Search

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.

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.

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]

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]

The article provides information about ice-nucleating particles (INPs) in the atmosphere, which play a crucial role in initiating ice formation in clouds, affecting weather and climate. It focuses on bio-INPs, a subset of these particles, and highlights their significance in initiating freezing processes in mixed-phase clouds at warmer temperatures.

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]