Cation-Driven Lipopolysaccharide Morphological Changes Impact Heterogeneous Reactions of Nitric Acid with Sea Spray Aerosol Particles

Abstract. Ice nucleating particles (INPs) are a rare subset of aerosol particles that initiate cloud droplet freezing at temperatures above the homogenous freezing point of water (−38 °C). Considering that the ocean covers 70 % of the earth's surface and represent a large potential source of INPs, it is imperative that the uncertainties in the identities and emissions of ocean INP become better understood. However, the specific underlying drivers of marine INP emissions and their identities remain largely unknown due to limited observations and the challenge involved in isolating exceptionally rare IN forming particles. By generating nascent sea spray aerosol (SSA) over a range of biological conditions, mesocosm studies show that microbes can contribute to marine INPs. Here, we identify 14 (30 %) cultivable halotolerant ice nucleating microbes and fungi among 47 total isolates recovered from precipitation and aerosol samples collected in coastal air in Southern California. IN isolates collected in coastal air were found to nucleate ice from extremely warm to moderate freezing temperatures (−2.3 to −18 °C). Air mass trajectory analyses, and cultivability in marine growth media indicate marine origins of these isolates. Further phylogenetic analysis confirmed that at least two of the 14 IN isolates were of marine origin. Moreover, results from cell washing experiments demonstrate that most IN isolates maintained freezing activity in the absence of nutrients and cell growth media. This study provides confirmation of previous studies' findings that implicated microbes as a potential source of marine INPs and additionally demonstrates links between precipitation, marine aerosol and IN microbes.

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Heterogeneous ice nucleation ability of aerosol particles generated from Arctic sea surface microlayer and surface seawater samples at cirrus temperatures

Atmospheric Chemistry and Physics ◽

10.5194/acp-21-13903-2021 ◽

2021 ◽

Vol 21 (18) ◽

pp. 13903-13930

Author(s):

Robert Wagner ◽

Luisa Ickes ◽

Allan K. Bertram ◽

Nora Els ◽

Elena Gorokhova ◽

...

Keyword(s):

Aerosol Particles ◽

Ice Nucleation ◽

Sea Surface ◽

Ice Formation ◽

Sea Spray ◽

Surface Microlayer ◽

Sea Surface Microlayer ◽

Sea Spray Aerosol ◽

Seawater Samples ◽

Heterogeneous Ice Nucleation

Abstract. Sea spray aerosol particles are a recognised type of ice-nucleating particles under mixed-phase cloud conditions. Entities that are responsible for the heterogeneous ice nucleation ability include intact or fragmented cells of marine microorganisms as well as organic matter released by cell exudation. Only a small fraction of sea spray aerosol is transported to the upper troposphere, but there are indications from mass-spectrometric analyses of the residuals of sublimated cirrus particles that sea salt could also contribute to heterogeneous ice nucleation under cirrus conditions. Experimental studies on the heterogeneous ice nucleation ability of sea spray aerosol particles and their proxies at temperatures below 235 K are still scarce. In our article, we summarise previous measurements and present a new set of ice nucleation experiments at cirrus temperatures with particles generated from sea surface microlayer and surface seawater samples collected in three different regions of the Arctic and from a laboratory-grown diatom culture (Skeletonema marinoi). The particles were suspended in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber and ice formation was induced by expansion cooling. We confirmed that under cirrus conditions, apart from the ice-nucleating entities mentioned above, also crystalline inorganic salt constituents can contribute to heterogeneous ice formation. This takes place at temperatures below 220 K, where we observed in all experiments a strong immersion freezing mode due to the only partially deliquesced inorganic salts. The inferred ice nucleation active surface site densities for this nucleation mode reached a maximum of about 5×1010 m−2 at an ice saturation ratio of 1.3. Much smaller densities in the range of 108–109 m−2 were observed at temperatures between 220 and 235 K, where the inorganic salts fully deliquesced and only the organic matter and/or algal cells and cell debris could contribute to heterogeneous ice formation. These values are 2 orders of magnitude smaller than those previously reported for particles generated from microlayer suspensions collected in temperate and subtropical zones. While this difference might simply underline the strong variability of the number of ice-nucleating entities in the sea surface microlayer across different geographical regions, we also discuss how instrumental parameters like the aerosolisation method and the ice nucleation measurement technique might affect the comparability of the results amongst different studies.

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