Ice Nucleating Particles Concentrations Research Articles

Ice Nucleating Particle Connections to Regional Argentinian Land Surface Emissions and Weather During the Cloud, Aerosol, and Complex Terrain Interactions Experiment

AbstractHere, we present a multi‐season study of ice‐nucleating particles (INPs) active via the immersion freezing mechanism, which took place in north‐central Argentina, a worldwide hotspot for mesoscale convective storms. INPs were measured untreated, after heating to 95°C, and after hydrogen peroxide digestion. No seasonal cycle of INP concentrations was observed. Heat labile INPs, which we define as “biological” herein, dominated the population active at −5 to −20°C, while non‐heat‐labile organic INPs (decomposed by peroxide) dominated at lower temperatures, from −20 to −28°C. Inorganic INPs (remaining after peroxide digestion), were minor contributors to the overall INP activity. Biological INP concentration active around −12°C peaked during rain events and under high relative humidity, reflecting emission mechanisms independent of the background aerosol concentration. The ratio of non‐heat‐labile organic and inorganic INPs was generally constant, suggesting they originated from the same source, presumably from regional arable topsoil based on air mass histories. Single particle mass spectrometry showed that soil particles aerosolized from a regionally common agricultural topsoil contained known mineral INP sources (K‐feldspar and illite) as well as a significant organic component. The INP activity observed in this study correlates well with agricultural soil INP activities from this and other regions of the world, suggesting that the observed INP spectra might be typical of many arable landscapes. These results demonstrate the strong influence of regional continental landscapes, emitting INPs of types that are not yet well represented in global models.

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.

Midlatitude mixed-phase stratocumulus clouds and their interactions with aerosols: how ice processes affect microphysical, dynamic, and thermodynamic development in those clouds and interactions?

Abstract. Midlatitude mixed-phase stratocumulus clouds and their interactions with aerosols remain poorly understood. This study examines the roles of ice processes in those clouds and their interactions with aerosols using a large-eddy simulation (LES) framework. Cloud mass becomes much lower in the presence of ice processes and the Wegener–Bergeron–Findeisen (WBF) mechanism in the mixed-phase clouds compared to that in warm clouds. This is because while the WBF mechanism enhances the evaporation of droplets, the low concentration of aerosols acting as ice-nucleating particles (INPs) and cloud ice number concentration (CINC) prevent the efficient deposition of water vapor. Note that the INP concentration in this study is based on the observed spatiotemporal variability of aerosols. This results in the lower CINC compared to that with empirical dependence of the INP concentrations on temperature in a previous study. In the mixed-phase clouds, the increasing concentration of aerosols that act as cloud condensation nuclei (CCN) decreases cloud mass by increasing the evaporation of droplets through the WBF mechanism and decreasing the intensity of updrafts. In contrast to this, in the warm clouds, the absence of the WBF mechanism makes the increase in the evaporation of droplets inefficient, eventually enabling cloud mass to increase with the increasing concentration of aerosols acting as CCN. Here, the results show that when there is an increasing concentration of aerosols that act as INPs, the deposition of water vapor is more efficient than when there is the increasing concentration of aerosols acting as CCN, which in turn enables cloud mass to increase in the mixed-phase clouds.

Sensitivity of precipitation formation to secondary ice production in winter orographic mixed-phase clouds

Abstract. The discrepancy between the observed concentration of ice nucleating particles (INPs) and the ice crystal number concentration (ICNC) remains unresolved and limits our understanding of ice formation and, hence, precipitation amount, location and intensity. Enhanced ice formation through secondary ice production (SIP) could account for this discrepancy. Here, in a region over the eastern Swiss Alps, we perform sensitivity studies of additional simulated SIP processes on precipitation formation and surface precipitation intensity. The SIP processes considered include rime splintering, droplet shattering during freezing and breakup through ice–graupel collisions. We simulated the passage of a cold front at Gotschnagrat, a peak at 2281 m a.s.l. (above sea level), on 7 March 2019 with the Consortium for Small-scale Modeling (COSMO), at a 1 km horizontal grid spacing, as part of the RACLETS (Role of Aerosols and CLouds Enhanced by Topography and Snow) field campaign in the Davos region in Switzerland. The largest simulated difference in the ICNC at the surface originated from the breakup simulations. Indeed, breakup caused a 1 to 3 orders of magnitude increase in the ICNC compared to SIP from rime splintering or without SIP processes in the control simulation. The ICNCs from the collisional breakup simulations at Gotschnagrat were in best agreement with the ICNCs measured on a gondola near the surface. However, these simulations were not able to reproduce the ice crystal habits near the surface. Enhanced ICNCs from collisional breakup reduced localized regions of higher precipitation and, thereby, improved the model performance in terms of surface precipitation over the domain.

Ice-nucleating particle concentration measurements from Ny-Ålesund during the Arctic spring–summer in 2018

Abstract. In this study, we present atmospheric ice-nucleating particle (INP) concentrations from the Gruvebadet (GVB) observatory in Ny-Ålesund (Svalbard). All aerosol particle sampling activities were conducted in April–August 2018. Ambient INP concentrations (nINP) were measured for aerosol particles collected on filter samples by means of two offline instruments: the Dynamic Filter Processing Chamber (DFPC) and the West Texas Cryogenic Refrigerator Applied to Freezing Test system (WT-CRAFT) to assess condensation and immersion freezing, respectively. DFPC measured nINPs for a set of filters collected through two size-segregated inlets: one for transmitting particulate matter of less than 1 µm (PM1), the other for particles with an aerodynamic diameter of less than 10 µm aerodynamic diameter (PM10). Overall, nINPPM10 measured by DFPC at a water saturation ratio of 1.02 ranged from 3 to 185 m−3 at temperatures (Ts) of −15 to −22 ∘C. On average, the super-micrometer INP (nINPPM10-nINPPM1) accounted for approximately 20 %–30 % of nINPPM10 in spring, increasing in summer to 45 % at −22 ∘C and 65 % at −15 ∘C. This increase in super-micrometer INP fraction towards summer suggests that super-micrometer aerosol particles play an important role as the source of INPs in the Arctic. For the same T range, WT-CRAFT measured 1 to 199 m−3. Although the two nINP datasets were in general agreement, a notable nINP offset was observed, particularly at −15 ∘C. Interestingly, the results of both DFPC and WT-CRAFT measurements did not show a sharp increase in nINP from spring to summer. While an increase was observed in a subset of our data (WT-CRAFT, between −18 and −21 ∘C), the spring-to-summer nINP enhancement ratios never exceeded a factor of 3. More evident seasonal variability was found, however, in our activated fraction (AF) data, calculated by scaling the measured nINP to the total aerosol particle concentration. In 2018, AF increased from spring to summer. This seasonal AF trend corresponds to the overall decrease in aerosol concentration towards summer and a concomitant increase in the contribution of super-micrometer particles. Indeed, the AF of coarse particles resulted markedly higher than that of sub-micrometer ones (2 orders of magnitude). Analysis of low-traveling back-trajectories and meteorological conditions at GVB matched to our INP data suggests that the summertime INP population is influenced by both terrestrial (snow-free land) and marine sources. Our spatiotemporal analyses of satellite-retrieved chlorophyll a, as well as spatial source attribution, indicate that the maritime INPs at GVB may come from the seawaters surrounding the Svalbard archipelago and/or in proximity to Greenland and Iceland during the observation period. Nevertheless, further analyses, performed on larger datasets, would be necessary to reach firmer and more general conclusions.

Two-year statistics of columnar-ice production in stratiform clouds over Hyytiälä, Finland: environmental conditions and the relevance to secondary ice production

Abstract. Formation of ice particles in clouds at temperatures of −10 ∘C or warmer was documented by using ground-based radar observations. At these temperatures, the number concentration of ice-nucleating particles (INPs) is not only expected to be small, but this number is also highly uncertain. In addition, there are a number of studies reporting that the observed number concentration of ice particles exceeds expected INP concentrations, indicating that other ice generation mechanisms, such as secondary ice production (SIP), may play an important role in such clouds. To identify formation of ice crystals and report conditions in which they are generated, W-band cloud radar Doppler spectra observations collected at the Hyytiälä station for more than 2 years were used. Given that at these temperatures ice crystals grow mainly as columns, which have distinct linear depolarization ratio (LDR) values, the spectral LDR was utilized to identify newly formed ice particles. It is found that in 5 %–13 % of clouds, where cloud top temperatures are −12 ∘C or warmer, production of columnar ice is detected. For colder clouds, this percentage can be as high as 33 %; 40 %–50 % of columnar-ice-producing events last less than 1 h, while 5 %–15 % can persist for more than 6 h. By comparing clouds where columnar crystals are produced and to the ones where these crystals are absent, the columnar-ice-producing clouds tend to have larger values of liquid water path and precipitation intensity. The columnar-ice-producing clouds were subdivided into three categories, using the temperature difference, ΔT, between the altitudes where columns are first detected and cloud top. The cases where ΔT is less than 2 K are typically single-layer shallow clouds where needles are produced at the cloud top. In multilayered clouds where 2 K < ΔT, columns are produced in a layer that is seeded by ice particles falling from above. This classification allows us to study potential impacts of various SIP mechanisms, such as the Hallet–Mossop process or freezing breakup, on columnar-ice production. To answer the question whether the observed ice particles are generated by SIP in the observed single-layer shallow clouds, ice particle number concentrations were retrieved and compared to several INP parameterizations. It was found that the ice number concentrations tend to be 1–3 orders of magnitude higher than the expected INP concentrations.

High homogeneous freezing onsets of sulfuric acid aerosol at cirrus temperatures

Abstract. Homogeneous freezing of aqueous solution aerosol particles is an important process for cloud ice formation in the upper troposphere. There the air temperature is low, the ice supersaturation can be high and the concentration of ice-nucleating particles is too low to initiate and dominate cirrus cloud formation by heterogeneous ice nucleation processes. The most common description to quantify homogeneous freezing processes is based on the water activity criterion (WAC) as proposed by Koop et al. (2000). The WAC describes the homogeneous nucleation rate coefficients only as a function of the water activity, which makes this approach well applicable in numerical models. In this study, we investigate the homogeneous freezing behavior of aqueous sulfuric acid aerosol particles by means of a comprehensive collection of laboratory-based homogeneous freezing experiments conducted at the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud simulation chamber, which were conducted as part of 17 measurement campaigns since 2007. The most recent experiments were conducted during October 2020 with special emphasis on temperatures below 200 K. Aqueous sulfuric acid aerosol particles of high purity were generated by particle nucleation in a gas flow composed of clean synthetic air and sulfuric acid vapor, which was added to the AIDA chamber. The resulting chamber aerosol had number concentrations from 30 cm−3 up to several thousand per cubic centimeter with particle diameters ranging from about 30 nm to 1.1 µm. Homogeneous freezing of the aerosol particles was measured at simulated cirrus formation conditions in a wide range of temperatures between 185 and 230 K with a steady increase of relative humidity during each experiment. At temperatures between about 205 K and about 230 K, the AIDA results agree well with the WAC-based predictions of homogeneous freezing onsets. At lower temperatures, however, the AIDA results show an increasing deviation from the WAC-based predictions towards higher freezing onsets. For temperatures between 185 and 205 K, the WAC-based ice saturation ratios for homogeneous freezing onsets increase from about 1.6 to 1.7, whereas the AIDA measurements show an increase from about 1.7 to 2.0 in the same temperature range. Based on the experimental results of our direct measurements, we suggest a new fit line to formulate the onset conditions of homogeneous freezing of sulfuric acid aerosol particles as an isoline for nucleation rate coefficients between 5×108 and 1013 cm−3 s−1. The potential significant impacts of the higher homogeneous freezing thresholds, as directly observed in the AIDA experiments under simulated cirrus formation conditions, on the model prediction of cirrus cloud occurrence and related cloud radiative effects are discussed.

Laboratory and field studies of ice-nucleating particles from open-lot livestock facilities in Texas

Abstract. In this work, an abundance of ice-nucleating particles (INPs) from livestock facilities was studied through laboratory measurements from cloud-simulation chamber experiments and field investigation in the Texas Panhandle. Surface materials from two livestock facilities, one in the Texas Panhandle and another from McGregor, Texas, were selected as dust proxies for laboratory analyses. These two samples possessed different chemical and biological properties. A combination of aerosol interaction and dynamics in the atmosphere (AIDA) measurements and offline ice spectrometry was used to assess the immersion freezing mode ice nucleation ability and efficiency of these proxy samples at temperatures above −29 ∘C. A dynamic filter processing chamber was also used to complement the freezing efficiencies of submicron and supermicron particles collected from the AIDA chamber. For the field survey, periodic ambient particle sampling took place at four commercial livestock facilities from July 2017 to July 2019. INP concentrations of collected particles were measured using an offline freezing test system, and the data were acquired for temperatures between −5 and −25 ∘C. Our AIDA laboratory results showed that the freezing spectra of two livestock dust proxies exhibited higher freezing efficiency than previously studied soil dust samples at temperatures below −25 ∘C. Despite their differences in composition, the freezing efficiencies of both proxy livestock dust samples were comparable to each other. Our dynamic filter processing chamber results showed on average approximately 50 % supermicron size dominance in the INPs of both dust proxies. Thus, our laboratory findings suggest the importance of particle size in immersion freezing for these samples and that the size might be a more important factor for immersion freezing of livestock dust than the composition. From a 3-year field survey, we measured a high concentration of ambient INPs of 1171.6 ± 691.6 L−1 (average ± standard error) at −25 ∘C for aerosol particles collected at the downwind edges of livestock facilities. An obvious seasonal variation in INP concentration, peaking in summer, was observed, with the maximum at the same temperature exceeding 10 000 L−1 on 23 July 2018. The observed high INP concentrations suggest that a livestock facility is a substantial source of INPs. The INP concentration values from our field survey showed a strong correlation with measured particulate matter mass concentration, which supports the importance of size in ice nucleation of particles from livestock facilities.

Retrievals of dust-related particle mass and ice-nucleating particle concentration profiles with ground-based polarization lidar and sun photometer over a megacity in central China

Abstract. The POLIPHON (polarization lidar photometer networking) method is a powerful pathway to retrieve the height profiles of dust-related particle mass and ice-nucleating particle (INP) concentrations. The conversion factors fitted from the sun photometer observation data are the major part of the POLIPHON computations, which can convert the polarization-lidar-derived dust extinction coefficients into dust-related particle mass and INP concentrations. For the central Chinese megacity of Wuhan (30.5∘ N, 114.4∘ E), located at the downstream area several thousands of kilometers far away from the source regions of Asian dust, dust particles always mix with other aerosols from local emissions. Therefore, very few dust case data sets can be available when using the column-integrated Ångström exponent (for 440–870 nm) <0.3 and aerosol optical depth (at 532 nm) >0.1 recorded by a sun photometer as the filtering criteria. Instead, we present another dust case data set screening scheme that applies the simultaneous polarization lidar observation to verify the occurrence of dust. Based on the 33 dust-intrusion days identified during 2011–2013, the extinction-to-volume (cv,d) and extinction-to-large particle (with radius >250 nm) number concentration (c250,d) conversion factors are determined to be (0.52±0.12)×10-12Mmm3m-3 and 0.19±0.05 Mm cm−3, respectively. The c250,d for Wuhan is 27 % larger than that observed at Lanzhou SACOL (36.0∘ N, 104.1∘ E), a site closer to the Gobi Desert, and tends to be closer to those observed in North Africa and the Middle East, indicating dust aerosols from these two sources are also possibly involved in the dust events observed over Wuhan. As a comparison, the conversion factor c290,c of 0.11±0.02Mmcm-3 for continental aerosol is much smaller than c250,d, indicating that there is no significant influence of urban aerosols on the retrievals of dust-related conversion factor over Wuhan. The conversion factors are applied in a dust event in Wuhan to reveal the typical dust-related immersion-mode INP concentration over East Asian cities. The proposed dust case data set screening scheme may potentially be extended to the other polluted city sites that are more influenced by mixed dust.

Oceanic Supply of Ice‐Nucleating Particles and Its Effect on Ice Cloud Formation: A Case Study in the Arctic Ocean During a Cold‐Air Outbreak in Early Winter

AbstractThe relationship between cloud phase, ice‐nucleating particles (INPs), and ocean state is vital in climate system modeling. High wave conditions induced by the Arctic sea‐ice decline and intensified atmospheric forcing over the ice‐free ocean increase dynamical geochemical oceanic mixing and sea spray supply containing organic substances, which could act as INPs promoting formation of lower tropospheric ice‐containing clouds. Here, we show that the surface ocean state regulates INP concentration and ice cloud presence in the boundary layer. Arctic research cruise data from the marginal ice zone in the Chukchi Sea in November 2018 revealed high number concentrations of INPs active greater than °C and ice‐containing clouds under high wave conditions. Chemical analysis revealed high contents of organic carbon and sea salt that coincided with the increased oceanic turbidity. The findings suggest that elevated levels of marine organics will contribute to modification of cloud phase from liquid droplets to ice crystals.

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.

Global Importance of Secondary Ice Production

AbstractMeasured ice crystal number concentrations are often orders of magnitude higher than the number concentrations of ice nucleating particles, indicating the existence of secondary ice production (SIP) in clouds. Here, we present the first study to examine the global importance of SIP through the droplet shattering during freezing of rain, ice‐ice collision fragmentation, and rime splintering, using a global climate model. Our results show that SIP happens quite uniformly in the two hemispheres and dominates the ice formation in the moderately cold clouds with temperatures warmer than −15°C. SIP decreases the global annual average liquid water path by −14.6 g m−2 (−22%), increases the ice water path by 8.7 g m−2 (23%), improving the model agreement with observations. SIP changes the global annual average shortwave, longwave, and net cloud forcing by 2.1, −1.0, and 1.1 W m−2, respectively, highlighting the importance of SIP on cloud properties on the global scale.

Study of ice nucleating particles in fog-haze weather at New Delhi, India: A case of polluted environment

Ice nucleating particles (INPs) concentration in deposition mode was measured and reported for a polluted urban site in New Delhi, India. The measurements were carried out during the winter period from December 2016 to January 2017. The INPs data, sampled under different meteorological conditions, were analysed using a thermal gradient static diffusion chamber. The observed INPs concentration ranges from 0.05 to 9.55 L−1 at mean nucleation temperature − 18.49 °C (SD = 0.27 °C). The mean INPs number concentration observed under three meteorological conditions was significantly different. No correlation was observed between particles size >0.5 μm, Particulate Matter and BC for the entire observation period, but correlation (r2 = 0.27, p < 0.001) was observed between INPs and BC under foggy conditions for January 2017 period. The activation fraction was ranges from 1:106 to 1:108 for the entire campaign. Scanning electron microscopy analyses revealed that particles chemistry was diverse, and particles were a mixture of BC, mineral dust, and soot. The enrichment factor indicates that elements like Nitrogen, Sulphur, and Chloride were of anthropogenic origin.

Ice‐Nucleating Particle Concentrations and Sources in Rainwater Over the Third Pole, Tibetan Plateau

AbstractThe ice‐nucleating particles (INPs) modulate the microphysics and radiative properties of clouds. However, less is known concerning their abundance and sources in the most pristine and climatic sensitive regions, such as the Tibetan Plateau (TP). Here, to our best knowledge, we conduct the first investigation on INPs in rainwater collected in the TP region under mixed‐phase cloud conditions. The value of INP concentrations varies from 0.002 to 0.675 L−1 air over the temperature range from −7.1 to −27.5°C. This is within the INP spectra derived from precipitation under worldwide geophysical conditions and is also comparable with INP concentrations in the Arctic regions. The heat‐sensitive INPs account for 57% ± 30% of the observed INPs at −20°C and become increasingly important at higher temperatures, indicating biological particles as major contributors to INPs at temperatures above −20°C over the TP, especially on the day with additional input of biogenic materials carried by dust particles. Chemical analysis demonstrates that the rainwater components are mixture of dust particles, marine aerosol, and anthropogenic pollutants. Combined with the backward trajectory analysis, we show that dust particles transported from the surrounding deserts and originated from ground surface of TP may contribute to the heat‐resistant INPs at temperatures below −20°C.

Development of the drop Freezing Ice Nuclei Counter (FINC), intercomparison of droplet freezing techniques, and use of soluble lignin as an atmospheric ice nucleation standard

Abstract. Aerosol–cloud interactions, including the ice nucleation of supercooled liquid water droplets caused by ice-nucleating particles (INPs) and macromolecules (INMs), are a source of uncertainty in predicting future climate. Because INPs and INMs have spatial and temporal heterogeneity in source, number, and composition, predicting their concentration and distribution is a challenge requiring apt analytical instrumentation. Here, we present the development of our drop Freezing Ice Nuclei Counter (FINC) for the estimation of INP and INM concentrations in the immersion freezing mode. FINC's design builds upon previous droplet freezing techniques (DFTs) and uses an ethanol bath to cool sample aliquots while detecting freezing using a camera. Specifically, FINC uses 288 sample wells of 5–60 µL volume, has a limit of detection of −25.4 ± 0.2 ∘C with 5 µL, and has an instrument temperature uncertainty of ± 0.5 ∘C. We further conducted freezing control experiments to quantify the nonhomogeneous behavior of our developed DFT, including the consideration of eight different sources of contamination. As part of the validation of FINC, an intercomparison campaign was conducted using an NX-illite suspension and an ambient aerosol sample from two other drop freezing instruments: ETH's DRoplet Ice Nuclei Counter Zurich (DRINCZ) and the University of Basel's LED-based Ice Nucleation Detection Apparatus (LINDA). We also tabulated an exhaustive list of peer-reviewed DFTs, to which we added our characterized and validated FINC. In addition, we propose herein the use of a water-soluble biopolymer, lignin, as a suitable ice-nucleating standard. An ideal INM standard should be inexpensive, accessible, reproducible, unaffected by sample preparation, and consistent across techniques. First, we compared lignin's freezing temperature across different drop freezing instruments, including on DRINCZ and LINDA, and then determined an empirical fit parameter for future drop freezing validations. Subsequently, we showed that commercial lignin has consistent ice-nucleating activity across product batches and demonstrated that the ice-nucleating ability of aqueous lignin solutions is stable over time. With these findings, we present lignin as a good immersion freezing standard for future DFT intercomparisons in the research field of atmospheric ice nucleation.

The temperature dependence of ice-nucleating particle concentrations affects the radiative properties of tropical convective cloud systems

Abstract. Convective cloud systems in the maritime tropics play a critical role in global climate, but accurately representing aerosol interactions within these clouds persists as a major challenge for weather and climate modelling. We quantify the effect of ice-nucleating particles (INPs) on the radiative properties of a complex tropical Atlantic deep convective cloud field using a regional model with an advanced double-moment microphysics scheme. Our results show that the domain-mean daylight outgoing radiation varies by up to 18 W m−2 depending on the chosen INP parameterisation. The key distinction between different INP parameterisations is the temperature dependence of ice formation, which alters the vertical distribution of cloud microphysical processes. The controlling effect of the INP temperature dependence is substantial even in the presence of Hallett–Mossop secondary ice production, and the effects of secondary ice formation depend strongly on the chosen INP parameterisation. Our results have implications for climate model simulations of tropical clouds and radiation, which currently do not consider a link between INP particle type and ice water content. The results also provide a challenge to the INP measurement community, as we demonstrate that INP concentration measurements are required over the full mixed-phase temperature regime, which covers around 10 orders of magnitude.

A two-component parameterization of marine ice-nucleating particles based on seawater biology and sea spray aerosol measurements in the Mediterranean Sea

Abstract. Ice-nucleating particles (INPs) have a large impact on the climate-relevant properties of clouds over the oceans. Studies have shown that sea spray aerosols (SSAs), produced upon bursting of bubbles at the ocean surface, can be an important source of marine INPs, particularly during periods of enhanced biological productivity. Recent mesocosm experiments using natural seawater spiked with nutrients have revealed that marine INPs are derived from two separate classes of organic matter in SSAs. Despite this finding, existing parameterizations for marine INP abundance are based solely on single variables such as SSA organic carbon (OC) or SSA surface area, which may mask specific trends in the separate classes of INP. The goal of this paper is to improve the understanding of the connection between ocean biology and marine INP abundance by reporting results from a field study and proposing a new parameterization of marine INPs that accounts for the two associated classes of organic matter. The PEACETIME cruise took place from 10 May to 10 June 2017 in the Mediterranean Sea. Throughout the cruise, INP concentrations in the surface microlayer (INPSML) and in SSAs (INPSSA) produced using a plunging aquarium apparatus were continuously monitored while surface seawater (SSW) and SML biological properties were measured in parallel. The organic content of artificially generated SSAs was also evaluated. INPSML concentrations were found to be lower than those reported in the literature, presumably due to the oligotrophic nature of the Mediterranean Sea. A dust wet deposition event that occurred during the cruise increased the INP concentrations measured in the SML by an order of magnitude, in line with increases in iron in the SML and bacterial abundances. Increases in INPSSA were not observed until after a delay of 3 days compared to increases in the SML and are likely a result of a strong influence of bulk SSW INPs for the temperatures investigated (T=-18 ∘C for SSAs, T=-15 ∘C for SSW). Results confirmed that INPSSA are divided into two classes depending on their associated organic matter. Here we find that warm (T≥-22 ∘C) INPSSA concentrations are correlated with water-soluble organic matter (WSOC) in the SSAs, but also with SSW parameters (particulate organic carbon, POCSSW and INPSSW,-16C) while cold INPSSA (T&lt;-22 ∘C) are correlated with SSA water-insoluble organic carbon (WIOC) and SML dissolved organic carbon (DOC) concentrations. A relationship was also found between cold INPSSA and SSW nano- and microphytoplankton cell abundances, indicating that these species might be a source of water-insoluble organic matter with surfactant properties and specific IN activities. Guided by these results, we formulated and tested multiple parameterizations for the abundance of INPs in marine SSAs, including a single-component model based on POCSSW and a two-component model based on SSA WIOC and OC. We also altered a previous model based on OCSSA content to account for oligotrophy of the Mediterranean Sea. We then compared this formulation with the previous models. This new parameterization should improve attempts to incorporate marine INP emissions into numerical models.

Ice-nucleating particles in precipitation samples from the Texas Panhandle

Abstract. Ice-nucleating particles (INPs) influence the formation of ice crystals in clouds and many types of precipitation. This study reports unique properties of INPs collected from 42 precipitation samples in the Texas Panhandle region from June 2018 to July 2019. We used a cold stage instrument called the West Texas Cryogenic Refrigerator Applied to Freezing Test system to estimate INP concentrations per unit volume of air (nINP) through immersion freezing in our precipitation samples with our detection capability of &gt; 0.006 INP L−1. A disdrometer was used for two purposes: (1) to characterize the ground-level precipitation type and (2) to measure the precipitation intensity as well as size of precipitating particles at the ground level during each precipitation event. While no clear seasonal variations of nINP values were apparent, the analysis of yearlong ground-level precipitation observation as well as INPs in the precipitation samples showed some INP variations, e.g., the highest and lowest nINP values at −25 ∘C both in the summer for hail-involved severe thunderstorm samples (3.0 to 1130 INP L−1), followed by the second lowest at the same temperature from one of our snow samples collected during the winter (3.2 INP L−1). Furthermore, we conducted bacteria community analyses using a subset of our precipitation samples to examine the presence of known biological INPs. In parallel, we also performed metagenomics characterization of the bacterial microbiome in suspended ambient dust samples collected at commercial open-lot livestock facilities (cattle feedyards hereafter) in the Texas Panhandle (i.e., the northernmost counties of Texas, also known as “West Texas”) to ascertain whether local cattle feedyards can act as a source of bioaerosol particles and/or INPs found in the precipitation samples. Some key bacterial phyla present in cattle feedyard samples appeared in precipitation samples. However, no known ice nucleation active species were detected in our samples. Overall, our results showed that cumulative nINP in our precipitation samples below −20 ∘C could be high in the samples collected while observing &gt; 10 mm h−1 precipitation with notably large hydrometeor sizes and an implication of cattle feedyard bacteria inclusion.

Measurement report: Ice nucleating abilities of biomass burning, African dust, and sea spray aerosol particles over the Yucatán Peninsula

Abstract. Most precipitation from deep clouds over the continents and in the intertropical convergence zone is strongly influenced by the presence of ice crystals whose formation requires the presence of ice nucleating particles (INPs). Although there are a large number of INP sources, the ice nucleating abilities of aerosol particles originating from oceans, deserts, and wildfires are poorly described at tropical latitudes. To fill this gap in knowledge, the National Autonomous University of Mexico micro-orifice uniform deposit impactor droplet freezing technique (UNAM-MOUDI-DFT) was constructed to measure the ice nucleating activity of aerosol samples that were collected in Sisal and Mérida, Yucatán (Mexico) under the influence of cold fronts, biomass burning (BB), and African dust (AD) intrusions during five short-term field campaigns between January 2017 and July 2018. The three different aerosol types were distinguished by their physicochemical properties. Marine aerosol (MA), BB, and AD air masses were found to contain INPs; the highest concentrations were in AD (from 0.071 to 36.07 L−1 at temperatures between −18 and −27 ∘C), followed by MA (from 0.068 to 18.90 L−1 at temperatures between −15 and −28 ∘C) and BB (from 0.063 to 10.21 L−1 at temperatures between −20 and −27 ∘C). However, MA had the highest surface active site densities (ns) between −15 and −30 ∘C. Additionally, supermicron particles contributed more than 72 % of the total INP concentration independent of aerosol type.

The seasonal cycle of ice-nucleating particles linked to the abundance of biogenic aerosol in boreal forests

Abstract. Ice-nucleating particles (INPs) trigger the formation of cloud ice crystals in the atmosphere. Therefore, they strongly influence cloud microphysical and optical properties and precipitation and the life cycle of clouds. Improving weather forecasting and climate projection requires an appropriate formulation of atmospheric INP concentrations. This remains challenging as the global INP distribution and variability depend on a variety of aerosol types and sources, and neither their short-term variability nor their long-term seasonal cycles are well covered by continuous measurements. Here, we provide the first year-long set of observations with a pronounced INP seasonal cycle in a boreal forest environment. Besides the observed seasonal cycle in INP concentrations with a minimum in wintertime and maxima in early and late summer, we also provide indications for a seasonal variation in the prevalent INP type. We show that the seasonal dependency of INP concentrations and prevalent INP types is most likely driven by the abundance of biogenic aerosol. As current parameterizations do not reproduce this variability, we suggest a new mechanistic description for boreal forest environments which considers the seasonal variation in INP concentrations. For this, we use the ambient air temperature measured close to the ground at 4.2 m height as a proxy for the season, which appears to affect the source strength of biogenic emissions and, thus, the INP abundance over the boreal forest. Furthermore, we provide new INP parameterizations based on the Ice Nucleation Active Surface Site (INAS) approach, which specifically describes the ice nucleation activity of boreal aerosols particles prevalent in different seasons. Our results characterize the boreal forest as an important but variable INP source and provide new perspectives to describe these new findings in atmospheric models.