scholarly journals A comparison of sea salt emission parameterizations in Northwestern Europe using a chemistry transport model setup

2016 ◽  
Author(s):  
Daniel Neumann ◽  
Volker Matthias ◽  
Johannes Bieser ◽  
Armin Aulinger ◽  
Markus Quante

Abstract. Atmospheric sea salt particles affect chemical and physical processes in the atmosphere. They provide surface area for condensation and reaction of nitrogen, sulfur, and organic species and are a vehicle of transport for these species. Additionally, HCl is released from sea salt. Hence, sea salt has a relevant impact on air quality, particularly in coastal regions with high anthropogenic emissions such as in the North Sea region. Therefore, the integration of sea salt emissions in modeling studies in these regions is necessary. However, it was found that sea salt concentrations are not represented with necessary accuracy in some situations. In this study, three sea salt emission parameterizations depending on different combinations of wind speed, salinity, sea surface temperature, and wave data were implemented and compared: GO03 (Gong, 2003), SP13 (Spada et al., 2013), and OV14 (Ovadnevaite et al., 2014). The aim is to improve modeled atmospheric sea salt concentrations by identifying the parameterization that predicts the sea salt PM10 mass concentrations at different distances to the source regions most accurately and that represents atmospheric sea salt particle size distributions most appropriately in the region under consideration. While the GO03 emissions yielded overestimations in the PM10 concentrations at coastal stations and underestimations of those at inland stations, OV14 emissions, vice versa, led to underestimations at coastal stations and overestimations at inland stations. Because of differently shaped particle size distributions of the GO03 and OV14 emission cases, the deposition velocity of the coarse particles differs between both cases which yields this distinct behavior at inland and coast stations. PM10 concentrations produced by the SP13 emissions generally overestimated measured concentrations. With respect to the size distribution, OV14 produced most accurate coarse particle concentrations, whereas GO03 produced most accurate fine particle concentrations. Overall, GO03 and OV14 produced most accurate results, but both parameterizations still reveal weaknesses in some situations.

2016 ◽  
Vol 16 (15) ◽  
pp. 9905-9933 ◽  
Author(s):  
Daniel Neumann ◽  
Volker Matthias ◽  
Johannes Bieser ◽  
Armin Aulinger ◽  
Markus Quante

Abstract. Atmospheric sea salt particles affect chemical and physical processes in the atmosphere. These particles provide surface area for condensation and reaction of nitrogen, sulfur, and organic species and are a vehicle for the transport of these species. Additionally, HCl is released from sea salt. Hence, sea salt has a relevant impact on air quality, particularly in coastal regions with high anthropogenic emissions, such as the North Sea region. Therefore, the integration of sea salt emissions in modeling studies in these regions is necessary. However, it was found that sea salt concentrations are not represented with the necessary accuracy in some situations.In this study, three sea salt emission parameterizations depending on different combinations of wind speed, salinity, sea surface temperature, and wave data were implemented and compared: GO03 (Gong, 2003), SP13 (Spada et al., 2013), and OV14 (Ovadnevaite et al., 2014). The aim was to identify the parameterization that most accurately predicts the sea salt mass concentrations at different distances to the source regions. For this purpose, modeled particle sodium concentrations, sodium wet deposition, and aerosol optical depth were evaluated against measurements of these parameters. Each 2-month period in winter and summer 2008 were considered for this purpose. The shortness of these periods limits generalizability of the conclusions on other years.While the GO03 emissions yielded overestimations in the PM10 concentrations at coastal stations and underestimations of those at inland stations, OV14 emissions conversely led to underestimations at coastal stations and overestimations at inland stations. Because of the differently shaped particle size distributions of the GO03 and OV14 emission cases, the deposition velocity of the coarse particles differed between both cases which yielded this distinct behavior at inland and coastal stations. The PM10 concentrations produced by the SP13 emissions generally overestimated the measured concentrations. The sodium wet deposition was generally underestimated by the model simulations but the SP13 cases yielded the least underestimations. Because the model tends to underestimate wet deposition, this result needs to be considered critically. Measurements of the aerosol optical depth (AOD) were underestimated by all model cases in the summer and partly in winter. None of the model cases clearly improved the modeled AODs. Overall, GO03 and OV14 produced the most accurate results, but both parameterizations revealed weaknesses in some situations.


2012 ◽  
Vol 12 (21) ◽  
pp. 10161-10179 ◽  
Author(s):  
C. Ochoa ◽  
D. Baumgardner ◽  
M. Grutter ◽  
J. Allan ◽  
J. Fast ◽  
...  

Abstract. This study extends the work of Baumgardner et al. (2009) in which measurements of trace gases and particles, at a remote, high altitude mountain site, 60 km from Mexico City were analyzed with respect to the origin of the air masses. In the current evaluation, the temperature, water vapor mixing ratio (WMR), ozone (O3), carbon monoxide (CO), sulfur dioxide (SO2) and acyl peroxy nitrate (APN) are simulated with the WRF-Chem chemical transport model and compared with the measurements at the mountain site. Comparisons between the model and measurements are also evaluated for particle size distributions (PSDs) of the mass concentrations of sulfate, nitrate, ammonium and organic mass (OM). The model predictions of the diurnal trends in temperature, WMR and trace gases were generally well correlated; 13 of the 18 correlations were significant at a confidence level of <0.01. Less satisfactory were the average hourly differences between model and measurements that showed predicted values within expected, natural variation for only 10 of the 18 comparisons. The model performed best when comparing with the measurements during periods when the air originated from the east. In that case all six of the parameters being compared had average differences between the model and measurements less than the expected standard deviation. For the cases when the air masses are from the southwest or west northwest, only two of the comparisons from each case showed differences less than the expected standard deviation. The differences appear to be a result of an overly rapid growth of the boundary layer predicted by the model and too much dilution. There also is more O3 being produced, most likely by photochemical production, downwind of the emission sources than is predicted by the model. The measured and modeled PSD compare very well with respect to their general shape and the diameter of the peak concentrations. The spectra are log normally distributed with most of the mass in the accumulation mode centered at 200 ± 20 nm and little observed or predicted changes with respect to the time when the RML is above the Altzomoni research station. Only the total mass changes with time and air mass origin. The invariability of average diameter of the accumulation mode suggests that there is very little growth of the particles by condensation or coagulation after six hours of aging downwind of the major sources of anthropogenic emissions in Mexico's Megapolis. This could greatly simplify parameterization in climate models although it is not known at this time if this invariance can be extended to other megacity regions.


2012 ◽  
Vol 12 (4) ◽  
pp. 9813-9856
Author(s):  
C. Ochoa ◽  
D. Baumgardner ◽  
M. Grutter ◽  
J. Allan ◽  
J. Fast ◽  
...  

Abstract. This study extends the work of Baumgardner et al. (2009) in which measurements of trace gases and particles, at a remote, high altitude mountain site, 60 km from Mexico City were analyzed with respect to the origin of the air masses. In the current evaluation, the temperature, water vapor, ozone (O3), carbon monoxide (CO), acyl peroxy nitrate (APN) and particle size distributions (PSDs) of the mass concentrations of sulfate, nitrate, ammonium and organic mass (OM) were simulated with the WRF-Chem chemical transport model and compared with the measurements at the mountain site. The model predictions of the diurnal trends of the gases were well correlated with the measurements before the regional mixed layer (RML) reached the measurement site but underestimated the concentration after that time. The differences are caused by an over rapid growth of the boundary layer by the model and too much dilution. There also is more O3 being actually produced by photochemical production downwind of the emission sources than predicted by the model. The measured and modeled PSDs compare very well with respect to their general shape and diameter of the peak concentrations. The spectra are lognormal with most of the mass in the accumulation mode and the geometric diameter centered at 200±20 nm, showing little observed or predicted change with respect to the time when the RML is above the Altzomoni research station. Only the total mass changed with time and air mass origin. The invariability of average diameter of the accumulation mode suggests that there is very little growth of the particles by condensation or coagulation past about six hours of aging downwind of the major sources of anthropogenic emissions in Mexico's Megapolis. This could greatly simplify parameterization in climate models although it is not known at this time if this invariance can be extended to other megacity regions.


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