Investigating the Heterogeneous Ice Nucleation of Sea Spray Aerosols UsingProchlorococcusas a Model Source of Marine Organic Matter

2018 ◽  
Vol 53 (3) ◽  
pp. 1139-1149 ◽  
Author(s):  
Martin J. Wolf ◽  
Allison Coe ◽  
Lilian A. Dove ◽  
Maria A. Zawadowicz ◽  
Keven Dooley ◽  
...  
Keyword(s):  
Organic Matter ◽  
Ice Nucleation ◽  
Sea Spray ◽  
Model Source ◽  
Marine Organic Matter ◽  
Heterogeneous Ice Nucleation

Heterogeneous Ice Nucleation on Simulated Sea-Spray Aerosol Using Raman Microscopy

2014 ◽  
Vol 118 (50) ◽  
pp. 29234-29241 ◽  
Author(s):  
Gregory P. Schill ◽  
Margaret A. Tolbert
Keyword(s):  
Ice Nucleation ◽  
Raman Microscopy ◽  
Sea Spray ◽  
Sea Spray Aerosol ◽  
Heterogeneous Ice Nucleation

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

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.

scholarly journals A physically based framework for modeling the organic fractionation of sea spray aerosol from bubble film Langmuir equilibria

2014 ◽  
Vol 14 (24) ◽  
pp. 13601-13629 ◽  
Author(s):  
S. M. Burrows ◽  
O. Ogunro ◽  
A. A. Frossard ◽  
L. M. Russell ◽  
P. J. Rasch ◽  
...  
Keyword(s):  
Organic Matter ◽  
Organic Carbon ◽  
Dissolved Organic Carbon ◽  
Chlorophyll A ◽  
Sea Spray ◽  
Model Parameters ◽  
Model Calculations ◽  
Langmuir Adsorption ◽  
Marine Organic Matter ◽  
Sea Spray Aerosol

Abstract. The presence of a large fraction of organic matter in primary sea spray aerosol (SSA) can strongly affect its cloud condensation nuclei activity and interactions with marine clouds. Global climate models require new parameterizations of the SSA composition in order to improve the representation of these processes. Existing proposals for such a parameterization use remotely sensed chlorophyll a concentrations as a proxy for the biogenic contribution to the aerosol. However, both observations and theoretical considerations suggest that existing relationships with chlorophyll a, derived from observations at only a few locations, may not be representative for all ocean regions. We introduce a novel framework for parameterizing the fractionation of marine organic matter into SSA based on a competitive Langmuir adsorption equilibrium at bubble surfaces. Marine organic matter is partitioned into classes with differing molecular weights, surface excesses, and Langmuir adsorption parameters. The classes include a lipid-like mixture associated with labile dissolved organic carbon (DOC), a polysaccharide-like mixture associated primarily with semilabile DOC, a protein-like mixture with concentrations intermediate between lipids and polysaccharides, a processed mixture associated with recalcitrant surface DOC, and a deep abyssal humic-like mixture. Box model calculations have been performed for several cases of organic adsorption to illustrate the underlying concepts. We then apply the framework to output from a global marine biogeochemistry model, by partitioning total dissolved organic carbon into several classes of macromolecules. Each class is represented by model compounds with physical and chemical properties based on existing laboratory data. This allows us to globally map the predicted organic mass fraction of the nascent submicron sea spray aerosol. Predicted relationships between chlorophyll a and organic fraction are similar to existing empirical parameterizations, but can vary between biologically productive and nonproductive regions, and seasonally within a given region. Major uncertainties include the bubble film thickness at bursting, and the variability of organic surfactant activity in the ocean, which is poorly constrained. In addition, polysaccharides may enter the aerosol more efficiently than Langmuir adsorption would suggest. Potential mechanisms for enrichment of polysaccharides in sea spray include the formation of marine colloidal particles that may be more efficiently swept up by rising bubbles, and cooperative adsorption of polysaccharides with proteins or lipids. These processes may make important contributions to the aerosol, but are not included here. This organic fractionation framework is an initial step towards a closer linking of ocean biogeochemistry and aerosol chemical composition in Earth system models. Future work should focus on improving constraints on model parameters through new laboratory experiments or through empirical fitting to observed relationships in the real ocean and atmosphere, as well as on atmospheric implications of the variable composition of organic matter in sea spray.

scholarly journals A physically-based framework for modelling the organic fractionation of sea spray aerosol from bubble film Langmuir equilibria

2014 ◽  
Vol 14 (5) ◽  
pp. 5375-5443 ◽  
Author(s):  
S. M. Burrows ◽  
O. Ogunro ◽  
A. A. Frossard ◽  
L. M. Russell ◽  
P. J. Rasch ◽  
...  
Keyword(s):  
Organic Matter ◽  
Organic Carbon ◽  
Dissolved Organic Carbon ◽  
Chlorophyll A ◽  
Sea Spray ◽  
Model Parameters ◽  
Model Calculations ◽  
Langmuir Adsorption ◽  
Marine Organic Matter ◽  
Sea Spray Aerosol

Abstract. The presence of a large fraction of organic matter in primary sea spray aerosol (SSA) can strongly affect its cloud condensation nuclei activity and interactions with marine clouds. Global climate models require new parameterizations of the SSA composition in order to improve the representation of these processes. Existing proposals for such a parameterization use remotely-sensed chlorophyll a concentrations as a proxy for the biogenic contribution to the aerosol. However, both observations and theoretical considerations suggest that existing relationships with chlorophyll a, derived from observations at only a few locations, may not be representative for all ocean regions. We introduce a novel framework for parameterizing the fractionation of marine organic matter into SSA based on a competitive Langmuir adsorption equilibrium at bubble surfaces. Marine organic matter is partitioned into classes with differing molecular weights, surface excesses, and Langmuir adsorption parameters. The classes include a lipid-like mixture associated with labile dissolved organic carbon (DOC), a polysaccharide-like mixture associated primarily with semi-labile DOC, a protein-like mixture with concentrations intermediate between lipids and polysaccharides, a processed mixture associated with recalcitrant surface DOC, and a deep abyssal humic-like mixture. Box model calculations have been performed for several cases of organic adsorption to illustrate the underlying concepts. We then apply the framework to output from a global marine biogeochemistry model, by partitioning total dissolved organic carbon into several classes of macromolecules. Each class is represented by model compounds with physical and chemical properties based on existing laboratory data. This allows us to globally map the predicted organic mass fraction of the nascent submicron sea spray aerosol. Predicted relationships between chlorophyll a and organic fraction are similar to existing empirical parameterizations, but can vary between biologically productive and non-productive regions, and seasonally within a given region. Major uncertainties include the bubble film thickness at bursting and the variability of organic surfactant activity in the ocean, which is poorly constrained. In addition, polysaccharides may enter the aerosol more efficiently than Langmuir adsorption would suggest. Potential mechanisms for include the formation of marine colloidal particles that may be more efficiently swept up by rising particles, and cooperative adsorption of polysaccharides with proteins or lipids. These processes may make important contributions to the aerosol, but are not included here. This organic fractionation framework is an initial step towards a closer linking of ocean biogeochemistry and aerosol chemical composition in Earth system models. Future work should focus on improving constraints on model parameters through new laboratory experiments or through empirical fitting to observed relationships in the real ocean and atmosphere, as well as on atmospheric implications of the variable composition of organic matter in sea spray.

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

2021 ◽  
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 salt 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 a large 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 two 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 amount of ice-nucleating entities in the sea surface microlayer across different geographical regions, we also discuss how far instrumental parameters like the aerosolisation method and the ice-nucleation measurement technique might affect the comparability of the results amongst different studies.

scholarly journals Efficiency of immersion mode ice nucleation on surrogates of mineral dust

2007 ◽  
Vol 7 (19) ◽  
pp. 5081-5091 ◽  
Author(s):  
C. Marcolli ◽  
S. Gedamke ◽  
T. Peter ◽  
B. Zobrist
Keyword(s):  
Contact Angle ◽  
Active Sites ◽  
Quantitative Agreement ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Aqueous Suspensions ◽  
Freezing Temperatures ◽  
Good Agreement ◽  
Heterogeneous Ice Nucleation

Abstract. A differential scanning calorimeter (DSC) was used to explore heterogeneous ice nucleation of emulsified aqueous suspensions of two Arizona test dust (ATD) samples with particle diameters of nominally 0–3 and 0–7 μm, respectively. Aqueous suspensions with ATD concentrations of 0.01–20 wt% have been investigated. The DSC thermograms exhibit a homogeneous and a heterogeneous freezing peak whose intensity ratios vary with the ATD concentration in the aqueous suspensions. Homogeneous freezing temperatures are in good agreement with recent measurements by other techniques. Depending on ATD concentration, heterogeneous ice nucleation occurred at temperatures as high as 256 K or down to the onset of homogeneous ice nucleation (237 K). For ATD-induced ice formation Classical Nucleation Theory (CNT) offers a suitable framework to parameterize nucleation rates as a function of temperature, experimentally determined ATD size, and emulsion droplet volume distributions. The latter two quantities serve to estimate the total heterogeneous surface area present in a droplet, whereas the suitability of an individual heterogeneous site to trigger nucleation is described by the compatibility function (or contact angle) in CNT. The intensity ratio of homogeneous to heterogeneous freezing peaks is in good agreement with the assumption that the ATD particles are randomly distributed amongst the emulsion droplets. The observed dependence of the heterogeneous freezing temperatures on ATD concentrations cannot be described by assuming a constant contact angle for all ATD particles, but requires the ice nucleation efficiency of ATD particles to be (log)normally distributed amongst the particles. Best quantitative agreement is reached when explicitly assuming that high-compatibility sites are rare and that therefore larger particles have on average more and better active sites than smaller ones. This analysis suggests that a particle has to have a diameter of at least 0.1 μm to exhibit on average one active site.

scholarly journals Simulating the influence of primary biological aerosol particles on clouds by heterogeneous ice nucleation

2018 ◽  
Vol 18 (20) ◽  
pp. 15437-15450 ◽  
Author(s):  
Matthias Hummel ◽  
Corinna Hoose ◽  
Bernhard Pummer ◽  
Caroline Schaupp ◽  
Janine Fröhlich-Nowoisky ◽  
...  
Keyword(s):  
Pseudomonas Syringae ◽  
Aerosol Particles ◽  
Fungal Spores ◽  
Ice Nucleation ◽  
Ice Crystals ◽  
Atmospheric Measurements ◽  
Cloud Ice ◽  
Biological Aerosol Particles ◽  
Ice Phase ◽  
Heterogeneous Ice Nucleation

Abstract. Primary ice formation, which is an important process for mixed-phase clouds with an impact on their lifetime, radiative balance, and hence the climate, strongly depends on the availability of ice-nucleating particles (INPs). Supercooled droplets within these clouds remain liquid until an INP immersed in or colliding with the droplet reaches its activation temperature. Only a few aerosol particles are acting as INPs and the freezing efficiency varies among them. Thus, the fraction of supercooled water in the cloud depends on the specific properties and concentrations of the INPs. Primary biological aerosol particles (PBAPs) have been identified as very efficient INPs at high subzero temperatures, but their very low atmospheric concentrations make it difficult to quantify their impact on clouds. Here we use the regional atmospheric model COSMO–ART to simulate the heterogeneous ice nucleation by PBAPs during a 1-week case study on a domain covering Europe. We focus on three highly ice-nucleation-active PBAP species, Pseudomonas syringae bacteria cells and spores from the fungi Cladosporium sp. and Mortierella alpina. PBAP emissions are parameterized in order to represent the entirety of bacteria and fungal spores in the atmosphere. Thus, only parts of the simulated PBAPs are assumed to act as INPs. The ice nucleation parameterizations are specific for the three selected species and are based on a deterministic approach. The PBAP concentrations simulated in this study are within the range of previously reported results from other modeling studies and atmospheric measurements. Two regimes of PBAP INP concentrations are identified: a temperature-limited and a PBAP-limited regime, which occur at temperatures above and below a maximal concentration at around −10 ∘C, respectively. In an ensemble of control and disturbed simulations, the change in the average ice crystal concentration by biological INPs is not statistically significant, suggesting that PBAPs have no significant influence on the average state of the cloud ice phase. However, if the cloud top temperature is below −15 ∘C, PBAP can influence the cloud ice phase and produce ice crystals in the absence of other INPs. Nevertheless, the number of produced ice crystals is very low and it has no influence on the modeled number of cloud droplets and hence the cloud structure.

scholarly journals Flotsam and jetsam: a global review of the role of inputs of marine organic matter in sandy beach ecosystems

2021 ◽  
Author(s):  
Glenn A. Hyndes ◽  
Emma Berdan ◽  
Cristian Duarte ◽  
Jenifer E. Dugan ◽  
Kyle A. Emery ◽  
...  
Keyword(s):  
Organic Matter ◽  
Food Webs ◽  
Food Source ◽  
Sandy Beach ◽  
Morphological Characteristics ◽  
Sandy Beaches ◽  
Marine Animals ◽  
Marine Organic Matter ◽  
Beach Cast

Sandy beaches are iconic interfaces that functionally link the ocean with the land by the flow of marine organic matter. These cross-ecosystem fluxes often comprise uprooted seagrass and dislodged macroalgae that can form substantial accumulations of detritus, termed ‘wrack’, on sandy beaches. In addition, the tissue of the carcasses of marine animals that regularly wash up on beaches form a rich food source (‘carrion’) for a diversity of scavenging animals. Here, we provide a global review of how wrack and carrion provide spatial subsidies that shape the structure and functioning of sandy beach ecosystems (sandy beaches and adjacent surf zones), which typically have little in situ primary production. We also examime the spatial scaling of the influence of these processes across the broader seascape and landscape, and identify key gaps in our knowledge to guide future research directions and priorities. Globally, large quantities of detrital kelp and seagrass can flow into sandy beach ecosystems, where microbial decomposers and animals remineralise and consume the imported organic matter. The supply and retention of wrack are influenced by the oceanographic processes that transport it, the geomorphology and landscape context of the recipient beaches, and the condition, life history and morphological characteristics of the taxa that are the ultimate source of wrack. When retained in beach ecosystems, wrack often creates hotspots of microbial metabolism, secondary productivity, biodiversity, and nutrient remineralization. Nutrients are produced during wrack break-down, and these can return to coastal waters in surface flows (swash) and the aquifier discharging into the subtidal surf. Beach-cast kelp often plays a key trophic role, being an abundant and preferred food source for mobile, semi-aquatic invertebrates that channel imported algal matter to predatory invertebrates, fish, and birds. The role of beach-cast marine carrion is likely to be underestimated, as it can be consumed rapidly by highly mobile scavengers (e.g. foxes, coyotes, raptors, vultures). These consumers become important vectors in transferring marine productivity inland, thereby linking marine and terrestrial ecosystems. Whilst deposits of organic matter on sandy beach ecosystems underpin a range of ecosystem functions and services, these can be at variance with aesthetic perceptions resulting in widespread activities, such ‘beach cleaning and grooming’. This practice diminishes the energetic base of food webs, intertidal fauna, and biodiversity. Global declines in seagrass beds and kelp forests (linked to global warming) are predicted to cause substantial reductions in the amounts of marine organic matter reaching many beach ecosystems, likely causing flow-on effects on food webs and biodiversity. Similarly, future sea-level rise and stormier seas are likely to profoundly alter the physical attributes of beaches, which in turn can change the rates at which beaches retain and process the influxes of wrack and animal carcasses. Conservation of the multi-faceted ecosystem services that sandy beaches provide will increasingly need to encompass a greater societal appreciation and the safeguarding of ecological functions reliant on beach-cast organic matter on innumerable ocean shores worldwide.

Roles of Surface Energy and Temperature in Heterogeneous Ice Nucleation

2017 ◽  
Vol 121 (21) ◽  
pp. 11552-11559 ◽  
Author(s):  
Chu Li ◽  
Xiang Gao ◽  
Zhigang Li
Keyword(s):  
Surface Energy ◽  
Ice Nucleation ◽  
Heterogeneous Ice Nucleation
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