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DOE OSTI2022

Ice‐Nucleating Particles That Impact Clouds and Climate: Observational and Modeling Research Needs

Abstract Atmospheric ice‐nucleating particles (INPs) play a critical role in cloud freezing processes, with important implications for precipitation formation and cloud radiative properties, and thus for weather and climate. Additionally, INP emissions respond to changes in the Earth System and climate, for example, desertification, agricultural practices, and fires, and therefore may introduce climate feedbacks that are still poorly understood. As knowledge of the nature and origins of INPs has advanced, regional and global weather, climate, and Earth system models have increasingly begun to link cloud ice processes to model‐simulated aerosol abundance and types. While these recent advances are exciting, coupling cloud processes to simulated aerosol also makes cloud physics simulations increasingly susceptible to uncertainties in simulation of INPs, which are still poorly constrained by observations. Advancing the predictability of INP abundance with reasonable spatiotemporal resolution will require an increased focus on research that bridges the measurement and modeling communities. This review summarizes the current state of knowledge and identifies critical knowledge gaps from both observational and modeling perspectives. In particular, we emphasize needs in two key areas: (a) observational closure between aerosol and INP quantities and (b) skillful simulation of INPs within existing weather and climate models. We discuss the state of knowledge on various INP particle types and briefly discuss the challenges faced in understanding the cloud impacts of INPs with present‐day models. Finally, we identify priority research directions for both observations and models to improve understanding of INPs and their interactions with the Earth System.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Deciphering the incipient phases of ice-mineral interactions as a precursor of physical weathering

Atmospheric ice formation influences Earth’s global hydrological cycle and is widely studied. In contrast, the intricacies of freeze-thaw processes in natural soils, such as whether ice nucleation on mineral surfaces is affected by biological activity, needs additional insight. In-situ ice formation on unreacted grains and grains exposed to field and laboratory weathering conditions was studied at the submicron scale using an ice nucleation chamber interfaced with an environmental scanning electron microscope. We found that ice nucleation activity differed by treatment. Unreacted grains and fungal-mineral interfaces displayed ice formation along edges and fractures. Conversely, grains with mineral coatings, seemingly from biological activity, exhibited water uptake and ice nucleation on the coatings themselves. Our results suggest that in natural soils, mineral coatings can influence where and how ice forms. This ultimately affects weathering and nutrient release to the biosphere, with direct consequences for interactions between the atmosphere and geosphere.

Lybrand, Rebecca A.↗

DOE OSTI2020

ExINP-ENA Ice-Nucleating Particle Concentrations - PINE

This data set comprises cumulative ambient ice-nucleating particle (INP) concentrations measured at the U.S. Department of Energy's Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) observatory on Graciosa Island, Azores (39.0916° N, 28.0257° W). Our INP data were generated using a combination of online instruments, the Portable Ice Nucleation Experiment chamber (PINE), and an offline assay instrument, the West Texas Cryogenic Refrigerator Applied to Freezing Test system (WT-CRAFT), for aerosol particle samples collected on polycarbonate filters (with 0.2-micron diameter pores).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Ice nucleating particle concentrations measured by the CSU-CFDC during the AGINSGP field experiment

Real-time, immersion mode ambient ice nucleating particle (INP) concentrations were measured at ARM’s Southern Great Plains (SGP) site during the AGINSGP field experiment using a continuous flow diffusion chamber (CFDC) from Colorado State University (CSU). The CSU-CFDC is an ice-thermal gradient diffusion chamber that optically detects the freezing of single aerosol particles (Rogers 1988; Rogers et al. 2001; and Eidhammer et al. 2010). The instrument was located in the guest instrument facility (GIF) and measured INP concentrations from April 8th to April 29th. Air was drawn into the GIF through custom aluminum stack inlets (6” inner diameter) attached vertically to the outer GIF wall and the GIF outside platform. A blower pulled air through the stacks at a velocity of 1 m/s. Aerosol instruments subsampled via wall ports, through either 3/8” or 1/4" copper lines, depending on sample flow of the instrument. Rogers, D. C., Development of a continuous flow thermal gradient diffusion chamber for ice nucleation studies, Atmospheric Research, 22(2), 149-181, doi:10.1016/0169-8095(88)90005-1, 1988. Rogers, D. C., P. J. DeMott, S. M. Kreidenweis and Y. Chen, A continuous flow diffusion chamber for airborne measurements of ice nuclei, J. Atmos. Oceanic Technol., 18, 725-741, doi:10.1175/1520-0426(2001)018<0725:ACFDCF>2.0.CO;2, 2001. Eidhammer, T., DeMott, P. J., Prenni, A. J., Petters, M. D., Twohy, C. H., Rogers, D. C., Stith, J., Heymsfield, A., Wang, Z., Haimov, S., French, J., Pratt, K., Prather, K., Murphy, S., Seinfeld, J., Subramanian, R., and Kreidenweis, S. M., Ice initiation by aerosol particles: Measured and predicted ice nuclei concentrations versus measured ice crystal concentrations in an orographic wave cloud, J. Atmos. Sci., 67, 2417-2436, doi:10.1175/2010JAS3266.1, 2010

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

ExINP NSA Ice Nucleating Particle Concentrations

This data set comprises cumulative ambient ice-nucleating particle (INP) concentrations measured at the National Oceanic and Atmospheric Administration's (NOAA’s) Barrow Atmospheric Baseline Observatory (71.3230° N, 156.6114° W, “BRW” hereafter), next to the Atmospheric Radiation Measurement (ARM) North Slope of Alaska (NSA) site and ~ 6 km northeast of the town of Utqiaġvik. Our INP abundance data were generated using a combination of online instrument, the Portable Ice Nucleation Experiment chamber ver. 3 (PINE-03), and an offline cold stage, the West Texas Cryogenic Refrigerator Applied to Freezing Test system (WT-CRAFT). Our online INP data are all from the Examining the Ice-Nucleating Particles from NSA (ExINP-NSA) campaign conducted from October 19, 2021 to May 24, 2024. The offline INP concentration analysis was performed at West Texas A&M University for aerosol particle samples collected on polycarbonate filters (with 0.2-micron diameter pores). The PINE-03 measurements, as well as sampling activities for offline INP measurements, were conducted using the BRW site. An inset laminar sampling stack was mounted to the instrument platform, allowing PINE-03 to intake particle-laden air. For most of the campaign period, the semi-autonomous PINE-03 chamber was remotely controlled from West Texas A&M University using the LabView interface through the BeyondTrust remote-access console. PINE-03 was set to conduct an immersion freezing expansion experiment (i.e., simulated adiabatic cooling along with RHw at or above 100%). Except during the scheduled maintenance periods, the time resolution of each expansion experiment was approximately 12 minutes. PINE-03 continuously measured INP concentrations during the entire campaign without any substantial breaks. For most of the campaign period, PINE scanned its set-point vessel air temperatures from -14 °C to -31 °C and back to -14 °C about every 120 minutes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

ExINP NSA Ice Nucleating Particle Concentrations

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Multi-seasonal measurements of the ground-level atmospheric ice-nucleating particle abundance on the North Slope of Alaska

Atmospheric ice-nucleating particles (INPs) are an important subset of aerosol particles that are responsible for the heterogeneous formation of ice crystals. INPs modulate the arctic cloud phase (liquid vs. ice), resulting in implications for radiative feedbacks. The number of arctic INP studies investigating specific INP episodes or sources increased recently. However, existing studies are based on short-duration field data, and long-term datasets are lacking. Continuous, long-term measurements are key to determining the abundance and variability of ambient arctic INPs and constraining aerosol–cloud interactions, e.g., to verify and/or improve simulations of mixed-phase clouds. Here, we present a new long-duration INP dataset from the Arctic: 2 years of predominantly immersion-mode INP concentrations (n INP ) measured continuously at the National Oceanic and Atmospheric Administration's Barrow Atmospheric Baseline Observatory (BRW) on the North Slope of Alaska. A portable ice nucleation experiment chamber (PINE-03), which simulates adiabatic expansion cooling, was used to directly measure the ground-level INP abundance with an approximately 12 min time resolution from October 2021 to December 2023. We document PINE-03 n INP measurements as well as estimated ice nucleation active surface site density (n s ) over a wide range of heterogeneous freezing temperatures from −16 to −31 °C from which we introduce new season-specific parameterizations suitable for modeling mixed-phase clouds. Collocated aerosol and meteorological data were analyzed to assess the correlation between ambient n INP , air mass origin region, and meteorological variability. Our findings suggest (1) very high freezing efficiency of INPs across the measured temperatures (n s ≈ 2×10 8 –10 10 m −2 for −16 to −31 °C), which is a factor of 10–1000 times greater efficiency as compared to that found in the previous mid-latitude INP measurements in fall using the same instrument; (2) surprisingly high n INP (≥ 1 L −1 at −25 °C) for the examined temperatures throughout the year that were not measured by PINE-03 at other sites; and (3) high n INP in spring, possibly related to arctic haze episodes. Relatively low concentrations of aerosol surface area and contrasting high-INP concentrations at BRW relative to mid-latitude sites are the possible reasons for the observed high freezing efficiency.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

ExINP-ENA Ice-Nucleating Particle Concentrations - CRAFT

47-mm Nuclepore filter sampler, West Texas Cryogen↗

NASA NTRS1981

Homogeneous condensation - Freezing nucleation rate measurements for small water droplets in an expansion cloud chamber

Experimental data on ice nucleation, presented in an earlier paper, are analyzed to yield information about the homogeneous nucleation rate of ice from supercooled liquid and the heights of energy barriers to that nucleation. The experiment consisted of using an expansion cloud chamber to nucleate from the vapor a cloud of supercooled pure water drops and the observation of the fraction of drops which subsequently froze. The analysis employed standard classical homogeneous nucleation theory. The data are used to extract the first experimental measurement (albeit indirect) of the activation energy for the transfer of a water molecule across the liquid-ice interface at temperatures near -40 C. The results provide further evidence that the local liquid structure becomes more icelike as the temperature is lowered.

Hagen, D. E.↗

DOE OSTI2020

Complex plant-derived organic aerosol as ice-nucleating particles – more than the sums of their parts?

Quantifying the impact of complex organic particles on the formation of ice crystals in clouds remains challenging, mostly due to the vast number of different sources ranging from sea spray to agricultural areas. In particular, there are many open questions regarding the ice nucleation properties of organic particles released from terrestrial sources such as decaying plant material. In this work, we present results from laboratory studies investigating the immersion freezing properties of individual organic compounds commonly found in plant tissue and complex organic aerosol particles from vegetated environments, without specifically investigating the contribution from biological particles, which may contribute to the overall ice nucleation efficiency observed at high temperatures. To characterize the ice nucleation properties of plant-related aerosol samples for temperatures between 242 and 267 K, we used the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber and the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT), which is a droplet freezing assay. Individual plant components (polysaccharides, lignin, soy and rice protein) were mostly less ice active, or similarly ice active, compared to microcrystalline cellulose, which has been suggested by recent studies to be a proxy for quantifying the primary cloud ice formation caused by particles originating from vegetation. In contrast, samples from ambient sources with a complex organic matter composition (agricultural soils and leaf litter) were either similarly ice active or up to 2 orders of magnitude more ice active than cellulose. Of all individual organic plant components, only carnauba wax (i.e., lipids) showed a similarly high ice nucleation activity as that of the samples from vegetated environments over a temperature range between 245 and 252 K. Hence, based on our experimental results, we suggest considering cellulose as being representative for the average ice nucleation activity of plant-derived particles, whereas lignin and plant proteins tend to provide a lower limit. In contrast, complex biogenic particles may exhibit ice nucleation activities which are up to 2 orders of magnitude higher than observed for cellulose, making ambient plant-derived particles a potentially important contributor to the population of ice-nucleating particles in the troposphere, even though major uncertainties regarding their transport to cloud altitude remain.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Implications of Aerosol Physicochemical Properties Including Ice Nucleation at ARM Mega Sites for Improved Understanding of Microphysical Atmospheric Cloud Processes (Final Technical Report)

Continuous, long-term measurements of atmospheric ice-nucleating particles (INPs) that influence clouds and precipitation were conducted to investigate the abundance and variability of ground-level INPs across the world. Three field campaigns were organized by the DOE Atmospheric Radiation Measurement (ARM) program, including Examining INP from Southern Great Plains (ExINP-SGP, 2019), Examining INP from Eastern North Atlantic (ExINP-ENA, 2020 – 2021), and Examining INP from North Slope of Alaska (ExINP-NSA, 2021 – 2024). Additional small-scale supporting field experiments were performed in 2019 and 2021 to collect airborne particulate matter at SGP for complementary laboratory characterization of the particles’ physical and chemical properties [Aerosol-Ice Formation Closure Pilot Study (AEROICESTUDY), 2019; ExINP-SGP II, 2021]. In these studies, the PI’s team measured INP concentration with both real-time and laboratory measurements in a wide range of freezing temperatures ($T$ from 0 °C to about –30 °C). This project elucidated spatial variability and seasonality in the abundance of immersion mode active INPs across three ARM sites using a single instrument, a Portable Ice Nucleation Experiment (PINE) chamber version 03 (PINE-03 hereafter). Collocated aerosol and meteorological data were analyzed to assess the correlation between ambient INP abundance, air mass origin region, and meteorological variability. Our findings suggest very high freezing efficiency of INPs at the NSA site across the measured temperatures (ice nucleation active surface site density, $n_s(T)$, $\approx 2 \times 10^{8} - 10^{10}$ m -2 for from –16 to –31 °C), which is a factor of 10 – 1000 times greater efficiency as compared to that found in the previous mid-latitude INP measurements in autumn using the same instrument; surprisingly high INP abundance ($\ge 1 \text{ L}^{-1}$ at –25 °C) for the examined temperatures throughout the year that PINE-03 did not measure at other sites; and high INP concentration in spring, possibly related to arctic haze episodes.

58 GEOSCIENCES↗

DOE OSTI2023

Metal Oxide Particles as Atmospheric Nuclei: Exploring the Role of Metal Speciation in Heterogeneous Efflorescence and Ice Nucleation

Mineral dust can indirectly impact climate by nucleation of atmospheric solids, for example, by heterogeneously nucleating ice in mixed-phase clouds or by impacting the phase of aerosols and clouds through contact nucleation. The effectiveness toward nucleation of individual components of mineral dust requires further study. Here, the nucleation behavior of metal oxide nanoparticle components of atmospheric mineral dust is investigated. A long-working-distance optical trap is used to study contact and immersion nucleation of ammonium sulfate by transition-metal oxides, and an environmental chamber is used to probe depositional ice nucleation on metal oxide particles. Previous theory dictates that ice nucleation and heterogeneous nucleation of atmospheric salts can be impacted by several factors including morphology, lattice match, and surface area. Here, we observe a correlation between the cationic oxidation states of the metal oxide heterogeneous nuclei and their effectiveness in causing nucleation in both contact efflorescence mode and depositional freezing mode. In contrast to the activity of contact efflorescence, the same metal oxide particles did not cause a significant increase in efflorescence relative humidity when immersed in the droplet. In conclusion, these experiments suggest that metal speciation, possibly as a result of cationic charge sites, may play a role in the effectiveness of nucleation that is initiated at particle surfaces.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1997

SUCCESS Evidence for Cirrus Cloud Ice Nucleation Mechanisms

During the SUCCESS mission, several measurements were made which should improve our understanding of ice nucleation processes in cirrus clouds. Temperature and water vapor concentration were made with a variety of instruments on the NASA DC-8. These observations should provide accurate upper tropospheric humidities. In particular, we will evaluate what humidities are required for ice nucleation. Preliminary results suggest that substantial supersaturations frequently exist in the upper troposphere. The leading-edge region of wave-clouds (where ice nucleation occurs) was sampled extensively at temperatures near -40 and -60C. These observations should give precise information about conditions required for ice nucleation. In addition, we will relate the observed aerosol composition and size distributions to the ice formation observed to evaluate the role of soot or mineral particles on ice nucleation. As an alternative technique for determining what particles act as ice nuclei, numerous samples of aerosols inside ice crystals were taken. In some cases, large numbers of aerosols were detected in each crystal, indicating that efficient scavenging occurred. Analysis of aerosols in ice crystals when only one particle per crystal was detected should help with the ice nucleation issue. Direct measurements of the ice nucleating activity of ambient aerosols drawn into airborne cloud chambers were also made. Finally, measurements of aerosols and ice crystals in contrails should indicate whether aircraft exhaust soot particles are effective ice nuclei.

Jensen, Eric↗

DOE OSTI2020

AEROICESTUDY Colorado State University Continuous Flow Diffusion Chamber (CFDC) version R0

This dataset comprises measurements of atmospheric ice nucleating particle (INP) number concentrations at ARM's Southern Great Plains (SGP) Site Guest Instrument Facility (GIF), in Lamont, Oklahoma, during the 2019 Aerosol-Ice Formation Closure Pilot Study (AEROICESTUDY). The results reported here are from the Colorado State University Continuous Flow Diffusion Chamber (CFDC-1H) and represent real-time measurements of ambient INPs.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

A new method for operating a continuous flow diffusion chamber to investigate immersion freezing: assessment and performance study

Glaciation in mixed-phase clouds predominately occurs through the immersion freezing mode where ice nucleating particles (INPs) immersed within supercooled droplets induce nucleation of ice. Currently, model representations of this process are a large source of uncertainty in simulating cloud radiative properties, and to constrain these estimates, continuous flow diffusion chamber (CFDC)-style INP devices are commonly used to assess the immersion freezing efficiencies of INPs. In this study, a new approach was explored to operating such an ice chamber that provides maximum activation of particles without droplet breakthrough and correction factor ambiguity to obtain high-quality INP measurements in a manner that has not been demonstrated as possible previously. The conditioning section of the chamber was maintained at ~ –20 °C and water relative humidity (RH w ) ~ 113 % conditions to maximize the droplet activation, and the droplets were supercooled with an independently temperature-controlled nucleation section at a steady cooling rate (0.5 °C min –1 ) to induce the freezing of droplets and evaporation of unfrozen droplets. The performance of the modified ice chamber was evaluated using four INP species: K-feldspar, illite-NX, Argentinian soil dust, and airborne arable dust that had shown ice nucleation over a wide span of supercooled temperatures. Dry dispersed and size-selected K-feldspar particles were generated in the laboratory. Illite-NX and soil dust particles were sampled during the second phase of the Fifth International Ice Nucleation Workshop (FIN-02) campaign, and airborne arable dust particles were sampled from the aerosol inlet located on the rooftop of the laboratory. The measured ice nucleation efficiencies of model aerosols with a surface active site density (n s ) metric were higher, but mostly agreed within one order of magnitude compared to literature results.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

A new method for operating a continuous-flow diffusion chamber to investigate immersion freezing: assessment and performance study

Abstract. Glaciation in mixed-phase clouds predominantly occurs through the immersion-freezing mode where ice-nucleating particles (INPs) immersed within supercooled droplets induce the nucleation of ice. Model representations of this process currently are a large source of uncertainty in simulating cloud radiative properties, so to constrain these estimates, continuous-flow diffusion chamber (CFDC)-style INP devices are commonly used to assess the immersion-freezing efficiencies of INPs. This study explored a new approach to operating such an ice chamber that provides maximum activation of particles without droplet breakthrough and correction factor ambiguity to obtain high-quality INP measurements in a manner that previously had not been demonstrated to be possible. The conditioning section of the chamber was maintained at −20 ∘C and water relative humidity (RHw) conditions of 113 % to maximize the droplet activation, and the droplets were supercooled with an independently temperature-controlled nucleation section at a steady cooling rate (0.5 ∘C min−1) to induce the freezing of droplets and evaporation of unfrozen droplets. The performance of the modified compact ice chamber (MCIC) was evaluated using four INP species: K-feldspar, illite-NX, Argentinian soil dust, and airborne soil dusts from an arable region that had shown ice nucleation over a wide span of supercooled temperatures. Dry-dispersed and size-selected K-feldspar particles were generated in the laboratory. Illite-NX and soil dust particles were sampled during the second phase of the Fifth International Ice Nucleation Workshop (FIN-02) campaign, and airborne soil dust particles were sampled from an ambient aerosol inlet. The measured ice nucleation efficiencies of model aerosols that had a surface active site density (ns) metric were higher but mostly agreed within 1 order of magnitude compared to results reported in the literature.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

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.

58 GEOSCIENCES↗

NASA NTRS1978

Rocket effluent: Its ice nucleation activity and related properties

To investigate the possibility of inadvertent weather modification from rocket effluent, aerosol samples were collected from an instrumented aircraft subsequent to the Voyager 1 and 2 launches. The aerosol's morphology, concentration, and size distribution were examined with an electron microscope. The elemental compositions of individual particles were analyzed with an X-ray energy spectrometer. Ice nucleus concentration was measured with a thermal diffusion chamber. The particles' physical and chemical properties were related to their ice nucleation activity. A laboratory experiment on rocket propellant exhaust was conducted under controlled conditions. Both laboratory and field experimental results indicated that rocket propellant exhaust can produce active ice nuclei and modify local weather in suitable meteorological conditions.

Parungo, F. P.↗