Ice Nucleating Particles Research Articles

Roles of marine biota in the formation of atmospheric bioaerosols, cloud condensation nuclei, and ice-nucleating particles over the North Pacific Ocean, Bering Sea, and Arctic Ocean

Abstract. We investigated the association of marine biological indicators (polysaccharides, protein-like gel particles, and chl a) with the formation of fluorescent aerosol particles, cloud condensation nuclei (CCNs), and ice-nucleating particles (INPs) over the North Pacific Ocean, Bering Sea, and Arctic Ocean during September–November 2019. The abundance of bioindicators was high in the North Pacific Ocean and the Bering Sea (e.g., up to 1.3 mg m−3 of chl a), suggesting high biological activity due to a phytoplankton bloom. In the North Pacific Ocean, particles were characterized by high mass fractions of organics and sulfate with a predominance of terrestrial air masses. Conversely, in the Bering Sea and the Arctic Ocean, particles were characterized by high mass fractions of sea salt and sulfate with a predominance of maritime air masses. The averaged range/value of the CCN concentration at 0.4 % supersaturation were 99–151, 43–139, and 36 cm−3 over the North Pacific Ocean with terrestrial influences, over the Bering Sea with marine biogenic influences, and over the Arctic Ocean with marine influences, respectively, and the corresponding range/value of the hygroscopicity parameter κ were 0.17–0.59, 0.42–0.68, and 0.66, respectively. The averaged INP concentration (NINP) measured at temperatures of −18 and −24 ∘C with marine sources in the North Pacific and Bering Sea was 0.01–0.09 and 0.1–2.5 L−1, respectively, and that over the Arctic Ocean was 0.001–0.016 and 0.012–0.27 L−1, respectively. When marine sources were dominant, fluorescent bioaerosols in the fine mode were strongly correlated with all bioindicator types (R: 0.81–0.88) when the effect of wind-induced uplift from the sea surface to the atmosphere was considered. Correlations between NINP measured at −18 and −24 ∘C and all bioindicator types (R: 0.58–0.95 and 0.79–0.93, respectively) were positive, even when the extreme outlier point was omitted, as were those between NINP and fluorescent bioaerosols (R: 0.50 and 0.60, respectively), suggesting that marine bioindicators contributed substantially as sources of bioaerosols and to cloud formation.

Cloud-Resolving ICON Simulations of Secondary Ice Production in Arctic Mixed-Phase Stratocumuli Observed during M-PACE

Abstract Field measurements and modeling studies suggest that secondary ice production (SIP) may close the gap between observed Arctic ice nucleating particle (INP) concentrations and ice crystal number concentrations ni. Here, we explore sensitivities with respect to the complexity of different INP parameterizations under the premise that ni is governed by SIP. Idealized, cloud-resolving simulations are performed for the marine cold air outbreak cloud deck sampled during the Mixed-Phase Arctic Cloud Experiment (M-PACE) with the Icosahedral Nonhydrostatic (ICON) model. The impact of the droplet shattering (DS) of raindrops and collisional breakup (BR) in addition to the existing Hallet–Mossop rime splintering mechanism were investigated. Overall, 12 different model experiments (12-h runs) were performed and analyzed. Despite the considerable amount of uncertainty remaining with regard to SIP mechanisms and their process representation in numerical models, we conclude from these experiments that (i) only simulations where DS dominates the SIP signal (potentially amplified by BR) capture observed ice-phase and liquid-phase cloud properties, and (ii) SIP events cluster around the convective outflow region and are structurally linked to mesoscale cloud organization. In addition, interactions with primary nucleation parameterizations of varied complexity were investigated. Here, our simulations show that (i) a stable long-lived mixed-phase cloud (MPC) can be maintained in the absence of primary nucleation once SIP is established, (ii) experiments using a computationally more efficient relaxation-based parameterization of primary nucleation are statistically invariant from simulations considering prognostic INP, and (iii) primary nucleation at cloud-top controls the areal extent of the mixed-phase cloud region, and reduces SIP efficacy via DS due to increased depletion of cloud liquid throughout the entire cloud column. Significance Statement Secondary ice production (SIP) remains a key challenge in our understanding of boundary layer mixed-phase clouds. Here, we use sensitivity experiments performed with the ICON model at the cloud-resolving scale to explore potential interactions between primary nucleation, SIP, and mesoscale cloud organization. We simulate an Arctic single-layer cold air outbreak stratocumulus deck that was sampled during the M-PACE campaign. We find that once established, SIP alone is sufficient to maintain the mixed-phase cloud state until the end of the simulation. Our sensitivity analysis also shows that numerically more efficient treatments of immersion freezing are statistically invariant from simulations with a full prognostic INP budget.

Cloud-Top Phase Characterization of Extratropical Cyclones over the Northeast and Midwest United States: Results from IMPACTS

Abstract Cloud-top phase (CTP) impacts cloud albedo and pathways for ice particle nucleation, growth, and fallout within extratropical cyclones. This study uses airborne lidar, radar, and Rapid Refresh analysis data to characterize CTP within extratropical cyclones as a function of cloud-top temperature (CTT). During the 2020, 2022, and 2023 Investigation of Microphysics and Precipitation for Atlantic Coast-Threatening Snowstorms (IMPACTS) field campaign deployments, the Earth Resources 2 (ER-2) aircraft flew 26 research flights over the northeast and midwest United States to sample the cloud tops of a variety of extratropical cyclones. A training dataset was developed to create probabilistic phase classifications based on Cloud Physics Lidar measurements of known ice and liquid clouds. These classifications were then used to quantify dominant CTP in the top 150 m of clouds sampled by the Cloud Physics Lidar in storms during IMPACTS. Case studies are presented illustrating examples of supercooled liquid water at cloud top at different CTT ranges (−3° < CTTs < −35°C) within extratropical cyclones. During IMPACTS, 19.2% of clouds had supercooled liquid water present at cloud top. Supercooled liquid was the dominant phase in extratropical cyclone cloud tops when CTTs were >−20°C. Liquid-bearing cloud tops were found at CTTs as cold as −37°C. Significance Statement Identifying supercooled liquid cloud tops’ frequency is crucial for understanding ice nucleation mechanisms at cloud top, cloud radiative effects, and aircraft icing. In this study, airborne lidar, radar, and model temperature data from 26 research flights during the NASA IMPACTS campaign are used to characterize extratropical cyclone cloud-top phase (CTP) as a function of cloud-top temperature (CTT). The results show that liquid was the dominant CTP present in extratropical cyclone cloud tops when CTTs were >−20°C with decreasing supercooled liquid cloud-top frequency at temperatures < −20°C. Nevertheless, liquid was present at CTTs as cold as −37°C.

Aerosol-related effects on the occurrence of heterogeneous ice formation over Lauder, New Zealand ∕ Aotearoa

Abstract. The presented study investigates the efficiency of heterogeneous ice formation in natural clouds over Lauder, New Zealand / Aotearoa. Aerosol conditions in the middle troposphere above Lauder are subject to huge contrasts. Clean, pristine air masses from Antarctica and the Southern Ocean arrive under southerly flow conditions, while high aerosol loads can occur when air masses are advected from nearby Australia. This study assesses how these contrasts in aerosol load affect the ice formation efficiency in stratiform midlevel clouds in the heterogeneous freezing range (−40 to 0 ∘C). For this purpose, an 11-year dataset was analyzed from a dual-wavelength polarization lidar system operated by National Institute of Water and Atmospheric Research (NIWA), Taihoro Nukurangi, at Lauder in collaboration with the National Institute for Environmental Studies in Japan and the Meteorological Research Institute of the Japan Meteorological Agency. These data were used to investigate the efficiency of heterogeneous ice formation in clouds over the site as a function of cloud-top temperature as in previous studies at other locations. The Lauder cloud dataset was put into context with lidar studies from contrasting regions such as Germany and southern Chile. The ice formation efficiency found at Lauder is lower than in polluted midlatitudes (i.e., Germany) but higher than, for example, in southern Chile. Both Lauder and southern Chile are subject to generally low free-tropospheric aerosol loads, which suggests that the low ice formation efficiency at these two sites is related to low ice-nucleating-particle (INP) concentrations. However, Lauder sees episodes of continental aerosol, more than southern Chile does, which seems to lead to the moderately increased ice formation efficiency. Trajectory-based tools and aerosol model reanalyses are used to relate this cloud dataset to the aerosol load and the air mass sources. Both analyses point clearly to higher ice formation efficiency for clouds which are more strongly influenced by continental aerosol and to lower ice formation efficiency for clouds which are more influenced by Antarctic/marine aerosol and air masses.

Radiative and Microphysical Impacts of the Saharan Dust on Two Concurrent Tropical Cyclones: Danielle and Earl (2010)

AbstractSaharan dust exerts profound impacts on the genesis and intensification of tropical cyclones (TCs). Such impacts on various stages of the TCs have yet to be explored. In this study, we utilize the Cloud‐Resolving weather research and forecasting model (WRF) to investigate the relative importance of the microphysical and radiative effects of dust on two hurricanes (Earl and Danielle) at different life stages under similar dynamical conditions in 2010. Both TCs were embedded in a dusty environment throughout their lifetime. A new dust ice nucleation scheme was implemented into the aerosol‐aware Texas A&M University two‐moment microphysical scheme in WRF. Moreover, the dust radiative effect was included in the Goddard Shortwave Scheme of WRF. Our sensitivity experiments show that the radiative effect of dust (DRAD) amplified the mid‐level ridge in the Central Atlantic Ocean through temperature perturbation, changing the tracks of Danielle and Earl. Further analyses reveal an early shift of Danielle's maximum intensity for 12 hours but a significantly suppressed Earl in DRAD. In addition, the microphysical effect of dust had little impact on the large‐scale dynamical fields and storm tracks. The inclusion of dust as ice nucleation particles results in more variations in the intensity of Danielle and Earl than in other scenarios. This is owing to the higher maximum diabatic heating rate in the rainband region that perturbs the size of the TC. This study shows the dominant dust radiative effects on both intensity and track of the storm. In addition, there is evidence that dust suppresses the early stage TC but provides favorable conditions for matured TC. Both findings have profound implications for hurricane forecast and address the importance of accounting for detailed cloud microphysics and aerosol‐TC interactions in the operational forecasting models.

Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions

Abstract. Sea spray aerosols (SSAs) represent one of the most abundant aerosol types on a global scale and have been observed at all altitudes including the upper troposphere. SSA has been explored in recent years as a source of ice-nucleating particles (INPs) in cirrus clouds due to the ubiquity of cirrus clouds and the uncertainties in their radiative forcing. This study expands upon previous works on low-temperature ice nucleation of SSA by investigating the effects of atmospheric aging of SSA and the ice-nucleating activity of newly formed secondary marine aerosols (SMAs) using an oxidation flow reactor. Polydisperse aerosol distributions were generated from a marine aerosol reference tank (MART) filled with 120 L of real or artificial seawater and were dried to very low relative humidity to crystallize the salt constituents of SSA prior to their subsequent freezing, which was measured using a continuous flow diffusion chamber (CFDC). Results show that for primary SSA (pSSA), as well as aged SSA and SMA (aSSA+SMA) at temperatures >220 K, homogeneous conditions (92 %–97 % relative humidity with respect to water – RHw) were required to freeze 1 % of the particles. However, below 220 K, heterogeneous nucleation occurs for both pSSA and aSSA+SMA at much lower RHw, where up to 1 % of the aerosol population freezes between 75 % and 80 % RHw. Similarities between freezing behaviors of the pSSA and aSSA+SMA at all temperatures suggest that the contributions of condensed organics onto the pSSA or alteration of functional groups in pSSA via atmospheric aging did not hinder the major heterogeneous ice nucleation process at these cirrus temperatures, which have previously been shown to be dominated by the crystalline salts. Occurrence of a 1 % frozen fraction of SMA, generated in the absence of primary SSA, was observed at or near water saturation below 220 K, suggesting it is not an effective INP at cirrus temperatures, similar to findings in the literature on other organic aerosols. Thus, any SMA coatings on the pSSA would only decrease the ice nucleation behavior of pSSA if the organic components were able to significantly delay water uptake of the inorganic salts, and apparently this was not the case. Results from this study demonstrate the ability of lofted primary sea spray particles to remain an effective ice nucleator at cirrus temperatures, even after atmospheric aging has occurred over a period of days in the marine boundary layer prior to lofting. We were not able to address aging processes under upper-tropospheric conditions.

Characterizing Ice Nucleating Particles Over the Southern Ocean Using Simultaneous Aircraft and Ship Observations

AbstractSupercooled liquid clouds are ubiquitous over the Southern Ocean (SO), even to temperatures below −20°C, and comprise a large fraction of the marine boundary layer (MBL) clouds. Earth system models and reanalysis products have struggled to reproduce the observed cloud phase distribution and occurrence of cloud ice in the region. Recent simulations found the microphysical representation of ice nucleation and growth has a large impact on these properties, however, measurements of SO ice nucleating particles (INPs) to validate simulations are sparse. This study presents measurements of INPs from simultaneous aircraft and ship campaigns conducted over the SO in austral summer 2018, which include the first in situ observations in and above cloud in the region. Our results confirm recent observations that INP concentrations are uniformly lower than measurements made in the late 1960s. While INP concentrations below and above cloud are similar, higher ice nucleation efficiency above cloud supports model simulations that the dominant INP composition varies with height. Model parameterizations based solely on aerosol properties capture the mean relationship between INP concentration and temperature but not the observed variability, which is likely related to the only modest correlations observed between INPs and environmental or aerosol metrics. Including wind speed in addition to activation temperature in a marine INP parameterization reduces bias but does not explain the large range of observed INP concentrations. Direct and indirect inference of marine INP size suggests MBL INPs, at least during Austral summer, are dominated by particles with diameters smaller than 500 nm.

Anthropogenic Dust as a Significant Source of Ice‐Nucleating Particles in the Urban Environment

AbstractAnthropogenic dust is an important constituent of airborne particles in the urban environment but its ice nucleation activity remains poorly investigated. Here, we studied the sources and ice nucleating properties of size‐resolved particles in the urban atmosphere under mixed‐phase cloud conditions. The heat‐resistant ice nucleating particles (INPs) unexpectedly contributed ∼70% of the supermicron INPs at temperatures below −15°C. A detailed chemical composition analysis of size‐resolved particles revealed that these INPs were associated with anthropogenic dust, such as traffic‐influenced road dust. A parameterization based on supermicron particles was developed to predict the anthropogenic dust INP concentration, given their correlations on concentration and similarity in chemical compositions. Once integrated into global models, this parameterization holds the potential to assess the contribution of anthropogenic dust to INPs on a global scale. Given the considerable presence of anthropogenic dust in the atmosphere and its significant role as INPs, we suggest it may be an important aerosol source influencing cloud microphysics and warrant further investigations.

Atomic structure and water arrangement on K-feldspar microcline (001).

The properties of clouds, such as their reflectivity or their likelihood to precipitate, depend on whether the cloud droplets are liquid or frozen. Thus, understanding the ice nucleation mechanisms is essential for the development of reliable climate models. Most ice nucleation in the atmosphere is heterogeneous, i.e., caused by ice nucleating particles such as mineral dusts or organic aerosols. In this regard, K-feldspar minerals have attracted great interest recently as they have been identified as one of the most important ice nucleating particles under mixed-phase cloud conditions. The mechanism by which feldspar minerals facilitate ice nucleation remains, however, elusive. Here, we present atomic force microscopy (AFM) experiments on microcline (001) performed in an ultrahigh vacuum and at the solid-water interface together with density functional theory (DFT) and molecular dynamics (MD) calculations. Our ultrahigh vacuum data reveal features consistent with a hydroxyl-terminated surface. This finding suggests that water in the residual gas readily reacts with the surface. Indeed, the corresponding DFT calculations confirm a dissociative water adsorption. Three-dimensional AFM measurements performed at the mineral-water interface unravel a layered hydration structure with two features per surface unit cell. A comparison with MD calculations suggests that the structure observed in AFM corresponds to the second hydration layer rather than the first water layer. In agreement with previous computation results, no ice-like structure is seen, questioning an explanation of the ice nucleation ability by lattice match. Our results provide an atomic-scale benchmark for the clean and water-covered microcline (001) plane, which is mandatory for understanding the ice nucleation mechanism on feldspar minerals.

Sharp decline of dust events induces regional wetting over arid and semi-arid Northwest China in the NCAR Community atmosphere model

Multiple lines of observational evidence have indicated a significant wetting over the arid and semi-arid Northwest China (NWC) during recent decades, coinciding with a simultaneous sharp decline of dust events. Although recent studies have attributed NWC wetting to different anthropogenic and natural forcings, the mechanisms are not definitive and the regional wetting has been greatly underestimated in the Coupled Model Intercomparison Project historical simulations. Based on sensitivity experiments with different dust emission amounts using the NCAR Community Atmospheric Model version 5 (CAM5), here we find that decreasing dusts exert significant impacts on mixed-phase clouds through reducing the concentration of ice nucleating particles, increase the NWC precipitation and thus induce regional wetting through enhancing convection precipitation. A possible convection invigoration mechanism whereby the atmospheric vertical temperature gradient and convective instability are strengthened by reduced dusts, leading to convection invigoration and increased precipitation. These results are reinforced by simulations over the dust region in North Africa where mixed-phase and ice clouds are rare and reduced dusts do not increase precipitation. This study highlights the possible mechanism of dust-ice cloud interactions in recent NWC wetting and future regional climate change.

Marine carbohydrates in Arctic aerosol particles and fog – diversity of oceanic sources and atmospheric transformations

Abstract. Carbohydrates, originating from marine microorganisms, enter the atmosphere as part of sea spray aerosol (SSA) and can influence fog and cloud microphysics as cloud condensation nuclei (CCN) or ice-nucleating particles (INP). Particularly in the remote Arctic region, significant knowledge gaps persist about the sources, the sea-to-air transfer mechanisms, atmospheric concentrations, and processing of this substantial organic group. In this ship-based field study conducted from May to July 2017 in the Fram Strait, Barents Sea, and central Arctic Ocean, we investigated the sea-to-air transfer of marine combined carbohydrates (CCHO) from concerted measurements of the bulk seawater, the sea surface microlayer (SML), aerosol particles and fog. Our results reveal a wide range of CCHO concentrations in seawater (22–1070 µg L−1), with notable variations among different sea-ice-related sea surface compartments. Enrichment factors in the sea surface microlayer (SML) relative to bulk water exhibited variability in both dissolved (0.4–16) and particulate (0.4–49) phases, with the highest values in the marginal ice zone (MIZ) and aged melt ponds. In the atmosphere, CCHO was detected in super- and submicron aerosol particles (CCHOaer,super: 0.07–2.1 ng m−3; CCHOaer,sub: 0.26–4.4 ng m−3) and fog water (CCHOfog,liquid: 18–22 000 µg L−1; CCHOfog,atmos: 3–4300 ng m−3). Enrichment factors for sea–air transfer varied based on assumed oceanic emission sources. Furthermore, we observed rapid atmospheric aging of CCHO, indicating both biological/enzymatic processes and abiotic degradation. This study highlights the diverse marine emission sources in the Arctic Ocean and the atmospheric processes shaping the chemical composition of aerosol particles and fog.

Opinion: Tropical cirrus – from micro-scale processes to climate-scale impacts

Abstract. Tropical cirrus clouds, i.e., any type of ice cloud with tops above 400 hPa, play a critical role in the climate system and are a major source of uncertainty in our understanding of global warming. Tropical cirrus clouds involve processes spanning a wide range of spatial and temporal scales, from ice microphysics on cloud scales to mesoscale convective organization and planetary wave dynamics. This complexity makes tropical cirrus clouds notoriously difficult to model and has left many important questions stubbornly unanswered. At the same time, their multi-scale nature makes them well-positioned to benefit from the rise of global, high-resolution simulations of Earth's atmosphere and a growing abundance of remotely sensed and in situ observations. Rapid progress on our understanding of tropical cirrus requires coordinated efforts to take advantage of these modern computational and observational abilities. In this opinion paper, we review recent progress in cirrus studies, highlight important unanswered questions, and discuss promising paths forward. Significant progress has been made in understanding the life cycle of convectively generated “anvil” cirrus and the response of their macrophysical properties to large-scale controls. On the other hand, much work remains to be done to fully understand how small-scale anvil processes and the climatological anvil radiative effect will respond to global warming. Thin, in situ formed cirrus clouds are now known to be closely tied to the thermal structure and humidity of the tropical tropopause layer, but microphysical uncertainties prevent a full understanding of this link, as well as the precise amount of water vapor entering the stratosphere. Model representation of ice-nucleating particles, water vapor supersaturation, and ice depositional growth continue to pose great challenges to cirrus modeling. We believe that major advances in the understanding of tropical cirrus can be made through a combination of cross-tool synthesis and cross-scale studies conducted by cross-disciplinary research teams.

The Effects of Aminium and Ammonium Cations on the Ice Nucleation Activity of K‐Feldspar

AbstractMineral dust is one of the most abundant types of ice nucleating particles in the atmosphere. During atmospheric transport, mineral dust particles can become coated with inorganic and organic solutes, which can impact their ice nucleation activity. Aminium cations formed from amines are one type of organic solute that can coat mineral dust particles in the atmosphere, but their effects on the ice nucleation activity of mineral dust have not been studied. We investigated the effects of primary, secondary, and tertiary aminium cations with methyl and ethyl groups, as well as ammonium cations, on the ice nucleation activity of K‐feldspar, an important type of mineral dust, in the immersion freezing mode at low cation concentrations (0.2–20 mM) using a droplet‐freezing apparatus. Ammonium cations substantially increased the ice nucleation activity of K‐feldspar, consistent with previous studies. In contrast, primary aminium cations significantly reduced K‐feldspar ice nucleation activity, and secondary and tertiary aminium cations had no significant effect (the effect was less than the uncertainty of our measurements). Our combined results are consistent with the following mechanisms: ammonium cations undergo ion exchange with K‐feldspar, providing exposed N–H groups for hydrogen bonding with ice; primary aminium cations undergo ion exchange with K‐feldspar, exposing a hydrophobic tail that is not effective at nucleating ice; secondary and tertiary aminium cations do not undergo ion exchange with K‐feldspar due to steric effects caused by the multiple hydrophobic groups on the cation.

A Numerical Simulation Study of Secondary Ice Productions in a Squall Line Case

Secondary ice productions (SIPs) can produce ice crystals with a number concentration much higher than that of ice nucleating particles in mixed-phase clouds and therefore influence cloud glaciation and precipitation. For midlatitude continental mesoscale convective systems (MCSs), how SIPs affect the microphysical properties and precipitation is still not clear. There are few studies of SIPs in midlatitude continental MCSs. This study investigates the roles of three SIPs (rime splintering, freezing drop shattering, and ice-ice collisional breakup) on a squall line case in North China on 18 August 2020 using the WRF model with a modified Morrison double-moment bulk microphysical scheme. Including SIPs, especially ice-ice collisional breakup, in the model simulations markedly improves the simulated convective area and convective precipitation rate of the squall line, while slightly improving the area and precipitation of the stratiform region. Within the mixed-phase layer in both the convective and stratiform regions of the squall line, ice-ice collisional breakup is the dominant process to generate ice crystals. In contrast, rime splintering generates an order of magnitude fewer ice crystals than ice-ice collisional breakup, while freezing drop shattering plays a negligible role due to the lack of large drops. Ice multiplication through ice-ice collisional breakup and rime splintering produces numerous snowflakes and graupel. This leads to enhanced depositional growth and weaker riming, which in turn weakens rime splintering. It is recommended to add SIP parameterization to the model.

Wildfire smoke triggers cirrus formation: lidar observations over the eastern Mediterranean

Abstract. 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.

Sensitivity of cloud-phase distribution to cloud microphysics and thermodynamics in simulated deep convective clouds and SEVIRI retrievals

Abstract. The formation of ice in clouds is an important process in mixed-phase clouds, and the radiative properties and dynamical developments of clouds strongly depend on their partitioning between the liquid and ice phases. In this study, we investigated the sensitivities of the cloud phase to the ice-nucleating particle (INP) concentration and thermodynamics. Moreover, passive satellite retrieval algorithms and cloud products were evaluated to identify whether they could detect cloud microphysical and thermodynamical perturbations. Experiments were conducted using the ICOsahedral Nonhydrostatic (ICON) model at the convection-permitting resolution of about 1.2 km on a domain covering significant parts of central Europe, and they were compared to two different retrieval products based on Spinning Enhanced Visible and InfraRed Imager (SEVIRI) measurements. We selected a day with multiple isolated deep convective clouds, reaching a homogeneous freezing temperature at the cloud top. The simulated cloud liquid pixel fractions were found to decrease with increasing INP concentration, both within clouds and at the cloud top. The decrease in the cloud liquid pixel fraction was not monotonic and was stronger in high-INP cases. Cloud-top glaciation temperatures shifted toward warmer temperatures with an increasing INP concentration by as much as 8 ∘C. Moreover, the impact of the INP concentration on cloud-phase partitioning was more pronounced at the cloud top than within the cloud. Furthermore, initial and lateral boundary temperature fields were perturbed with increasing and decreasing temperature increments from 0 to ±3 and ±5 K between 3 and 12 km, respectively. Perturbing the initial thermodynamic state was also found to systematically affect the cloud-phase distribution. However, the simulated cloud-top liquid pixel fraction, diagnosed using radiative transfer simulations as input to a satellite forward operator and two different satellite remote-sensing retrieval algorithms, deviated from one of the satellite products regardless of perturbations in the INP concentration or the initial thermodynamic state for warmer subzero temperatures while agreeing with the other retrieval scheme much better, in particular for the high-INP and high-CAPE (convective available potential energy) scenarios. Perturbing the initial thermodynamic state, which artificially increases the instability of the mid- and upper-troposphere, brought the simulated cloud-top liquid pixel fraction closer to the satellite observations, especially in the warmer mixed-phase temperature range.

An open-hardware community ice nucleation cold stage for research and teaching

Aerosol particles with rare specific properties act as nuclei for ice formation. The presence of ice nucleating particles in the atmosphere leads to heterogeneous freezing at warm temperatures and thus these particles play an important role in modulating microphysical properties of clouds. This work presents an ice nucleation cold stage instrument for measuring the concentration of ice nucleating particles in liquids. The cost is ∼ $10 k including an external chiller. Using a lower cost heat sink reduces the cost to ∼ $6 k. The instrument is suitable for studying ambient ice nucleating particle concentrations and laboratory-based process-level studies of ice nucleation. The design plans allow individuals to self-manufacture the cold-stage using 3D printing, off-the-shelf parts, and a handful of standard tools. Software to operate the instrument and analyze the data is also provided. The design is intended to be simple enough that a graduate student can build it as part of a course or thesis project. Costs are kept to a minimum to facilitate use in classroom demonstrations and laboratory classes.

Analysis of insoluble particles in hailstones in China

Abstract. Insoluble particles influence weather and climate by means of heterogeneous freezing process. Current weather and climate models face considerable uncertainties in freezing-process simulation due to limited information regarding species and number concentrations of heterogeneous ice-nucleating particles, particularly insoluble particles. Here, for the first time, the size distribution and species of insoluble particles are analyzed in 30 shells of 12 hailstones collected from China using scanning electron microscopy and energy-dispersive X-ray spectrometry. A total of 289 461 insoluble particles were detected and divided into three species – organics, dust, and bioprotein – utilizing machine learning methods. The size distribution of the insoluble particles of each species varies greatly among the different hailstones but little in their shells. Further, a classic size distribution of organics and dust followed logarithmic normal distributions, which could potentially be adapted in future weather and climate models despite the existence of uncertainties. Our findings highlight the need for atmospheric chemistry to be considered in the simulation of ice-freezing processes.

Aircraft ice-nucleating particle and aerosol composition measurements in the western North American Arctic

Abstract. Knowledge of the temperature-dependent concentration of ice-nucleating particles (INPs) is crucial to understanding the properties of mixed-phase clouds. However, the sources, transport and removal of INPs around the globe, and particularly in the Arctic region, are poorly understood. In the Arctic winter and spring, when many local sources are covered by ice and snow, it is not clear which INP types are important. In this study, we present a new dataset of aircraft-based immersion mode INP measurements and aerosol size-resolved composition in the western North American Arctic from 11 to 21 March 2018. Aerosol samples were collected between ∼ 70 and 600 m above the surface on filters that were analysed using both a freezing droplet-based assay and scanning electron microscopy with energy dispersive spectroscopy (SEM-EDS). The measured INP concentrations were at or close to the limit of detection, with concentrations at −20 ∘C of 1 L−1 or below. The size-resolved composition measurements indicates that the aerosol concentrations were low, dominated mostly by sea spray aerosol and mineral dust. Further analysis shows that mineral dust is important for the ice-nucleating properties of our samples, dominating over the sea spray aerosol particles in the four cases we analysed, suggesting that mineral dust is a relevant type of INP in the Alaskan springtime Arctic. Furthermore, the INP concentrations are more consistent with fertile soil dusts that have an ice-active biological component than what would be expected for the ice-active mineral K-feldspar alone. While we cannot rule out local high-latitude sources of dust, the relatively small size of the mineral dust implies that the dust was from distant sources.

The Vertical Distribution of Ice-Nucleating Particles over the North China Plain: A Case of Cold Front Passage

Ice-nucleating particles (INPs) are crucial for cloud freezing processes in the atmosphere. Given the limited knowledge about the vertical distribution of INPs and its relation to aerosols in China, we present two aircraft observations of INPs over the North China Plain on 23 October 2019 and 25 October 2019, before and after a cold front passage. We used a well-established method to identify the INPs on a silicon wafer and then performed single-particle chemical composition analysis using an environmental scanning electron microscope-energy dispersive spectrometer (ESEM-EDS). The INP concentrations range from 0.1 to 9.2 L−1 within activation temperatures from −20 to −29 °C. INPs are mostly concentrated within the boundary layer, and their concentration shows a decreasing trend with height (0.5~6 km) before the cold front passage. However, the highest INP concentration always appears at higher altitudes (4~5 km) after the cold front passage. The cold front passage also significantly weakens the correlations between the concentrations of INPs and aerosol particles at different sizes. The activated fraction (AF) of total aerosols increases from 10−6 to 10−4 with height from near ground to 6 km, reflecting a better nucleating capacity of the aerosols at higher altitudes. There is no obvious variation in AF after the cold front passage. Chemical analysis reveals that the INPs containing mineral dust components comprise the majority of total INPs during both flights. The proportion of pure mineral dust declines from 52.2% to 43.5% after the cold front passage while the proportion of mixed mineral dust increases from 23.9% to 45.7%, suggesting that an increased probability of aging or coating of INPs is introduced by the cold front during their long-distance transport. In addition, 88% of INPs have a diameter larger than 1 μm. This indicates that larger aerosols (>1 μm) are the major contributors to INPs at high altitudes despite their relatively low abundance. Our results demonstrate a significant impact of transport events on the sources and vertical distribution of INPs in the atmosphere.