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At least 19 records

Global Simulations Suggest Biomass Burning Aerosol Emissions From Grassland Fires Could Be Important Ice Nucleating Particles

Ice nucleating particles (INP) capable of nucleating ice crystals via immersion freezing at temperatures above approximately −35°C may strongly influence cloud glaciation, with implications for global precipitation and climate feedback. In addition to mineral dust, soil dust, and marine organics, laboratory and field measurements suggest biomass burning aerosols (BBA) can act as immersion-mode INP between around −30°C and −15°C. However, the contribution of BBA to the global INP budget remains poorly understood due to poor knowledge of which fuels yield INPs, uncertainties in global coverage of those fuels, and unknown size distributions of the INPs in the BBA. Nonetheless, with some understanding of these uncertainties from sensitivity studies, the relative importance of ice nucleation activity of BBA compared to other INP sources can be quantified. In this work, we investigate the potential global importance of BBA as INP using a global aerosol-climate model, specifically the UK Met Office Unified Model (UM). We evaluate the model using field campaign data sets. We examine potential uncertainties in fuel types and particle sizes on BBA-based INP concentrations. Averaged over June–September between 15°S and 50°S, BBA is a more important INP than dust and marine INP about 30% of the time at altitudes with temperatures between −30°C and −20°C. Our simulations therefore suggest BBA INPs may be at least as important as mineral dust and marine INP over the atmospheric regions and seasons where grassland fires are frequent.

Gohil, Kanishk [Carnegie Mellon University, Pittsb↗

A biogenic secondary organic aerosol source of cirrus ice nucleating particles

Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at –46°C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L –1 . Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Abundance and Sources of Ice Nucleating Particles Within Alaskan Ice Fog

Abstract The Alaskan Layered Pollution and Chemical Analysis (ALPACA) field campaign included deployment of a suite of atmospheric measurements in January–February 2022 with the goal of better understanding atmospheric processes and pollution under cold and dark conditions in Fairbanks, Alaska. We report on measurements of particle composition, particle size, ice nucleating particle (INP) composition, and INP size during an ice fog period (29 January–3 February). During this period, coarse particulate matter (PM 10 ) concentrations increased by 150% in association with a decrease in air temperature, a stronger temperature inversion, and relatively stagnant conditions. Results also show a 18%–78% decrease in INPs during the ice fog period, indicating that particles had activated into the ice fog via nucleation. Peroxide and heat treatments performed on INPs indicated that, on average, the largest contributions to the INP population were heat‐labile (potentially biological, 63%), organic (31%), then inorganic (likely dust, 6%). Measurements of levoglucosan and bulk and single‐particle composition corroborate the presence of dust and aerosols from combustion sources. Heat‐labile and organic INPs decreased during the peak period of the ice fog, indicating those were preferentially activated, while inorganic INPs increased, suggesting they remained as interstitial INPs. In general, INP concentrations were unexpectedly high in Fairbanks compared to other locations in the Arctic during winter. The fact that these INPs likely facilitated ice fog formation in Fairbanks has implications for other high latitude locations subject to the hazards associated with ice fog.

Meteorology & Atmospheric Sciences↗

The Portable Ice Nucleation Experiment (PINE): a new online instrument for laboratory studies and automated long-term field observations of ice-nucleating particles

Atmospheric ice-nucleating particles (INPs) play an important role in determining the phase of clouds, which affects their albedo and lifetime. A lack of data on the spatial and temporal variation of INPs around the globe limits our predictive capacity and understanding of clouds containing ice. Automated instrumentation that can robustly measure INP concentrations across the full range of tropospheric temperatures is needed in order to address this knowledge gap. In this study, we demonstrate the functionality and capacity of the new Portable Ice Nucleation Experiment (PINE) to study ice nucleation processes and to measure INP concentrations under conditions pertinent for mixed-phase clouds, with temperatures from about -10 to about -40°C. PINE is a cloud expansion chamber which avoids frost formation on the cold walls and thereby omits frost fragmentation and related background ice signals during the operation. The development, working principle and treatment of data for the PINE instrument is discussed in detail. We present laboratory-based tests where PINE measurements were compared with those from the established AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber. Within experimental uncertainties, PINE agreed with AIDA for homogeneous freezing of pure water droplets and the immersion freezing activity of mineral aerosols. Results from a first field campaign conducted at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) observatory in Oklahoma, USA, from 1 October to 14 November 2019 with the latest PINE design (a commercially available PINE chamber) are also shown, demonstrating PINE's ability to make automated field measurements of INP concentrations at a time resolution of about 8 min with continuous temperature scans for INP measurements between -10 and -30°C. During this field campaign, PINE was continuously operated for 45 d in a fully automated and semi-autonomous way, demonstrating the capability of this new instrument to also be used for longer-term field measurements and INP monitoring activities in observatories.

54 ENVIRONMENTAL SCIENCES↗

Long-term measurements of ice nucleating particles at Atmospheric Radiation Measurement (ARM) sites worldwide

Ice nucleating particles (INPs) play a critical role in cloud microphysics and precipitation formation, yet long-term, spatially extensive observational datasets remain limited. Here, we present one of the most comprehensive publicly available datasets of immersion-mode INP concentrations using a single analytical method, generated through the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility. INP filter samples have been collected across a broad range of environments – including agricultural plains, Arctic coastlines, high-elevation mountain sites, marine regions, and urban areas – via fixed observatories, mobile facility deployments, and vertically-resolved tethered balloon system operations. We describe the standardized processing and quality assurance pipeline, from filter collection and processing using the Ice Nucleation Spectrometer to final data products archived on the ARM Data Discovery portal. The dataset includes both total INP concentrations and selectively treated samples, allowing for classification of biological, organic, and inorganic INP types. It features a continuous 5-year record of INP measurements from a central U.S. site, with data collection still ongoing. Seasonal and site-specific differences in INP concentrations are illustrated through intercomparisons at −10 and −20 °C, revealing distinct regional sources and atmospheric drivers. We also outline mechanisms for researchers to access existing data, request additional sample analyses, and propose future field campaigns involving ARM INP measurements. This dataset supports a wide range of scientific applications, from observational and mechanistic studies to model development, and provides critical constraints on aerosol-cloud interactions across diverse atmospheric regimes (Creamean et al., 2024, 2020b; https://doi.org/10.5439/1770816).

Creamean, Jessie M. [Colorado State Univ., Fort Co↗

How the Emitted Size Distribution and Mixing State of Feldspar Affect Ice Nucleating Particles in a Global Model

The effect of aerosol particles on ice nucleation and, in turn, the formation of ice and mixed phase clouds is recognized as one of the largest sources of uncertainty in climate prediction. We apply an improved dust mineral specific aerosol module in the NASA GISS Earth System ModelE, which takes into account soil aggregates and their fragmentation at emission as well as the emission of large particles. We calculate ice nucleating particle concentrations from K-feldspar abundance for an active site parameterization for a range of activation temperatures and external and internal mixing assumption. We find that the globally averaged INP concentration is reduced by a factor of two to three, compared to a simple assumption on the size distribution of emitted dust minerals. The decrease can amount to a factor of five in some geographical regions. The results vary little between external and internal mixing and different activation temperatures, except for the coldest temperatures. In the sectional size distribution, the size range 24 micrometer contributes the largest INP number.

Perlwitz, Jan P.↗

On the Role of Airborne Ice Nucleating Particles in Primary and Secondary Ice Formation Processes in Convective Midlatitude Clouds

Abstract Formation of ice in mixed-phase clouds may proceed via primary nucleation and secondary ice production (SIP). Primary nucleation involves the presence of ice nucleating particles (INPs), while SIP follows primary nucleation, resulting in ice crystal number concentrations N ice exceeding the number of INPs. The ice formation pathways in young congestus clouds are not well understood nor are the environmental conditions favorable for the onset of SIP. Coincident airborne measurements of INPs and N ice collected during the Secondary Production of Ice in Cumulus Experiment (SPICULE) campaign over the U.S. central Great Plains are reported for young congestus clouds. Number concentrations of INPs and N ice at temperatures between −10° and −20°C were used to categorize whether SIP was active in each analyzed cloud pass. Observational data suggested that fragmentation of freezing droplets (FFDs) was occurring and the most likely SIP mechanism for ice enhancement during the early stages of the sampled clouds, where higher cloud-base temperatures and stronger updrafts produced conditions favorable for the onset of FFD. Simple model simulations of a congestus cloud were used to compare predictions of N ice from newly implemented SIP mechanisms (including FFD) alongside those from the existing Hallett–Mossop (HM) mechanism. Although predicted N ice , when all SIP mechanisms were active, was in good agreement with observations, the dominant SIP mechanism in the model was predicted to be HM. The rate of heterogeneous freezing in raindrops was likely inhibiting realistic FFD rates in the simulated cloud. These discrepancies between the observations and simulations underscore the need for extended laboratory studies to formulate improved model representations of SIP in convective clouds.

Patnaude, Ryan J. [Department of Atmospheric Scien↗

Pragmatic protocols for working cleanly when measuring ice nucleating particles

We report that measuring ice nucleating particles (INPs) is critical for understanding, and modeling, cloud formation, reflectivity, and precipitation patterns. However, because INPs are very rare in the atmosphere, but abundant—sometimes alarmingly so—in the dust that covers all work surfaces, contamination during processing of collected aerosol samples can be a significant hindrance to obtaining accurate measures of INPs. In preparing this technical note, we questioned the cleanliness of every collection and processing step involved in making immersion freezing measurements of INPs re-suspended from filter samples. The aim was to identify, and then minimize, all potential sources of significant contamination, including containers and tools used to store filters and prepare liquid suspensions, gloves, work surfaces, and the polymerase chain reaction (PCR) trays commonly used for sample analysis. While plasticware released few INPs, most gloves readily shed them, but this can be mitigated by using washed cleanroom vinyl or polyethylene gloves. Work surfaces, even those that had been cleaned, were prodigious reservoirs of contaminating INPs, but simply covering them with aluminum foil will provide an INP-free surface. By applying these practices, we developed a method to reduce the background level of INPs on Nuclepore™ polycarbonate filters in our tests to 0 at -25 °C and < 20 at -27 °C, making them suitable for use in all sampling environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Application of aerosol-ice nucleating particle closure to establish the leading parameters governing ice crystal number concentration under commonly observed mixed-phase cloud conditions

This is the final technical report for DOE DE-SC0021034 award entitled “Application of aerosol-ice nucleating particle closure to establish the leading parameters governing ice crystal number concentration under commonly observed mixed-phase cloud conditions”. The overarching objective of this project was to gain a predictive understanding of the processes that lead from aerosols to ice-nucleating particles (INPs) to ice crystal number concentrations (ICNCs) in stratiform mixed-phase clouds where supercooled water droplets and ice crystals coexist, and to inform climate model parameterizations. During this four-year project we addressed the three main research goals of this objective: 1) Study the aerosol-INP link; 2) Develop an aerosol-cloud column model (AC-1D); and 3) Study the INP-ICNC link. Those activities significantly advanced our predictive understanding of how to represent INPs in could models and its implications on ice crystal number concentrations. The results have been published in five peer-reviewed publications with three more in review and preparation. It allowed for collaboration resulting in additional fourteen peer-reviewed publications that are concerned with the objective of this research project. This research has been communicated to the scientific community at national and international meetings and conferences by numerous talks, seminars, and posters including fifteen invited presentations. This project allowed training of four graduate students and one postdoctoral research associate resulting in one M.S. thesis and advancement to Ph.D. candidacy.

54 ENVIRONMENTAL SCIENCES↗

Ejection of Dust From the Ocean as a Potential Source of Marine Ice Nucleating Particles

Oceans are, generally, relatively weak sources of ice nucleating particles (INPs). Thus, dust transported from terrestrial regions can dominate atmospheric INP concentrations even in remote marine regions. Studies of ocean-emitted INPs have focused upon sea spray aerosols containing biogenic species. Even though large concentrations of dust are transported over marine regions, resuspended dust has never been explicitly considered as another possible source of ocean-emitted INPs. Current models assume that deposited dust is not re-emitted from surface waters. Our laboratory studies of aerosol particles produced from coastal seawater and synthetic seawater doped with dust show that dust can indeed be ejected from water during bubble bursting. INP concentration measurements show these ejected dust particles retain ice nucleating activity. Doping synthetic seawater to simulate a strong dust deposition event produced INPs active at temperatures colder than -13 °C and INP concentrations one to two orders of magnitude greater than either lab sea spray or marine boundary layer measurements. The relevance of these laboratory findings is highlighted by single particle composition measurements along the Californian coast where at least 9% of dust particles were mixed with sea salt. Additionally, global modeling studies show that resuspension of dust from the ocean could exert the most impact over the Southern Ocean, where ocean-emitted INPs are thought to dominate atmospheric INP populations. More work characterizing the factors governing the resuspension of dust particles is required to understand the potential impact upon clouds.

54 ENVIRONMENTAL SCIENCES↗

Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic

Abstract. Formation of atmospheric ice plays a crucial role in the microphysical evolution of mixed-phase and cirrus clouds and thus climate. How aerosol particles impact ice crystal formation by acting as ice-nucleating particles (INPs) is a subject of intense research activities. To improve understanding of atmospheric INPs, we examined daytime and nighttime particles collected during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign conducted in summer 2017. Collected particles, representative of a remote marine environment, were investigated for their propensity to serve as INPs in the immersion freezing (IMF) and deposition ice nucleation (DIN) modes. The particle population was characterized by chemical imaging techniques such as computer-controlled scanning electron microscopy with energy-dispersive X-ray analysis (CCSEM/EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine-structure spectroscopy (STXM/NEXAFS). Four major particle-type classes were identified where internally mixed inorganic–organic particles make up the majority of the analyzed particles. Following ice nucleation experiments, individual INPs were identified and characterized by SEM/EDX. The identified INP types belong to the major particle-type classes consisting of fresh sea salt with organics or processed sea salt containing dust and sulfur with organics. Ice nucleation experiments show IMF events at temperatures as low as 231 K, including the subsaturated regime. DIN events were observed at lower temperatures of 210 to 231 K. IMF and DIN observations were analyzed with regard to activated INP fraction, ice-nucleation active site (INAS) densities, and a water activity-based immersion freezing model (ABIFM) yielding heterogeneous ice nucleation rate coefficients. Observed IMF and DIN events of ice formation and corresponding derived freezing rates demonstrate that the marine boundary layer aerosol particles can serve as INPs under typical mixed-phase and cirrus cloud conditions. The derived IMF and DIN parameterizations allow for implementation in cloud and climate models to evaluate predictive effects of atmospheric ice crystal formation.

54 ENVIRONMENTAL SCIENCES↗

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↗

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↗

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↗

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

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

54 ENVIRONMENTAL SCIENCES↗

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.

54 ENVIRONMENTAL SCIENCES↗

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

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

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗