Ice Nucleating Particles Concentrations Research Articles

Simulations of the impact of cloud condensation nuclei and ice-nucleating particles perturbations on the microphysics and radar reflectivity factor of stratiform mixed-phase clouds

Abstract. In this research, we delve into the influence of cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations on the morphology and abundance of ice particles in mixed-phase clouds, emphasizing the consequential impact of ice particle shape, number, and size on cloud dynamics and microphysics. Leveraging the synergy of the Advanced Microphysics Prediction System (AMPS) and the Kinematic Driver (KiD) model, we conducted simulations to capture cloud microphysics across diverse CCN and INP concentrations. The Passive and Active Microwave radiative TRAnsfer (PAMTRA) radar forward simulator further augmented our study, offering insights into how the concentrations of CCN and INPs affect radar reflectivities. Our experimental framework encompassed CCN concentrations ranging from 10 to 5000 cm−3 and INP concentrations from 0.001 to 10 L−1. Central to our findings is the observation that higher INP concentrations yield smaller ice particles, while an increase in CCN concentrations leads to a subtle growth in their dimensions. Consistent with existing literature, our results spotlight oblate-like crystals as dominant between temperatures of −20 and −16 °C. Notably, high-INP scenarios unveiled a significant prevalence of irregular polycrystals. The aspect ratio (AR) of ice particles exhibited a decline with the rise in both CCN and INP concentrations, highlighting the nuanced interrelation between CCN levels and ice particle shape, especially its ramifications on the riming mechanism. The forward-simulated radar reflectivities, spanning from −11.83 dBZ (low INP, 0.001 L−1) to 4.65 dBZ (high INP, 10 L−1), elucidate the complex dynamics between CCN and INPs in determining mixed-phase cloud characteristics. Comparable differences in radar reflectivity were also reported from observational studies of stratiform mixed-phase clouds in contrasting aerosol environments. Our meticulous analysis of KiD-AMPS simulation outputs, coupled with insights into aerosol-driven microphysical changes, thus underscores the significance of this study in refining our ability to understand and interpret observations and climate projections.

Measurement report: A comparison of ground-level ice-nucleating-particle abundance and aerosol properties during autumn at contrasting marine and terrestrial locations

Abstract. Ice-nucleating particles (INPs) are an essential class of aerosols found worldwide that have far-reaching but poorly quantified climate feedback mechanisms through interaction with clouds and impacts on precipitation. These particles can have highly variable physicochemical properties in the atmosphere, and it is crucial to continuously monitor their long-term concentration relative to total ambient aerosol populations at a wide variety of sites to comprehensively understand aerosol–cloud interactions in the atmosphere. Hence, our study applied an in situ forced expansion cooling device to measure ambient INP concentrations and test its automated continuous measurements at atmospheric observatories, where complementary aerosol instruments are heavily equipped. Using collocated aerosol size, number, and composition measurements from these sites, we analyzed the correlation between sources and abundance of INPs in different environments. Toward this aim, we have measured ground-level INP concentrations at two contrasting sites, one in the Southern Great Plains (SGP) region of the United States with a substantial terrestrially influenced aerosol population and one in the Eastern North Atlantic Ocean (ENA) region with a primarily marine-influenced aerosol population. These measurements examined INPs mainly formed through immersion freezing and were performed at a ≤ 12 min resolution and with a wide range of heterogeneous freezing temperatures (Ts above −31 °C) for at least 45 d at each site. The associated INP data analysis was conducted in a consistent manner. We also explored the additional offline characterization of ambient aerosol particle samples from both locations in comparison to in situ data. From our ENA data, on average, INP abundance ranges from ≈ 1 to ≈ 20 L−1 (−30 °C ≤ T ≤ −20 °C) during October–November 2020. Backward air mass trajectories reveal a strong marine influence at ENA with 75.7 % of air masses originating over the Atlantic Ocean and 96.6 % of air masses traveling over open water, but analysis of particle chemistry suggests an additional INP source besides maritime aerosols (e.g., sea spray aerosols) at ENA. In contrast, 90.8 % of air masses at the SGP location originated from the North American continent, and 96.1 % of the time, these air masses traveled over land. As a result, organic-rich SGP aerosols from terrestrial sources exhibited notably high INP abundance from ≈ 1 to ≈ 100 L−1 (−30 °C ≤ T ≤ −15 °C) during October–November 2019. The probability density function of aerosol surface area-scaled immersion freezing efficiency (ice nucleation active surface site density; ns) was assessed for selected freezing temperatures. While the INP concentrations measured at SGP are higher than those of ENA, the ns(T) values of SGP (≈ 105 to ≈ 107 m−2 for −30 °C ≤ T ≤ −15 °C) are reciprocally lower than ENA for approximately 2 orders of magnitude (≈ 107 to ≈ 109 m−2 for −30 °C ≤ T ≤ −15 °C). The observed difference in ns(T) mainly stems from varied available aerosol surface areas, Saer, from two sites (Saer,SGP > Saer,ENA). INP parameterizations were developed as a function of examined freezing temperatures from SGP and ENA for our study periods.

A cloud-by-cloud approach for studying aerosol–cloud interaction in satellite observations

Abstract. The effective radiative forcing (ERF) due to aerosol–cloud interactions (ACIs) and rapid adjustments (ERFaci) still causes the largest uncertainty in the assessment of climate change. It is understood only with medium confidence and is studied primarily for warm clouds. Here, we present a novel cloud-by-cloud (C×C) approach for studying ACI in satellite observations that combines the concentration of cloud condensation nuclei (nCCN) and ice nucleating particles (nINP) from polar-orbiting lidar measurements with the development of the properties of individual clouds by tracking them in geostationary observations. We present a step-by-step description for obtaining matched aerosol–cloud cases. The application to satellite observations over central Europe and northern Africa during 2014, together with rigorous quality assurance, leads to 399 liquid-only clouds and 95 ice-containing clouds that can be matched to surrounding nCCN and nINP respectively at cloud level. We use this initial data set for assessing the impact of changes in cloud-relevant aerosol concentrations on the cloud droplet number concentration (Nd) and effective radius (reff) of liquid clouds and the phase of clouds in the regime of heterogeneous ice formation. We find a Δln⁡Nd/Δln⁡nCCN of 0.13 to 0.30, which is at the lower end of commonly inferred values of 0.3 to 0.8. The Δln⁡reff/Δln⁡nCCN between −0.09 and −0.21 suggests that reff decreases by −0.81 to −3.78 nm per increase in nCCN of 1 cm−3. We also find a tendency towards more cloud ice and more fully glaciated clouds with increasing nINP that cannot be explained by the increasingly lower cloud top temperature of supercooled-liquid, mixed-phase, and fully glaciated clouds alone. Applied to a larger number of observations, the C×C approach has the potential to enable the systematic investigation of warm and cold clouds. This marks a step change in the quantification of ERFaci from space.

Measurement report: Atmospheric ice nuclei in the Changbai Mountains (2623 m a.s.l.) in northeastern Asia

Abstract. Atmospheric ice nucleation plays an important role in modulating the global hydrological cycle and atmospheric radiation balance. To date, few comprehensive field observations of ice nuclei have been carried out at high-altitude sites, which are close to the height of mixed-phase cloud formation. In this study, we measured the concentration of ice-nucleating particles (INPs) in the immersion freezing mode at the summit of the Changbai Mountains (2623 m above sea level), northeast Asia, in summer 2021. The cumulative number concentration of INPs varied from 1.6 × 10−3 to 78.3 L−1 over the temperature range of −5.5 to −29.0 °C. Proteinaceous-based biological materials accounted for the majority of INPs, with the proportion of biological INPs (bio-INPs) exceeding 67 % across the entire freezing-temperature range, with this proportion even exceeding 90 % above −13.0 °C. At freezing temperatures ranging from −11.0 to −8.0 °C, bio-INPs were found to significantly correlate with wind speed (r = 0.5–0.8, p < 0.05) and Ca2+ (r = 0.6–0.9), and good but not significant correlation was found with isoprene (r = 0.6–0.7) and its oxidation products (isoprene × O3) (r = 0.7), suggesting that biological aerosols may attach to or mix with soil dust and contribute to INPs. During the daytime, bio-INPs showed a positive correlation with the planetary boundary layer (PBL) height at freezing temperatures ranging from −22.0 to −19.5 °C (r > 0.7, p < 0.05), with the valley breezes from southern mountainous regions also influencing the concentration of INPs. Moreover, the long-distance transport of air mass from the Japan Sea and South Korea significantly contributed to the high concentrations of bio-INPs. Our study emphasizes the important role of biological sources of INPs in the high-altitude atmosphere of northeastern Asia and the significant contribution of long-range transport to the INP concentrations in this region.

The Puy de Dôme ICe Nucleation Intercomparison Campaign (PICNIC): comparison between online and offline methods in ambient air

Abstract. Ice crystal formation in mixed-phase clouds is initiated by specific aerosol particles, termed ice-nucleating particles (INPs). Only a tiny fraction of all aerosol particles are INPs, providing a challenge for contemporary INP measurement techniques. Models have shown that the presence of INPs in clouds can impact their radiative properties and induce precipitation formation. However, for a qualified implementation of INPs in models, measurement techniques able to accurately detect the temperature-dependent INP concentration are needed. Here we present measurements of INP concentrations in ambient air under conditions relevant to mixed-phase clouds from a total of 10 INP methods over 2 weeks in October 2018 at the Puy de Dôme observatory in central France. A special focus in this intercomparison campaign was placed on having overlapping sampling periods. Although a variety of different measurement principles were used, the majority of the data show INP concentrations within a factor of 5 of one another, demonstrating the suitability of the instruments to derive model-relevant INP data. Lower values of comparability are likely due to instrument-specific features such as aerosol lamina spreading in continuous-flow diffusion chambers, demonstrating the need to account for such phenomena when interpreting INP concentration data from online instruments. Moreover, consistently higher INP concentrations were observed from aerosol filters collected on the rooftop at the Puy de Dôme station without the use of an aerosol inlet.

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.

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.

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.

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.

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.

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.

The chance of freezing – a conceptional study to parameterize temperature-dependent freezing by including randomness of ice-nucleating particle concentrations

Abstract. Ice-nucleating particle concentrations (INPCs) can spread over several orders of magnitude at any given temperature. However, this variability is rarely accounted for in heterogeneous ice-nucleation parameterizations. In this paper, we present an approach to incorporate the random variation in the INPC into the parameterization of immersion freezing and analyze this novel concept with various sensitivity tests. In the new scheme, the INPC is drawn from a relative frequency distribution of cumulative INPCs. At each temperature, this distribution describing the INPCs is expressed as a lognormal frequency distribution. The new parameterization scheme does not require aerosol information from the driving model to represent the heterogeneity of INPCs. The scheme's performance is tested in a large-eddy simulation of a relatively warm Arctic mixed-phase stratocumulus. We find that it leads to reasonable ice masses in the cloud, especially when compared to immersion freezing schemes that yield one fixed INPC per temperature and lead to almost no ice production in the simulated cloud. The scheme is sensitive to the median of the frequency distribution and highly sensitive to the standard deviation of the distribution, as well as to the frequency of drawing a new INPC and the resolution of the model. Generally, a higher probability of drawing large INPCs leads to substantially more ice in the simulated cloud. We expose inherent challenges to introducing such a parameterization and explore possible solutions and potential developments.

Molecular simulations reveal that heterogeneous ice nucleation occurs at higher temperatures in water under capillary tension

Abstract. Heterogeneous ice nucleation is thought to be the primary pathway for the formation of ice in mixed-phase clouds, with the number of active ice-nucleating particles (INPs) increasing rapidly with decreasing temperature. Here, molecular-dynamics simulations of heterogeneous ice nucleation demonstrate that the ice nucleation rate is also sensitive to pressure and that negative pressure within supercooled water shifts freezing temperatures to higher temperatures. Negative pressure, or tension, occurs naturally in water capillary bridges and pores and can also result from water agitation. Capillary bridge simulations presented in this study confirm that negative Laplace pressure within the water increases heterogeneous-freezing temperatures. The increase in freezing temperatures with negative pressure is approximately linear within the atmospherically relevant range of 1 to −1000 atm. An equation describing the slope depends on the latent heat of freezing and the molar volume difference between liquid water and ice. Results indicate that negative pressures of −500 atm, which correspond to nanometer-scale water surface curvatures, lead to a roughly 4 K increase in heterogeneous-freezing temperatures. In mixed-phase clouds, this would result in an increase of approximately 1 order of magnitude in active INP concentrations. The findings presented here indicate that any process leading to negative pressure in supercooled water may play a role in ice formation, consistent with experimental evidence of enhanced ice nucleation due to surface geometry or mechanical agitation of water droplets. This points towards the potential for dynamic processes such as contact nucleation and droplet collision or breakup to increase ice nucleation rates through pressure perturbations.

Physicochemical characterization and source apportionment of Arctic ice-nucleating particles observed in Ny-Ålesund in autumn 2019

Abstract. Ice-nucleating particles (INPs) initiate primary ice formation in Arctic mixed-phase clouds (MPCs), altering cloud radiative properties and modulating precipitation. For atmospheric INPs, the complexity of their spatiotemporal variations, heterogeneous sources, and evolution via intricate atmospheric interactions challenge the understanding of their impact on microphysical processes in Arctic MPCs and induce an uncertain representation in climate models. In this work, we performed a comprehensive analysis of atmospheric aerosols at the Arctic coastal site in Ny-Ålesund (Svalbard, Norway) from October to November 2019, including their ice nucleation ability, physicochemical properties, and potential sources. Overall, INP concentrations (NINP) during the observation season were approximately up to 3 orders of magnitude lower compared to the global average, with several samples showing degradation of NINP after heat treatment, implying the presence of proteinaceous INPs. Particle fluorescence was substantially associated with INP concentrations at warmer ice nucleation temperatures, indicating that in the far-reaching Arctic, aerosols of biogenic origin throughout the snow- and ice-free season may serve as important INP sources. In addition, case studies revealed the links between elevated NINP and heat lability, fluorescence, high wind speeds originating from the ocean, augmented concentration of coarse-mode particles, and abundant organics. Backward trajectory analysis demonstrated a potential connection between high-latitude dust sources and high INP concentrations, while prolonged air mass history over the ice pack was identified for most scant INP cases. The combination of the above analyses demonstrates that the abundance, physicochemical properties, and potential sources of INPs in the Arctic are highly variable despite its remote location.

Bioaerosols are the dominant source of warm-temperature immersion-mode INPs and drive uncertainties in INP predictability.

Ice-nucleating particles (INPs) are rare atmospheric aerosols that initiate primary ice formation, but accurately simulating their concentrations and variability in large-scale climate models remains a challenge. Doing so requires both simulating major particle sources and parameterizing their ice nucleation (IN) efficiency. Validating and improving model predictions of INP concentrations requires measuring their concentrations delineated by particle type. We present a method to speciate INP concentrations into contributions from dust, sea spray aerosol (SSA), and bioaerosol. Field campaign data from Bodega Bay, California, showed that bioaerosols were the primary source of INPs between -12° and -20°C, while dust was a minor source and SSA had little impact. We found that recent parameterizations for dust and SSA accurately predicted ambient INP concentrations. However, the model did not skillfully simulate bioaerosol INPs, suggesting a need for further research to identify major factors controlling their emissions and INP efficiency for improved representation in models.

Distinct secondary ice production processes observed in radar Doppler spectra: insights from a case study

Abstract. Secondary ice production (SIP) has an essential role in cloud and precipitation microphysics. In recent years, substantial insights were gained into SIP by combining experimental, modeling, and observational approaches. Remote sensing instruments, among them meteorological radars, offer the possibility of studying clouds and precipitation in extended areas over long time periods and are highly valuable to understand the spatiotemporal structure of microphysical processes. Multi-modal Doppler spectra measured by vertically pointing radars reveal the coexistence, within a radar resolution volume, of hydrometeor populations with distinct properties; as such, they can provide decisive insight into precipitation microphysics. This paper leverages polarimetric radar Doppler spectra as a tool to study the microphysical processes that took place during a snowfall event on 27 January 2021 in the Swiss Jura Mountains during the ICE GENESIS campaign. A multi-layered cloud system was present, with ice particles sedimenting through a supercooled liquid water (SLW) layer in a seeder–feeder configuration. Building on a Doppler peak detection algorithm, we implement a peak labeling procedure to identify the particle type(s) that may be present within a radar resolution volume. With this approach, we can visualize spatiotemporal features in the radar time series that point to the occurrence of distinct mechanisms during different stages of the event. By focusing on three 30 min phases of the case study and by using the detailed information contained in the Doppler spectra, together with dual-frequency radar measurements, aircraft in situ images, and simulated profiles of atmospheric variables, we narrow down the possible processes that could be responsible for the observed signatures. Depending on the availability of SLW and the droplet sizes, on the temperature range, and on the interaction between the liquid and ice particles, various SIP processes are identified as plausible, with distinct fingerprints in the radar Doppler spectra. A simple modeling approach suggests that the ice crystal number concentrations likely exceed typical concentrations of ice-nucleating particles by 1 to 4 orders of magnitude. While a robust proof of occurrence of a given SIP mechanism cannot be easily established, the multi-sensor data provide various independent elements each supporting the proposed interpretations.

Southern Alaska as a source of atmospheric mineral dust and ice-nucleating particles.

Ice-nucleating particles (INPs) influence cloud radiative properties and climate; however, INP sources and concentrations are poorly constrained, particularly in high-latitude regions. Southern Alaska is a known source of high-latitude dust, but its contribution to atmospheric mineral dust and INP concentrations has not been quantified. We show that glacial dust collected in southern Alaska is an effective ice-nucleating material under conditions relevant for mixed-phase clouds and is more active than low-latitude dust because of a biological component that enhances its activity. We use dispersion modeling to show that this source contributes to the regional INP population and that the dust emitted is transported over a broad area of North America, reaching altitudes where it could cause cloud glaciation. Our results highlight the importance of quantifying emissions and ice-nucleating characteristics of high-latitude dusts and suggest that the ice-nucleating ability of emitted dust in these regions should be represented in models using different parametrizations to low-latitude dust.

A bin microphysics parcel model investigation of secondary ice formation in an idealised shallow convective cloud

Abstract. We provide the first systematic study of ice formation in idealised shallow clouds from collisions of supercooled water drops with ice particles (mode 2). Using the University of Manchester bin microphysics parcel model, we investigated the sensitivity of ice formation due to mode 2 for a wide range of parameters, including aerosol particle size distribution, updraft speed, cloud-base temperature, cloud depth, ice-nucleating particle concentration, and freezing fraction of mode 2. We provide context to our results with other secondary ice production mechanisms as single mechanisms and combinations (rime splintering, spherical freezing fragmentation of drops (mode 1), and ice–ice collisions). There was a significant sensitivity to aerosol particle size distribution when updraft speeds were low (0.5 m s−1); secondary ice formation did not occur when the aerosol particle size distribution mimicked polluted environments. Where secondary ice formation did occur in simulated clouds, significant ice formation in the shallower clouds (1.3 km deep) was due to mode 2 or a combination which included mode 2. The deeper clouds (2.4 km deep) also had significant contributions from rime splintering or ice–ice collisional breakup secondary ice production (SIP) mechanisms. While simulations with cloud-base temperatures of 7 ∘C were relatively insensitive to ice-nucleating particle concentrations, there was a sensitivity in simulations with cloud-base temperatures of 0 ∘C. Increasing the ice-nucleating particle concentration delayed ice formation. Our results suggest that collisions of supercooled water drops with ice particles may be a significant ice formation mechanism within shallow convective clouds where rime splintering is not active.