Sea State and Boundary Layer Stability Limit Sea Spray Aerosol Lifetime over the Southern Ocean

Abstract. Ice nucleating particles (INPs) in the Arctic can influence climate and precipitation in the region; yet our understanding of the concentrations and sources of INPs in this region remain uncertain. In the following, we (1) measured concentrations of INPs in the immersion mode in the Canadian Arctic marine boundary layer during summer 2014 on board the CCGS Amundsen, (2) determined ratios of surface areas of mineral dust aerosol to sea spray aerosol, and (3) investigated the source region of the INPs using particle dispersion modelling. Average concentrations of INPs at −15, −20, and −25 ∘C were 0.005, 0.044, and 0.154 L−1, respectively. These concentrations fall within the range of INP concentrations measured in other marine environments. For the samples investigated the ratio of mineral dust surface area to sea spray surface area ranged from 0.03 to 0.09. Based on these ratios and the ice active surface site densities of mineral dust and sea spray aerosol determined in previous laboratory studies, our results suggest that mineral dust is a more important contributor to the INP population than sea spray aerosol for the samples analysed. Based on particle dispersion modelling, the highest concentrations of INPs were often associated with lower-latitude source regions such as the Hudson Bay area, eastern Greenland, or north-western continental Canada. On the other hand, the lowest concentrations were often associated with regions further north of the sampling sites and over Baffin Bay. A weak correlation was observed between INP concentrations and the time the air mass spent over bare land, and a weak negative correlation was observed between INP concentrations and the time the air mass spent over ice and open water. These combined results suggest that mineral dust from local sources is an important contributor to the INP population in the Canadian Arctic marine boundary layer during summer 2014.

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Effect of primary organic sea spray emissions on cloud condensation nuclei concentrations

Atmospheric Chemistry and Physics ◽

10.5194/acp-12-89-2012 ◽

2012 ◽

Vol 12 (1) ◽

pp. 89-101 ◽

Cited By ~ 46

Author(s):

D. M. Westervelt ◽

R. H. Moore ◽

A. Nenes ◽

P. J. Adams

Keyword(s):

Surface Tension ◽

Southern Ocean ◽

Source Function ◽

Cloud Condensation Nuclei ◽

Organic Aerosol ◽

Sea Salt ◽

Sea Spray ◽

Aerosol Emission ◽

Sea Spray Aerosol ◽

Surfactant Effects

Abstract. This work estimates the primary marine organic aerosol global emission source and its impact on cloud condensation nuclei (CCN) concentrations by implementing an organic sea spray source function into a series of global aerosol simulations. The source function assumes that a fraction of the sea spray emissions, depending on the local chlorophyll concentration, is organic matter in place of sea salt. Effect on CCN concentrations (at 0.2% supersaturation) is modeled using the Two-Moment Aerosol Sectional (TOMAS) microphysics algorithm coupled to the GISS II-prime general circulation model. The presence of organics affects CCN activity in competing ways: by reducing the amount of solute available in the particle and decreasing surface tension of CCN. To model surfactant effects, surface tension depression data from seawater samples taken near the Georgia coast were applied as a function of carbon concentrations. A global marine organic aerosol emission rate of 17.7 Tg C yr−1 is estimated from the simulations. Marine organics exert a localized influence on CCN(0.2%) concentrations, decreasing regional concentrations by no more than 5% and by less than 0.5% over most of the globe, assuming direct replacement of sea salt aerosol with organic aerosol. The decrease in CCN concentrations results from the fact that the decrease in particle solute concentration outweighs the organic surfactant effects. The low sensitivity of CCN(0.2%) to the marine organic emissions is likely due to the small compositional changes: the mass fraction of OA in accumulation mode aerosol increases by only ~15% in a biologically active region of the Southern Ocean. To test the sensitivity to uncertainty in the sea spray emissions process, we relax the assumption that sea spray aerosol number and mass remain fixed and instead can add to sea spray emissions rather than replace existing sea salt. In these simulations, we find that marine organic aerosol can increase CCN by up to 50% in the Southern Ocean and 3.7% globally during the austral summer. This vast difference in CCN impact highlights the need for further observational exploration of the sea spray aerosol emission process as well as evaluation and development of model parameterizations.

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Meridional and vertical variations of the water vapour isotopic composition in the marine boundary layer over the Atlantic and Southern Ocean

Atmospheric Chemistry and Physics ◽

10.5194/acp-20-5811-2020 ◽

2020 ◽

Vol 20 (9) ◽

pp. 5811-5835 ◽

Cited By ~ 2

Author(s):

Iris Thurnherr ◽

Anna Kozachek ◽

Pascal Graf ◽

Yongbiao Weng ◽

Dimitri Bolshiyanov ◽

...

Keyword(s):

Boundary Layer ◽

Time Series ◽

Wind Speed ◽

Southern Ocean ◽

Water Vapour ◽

Turbulent Mixing ◽

Large Scale ◽

Marine Boundary Layer ◽

Sea Spray ◽

Moisture Source

Abstract. Stable water isotopologues (SWIs) are useful tracers of moist diabatic processes in the atmospheric water cycle. They provide a framework to analyse moist processes on a range of timescales from large-scale moisture transport to cloud formation, precipitation and small-scale turbulent mixing. Laser spectrometric measurements on research vessels produce high-resolution time series of the variability of the water vapour isotopic composition in the marine boundary layer. In this study, we present a 5-month continuous time series of such ship-based measurements of δ2H and δ18O from the Antarctic Circumnavigation Expedition (ACE) in the Atlantic and the Southern Ocean in the time period from November 2016 to April 2017. We analyse the drivers of meridional SWI variations in the marine boundary layer across diverse climate zones in the Atlantic and Southern Ocean using Lagrangian moisture source diagnostics and relate vertical SWI differences to near-surface wind speed and ocean surface state. The median values of δ18O, δ2H and deuterium excess during ACE decrease continuously from low to high latitudes. These meridional SWI distributions reflect climatic conditions at the measurement and moisture source locations, such as air temperature, specific humidity and relative humidity with respect to sea surface temperature. The SWI variability at a given latitude is highest in the extratropics and polar regions with decreasing values equatorwards. This meridional distribution of SWI variability is explained by the variability in moisture source locations and its associated environmental conditions as well as transport processes. The westward-located moisture sources of water vapour in the extratropics are highly variable in extent and latitude due to the frequent passage of cyclones and thus widen the range of encountered SWI values in the marine boundary layer. Moisture loss during transport further contributes to the high SWI variability in the extratropics. In the subtropics and tropics, persistent anticyclones lead to well-confined narrow easterly moisture source regions, which is reflected in the weak SWI variability in these regions. Thus, the expected range of SWI signals at a given latitude strongly depends on the large-scale circulation. Furthermore, the ACE SWI time series recorded at 8.0 and 13.5 m above the ocean surface provide estimates of vertical SWI gradients in the lowermost marine boundary layer. On average, the vertical gradients with height found during ACE are -0.1‰m-1 for δ18O, -0.5‰m-1 for δ2H and 0.3 ‰ m−1 for deuterium excess. Careful calibration and post-processing of the SWI data and a detailed uncertainty analysis provide a solid basis for the presented gradients. Using sea spray concentrations and sea state conditions, we show that the vertical SWI gradients are particularly large during high wind speed conditions with increased contribution of sea spray evaporation or during low wind speed conditions due to weak vertical turbulent mixing. Although further SWI measurements at a higher vertical resolution are required to validate these findings, the simultaneous SWI measurements at several heights during ACE show the potential of SWIs as tracers for vertical mixing and sea spray evaporation in the lowermost marine boundary layer.

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Sea spray aerosol as a unique source of ice nucleating particles

Proceedings of the National Academy of Sciences ◽

10.1073/pnas.1514034112 ◽

2015 ◽

Vol 113 (21) ◽

pp. 5797-5803 ◽

Cited By ~ 174

Author(s):

Paul J. DeMott ◽

Thomas C. J. Hill ◽

Christina S. McCluskey ◽

Kimberly A. Prather ◽

Douglas B. Collins ◽

...

Keyword(s):

Boundary Layer ◽

Radiative Forcing ◽

Marine Boundary Layer ◽

Strong Increase ◽

Sea Spray ◽

Surface Boundary ◽

Surface Boundary Layer ◽

Surface Areas ◽

Order Of Magnitude ◽

Sea Spray Aerosol

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.

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The sensitivity of Southern Ocean aerosol concentrations to sea spray and DMS emissions in the HadGEM3-GA7.1 chemistry–climate model

10.5194/egusphere-egu2020-5976 ◽

2020 ◽

Author(s):

Laura Revell ◽

Stefanie Kremser ◽

Sean Hartery ◽

Mike Harvey ◽

Jane Mulcahy ◽

...

Keyword(s):

Wind Speed ◽

Southern Ocean ◽

Source Function ◽

Climate Model ◽

Cloud Condensation Nuclei ◽

Number Concentration ◽

Sea Spray ◽

Condensation Nuclei ◽

Sea Spray Aerosol ◽

Aerosol Source

<p>With low concentrations of tropospheric aerosol, the Southern Ocean offers a "natural laboratory" for studies of aerosol&#8211;cloud interactions. Aerosols over the Southern Ocean are produced from biogenic activity in the ocean, which generates sulfate aerosol via dimethylsulfide (DMS) oxidation, and from strong winds and waves that lead to bubble bursting and sea spray emission. Here, we evaluate the representation of Southern Ocean aerosols in the Hadley Centre Global Environmental Model version 3, Global Atmosphere 7.1 (HadGEM3-GA7.1) chemistry&#8211;climate model. Compared with aerosol optical depth (AOD) observations from two satellite instruments (the Moderate Resolution Imaging Spectroradiometer, MODIS-Aqua c6.1, and the Multi-angle Imaging Spectroradiometer, MISR), the model simulates too-high AOD during winter and too-low AOD during summer. By switching off DMS emission in the model, we show that sea spray aerosol is the dominant contributor to AOD during winter. In turn, the simulated sea spray aerosol flux depends on near-surface wind speed. By examining MODIS AOD as a function of wind speed from the ERA-Interim reanalysis and comparing it with the model, we show that the sea spray aerosol source function in HadGEM3-GA7.1 overestimates the wind speed dependency. We test a recently developed sea spray aerosol source function derived from measurements made on a Southern Ocean research voyage in 2018. In this source function, the wind speed dependency of the sea spray aerosol flux is less than in the formulation currently implemented in HadGEM3-GA7.1. The new source function leads to good agreement between simulated and observed wintertime AODs over the Southern Ocean; however, it reveals partially compensating errors in DMS-derived AOD. While previous work has tested assumptions regarding the seawater climatology or sea&#8211;air flux of DMS, we test the sensitivity of simulated AOD, cloud condensation nuclei and cloud droplet number concentration to three atmospheric sulfate chemistry schemes. The first scheme adds DMS oxidation by halogens and the other two test a recently developed sulfate chemistry scheme for the marine troposphere; one tests gas-phase chemistry only, while the second adds extra aqueous-phase sulfate reactions. We show how simulated sulfur dioxide and sulfuric acid profiles over the Southern Ocean change as a result and how the number concentration and particle size of the soluble Aitken, accumulation and coarse aerosol modes are affected. The new DMS chemistry scheme leads to a 20% increase in the number concentration of cloud condensation nuclei and cloud droplets, which improves agreement with observations. Our results highlight the importance of atmospheric chemistry for simulating aerosols and clouds accurately over the Southern Ocean.</p>

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Evaluation of Southern Ocean cloud in the HadGEM3 general circulation model and MERRA-2 reanalysis using ship-based observations

10.5194/acp-2019-201 ◽

2019 ◽

Cited By ~ 2

Author(s):

Peter Kuma ◽

Adrian J. McDonald ◽

Olaf Morgenstern ◽

Simon P. Alexander ◽

John J. Cassano ◽

...

Keyword(s):

Boundary Layer ◽

Southern Ocean ◽

Surface Temperature ◽

General Circulation ◽

Cloud Cover ◽

Austral Summer ◽

Boundary Layer Stability ◽

Subgrid Scale ◽

Low Cloud ◽

The Difference

Abstract. Southern Ocean (SO) shortwave (SW) radiation biases are a common problem in contemporary general circulation models (GCMs), with most models exhibiting a tendency to absorb too much incoming SW radiation. These biases have been attributed to deficiencies in the representation of clouds during the austral summer months, either due to cloud cover or cloud optical thickness being too low. The problem has been the focus of many studies, most of which utilised satellite datasets for model evaluation. We use multi-year ship based observations and the CERES spaceborne radiation budget measurements to contrast cloud representation and SW radiation in the atmospheric component Global Atmosphere (GA) version 7.0 and 7.1 of the HadGEM3 GCM and the MERRA-2 reanalysis. We find that MERRA-2 is biased in the opposite direction to GA (reflects too much SW radiation). In addition, MERRA-2 performs better in terms of absolute SW bias than nudged runs of GA7.0 and GA7.1 in the 60–70° S latitude band. GA7.1 reduces the SO SW radiation biases relative to GA7.0, but significant errors remain at up to 20 W m−2 between 60 and 70° S in the austral summer months. Using ship-based ceilometer observations, we find low cloud below 2 km to be predominant in the Ross Sea and the Indian Ocean sector of the SO. Utilising a novel surface lidar simulator developed for this study, derived from an existing COSP-ACTSIM spaceborne lidar simulator, we find that GA7.0 and MERRA-2 both underestimate low cloud occurrence relative to the ship observations by 18–25 % on average, though the cloud cover in MERRA-2 is closer to observations by about 7 %. Based on radiosonde observations, we also find the low cloud to be strongly linked to boundary-layer atmospheric stability and the sea surface temperature. GA7.0 and MERRA-2 agree well with observations in terms of boundary-layer stability, suggesting that subgrid-scale parametrisations do not generate enough cloud in response to the thermodynamic profile of the atmosphere and the surface temperature. Our analysis shows that MERRA-2 has a much greater proportion of cloud liquid water in the SO in January than GA7.0, a likely key contributor to the difference in SW radiation. We show that boundary-layer stability and relative humidity fields are very similar in GA7.0 and MERRA-2, and unlikely to be the cause of the different cloud representation, suggesting that subgrid-scale parametrisations are responsible for the difference between the models.

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A numerical framework for simulating episodic emissions of high-temperature marine INPs

10.5194/acp-2021-316 ◽

2021 ◽

Author(s):

Isabelle Steinke ◽

Paul J. DeMott ◽

Grant Deane ◽

Thomas C. J. Hill ◽

Mathew Maltrud ◽

...

Keyword(s):

Boundary Layer ◽

High Temperature ◽

Atmospheric Boundary Layer ◽

Heterotrophic Bacteria ◽

Sea Spray ◽

Surface Microlayer ◽

Partial Explanation ◽

Sea Surface Microlayer ◽

Sea Spray Aerosol ◽

Field Campaigns

Abstract. We present a framework for estimating concentrations of episodically elevated high-temperature marine ice nucleating particles (INPs) in the sea surface microlayer and their subsequent emission into the atmospheric boundary layer. These episodic INPs have been observed in multiple ship-based and coastal field campaigns, but the processes controlling their ocean concentrations and transfer to the atmosphere are not yet fully understood. We use a combination of empirical constraints and simulation outputs from an Earth System Model to explore different hypotheses for explaining the variability of INP concentrations, and the occurrence of episodic INPs, in the marine atmosphere. In our calculations, we examine two proposed oceanic sources of high-temperature INPs: heterotrophic bacteria and marine biopolymer aggregates (MBPAs). Furthermore, we assume that the emission of these INPs is determined by the production of supermicron sea spray aerosol formed from jet drops, with an entrainment probability that is described by Poisson statistics. The concentration of jet drops is derived from the number concentration of supermicron sea spray aerosol calculated from model runs. We then derive the resulting number concentrations of marine high-temperature INPs (≥ 253 K) in the atmospheric boundary layer and compare their variability to atmospheric observations of INP variability. Specifically, we compare against concentrations of episodically occurring high-temperature INPs observed during field campaigns in the Southern Ocean, the Equatorial Pacific, and the North Atlantic. We find that heterotrophic bacteria and MBPAs acting as INPs provide only a partial explanation for the observed high INP concentrations. We note, however, that there are still substantial knowledge gaps, particularly concerning the identity of the oceanic INPs contributing most frequently to episodic high-temperature INPs, their specific ice nucleation activity, and the enrichment of their concentrations during the sea-air transfer process. Therefore, targeted measurements investigating the composition of these marine INPs as well as drivers for their emission are needed, ideally in combination with modeling studies focused on the potential cloud impacts of these high-temperature INPs.

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Evidence of Sea-State Dependence of Aerosol Concentration in the Marine Atmospheric Boundary Layer

Journal of Physical Oceanography ◽

10.1175/jpo-d-16-0058.1 ◽

2017 ◽

Vol 47 (1) ◽

pp. 69-84 ◽

Cited By ~ 9

Author(s):

Luc Lenain ◽

W. Kendall Melville

Keyword(s):

Boundary Layer ◽

Atmospheric Boundary Layer ◽

Wave Breaking ◽

State Dependence ◽

Aerosol Concentration ◽

Sea Spray ◽

Marine Atmospheric Boundary Layer ◽

Sea State ◽

Wave Parameters ◽

Interaction Experiment

AbstractSea spray aerosols represent a large fraction of the aerosols present in the maritime environment. Despite evidence of the importance of surface wave– and wave breaking–related processes in coupling the ocean with the atmosphere, sea spray source generation functions are traditionally parameterized by the 10-m wind speed U10 alone. It is clear that unless the wind and wave field are fully developed, the source function will be a function of both wind and wave parameters. This study reports primarily on the aerosol component of an air–sea interaction experiment, the phased-resolved High-Resolution Air–Sea Interaction Experiment (HIRES), conducted off the coast of northern California in June 2010. Detailed measurements of aerosol number concentration in the marine atmospheric boundary layer (MABL) at altitudes ranging from as low as 30 m up to 800 m above mean sea level (MSL) over a broad range of environmental conditions (significant wave height Hs of 2 to 4.5 m and U10 from 10 to 18 m s−1) collected from an instrumented research aircraft are presented. Aerosol number densities and volume are computed over a range of particle diameters from 0.1 to 200 μm, while the sea surface conditions, including Hs, moments of the breaker length distribution Λ(c), and wave breaking dissipation, were measured by a suite of electro-optical sensors that included the NASA Airborne Topographic Mapper (ATM). The sea-state dependence of the aerosol concentration in the MABL is evident, stressing the need to incorporate wave parameters in the spray source generation functions that are traditionally parameterized by surface winds alone.

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Meridional and vertical variations of the water vapour isotopic composition in the marine boundary layer over the Atlantic and Southern Ocean

10.5194/acp-2019-782 ◽

2019 ◽

Author(s):

Iris Thurnherr ◽

Anna Kozachek ◽

Pascal Graf ◽

Yongbiao Weng ◽

Dimitri Bolshiyanov ◽

...

Keyword(s):

Boundary Layer ◽

Time Series ◽

Wind Speed ◽

Southern Ocean ◽

Water Vapour ◽

Turbulent Mixing ◽

Large Scale ◽

Marine Boundary Layer ◽

Sea Spray ◽

Moisture Source

Abstract. Stable water isotopologues (SWIs) are useful tracers of moist diabatic processes in the atmospheric water cycle. They provide a framework to analyse moist processes on a range of time scales from large-scale moisture transport to cloud formation, precipitation, and small-scale turbulent mixing. Laser spectrometric measurements on research vessels produce high-resolution time series of the variability of the water vapour isotopic composition in the marine boundary layer. In this study, we present a five-month continuous time series of such ship-based measurements of δ2H and δ18O from the Antarctic Circumnavigation Expedition (ACE) in the Atlantic and the Southern Ocean in the time period from November 2016 to April 2017. We analyse the drivers of meridional SWI variations in the marine boundary layer across diverse climate zones in the Atlantic and Southern Ocean using Lagrangian moisture source diagnostics and relate vertical SWI differences to near-surface wind speed and ocean surface state. The median values of δ18O, δ2H and d-excess during ACE decrease continuously from low to high latitudes. These meridional SWI distributions reflect climatic conditions at the measurement and moisture source sites, such as air temperature, specific humidity, and relative humidity with respect to sea surface temperature. The SWI variability at a given latitude is highest in the extratropics and polar regions with decreasing values equatorwards. This meridional distribution of SWI variability is explained by the variability in moisture source locations and its associated environmental conditions as well as transport processes. The westward located moisture sources of water vapour in the extratropics are highly variable in extent and latitude due to the frequent passage of cyclones and thus widen the range of encountered SWI values in the marine boundary layer. Moisture loss during transport further contributes to the high SWI variability in the extratropics. In the subtropics and tropics, persistent anticyclones lead to well-confined narrow easterly moisture source regions, which is reflected in the low SWI variability in these regions. Thus, the expected range of SWI signals at a given latitude strongly depends on the large-scale circulation. Furthermore, the ACE SWI time series recorded at different heights above the ocean surface provide estimates of vertical SWI gradients in the lowermost marine boundary layer. On average, the vertical gradients with height found during ACE are −0.1 ‰ m−1 for δ18O, −0.5 ‰ m−1 for δ2H and 0.3 ‰ m−1 for d-excess. Careful calibration and post-processing of the SWI data and a detailed uncertainty analysis provide a solid basis for the presented gradients. Using sea spray concentrations and sea state conditions, we show that the vertical SWI gradients are particularly large during high wind speed conditions with increased contribution of sea spray evaporation or during low wind speed conditions due to weak vertical turbulent mixing and dominating effects from non-equilibrium fractionation. Although further SWI measurements at a higher vertical resolution are required to validate these findings, the simultaneous SWI measurements at several heights during ACE show the potential of SWIs as tracers for vertical mixing and sea spray evaporation in the lowermost marine boundary layer.

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