scholarly journals Modelling of sea salt pollution over Europe: key uncertainties and comparison with observations

2011 ◽  
Vol 11 (4) ◽  
pp. 11143-11204
Author(s):  
S. Tsyro ◽  
W. Aas ◽  
J. Soares ◽  
M. Sofiev ◽  
H. Berge ◽  
...  
Keyword(s):  
Air Quality ◽  
Source Function ◽  
Temporal Correlation ◽  
Sea Salt ◽  
Sea Spray ◽  
Model Calculations ◽  
Sea Salt Aerosol ◽  
Calculation Results ◽  
Meteorological Input ◽  
Removal Processes

Abstract. Sea spray can significantly affect the air quality. Sea salt can cause enhanced concentrations of particulate matter and change particle chemical composition, in particular in coastal areas, and therefore should be accounted for in air quality modelling. We have used an EMEP Unified model to calculate sea salt concentrations and depositions over Europe, focusing on studying the effects of uncertainties in sea salt production and lifetime on calculation results. Model calculations of sea salt have been compared with EMEP observations of sodium concentrations in air and precipitation for a four year period, from 2004 to 2007, including size (fine/coarse) resolved EMEP intensive measurements in 2006 and 2007. In the presented calculations, sodium air concentrations are between 8 and 46% overestimated, whereas concentrations in precipitation are systematically underestimated by 65–70% for years 2004–2007. Unfortunately, thus far performed tests have failed to give a clear answer regarding the reason for this underestimation and further studies are needed. The model is found to reproduce fairly well the spatial distribution of Na+ in air and precipitation over Europe, and to capture most of sea salt episodes. The paper presents the main findings from a series of tests in which we compare several different sea spray source functions and also look at the effects of meteorological input and the efficiency of removal processes on calculated sea salt concentrations. Finally, sea salt calculations with the EMEP model have been compared with results from the SILAM model and observations for 2007. While the models produce fairly close results for Na+ at most of 26 measurement sites, discrepancies in terms of bias and temporal correlation are also found. Those differences are probably due to differences in the representation of source function and treatment of sea salt aerosol, and also due to different meteorology used for model runs and due to a finer grid resolution of the SILAM model compared to EMEP. This study contributes to getting a better insight on uncertainties associated with sea salt calculations with the EMEP model and towards further improvement of EMEP aerosol modelling.

scholarly journals Modelling of sea salt concentrations over Europe: key uncertainties and comparison with observations

2011 ◽  
Vol 11 (20) ◽  
pp. 10367-10388 ◽  
Author(s):  
S. Tsyro ◽  
W. Aas ◽  
J. Soares ◽  
M. Sofiev ◽  
H. Berge ◽  
...  
Keyword(s):  
Air Quality ◽  
Source Function ◽  
Temporal Correlation ◽  
Sea Salt ◽  
Air Quality Modelling ◽  
Model Calculations ◽  
Sea Salt Aerosol ◽  
Calculation Results ◽  
Meteorological Input ◽  
Removal Processes

Abstract. Sea salt aerosol can significantly affect the air quality. Sea salt can cause enhanced concentrations of particulate matter and change particle chemical composition, in particular in coastal areas, and therefore should be accounted for in air quality modelling. We have used an EMEP Unified model to calculate sea salt concentrations and depositions over Europe, focusing on studying the effects of uncertainties in sea salt production and lifetime on calculation results. Model calculations of sea salt have been compared with EMEP observations of sodium concentrations in air and precipitation for a four year period, from 2004 to 2007, including size (fine/coarse) resolved EMEP intensive measurements in 2006 and 2007. In the presented calculations, sodium air concentrations are between 8% and 46% overestimated, whereas concentrations in precipitation are systematically underestimated by 65–70% for years 2004–2007. A series of model tests have been performed to investigate the reasons for this underestimation, but further studies are needed. The model is found to reproduce the spatial distribution of Na+ in air and precipitation over Europe fairly well, and to capture most of sea salt episodes. The paper presents the main findings from a series of tests in which we compare several different sea spray source functions and also look at the effects of meteorological input and the efficiency of removal processes on calculated sea salt concentrations. Finally, sea salt calculations with the EMEP model have been compared with results from the SILAM model and observations for 2007. While the models produce quite close results for Na+ at the majority of 26 measurement sites, discrepancies in terms of bias and temporal correlation are also found. Those differences are believed to occur due to differences in the representation of source function and size distribution of sea salt aerosol, different meteorology used for model runs and the different models' resolution. This study contributes to getting a better insight on uncertainties associated with sea salt calculations and thus facilitates further improvement of aerosol modelling on both regional and global scales.

scholarly journals Inorganic bromine in the marine boundary layer: a critical review

2003 ◽  
Vol 3 (3) ◽  
pp. 2963-3050 ◽  
Author(s):  
R. Sander ◽  
W. C. Keene ◽  
A. A. P. Pszenny ◽  
R. Arimoto ◽  
G. P. Ayers ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Gas Phase ◽  
Marine Boundary Layer ◽  
Sea Water ◽  
Ocean Surface ◽  
Sea Salt ◽  
Future Research ◽  
Laboratory Studies ◽  
Model Calculations ◽  
Sea Salt Aerosol

Abstract. The cycling of inorganic bromine in the marine boundary layer (mbl) has received increased attention in recent years. Bromide, a constituent of sea water, is injected into the atmosphere in association with sea-salt aerosol by breaking waves on the ocean surface. Measurements reveal that supermicrometer sea-salt aerosol is depleted in bromine by about 50% relative to conservative tracers, whereas marine submicrometer aerosol is often enriched in bromine. Model calculations, laboratory studies, and field observations strongly suggest that these depletions reflect the chemical transformation of particulate bromide to reactive inorganic gases that influence the processing of ozone and other important constituents of marine air. However, currently available techniques cannot reliably quantify many \\chem{Br}-containing compounds at ambient concentrations and, consequently, our understanding of inorganic Br cycling over the oceans and its global significance are uncertain. To provide a more coherent framework for future research, we have reviewed measurements in marine aerosol, the gas phase, and in rain. We also summarize sources and sinks, as well as model and laboratory studies of chemical transformations. The focus is on inorganic bromine over the open oceans, excluding the polar regions. The generation of sea-salt aerosol at the ocean surface is the major tropospheric source producing about 6.2 Tg/a of bromide. The transport of  Br from continents (as mineral aerosol, and as products from biomass-burning and fossil-fuel combustion) can be of local importance. Transport of degradation products of long-lived Br-containing compounds from the stratosphere and other sources contribute lesser amounts. Available evidence suggests that, following aerosol acidification, sea-salt bromide reacts to form Br2 and BrCl that volatilize to the gas phase and photolyze in daylight to produce atomic Br and Cl. Subsequent transformations can destroy tropospheric ozone, oxidize dimethylsulfide (DMS) and hydrocarbons in the gas phase and S(IV) in aerosol solutions, and thereby potentially influence climate. The diurnal cycle of gas-phase \\Br and the corresponding particulate Br deficits are correlated. Higher values of Br in the gas phase during daytime are consistent with expectations based on photochemistry. Mechanisms that explain the widely reported accumulation of particulate Br in submicrometer aerosols are not yet understood. We expect that the importance of inorganic Br cycling will vary in the future as a function of both increasing acidification of the atmosphere (through anthropogenic emissions) and climate changes. The latter affects bromine cycling via meteorological factors including global wind fields (and the associated production of sea-salt aerosol), temperature, and relative humidity.

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

2012 ◽  
Vol 12 (1) ◽  
pp. 89-101 ◽  
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.

scholarly journals Atmospheric Ageing of Inorganic Sea Spray Aerosol: Implications for Hygroscopicity and Cloud Activation Potential

2020 ◽  
Author(s):  
Bernadette Rosati ◽  
Sigurd Christiansen ◽  
Anders Dinesen ◽  
Pontus Roldin ◽  
Andreas Massling ◽  
...  
Keyword(s):  
Uv Light ◽  
Sea Salt ◽  
Sea Spray ◽  
Hygroscopic Growth ◽  
Sea Salt Aerosol ◽  
Activation Potential ◽  
Sea Spray Aerosol ◽  
Marine Areas ◽  
Cloud Activation ◽  
Additional Explanation

Abstract Sea spray aerosol (SSA) contributes significantly to natural aerosol particle concentrations globally, in marine areas even dominantly. The potential changes of the omnipresent inorganic fraction of SSA due to atmospheric ageing is largely unexplored. We demonstrate that ageing of liquid NaCl and artificial sea salt aerosol by exposure to ozone and UV light leads to a substantial decrease in hygroscopicity and cloud activation potential. The results point towards surface reactions that are more crucial for small particles and the formation of salt structures with water bound within the aerosols, termed hydrates. Our findings suggest an increased formation of hydrate forming salts during ageing and the presence of hydrates in dried SSA. Field observations indicate a reduced hygroscopic growth of sub-micrometre SSA in the marine atmosphere compared to pure NaCl which is typically attributed to organic matter or sulphates. Aged inorganic sea salt offers an additional explanation for reduced hygroscopicity and cloud activation potential.

scholarly journals Inorganic bromine in the marine boundary layer: a critical review

2003 ◽  
Vol 3 (5) ◽  
pp. 1301-1336 ◽  
Author(s):  
R. Sander ◽  
W. C. Keene ◽  
A. A. P. Pszenny ◽  
R. Arimoto ◽  
G. P. Ayers ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Gas Phase ◽  
Marine Boundary Layer ◽  
Sea Water ◽  
Ocean Surface ◽  
Sea Salt ◽  
Future Research ◽  
Laboratory Studies ◽  
Model Calculations ◽  
Sea Salt Aerosol

Abstract. The cycling of inorganic bromine in the marine boundary layer (mbl) has received increased attention in recent years. Bromide, a constituent of sea water, is injected into the atmosphere in association with sea-salt aerosol by breaking waves on the ocean surface. Measurements reveal that supermicrometer sea-salt aerosol is substantially depleted in bromine (often exceeding 50%) relative to conservative tracers, whereas marine submicrometer aerosol is often enriched in bromine. Model calculations, laboratory studies, and field observations strongly suggest that the supermicrometer depletions reflect the chemical transformation of particulate bromide to reactive inorganic gases that influence the processing of ozone and other important constituents of marine air. Mechanisms for the submicrometer enrichments are not well understood. Currently available techniques cannot reliably quantify many Br containing compounds at ambient concentrations and, consequently, our understanding of inorganic Br cycling over the oceans and its global significance are uncertain. To provide a more coherent framework for future research, we have reviewed measurements in marine aerosol, the gas phase, and in rain. We also summarize sources and sinks, as well as model and laboratory studies of chemical transformations. The focus is on inorganic bromine over the open oceans outside the polar regions. The generation of sea-salt aerosol at the ocean surface is the major tropospheric source producing about 6.2 Tg/a of bromide. The transport of Br from continents (as mineral aerosol, and as products from biomass-burning and fossil-fuel combustion) can be of local importance. Transport of degradation products of long-lived Br containing compounds from the stratosphere and other sources contribute lesser amounts. Available evidence suggests that, following aerosol acidification, sea-salt bromide reacts to form Br2 and BrCl that volatilize to the gas phase and photolyze in daylight to produce atomic Br and Cl. Subsequent transformations can destroy tropospheric ozone, oxidize dimethylsulfide (DMS) and hydrocarbons in the gas phase and S(IV) in aerosol solutions, and thereby potentially influence climate. The diurnal cycle of gas-phase Br and the corresponding particulate Br deficits are correlated. Higher values of Br in the gas phase during daytime are consistent with expectations based on photochemistry. We expect that the importance of inorganic Br cycling will vary in the future as a function of both increasing acidification of the atmosphere (through anthropogenic emissions) and climate changes. The latter affects bromine cycling via meteorological factors including global wind fields (and the associated production of sea-salt aerosol), temperature, and relative humidity.

scholarly journals Primary marine aerosol emissions: size resolved eddy covariance measurements with estimates of the sea salt and organic carbon fractions

2007 ◽  
Vol 7 (5) ◽  
pp. 13345-13400 ◽  
Author(s):  
E. D. Nilsson ◽  
E. M. Mårtensson ◽  
J. S. Van Ekeren ◽  
G. de Leeuw ◽  
M. Moerman ◽  
...  
Keyword(s):  
Wind Speed ◽  
Organic Carbon ◽  
Eddy Covariance ◽  
Sea Salt ◽  
Sea Spray ◽  
Marine Aerosol ◽  
Particle Counter ◽  
Wind Speeds ◽  
Sea Salt Aerosol ◽  
Aerosol Emissions

Abstract. Primary marine aerosol fluxes were measured using eddy covariance (EC), a condensation particle counter (CPC) and an optical particle counter (OPC) with a heated inlet. The later was used to discriminate between sea salt and total aerosol. Measurements were made from the 25 m tower at the research station Mace Head at the Irish west coast, May to September 2002. The aerosol fluxes were dominated by upward fluxes, sea spray from bubble bursting at the ocean surface. The sea salt aerosol number emissions increased two orders of magnitude with declining diameter from 1 to 0.1 μm where it peaked at values of 105 to 107 particles m−2s−1. The sea salt emissions increased at all sizes in the wind range 4 to 22 ms−1, in consistency with a power function of the wind speed. The sea salt emission data were compared to three recent sub micrometer sea salt source parameterisations. The best agreement was with Mårtensson et al. (2003), which appear to apply from 0.1 to 1.1 μm diameters in temperate water (12°C) as well as tropical water (25°C). The total aerosol emissions were independent of the wind speed below 10 ms−1, but increased with the wind above 10 ms−1. The aerosol volume emissions were larger for the total aerosol than for the sea salt at all wind speeds, while the sea salt number emissions approached the total number emissions at 15 ms−1. It is speculated that this is caused by organic carbon in the surface water that is depleted at high wind speeds. The data are consistent with an internal aerosol mixture of sea salt, organic carbon and water. Using the aerosol model by Ellison et al. (1999) (a mono-layer of organic carbon surrounding a water-sea-salt brine) we show that the total and sea salt aerosol emissions are consistent. This predict that the organic carbon fraction increase with decreasing diameter from a few % at 1 μm over 50% at about 0.5 μm to about 90% at 0.1 μm, in consistency with simultaneous chemical data by Cavalli et al. (2004). The combined models of Mårtensson et al. (2003) and Ellison et al. (1999) reproduce the observed total aerosol emissions and offer an approach to model the organic sea spray fraction.

scholarly journals Modeling sea-salt aerosol in a coupled climate and sectional microphysical model: mass, optical depth and number concentration

2010 ◽  
Vol 10 (10) ◽  
pp. 24499-24561 ◽  
Author(s):  
T. Fan ◽  
O. B. Toon
Keyword(s):  
Wind Speed ◽  
Size Distribution ◽  
Optical Depth ◽  
Source Function ◽  
Removal Rate ◽  
Global Climate Model ◽  
Number Concentration ◽  
Sea Salt ◽  
Aerosol Size Distribution ◽  
Sea Salt Aerosol

Abstract. Sea-salt aerosol mass, optical depth, and number concentration over the global oceans have significant implications for aerosol direct and indirect climate effects. We modeled sea-salt aerosol in a coupled climate and sectional microphysical model, CAM/CARMA, with aerosol dynamics including sea salt emission, gravitational sedimentation, dry deposition, wet scavenging, and particle swelling. We aimed at finding an integrated sea salt source function parameterization in the global climate model to simultaneously represent mass, optical depth, and number concentration. Each of these quantities is sensitive to a different part of the aerosol size distribution, which requires a size resolved microphysical model to treat properly. The CMS source function introduced in the research, based upon several earlier source functions, reproduced measurements of mass, optical depth and number concentration as well as the size distribution better than other source function choices we tried. However, as we note, it is also important to properly set the removal rate of the particles. The source function and removal rate are coupled in producing observed abundances. We find that sea-salt mass and optical depth peak in the winter, when winds are highest. However, surprisingly, particle numbers and CCN concentrations peak in summer when rainfall is lowest. The quadratic dependence of sea salt optical depth on wind speed, observed by some, is well represented in the model. We also found good agreement with the wind speed dependency of the number concentration at the measurement location and the regional scale. The work is the basis for further investigation of the effects of sea-salt aerosol on climate and atmospheric chemistry.

scholarly journals Modeling sea-salt aerosol in a coupled climate and sectional microphysical model: mass, optical depth and number concentration

2011 ◽  
Vol 11 (9) ◽  
pp. 4587-4610 ◽  
Author(s):  
T. Fan ◽  
O. B. Toon
Keyword(s):  
Wind Speed ◽  
Size Distribution ◽  
Optical Depth ◽  
Source Function ◽  
Removal Rate ◽  
Global Climate Model ◽  
Number Concentration ◽  
Sea Salt ◽  
Aerosol Size Distribution ◽  
Sea Salt Aerosol

Abstract. Sea-salt aerosol mass, optical depth, and number concentration over the global oceans have significant implications for aerosol direct and indirect climate effects. We model sea-salt aerosol in a coupled climate and sectional microphysical model, CAM/CARMA, with aerosol dynamics including sea-salt emission, gravitational sedimentation, dry deposition, wet scavenging, and hygroscopic growth. We aim to find an integrated sea-salt source function parameterization in the global climate model to simultaneously represent mass, optical depth, and number concentration. Each of these quantities is sensitive to a different part of the aerosol size distribution, which requires a size resolved microphysical model to treat properly. The CMS source function introduced in this research, based upon several earlier source functions, reproduces measurements of mass, optical depth and number concentration as well as the size distribution better than other source function choices we tried. However, as we note, it is also important to properly set the removal rate of the particles. The source function and removal rate are coupled in producing observed abundances. We find that sea salt mass and optical depth peak in the winter, when winds are highest. However, surprisingly, particle numbers and CCN concentrations peak in summer when rainfall is lowest. The quadratic dependence of sea-salt optical depth on wind speed, observed by some, is well represented in the model. We also find good agreement with the wind speed dependency of the number concentration at the measurement location and the regional scale. The work is the basis for further investigation of the effects of sea-salt aerosol on climate and atmospheric chemistry.

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