Sea Spray Aerosol Formation: Laboratory Results on the Role of Air Entrainment, Water Temperature, and Phytoplankton Biomass

Abstract. We have developed an inorganic sea spray source function that is based upon state-of-the-art measurements of sea spray aerosol production using a temperature-controlled plunging jet sea spray aerosol chamber. The size-resolved particle production was measured between 0.01 and 10 μm dry diameter. Particle production decreased non-linearly with increasing seawater temperature (between −1 and 30 °C) similar to previous findings. In addition, we observed that the particle effective radius as well as the particle-surface, -volume and -mass, increased with increasing seawater temperature due to increased production of super-micron particles. By combining these measurements with the volume of air entrained by the plunging jet we have determined the size-resolved particle flux as a function of air entrainment. Through the use of existing parameterisations of air entrainment as a function of wind speed we were subsequently able to scale our laboratory measurements of particle production to wind speed. By scaling in this way we avoid the difficulties associated with defining the "white-area" of the laboratory whitecap – a contentious issue when relating laboratory measurements of particle production to oceanic whitecaps using the more frequently applied whitecap method. The here-derived inorganic sea spray sea spray source function was implemented in a Lagrangian particle dispersion model (FLEXPART). An estimated annual global flux of inorganic sea spray aerosol of 5.9 ± 0.2 Pg yr−1 was derived that is close to the median of estimates from the same model using a wide range of existing sea spray source functions. When using the source function derived here, the model also showed good skill in predicting measurements of Na+ concentration at a number of field sites further underlining the validity of our source function. In a final step, the sensitivity of a large-scale model (NorESM) to our new source function was tested. Compared to the previously implemented parameterisation, a clear decrease of sea spray aerosol number flux and increase in aerosol residence time was observed, especially over the Southern Ocean. At the same time an increase in aerosol optical depth due to an increase in the number of particles with optically relevant sizes was found. That there were noticeable regional differences may have important implications for aerosol optical properties and number concentrations, subsequently also affecting the indirect radiative forcing by non-sea spray anthropogenic aerosols.

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Molecular size of surfactants affects their degree of enrichment in the sea spray aerosol formation

Environmental Research ◽

10.1016/j.envres.2021.112555 ◽

2021 ◽

pp. 112555

Author(s):

Lingrui Liu ◽

Lin Du ◽

Li Xu ◽

Jianlong Li ◽

Narcisse T. Tsona

Keyword(s):

Molecular Size ◽

Sea Spray ◽

Aerosol Formation ◽

Sea Spray Aerosol

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An empirically derived inorganic sea spray source function incorporating sea surface temperature

Atmospheric Chemistry and Physics ◽

10.5194/acp-15-11047-2015 ◽

2015 ◽

Vol 15 (19) ◽

pp. 11047-11066 ◽

Cited By ~ 33

Author(s):

M. E. Salter ◽

P. Zieger ◽

J. C. Acosta Navarro ◽

H. Grythe ◽

A. Kirkevåg ◽

...

Keyword(s):

Wind Speed ◽

Source Function ◽

Particle Production ◽

Dispersion Model ◽

Seawater Temperature ◽

Air Entrainment ◽

Particle Dispersion ◽

Sea Spray ◽

Laboratory Measurements ◽

Sea Spray Aerosol

Abstract. We have developed an inorganic sea spray source function that is based upon state-of-the-art measurements of sea spray aerosol production using a temperature-controlled plunging jet sea spray aerosol chamber. The size-resolved particle production was measured between 0.01 and 10 μm dry diameter. Particle production decreased non-linearly with increasing seawater temperature (between −1 and 30 °C) similar to previous findings. In addition, we observed that the particle effective radius, as well as the particle surface, particle volume and particle mass, increased with increasing seawater temperature due to increased production of particles with dry diameters greater than 1 μm. By combining these measurements with the volume of air entrained by the plunging jet we have determined the size-resolved particle flux as a function of air entrainment. Through the use of existing parameterisations of air entrainment as a function of wind speed, we were subsequently able to scale our laboratory measurements of particle production to wind speed. By scaling in this way we avoid some of the difficulties associated with defining the "white area" of the laboratory whitecap – a contentious issue when relating laboratory measurements of particle production to oceanic whitecaps using the more frequently applied whitecap method. The here-derived inorganic sea spray source function was implemented in a Lagrangian particle dispersion model (FLEXPART – FLEXible PARTicle dispersion model). An estimated annual global flux of inorganic sea spray aerosol of 5.9 ± 0.2 Pg yr−1 was derived that is close to the median of estimates from the same model using a wide range of existing sea spray source functions. When using the source function derived here, the model also showed good skill in predicting measurements of Na+ concentration at a number of field sites further underlining the validity of our source function. In a final step, the sensitivity of a large-scale model (NorESM – the Norwegian Earth System Model) to our new source function was tested. Compared to the previously implemented parameterisation, a clear decrease of sea spray aerosol number flux and increase in aerosol residence time was observed, especially over the Southern Ocean. At the same time an increase in aerosol optical depth due to an increase in the number of particles with optically relevant sizes was found. That there were noticeable regional differences may have important implications for aerosol optical properties and number concentrations, subsequently also affecting the indirect radiative forcing by non-sea spray anthropogenic aerosols.

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Wintertime Arctic Ocean sea water properties and primary marine aerosol concentrations

Atmospheric Chemistry and Physics ◽

10.5194/acp-12-10405-2012 ◽

2012 ◽

Vol 12 (21) ◽

pp. 10405-10421 ◽

Cited By ~ 24

Author(s):

J. Zábori ◽

R. Krejci ◽

A. M. L. Ekman ◽

E. M. Mårtensson ◽

J. Ström ◽

...

Keyword(s):

Water Temperature ◽

Arctic Ocean ◽

Size Distribution ◽

Primary Particle ◽

Sea Water ◽

Strong Dependence ◽

The Arctic ◽

Aerosol Size Distribution ◽

Sea Spray ◽

Sea Spray Aerosol

Abstract. Sea spray aerosols are an important part of the climate system through their direct and indirect effects. Due to the diminishing sea ice, the Arctic Ocean is one of the most rapidly changing sea spray aerosol source areas. However, the influence of these changes on primary particle production is not known. In laboratory experiments we examined the influence of Arctic Ocean water temperature, salinity, and oxygen saturation on primary particle concentration characteristics. Sea water temperature was identified as the most important of these parameters. A strong decrease in sea spray aerosol production with increasing water temperature was observed for water temperatures between −1°C and 9°C. Aerosol number concentrations decreased from at least 1400 cm−3 to 350 cm−3. In general, the aerosol number size distribution exhibited a robust shape with one mode close to dry diameter Dp 0.2 μm with approximately 45% of particles at smaller sizes. Changes in sea water temperature did not result in pronounced change of the shape of the aerosol size distribution, only in the magnitude of the concentrations. Our experiments indicate that changes in aerosol emissions are most likely linked to changes of the physical properties of sea water at low temperatures. The observed strong dependence of sea spray aerosol concentrations on sea water temperature, with a large fraction of the emitted particles in the typical cloud condensation nuclei size range, provide strong arguments for a more careful consideration of this effect in climate models.

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Wintertime Arctic Ocean sea water properties and primary marine aerosol concentrations

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-16085-2012 ◽

2012 ◽

Vol 12 (6) ◽

pp. 16085-16130 ◽

Cited By ~ 2

Author(s):

J. Zábori ◽

R. Krejci ◽

A. M. L. Ekman ◽

E. M. Mårtensson ◽

J. Ström ◽

...

Keyword(s):

Water Temperature ◽

Arctic Ocean ◽

Size Distribution ◽

Primary Particle ◽

Sea Water ◽

Strong Dependence ◽

The Arctic ◽

Aerosol Size Distribution ◽

Sea Spray ◽

Sea Spray Aerosol

Abstract. Sea spray aerosols are an important part of the climate system through their direct and indirect effects. Due to the diminishing sea ice, the Arctic Ocean is one of the most rapidly changing sea spray aerosol source areas. However, the influence of these changes on primary particle production is not known. In laboratory experiments we examined the influence of Arctic Ocean water temperature, salinity and oxygen saturation on primary particle concentration characteristics. Sea water temperature was identified as the most important of these parameters. A strong decrease in sea spray aerosol production with increasing water temperature was observed for water temperatures between −1 °C and 9 °C. Aerosol number concentrations decreased from at least 1400 cm−3 to 350 cm−3. In general, the aerosol number size distribution exhibited a robust shape with one mode close to Dp 0.2 μm with approximately 45% of particles at smaller sizes. Changes in sea water temperature did not result in pronounced change of the shape of the aerosol size distribution, only in the magnitude of the concentrations. Our experiments indicate that changes in aerosol emissions are most likely linked to changes of the physical properties of sea water at low temperatures. The observed strong dependence of sea spray aerosol concentrations on sea water temperature, with a large fraction of the emitted particles in the typical cloud condensation nuclei size range, provide strong arguments for a more careful consideration of this effect in climate models.

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Sea Spray Aerosol Chamber Study on Selective Transfer and Enrichment of Free and Combined Amino Acids

ACS Earth and Space Chemistry ◽

10.1021/acsearthspacechem.1c00080 ◽

2021 ◽

Author(s):

Nadja Triesch ◽

Manuela van Pinxteren ◽

Matthew Salter ◽

Christian Stolle ◽

Ryan Pereira ◽

...

Keyword(s):

Amino Acids ◽

Sea Spray ◽

Selective Transfer ◽

Chamber Study ◽

Sea Spray Aerosol ◽

Aerosol Chamber

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Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

10.5194/acp-2016-36 ◽

2016 ◽

Author(s):

Sara D. Forestieri ◽

Gavin C. Cornwell ◽

Taylor M. Helgestad ◽

Kathryn A. Moore ◽

Christopher Lee ◽

...

Keyword(s):

Light Scattering ◽

Relative Humidity ◽

Salt Content ◽

Sea Salt ◽

Sea Spray ◽

Hygroscopic Growth ◽

Phytoplankton Blooms ◽

Aerosol Composition ◽

Sea Spray Aerosol ◽

Indoor And Outdoor

Abstract. The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA) particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 %)) of SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs). One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. GF(85 %) values for SSA particles were derived from measurements of light scattering and particle size distributions, concurrently with online single particle and bulk aerosol composition measurements. During both microcosm experiments, the observed bulk average GF(85 %) values were depressed substantially relative to pure, inorganic sea salt, by 10 to 19 %, with a one (indoor MART) and six (outdoor MART) day lag between GF(85 %) depression and the peak chlorophyll-a concentrations. The fraction of organiccontaining SSA particles generally increased after the peak of the phytoplankton blooms. The GF(85 %) values were inversely correlated with the fraction of particles containing organic or other biological markers. This indicates these particles were less hygroscopic than the particles identified as predominately sea salt containing and demonstrates a clear relationship between SSA particle composition and the sensitivity of light scattering to variations in relative humidity. The implications of these observations to the direct climate effects of SSA particles are discussed.

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

Geoscientific Model Development ◽

10.5194/gmd-7-2557-2014 ◽

2014 ◽

Vol 7 (6) ◽

pp. 2557-2579 ◽

Cited By ~ 30

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.

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