Mixed-phase clouds at high latitudes contribute to the uncertainty in predicting cloud feedbacks and climate sensitivity, mainly due to the complexity of microphysical processes that influence the partitioning between the supercooled liquid and ice phases, and hence, cloud radiative effects on regional scales. Particularly in Arctic mixed-phase clouds, the activation of ice-nucleating particles (INPs) from various aerosol populations remains a leading source of uncertainty. We developed an aerosol-cloud one-dimensional (AC-1D) model, which provides a novel framework to prognostically treat INP and ice crystal budgets while explicitly accounting for polydisperse and multicomponent aerosol that activate INPs following different freezing parameterizations. The AC-1D model is informed by large-eddy simulations to probe the impact of INP representation on predicted ice crystal number concentrations (Ni) and ice crystal budgets in mixed-phase Arctic stratus. We apply three immersion freezing (IMF) parameterizations, two time-independent (singular) and one time-dependent (classical nucleation theory), to predict the evolution of the INP reservoir and resulting ice crystal budget from polydisperse mineral dust, organic (humic-like substances), and sea spray aerosol particle size distributions. Our analysis focuses on how variations in aerosol number concentration and cloud system parameters such as cloud cooling rate, cloud-top entrainment rate, and ice crystal fall speed influence the INP reservoir and ice crystal budgets. Furthermore, this study investigates the competitive ice nucleation dynamics in mixed aerosol environments and provides a process-level quantification of the INP budget terms, which directly controls ice crystal budgets. For all studied case scenarios, the aerosol types and associated particle size distributions significantly impact INP and Ni, and the choice between a time-dependent and a singular freezing description yields orders-of-magnitude differences in the predicted INP and Ni over the 10 h simulation time, reflecting typical cloud lifetimes. Our results show that the influence of cloud cooling, INP entrainment, and sedimentation varies significantly depending on the chosen freezing parameterization. These findings underscore the critical need for robust IMF parameterizations and precise cloud system observations to enhance the accuracy of models in predicting mixed-phase cloud structure and evolution.

Immersion freezing, initiated by ice-nucleating particles (INPs) in supercooled aqueous droplets, plays an important role in the formation of ice crystals within clouds. The efficiency of immersion freezing depends strongly on INP composition and, crucially, on the mixing state - how chemical species are distributed across the particle population. Here, we quantify the impact of aerosol mixing state on immersion freezing using a combined theoretical and particle-resolved modeling approach. We derive analytical expressions for the frozen fraction of internally and externally mixed INP populations based on classical nucleation theory, showing that the frozen fraction is sensitive to whether ice-active species are present in all particles or only in a subset of the population. We introduce a multi-species immersion freezing scheme into the particle-resolved model PartMC, using the water activity-based immersion freezing model (ABIFM) to compute freezing probabilities for mixed-composition particles. To improve computational efficiency, we implement a Binned Tau-Leaping algorithm and demonstrate an order-of-magnitude speedup with minimal accuracy loss. Simulations reproduce the analytical trends in limiting cases and extend the analysis to more general aerosol populations, where mixing state continues to exert a substantial control on frozen fraction. Sensitivity analyses across particle size, species type, and cooling condition reveal that the mixing state effect is most pronounced when small amounts of highly efficient INPs are mixed with less efficient materials. These findings underscore the need to represent aerosol mixing state explicitly in models of heterogeneous ice nucleation to reduce uncertainty in cloud-phase partitioning.

The potential impact of wildfire smoke on Arctic cirrus formation is discussed based on lidar and radar observations during the winter half year of the 1-year MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition. Aerosol and ice cloud observations were performed aboard the icebreaker Polarstern at latitudes > 85° N. Aged Siberian wildfire smoke polluted the tropopause region over the central Arctic during the entire winter half year of 2019–2020. The smoke particle surface area concentration at the tropopause was of the order of 5–15 µm2 cm−3 and indicated considerably enhanced levels of aerosol pollution for more than 6 months. Numerous cirrus systems with cloud-top temperatures between −60 and −75 °C developed in the polluted upper troposphere. We analyzed all MOSAiC winter cirrus layers with respect to their geometrical and optical properties and a subgroup of 20 cirrus events with respect to their ice water content (IWC) and ice crystal number concentration (ICNC). In individual ice fallstreaks that are connected to individual ice nucleation events, ICNCs typically ranged from 1 to 10 crystals L−1 but were frequently also as high as 20–50 L−1; however, observations > 100 L−1 were rare. Three observational facts corroborate our hypothesis that smoke significantly influenced Arctic cirrus formation: (1) the occurrence of a long-lasting, persistent smoke pollution layer in the upper troposphere so that favorable conditions for heterogeneous ice nucleation on smoke particles were always given and, at the same time, homogeneous freezing of background aerosol was probably widely suppressed; (2) the high smoke particle surface area concentrations, which were high enough to significantly trigger ice nucleation on smoke particles (as shown in Part 2, the companion paper to this article; Ansmann et al., 2025); and (3) the frequently found maximum cirrus ice saturation ratios of 1.3–1.5, which point to the dominance of heterogeneous ice nucleation processes, initiated by inefficient ice-nucleating particles (INPs), as expected when aged smoke particles (i.e., organic aerosol particles) serve as INPs. The studies are continued in the simulation portion of this work (Part 2; Ansmann et al., 2025).

A simulation study of the potential impact of wildfire smoke on Arctic cirrus formation is presented. The simulations complement the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) field observations, discussed in Part 1 (Ansmann et al., 2025) of this work. The observations suggest that Siberian wildfire smoke had a strong impact on Arctic cirrus formation in the winter of 2019–2020. Via simulations, a detailed insight into the potential of wildfire smoke to influence Arctic cirrus formation as a function of observed meteorological and environmental conditions (temperature, relative humidity, large-scale and gravity-wave-induced lofting conditions, and ice-nucleating particle (INP) concentration) is provided. Lidar-derived values of the INP concentration serve as input, and ice crystal number concentration (ICNC) values retrieved from combined lidar–radar observations are used for comparison with the simulation results. The simulations show that the observed smoke pollution levels in the upper troposphere were high enough to trigger strong ice nucleation. The simulations also corroborate the hypothesis stated in Part 1 (Ansmann et al., 2025): the persistent smoke layer, continuously observed over the central Arctic during the winter half year 2019–2020, was able to widely suppress homogeneous freezing so that the smoke aerosol most probably controlled cirrus formation and properties. The observations suggest that the INP reservoir was continuously refilled from the lower stratosphere. Furthermore, the simulations confirm that the observed high ice saturation ratios of 1.3–1.5 over the North Pole region at cirrus tops (with top temperatures of −60 to −75 °C) point to inefficient INPs, as expected when wildfire smoke particles (organic particles) serve as INPs. Finally, the simulations revealed that ice nucleation in widespread and frequently occurring shallow updrafts (with low amplitudes) seems to be responsible for the observed low ICNC values of typically 1–50 crystals L−1 in the Arctic cirrus virga.

Vertically resolved observations of the temporal evolution of mixed-phase clouds (MPCs) were performed over the central Arctic during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition, which lasted from October 2019 to September 2020. The research icebreaker Polarstern, drifting with the pack ice for more than 7 months, mostly at latitudes > 85 degrees N, served as a platform for state-of-the-art remote sensing of aerosols and clouds. The use of the recently introduced dual field-of-view (FOV) polarization lidar technique in combination with the well-established lidar-radar retrieval technique provided, for the first time, a robust instrumental basis to monitor the evolution of the liquid and the ice phase of MPCs and the interplay between the two phases. Two long-lasting Arctic MPC events observed close to the North Pole in mid-winter (December 2019) and late summer (September 2020) are discussed to provide new insight into Arctic MPC evolution processes. In the second part of the article, cloud statistics, covering all seasons of a year, are presented. The focus is on the optical and microphysical properties of the liquid phase. These results are solely derived from the dual-FOV lidar observations. The key findings of the study can be summarized as follows: persistent activation of aerosol particles to form water droplets is of great importance for the longevity of MPCs. The observations confirm that ice formation occurs predominantly via immersion freezing. The field studies suggest that the free tropospheric reservoirs of cloud condensation nuclei (CCN) and of ice-nucleating particles (INPs) were always well filled, i.e., the clouds did not exhaust their supply of activatable and activated particles. The observation of long-lasting MPC events, low ice production rates, and a sufficiently large INP reservoir leads to the recommendation to use a time-dependent immersion freezing parameterization in MPC modeling efforts.

Cloud droplets containing immersed ice-nucleating particles (INPs) may freeze at temperatures above the homogeneous freezing threshold temperature in a process referred to as immersion freezing. In modeling studies, immersion freezing is often described using either so-called "singular" or "time-dependent" parameterizations. Here, we compare both approaches and discuss them in the context of probabilistic particle-based (super-droplet) cloud microphysics modeling. First, using a box model, we contrast how both parameterizations respond to idealized ambient cooling rate profiles and quantify the impact of the polydispersity of the immersed surface spectrum on the frozen fraction evolution. Presented simulations highlight that the singular approach, constituting a time-integrated form of a more general time-dependent approach, is only accurate under a limited range of ambient cooling rates. The time-dependent approach is free from this limitation. Second, using a prescribed-flow two-dimensional cloud model, we illustrate the macroscopic differences in the evolution in time of ice particle concentrations in simulations with flow regimes relevant to ambient cloud conditions. The flow-coupled aerosol-budget-resolving simulations highlight the benefits and challenges of modeling cloud condensation nuclei activation and immersion freezing on insoluble ice nuclei with super-particle methods. The challenges stem, on the one hand, from heterogeneous ice nucleation being contingent on the presence of relatively sparse immersed INPs, and on the other hand, from the need to represent a vast population of particles with relatively few so-called super particles (each representing a multiplicity of real particles). We discuss the critical role of the sampling strategy for particle attributes, including the INP size, the freezing temperature (for singular scheme) and the multiplicity.

Abstract. A simulation study on the impact of wildfire smoke (aged organic aerosol particles) on cirrus formation in the central Arctic is presented. The simulations in this part 2 of a series of two articles complement the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) field observations, presented and discussed in part 1. The measurements were performed with lidar and radar aboard the ice breaker Polarstern at latitudes > 85° N during the winter half year 2019–2020. Main goal of the MOSAiC data analysis in part 1 was to gather a consistent set of indications for an impact of the observed aged Siberian wildfire smoke on the formation of embedded ice clouds. The combination of (a) mostly low ice crystal number concentration (ICNC) of 0.1–10 L−1 in almost all of the observed cirrus cloud virga, pointing to heterogeneous ice nucleation, (b) typically high ice saturation ratios in the upper part of the analyzed cirrus systems of around 1.3–1.4, and (c) significantly enhanced levels of smoke pollution characterized by particle surface area concentrations of the order of 5–15 µm2 cm−3 corroborate our hypothesis that wildfire smoke particles served as ice nucleating particles (INPs) in Arctic cirrus with typical cloud top temperatures of −60 to −75 °C. The observed high ice saturation ratios suggest relatively inefficient ice-active aerosol particles, as expected in the case of wildfire smoke. Main goal of the simulations in part 2 is to gain a deeper insight into the potential smoke influence on cirrus formation as a function of aerosol and meteorological conditions (temperature, relative humidity) and by considering realistic gravity wave characteristics (updraft speed, wave amplitude). The modeling effort uses lidar-derived values of INP number concentration as input and ICNC values retrieved from combined lidar-radar observations for comparison with the simulation results. The model allows us to simulate adiabatic lofting of air parcels triggered by gravity waves, nucleation of ice crystals on smoke particles (deposition ice nucleation), homogeneous freezing of background aerosol particles, the growth of the nucleated ice particles by deposition of water vapor on the crystals, and sedimentation effects. Observations of meteorological state parameters (temperature, relative humidity) with four radiosondes per day and of the aerosol and cirrus properties from continuous lidar and radar profiling permitted a realistic model-based investigation of the smoke influence on Arctic cirrus evolution. The simulations confirm that the smoke INPs were able to suppress homogeneous freezing of background aerosol particles and to trigger ice nucleation at high ice saturation ratios of 1.3–1.5 over the North Pole region at cirrus top temperatures mostly < −60 °C. The simulations further reveal that shallow gravity waves with amplitudes of the order of < 100 m and the comparably low ice nucleation efficiency of the smoke INPs provided favorable conditions for the evolution of thin ice clouds with low ICNC as observed.

The prediction of how ice crystals form represents one of the great conundrums in the atmospheric sciences with important implications for the hydrological cycle and climate. Ice-nucleating particles (INPs), typically consisting of sub-and supermicrometer-sized aerosol particles which can be inorganic, organic, biogenic, or biological, initiate heterogeneous ice nucleation processes leading to ice crystal formation. Heterogeneous ice nucleation commences on the nanoscale at the substrate surface and depends on ambient temperature and humidity. Microanalysis techniques are uniquely suited to examine the physicochemical features of the INPs under relevant atmospheric conditions thereby advancing our understanding of the principal processes that promote ice nucleation. In the atmosphere ice crystals experience growth and sublimation resulting in complex microscopic morphologies which, in turn, impact the ice crystal’s properties. This chapter provides an overview of microanalysis techniques employed in either a multimodal or in situ manner, which shed light on the atmospheric heterogeneous ice nucleation process and how these techniques are applied to explore the complex morphologies of ice crystals. The first section introduces the various atmospheric ice nucleation pathways, provides a brief outline of the underlying nucleation theory demonstrating that nucleation proceeds on the nanoscale, and describes the different ice crystal habits of growth. Section two provides an overview of the microanalysis techniques and experiments to study INPs or ice-nucleating substrates including multimodal instrument approaches followed by in situ ice nucleation studies. Examples of techniques include Raman, atomic force, electron, and X-ray microscopy with discussion of the techniques’ unique capabilities to examine the physical and chemical properties of the ice-nucleating substrate. The third section presents electron microscopy studies of ice crystals during growth and sublimation displaying the morphological complexities of ice crystals. Lastly, section four discusses typical experimental requirements including sample sizes, radiation effects, and the role of standard INPs.

Adsorption and desorption of gases on liquid or solid substrates are involved in multiphase processes and heterogeneous chemical reactions. The desorption energy ( E des 0 ), which depends on the intermolecular forces between adsorbate and substrate, determines the residence time of chemical species at interfaces. We show how E des 0 and temperature influence the net uptake or release of gas species, the rates of surface-bulk exchange and surface or bulk reactions, and the equilibration timescales of gas-particle partitioning. Using literature data, we derive a parameterization to estimate E des 0 for a wide range of chemical species based on the molecular mass, polarizability, and oxygen-to-carbon ratio of the desorbing species independent of substrate-specific properties, which is possible because of the dominant role of the desorbing species' properties. Correlations between E des 0 and the enthalpies of vaporization and solvation are rooted in molecular interactions. The relation between E des 0 and desorption kinetics reflects the key role of interfacial exchange in multiphase processes. For small molecules and semi-volatile organics (VOC, IVOC, SVOC), E des 0 values around 10-100 kJ mol - 1 correspond to desorption lifetimes around nanoseconds to days at room temperature. Even higher values up to years are obtained at low temperatures and for low volatile organic compounds (LVOC, ELVOC/ULVOC) relevant for secondary organic aerosols (SOA). Implications are discussed for SOA formation, gas-particle partitioning, organic phase changes, and indoor surface chemistry. We expect these insights to advance the mechanistic and kinetic understanding of multiphase processes in atmospheric and environmental physical chemistry, aerosol science, materials science, and chemical engineering.

Abstract. The number of wildfire smoke layers in the upper troposphere per fire season increased at mid and high northern latitudes during the last years. To consider smoke in weather and climate models appropriately, the influence of smoke on a variety of atmospheric processes needs to be explored in detail. In this study, we focus on the potential impact of wildfire smoke on cirrus formation. For the first time, state-of-the-art aerosol and cirrus observations with lidar and radar, presented in part 1 of a series of two articles, are closely linked to comprehensive modeling of gravity-wave-induced ice nucleation in cirrus evolution processes, presented in part 2. The complex study is based on aerosol and ice cloud observations in the central Arctic during the one-year MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition. For almost a year (from the summer of 2019 to the spring of 2020), aged Siberian wildfire smoke polluted the tropopause region over the central Arctic and many cirrus systems developed in the polluted upper troposphere. Goal of the data analysis (part 1) is to provide observational evidence for a dominating impact of aged wildfire smoke (organic aerosol particles) on cirrus formation in the central Arctic (over the MOSAiC research icebreaker Polarstern) during the winter half year of 2019–2020. Aim of the simulations in part 2 is to gain a deeper and more detailed insight into the potential smoke impact on ice nucleation as a function of observed aerosol and meteorological conditions (temperature, relative humidity) and by considering realistic gravity wave characteristics (updraft speed, wave amplitude). Vertical movements of air parcels are essential to initiate cloud formation. The measurements presented in part 1 were conducted during the winter half year (October to March), aboard the ice breaker Polarstern. The research vessel Polarstern drifted with the pack ice in the central Arctic mainly at latitudes >85 °N during the winter half year. The cirrus statistics show typical properties of ice clouds of the synoptic cirrus category (top-down generation of cirrus structures). The ice clouds mostly started to evolve at heights close to the tropopause. Cirrus top temperatures accumulated between −60 and −75 °C. The cirrus optical thickness (COT at 532 nm) of the ice clouds covered a wide range of values from < 0.03 (subvisible cirrus fraction, 25 % out of all cases) over 0.03–0.3 (visible thin cirrus, 40 %) to > 0.3 (opaque cirrus fraction, 35 %). In about 30 % out of all high altitude lidar observations, cirrus signatures were detected, much more than expected (10 %). This fact may be taken as a first hint that wildfire smoke was significantly involved in Arctic cirrus formation. The smoke particle surface area concentration around the tropopause was of the order of 5–15 µm2 cm−3 and indicated considerably enhanced levels of aerosol pollution in the upper troposphere. Based on the combined lidar-radar measurements, we analyzed 20 cirrus cases in terms of profiles of the ice water content (IWC), ice crystal number concentration (ICNC), and visible extinction coefficient. IWC mostly ranged from 0.001–0.01 g/m−3 and ICNC (in the ice virga) accumulated in the range from 0.01 to 10 L−1. Three facts (in combination) corroborate our hypothesis that aged wildfire smoke triggered ice formation in many of the observed cirrus systems: (1) The low ICNC values point to heterogeneous ice nucleation, (2) the elevated smoke pollution levels (in terms of particle surface area concentrations) were high enough to significantly influence ice nucleation in the upper troposphere, and (3) the high ice saturation ratios accumulating around 1.3–1.4 in the upper part of the observed and analyzed cirrus decks indicate quite inefficient INPs as expected in the case of organic aerosol particles (wild fire smoke particles).

The MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition was the largest Arctic field campaign ever conducted. MOSAiC offered the unique opportunity to monitor and characterize aerosols and clouds with high vertical resolution up to 30 km height at latitudes from 80 to 90∘ N over an entire year (October 2019 to September 2020). Without a clear knowledge of the complex aerosol layering, vertical structures, and dominant aerosol types and their impact on cloud formation, a full understanding of the meteorological processes in the Arctic, and thus advanced climate change research, is impossible. Widespread ground-based in situ observations in the Arctic are insufficient to provide these required aerosol and cloud data. In this article, a summary of our MOSAiC observations of tropospheric aerosol profiles with a state-of-the-art multiwavelength polarization Raman lidar aboard the icebreaker Polarstern is presented. Particle optical properties, i.e., light-extinction profiles and aerosol optical thickness (AOT), and estimates of cloud-relevant aerosol properties such as the number concentration of cloud condensation nuclei (CCN) and ice-nucleating particles (INPs) are discussed, separately for the lowest part of the troposphere (atmospheric boundary layer, ABL), within the lower free troposphere (around 2000 m height), and at the cirrus level close to the tropopause. In situ observations of the particle number concentration and INPs aboard Polarstern are included in the study. A strong decrease in the aerosol amount with height in winter and moderate vertical variations in summer were observed in terms of the particle extinction coefficient. The 532 nm light-extinction values dropped from >50 Mm−1 close to the surface to <5 Mm−1 at 4–6 km height in the winter months. Lofted, aged wildfire smoke layers caused a re-increase in the aerosol concentration towards the tropopause. In summer (June to August 2020), much lower particle extinction coefficients, frequently as low as 1–5 Mm−1, were observed in the ABL. Aerosol removal, controlled by in-cloud and below-cloud scavenging processes (widely suppressed in winter and very efficient in summer) in the lowermost 1–2 km of the atmosphere, seems to be the main reason for the strong differences between winter and summer aerosol conditions. A complete annual cycle of the AOT in the central Arctic could be measured. This is a valuable addition to the summertime observations with the sun photometers of the Arctic Aerosol Robotic Network (AERONET). In line with the pronounced annual cycle in the aerosol optical properties, typical CCN number concentrations (0.2 % supersaturation level) ranged from 50–500 cm−3 in winter to 10–100 cm−3 in summer in the ABL. In the lower free troposphere (at 2000 m), however, the CCN level was roughly constant throughout the year, with values mostly from 30 to 100 cm−3. A strong contrast between winter and summer was also given in terms of ABL INPs which control ice production in low-level clouds. While soil dust (from surrounding continents) is probably the main INP type during the autumn, winter, and spring months, local sea spray aerosol (with a biogenic aerosol component) seems to dominate the ice nucleation in the ABL during the summer months (June–August). The strong winter vs. summer contrast in the INP number concentration by roughly 2–3 orders of magnitude in the lower troposphere is, however, mainly caused by the strong cloud temperature contrast. A unique event of the MOSAiC expedition was the occurrence of a long-lasting wildfire smoke layer in the upper troposphere and lower stratosphere. Our observations suggest that the smoke particles frequently triggered cirrus formation close to the tropopause from October 2019 to May 2020.

Mixed‐phase clouds (MPCs) have been identified as significant contributors to uncertainties in climate projections, attributable to model representation of processes controlling the formation and loss of supercooled water droplets and ice particles from the atmosphere. Arctic MPCs are commonly widespread and long‐lived, with sustained ice crystal formation processes that challenge current understanding. This study examines the ice‐nucleating particle (INP) reservoir dynamics governing immersion‐mode heterogeneous freezing in an observed case of Arctic MPCs using a simplified 1D aerosol‐cloud model. The model setup includes prescribed dynamical forcings and thermodynamic profiles, and represents INPs as multicomponent and polydisperse particle size distributions. Diagnostic and prognostic approaches to immersion freezing parameterization are compared, including time‐independent (singular) number‐ and surface area‐based descriptions and a time‐dependent description following classical nucleation theory (CNT). The choice of freezing parameterization defines the size of the INP reservoir. The CNT‐based description yields an orders of magnitude larger INP reservoir than the singular parameterizations, which is the dominant factor for sustained ice crystal formation. The efficiency of the freezing process and cloud cooling are of secondary importance. A diagnostic treatment neglecting INP loss is only accurate when the INP reservoir size is large and INP depletion weak. Since a larger INP reservoir sustains ice crystal formation substantially longer, and ice water path scales with ice crystal concentrations for the conditions considered, resolving the source of differences in INP reservoir dynamics due to model implementation is a high priority for advancing climate model physics.

Atmospheric ice nucleation is crucial for global precipitation and affects the structure, lifetime and reflectivity of clouds, thereby impacting climate. Ice nucleates in various ways from aerosol particles, termed ice-nucleating particles, over an extensive temperature and humidity range. Quantifying the kinetic and thermodynamic regimes of nucleation is necessary to relate fundamental physics to theoretically based predictions of ice formation for implementation in cloud and climate models. We review how the molecular picture of ice nucleation has advanced in recent years and consequential impacts on the interpretation and parameterization of ice nucleation. Advances include the role of interfacial free energy and pressure on ice nucleation rates, mobility regions of water that generate the critical ice nucleus, classical and non-classical pathways of nucleation, the type of ice polymorph that forms, the impact of solutes on freezing and the role of nanopores as surface features promoting ice nucleation. We also introduce currently debated and evaluated freezing parameterizations for application in model environments. Finally, we outline what we believe are the current needs for improving predictive understanding of ice nucleation. Predicting atmospheric ice formation from aerosol particles for cloud and climate modelling remains challenging. This Review summarizes recent fundamental advances on the governing parameters that lead to ice nucleation from liquid droplets and solid substrates, applying experiments and computational theory.

The number of intense wildfires may increase further in upcoming years as a consequence of climate change. It is therefore necessary to improve our knowledge about the role of smoke in the climate system, with emphasis on the impact of smoke particles on the evolution of clouds, precipitation, and cloud radiative properties. Presently, one key aspect of research is whether or not wildfire smoke particles can initiate cirrus formation. In this study, we present lidar observations over Limassol, Cyprus, from 27 October to 3 November 2020, when extended wildfire smoke fields crossed the Mediterranean Basin from Portugal to Cyprus. We found strong evidence that aged smoke (organic aerosol particles) originating from wildfires in North America triggered significant ice nucleation at temperatures from −47 to −53 ∘C and caused the formation of extended cirrus layers. The observations suggest that the ice crystals were nucleated just below the tropopause in the presence of smoke particles serving as ice-nucleating particles (INPs). The main part of the 2–3 km thick smoke layer was, however, in the lower stratosphere just above the tropopause. With actual radiosonde observations of temperature and relative humidity and lidar-derived smoke particle surface area concentrations used as starting values, gravity wave simulations show that the lofting of air by 100–200 m is sufficient to initiate significant ice nucleation on the smoke particles, leading to ice crystal number concentrations of 1–100 L−1.

Abstract. Atmospheric ice nucleation impacts the hydrological cycle and climate by modifying the radiative properties of clouds. To improve our predictive understanding of ice formation, ambient ice-nucleating particles (INPs) need to be collected and characterized. Measurements of INPs at lower latitudes in a remote marine region are scarce. The Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign, in the region of the Azores islands, provided the opportunity to collect particles in the marine boundary layer (MBL) and free troposphere (FT) by aircraft during the campaign's summer and winter intensive operation period. The particle population in samples collected was examined by scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy. The identified INPs were analyzed by scanning electron microscopy with energy-dispersive X-ray analysis. We observed differences in the particle population characteristics in terms of particle diversity, mixing state, and organic volume fraction between seasons, mostly due to dry intrusion events during winter, as well as between the sampling locations of the MBL and FT. These differences are also reflected in the temperature and humidity conditions under which water uptake, immersion freezing (IMF), and deposition ice nucleation (DIN) proceed. Identified INPs reflect typical particle types within the particle population on the samples and include sea salt, sea salt with sulfates, and mineral dust, all associated with organic matter, as well as carbonaceous particles. IMF and DIN kinetics are analyzed with respect to heterogeneous ice nucleation rate coefficients, Jhet, and ice nucleation active site density, ns, as a function of the water criterion Δaw. DIN is also analyzed in terms of contact angles following classical nucleation theory. Derived MBL IMF kinetics agree with previous ACE-ENA ground-site INP measurements. FT particle samples show greater ice nucleation propensity compared to MBL particle samples. This study emphasizes that the types of INPs can vary seasonally and with altitude depending on sampling location, thereby showing different ice nucleation propensities, which is crucial information when representing mixed-phase cloud and cirrus cloud microphysics in models.

Sea spray aerosol (SSA) is a widely recognized important source of ice-nucleating particles (INPs) in the atmosphere. However, composition-specific identification, nucleation processes, and ice nucleation rates of SSA-INPs have not been well constrained. Microspectroscopic characterization of ambient and laboratory-generated SSA confirms that water-borne exudates from planktonic microorganisms composed of a mixture of proteinaceous and polysaccharidic compounds act as ice-nucleating agents (INAs). These data and data from previously published mesocosm and wave channel studies are subsequently used to further develop the stochastic freezing model (SFM) producing ice nucleation rate coefficients for SSA-INPs. The SFM simultaneously predicts immersion freezing and deposition and homogeneous ice nucleation by SSA particles under tropospheric conditions. Predicted INP concentrations agree with ambient and laboratory measurements. In addition, this holistic freezing model is independent of the source and exact composition of the SSA particles, making it well suited for implementation in cloud and climate models.

With their extensive coverage, marine low clouds greatly impact global climate. Presently, marine low clouds are poorly represented in global climate models, and the response of marine low clouds to changes in atmospheric greenhouse gases and aerosols remains the major source of uncertainty in climate simulations. The eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In addition, the ENA is periodically impacted by continental aerosols, making it an excellent location to study the cloud condensation nuclei (CCN) budget in a remote marine region periodically perturbed by anthropogenic emissions, and to investigate the impacts of long-range transport of aerosols on remote marine clouds. The Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) campaign was motivated by the need of comprehensive in situ measurements for improving the understanding of marine boundary layer CCN budget, cloud and drizzle microphysics, and the impact of aerosol on marine low cloud and precipitation. The airborne deployments took place from 21 June to 20 July 2017 and from 15 January to 18 February 2018 in the Azores. The flights were designed to maximize the synergy between in situ airborne measurements and ongoing long-term observations at a ground site. Here we present measurements, observation strategy, meteorological conditions during the campaign, and preliminary findings. Finally, we discuss future analyses and modeling studies that improve the understanding and representation of marine boundary layer aerosols, clouds, precipitation, and the interactions among them.

A record-breaking stratospheric ozone loss was observed over the Arctic and Antarctica in 2020. Strong ozone depletion occurred over Antarctica in 2021 as well. The ozone holes developed in smoke-polluted air. In this article, the impact of Siberian and Australian wildfire smoke (dominated by organic aerosol) on the extraordinarily strong ozone reduction is discussed. The study is based on aerosol lidar observations in the North Pole region (October 2019–May 2020) and over Punta Arenas in southern Chile at 53.2∘ S (January 2020–November 2021) as well as on respective NDACC (Network for the Detection of Atmospheric Composition Change) ozone profile observations in the Arctic (Ny-Ålesund) and Antarctica (Neumayer and South Pole stations) in 2020 and 2021. We present a conceptual approach on how the smoke may have influenced the formation of polar stratospheric clouds (PSCs), which are of key importance in the ozone-depleting processes. The main results are as follows: (a) the direct impact of wildfire smoke below the PSC height range (at 10–12 km) on ozone reduction seems to be similar to well-known volcanic sulfate aerosol effects. At heights of 10–12 km, smoke particle surface area (SA) concentrations of 5–7 µm2 cm−3 (Antarctica, spring 2021) and 6–10 µm2 cm−3 (Arctic, spring 2020) were correlated with an ozone reduction in terms of ozone partial pressure of 0.4–1.2 mPa (about 30 % further ozone reduction over Antarctica) and of 2–3.5 mPa (Arctic, 20 %–30 % reduction with respect to the long-term springtime mean). (b) Within the PSC height range, we found indications that smoke was able to slightly increase the PSC particle number and surface area concentration. In particular, a smoke-related additional ozone loss of 1–2 mPa (10 %–20 % contribution to the total ozone loss over Antarctica) was observed in the 14–23 km PSC height range in September–October 2020 and 2021. Smoke particle number concentrations ranged from 10 to 100 cm−3 and were about a factor of 10 (in 2020) and 5 (in 2021) above the stratospheric aerosol background level. Satellite observations indicated an additional mean column ozone loss (deviation from the long-term mean) of 26–30 Dobson units (9 %–10 %, September 2020, 2021) and 52–57 Dobson units (17 %–20 %, October 2020, 2021) in the smoke-polluted latitudinal Antarctic belt from 70–80∘ S.