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The Alaskan Layered Pollution And Chemical Analysis (ALPACA) field experiment was a collaborative study designed to improve understanding of pollution sources and chemical processes during winter (cold climate and low-photochemical activity), to investigate indoor pollution, and to study dispersion of pollution as affected by frequent temperature inversions. A number of the research goals were motivated by questions raised by residents of Fairbanks, Alaska, where the study was held. This paper describes the measurement strategies and the conditions encountered during the January and February 2022 field experiment, and reports early examples of how the measurements addressed research goals, particularly those of interest to the residents. Outdoor air measurements showed high concentrations of particulate matter and pollutant gases including volatile organic carbon species. During pollution events, low winds and extremely stable atmospheric conditions trapped pollution below 73 m, an extremely shallow vertical scale. Tethered-balloon-based measurements intercepted plumes aloft, which were associated with power plant point sources through transport modeling. Because cold climate residents spend much of their time indoors, the study included an indoor air quality component, where measurements were made inside and outside a house to study infiltration and indoor sources. In the absence of indoor activities such as cooking and/or heating with a pellet stove, indoor particulate matter concentrations were lower than outdoors; however, cooking and pellet stove burns often caused higher indoor particulate matter concentrations than outdoors. The mass-normalized particulate matter oxidative potential, a health-relevant property measured here by the reactivity with dithiothreiol, of indoor particles varied by source, with cooking particles having less oxidative potential per mass than pellet stove particles.

The Arctic is warming faster than anywhere else on Earth, prompting glacial melt, permafrost thaw, and sea ice decline. These severe consequences induce feedbacks that contribute to amplified warming, affecting weather and climate globally. Aerosols and clouds play a critical role in regulating radiation reaching the Arctic surface. However, the magnitude of their effects is not adequately quantified, especially in the central Arctic where they impact the energy balance over the sea ice. Specifically, aerosols called ice nucleating particles (INPs) remain understudied yet are necessary for cloud ice production and subsequent changes in cloud lifetime, radiative effects, and precipitation. Here, we report observations of INPs in the central Arctic over a full year, spanning the entire sea ice growth and decline cycle. Further, these observations are size-resolved, affording valuable information on INP sources. Our results reveal a strong seasonality of INPs, with lower concentrations in the winter and spring controlled by transport from lower latitudes, to enhanced concentrations of INPs during the summer melt, likely from marine biological production in local open waters. This comprehensive characterization of INPs will ultimately help inform cloud parameterizations in models of all scales.

Knowledge of the chemical composition and mixing state of aerosols at a single-particle level is critical for gaining insights into atmospheric processes. One common tool to make these measurements is single-particle mass spectrometry. There remains a need to compare the performance of different single-particle mass spectrometers (SPMSs). An intercomparison of SPMSs was conducted at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber at the Karlsruhe Institute of Technology (KIT) in November 2014, as part of the first phase of the Fifth International Workshop on Ice Nucleation (FIN-01). In this paper we compare size distributions and mass spectra of atmospherically relevant particle types measured by five SPMSs. These include different minerals, desert and soil dusts, soot, bioaerosol (Snomax; protein granule), secondary organic aerosol (SOA), and SOA-coated mineral particles. Most SPMSs reported similar vacuum aerodynamic diameter (dva) within typical instrumental ranges from ∼100 –200 nm (lower limit) to ∼2 –3 µm (upper limit). In general, all SPMSs exhibited a wide dynamic range (up to ∼103) and high signal-to-noise ratio (up to ∼104) in mass spectra. Common spectral features with small diversities in mass spectra were found with high average Pearson's correlation coefficients, i.e., for average positive spectra ravg-pos=0.74 ± 0.12 and average negative spectra ravg-neg=0.67 ± 0.22. We found that instrument-specific detection efficiency (DE) was more dependent on particle size than particle type, and particle identification favored the use of bipolar, rather than monopolar, instruments. Particle classification from "blind experiments" showed that all instruments differentiated SOA, soot, and soil dust and detected subtle changes in the particle internal mixing but had difficulties differentiating among specific mineral types and dusts. This study helps to further understand the capabilities and limitations of the single-particle mass spectrometry technique in general and the specific performance of the instrument in characterizing atmospheric aerosol particles. [ABSTRACT FROM AUTHOR]

Heterogeneous ice nucleation in the atmosphere regulates cloud properties, such as phase (ice versus liquid) and lifetime. Aerosol particles of marine origin are relevant ice nucleating particle sources when marine aerosol layers are lifted over mountainous terrain and in higher latitude ocean boundary layers, distant from terrestrial aerosol sources. Among many particle compositions associated with ice nucleation by sea spray aerosols are highly saturated fatty acids. Previous studies have not demonstrated their ability to freeze dilute water droplets. This study investigates ice nucleation by monolayers at the surface of supercooled droplets and as crystalline particles at temperatures exceeding the threshold for homogeneous freezing. Results show the poor efficiency of long chain fatty acid (C16, C18) monolayers in templating freezing of pure water droplets and seawater subphase to temperatures of at least -30 °C, consistent with theory. This contrasts with freezing of fatty alcohols (C22 used here) at nearly 20 °C warmer. Evaporation of μL-sized droplets to promote structural compression of a C19 acid monolayer did not favor warmer ice formation of drops. Heterogeneous ice nucleation occurred for nL-sized droplets condensed on 5 to 100 μm crystalline particles of fatty acid (C12 to C20) at a range of temperatures below -28 °C. These experiments suggest that fatty acids nucleate ice at warmer than -36 °C only when the crystalline phase is present. Rough estimates of ice active site densities are consistent with those of marine aerosols, but require knowledge of the proportion of surface area comprised of fatty acids for application.

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 (PM10) 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. Plain Language Summary: The Alaskan Layered Pollution and Chemical Analysis field campaign occurred January–February 2022 with the goal of better understanding the atmosphere and atmospheric pollution during the winter in Fairbanks, Alaska. We studied a rare subset of atmospheric particles called ice nucleating particles which facilitate the formation of ice fog by allowing water to freeze at temperatures above −38°C. During our study, there was an ice fog event that coincided with a pollution event. During this event, there was a significant increase in coarse particulate matter associated with a decrease in temperature and calm winds. Ice nucleating particle concentration in the air decreased during the ice fog event indicating that the INPs had activated into the ice fog and were not able to be captured. We determined that most INPs were heat‐labile (potentially biological), followed by organic. Very few INPs were inorganic. Inorganic INPs increased during the ice fog period while heat‐labile and organic INPs decreased indicating that they were being selectively activated into the fog. Overall, INP concentrations in Fairbanks were quite high compared to other Arctic locations and carries implications for ice fog formation in other high‐latitude locations. Key Points: Fairbanks had higher wintertime ice nucleating particle (INP) concentrations than other high‐latitude locationsINP concentrations in Fairbanks decreased during the ice fog period, indicating that INPs were activated into the fogINP composition in Fairbanks was dominated by heat‐labile INPs [ABSTRACT FROM AUTHOR]

Ice nucleating particles (INPs) are rare particles that initiate primary ice formation, a critical step required for subsequent important cloud microphysical processes that ultimately govern cloud phase and cloud radiative properties. Laboratory studies have found that organic‐rich dusts, such as those found in soils, are more efficient INPs compared to mineral dust. However, the atmospheric relevance of these organic‐rich dusts are not well understood, particularly in regions with significant agricultural activity. The Agricultural Ice nuclei at the Southern Great Plains field campaign (AGINSGP) was conducted in rural Oklahoma to investigate how soil dusts contribute to INP populations in the Great Plains. We present chemical characterization of ambient and ice crystal residual particles from a single day of sampling, using single particle mass spectrometry (SPMS) and scanning microscopy. Ambient particles were primarily carbonaceous or secondary aerosol, while the fraction of dust particles was higher in the residual particles. We also observed an unusual particle type consisting of a carbonaceous core mixed with dust fragments on the surface, which was found in higher proportion in residuals. Dust particles measured during residual sampling contained greater proportions of phosphate (63PO2− ${\text{PO}}_{2}^{-}$ and 79PO3− ${\text{PO}}_{3}^{-}$) and lead (206Pb+). Strong sulfate signals were not seen in the residual dust particles measured by the SPMS, while nitrate was slightly depleted relative to ambient dust. This study shows that organic‐rich soils may be important contributors to the ambient INP population in agricultural regions. Plain Language Summary: Ice nucleating particles (INPs) affect climate by causing clouds to freeze at warmer temperatures. However, they are very rare which this means that they are challenging to characterize. Agricultural soils have exhibited high ice nucleation activity in lab studies though their relevance to ambient INP populations is unknown. In this work, we directly measure INP composition in a field campaign at a site in the middle of farmlands to determine whether they are an important source of INPs. We show that dust particles, along with carbonaceous particles mixed with dust, are enriched in INP samples relative to ambient particles. We also show that phosphate (presumed to come from biological fragments) and lead may enhance the IN activity of dust particles. Key Points: Ice nucleating particle composition was directly measured with the ice crystal residual method using two characterization techniquesDust residual particles contained greater phosphate and lead relative to ambient dust particlesCarbonaceous particles internally mixed with dust fragments were found in residual particles measured by SEM/EDX [ABSTRACT FROM AUTHOR]

Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using "dry" geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean.

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

With the oceans covering 71% of the Earth, sea spray aerosol (SSA) particles profoundly impact climate through their ability to scatter solar radiation and serve as seeds for cloud formation. The climate properties can change when sea salt particles become mixed with insoluble organic material formed in ocean regions with phytoplankton blooms. Currently, the extent to which SSA chemical composition and climate properties are altered by biological processes in the ocean is uncertain. To better understand the factors controlling SSA composition, we carried out a mesocosm study in an isolated ocean-atmosphere facility containing 3,400 gallons of natural seawater. Over the course of the study, two successive phytoplankton blooms resulted in SSA with vastly different composition and properties. During the first bloom, aliphatic-rich organics were enhanced in submicron SSA and tracked the abundance of phytoplankton as indicated by chlorophyll-a concentrations. In contrast, the second bloom showed no enhancement of organic species in submicron particles. A concurrent increase in ice nucleating SSA particles was also observed only during the first bloom. Analysis of the temporal variability in the concentration of aliphatic-rich organic species, using a kinetic model, suggests that the observed enhancement in SSA organic content is set by a delicate balance between the rate of phytoplankton primary production of labile lipids and enzymatic induced degradation. This study establishes a mechanistic framework indicating that biological processes in the ocean and SSA chemical composition are coupled not simply by ocean chlorophyll-a concentrations, but are modulated by microbial degradation processes. This work provides unique insight into the biological, chemical, and physical processes that control SSA chemical composition, that when properly accounted for may explain the observed differences in SSA composition between field studies.

The Atmospheric Radiation Measurement Mobile Facility‐2 was installed onboard the research vessel Aurora Australis to measure aerosol properties during the 2017–2018 Measurement of Aerosols, Radiation, and CloUds over the pristine Southern ocean (MARCUS) Experiment, providing unique data on aerosols latitudinal and seasonal variation, including south of 60°S where previous observations are scarce. Data from a Cloud Condensation Nuclei (CCN) counter and Ultra‐High‐Sensitivity Aerosol Spectrometer show that both the number concentration (NCCN) and size distribution of CCN‐active aerosols, with diameters (D) between 60 nm < D < 1,000 nm are different over the North Southern Ocean (NSO) (50°S–60°S) and the South Southern Ocean (SSO) (62°S–68°S). The average NSO NCCN at 0.2% and 0.5% supersaturation were 28% and 49% less than that over the SSO. This increase of CCN over the SSO is caused by the increase of aerosols with 60 nm < D < 200 nm, consistent with calculations of Aerosol Scattering Angstrom Exponents derived from a nephelometer. Aerosol hygroscopicity growth factor measured by the Hygroscopic Tandem Differential Mobility Analyzer stayed close to 1.41 for aerosols with 50 nm < D < 250 nm over the SSO, but increased from 1.30 to 1.67 over the NSO, indicating different chemical compositions. Both CCN and Ice Nucleating Particles (INPs) showed a stronger variation with season than with latitude. The variation of heat‐labile and presumably proteinacous INPs suggests an increase of ice nucleating‐active microbes in summer. Plain Language Summary: The Atmospheric Radiation Measurement Mobile Facility‐2 was installed onboard an ice breaker to measure small particles suspended in the air (aerosols), particularly those with potential influences on cloud formation and evolution. The 2017–2018 Measurement of Aerosols, Radiation, and CloUds over the pristine Southern ocean (MARCUS) measurement campaign provides unique data on the latitudinal and seasonal variation of the suspended particles, including south of 60°S where previous observations are scarce. Data show that both the number concentration and size distribution of particles that serve as embryos of cloud droplets are different over the North Southern Ocean (NSO) (50°S–60°S) and the South Southern Ocean (SSO) (62°S–68°S). There are greater concentrations of these embryos over the SSO for increased total amount of suspended particles there. These observations are consistent with data collected by other instruments that show differences over the NSO and SSO in how these suspended particles scatter radiation and how they absorb water vapor, which shows the particles have different sizes and chemical compositions respectively. The concentrations of both particles that serve as embryos for cloud drops and ice crystals both vary more with season than latitude, which has an implication for the energy balance of the Southern Ocean. Key Points: Machine Learning is applied to identify ship stack contamination of ship‐borne aerosol measurementsSurface Cloud Condensation Nuclei number concentration and its seasonal variation over 62°S–68°S is higher than over 50°S–60°SIce Nucleating Particles over the Southern Ocean originate from primarily organic and biological sources during MARCUS [ABSTRACT FROM AUTHOR]

The aerosol particles that provide cloud condensation and ice nuclei contribute to key cloud processes associated with cold-air outbreak (CAO) events but are poorly constrained in climate models due to sparse observations. Here we retrieve aerosol size distribution modes from measurements at Andenes, Norway during the Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) and at Zeppelin Observatory, approximately 1000 km upwind in Svalbard. During CAO events at Andenes, the sea spray mode number concentration is correlated to strong over-ocean winds with a mean of 8±4 cm-3 that is 71 % higher than during non-CAO conditions. Additionally during CAO events at Andenes, the mean Hoppel minimum diameter is 6 nm smaller than during non-CAO conditions though the estimated supersaturation is lower and the number concentration of particles that likely activated in-cloud is 109±61 cm-3 (similar to non-CAO conditions). For CAO trajectories between Zeppelin Observatory and Andenes, the upwind-to-downwind change in number concentration is largest for the accumulation mode with a mean decrease of 93±95 cm-3, likely attributable primarily to precipitation scavenging. These characteristic properties of aerosol size distributions during CAO events provide guidance for evaluating CAO aerosol-cloud interaction processes in models. [ABSTRACT FROM AUTHOR]

Ice crystal formation in mixed-phase clouds is initiated by specific aerosol particles, termed ice-nucleating particles (INPs). Only a tiny fraction of all aerosol particles are INPs, providing a challenge for contemporary INP measurement techniques. Models have shown that the presence of INPs in clouds can impact their radiative properties and induce precipitation formation. However, for a qualified implementation of INPs in models, measurement techniques able to accurately detect the temperature-dependent INP concentration are needed. Here we present measurements of INP concentrations in ambient air under conditions relevant to mixed-phase clouds from a total of 10 INP methods over 2 weeks in October 2018 at the Puy de Dôme observatory in central France. A special focus in this intercomparison campaign was placed on having overlapping sampling periods. Although a variety of different measurement principles were used, the majority of the data show INP concentrations within a factor of 5 of one another, demonstrating the suitability of the instruments to derive model-relevant INP data. Lower values of comparability are likely due to instrument-specific features such as aerosol lamina spreading in continuous-flow diffusion chambers, demonstrating the need to account for such phenomena when interpreting INP concentration data from online instruments. Moreover, consistently higher INP concentrations were observed from aerosol filters collected on the rooftop at the Puy de Dôme station without the use of an aerosol inlet. [ABSTRACT FROM AUTHOR]

Supercooled liquid clouds are ubiquitous over the Southern Ocean (SO), even to temperatures below −20°C, and comprise a large fraction of the marine boundary layer (MBL) clouds. Earth system models and reanalysis products have struggled to reproduce the observed cloud phase distribution and occurrence of cloud ice in the region. Recent simulations found the microphysical representation of ice nucleation and growth has a large impact on these properties, however, measurements of SO ice nucleating particles (INPs) to validate simulations are sparse. This study presents measurements of INPs from simultaneous aircraft and ship campaigns conducted over the SO in austral summer 2018, which include the first in situ observations in and above cloud in the region. Our results confirm recent observations that INP concentrations are uniformly lower than measurements made in the late 1960s. While INP concentrations below and above cloud are similar, higher ice nucleation efficiency above cloud supports model simulations that the dominant INP composition varies with height. Model parameterizations based solely on aerosol properties capture the mean relationship between INP concentration and temperature but not the observed variability, which is likely related to the only modest correlations observed between INPs and environmental or aerosol metrics. Including wind speed in addition to activation temperature in a marine INP parameterization reduces bias but does not explain the large range of observed INP concentrations. Direct and indirect inference of marine INP size suggests MBL INPs, at least during Austral summer, are dominated by particles with diameters smaller than 500 nm. Plain Language Summary: Although Antarctica is remote, the continent and the Southern Ocean (SO) that surrounds it play a fundamental role in shaping regional and global climate. The clouds in this region are unique, with less ice and more liquid water present at low temperatures than in other areas. This is likely related to very low concentrations of rare aerosol particles called ice nucleating particles (INPs), which cause liquid water droplets in clouds to freeze. Largely due to a lack of observations, SO clouds are poorly represented in global models, and the interactions between aerosol particles and clouds are one of the largest remaining uncertainties. This study presents results of INP measurements from several recent field campaigns over the SO, including the first observations within and above clouds in the region. Our results suggest different types of particles are present below and above clouds, which have varying ability to nucleate ice. They also highlight the need for additional measurements of INP composition and size, which are key variables needed to improve model simulations. Key Points: First vertically resolved measurements of ice nucleating particles (INPs) over the Southern Ocean, including in‐cloud observationsCorrelation between normalized INP concentrations and wind speed suggests marine active site density is variableHigher ice nucleation efficiency observed above cloud, consistent with an increasing influence of mineral dust with height [ABSTRACT FROM AUTHOR]

Rapid Arctic climate warming, amplified relative to lower-latitude regions, has led to permafrost thaw and associated thermokarst processes. Recent work has shown permafrost is a rich source of ice-nucleating particles (INPs) that can initiate ice formation in supercooled liquid clouds. Since the phase of Arctic clouds strongly affects the surface energy budget, especially over ice-laden surfaces, characterizing INP sources in this region is critical. For the first time, we provide a large-scale survey of potential INP sources in tundra terrain where thermokarst processes are active and relate to INPs in the air. Permafrost, seasonally thawed active layer, ice wedge, vegetation, water, and aerosol samples were collected near Utqiaġvik, Alaska, in late summer and analyzed for their INP contents. Permafrost was confirmed as a rich source of INPs that was enhanced near the coast. Sensitivity to heating revealed differences in INPs from similar sources, such as the permafrost and active layer. Water, vegetation, and ice wedge INPs had the highest heat-labile percentage. The aerosol likely contained a mixture of known and unsurveyed INP types that were inferred as biological. Arctic water bodies were shown to be potential important links of sources to the atmosphere in thermokarst regions. Therefore, a positive relationship found with total organic carbon considering all water bodies gives a mechanism for future parameterization as permafrost continues to thaw and drive regional landscape shifts. [ABSTRACT FROM AUTHOR]

Single‐ and multi‐layer clouds are commonly observed over the Southern Ocean in varying synoptic settings, yet few studies have characterized and contrasted their properties. This study provides a statistical analysis of the microphysical properties of single‐ and multi‐layer clouds using in‐situ observations acquired during the Southern Ocean Cloud‐Radiation Aerosol Transport Experimental Study. The relative frequencies of ice‐containing samples (i.e., mixed and ice phase) for multi‐layer clouds are 0.05–0.25 greater than for single‐layer clouds, depending on cloud layer height. In multi‐layer clouds, the lowest cloud layers have the highest ice‐containing sample frequencies, which decrease with increasing cloud layer height up to the third highest cloud layer. This suggests a prominent seeder‐feeder mechanism over the region. Ice nucleating particle (cloud condensation nuclei) concentrations are positively (negatively) correlated with ice‐containing sample frequencies in select cases. Differences in microphysical properties are observed for single‐ and multi‐layer clouds. Drop concentrations (size distributions) are greater (narrower) for single‐layer clouds compared with the lowest multi‐layer clouds. When differentiating cloud layers by top (single‐ and highest multi‐layer clouds) and non‐top layers (underlying multi‐layer clouds), total particle size distributions (including liquid and ice) are similarly broader for non‐top cloud layers. Additionally, drop concentrations in coupled environments are approximately double those in decoupled environments. Plain Language Summary: Weather and climate models continue to struggle simulating cloud microphysical properties over the Southern Ocean, including cloud phase occurrence frequencies. High resolution observations of Southern Ocean clouds are crucial toward improving model simulations. This paper uses in situ observations to compare and contrast microphysical properties and phase frequencies of single‐ and multi‐layer clouds, as well as relates phase frequencies with ice nucleating particle and cloud condensation nuclei number concentrations. In situ observations used in this study were acquired during the Southern Ocean Cloud‐Radiation Aerosol Transport Experimental Study. A suite of cloud probe instrumentation is used to classify 1 Hz cloud samples as either liquid, ice or mixed phase (i.e., liquid and ice particles in the same sample volume). The lowest occurrence frequency of liquid phase samples is observed in the lowest cloud layers of multi‐layer clouds, whereas the highest frequency is observed in single‐layer clouds. Ice nucleating particle number concentrations are negatively correlated with liquid phase occurrence frequencies in select cases. In contrast, cloud condensation nuclei number concentrations are positively correlated with liquid phase frequencies, although this is only observed for clouds above the boundary layer. Key Points: The occurrence frequency of ice is greater in multi‐layer clouds than in single‐layer cloudsDrop number size distributions are broader in multi‐layer clouds compared to single‐layer cloudsLiquid drop number concentrations are approximately double in environments coupled with the surface compared to decoupled environments [ABSTRACT FROM AUTHOR]

Sea spray aerosols (SSA) represent one of the most abundant aerosol types on a global scale and have been observed at all altitudes including the upper troposphere. SSA has been explored in recent years as a source of ice nucleating particles (INPs) in cirrus clouds due to the ubiquity of cirrus clouds and the uncertainties in their radiative forcing. This study expands upon previous works on low temperature ice nucleation of SSA by investigating the effects of atmospheric aging of SSA and the ice nucleating activity of newly formed secondary marine aerosols (SMA) using an oxidation flow reactor. Polydisperse aerosol distributions were generated from a Marine Aerosol Reference Tank (MART) filled with 120 L of real or artificial seawater and their subsequent freezing was measured using a Continuous Flow Diffusion Chamber (CFDC). Results show that for both primary SSA (pSSA), and the aged SSA and SMA (aSSA+SMA) at temperatures > 220 K, 1 % of the particles freeze via homogeneous nucleation. However, below 220 K, heterogeneous nucleation occurs for both pSSA and aSSA+SMA at much lower relative humidities (RHs), where up to 1 % of the aerosol population freezes between 75--80 % RH. Similarities between freezing behaviors of the pSSA and aSSA+SMA at all temperatures suggest atmospheric aging has little effect on the heterogeneous freezing behavior of SSA at these cirrus temperatures and remains dominated by the crystalline salts. Occurrence of 1 % frozen fraction of SMA, generated in the absence of primary SSA, was observed at/near water saturation below 220 K, suggesting it is not an effective INP at cirrus temperatures, similar to findings in the literature of other organic aerosols. Thus, any SMA coatings on the pSSA are also unlikely to modify the ice nucleation behavior of pSSA. These results demonstrate the ability of lofted primary sea spray particles to remain an effective ice nucleator at cirrus temperatures, even after atmospheric aging. [ABSTRACT FROM AUTHOR]