scholarly journals Surface source function for sea-salt aerosol and aerosol dry deposition to the ocean surface

2002 ◽  
Vol 107 (D19) ◽  
Author(s):  
W. A. Hoppel
2003 ◽  
Vol 3 (3) ◽  
pp. 2963-3050 ◽  
Author(s):  
R. Sander ◽  
W. C. Keene ◽  
A. A. P. Pszenny ◽  
R. Arimoto ◽  
G. P. Ayers ◽  
...  

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.


2011 ◽  
Vol 11 (4) ◽  
pp. 11143-11204
Author(s):  
S. Tsyro ◽  
W. Aas ◽  
J. Soares ◽  
M. Sofiev ◽  
H. Berge ◽  
...  

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.


2003 ◽  
Vol 3 (5) ◽  
pp. 1301-1336 ◽  
Author(s):  
R. Sander ◽  
W. C. Keene ◽  
A. A. P. Pszenny ◽  
R. Arimoto ◽  
G. P. Ayers ◽  
...  

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.


2010 ◽  
Vol 10 (10) ◽  
pp. 24499-24561 ◽  
Author(s):  
T. Fan ◽  
O. B. Toon

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.


2011 ◽  
Vol 11 (9) ◽  
pp. 4587-4610 ◽  
Author(s):  
T. Fan ◽  
O. B. Toon

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.


2011 ◽  
Vol 11 (20) ◽  
pp. 10367-10388 ◽  
Author(s):  
S. Tsyro ◽  
W. Aas ◽  
J. Soares ◽  
M. Sofiev ◽  
H. Berge ◽  
...  

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.


2011 ◽  
Vol 11 (10) ◽  
pp. 4833-4850 ◽  
Author(s):  
P. Jiménez-Guerrero ◽  
O. Jorba ◽  
M. T. Pay ◽  
J. P. Montávez ◽  
S. Jerez ◽  
...  

Abstract. A number of attempts have been made to incorporate sea-salt aerosol (SSA) source functions in chemistry transport models with varying results according to the complexity of the scheme considered. This contribution compares the inclusion of two different SSA algorithms in two chemistry transport models: CMAQ and CHIMERE. The main goal is to examine the differences in average SSA mass and composition and to study the seasonality of the prediction of SSA when applied to the Mediterranean area with high resolution for a reference year. Dry and wet deposition schemes are also analyzed to better understand the differences observed between both models in the target area. The applied emission algorithm in CHIMERE uses a semi-empirical formulation which obtains the surface emission rate of SSA as a function of the particle size and the surface wind speed raised to the power 3.41. The emission parameterization included within CMAQ is somehow more sophisticated, since fluxes of SSA are corrected with relative humidity. In order to evaluate their strengths and weaknesses, the participating algorithms as implemented in the chemistry transport models were evaluated against AOD measurements from Aeronet and available surface measurements in Southern Europe and the Mediterranean area, showing biases around −0.002 and −1.2 μg m−3, respectively. The results indicate that both models represent accurately the patterns and dynamics of SSA and its non-uniform behavior in the Mediterranean basin, showing a strong seasonality. The levels of SSA strongly vary across the Western and the Eastern Mediterranean, reproducing CHIMERE higher annual levels in the Aegean Sea (12 μg m−3) and CMAQ in the Gulf of Lion (9 μg m−3). The large difference found for the ratio PM2.5/total SSA in CMAQ and CHIMERE is also investigated. The dry and wet removal rates are very similar for both models despite the different schemes implemented. Dry deposition essentially follows the surface drag stress patterns, meanwhile wet deposition is more scattered over the continent. CMAQ tends to provide larger amounts of SSA dry deposition over the Northern Mediterranean (0.7–1.0 g m−2 yr−1), meanwhile the Southeastern Mediterranean accounts for the maximum annual dry deposition in the CHIMERE model (0.9–1.5 g m−2 yr−1). The wet deposition is dominated by the accumulation mode and is strongly correlated to the precipitation patterns, showing CMAQ a higher wet deposition/total deposition ratio over coastal mountain chains. The results of both models constitute a step towards increasing the understanding of the SSA dynamics in a complex area as the Mediterranean.


2015 ◽  
Vol 101 ◽  
pp. 41-48 ◽  
Author(s):  
M. Spada ◽  
O. Jorba ◽  
C. Pérez García-Pando ◽  
Z. Janjic ◽  
J.M. Baldasano
Keyword(s):  
Sea Salt ◽  

Sign in / Sign up

Export Citation Format

Share Document