Influence of sea surface microlayers and phytoplankton blooms on sea spray aerosol hygroscopicity and the possible implications for mixed-phase clouds

2021 ◽  
Author(s):  
Sigurd Christiansen ◽  
Luisa Ickes ◽  
Ines Bulatovic ◽  
Caroline Leck ◽  
Benjamin Murray ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Mixed Phase ◽  
Sea Surface ◽  
Sea Spray ◽  
Surface Microlayer ◽  
Cloud Properties ◽  
Aerosol Emission ◽  
Sea Spray Aerosol ◽  
Mixed Phase Clouds ◽  
Aerosol Hygroscopicity

<p><em>Introduction:<br></em>Breaking waves on the ocean surface lead to sea spray aerosol emission to the atmosphere. Sea spray aerosols are a major source of uncertainty in climate models. The physical processes governing sea spray aerosol production play an important part in determining sea spray aerosol emission, size distribution, and chemical composition. Sea spray often contains organic material, but it is unclear how this material affects the ability of particles to act as cloud condensation nuclei (CCN).</p><p><em>Methods:</em><br>We have measured the CCN-derived hygroscopicity of different types of aerosol particles generated from the following seawater proxies and real seawater using a sea spray simulation tank (Christiansen et al., 2019), AEGOR, or an atomizer in a laboratory setup (Christiansen et al., 2020): </p><ul><li>Artificial seawater</li> <li>Artificial seawater spiked with diatoms cultured in the laboratory</li> <li>Samples of sea surface microlayer (SML) collected during field campaigns in the North Atlantic and Arctic Ocean.</li> <li>A continuous supply of fresh seawater during a three-week field campaign (June 2019) on the Faroe Islands, while following oceanic biogeochemical parameters.   </li> </ul><p>Large-eddy simulation (LES) has been used to evaluate the general role of aerosol hygroscopicity in governing mixed-phase low-level cloud properties in the high Arctic.</p><p><em>Conclusions: <br></em></p><ul><li>We show that sea spray aerosols generated using diatom cultures and surface microlayer water exhibit CCN activity similar to that of inorganic sea salt (κ value of ∼1.0), independent of dry particle size (50, 75, and 100 nm).</li> <li>The critical supersaturation of dry 80 nm SSA was relatively invariable (0.158±0.04%), corresponding to the overall hygroscopicity parameter κ of 1.08±0.05% derived from CCN during the phytoplankton bloom. This is despite indications that the chemical composition of both the seawater and the SSA were impacted by the presence of the phytoplankton.</li> <li>For accumulation mode aerosol, the simulated mixed-phase cloud properties do not depend strongly on κ, unless κ < 0.4. In addition, the cloud is sustained for all simulated cases.</li> <li>For Aitken mode aerosol, the hygroscopicity is more important changing the microphysical structure of the cloud and its radiative properties; here the particles can sustain the cloud only when κ ≥ 0.4. </li> </ul><p>The experimental and model results combined suggest that the internal mixing of biogenic organic components in SSA does not have a substantial impact on the cloud droplet activation process and the cloud lifetime in Arctic mixed-phase clouds.</p><p><em>References:</em><br>Christiansen et al. (2020). J. Geophys. Res. Atm. https://doi.org/10.1029/2020JD032808<br>Christiansen et al. (2019). Environ. Sci. Technol. https://doi.org/10.1021/acs.est.9b04078 </p>

scholarly journals The role of jet and film drops in controlling the mixing state of submicron sea spray aerosol particles

2017 ◽  
Vol 114 (27) ◽  
pp. 6978-6983 ◽  
Author(s):  
Xiaofei Wang ◽  
Grant B. Deane ◽  
Kathryn A. Moore ◽  
Olivia S. Ryder ◽  
M. Dale Stokes ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Volume Fraction ◽  
Water Soluble ◽  
Sea Surface ◽  
Sea Spray ◽  
Surface Microlayer ◽  
Mixing State ◽  
Organic Species ◽  
Sea Surface Microlayer ◽  
Sea Spray Aerosol

The oceans represent a significant global source of atmospheric aerosols. Sea spray aerosol (SSA) particles comprise sea salts and organic species in varying proportions. In addition to size, the overall composition of SSA particles determines how effectively they can form cloud droplets and ice crystals. Thus, understanding the factors controlling SSA composition is critical to predicting aerosol impacts on clouds and climate. It is often assumed that submicrometer SSAs are mainly formed by film drops produced from bursting bubble-cap films, which become enriched with hydrophobic organic species contained within the sea surface microlayer. In contrast, jet drops formed from the base of bursting bubbles are postulated to mainly produce larger supermicrometer particles from bulk seawater, which comprises largely salts and water-soluble organic species. However, here we demonstrate that jet drops produce up to 43% of total submicrometer SSA number concentrations, and that the fraction of SSA produced by jet drops can be modulated by marine biological activity. We show that the chemical composition, organic volume fraction, and ice nucleating ability of submicrometer particles from jet drops differ from those formed from film drops. Thus, the chemical composition of a substantial fraction of submicrometer particles will not be controlled by the composition of the sea surface microlayer, a major assumption in previous studies. This finding has significant ramifications for understanding the factors controlling the mixing state of submicrometer SSA particles and must be taken into consideration when predicting SSA impacts on clouds and climate.

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.

Calcium bridging drives polysaccharide co-adsorption to a proxy sea surface microlayer

2021 ◽  
Author(s):  
Kimberly Anne Carter-Fenk ◽  
Abigal Dommer ◽  
Michelle E. Fiamingo ◽  
Jeongin Kim ◽  
Rommie Amaro ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Mass Fraction ◽  
Co Adsorption ◽  
Ocean Surface ◽  
Sea Surface ◽  
Sea Spray ◽  
Surface Microlayer ◽  
Sea Surface Microlayer ◽  
Sea Spray Aerosol ◽  
Significant Mass

Saccharides comprise a significant mass fraction of organic carbon in sea spray aerosol (SSA), but the mechanisms through which saccharides are transferred from seawater to the ocean surface and eventually...

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 Gaseous chemistry and aerosol mechanism developments for version 3.5.1 of the online regional model, WRF-Chem

2014 ◽  
Vol 7 (6) ◽  
pp. 2557-2579 ◽  
Author(s):  
S. Archer-Nicholls ◽  
D. Lowe ◽  
S. Utembe ◽  
J. Allan ◽  
R. A. Zaveri ◽  
...  
Keyword(s):  
Gas Phase ◽  
Chemical Mechanism ◽  
Reduced Form ◽  
Sea Spray ◽  
Wind Fields ◽  
Aerosol Composition ◽  
Aerosol Emission ◽  
Sea Spray Aerosol ◽  
The Impact ◽  
Phase Chemical

Abstract. We have made a number of developments to the Weather, Research and Forecasting model coupled with Chemistry (WRF-Chem), with the aim of improving model prediction of trace atmospheric gas-phase chemical and aerosol composition, and of interactions between air quality and weather. A reduced form of the Common Reactive Intermediates gas-phase chemical mechanism (CRIv2-R5) has been added, using the Kinetic Pre-Processor (KPP) interface, to enable more explicit simulation of VOC degradation. N2O5 heterogeneous chemistry has been added to the existing sectional MOSAIC aerosol module, and coupled to both the CRIv2-R5 and existing CBM-Z gas-phase schemes. Modifications have also been made to the sea-spray aerosol emission representation, allowing the inclusion of primary organic material in sea-spray aerosol. We have worked on the European domain, with a particular focus on making the model suitable for the study of nighttime chemistry and oxidation by the nitrate radical in the UK atmosphere. Driven by appropriate emissions, wind fields and chemical boundary conditions, implementation of the different developments are illustrated, using a modified version of WRF-Chem 3.4.1, in order to demonstrate the impact that these changes have in the Northwest European domain. These developments are publicly available in WRF-Chem from version 3.5.1 onwards.

The ice nucleating ability of macromolecules in immersion freezing decreases in the presence of salts: Implications for freezing point depression calculations

2021 ◽  
Author(s):  
Jon F. Went ◽  
Jeanette D. Wheeler ◽  
François J. Peaudecerf ◽  
Nadine Borduas-Dedekind
Keyword(s):  
Sea Water ◽  
Freezing Point ◽  
Pure Water ◽  
Salt Content ◽  
Mixed Phase ◽  
Cloud Formation ◽  
Sea Spray ◽  
Freezing Point Depression ◽  
Immersion Freezing ◽  
Mixed Phase Clouds

<p>Cloud formation represents a large uncertainty in current climate predictions. In particular, ice in mixed-phase clouds requires the presence of ice nucleating particles (INPs) or ice nucleating macromolecules (INMs). An influential population of INPs has been proposed to be organic sea spray aerosols in otherwise pristine ocean air. However, the interactions between INMs present in sea water and their freezing behavior under atmospheric immersion freezing conditions warrants further research to constrain the role of sea spray aerosols on cloud formation. Indeed, salt is known to lower the freezing temperature of water, through a process called freezing point depression (FPD). Yet, current FPD corrections are solely based on the salt content and assume that the INMs’ ice nucleation abilities are identical with and without salt. Thus, we measured the effect of salt content on the ice nucleating ability of INMs, known to be associated with marine phytoplankton, in immersion freezing experiments in the Freezing Ice Nuclei Counter (FINC) (Miller et al., AMTD, 2020). We measured eight INMs, namely taurine, isethionate, xylose, mannitol, dextran, laminarin, and xanthan as INMs in pure water at temperatures relevant for mixed-phase clouds (e.g. 50% activated fraction at temperatures above –23 °C at 10 mM concentration). Subsequently, INMs were analyzed in artificial sea water containing 36 g salt L<sup>-1</sup>. Most INMs, except laminarin and xanthan, showed a loss of ice activity in artificial sea water compared to pure water, even after FPD correction. Based on our results, we hypothesize sea salt has an inhibitory effect on the ice activity of INMs. This effect influences our understanding of how INMs nucleate ice as well as challenges our use of FPD correction and subsequent extrapolation to ice activity under mixed-phase cloud conditions.</p>

Towards a molecular-based parameterization of the ice nucleation activity of biological macromolecules and its implications for aerosol-cloud interactions

2021 ◽  
Author(s):  
Minghui Zhang ◽  
Amina Khaled ◽  
Pierre Amato ◽  
Anne-Marie Delort ◽  
Barbara Ervens
Keyword(s):  
Fungal Spores ◽  
Chemical Properties ◽  
Active Surface ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Biological Macromolecules ◽  
Cloud Properties ◽  
Nucleation Activity ◽  
Mixed Phase Clouds ◽  
Ice Nucleation Activity

<p>Primary biological aerosol particles (PBAPs) play an important role in mixed-phase clouds as they nucleate ice even at temperatures of T > -10 °C. Current parameterizations of PBAP ice nucleation are based on ice nucleation active surface site (INAS) densities that are derived from freezing experiments. However, only a small fraction of the PBAP surface is responsible for their ice nucleation activity, such as proteins of bacteria cells, fungal spores, pollen polysaccharides and other (unidentified) macromolecules. Based on literature data, we refine the INAS density parameterizations by further parameters:</p><p>1) We demonstrate that the ice nucleation activity of such individual macromolecules is much higher than that of PBAPs. It can be shown that INAS of PBAPs can be scaled by the surface fraction of these ice-nucleating molecules.</p><p>2) Previous studies suggested that ice nucleation activity tends to be higher for larger macromolecules and their aggregates. We show that these trends hold true for various groups of macromolecules that comprise PBAPs.</p><p>Based on these trends, we suggest a more refined parameterization for ice-nucleating macromolecules in different types of PBAPs and even for different species of bacteria, fungi, and pollen. This new parameterization can be considered a step towards a molecular-based approach to predict the ice nucleation activity of the macromolecules in PBAPs based on their biological and chemical properties.</p><p>We implement both the traditional INAS parameterization for complete PBAPs and our parameterization for individual molecules in an adiabatic cloud parcel model. The extent will be discussed to which the two parameterizations result in different cloud properties of mixed-phase clouds.</p>

scholarly journals Chemical composition and mixing-state of ice residuals sampled within mixed phase clouds

2011 ◽  
Vol 11 (6) ◽  
pp. 2805-2816 ◽  
Author(s):  
M. Ebert ◽  
A. Worringen ◽  
N. Benker ◽  
S. Mertes ◽  
E. Weingartner ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Carbonaceous Material ◽  
Mixed Phase ◽  
Research Station ◽  
Mixing State ◽  
Anthropogenic Component ◽  
Significant Enrichment ◽  
Alpine Research ◽  
Main Component ◽  
Mixed Phase Clouds

Abstract. During an intensive campaign at the high alpine research station Jungfraujoch, Switzerland, in February/March 2006 ice particle residuals within mixed-phase clouds were sampled using the Ice-counterflow virtual impactor (Ice-CVI). Size, morphology, chemical composition, mineralogy and mixing state of the ice residual and the interstitial (i.e., non-activated) aerosol particles were analyzed by scanning and transmission electron microscopy. Ice nuclei (IN) were identified from the significant enrichment of particle groups in the ice residual (IR) samples relative to the interstitial aerosol. In terms of number lead-bearing particles are enriched by a factor of approximately 25, complex internal mixtures with silicates or metal oxides as major components by a factor of 11, and mixtures of secondary aerosol and carbonaceous material (C-O-S particles) by a factor of 2. Other particle groups (sulfates, sea salt, Ca-rich particles, external silicates) observed in the ice-residual samples cannot be assigned unambiguously as IN. Between 9 and 24% of all IR are Pb-bearing particles. Pb was found as major component in around 10% of these particles (PbO, PbCl2). In the other particles, Pb was found as some 100 nm sized agglomerates consisting of 3–8 nm sized primary particles (PbS, elemental Pb). C-O-S particles are present in the IR at an abundance of 17–27%. The soot component within these particles is strongly aged. Complex internal mixtures occur in the IR at an abundance of 9–15%. Most IN identified at the Jungfraujoch station are internal mixtures containing anthropogenic components (either as main or minor constituent), and it is concluded that admixture of the anthropogenic component is responsible for the increased IN efficiency within mixed phase clouds. The mixing state appears to be a key parameter for the ice nucleation behaviour that cannot be predicted from the sole knowledge of the main component of an individual particle.

Finding linkages between ocean ecosystems and natural marine aerosols in the minimally polluted North Atlantic atmosphere

2020 ◽  
Author(s):  
Patricia Quinn ◽  
Tim Bates ◽  
Eric Saltzman ◽  
Tom Bell ◽  
Mike Behrenfeld
Keyword(s):  
North Atlantic ◽  
Cloud Condensation Nuclei ◽  
Sea Spray ◽  
Marine Aerosols ◽  
Condensation Nuclei ◽  
Surface Ocean ◽  
Cloud Properties ◽  
Sea Spray Aerosol ◽  
Ocean Ecosystems ◽  
Aerosol Properties

<p>The emission of sea spray aerosol (SSA) and dimethylsulfide (DMS) from the ocean results in marine boundary layer aerosol particles that can impact Earth’s radiation balance by directly scattering solar radiation and by acting as cloud condensation nuclei (CCN), thereby altering cloud properties. The surface ocean is projected to warm by 1.3 to 2.8°C globally over the 21<sup>st</sup> century. Impacts of this warming on plankton blooms, ocean ecosystems, and ocean-to-atmosphere fluxes of aerosols and their precursor gases are highly uncertain. A fundamental understanding of linkages between surface ocean ecosystems and ocean-derived aerosols is required to address this uncertainty. One approach for improved understandings of these linkages is simultaneous measurements of relevant surface ocean and aerosol properties in an ocean region with seasonally varying plankton blooms and a minimally polluted overlying atmosphere. The western North Atlantic hosts the largest annual phytoplankton bloom in the global ocean with a large spatial and seasonal variability in plankton biomass and composition. Periods of low aerosol number concentrations associated with unpolluted air masses allow for the detection of linkages between ocean ecosystems and ocean-derived aerosol.</p><p> </p><p>Five experiments were conducted in the western North Atlantic between 2014 and 2018 with the objective of finding links between the bloom and marine aerosols. These experiments include the second Western Atlantic Climate Study (WACS-2) and four North Atlantic Aerosol and Marine Ecosystem Study (NAAMES) cruises. This series of cruises was the first time the western North Atlantic bloom was systematically sampled during every season with extensive ocean and atmosphere measurements able to assess how changes in the state of the bloom might impact ocean-derived aerosol properties. Measurements of unheated and heated number size distributions, cloud condensation nuclei (CCN) concentrations, and aerosol composition were used to identify primary and secondary aerosol components that could be related to the state of the bloom. Only periods of clean marine air, as defined by radon, particle number concentration, aerosol light absorption coefficient, and back trajectories, were included in the analysis.</p><p> </p><p>CCN concentrations at 0.1% supersaturation were best correlated (r<sup>2</sup> = 0.73) with accumulation mode nss SO<sub>4</sub><sup>=</sup>. Sea spray aerosol (SSA) was only correlated with CCN during November when bloom accumulation had not yet occurred and dimethylsulfide (DMS) concentrations were at a minimum. The fraction of CCN attributable to SSA was less than 20% during March, May/June, and September, indicating the limited contribution of SSA to the CCN population of the western North Atlantic atmosphere. The strongest link between the plankton bloom and aerosol and cloud properties appears to be due to biogenic non-seasalt SO<sub>4</sub><sup>=</sup>.</p><p> </p>

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