Ice Nucleation Rate Research Articles

Quantifying the effect of particulate impurities on the ice nucleation behavior of pharmaceutical solutions.

Numerous commercially available biopharmaceuticals are frozen or freeze-dried in vials. The temperature at which ice nucleates and its distribution across vials in a batch is critical to the design of freezing and freeze-drying processes. Here we study experimentally how the level of particulate impurities - a key parameter in pharmaceutical manufacturing - affects the ice nucleation behavior. Samples prepared under particulate-free conditions were found to nucleate at significantly lower temperatures and with more variability than samples of the same composition that were prepared under standard laboratory conditions, i.e., without using any means of lowering particulate counts. In contrast, spiking solutions with silver iodide particles resulted in significantly higher and less variable nucleation temperatures. These findings confirm that the level of particulates has a relevant effect on the rate of ice nucleation under conditions of industrial relevance. We further assessed the nucleation behavior of two biopharmaceuticals, a vaccine based on a viral vector and a mAb, and observed major differences in their nucleation behavior. This emphasizes the importance of measuring the ice nucleation behavior of biopharmaceuticals during process design.

Quantifying and Modeling the Impact of Phase State on the Ice Nucleation Abilities of 2-Methyltetrols as a Key Component of Secondary Organic Aerosol Derived from Isoprene Epoxydiols.

Organic aerosols (OAs) may serve as ice-nucleating particles (INPs), impacting the formation and properties of cirrus clouds when their phase state and viscosity are in the semisolid to glassy range. However, there is a lack of direct parameterization between aerosol viscosity and their ice nucleation capabilities. In this study, we experimentally measured the ice nucleation rate of 2-methyltetrols (2-MT) aerosols, a key component of isoprene-epoxydiol-derived secondary organic aerosols (IEPOX-SOA), at different viscosities. These results demonstrate that the phase state has a significant impact on the ice nucleation abilities of OA under typical cirrus cloud conditions, with the ice nucleation rate increasing by 2 to 3 orders of magnitude when the phase state changes from liquid to semisolid. An innovative parametric model based on classical nucleation theory was developed to directly quantify the impact of viscosity on the heterogeneous nucleation rate. This model accurately represents our laboratory measurement and can be implemented into climate models due to its simple, equation-based form. Based on data collected from the ACRIDICON-CHUVA field campaign, our model predicts that the INP concentration from IEPOX-SOA can reach the magnitude of 1 to tens per liter in the cirrus cloud region impacted by the Amazon rainforest, consistent with recent field observations and estimations. This novel parameterization framework can also be applied in regional and global climate models to further improve representations of cirrus cloud formation and associated climate impacts.

Inverse Relationship Between Ice Nucleation and Ice Growth Rates in Frozen Foods

Inverse Relationship Between Ice Nucleation and Ice Growth Rates in Frozen Foods

Ice nucleation in supercooled water under shear

Classical nucleation theory (CNT) provides a good framework for understanding the nucleation phenomenon in metastable conditions. However, there is still no satisfactory understanding of the shear effect. Here, we propose an ice nucleation model considering the rebounded deformation energy to analyze the ice nucleation rate. It is concluded that: (1) The effect is more pronounced by changing the contact angle to regulate the free energy when both the supercooled degree and the shear rate are small. (2) The variation trend of the nucleation ratio Jhet,sh/Jhet,no increases at first but it may decrease when the contact angle is small, or keeps increasing when the contact angle is large. (3) The probability of the shear nucleation is about several ten orders of magnitude to that of static nucleation. (4) The key factor in the acceleration of the supercooled liquid nucleation is the released deformation energy after encountering the obstruction.

Single particle characteristics and ice nucleation potential of particles collected during Asian dust storms in 2021

Dust storms have great impacts on air quality and climate. Dust can influence cloud microphysical properties and determine their radiative forcing and precipitation. Asian dust storms (ADS) are important sources of global aerosol. However, the physiochemical characteristics of dust from ADS at a single particle level are less understood, and the exact particles that can serve as ice nucleating particles (INPs) remain unclear. Here, we present the physicochemical properties and ice nucleation ability of dust particles collected in Beijing during two major ADS in March 2021. The particles from two ADS were classified into Illite, Kaolinite, Feldspar, Quartz, Chlorite, Mixed-dust, and Non-dust particles, which contributed 28.6 % ± 3.3 %, 20.0 % ± 3.9 %, 12.3 % ± 2.3 %, 11.1 % ± 2.8 %, 9.8 % ± 0.8 %, 13.7 % ± 1.8 %, and 4.4 % ± 1.7 % in number, respectively. On average, the ADS particles formed ice crystals via deposition ice nucleation from relative humidity with respect to ice (RHice) of 112 % ± 1 % at 250 K to 154 % ± 15 % RHice at 205 K. Part of the samples also formed ice via immersion freezing between 230 K and 250 K. Among the 149 identified INPs, Clay-like particles (Chlorite, Illite, and Kaolinite) contributed 71.1 % ± 6.2 % in number and followed by Mixed-dust-like particles (16.9 % ± 8.7 %) and Feldspar-like particles (10.4 % ± 6.3 %). Enrichment factor of each particle type in INPs is calculated as the ratio of its number fractions in INPs and the aerosol population. It ranges from 0.6 ± 0.7 to 1.3 ± 2.2. The contribution of each particle type to INP was correlated with its fraction in the population. These results imply that each particle type can serve as INP. Clay-like particles are the dominant INPs during the ADS. We conducted ice nucleation kinetic analysis and provided parameterizations of heterogeneous ice nucleation rate coefficient and contact angle for ADS. These parameterizations can be used in the modeling study to evaluate the impact of ADS in atmospheric ice crystal formation in clouds.

Detonation Soot: A New Class of Ice Nucleating Particle

AbstractTemperatures and pressures from high explosive detonations far exceed atmospheric conditions in typical combustion reactions, and consequently, detonation soot forms with physiochemical properties distinct from soot formed by combustion. In this study, samples of detonation soot from two high explosives, PBX 9502 and Composition B‐3, were analyzed. Ice nucleation experiments on soot collected after controlled detonations were conducted in the laboratory to probe immersion and contact mode freezing. Samples nucleated ice at temperatures warmer than commercially available nanodiamonds, which has a mean nucleation temperature of −20.7°C. Ice nucleation rate coefficients increase rapidly by two to three orders of magnitude below −20°C for every sample. Size‐selected 137 μm diameter particles produced during detonation in an ambient air atmosphere yield bimodal distributions of freezing temperature with primary and secondary nucleation modes centered at −20°C and −13°C, respectively. The presence of a secondary mode allows for enhanced ice nucleation rate coefficients (one to two orders of magnitude greater than samples without a secondary mode) at temperatures outside the influence of the primary mode (>−17°C). Given the observed onset nucleation temperatures of −9.2°C, our results imply that detonation soot of the type studied here would only need to reach an altitude of approximately 4 km to facilitate ice formation.

Diverse sources and aging change the mixing state and ice nucleation properties of aerosol particles over the western Pacific and Southern Ocean

Abstract. Atmospheric particles can impact cloud formation and play a critical role in regulating cloud properties. However, particle characteristics at the single-particle level and their ability to act as ice-nucleating particles (INPs) over the marine atmosphere are poorly understood. In this study, we present micro-spectroscopic characterizations and ice nucleation properties of particles collected during a cruise from South Korea to Antarctica in 2019. Most of the samples were dominated by fresh sea salt, aged sea salt, and sea salt mixed with sulfate particles, with total number percentages ranging from 48 % to 99 % over the western Pacific and the Southern Ocean. The mixing-state index of the particle population ranged from 50 % to 95 % over the Northern Hemisphere and Southern Hemisphere. Multiphase processes on sea salt particles resulted in chlorine deficiency. This selective aging process made the marine particle population more externally mixed. Ice nucleation onset conditions primarily for the deposition mode were measured and the investigated particles showed diverse ice nucleation abilities. The fresh sea salt particles with organic coatings exhibited the highest ice nucleation ability at a relative humidity with respect to ice as low as 121 %. The sea salt mixed sulfate particle was enriched in INPs by a factor of 1.9. Aging processes affected both the mixing state of the particles and their ice nucleation abilities. Our analysis shows that assuming an internally mixed particle population in the marine atmosphere can lead to errors of several orders of magnitude in predicting ice nucleation rates.

Effect of multiple environmental conditions on the formation process and adhesion strength of ice on asphalt binder surface

Road icing caused by freezing rain significantly impacts driving safety. Since asphalt binder plays a pivotal role in pavement infrastructure, understanding the formation process and adhesion strength of ice on asphalt binder surfaces is crucial for assessing road icing risk. This work investigated the effect of different environmental conditions on asphalt-ice interface adhesion strength via a self-designed low-temperature adhesion testing system. In addition, the icing process on asphalt binder surfaces was observed to analyze the asphalt-ice adhesion strength formation mechanism. Results show that the completion time of water-ice phase transition signified the initial development of asphalt-ice adhesion strength. Moreover, as the internal structure of the ice evolved from transparent to needle-like fine lines to dense, the asphalt-ice adhesion strength gradually increased until it reached stability. At asphalt-ice adhesion began forming after 40 min and stabilized after 80 min, whereas at −8°C, adhesion strength started forming after 20 min and stabilized by 60 min. The growth rates of asphalt-ice adhesion strength for temperatures ranging from −2°C to −10°C were approximately 7.92 kPa/°C, 6.56 kPa/°C, 5.14 kPa/°C, 3.29 kPa/°C, and 1.49 kPa/°C, respectively, showing a positive correlation with temperature and a negative correlation with time. According to heterogeneous nucleation theory, the influence mechanism of temperature and water depth on the nucleation icing process and asphalt-ice adhesion strength is analyzed. lower temperatures lead to asphalt-ice adhesion strength increase originating from the larger supercooling, which reduces the critical nucleation energy and thus accelerates the ice nucleation rate. In addition, the increase in water depth promotes the formation of nucleation sites and further enhances the asphalt-ice adhesion strength. Finally, an asphalt-ice adhesion strength prediction model was developed, with PSO-SVM-G achieving over 90 % accuracy. These results provide insights for evaluating ice adhesion behavior on asphalt surfaces and designing anti-icing asphalt materials.

Exploring ice Ic nucleation and structural relaxation in supercooled water

Despite intensive research efforts, understanding how water freezes remains an open and relevant question with profound implications. In this study, we examine ice Ic nucleation and water relaxation at the atomic level, employing molecular dynamics (MD) simulations and Classical Nucleation Theory (CNT). Our key findings address the following foundational issues: (i) Routes to cubic ice. Ice Ic seeding liquid water results in equal amounts of ice Ic and Ih structures at T<235K, while ice Ic predominates at T⩾235K along zero isobar. Moreover, ice produced from spontaneous nucleation at T=205-215K is more cubic compared with that grown on ice Ic seeds; (ii) CNT validity. Using MD-generated data, CNT accurately predicts ice nucleation rates without any fitting parameter, thereby bridging the gap between simulations and experiments; (iii) Kinetic crossroads. We determined a kinetic spinodal for high-density water as an intersection of relaxation and nucleation time curves at TKS=199K for a MD sample and TKS=233K for a macroscopic sample, which coincides with the experimental homogenous freezing limit; (iv) Kauzmann conundrum. Finally, we indicated that if the Kauzmann temperature exists, estimated as TK=190K, it might be inaccessible for high-density water due to the kinetic spinodal at a higher temperature, TKS>TK, thus resolving the long-standing entropy paradox. Overall, this research provides valuable insights into fundamental aspects related to water crystallization.

Ice nucleation in the presence of nucleation promoters dispersed in tetrabutylammonium bromide (TBAB) solutions

Ice nucleation is the initial step of ice formation that has significant impact on global climate, several engineering and structural surfaces and other systems like clathrate hydrates. The nucleation promoters for ice have been studied for decades but some problems or mechanisms remain unclear. In our earlier study [1], Snomax was found to be the most effective promoter among the common ice nucleation promoters we had tested and it was postulated that the efficacy of Snomax might be aided by its larger interfacial area available for heterogeneous nucleation because it could be easily dispersed in water. Here we attempted to disperse the three ice nucleation promoters which we had previously found to be effective – AgI, kaolinite and cholesterol – into liquid water to increase the interfacial area with water and the heterogeneous nucleation rate of ice. We found dispersion of these promoters into water to be difficult and required addition of Tetrabutylammonium bromide (TBAB) to the aqueous phase before they could be dispersed. We then investigated the nucleation rates of ice in the dispersed nucleation promoter suspensions. We found (1) addition of TBAB alone unexpectedly promoted the nucleation of ice, (2) dispersing AgI into 1 mM TBAB solutions further promoted ice nucleation, (3) dispersing kaolinite or cholesterol in TBAB solutions did not promote ice nucleation more so than the TBAB solutions without kaolinite or cholesterol.

A universal and accurate LPMI method for calculating mismatch in heterogeneous ice nucleation.

The interfacial correlation factor f(m,x), where m refers to the interaction among ice, water and the substrate and x refers to the ratio of the critical nucleation size to the surface topography characteristic size of the substrate, plays a crucial role in the classical theory of heterogeneous ice nucleation as it significantly impacts the energy of nucleation. Generally, a smaller value of f(m,x) indicates a higher propensity for ice nucleation. The degree of structural compatibility between ice and the substrate greatly influences f(m,x), particularly on specific substrates. Several approaches have been proposed to calculate the lattice matching based on this idea, which allows whether a surface is favorable for nucleation to be determined. However, none of these methods adequately correlates the mismatch index with ice growth phenomena. In this paper, we embarked on a new attempt to calculate the mismatch index by combining the lattice parameter and Miller index (LPMI). Droplet freezing experiments have been carried out on α-Al2O3 and silicon surfaces with different Miller indices to verify the rationality of the LPMI method. Furthermore, we validated the LPMI method extensively against other works and further demonstrated its readiness, accuracy and universality for freezing problems. The results consistently show that δd = 2|di - ds|/(di + ds) with interplanar spacing more accurately predicts heterogeneous ice nucleation rates across a wide range of substrates than δ1 = (ai - as)/ai with the lattice parameter of ice and the substrate and is more generally applicable than δ2D = (di - di)/di with the distances between two adjacent and congener atoms on the same plane. We believe that the proposed approach will aid in the selection of substrates for promoting or inhibiting heterogeneous nucleation on a specific substrate.

The Effects of AC Electric Field on Ice Nucleation in the Super‐Cooling of a Distilled Water

The effects of an AC electric field on ice nucleation temperature and nucleation rate were investigated by freezing distilled water while exposing it to varied AC electric field strengths and frequencies. To eliminate the influence of ion injections and electric field concentrations at a metal electrode surface on ice nucleation, distilled water filled in resin cuvettes are used as samples. The samples are exposed to AC electric field induced by parallel plate electrodes placed outside of the cuvettes. The cuvettes and parallel plate electrodes placed in a freezer with an inside temperature fixed at −15°C. The electric field strength in the sample is 2 or 7.5 kV/m and frequency varies from 50 Hz to 10 kHz. The ice nucleation temperature and the nucleation rate of distilled water increase with increasing the electric field strength and the frequency. © 2023 Institute of Electrical Engineer of Japan and Wiley Periodicals LLC.

3He spin-echo scattering indicates hindered diffusion of isolated water molecules on graphene-covered Ir(111).

The dynamics of water diffusion on carbon surfaces are of interest in fields as diverse as furthering the use of graphene as an industrial-coating technology and understanding the catalytic role of carbon-based dust grains in the interstellar medium. The early stages of water-ice growth and the mobility of water adsorbates are inherently dependent on the microscopic mechanisms that facilitate water diffusion. Here, we use 3He spin-echo quasi-inelastic scattering to probe the microscopic mechanisms responsible for the diffusion of isolated water molecules on graphene-covered and bare Ir(111). The scattering of He atoms provides a non-invasive and highly surface-sensitive means to measure the rate at which absorbates move around on a substrate at very low coverage. Our results provide an approximate upper limit on the diffusion coefficient for water molecules on GrIr(111) of m2/s, an order of magnitude lower than the coefficient that describes the diffusion of water molecules on the bare Ir(111) surface. We attribute the hindered diffusion of water molecules on the GrIr(111) surface to water trapping at specific areas of the corrugated moiré superstructure. Lower mobility of water molecules on a surface is expected to lead to a lower ice nucleation rate and may enhance the macroscopic anti-icing properties of a surface.

Effects of surface temperature and Weber number on the dynamic and freezing behavior of impacting water droplets on a superhydrophobic ultra-cold surface

The dynamic and freezing behavior of a water droplet impacting a superhydrophobic cold surface is worthy of investigation. In this study, experiments are conducted to examine the impact and freezing of a water droplet on a cold superhydrophobic surface whose temperature changes in a wide range between −10 °C and −60 °C. A numerical model that introduces a continuous energy balance equation is developed to investigate the process numerically. The effects of surface temperature, Weber number, and initial droplet temperature on the droplet morphology, spread factor, contact time, and rebound height are investigated. The droplet exhibits three different behaviors as the surface temperature decreases: full rebound, partial rebound, and full adhesion. For the full rebound case, the results indicate that the growth rate of the contact time with decreasing surface temperature increases as the Weber number decreases. For the full adhesion case, the variation in the surface temperature minimally affects the dynamic behavior of the droplet impacting on an ultracold superhydrophobic surface (below −40 °C). The effect of surface temperature on the maximum spread factor is more pronounced at higher Weber numbers. Additionally, the ice nucleation rate is analyzed theoretically. The results show that the nucleation rate of droplets impacting an ultracold surface remains almost constant regardless of the surface temperature and surface roughness. Moreover, a regime map showing the different droplet morphologies correlating with the surface temperature and Weber number is established. The critical surface temperatures for different droplet morphologies of supercooled and room-temperature droplets are analyzed. This study allows us to better understand the dynamic and heat transfer mechanisms involved in the impact and freezing of a water droplet on a superhydrophobic surface.

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.

Deposition freezing, pore condensation freezing and adsorption: three processes, one description?

Abstract. Heterogeneous ice nucleation impacts the hydrological cycle and climate through affecting cloud microphysical state and radiative properties. Despite decades of research, a quantitative description and understanding of heterogeneous ice nucleation remains elusive. Parameterizations are either fully empirical or heavily rely on classical nucleation theory (CNT), which does not consider molecular-level properties of the ice-nucleating particles – which can alter ice nucleation rates by orders of magnitude through impacting pre-critical stages of ice nucleation. The adsorption nucleation theory (ANT) of heterogeneous droplet nucleation has the potential to remedy this fundamental limitation and provide quantitative expressions in particular for heterogeneous freezing in the deposition mode (the existence of which has even been questioned recently). In this paper we use molecular simulations to understand the mechanism of deposition freezing and compare it with pore condensation freezing and adsorption. Based on the results of our case study, we put forward the plausibility of extending the ANT framework to ice nucleation (using black carbon as a case study) based on the following findings: (i) the quasi-liquid layer at the free surface of the adsorbed droplet remains practically intact throughout the entire adsorption and freezing process; therefore, the attachment of further water vapor to the growing ice particles occurs through a disordered phase, similar to liquid water adsorption. (ii) The interaction energies that determine the input parameters of ANT (the parameters of the adsorption isotherm) are not strongly impacted by the phase state of the adsorbed phase. Thus, not only is the extension of ANT to the treatment of ice nucleation possible, but the input parameters are also potentially transferable across phase states of the nucleating phase at least for the case of the graphite/water model system.

Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic

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

On the possible locus of the liquid-liquid critical point in real water from studies of supercooled water using the TIP4P/Ice model.

One of the most accepted hypothesis to explain the anomalous behavior of water is the presence of a critical point between two liquids, the liquid-liquid critical point (LLCP), buried within the deep supercooled regime. Unfortunately, such hypothesis is hard to be experimentally confirmed due to fast freezing. Here, we show that the TIP4P/Ice water potential shifted by 400 bar can reproduce with unprecedented accuracy the experimental isothermal compressibility of water and its liquid equation of state for a wide pressure and temperature range. We find, both by extrapolation of response function maxima and by a Maxwell construction, that the location of the model LLCP is consistent with previous calculations. According to the pressure shift needed to recover the experimental behavior of supercooled water, we estimate the experimental LLCP to be located around 1250 bar and 195K. We use the model to estimate the ice nucleation rate (J) in the vicinity of the hypothesized LLCP experimental location and obtain J = 1024 m-3 s-1. Thereby, experiments where the ratio between the cooling rate and the sample volume is equal or larger than the estimated nucleation rate could probe liquid-liquid equilibrium before freezing. Such conditions are not accessible in common experiments with microdroplets cooled at a few kelvin per second, but they could be, for instance, using nanodroplets of around 50nm radius observed in a millisecond timescale.

Micro-thermography for imaging ice crystal growth and nucleation inside non-transparent materials

Ice crystal growth and nucleation rate measurements are usually done using light microscopy in liquid and transparent samples. Yet, the understanding of important practical problems depends on monitoring ice growth inside solid materials, for example how rapid ice growth leads to structural damage of food, or how the final structure of cementitious materials is affected by ice during curing. Imaging crystal growth inside solid materials cannot be done with visible light and is intrinsically more challenging than visible light imaging. Thermography is a technique that uses thermal (infrared) cameras to monitor temperature changes in a material, and it has been used to provide a qualitative description of ice propagation with a low spatial resolution. Here, we describe a method that uses a novel micro-thermography system to image ice nucleation and growth inside non-transparent samples. This method relies on two major components: a cold stage with accurate temperature control (±0.001 °C) and a thermal camera with high spatial and temperature resolution. Our experiments include imaging of ice formation and growth in pure water first and then inside plant leaves used as a model for a non-transparent material. An ice growth rate of 2.2 mm/s was measured inside a plant leaf at -12 °C, and ice nucleation in single plant cells was observed as a hotspot having a diameter of 160 µm. The results presented here provide an experimental proof that high-quality imaging of ice growth is achievable, thus paving the way for quantitative measurements of ice growth kinetics and ice nucleation in solid materials.

Ice-nucleating agents in sea spray aerosol identified and quantified with a holistic multimodal freezing model.

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