where the greatest differentiation is seen. As well, previous studies have focused on a yearly average rather than a single season, which may also lead to greater variation. There is also variation in the heat-sensitivity of the INP samples, with continental samples from Graciosa Island showing the least heat sensitivity. Carefully comparing a large dataset containing a variety of aerosol property information including INP and CCN concentrations will allow us to determine patterns in the global distribution of aerosols that will be important as future climate models are developed.

Cirrus are high-level clouds composed uniquely of ice crystals. To correctly estimate their radiative contribution to the Earth’s energy budget, it is necessary to know their optical properties, which in turn depend on the formation mechanism. Cirrus clouds can form either by homogeneous freezing of supercooled aqueous solution droplets or by heterogeneous freezing with the contribution of an ice nucleating particle (INP). Therefore, it is fundamental to understand which aerosol particles are present in the upper troposphere and contribute to initiate heterogeneous ice nucleation.Sulphate particles are among the most abundant aerosol types in the upper troposphere, and their degree of neutralization with ammonia significantly varies with geographical location and altitude. According to the ammonium-to-sulphate ratio (ASR), three pure inorganic salts can form in the H2SO4/NH3/H2O system: ammonium bisulphate (NH4HSO4, ASR = 1), letovicite (NH4)3H(SO4)2, ASR = 1.5), and ammonium sulphate ((NH4)2SO4, ASR = 2). However, the transport, ageing and processing of atmospheric aerosols are more likely to lead to a variety of mixtures of the different salts than to particles with exact stoichiometry. The ice nucleation ability of aqueous sulphuric acid (ASR=0) and fully neutralized crystalline ammonium sulphate particles has been extensively investigated in the past. The low-temperature phase state and ice nucleation ability of partially neutralized particles, instead, has never been measured before.In this contribution, we present new AIDA cloud chamber experiments on the crystallization, deliquescence, and ice nucleation ability of partially neutralized particles in the H2SO4/NH3/H2O system (1Our results show that in the cirrus cloud temperature range, the phase state and ice nucleation ability of particles in the H2SO4/NH3/H2O system depend on their degree of neutralization. In particular, we measured an increased ice nucleation ability with increasing degree of neutralization. Quantifying the abundance and neutralization degree of ammoniated sulphate particles in the upper troposphere may thus be critical to correctly represent their direct and indirect effect on climate.

In mixed-phase clouds, primary ice formation occurs only in the presence of ice-nucleating particles (INPs) [Vali et al., 2015], which are a very rare subset of the aerosols in the atmosphere. INPs are an important part of the earth climate system, as they can initiate the formation of precipitation [Mülmenstädt et al., 2015] and have an influence on the cloud radiative properties [Murray et. al, 2021]. In the last decades, different INP measurements have been performed within the atmospheric boundary layer at mixed-phase clouds conditions [Kanji et. al, 2017]. INP measurements in the free troposphere are challenging, as they can only be conducted by aircraft-based measurements or at high altitude mountain stations. However, it is important to study long-term INP concentrations at different altitudes and geographical locations to get a better understanding of the presence of INPs in the atmosphere.The Sonnblick Observatory (SBO) in the Austrian Alps is located at an altitude of 3106 m above sea level and is an ideal location to investigate the INP concentration in the free troposphere, as the measured INPs are directly relevant for ice formation. Since August 2019, we continuously measure the INP concentration at the SBO via filter collection and offline analysis with INSEKT (Ice Nucleation Spectrometer of the Karlsruhe Institute of Technology) [Schneider et. al, 2020]. The analysis of the sampled aerosols gives us the temperature dependent number concentration of INPs at temperatures above -25°C with a time resolution of one week. In order to receive a better insight into short-term fluctuations, we performed additional measurements with the online INP measurement PINE (Portable Ice Nucleation Experiment) [Möhler et al., 2021], since the end of July 2021. PINE has a time resolution of 5 – 6 min and usually measures at a constant temperature of ~ -23°C. In addition, INP activity screenings in the range from -15°C to -30°C are performed in regular intervals and during interesting meteorological periods such as Saharan dust events. The overlap in temperature ranges of INSEKT and PINE enables a comparison between the two measuring instruments.Our results show that there are significant seasonal variations in the INP concentration. Especially during the summer time, strong diurnal variations in the INP concentration were observed, which could be explained by the influence of convectively lifted air from the boundary layer during the day. Correlations of the measured INP concentrations to meteorological parameters, aerosol properties and boundary layer stability will be discussed. In addition, we will present a case study of a dust event, which shows a sudden, strong increase in the INP concentration.

Dust particles from high latitudes have a potentially large local, regional, and global significance to climate and the environment as short-lived climate forcers, air pollutants, and nutrient sources. Identifying the locations of local dust sources and their emission, transport, and deposition processes is important for understanding the multiple impacts of high-latitude dust (HLD) on the Earth's systems. Here, we identify, describe, and quantify the source intensity (SI) values, which show the potential of soil surfaces for dust emission scaled to values 0 to 1 concerning globally best productive sources, using the Global Sand and Dust Storms Source Base Map (G-SDS-SBM). This includes 64 HLD sources in our collection for the northern (Alaska, Canada, Denmark, Greenland, Iceland, Svalbard, Sweden, and Russia) and southern (Antarctica and Patagonia) high latitudes. Activity from most of these HLD sources shows seasonal character. It is estimated that high-latitude land areas with higher (SI ≥0.5), very high (SI ≥0.7), and the highest potential (SI ≥0.9) for dust emission cover >1 670 000 km2, >560 000 km2, and >240 000 km2, respectively. In the Arctic HLD region (≥60∘ N), land area with SI ≥0.5 is 5.5 % (1 035 059 km2), area with SI ≥0.7 is 2.3 % (440 804 km2), and area with SI ≥0.9 is 1.1 % (208 701 km2). Minimum SI values in the northern HLD region are about 3 orders of magnitude smaller, indicating that the dust sources of this region greatly depend on weather conditions. Our spatial dust source distribution analysis modeling results showed evidence supporting a northern HLD belt, defined as the area north of 50∘ N, with a “transitional HLD-source area” extending at latitudes 50–58∘ N in Eurasia and 50–55∘ N in Canada and a “cold HLD-source area” including areas north of 60∘ N in Eurasia and north of 58∘ N in Canada, with currently “no dust source” area between the HLD and low-latitude dust (LLD) dust belt, except for British Columbia. Using the global atmospheric transport model SILAM, we estimated that 1.0 % of the global dust emission originated from the high-latitude regions. About 57 % of the dust deposition in snow- and ice-covered Arctic regions was from HLD sources. In the southern HLD region, soil surface conditions are favorable for dust emission during the whole year. Climate change can cause a decrease in the duration of snow cover, retreat of glaciers, and an increase in drought, heatwave intensity, and frequency, leading to the increasing frequency of topsoil conditions favorable for dust emission, which increases the probability of dust storms. Our study provides a step forward to improve the representation of HLD in models and to monitor, quantify, and assess the environmental and climate significance of HLD.

Dust particles emitted from high latitudes (≥ 50° N and ≥ 40° S, including Arctic as a subregion ≥ 60° N), have a potentially large local, regional, and global significance to climate and environment as short-lived climate forcers, air pollutants and nutrient sources. To understand the multiple impacts of the High Latitude Dust (HLD) on the Earth systems, it is foremost to identify the geographic locations and characteristics of local dust sources. Here, we identify, describe, and quantify the Source Intensity (SI) values using the Global Sand and Dust Storms Source Base Map (G-SDS-SBM), for sixty-four HLD sources included in our collection in the Northern (Alaska, Canada, Denmark, Greenland, Iceland, Svalbard, Sweden, and Russia) and Southern (Antarctica and Patagonia) high latitudes. Activity from most of these HLD dust sources show seasonal character. The environmental and climatic effects of dust on clouds and climatic feedbacks, atmospheric chemistry, marine environment, and cryosphere-atmosphere feedbacks at high latitudes are discussed, and regional-scale modelling of dust atmospheric transport from potential Arctic dust sources is demonstrated. It is estimated that high latitude land area with higher (SI ≥ 0.5), very high (SI ≥ 0.7) and the highest potential (SI ≥ 0.9) for dust emission cover >1 670 000 km2, >560 000 km2, and >240 000 km2, respectively. In the Arctic HLD region, land area with SI ≥ 0.5 is 5.5 % (1 035 059 km2), area with SI ≥ 0.7 is 2.3 % (440 804 km2), and with SI ≥ 0.9 it is 1.1 % (208 701 km2). Minimum SI values in the north HLD region are about three orders of magnitude smaller, indicating that the dust sources of this region are highly dependable on weather conditions. In the south HLD region, soil surface conditions are favourable for dust emission during the whole year. Climate change can cause decrease of snow cover duration, retrieval of glaciers, permafrost thaw, and increase of drought and heat waves intensity and frequency, which all lead to the increasing frequency of topsoil conditions favourable for dust emission and thereby increasing probability for dust storms. Our study provides a step forward to improve the representation of HLD in models and to monitor, quantify and assess the environmental and climate significance of HLD in the future.

Swabian MOSES 2021 ist eine hydro-meteorologische Messkampagne, die zwischen Mai und Oktober 2021 im Neckartal und auf der Schwäbischen Alb im Südwesten Deutschlands im Verbund von zehn deutschen wissenschaftlichen Einrichtungen und unter Beteiligung von über 30 Forschenden durchgeführt wurde. Im Fokus von Swabian MOSES 2021 stehen zwei Wetterextreme, die nicht nur für das Untersuchungsgebiet von großer Relevanz sind: Starkniederschläge durch hochreichende Konvektion (Gewitter) und Hitzewellen mit den damit verbundenen Trockenperioden. Mehrere heftige Unwetterereignisse, aber auch sogenannte "non cases", bei denen trotz guter prä-konvektiver Bedingungen keine Gewitter entstanden, lieferten einen umfangreichen Datensatz. Mit diesem lässt sich die gesamte Ereigniskette abbilden: von der Entstehung hochreichender Konvektion über die Intensivierung und den Zerfall der Gewittersysteme, die Dynamik der damit verbundenen Begleiterscheinungen (z.B. Starkregen, Hagel, Windböen) bis hin zu Abflüssen und Schadstoffeinträgen in Fließgewässern sowie zum Wasserdampftransport in die untere Stratosphäre. Eine Hitzewelle mit Dürreepisoden hat sich dagegen nicht eingestellt. Swabian MOSES 2021 ist Teil der Implementierungsphase von MOSES (Modular Observation Solutions for Earth Systems), einem Beobachtungssystem, das vom Forschungsbereich "Erde und Umwelt" der Helmholtz-Gemeinschaft entwickelt wird. Die Koordination von MOSES liegt beim Zentrum für Umweltforschung (UFZ) in Leipzig. Federführendes Institut bei Swabian MOSES 2021 ist das Institut für Meteorologie und Klimaforschung (IMK-TRO) des Karlsruher Instituts für Technologie (KIT), welches sein mobiles integriertes Atmosphärenbeobachtungssystem KITcube als größte Messinfrastruktur einbrachte. Insgesamt wurden an über 20 Standorten im Untersuchungsgebiet in situ und Fernerkundungssysteme wie z.B. Regen- und Wolkenradar, Aerosolmessgeräte, Wasserprobenahmesysteme, ein Infraschallsensor, Energiebilanz- und Eddy-Kovarianz-Stationen, Wolkenkameras, eine Station für Ballonsondierungen sowie Netzwerke aus Windlidaren, Niederschlags-, Hagel- und Bodenfeuchtesensoren von den Projektbeteiligten installiert und betrieben. Zum Messkonzept gehörten zudem die Forschungsflugzeuge D-ILAB, D-IBUF und D-CFFU, der UFZ-Rover zur Messung der Bodenfeuchte mittels Neutronensensoren und kleine Schwarmsonden, die ein Team aus "Gewitterjägern" im unmittelbaren Vorfeld von Gewittern startete. Präsentiert werden zum einen das Konzept des interdisziplinären Forschungsprojekts und die abgestimmten Messstrategien der verschiedenen beteiligten Gruppen. Zum anderen wird ein Überblick über die zugrundeliegenden wissenschaftlichen Fragestellungen und Ziele gegeben und diese anhand erster Messergebnisse veranschaulicht. Zu den Fragestellungen und Zielen, die auch die Standorte der Messgeräte bestimmten, gehören unter anderem die Rolle der topografischen Strömungsmodifikation auf die Gewitterauslösung sowie der Einfluss von Aerosolpartikeln (z.B. Saharastaub) auf die Veränderung der atmosphärischen Stabilität und die Entstehung konvektiver Zellen. Weiterhin erlaubt das dichte Messnetz die Untersuchung der Inhomogenität von Starkregen, Hagel und Bodenfeuchte bei konvektiven Ereignissen. Wie der Einsatz der teils neuartigen mobilen Messsysteme zeigt, nimmt neben den inhaltlichen hydro-meteorologischen Forschungsfragen auch die (Weiter-)Entwicklung neuer Messtechniken einen wichtigen Platz in der Messkampagne ein. Zum Abschluss wird ein Ausblick auf die geplante Folgekampagne im Jahr 2023 gegeben, an der weitere Forschungspartner teilnehmen können.

Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite of products covering a wide range of volatilities. Highly oxygenated organic molecules (HOMs) comprise a fraction of the oxidation products formed. While it is known that HOMs contribute to secondary organic aerosol (SOA) formation, including NPF, they have not been well studied in newly formed particles due to their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies of α-pinene oxidation, including in the presence of isoprene, at temperatures (−50 and −30 ∘C) and relative humidities (20 % and 60 %) relevant in the upper free troposphere. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. The particle chemical composition was analyzed by a thermal desorption differential mobility analyzer (TD-DMA) coupled to a nitrate chemical ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) mass spectrometer. CI-APi-TOF was used for particle- and gas-phase measurements, applying the same ionization and detection scheme. Our measurements revealed the presence of C8−10 monomers and C18−20 dimers as the major compounds in the particles (diameter up to ∼ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5−7) and C15 compounds (C15H24O5−10) were detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene oxidation products enhance the growth of particles larger than 15 nm. Additionally, we report on the nucleation rates measured at 1.7 nm (J1.7 nm) and compared with previous studies, we found lower J1.7 nm values, very likely due to the higher α-pinene and ozone mixing ratios used in the present study.

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

The formation of ice particles in Earth’s atmosphere strongly influences the dynamics and optical properties of clouds and their impacts on the climate system. Ice formation in clouds is often triggered heterogeneously by ice nucleating particles (INPs) that represent a very low number of particles in the atmosphere. To date, many sources of INPs, such as mineral and soil dust, have been investigated and identified in the lower latitudes. Although less is known about the sources of ice nucleation at higher latitudes, efforts have been made to identify the sources of INPs in the Arctic and boreal environments. In this study, we investigate the INP emission potential from high latitude boreal forests. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiälä, Finland between February and June 2018. The campaign utilized the infrastructure of the SMEAR II research station with additional instrumentation for measuring INPs to quantify the concentrations and sources of INPs in the boreal environment. In this contribution, we describe the measurement infrastructure and operating procedures during HyICE-2018 and we report results from specific time periods where INP instruments were run in parallel for inter-comparison purposes. Our results show that the suite of instruments deployed during HyICE-2018 reports consistent results and therefore lays the foundation for forthcoming results to be considered holistically. In addition, we compare the INP concentration we measured to INP parameterizations, and we show a very good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA.

New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN)

A porous composite of 3-dimensional (3D) reduced graphene oxide (rGO) and silica dioxide nanoparticles (PrGO-SN) was synthesized via a single-step hydrothermal process, which can initiate facile ic...

Formation of ice particles in clouds at the temperatures of −10 °C or warmer was documented by using ground-based remote sensing observations. At these temperatures, the number concentration of ice nucleating particles (INP) is not only expected to be small, but also this number is highly uncertain. In addition, there are a number of studies reporting that the observed number concentration of ice particles exceeds expected INP concentrations, indicating that other ice generation mechanisms, such as secondary ice production (SIP), may play an important role in such clouds. To identify the formation of ice crystals and report conditions in which they are generated, W-band cloud radar Doppler spectra observations collected at the Hyytiälä station for more than two years were used. Given that at these temperatures ice crystals grow mainly as columns, which have distinct linear depolarization ratio (LDR) values, spectral LDR was utilized to identify newly formed ice particles. Our results indicate that that the columnar ice production took place in 5 to 13 % of clouds, where cloud top temperatures were −12 °C or higher. For colder clouds, this percentage can be as high as 33 %. 40 ~ 50 % of columnar-ice-producing events last less than 1 hour, while 5 ~ 15 % can persist for more than 6 hours. By comparing clouds where columnar crystals were produced with the ones where these crystals were absent, we found that the columnar-ice-producing clouds tend to have larger values of liquid water path and precipitation intensity. The columnar-ice-producing clouds were subdivided into subcategories, using the temperature difference, Δ T, between the altitudes where columns are first detected and the cloud top altitude. The cases where Δ T is less than 2 °C are typically single-layer shallow clouds where needles are produced at the cloud top. In multilayered clouds, where Δ T > 2 °C, columns are produced in a layer that is seeded by ice particles falling from above. This classification allows to study potential impacts of various SIP mechanisms, such as Hallet-Mossop process or freezing breakup, on columnar ice production. To answer the question whether the observed ice particles are generated by SIP in the observed single-layer shallow clouds, ice particle number concentrations were retrieved and compared to several INP parameterizations. It was found that the ice number concentrations tend to be 1 ~ 3 orders of magnitude higher than the expected INP concentrations.

Here, we present a multi-season study of ice-nucleating particles (INPs) active via the immersion freezing mechanism, which took place in north-central Argentina, a worldwide hotspot for mesoscale convective storms. INPs were measured untreated, after heating to 95°C, and after hydrogen peroxide digestion. No seasonal cycle of INP concentrations was observed. Heat labile INPs, which we define as “biological” herein, dominated the population active at −5 to −20°C, while non-heat-labile organic INPs (decomposed by peroxide) dominated at lower temperatures, from −20 to −28°C. Inorganic INPs (remaining after peroxide digestion), were minor contributors to the overall INP activity. Biological INP concentration active around −12°C peaked during rain events and under high relative humidity, reflecting emission mechanisms independent of the background aerosol concentration. The ratio of non-heat-labile organic and inorganic INPs was generally constant, suggesting they originated from the same source, presumably from regional arable topsoil based on air mass histories. Single particle mass spectrometry showed that soil particles aerosolized from a regionally common agricultural topsoil contained known mineral INP sources (K-feldspar and illite) as well as a significant organic component. The INP activity observed in this study correlates well with agricultural soil INP activities from this and other regions of the world, suggesting that the observed INP spectra might be typical of many arable landscapes. These results demonstrate the strong influence of regional continental landscapes, emitting INPs of types that are not yet well represented in global models., Journal of Geophysical Research: Atmospheres, 126 (23), ISSN:0148-0227, ISSN:2169-897X

Homogeneous freezing of aqueous solution aerosol particles is an important process for cloud ice formation in the upper troposphere. There the air temperature is low, the ice supersaturation can be high and the concentration of ice-nucleating particles is too low to initiate and dominate cirrus cloud formation by heterogeneous ice nucleation processes. The most common description to quantify homogeneous freezing processes is based on the water activity criterion (WAC) as proposed by Koop et al. (2000). The WAC describes the homogeneous nucleation rate coefficients only as a function of the water activity, which makes this approach well applicable in numerical models. In this study, we investigate the homogeneous freezing behavior of aqueous sulfuric acid aerosol particles by means of a comprehensive collection of laboratory-based homogeneous freezing experiments conducted at the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud simulation chamber, which were conducted as part of 17 measurement campaigns since 2007. The most recent experiments were conducted during October 2020 with special emphasis on temperatures below 200 K. Aqueous sulfuric acid aerosol particles of high purity were generated by particle nucleation in a gas flow composed of clean synthetic air and sulfuric acid vapor, which was added to the AIDA chamber. The resulting chamber aerosol had number concentrations from 30 cm−3 up to several thousand per cubic centimeter with particle diameters ranging from about 30 nm to 1.1 µm. Homogeneous freezing of the aerosol particles was measured at simulated cirrus formation conditions in a wide range of temperatures between 185 and 230 K with a steady increase of relative humidity during each experiment. At temperatures between about 205 K and about 230 K, the AIDA results agree well with the WAC-based predictions of homogeneous freezing onsets. At lower temperatures, however, the AIDA results show an increasing deviation from the WAC-based predictions towards higher freezing onsets. For temperatures between 185 and 205 K, the WAC-based ice saturation ratios for homogeneous freezing onsets increase from about 1.6 to 1.7, whereas the AIDA measurements show an increase from about 1.7 to 2.0 in the same temperature range. Based on the experimental results of our direct measurements, we suggest a new fit line to formulate the onset conditions of homogeneous freezing of sulfuric acid aerosol particles as an isoline for nucleation rate coefficients between 5×108 and 1013 cm−3 s−1. The potential significant impacts of the higher homogeneous freezing thresholds, as directly observed in the AIDA experiments under simulated cirrus formation conditions, on the model prediction of cirrus cloud occurrence and related cloud radiative effects are discussed.

Ice-nucleating particles (INPs) are aerosol particles that catalyze the heterogeneous formation of ice crystals under ice supersaturation conditions. These INPs can change cloud characteristics on wide spatiotemporal scales, including albedo and radiative effects, as well as precipitation types and amounts, thus affecting both weather and climate. However, INP measurements with reasonable temporal resolution have been challenging in terms of both technology and logistics in our research community. Here we present preliminary results of our recent six-month effort from the Eastern North Atlantic (ENA) field campaign to advance the research and explore remote operation of the plug-and-play Portable Ice Nucleation Experiment (PINE) chamber to semi-autonomously measure marine boundary layer INP concentrations. In this campaign we deployed our PINE chamber at the U.S. Department of Energy Atmospheric Radiation Measurement (DOE ARM) ENA site on Graciosa Island, Azores (39° 5′ 29.76″ N, 28° 1′ 32.52″ W). The PINE chamber has been continuously operated since October 2020 with supervision and periodic remote maintenance by scientists in West Texas. The INP measurements were conducted at mixed-phase cloud conditions at temperatures between -14°C and -33°C. These measurements, along with other aerosol particle and meteorological measurements made by a suite of instruments collocated at the DOE ARM site, give unique insights on the response of INP concentrations to local and mesoscale dynamics and thermodynamic processes. This study provides the first remote and continuous INP measurements over two meteorological seasons made in the ENA region within the marine boundary layer, giving insights into an area with prominent marine influences on aerosol populations. Graciosa Island is a small island (only 61 km2) surrounded by oligotrophic oceans, and these measurements were made during the most biologically productive time of year for phytoplankton in the surrounding ocean waters. The long-term and continuous nature of these measurements allows a unique comparison of marine biological productivity, using satellite-derived chlorophyll a as a proxy for biomass, and INP concentrations. The median INP concentrations at -25 °C and -30 °C were around 4 INP L-1 and 27 INP L-1 respectively. Our preliminary data suggest that INP concentrations measured by the PINE chamber at the ENA site are comparable to other studies at locations with primarily marine INPs. More details will be offered in our presentation.

Infrared spectroscopic observations have shown that crystalline ammonium nitrate (AN) particles are an abundant constituent of the upper tropospheric aerosol layer which is formed during the Asian summer monsoon period, the so-called Asian Tropopause Aerosol Layer (ATAL). At upper tropospheric temperatures, the thermodynamically stable phase of AN is different from that at 298 K, meaning that presently available room-temperature optical constants of AN, that is, the real and imaginary parts of the complex refractive index, cannot be applied for the quantitative analysis of these infrared measurements. In this work, we have retrieved the first low-temperature data set of optical constants for crystalline AN in the 800–6000 cm−1 wavenumber range with a spectral resolution of 0.5 cm−1. The optical constants were iteratively derived from an infrared extinction spectrum of 1 µm sized AN particles suspended in a cloud chamber at 223 K. The uncertainties of the new data set were carefully assessed in a comprehensive sensitivity analysis. We show that our data accurately fit aircraft-borne infrared measurements of ammonium nitrate particles in the ATAL.

Volcanic ash (VA) from explosive eruptions contributes to aerosol loadings in the atmosphere. Aside from the negative impact of VA on air quality and aviation, these particles can alter the optical and microphysical properties of clouds by triggering ice formation, thereby influencing precipitation and climate. Depending on the volcano and eruption style, VA displays a wide range of different physical, chemical, and mineralogical properties. Here, we present a unique data set on the ice nucleation activity of 15 VA samples obtained from different volcanoes worldwide. The ice nucleation activities of these samples were studied in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud simulation chamber as well as with the Ice Nucleation Spectrometer of the Karlsruhe Institute of Technology (INSEKT). All VA particles nucleated ice in the immersion freezing mode from 263 to 238K with ice nucleation active site (INAS) densities ranging from ∼105 to 1011 m−2, respectively. The variabilities observed among the VA samples, at any given temperature, range over 3.5 orders of magnitude. The ice‐nucleating abilities of VA samples correlate to varying degrees with their bulk pyroxene and plagioclase contents as a function of temperature. We combined our new data set with existing literature data to develop an improved ice nucleation parameterization for natural VA in the immersion freezing mode. This should be useful for modeling the impact of VA on clouds., Plain Language Summary: Volcanic ash particles, which are generated during volcanic eruptions, can initiate ice formation in clouds. The clouds formed by these volcanic ash particles can influence precipitation, and in turn, weather and climate. In our study, we investigated the ability with which volcanic ash particles form ice in clouds. We performed our study in a state‐of‐the‐art aerosol and cloud simulation chamber and on a cold‐stage instrument. The findings show that volcanic ash particles can form ice as effectively as mineral dust particles or their components. These results will help scientists to have a better understanding of the impact of volcanic ash particles on clouds., Key Points: The ice‐nucleating ability of natural volcanic ash particles in the immersion freezing mode can vary by 3.5 orders of magnitude. Ice‐nucleating properties of volcanic ash particles correlate to varying degrees with their pyroxene and plagioclase contents. The temperature‐dependent immersion freezing ability of volcanic ash is approximated with an exponential fit line., Alexander von Humboldt‐Stiftung (Humboldt‐Stiftung) http://dx.doi.org/10.13039/100005156, Marie Skłodowska‐Curie Actions, ERC 2018 ADG, Deutsche Forschungsgemeinschaft (DFG) http://dx.doi.org/10.13039/501100001659, Helmholtz Association of German Research Centres, EUROCHAMP 2020 Infrastructure Activity

This study presents a comprehensive investigation of ice-nucleating particles (INPs) in the surface materials and aerosol particles from U.S. cattle feeding facilities. Using a modern suite of online and offline aerosol particle characterization instruments, we conducted a three-year field survey (2016–2019), Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber experiments, and ice crystal residual (ICR) analyses for the feedlot sample. Our results showed unique supermicron size dominance in the feedlot INPs with a high concentration of INPs (several hundred and thousand INPs L−1 at −20 °C and −25 °C, respectively). Thus, agricultural fields, especially animal feeding facilities, represent important INP sources if these particles rise to sufficient height in the atmosphere. New data on the ice nucleation (IN) properties of agricultural dust at heterogeneous freezing temperatures (Ts > −29 °C) were generated, providing statistical context. Overall, we successfully characterized physical, chemical, and biological properties of aerosol particles found at a cattle feedlot, thereby finding their unique heat-tolerant nature. The relationship between these measured properties and atmospheric IN parameterization relevant to mixed-phase clouds is discussed. Our INP parameterization and ICR characterization are meaningful for improved understanding of INP emission and cloud microphysical processes in the supermicron-particle laden region. These unique INPs may directly influence the lifetime of supercooled clouds in a unique manner for this region. An application of our IN parameterization is crucial to explore INP relations to supercooled cloud properties over such a predominant agricultural area.

We present our field results of ice-nucleating particle (INP) measurements from the commercialized version of the Portable Ice Nucleation Experiment (PINE) chamber from two different campaigns. Our first field campaign, TxTEST, was conducted at West Texas A&M University (July–August 2019), and the other campaign, ExINP-SGP, was held at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site (October–November 2019). In both campaigns, the PINE made semi-autonomous INP measurements at a high-time-resolution of 8 min for individual expansions with continuous temperature scans from −5 to −35 °C in 90 min. The PINE instrument was set to have a minimum detection capability of ~0.3 INPs per liter of air. To complement our online PINE measurements, polycarbonate filter impactor and liquid impinger samples were also collected next to the PINE. Offline droplet-freezing assays were later conducted from the filter and impinger samples for the immersion freezing mode. Our preliminary results suggested that the immersion freezing mode was the dominant ice-nucleation mechanism at the SGP site compared to the deposition mode. We did not find any statistical correlation between cloud condensation nuclei (CCN) and INP concentration during our ExINP-SGP period, suggesting that CCN activation is not a significant prerequisite for ice nucleation at the SGP site. In addition, we analyzed the relationship between various aerosol particle size ranges and INP abundance. At SGP, we found an increase in INPs with the super-micron particles, especially for diameters >2 μm across the entire heterogeneous freezing temperature range examined by PINE. Lastly, we computed a variety of INP parameters, such as, ice nucleation active surface site density, water activity-based freezing, and cumulative INP per liter of air, representing the ambient INPs in the SGP. Our field campaign results demonstrated the PINE’s ability to make remote INP measurements, promising future long-term operations including at isolated locations.

This study considers how feedlot dust size and composition contribute to atmosphericice nucleation and the formation of local cloud and precipitation in the Texas Panhandle. [...]

Ice-nucleating particles (INPs) trigger the formation of cloud ice crystals in the atmosphere. Therefore, they strongly influence cloud microphysical and optical properties and precipitation and the life cycle of clouds. Improving weather forecasting and climate projection requires an appropriate formulation of atmospheric INP concentrations. This remains challenging as the global INP distribution and variability depend on a variety of aerosol types and sources, and neither their short-Term variability nor their long-Term seasonal cycles are well covered by continuous measurements. Here, we provide the first year-long set of observations with a pronounced INP seasonal cycle in a boreal forest environment. Besides the observed seasonal cycle in INP concentrations with a minimum in wintertime and maxima in early and late summer, we also provide indications for a seasonal variation in the prevalent INP type. We show that the seasonal dependency of INP concentrations and prevalent INP types is most likely driven by the abundance of biogenic aerosol. As current parameterizations do not reproduce this variability, we suggest a new mechanistic description for boreal forest environments which considers the seasonal variation in INP concentrations. For this, we use the ambient air temperature measured close to the ground at 4.2 m height as a proxy for the season, which appears to affect the source strength of biogenic emissions and, thus, the INP abundance over the boreal forest. Furthermore, we provide new INP parameterizations based on the Ice Nucleation Active Surface Site (INAS) approach, which specifically describes the ice nucleation activity of boreal aerosols particles prevalent in different seasons. Our results characterize the boreal forest as an important but variable INP source and provide new perspectives to describe these new findings in atmospheric models. publishedVersion

We describe a new tunable diode laser (TDL) absorption instrument, the Chicago Water Isotope Spectrometer, designed for measurements of vapor-phase water isotopologues in conditions characteristic of the upper troposphere [190-235 K temperature and 2-500 parts per million volume (ppmv) water vapor]. The instrument is primarily targeted for measuring the evolving ratio of HDO/H2O during experiments in the "Aerosol Interaction and Dynamics in the Atmosphere" (AIDA) cloud chamber. The spectrometer scans absorption lines of both H2O and HDO near the 2.64 µm wavelength in a single current sweep, increasing the accuracy of isotopic ratio measurements. At AIDA, the instrument is configured with a 256-m path length White cell for in situ measurements, and effective sensitivity can be augmented by enhancing the HDO content of chamber water vapor by an order of magnitude. The instrument has participated to date in the 2012-2013 IsoCloud campaigns studying isotopic partitioning during the formation of cirrus clouds and in the AquaVIT-II instrument intercomparison campaign. Realized precisions for 1-s measurements during these campaigns were 22 ppbv for H2O and 16 ppbv for HDO, equivalent to relative precisions of less than 0.5% for each species at 8 ppmv water vapor. The 1-s precision of the [HDO]/[H2O] ratio measurement ranged from 1.6‰ to 5.6‰ over the range of experimental conditions. H2O measurements showed agreement with calculated saturation vapor pressure to within 1% in conditions of sublimating ice and agreement with other AIDA instruments (the AIDA SP-APicT reference TDL instrument and an MBW 373LX chilled mirror hygrometer) to within 2.5% and 3.8%, respectively, over conditions suitable for all instruments (temperatures from 204 K to 234 K and H2O content equivalent to 15-700 ppmv at 200 hPa).

In recent years, sea spray and the biological material it contains has received increased attention as a source of ice nucleating particles (INPs). Such INPs may play a role in remote marine regions, where other sources of INPs are scarce or absent. Marine aerosol is of diverse nature, so identifying sources of INPs is challenging. One fraction of marine bioaerosol, phytoplankton and their exudates, has been a particular focus of marine INP research. In our study we attempt to address three main questions. Firstly, we compare the ice nucleating ability of two common phytoplankton species with Arctic seawater microlayer samples using the same instrumentation to see if these phytoplankton species produce ice nucleating material with sufficient activity to account for the ice nucleation observed in Arctic microlayer samples. We present first measurements of the ice nucleating ability of two predominant phytoplankton species, Melosira arctica, a common Arctic diatom species and Skeletonema marinoi, a ubiquitous diatom species across oceans worldwide. To determine the potential effect of nutrient conditions and characteristics of the algal culture, such as the amount of organic carbon associated with algal cells, on the ice nucleation activity, the Skeletonema marinoi was grown under different nutrient regimes. From comparison of the ice nucleation data of the algal cultures to those obtained from a range of sea surface microlayer (SML) samples obtained during three different field expeditions to the Arctic (ACCACIA, NETCARE, ASCOS) we found that although these diatoms do produce ice nucleating material, they were not as ice active as the investigated microlayer samples. Secondly, to improve our understanding of local Arctic marine sources as atmospheric INP we applied several aerosolisation techniques to analyse the ice nucleating ability of aerosolised microlayer and algae samples. The aerosols were generated either by direct nebulisation of the undiluted bulk solutions, or by the addition of the samples to a sea spray simulation chamber filled with artificial seawater. The latter method generates aerosol particles using a plunging jet to mimic the process of oceanic wave-breaking. We observed that the aerosols produced using this approach can be ice active indicating that the ice nucleating material in seawater can indeed transfer to the aerosol phase. Thirdly, we attempted to measure ice nucleation activity across the entire temperature range relevant for mixed-phase clouds using a suite of ice nucleation measurement techniques- an expansion cloud chamber, a continuous flow diffusion chamber, and a cold stage. In order to compare the measurements made using the different instruments, we have normalised the data in relation to the mass of salt present in the nascent sea spray aerosol. At temperatures above 248 K some of the SML samples were very effective at nucleating ice, but there was substantial variability between the different samples. In contrast, there was much less variability between samples below 248 K.