Primary Ice Formation Research Articles

Impact of Asian Dust on Cirrus Formation Over the Central Pacific: CALIOP‐ and CloudSat‐Observation‐Based Case Studies

AbstractCirrus clouds are of great importance to the global climate, with their net radiative forcing strongly dependent on the microphysical properties that are related to the ice‐nucleating regime. However, the influence of long‐range transport of dust on primary ice formation in cirrus clouds is limitedly understood, specifically over the clean remote ocean regions. Here, two case studies show that transpacific Asian dust can impact the ice formation of cirrus clouds over the central Pacific based on Cloud‐Aerosol Lidar with Orthogonal Polarization and Cloud Profiling Radar (CPR, CloudSat) observations. One case shows a well‐developed horizontally extended cirrus embedded in a pure dust layer, with an average dust‐related ice‐nucleating particle concentration (INPC) of 7 L−1 and 96 L−1 for an ice saturation ratio Si of 1.15 and 1.25, respectively; ice crystal number concentration (ICNC) with diameters >25 and 100 μm (denoted as nice,25 μm and nice,100 μm) are 64 L−1 and 7 L−1, respectively. Another case shows that cirrus clouds with a much smaller horizontal extent appeared in the vicinity of polluted dust, with an average INPC of 42–310 L−1 for the typical higher Si of 1.25–1.35 by considering a tenfold reduction of the ice nucleation efficiency of ice crystals; nice,25 μm and nice,100 μm are 168 L−1 and 20 L−1, respectively. The estimated INPC and ICNC values suggest the dominance of ice formation by dust‐induced heterogeneous nucleation, proving that the long‐range transport of dust toward the upper troposphere and the potential influence on cirrus formation over the central Pacific should be well considered in atmospheric models.

Enrichment of Phosphates, Lead, and Mixed Soil‐Organic Particles in INPs at the Southern Great Plains Site

AbstractIce nucleating particles (INPs) are rare particles that initiate primary ice formation, a critical step required for subsequent important cloud microphysical processes that ultimately govern cloud phase and cloud radiative properties. Laboratory studies have found that organic‐rich dusts, such as those found in soils, are more efficient INPs compared to mineral dust. However, the atmospheric relevance of these organic‐rich dusts are not well understood, particularly in regions with significant agricultural activity. The Agricultural Ice nuclei at the Southern Great Plains field campaign (AGINSGP) was conducted in rural Oklahoma to investigate how soil dusts contribute to INP populations in the Great Plains. We present chemical characterization of ambient and ice crystal residual particles from a single day of sampling, using single particle mass spectrometry (SPMS) and scanning microscopy. Ambient particles were primarily carbonaceous or secondary aerosol, while the fraction of dust particles was higher in the residual particles. We also observed an unusual particle type consisting of a carbonaceous core mixed with dust fragments on the surface, which was found in higher proportion in residuals. Dust particles measured during residual sampling contained greater proportions of phosphate (63 and 79) and lead (206Pb+). Strong sulfate signals were not seen in the residual dust particles measured by the SPMS, while nitrate was slightly depleted relative to ambient dust. This study shows that organic‐rich soils may be important contributors to the ambient INP population in agricultural regions.

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.

Retrieving ice-nucleating particle concentration and ice multiplication factors using active remote sensing validated by in situ observations

Abstract. Understanding the evolution of the ice phase within mixed-phase clouds (MPCs) is necessary to reduce uncertainties related to the cloud radiative feedback in climate projections and precipitation initiation. Both primary ice formation via ice-nucleating particles (INPs) and secondary ice production (SIP) within MPCs are unconstrained, not least because of the lack of atmospheric observations. In the past decades, advanced remote sensing methods have emerged which provide high-resolution data of aerosol and cloud properties and could be key in understanding microphysical processes on a global scale. In this study, we retrieved INP concentrations and ice multiplication factors (IMFs) in wintertime orographic clouds using active remote sensing and in situ observations obtained during the RACLETS campaign in the Swiss Alps. INP concentrations in air masses dominated by Saharan dust and continental aerosol were retrieved from a polarization Raman lidar and validated with aerosol and INP in situ observations on a mountaintop. A calibration factor of 0.0204 for the global INP parameterization by DeMott et al. (2010) is derived by comparing in situ aerosol and INP measurements, improving the INP concentration retrieval for continental aerosols. Based on combined lidar and radar measurements, the ice crystal number concentration and ice water content were retrieved and validated with balloon-borne in situ observations, which agreed with the balloon-borne in situ observations within an order of magnitude. For seven cloud cases the ice multiplication factors (IMFs), defined as the quotient of the ice crystal number concentration to the INP concentration, were calculated. The median IMF was around 80, and SIP was active (defined as IMFs > 1) nearly 85 % of the time. SIP was found to be active at all observed temperatures (−30 to −5 ∘C), with the highest IMFs between −20 and −5 ∘C. The introduced methodology could be extended to larger datasets to better understand the impact of SIP not only over the Alps but also at other locations and for other cloud types.

Measurement report: Ice-nucleating particles active ≥ −15 °C in free tropospheric air over western Europe

Abstract. Ice-nucleating particles (INPs) initiate ice formation in supercooled clouds, typically starting in western Europe at a few kilometres above the ground. However, little is known about the concentration and composition of INPs in the lower free troposphere (FT). Here, we analysed INPs active at −10 ∘C (INP−10) and −15 ∘C (INP−15) that were collected under FT conditions at the high-altitude observatory Jungfraujoch between January 2019 and March 2021. We relied on continuous radon measurements to distinguish FT conditions from those influenced by the planetary boundary layer. Median concentrations in the FT were 2.4 INP−10 m−3 and 9.8 INP−15 m−3, with a multiplicative standard deviation of 2.0 and 1.6 respectively. A majority of INPs were deactivated after exposure to 60 ∘C; thus, they probably originated from certain epiphytic bacteria or fungi. Subsequent heating to 95 ∘C deactivated another 15 % to 20 % of the initial INPs, which were likely other types of fungal INPs that might have been associated with soil organic matter or with decaying leaves. Very few INP−10 withstood heating to 95 ∘C, but on average 20 % of INP−15 in FT samples did so. This percentage doubled during Saharan dust intrusions, which had practically no influence on INP−10. Overall, the results suggest that aerosolised epiphytic microorganisms, or parts thereof, are responsible for the majority of primary ice formation in moderately supercooled clouds above western Europe.

The contribution of Saharan dust to the ice-nucleating particle concentrations at the High Altitude Station Jungfraujoch (3580 m a.s.l.), Switzerland

Abstract. The ice phase in mixed-phase clouds has a pivotal role in global precipitation formation as well as for Earth's radiative budget. Above 235 K, sparse particles with the special ability to initiate ice formation, ice-nucleating particles (INPs), are responsible for primary ice formation within these clouds. Mineral dust has been found to be one of the most abundant INPs in the atmosphere at temperatures colder than 258 K. However, the extent of the abundance and distribution of INPs remains largely unknown. To better constrain and quantify the impact of mineral dust on ice nucleation, we investigate the frequency of Saharan dust events (SDEs) and their contribution to the INP number concentration at 243 K and at a saturation ratio with respect to liquid water (Sw) of 1.04 at the High Altitude Research Station Jungfraujoch (JFJ; 3580 m a.s.l.) from February to December 2020. Using the single-scattering albedo Ångström exponent retrieved from a nephelometer and an Aethalometer, satellite-retrieved dust mass concentrations, simulated tropospheric residence times, and the attenuated backscatter signal from a ceilometer as proxies, we detected 26 SDEs, which in total contributed to 17 % of the time span analyzed. We found every SDE to show an increase in median INP concentrations compared to those of all non-SDE periods; however, they were not always statistically significant. Median INP concentrations of individual SDEs spread between 1.7 and 161 INP std L−1 and thus 2 orders of magnitude. In the entire period analyzed, 74.7 ± 0.2 % of all INPs were measured during SDEs. Based on satellite-retrieved dust mass concentrations, we argue that mineral dust is also present at JFJ outside of SDEs but at much lower concentrations, thus still contributing to the INP population. We estimate that 97 % of all INPs active in the immersion mode at 243 K and Sw=1.04 at JFJ are dust particles. Overall, we found INP number concentrations to follow a leptokurtic lognormal frequency distribution. We found the INP number concentrations during SDEs to correlate with the ceilometer backscatter signals from a ceilometer located 4.5 km north of JFJ and 1510 m lower in altitude, thus scanning the air masses at the same altitude as JFJ. Using the European ceilometer network allows us to study the atmospheric pathway of mineral dust plumes over a large domain, which we demonstrate in two case studies. These studies showed that mineral dust plumes form ice crystals at cirrus altitudes, which then sediment to lower altitudes. Upon sublimation in dryer air layers, the residual particles are left potentially pre-activated. Future improvements to the sampling lines of INP counters are required to study whether these particles are indeed pre-activated, leading to larger INP number concentrations than reported here.

Sources and nature of ice-nucleating particles in the free troposphere at Jungfraujoch in winter 2017

Abstract. Primary ice formation in mixed-phase clouds is initiated by a minute subset of the ambient aerosol population, called ice-nucleating particles (INPs). The knowledge about their atmospheric concentration, composition, and source in cloud-relevant environments is still limited. During the 2017 joint INUIT/CLACE (Ice Nuclei research UnIT/CLoud–Aerosol Characterization Experiment) field campaign, observations of INPs as well as of aerosol physical and chemical properties were performed, complemented by source region modeling. This aimed at investigating the nature and sources of INPs. The campaign took place at the High-Altitude Research Station Jungfraujoch (JFJ), a location where mixed-phase clouds frequently occur. Due to its altitude of 3580 m a.s.l., the station is usually located in the lower free troposphere, but it can also receive air masses from terrestrial and marine sources via long-range transport. INP concentrations were quasi-continuously detected with the Horizontal Ice Nucleation Chamber (HINC) under conditions representing the formation of mixed-phase clouds at −31 ∘C. The INP measurements were performed in parallel to aerosol measurements from two single-particle mass spectrometers, the Aircraft-based Laser ABlation Aerosol MAss Spectrometer (ALABAMA) and the laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF). The chemical identity of INPs is inferred by correlating the time series of ion signals measured by the mass spectrometers with the time series of INP measurements. Moreover, our results are complemented by the direct analysis of ice particle residuals (IPRs) by using an ice-selective inlet (Ice-CVI) coupled with the ALABAMA. Mineral dust particles and aged sea spray particles showed the highest correlations with the INP time series. Their role as INPs is further supported by source emission sensitivity analysis using atmospheric transport modeling, which confirmed that air masses were advected from the Sahara and marine environments during times of elevated INP concentrations and ice-active surface site densities. Indeed, the IPR analysis showed that, by number, mineral dust particles dominated the IPR composition (∼58 %), and biological and metallic particles are also found to a smaller extent (∼10 % each). Sea spray particles are also found as IPRs (17 %), and their fraction in the IPRs strongly varied according to the increased presence of small IPRs, which is likely due to an impact from secondary ice crystal formation. This study shows the capability of combining INP concentration measurements with chemical characterization of aerosol particles using single-particle mass spectrometry, source region modeling, and analysis of ice residuals in an environment directly relevant for mixed-phase cloud formation.

Terrestrial or marine – indications towards the origin of ice-nucleating particles during melt season in the European Arctic up to 83.7° N

Abstract. Ice-nucleating particles (INPs) initiate the primary ice formation in clouds at temperatures above ca. −38 ∘C and have an impact on precipitation formation, cloud optical properties, and cloud persistence. Despite their roles in both weather and climate, INPs are not well characterized, especially in remote regions such as the Arctic. We present results from a ship-based campaign to the European Arctic during May to July 2017. We deployed a filter sampler and a continuous-flow diffusion chamber for offline and online INP analyses, respectively. We also investigated the ice nucleation properties of samples from different environmental compartments, i.e., the sea surface microlayer (SML), the bulk seawater (BSW), and fog water. Concentrations of INPs (NINP) in the air vary between 2 to 3 orders of magnitudes at any particular temperature and are, except for the temperatures above −10 ∘C and below −32 ∘C, lower than in midlatitudes. In these temperature ranges, INP concentrations are the same or even higher than in the midlatitudes. By heating of the filter samples to 95 ∘C for 1 h, we found a significant reduction in ice nucleation activity, i.e., indications that the INPs active at warmer temperatures are biogenic. At colder temperatures the INP population was likely dominated by mineral dust. The SML was found to be enriched in INPs compared to the BSW in almost all samples. The enrichment factor (EF) varied mostly between 1 and 10, but EFs as high as 94.97 were also observed. Filtration of the seawater samples with 0.2 µm syringe filters led to a significant reduction in ice activity, indicating the INPs are larger and/or are associated with particles larger than 0.2 µm. A closure study showed that aerosolization of SML and/or seawater alone cannot explain the observed airborne NINP unless significant enrichment of INP by a factor of 105 takes place during the transfer from the ocean surface to the atmosphere. In the fog water samples with −3.47 ∘C, we observed the highest freezing onset of any sample. A closure study connecting NINP in fog water and the ambient NINP derived from the filter samples shows good agreement of the concentrations in both compartments, which indicates that INPs in the air are likely all activated into fog droplets during fog events. In a case study, we considered a situation during which the ship was located in the marginal sea ice zone and NINP levels in air and the SML were highest in the temperature range above −10 ∘C. Chlorophyll a measurements by satellite remote sensing point towards the waters in the investigated region being biologically active. Similar slopes in the temperature spectra suggested a connection between the INP populations in the SML and the air. Air mass history had no influence on the observed airborne INP population. Therefore, we conclude that during the case study collected airborne INPs originated from a local biogenic probably marine source.

Impact of vertical air motions on ice formation rate in mixed-phase cloud layers

The relationship between vertical air velocity at cloud base and primary ice formation has been measured for shallow mixed-phase cloud layers (thickness <380 m) by means of ground-based cloud radar and Doppler lidar. For layers with a cloud-top temperature below −12 °C, an increase of vertical-velocity standard deviation from 0.1 to 1.0 m s−1 leads to an increase in the mass flux of ice water by two orders of magnitude. The cloud layers under study were selected in such a way that secondary ice-formation processes played a minor role, and primary ice formation was the dominant source of ice formation. Phenomenological parameterizations of the ice mass and the ice mass flux as functions of standard deviation of vertical air velocity are given.

New type of evidence for secondary ice formation at around −15 °C in mixed-phase clouds

Abstract. Ice crystal numbers can exceed the numbers of ice-nucleating particles (INPs) observed in mixed-phase clouds (MPCs) by several orders of magnitude, also at temperatures that are colder than −8 ∘C. This disparity provides circumstantial evidence of secondary ice formation, also other than via the Hallett–Mossop process. In a new approach, we made use of the fact that planar, branched ice crystals (e.g. dendrites) grow within a relatively narrow temperature range (i.e. −12 to −17 ∘C) and can be analysed individually for INPs using a field-deployable drop-freezing assay. The novelty of our approach lies in comparing the growth temperature encoded in the habit of an individual crystal with the activation temperature of the most efficient INP contained within the same crystal to tell whether it may be the result of primary ice formation. In February and March 2018, we analysed a total of 190 dendritic crystals (∼3 mm median size) deposited within MPCs at the high-altitude research station Jungfraujoch (3580 m a.s.l.). Overall, one in eight of the analysed crystals contained an INP active at −17 ∘C or warmer, while the remaining seven most likely resulted from secondary ice formation within the clouds. The ice multiplication factor we observed was small (8), but relatively stable throughout the course of documentation. These measurements show that secondary ice can be observed at temperatures around −15 ∘C and thus advance our understanding of the extent of secondary ice formation in MPCs, even where the multiplication factor is smaller than 10.

Simulating the influence of primary biological aerosol particles on clouds by heterogeneous ice nucleation

Abstract. Primary ice formation, which is an important process for mixed-phase clouds with an impact on their lifetime, radiative balance, and hence the climate, strongly depends on the availability of ice-nucleating particles (INPs). Supercooled droplets within these clouds remain liquid until an INP immersed in or colliding with the droplet reaches its activation temperature. Only a few aerosol particles are acting as INPs and the freezing efficiency varies among them. Thus, the fraction of supercooled water in the cloud depends on the specific properties and concentrations of the INPs. Primary biological aerosol particles (PBAPs) have been identified as very efficient INPs at high subzero temperatures, but their very low atmospheric concentrations make it difficult to quantify their impact on clouds. Here we use the regional atmospheric model COSMO–ART to simulate the heterogeneous ice nucleation by PBAPs during a 1-week case study on a domain covering Europe. We focus on three highly ice-nucleation-active PBAP species, Pseudomonas syringae bacteria cells and spores from the fungi Cladosporium sp. and Mortierella alpina. PBAP emissions are parameterized in order to represent the entirety of bacteria and fungal spores in the atmosphere. Thus, only parts of the simulated PBAPs are assumed to act as INPs. The ice nucleation parameterizations are specific for the three selected species and are based on a deterministic approach. The PBAP concentrations simulated in this study are within the range of previously reported results from other modeling studies and atmospheric measurements. Two regimes of PBAP INP concentrations are identified: a temperature-limited and a PBAP-limited regime, which occur at temperatures above and below a maximal concentration at around −10 ∘C, respectively. In an ensemble of control and disturbed simulations, the change in the average ice crystal concentration by biological INPs is not statistically significant, suggesting that PBAPs have no significant influence on the average state of the cloud ice phase. However, if the cloud top temperature is below −15 ∘C, PBAP can influence the cloud ice phase and produce ice crystals in the absence of other INPs. Nevertheless, the number of produced ice crystals is very low and it has no influence on the modeled number of cloud droplets and hence the cloud structure.

Partitioning the primary ice formation modes in large eddy simulations of mixed-phase clouds

Abstract. State-of-the-art aerosol-dependent parameterisations describing each heterogeneous ice nucleation mode (contact, immersion, and deposition ice nucleation), as well as homogeneous nucleation, were incorporated into a large eddy simulation model. Several cases representing commonly occurring cloud types were simulated in an effort to understand which ice nucleation modes contribute the most to total concentrations of ice crystals. The cases include a completely idealised warm bubble, semi-idealised deep convection, an orographic cloud, and a stratiform case. Despite clear differences in thermodynamic conditions between the cases, the results are remarkably consistent between the different cloud types. In all the investigated cloud types and under normal aerosol conditions, immersion freezing dominates and contact freezing also contributes significantly. At colder temperatures, deposition nucleation plays only a small role, and homogeneous freezing is important. To some extent, the temporal evolution of the cloud determines the dominant freezing mechanism and hence the subsequent microphysical processes. Precipitation is not correlated with any one ice nucleation mode, instead occurring simultaneously when several nucleation modes are active. Furthermore, large variations in the aerosol concentration do affect the dominant ice nucleation mode; however, they have only a minor influence on the precipitation amount.

Leipzig Ice Nucleation chamber Comparison (LINC): intercomparison of four online ice nucleation counters

Abstract. Ice crystal formation in atmospheric clouds has a strong effect on precipitation, cloud lifetime, cloud radiative properties, and thus the global energy budget. Primary ice formation above 235 K is initiated by nucleation on seed aerosol particles called ice-nucleating particles (INPs). Instruments that measure the ice-nucleating potential of aerosol particles in the atmosphere need to be able to accurately quantify ambient INP concentrations. In the last decade several instruments have been developed to investigate the ice-nucleating properties of aerosol particles and to measure ambient INP concentrations. Therefore, there is a need for intercomparisons to ensure instrument differences are not interpreted as scientific findings.In this study, we intercompare the results from parallel measurements using four online ice nucleation chambers. Seven different aerosol types are tested including untreated and acid-treated mineral dusts (microcline, which is a K-feldspar, and kaolinite), as well as birch pollen washing waters. Experiments exploring heterogeneous ice nucleation above and below water saturation are performed to cover the whole range of atmospherically relevant thermodynamic conditions that can be investigated with the intercompared chambers. The Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the Portable Immersion Mode Cooling chAmber coupled to the Portable Ice Nucleation Chamber (PIMCA-PINC) performed measurements in the immersion freezing mode. Additionally, two continuous-flow diffusion chambers (CFDCs) PINC and the Spectrometer for Ice Nuclei (SPIN) are used to perform measurements below and just above water saturation, nominally presenting deposition nucleation and condensation freezing.The results of LACIS and PIMCA-PINC agree well over the whole range of measured frozen fractions (FFs) and temperature. In general PINC and SPIN compare well and the observed differences are explained by the ice crystal growth and different residence times in the chamber. To study the mechanisms responsible for the ice nucleation in the four instruments, the FF (from LACIS and PIMCA-PINC) and the activated fraction, AF (from PINC and SPIN), are compared. Measured FFs are on the order of a factor of 3 higher than AFs, but are not consistent for all aerosol types and temperatures investigated. It is shown that measurements from CFDCs cannot be assumed to produce the same results as those instruments exclusively measuring immersion freezing. Instead, the need to apply a scaling factor to CFDCs operating above water saturation has to be considered to allow comparison with immersion freezing devices. Our results provide further awareness of factors such as the importance of dispersion methods and the quality of particle size selection for intercomparing online INP counters.

On homogeneous ice formation in liquid clouds

Primary ice formation by homogeneous freezing of supercooled cloud droplets in moist adiabatic air parcels is investigated theoretically and by means of numerical simulations. Dependencies of nucleated ice crystal number and size and associated freezing temperatures are systematically studied as functions of updraught speed and cloud droplet number and size. Droplet freezing temperatures range between 235 and 239 K, depending on dynamical forcing and liquid water content. Vertical resolutions on the order of 10 m are required in numerical cloud models to resolve the thin layers in which homogeneous ice formation processes unfold. Only a fraction of droplets freeze in weakly forced clouds. Small‐scale variability in updraught speeds encountered by air parcels containing supercooled cloud droplets results in broad ice crystal number distributions when sampled across a parcel ensemble. The strong dynamical control of ice initiation in tropospheric clouds initiates homogeneous freezing in the presence of heterogeneous ice nuclei even at moderate mean updraught speeds, suggesting that such particles play a limited role in affecting droplet freezing in cold convective cloud outflow regions. These findings have important implications for microphysical and optical properties of condensed‐phase convective detrainment, setting the stage for the evolution of anvil cirrus.

Ice nucleation by combustion ash particles at conditions relevant to mixed-phase clouds

Abstract. Ice-nucleating particles can modify cloud properties with implications for climate and the hydrological cycle; hence, it is important to understand which aerosol particle types nucleate ice and how efficiently they do so. It has been shown that aerosol particles such as natural dusts, volcanic ash, bacteria and pollen can act as ice-nucleating particles, but the ice-nucleating ability of combustion ashes has not been studied. Combustion ashes are major by-products released during the combustion of solid fuels and a significant amount of these ashes are emitted into the atmosphere either during combustion or via aerosolization of bottom ashes. Here, we show that combustion ashes (coal fly ash, wood bottom ash, domestic bottom ash, and coal bottom ash) nucleate ice in the immersion mode at conditions relevant to mixed-phase clouds. Hence, combustion ashes could play an important role in primary ice formation in mixed-phase clouds, especially in clouds that are formed near the emission source of these aerosol particles. In order to quantitatively assess the impact of combustion ashes on mixed-phase clouds, we propose that the atmospheric abundance of combustion ashes should be quantified since up to now they have mostly been classified together with mineral dust particles. Also, in reporting ice residue compositions, a distinction should be made between natural mineral dusts and combustion ashes in order to quantify the contribution of combustion ashes to atmospheric ice nucleation.

Ice formation and development in aged, wintertime cumulus over the UK: observations and modelling

Abstract. In situ high resolution aircraft measurements of cloud microphysical properties were made in coordination with ground based remote sensing observations of a line of small cumulus clouds, using Radar and Lidar, as part of the Aerosol Properties, PRocesses And InfluenceS on the Earth's climate (APPRAISE) project. A narrow but extensive line (~100 km long) of shallow convective clouds over the southern UK was studied. Cloud top temperatures were observed to be higher than −8 °C, but the clouds were seen to consist of supercooled droplets and varying concentrations of ice particles. No ice particles were observed to be falling into the cloud tops from above. Current parameterisations of ice nuclei (IN) numbers predict too few particles will be active as ice nuclei to account for ice particle concentrations at the observed, near cloud top, temperatures (−7.5 °C). The role of mineral dust particles, consistent with concentrations observed near the surface, acting as high temperature IN is considered important in this case. It was found that very high concentrations of ice particles (up to 100 L−1) could be produced by secondary ice particle production providing the observed small amount of primary ice (about 0.01 L−1) was present to initiate it. This emphasises the need to understand primary ice formation in slightly supercooled clouds. It is shown using simple calculations that the Hallett-Mossop process (HM) is the likely source of the secondary ice. Model simulations of the case study were performed with the Aerosol Cloud and Precipitation Interactions Model (ACPIM). These parcel model investigations confirmed the HM process to be a very important mechanism for producing the observed high ice concentrations. A key step in generating the high concentrations was the process of collision and coalescence of rain drops, which once formed fell rapidly through the cloud, collecting ice particles which caused them to freeze and form instant large riming particles. The broadening of the droplet size-distribution by collision-coalescence was, therefore, a vital step in this process as this was required to generate the large number of ice crystals observed in the time available. Simulations were also performed with the WRF (Weather, Research and Forecasting) model. The results showed that while HM does act to increase the mass and number concentration of ice particles in these model simulations it was not found to be critical for the formation of precipitation. However, the WRF simulations produced a cloud top that was too cold and this, combined with the assumption of continual replenishing of ice nuclei removed by ice crystal formation, resulted in too many ice crystals forming by primary nucleation compared to the observations and parcel modelling.

Resurgence in Ice Nuclei Measurement Research

Understanding cloud and precipitation responses to variations in atmospheric aerosols remains an important research topic for improving the prediction of climate. Knowledge is most uncertain, and the potential impact on climate is largest with regard to how aerosols impact ice formation in clouds. In this paper, we show that research on atmospheric ice nucleation, including the development of new measurement systems, is occurring at a renewed and historically unparalleled level. A historical perspective is provided on the methods and challenges of measuring ice nuclei, and the various factors that led to a lull in research efforts during a nearly 20-yr period centered about 30 yr ago. Workshops played a major role in defining critical needs for improving measurements at that time and helped to guide renewed efforts. Workshops were recently revived for evaluating present research progress. We argue that encouraging progress has been made in the consistency of measurements using the present generation of ice nucleation instruments. Through comparison to laboratory cloud simulations, these ice nuclei measurements have provided increased confidence in our ability to quantify primary ice formation by atmospheric aerosols.

How Well Does Water Activity Determine Homogeneous Ice Nucleation Temperature in Aqueous Sulfuric Acid and Ammonium Sulfate Droplets?

AbstractFrozen fraction measurements made using a droplet free-fall freezing tube apparatus are presented and used, along with other recent laboratory measurements, to evaluate how well both the water activity idea and the translated melting-point curve idea of Koop et al. predict homogeneous freezing-point temperatures for aqueous ammonium sulfate and sulfuric acid solution droplets. The new freezing-point temperature datasets agree with the previous lowest-temperature results for both solutes. The lowest measured freezing-point temperatures for aqueous ammonium sulfate solutions agree with a curve shaped like the translated melting-point curve. However, those for aqueous sulfuric acid solutions are significantly lower than predicted by the translated melting-point curve idea, and a single water activity freezing-point temperature curve does not represent the lowest-temperature freezing-point temperature data for both solutes. A linear extrapolation of the new aqueous sulfuric acid solution freezing data to low temperatures predicts that high critical supersaturations in cloud-free regions of the upper troposphere will occur when homogeneous ice nucleation in an aqueous sulfuric acid aerosol is the primary ice formation mechanism.

Observation of high ice particle concentrations in convective cells and cloud glaciation evolution

During an investigation into convective cloud at a single temperature level near −6°C, observations by aircraft have found ice crystal concentrations significantly in excess (up to 600 L−1) of those to be expected from primary ice formation (i.e. ice multiplication). Despite the fact that the main conditions for the operation of the Hallet-Mossop secondary ice multiplication process were fulfilled, the corresponding rate of ice production, as calculated, appeared to be lower than was observed in the cloud. This suggests that other ice-enhancement processes might be at work during the ice-forming stage. A small-scale (100m) analysis of the data revealed that ice-multiplication processes operated only in the fringes of the updraught regions of growing cells. It was also observed that a sudden occurrence of the ice usually coincided with the decay of the updraught. From these observations and from an evaluation of the amount of heat released by riming and vapour deposition processes, we suggest that the cell cores are auto-seeded by the mixing or recycling of numerous ice crystals and that the rapid glaciation tends to be ineffective in increasing the buoyancy of the cell.