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This study develops an advanced physically‐based parameterization of heterogeneous ice nucleation in cirrus clouds that includes an updated parameterization of stochastic homogeneous freezing of supercooled solution droplets. Both components are formulated based on the same methodology and level of approximation, without numerical integration of the underlying ice supersaturation equation. The new scheme includes measured ice nucleation spectra describing deterministic ice activation from an arbitrary number of types of ice‐nucleating particles (INPs), tracks the competition for available water vapor between the different ice nucleation modes, and allows for new ice formation and growth within pre‐existing cirrus clouds. The computationally efficient scheme works with a minimal set of physical input parameters and predicts total nucleated ice crystal number concentrations (ICNCs) along with the maximum ice supersaturation attained during cirrus formation events. Aspects of its implementation into host models are discussed, including the provision of suitably parameterized vertical wind speeds. The parameterization is validated by comparisons to numerical simulations. First off‐line applications to mineral dust and aviation soot particles are presented, including ICNC ensemble statistics resulting from the coupling with statistics of updraft speed variability., Plain Language Summary: Two decades after introduction of the first parameterization of cirrus cloud formation by freezing of ubiquitous liquid solution droplets, an improved version is developed based on the latest experimental findings regarding solid ice‐nucleating particles, a small subset of the atmospheric aerosol. The new scheme allows to predict ice crystal formation in cirrus from competing homogeneous freezing and heterogeneous ice activation more realistically and with greater computational efficiency. It considers new developments regarding the properties of vertical wind speeds (triggering ice formation) and the molecular kinetics of water vapor uptake onto ice crystals (controlling ice growth). This study explains the foundation of cirrus ice formation and growth based on cloud physical theory, derives and explains the parameterization, discusses its use in host models to facilitate applications, checks its performance by comparison to comprehensive numerical simulations, and presents first results involving mineral dust and aircraft‐emitted soot particles as examples for good and poor atmospheric ice‐nucleating particles, respectively., Key Points: Competing ice nucleation processes in cirrus are predicted reliably and efficiently. Partial activation of dust particles may occur frequently in cirrus formation. Nucleation of ice within already‐existing cirrus requires high updraft speeds.

Among the different aerosol mineral particles that contribute to induce ice nucleation (IN) in the troposphere, feldspars have been identified as the most active. Nevertheless, which surface properties make some feldspars more efficient than others, i.e. able to induce IN at higher temperatures, is still unclear. In addition to that, surface properties of such materials can change as they are exposed to a variety of environmental conditions while traveling through the troposphere. Here, freezing temperature of water droplets deposited on feldspar minerals has been measured as a function of consecutive freeze-thaw cycles. We found an increase of the freezing temperature for the initial cycles followed by approximately constant freezing temperature for consecutive cycles. We call this a "history effect". This effect is more evident for samples aged in standard room conditions and it disappears if the sample is exposed to oxygen plasma. Oxygen plasma generates OH groups at the surface, facilitating IN and cleans the surface from organic contamination, unblocking pores at the surface, believed to be the most active IN sites on feldspars. A similar process is suggested to happen during the history effect, when consecutive freeze-thaw events unblock IN sites., The authors thank C. Marcolli for discussion on results and their interpretation. This work has been supported by the Spanish Government under the project PID2019-110907GB-I00 and the ‘‘Severo Ochoa’’ Program for Centres of Excellence in R&D (CEX2019-000917-S). E. Pach acknowledges the Spanish Ministry of Science and Technology for the Juan de la Cierva Formation grant., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).

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.

Atmospheric ice nucleating aerosol particles (INPs) can influence the climate system by modifying cloud properties and consequently the Earth’s radiation budget. However, these aerosol-cloud interactions and their effects on the global scale, especially regarding cirrus clouds, are still only poorly understood, and subject to large uncertainties. In this thesis INP-induced modifications of cirrus clouds are analysed by employing the atmospheric chemistry general circulation model EMAC, including the aerosol microphysics submodel MADE3. To facilitate the analysis of INP-effects, model improvements and developments with respect to the representation of ice nucleating particles are applied. Besides mineral dust and soot aerosols, additional types of INPs are implemented, i.e. crystalline ammonium sulfate and glassy organic particles. A global climatology of the different INP-types is presented and global effects on cirrus coud properties and the radiative balance are quantified. Sensitivities with respect to the freezing efficiency of INPs, to the vertical velocities during cloud formation, and the effects of anthropogenic INPs are analysed., Eisbildende Aerosolpartikel in der globalen Atmosphäre, auch Eiskerne genannt, können durch Beeinflussung von Wolkeneigenschaften und damit verbundenen Modifikationen des Strahlungshaushaltes wichtige Klimaänderungen bewirken. Aerosol-Wolken-Wechselwirkungen, besonders im Hinblick auf Zirruswolken, sind allerdings mit großen Unsicherheiten behaftet. In dieser Dissertation werden Eiskern-Effekte auf Zirruswolken und Strahlung mithilfe des globalen Klima-Chemie Modells EMAC analysiert, welches das Aerosol-Mikrophysik Modul MADE3 beinhaltet. Zur Analyse der globalen Eiskerneffekte wird die Modelldarstellung eisbildender Aerosole weiterentwickelt und, neben Mineralstaub und Ruß, um zusätzliche Eiskerntypen erweitert: kristallines Ammoniumsulfat und hochviskose organische Partikel. Eine globale Klimatologie der verschiedenen Eiskern-Typen wird präsentiert und globale Effekte auf Zirruswolken-Eigenschaften und Strahlungsbilanz werden quantifiziert. Sensitivitäten im Hinblick auf die Gefriereigenschaften der Eiskerne, die Vertikalgeschwindigkeiten während der Wolkenbildung und die Effekte anthropogener Eiskerne werden analysiert.

Ice-nucleating particles (INPs) have a large impact on the climate-relevant properties of clouds over the oceans. Studies have shown that sea spray aerosols (SSAs), produced upon bursting of bubbles at the ocean surface, can be an important source of marine INPs, particularly during periods of enhanced biological productivity. Recent mesocosm experiments using natural seawater spiked with nutrients have revealed that marine INPs are derived from two separate classes of organic matter in SSAs. Despite this finding, existing parameterizations for marine INP abundance are based solely on single variables such as SSA organic carbon (OC) or SSA surface area, which may mask specific trends in the separate classes of INP. The goal of this paper is to improve the understanding of the connection between ocean biology and marine INP abundance by reporting results from a field study and proposing a new parameterization of marine INPs that accounts for the two associated classes of organic matter. The PEACETIME cruise took place from 10 May to 10 June 2017 in the Mediterranean Sea. Throughout the cruise, INP concentrations in the surface microlayer r (INPSML) and in SSAs (INPSSA) produced using a plunging aquarium apparatus were continuously monitored while surface seawater (SSW) and SML biological properties were measured in parallel. The organic content of artificially generated SSAs was also evaluated. INPSML concentrations were found to be lower than those reported in the literature, presumably due to the oligotrophic nature of the Mediter ranean Sea. A dust wet deposition event that occurred during the cruise increased the INP concentrations measured in the SML by an order of magnitude, in line with increases in iron in the SML and bacterial abundances. Increases in INPSSA were not observed until after a delay of 3 days compared to increases in the SML and are likely a result of a strong in fluence of bulk SSW INPs for the temperatures investigated (T =-18 °C for SSAs, T =-15 °C for SSW). Results con firmed that INPSSA are divided into two classes depending on their associated organic matter. Here we find that warm (T >=-22 °C) INPSSA concentrations are correlated with water soluble organic matter (WSOC) in the SSAs, but also with SSW parameters (particulate organic carbon, POCSSW and INPSSW,-16C) while cold INPSSA (T

Secondary ice production via rime-splintering is considered to be an important process for rapid glaciation and high ice crystal numbers observed in mixed-phase convective clouds. An open question is how rime-splintering is triggered in the relatively short time between cloud formation and observations of high ice crystal numbers. We use idealised simulations of a deep convective cloud system to investigate the thermodynamic and cloud microphysical evolution of air parcels, in which the model predicts secondary ice formation. The Lagrangian analysis suggests that the &ldquo, in-situ&rdquo, formation of rimers either by growth of primary ice or rain freezing does not play a major role in triggering secondary ice formation. Instead, rimers are predominantly imported into air parcels through sedimentation form higher altitudes. While ice nucleating particles (INPs) initiating heterogeneous freezing of cloud droplets at temperatures warmer than &minus, 10 ∘ C have no discernible impact of the occurrence of secondary ice formation, in a scenario with rain freezing secondary ice production is initiated slightly earlier in the cloud evolution and at slightly different places, although with no major impact on the abundance or spatial distribution of secondary ice in the cloud as a whole. These results suggest that for interpreting and analysing observational data and model experiments regarding cloud glaciation and ice formation it is vital to consider the complex vertical coupling of cloud microphysical processes in deep convective clouds via three-dimensional transport and sedimentation.

Glaciation in mixed-phase clouds predominantly occurs through the immersion-freezing mode where ice-nucleating particles (INPs) immersed within supercooled droplets induce the nucleation of ice. Model representations of this process currently are a large source of uncertainty in simulating cloud radiative properties, so to constrain these estimates, continuous-flow diffusion chamber (CFDC)-style INP devices are commonly used to assess the immersion-freezing efficiencies of INPs. This study explored a new approach to operating such an ice chamber that provides maximum activation of particles without droplet breakthrough and correction factor ambiguity to obtain high-quality INP measurements in a manner that previously had not been demonstrated to be possible. The conditioning section of the chamber was maintained at −20 ∘C and water relative humidity (RHw) conditions of 113 % to maximize the droplet activation, and the droplets were supercooled with an independently temperature-controlled nucleation section at a steady cooling rate (0.5 ∘C min−1) to induce the freezing of droplets and evaporation of unfrozen droplets. The performance of the modified compact ice chamber (MCIC) was evaluated using four INP species: K-feldspar, illite-NX, Argentinian soil dust, and airborne soil dusts from an arable region that had shown ice nucleation over a wide span of supercooled temperatures. Dry-dispersed and size-selected K-feldspar particles were generated in the laboratory. Illite-NX and soil dust particles were sampled during the second phase of the Fifth International Ice Nucleation Workshop (FIN-02) campaign, and airborne soil dust particles were sampled from an ambient aerosol inlet. The measured ice nucleation efficiencies of model aerosols that had a surface active site density (ns) metric were higher but mostly agreed within 1 order of magnitude compared to results reported in the literature.

Heterogeneous ice nucleation in the atmosphere is not fully understood. In particular, our knowledge of biological materials and their atmospheric ice nucleation properties remains scarce. Here, we present the results from systematic investigations of the ice nucleation activity of plant materials using cryo-microscopy. We examined berry juices, frozen berries, as well as extracts of leaves and dried berries of plants native to boreal regions. All of our samples possess reasonable ice nucleation activity. Their ice nucleating particle concentrations per unit of water volume vary between 9.7 &times, 105 and 9.2 &times, 109 cm&minus, 3 when examined within temperatures of &minus, 12 to &minus, 34 &deg, C. Mean freezing temperatures ranged from &minus, 18.5 to &minus, 45.6 &deg, C. We show that all samples contained ice nuclei in a size range below 0.2 &micro, m and remain active if separated from coarse plant tissue. The results of examining ice nucleation properties of leaves and dry berry extracts suggests that their ice-nucleating components can be easily suspended in water. Sea buckthorn and black currant were analyzed using subtilisin (a protease) and urea. Results suggest proteinaceous compounds to play an important role in their ice nucleation activity. These results show that separation between ice nucleation particles stemming from microorganisms and those stemming from plants cannot be differentiated solely on proteinaceous features. Further oxidation experiments with ozone showed that black currant is highly stable towards ozone oxidation, indicating a long atmospheric life time.

Sea spray aerosol (SSA) generated by bubble bursting at the ocean surface is an important component of aerosol-cloud interactions over remote oceans, providing the atmosphere with ice-nucleating particles (INPs) or particles required for heterogeneous ice nucleation. Studies have shown that organic INPs are emitted during phytoplankton blooms, but changes in INP number concentrations (nINPs) due to ocean biological activity have not been directly demonstrated in natural SSA. In this study, a clean sector sampler was used to differentiate ice nucleation and composition of pristine SSA from terrestrial aerosol at the Mace Head Research Station in August 2015. Average nINPs active at −15 °C (nINPs,−15 °C) were 0.0011 L−1, and large variability (up to a factor of 200) was observed for INPs active warmer than −22 °C. Highest nINPs in the clean sector occurred during a period of elevated marine organic aerosol from offshore biological activity (M1, nINPs,−15 °C = 0.0077 L−1). A peak in nINPs was also observed in terrestrial organic aerosol (T1, nINPs,−15 °C = 0.0076 L−1). The impacts of heating and hydrogen peroxide digestion on nINPs indicate that INPs at Mace Head Research Station were largely organic and that INPs observed during M1 and T1 were biological (i.e., protein containing). Complexities of predicting increases in nINPs due to offshore biological activity are explored. A parameterization for pristine SSA INPs over the North Atlantic Ocean was developed, illustrating that SSA is associated with a factor of 1,000 fewer ice-nucleating sites per surface area of aerosol compared to mineral dust. ©2018. American Geophysical Union. All Rights Reserved.

15 pages, 2 figures, The cryosphere, which comprises a large portion of Earth’s surface, is rapidly changing as a consequence of global climate change. Ice, snow, and frozen ground in the polar and alpine regions of the planet are known to directly impact atmospheric composition, which for example is observed in the large influence of ice and snow on polar boundary layer chemistry. Atmospheric inputs to the cryosphere, including aerosols, nutrients, and contaminants, are also changing in the anthropocene thus driving cryosphere-atmosphere feedbacks whose understanding is crucial for understanding future climate. Here, we present the Cryosphere and ATmospheric Chemistry initiative (CATCH) which is focused on developing new multidisciplinary research approaches studying interactions of chemistry, biology, and physics within the coupled cryosphere – atmosphere system and their sensitivity to environmental change. We identify four key science areas: (1) micro-scale processes in snow and ice, (2) the coupled cryosphere-atmosphere system, (3) cryospheric change and feedbacks, and (4) improved decisions and stakeholder engagement. To pursue these goals CATCH will foster an international, multidisciplinary research community, shed light on new research needs, support the acquisition of new knowledge, train the next generation of leading scientists, and establish interactions between the science community and society, CATCH is sponsored by the International Global Atmospheric Chemistry (IGAC) project igacproject.org, the International Surface Ocean – Lower Atmosphere Study (SOLAS) project solas-int.org, and the International Arctic Science Committee (IASC, iasc.info). Support for CATCH activities has been provided by the French Chantier Arctique Project Pollution in the Arctic System (PARCS). This work was supported by the H2020 ERA-PLANET (689443) iCUPE project

The Arctic is warming at more than twice the rate of the global average. This warming is influenced by clouds, which modulate the solar and terrestrial radiative fluxes and, thus, determine the surface energy budget. However, the interactions among clouds, aerosols, and radiative fluxes in the Arctic are still poorly understood. To address these uncertainties, the Ny-angstrom lesund Aerosol Cloud Experiment (NASCENT) study was conducted from September 2019 to August 2020 in Ny-angstrom lesund, Svalbard. The campaign's primary goal was to elucidate the life cycle of aerosols in the Arctic and to determine how they modulate cloud properties throughout the year. In situ and remote sensing observations were taken on the ground at sea level, at a mountaintop station, and with a tethered balloon system. An overview of the meteorological and the main aerosol seasonality encountered during the NASCENT year is introduced, followed by a presentation of first scientific highlights. In particular, we present new findings on aerosol physicochemical and molecular properties. Further, the role of cloud droplet activation and ice crystal nucleation in the formation and persistence of mixed-phase clouds, and the occurrence of secondary ice processes, are discussed and compared to the representation of cloud processes within the regional Weather Research and Forecasting Model. The paper concludes with research questions that are to be addressed in upcoming NASCENT publications.